Exploiting bond exchange reaction to optimize mechanical properties of 3D printed composites

By Audrey Laventure, Community Board member.

Additive manufacturing is a polymer processing method enabling the preparation of 3D architectures with a high level of design freedom. While some of the additive manufacturing technologies, such as fused deposition modeling (FDM) are commonly used at an industrial level for prototyping, there are still numerous challenges to tackle for achieving a 3D architecture that possesses state-of-the-art thermomechanical properties, compared to those obtained via conventional methods. Considering the sustainability aspect of the selected additive manufacturing method, including the management of the failed 3D parts, is also of utmost importance in the context of sustainable laboratories.

As recently reported by Jiang et al., there are additional challenges for the additive manufacturing of continuous fiber composites which are made of a carbon fiber that is surrounded by a polymer matrix. FDM is often used to prepare such samples, where the continuous carbon fiber and the thermoplastic filament are fed separately during the processing of the materials. While this strategy works to produce continuous fiber composites, the resulting mechanical properties are mostly dictated by those of the thermoplastic polymer. To optimize the mechanical properties of such samples, an interesting alternative strategy consists of using a thermoset polymer matrix processed via direct-ink writing (DIW). While some successes have been reported exploiting DIW, the rheological properties of the thermoset in the pre-printing stage needs to meet specific requirements to enable the extrusion of the formulation, including shear-thinning and thixotropy. The solidification kinetics of the thermoset formulation occurring upon exposure of the 3D printed formulation to heat is usually slow and leads to a uniform curing, but also leads to difficulties in obtaining a 3D printed architecture with a high level of post-treatment print fidelity. To circumvent this problem, UV curable resins, once again printed via direct-ink writing, can be used as a polymer matrix for the continuous fiber composite as their solidification kinetics are often faster than those of thermosets. While this process is efficient, the presence of the continuous fiber may impede the penetration of the irradiation, usually leading to a fast yet non-uniform curing.

To address the challenges involved in the preparation of continuous fiber composites linked to the DIW of either the thermoset or the UV curable resin, Jiang et al. designed a formulation capable of undergoing a two-stage curing process, therefore successfully combining the advantages of both UV curing (fast solidification) and heat-based curing (uniform curing). They combined the 2-hydroxy-3-phenoxypropyl acrylate monomer, the phenylbis (2,4,6-glycerolate diacrylate) photoinitiator, and a triazabicyclodecene as the bond exchange reaction catalyst. As illustrated in Figure 1, the first stage (UV irradiation) allows for the free-radical polymerization to occur while the second stage (heat) is used to increase the resulting material’s crosslinking density via the transesterification reactions occurring between the hydroxyl and the ester functional groups of the material.

Figure 1. a) Chemical structures composing the two-stage curable resin undergoing b) UV curing and c) heating illustrating the bond exchange reaction involved in the optimization of the thermomechanical properties of the 3D printed architectures. Reproduced from DOI: 10.1039/d3mh01304a with permission from the Royal Society of Chemistry.

This transesterification, also referred to as bond exchange reaction, is crucial to optimize the thermomechanical properties of the 3D printed continuous fiber composites, which results in high performance applications for these architectures. Jiang et al. reported not only a ~11-fold increase in the modulus of the two-stage cured samples compared to the UV cured only samples, but also a better adhesion (referred to as welding) between the layers deposited on top of one another. This enhanced adhesion is a consequence of the covalent bond created between the layers upon the heating step which is, once again, facilitated by the bond exchange reaction.

The capability of the 3D printed architectures to undergo bond exchange reaction also allows for the repairing and reshaping of the architectures. It was shown that the 3D printed architectures could be recycled via depolymerization in ethylene glycol at high temperature (160°C), which is an important asset for a thermoset based composite, especially in the context of sustainable materials and processing. This proof-of-concept has been extended to acrylate/epoxy-based commercial resins, opening the door to fundamental studies of the mechanisms of bond exchange reactions in similar resins where further understanding of the structure-processing-property relationships could be established to lead to the rational design of custom resins for the 3D printing of continuous fiber composites.

To find out more, please read:

3D Printing of continuous fiber composites using two-stage UV curable resin
Huan Jiang, Arif M. Abdullah, Yuchen Ding, Christopher Chung, Martin L. Dunn and Kai Yu
Mater. Horiz., 2023, 10, 5508-5520, DOI: 10.1039/D3MH01304A

 


About the blogger


 

Audrey Laventure is an assistant professor in the Department of Chemistry at the Université de Montréal (UdeM), QC, Canada, and a member of the Materials Horizons Community Board. Since 2021, she holds the Canada Research Chair in Functional Polymer Materials. Her expertise lies at the intersection of physical chemistry, polymer processing and advanced materials characterization. In 2023, Audrey was selected to lead the molecular materials axis of the new Institut Courtois at UdeM. Audrey was also part of the first Youth Council of the Chief Science Advisor of Canada (2020-2023) and the Science Meets Parliament 2023 cohort.

 

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Revolutionary Room-Temperature F-Ion Batteries: Harnessing Sulfone Electrolytes and Anion Acceptor Additives

By Edison Huixiang Ang, Community Board member.

In the realm of large-scale energy storage, the quest for low-cost, high-energy battery technologies has spurred the emergence of various alternatives. Lithium batteries utilizing Co-free conversion-type cathodes, alongside multivalent cation, and halogen anion batteries, stand out among the contenders. Conversion-type cathodes like iron fluorides in lithium batteries offer cost efficiency, higher capacity, and higher energy density compared to cathodes containing expensive transition metals. However, the use of lithium metal anodes presents safety and cost challenges, inhibiting effective real-world battery performance. Similarly, while multivalent cation batteries, such as those based on Mg2+, boast abundant reserves, their strong coulombic interactions with host materials create challenges with charge carrier migration. To address these issues and develop batteries with favourable reaction kinetics and reversibility, the burgeoning field of halogen anion batteries, particularly fluoride ion batteries (FIBs), holds promise.

 

Fig. 1 Preparation and characterization of electrolytes. (a) Preparation process of the CTD3 electrolyte. (b) Illustration of adsorption of the TG molecule to F and its adsorption energy. (c) 1 H NMR spectra of TG, CTD1 and CTD3. (d) FT-IR spectrum of CTD3. Reproduced from DOI: 10.1039/D3MH01039B with permission from the Royal Society of Chemistry.

 

FIBs, leveraging the unique properties of fluorine as the lightest and most electronegative element among halogens, offer the highest theoretical energy density. Despite this potential, realizing practical applications has been hindered by the lack of suitable electrolytes with high ionic conductivity at room temperature. The insolubility of fluoride salts in aprotic solvents has been a primary challenge. While boron-based anion acceptors (AAs) aid in dissociating fluoride salts, their strong Lewis acidity impedes fluoride transport, leading to unsatisfactory electrolyte conductivity. Addressing this limitation, a novel AA with mild Lewis acidity has been developed, facilitating fluoride salt dissociation while avoiding strong AA-F bonding. This breakthrough enables prepared electrolytes to achieve high ionic conductivity, reaching up to 2.4 mS cm-1 at room temperature, enabling successful FIB operation with a reversible capacity of 126 mA h g-1 after 40 cycles.

Moreover, understanding the regulation effect of salt concentration on the cathode interface has unveiled insights into improving FIB performance, emphasizing the critical role of rational electrode-electrolyte interface design in future FIB development. FIBs hold significant promise owing to their potential for high energy density and favourable compatibility with high-voltage electrode materials. Notably, fluorine’s abundance—two orders of magnitude higher in global production than lithium—further accentuates their appeal. Conversion-type FIBs, with a theoretical energy density of 5000 W h L-1, exhibit substantial energy density even at leaner stack levels, offering a cost as low as $20 per kW h-1 according to techno-economic analysis. Despite these merits, the experimental realization of the remarkable energy density of FIB is hindered by the lack of well-tailored electrolytes with suitable ionic transport abilities and electrochemical stability.

Liquid electrolytes for FIBs have garnered interest due to their high room-temperature ionic conductivity and better wettability compared to solid-state electrolytes. However, challenges persist, mainly the insolubility of fluoride salts in regular organic aprotic solvents due to strong electrostatic interactions. To address this, efforts have been directed toward designing softer Lewis acidity AAs that facilitate fluoride salt dissolution without excessive solvation, crucial for practical liquid electrolytes. Innovations in this work have introduced a novel sulfone electrolyte based on a new molecular-type H-donor AA (6-thioguanine, TG) with moderate Lewis acidity. Demonstrated through various analyses, this electrolyte achieves impressive ionic conductivity at room temperature, enabling the reversible cycling of FIBs. The superior reversibility is attributed to the electrolyte’s high ionic conductivity, improved desolvation capability of fluoride ions, and a well-designed interface layer.

In summary, the pioneering advancements in electrolyte design for fluoride ion batteries set the stage for increasingly viable and effective energy storage solutions, offering improved reversibility and reliable performance at ambient temperatures.

To find out more, please read:

Room-temperature reversible F-ion batteries based on sulfone electrolytes with a mild anion acceptor additive
Yifan Yu, Meng Lei and Chilin Li
Mater. Horiz., 2023, Advance Article, DOI: 10.1039/D3MH01039B

 


About the blogger


 

Edison Huixiang Ang serves as an Assistant Professor at the National Institute of Education/Nanyang Technological University, Singapore, and a member of the Materials Horizons Community Board. Dr. Edison specializes in nanotechnology, particularly exploring 2D nanomaterials for applications in energy storage, membrane technology, catalysis, and sensors. Stay updated on his work by following him on X (formerly Twitter) @edisonangsg.

 

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Materials Horizons 10th Anniversary ‘Community Spotlight’ – Meet our Emerging Investigators Part 3

Introducing Materials Horizons’ Emerging Investigators 2022.

This year we are pleased to celebrate the tenth anniversary of Materials Horizons. We are so grateful to our fantastic community of authors, reviewers, Board members and readers and wanted to showcase just some of them in a series of ‘Community Spotlight’ blog articles.

In our fifth ‘Community Spotlight’, we feature some of our past ‘Emerging Investigators’ who have contributed their outstanding research to Materials Horizons.

Our Emerging Investigators series highlights early career scientists who have excelled in their field and work to provide quality research and communications in order to contribute to the constant evolution of chemical sciences. We asked some of our past Emerging Investigators about their experience as up-and-coming researchers and how their work has developed from early career stage to now. Check out their interview responses below.

 

Dr. Filip Podjaski, Emerging Investigator 2022

Imperial Collage London, UK

“My parents immigrated from Poland to Germany when I was a child. I grew up bilingually, which was very helpful to learn foreign languages (English, French, Spanish, Russian) and to get in touch with different cultures and mindsets. Since adolescence I was fascinated by the natural sciences and what technologies they enable. Consequently, I studied physics, at the University of Göttingen (D) and in Lyon (FR) with a focus on material properties and energy related applications.

During my PhD in the Nanochemistry department (Prof. Lotsch) at the MPI for Solid State Research (D) and at EPFL (CH), I broadened my horizons in physical chemistry and worked on photocatalysis and electrocatalysis for green hydrogen production as well as on organic materials combining light absorption and battery like energy storage intrinsically – a new and promising technology still fascinating me. I hence stayed at MPI as postdoc and became group leader to drive its development for 3 more years. Research placements at UC Santa Barbara, USA (Prof. Seshadri) and in the Institute of Material Science Seville, ES (Prof. Míguez) strongly enriched me.

Since August 2022, I am a UKRI Research Fellow in the group of Prof. James Durrant, Imperial College London (UK), where I deepen my knowledge in probing fundamental photophysical properties of light driven organic semiconductors on different time scales to better understand and tailor their function for solar fuel production.

My research interests are related to energy conversion applications and tailored material property modifications, which can be driven by light or electricity. They span over the disciplines of physics and chemistry, and partially affect biomedical applications.

 

Being concerned by increasing environmental challenges, I focus on fundamental processes of electrocatalytic and photocatalytic renewable fuel synthesis, mostly for green hydrogen production. Especially complex and organic based semiconductor systems fascinate me in this context, since they are tailorable bottom-up in principle in their structure and function. But there is much to discover about their photophysical properties and its coupling to performance. At Imperial College London, I currently investigate which chemical adaptations are helpful to make organic photocatalysts work efficiently in more natural environments, and not only in ultra-pure lab conditions.

 

Photocharging materials and resulting property modification effects are my other main research interest. Such a function typically relies on ionic interactions and goes in hand with energy and information storage. But relatively little is known about this growing field. I am keen to explore their thermodynamic and kinetic property requirements, to establish efficient structure-property relationships and new technological applications for such novel and adaptive materials. Examples for photocharging materials’ applications I recently showed with colleagues are solar batteries that enable to use renewable electricity on demand, or photo-memristive sensors that intrinsically store concentration information of analytes they can interact with in biological contexts. Light-driven micro-robotics I studied with colleagues from MPI-IS (Prof. Sitti) in biological contexts are another practical example. Remote charging or propulsion by light, as well as its use for local sensing and drug delivery has exciting potential. And if such materials and devices were tailored from organic semiconductors, more technology could become fully green and sustainable.”

 

What inspired you to pursue a career in your specific field of research?

“Primary inspiration probably came from good teachers at school (math, physics, chemistry). I chose a career in applied natural sciences for three reasons: (i) personal curiosity for profound understanding of physics and chemistry and how this translates into technology, (ii) for altruistic reasons – I wanted to contribute something good, new and lasting to our society by research and development, and (iii) because of my creativity and joy in working with different people, which in my opinion is best applied in natural sciences and with academic freedom. Research on renewable energy conversion and sustainable fuel production (photocatalysis, electrocatalysis) was my first choice due to its obvious immediate need, and because it requires interdisciplinary knowledge I wanted to develop. My enthusiastic PhD supervisors Prof. Bettina Lotsch and Prof. Anna Fontcubetra i Morral, as well as my current host and mentor Prof. James Durrant further inspired me as people who take a lot of joy and personal energy from driving fundamental research and understanding. Further inspiration comes from amazing community feedback on the relatively new topic of photocharging materials. I want to focus even more on it in future – for its relevance to energy supply technology and its broad applicability beyond (see next question). The interdisciplinary and creative research required here is also a beautiful challenge and inspiration to me.”

 

What are some of the current trends or emerging areas of research within your field that you find particularly exciting or promising?

“I think the relatively young research area of photocharging materials is particularly exciting and promising. Combing the function of solar cells and batteries in single bifunctional materials is what I feel is highly demanded in times of climate change and (potential) conflicts arising for access to natural resources. However, photo-battery concepts relying on such bifunctional materials are still scarce, have very limited efficiencies and require much more research. Photocharging effects can in principle also affects materials used for photoelectrochemistry or photocatalysis, which become more efficient due to doping or trap passivation going in hand with photo-induced charge accumulation. In parallel, structural and physical or chemical material properties can be modified by photocharging, akin to photo-switches. Their analysis can be used for sensing applications. Related research areas are the just emerging optoionics, where light induces changes in ionic concentrations and conductivity, thereby potentially improving material performance. Since photocharging can also be seen as memristive effect that captures light driven processes over time, its use for information processing is also foreseeable. Memristors as logical circuit elements are also being discussed for so called neuromorphic computing and information processing applications that could well interface with next generation IT or biomedical applications. I would be happy to help developing these areas. It represents a complex field bridging semiconductor physics, battery research, electrochemistry, photocatalysis and engineering, which are rarely combined. So little people have a holistic view and understanding. But I hope that it will change soon and that more and more people will follow up.

In terms of solar fuel production, I think that hydrogen is obviously of highest relevance. Especially when it comes to its generation by cost-efficient organic based materials and in more natural conditions, which is rarely the case, more research is needed. We need hydrogen not only as energy carrier, but also for other (photo)synthetic process such as syngas and ammonia production. In line with this, I am highly convinced of the promise in nitrogen reduction research, since ammonia is one of the products. Besides being a convenient, safe and high energy density fuel, it is also required for many industrialized processes and fertilizer synthesis, while already having a good distribution infrastructure.”

 

Read Filip’s featured Materials Horizons article here:

Photomemristive sensing via charge storage in 2D carbon nitrides.

Andreas Gouder, Alberto Jiménez-Solano, Nella M. Vargas-Barbosa, Filip Podjaski and Bettina V. Lotsch.

Mater. Horiz., 2022,9, 1866-1877. DOI: 10.1039/D2MH00069E

 

 

 

Dr Jie Jang, Emerging Investigator 2022

Central South University, China

 

Jie Jiang is an Associate Professor of School of Physics and Electronics at Central South University. He obtained the B.E. degree (2007), M.E. degree (2009), and the Ph.D. degree (2012) from Hunan University. He was a Post-doctoral Fellow in Nanyang Technological University (2012-2013 in Singapore) and Auburn University (2014-2015 in USA), respectively. His research interests focus on neuromorphic photoelectric hybrid devices based on thin-film oxide and 2D semiconductor materials. He is the Youth Editor in Nano-Micro Letters, Science China-Materials, Brain-X, International Journal of Extreme Manufacturing. He has published as first author/corresponding author about 60 papers which are often highlighted by NPG Asia Materials, Material Views-China, X-MOL, etc.

 

What inspired you to pursue a career in your specific field of research?

“When I was young, I was very interested in nature. When I grew up, I was more interested in the mathematics. However, I wanted to start my research career facing modern industry. Therefore, my current research is focused on the advanced semiconductor devices, especially for the neuromorphic intelligent devices.”

 

How would you summarise the research which lead to your recognition as an Emerging Investigator for Materials Horizons?

“I think the polarization light detector has seen growing attention. However, my research demonstrates that it can also extended to be used in the polarization-sensitive neuromorphic computing which has been never reported. It may provide a promising opportunity for the next-generation of intelligent optoelectronics.”

 

Since becoming an Emerging Investigator, how do you feel your research has developed over time?

“I am very honored to be an Emerging Investigator. It seems that my research has gone well since.”

 

What are some of the current trends or emerging areas of research within your field that you find particularly exciting or promising?

“I think the chip-integrated neuromorphic electronics and polarization-perceptual neuromorphic optoelectronics are two exciting points in my research field.”

 

What advice would you give to aspiring scientists who hope to make a significant impact in their respective fields?

The interest is most important thing. The research should also be guided toward the direction which is most different from others.”

 

What are some of the main challenges or obstacles you have encountered while conducting your research, and how have you overcome them?

“Sometimes my lab doesn’t have the equipment we need. Therefore, we must either get help from others or do the work that we can.”

 

Read Dr Jang’s featured Materials Horizons article here:

Polarization-perceptual anisotropic two-dimensional ReS2 neuro-transistor with reconfigurable neuromorphic vision.

Dingdong Xie, Kai Yin, Zhong-Jian Yang, Han Huang, Xiaohui Li, Zhiwen Shu, Huigao Duan, Jun He and Jie Jiang.

Mater. Horiz., 2022,9, 1448-1459. DOI: 10.1039/D1MH02036F

 

 

 

Dr Mohammad Mirkhalaf, Emerging Investigator 2022

Queensland University, Australia.

Mohammad Mirkhalaf is a Lecturer and ARC DECRA fellow at the Queensland University of Technology (QUT). He has obtained his PhD from McGill University, Master’s from Nanyang Technological University (NTU), and Bachelor’s from Isfahan University of Technology (IUT). After finishing PhD in 2015, he joined the National Research Council of Canada as a postdoctoral fellow working closely with his previous lab at McGill till August 2018 when he joined the University of Sydney. He joined QUT in Jan 2022. His research is on tailoring materials’ internal architecture to achieve properties and functionalities beyond those of constituents.

 

What inspired you to pursue a career in your specific field of research?

“We are all part of nature. After all, we can be perceived as live materials with intelligence. Doing research in natural and bioinspired materials has been perhaps a way for me to try to understand nature and, as such, human better.”

 

 

How would you summarise the research which lead to your recognition as an Emerging Investigator for Materials Horizons?

“Besides research, recognition is a result of being with supportive and understanding people. Let us pay our deepest respect to the people who contribute to providing supportive environments for their younger (and usually less experienced) colleagues.

In terms of research, whatever is triggered by scientific curiosity is exciting: enthusiasm to understand something better or to develop something new or more efficient brings the capacity to do so. We should just not forget that it takes time and continuous effort. I think the research that was kindly highlighted in the emerging investigator series was driven by the excitement to find a way to form ceramics into complex shapes using an efficient and relatively easy pathway.“

 

Since becoming an Emerging Investigator, how do you feel your research has developed over time?

“I think trust is a fundamental element in progress. Trust in your ability to do something but also trust in people who are there to help you. I think being featured as an emerging investigator strengthened both elements (of trust) in me. Thanks for the opportunity.”

 

What are some of the current trends or emerging areas of research within your field that you find particularly exciting or promising?

“We do certain things to pay our bills and have a protective roof. But beyond that, whatever we do should be responsibly done for the next generations. They are our continuation. With their being is our being. So in the future, I will aim to find ways to perform my research (which is on developing new materials and architectures) sustainably from nature, for nature (all beings), to nature.

We are going to lack resources and so are in search of life/resources on other planets. Much research, including on new materials, is channelled towards this goal. The question is: if in this search for life in other planets, we are harming our own earth, aren’t we defeating the purpose? We perhaps need to first keep our mother earth as intact as possible through sustainable technologies and then satisfy our other curiosities based on this principle of sustainability. We (scientists and engineers) can play a major role here. Other areas that interest me currently are using engineering mechanisms to reversibly and drastically tailor the internal architecture of materials, and the ethical aspects of live materials and artificial intelligence.”

 

What advice would you give to aspiring scientists who hope to make a significant impact in their respective fields?

“I am still in the early- to-mid stages of my career, so I am not sure if I am eligible to answer this question. But I am happy to have a discussion on this. I guess one important aspect is to go to the core of the problem. Every problem has a surface, but the beauty lies within the deeper layers. For example, a few hundred years ago, a designer could think of this problem: how thick the feet of a wooden chair should be to resist one’s weight? Or going to deeper layers, one could ask: what governs the deformation and failure of the chair’s feet? How can we prevent excessive deformation/failure? Are these governing rules the same for all materials? Trying to answer the latter set of questions has led to significant contributions to the mechanics of materials. Answering the former question would result in a chair on which people could sit. Both are valuable but satisfy different desires.

I think another key is trust as we discussed. There are elite people in academia who know much more than early career researchers about academic progress/potential. Being in touch with these people and trusting them brings stability and focus to a curious soul.”

 

What are some of the main challenges or obstacles you have encountered while conducting your research, and how have you overcome them?

“Our biggest enemy lies within us. In search of truth, one should be truthful. I must admit it might be hard for a scientific mind to carry the burden of a societal construction and politics that tend to be quite good at (sometimes) bending the truth. But we (humans) have made significant progress in discovering the essence of things properly, and I think we will get better. Intellectuals, many of whom work in academia (including my current and previous mentors), have taught us the way to scientific discoveries: reading/understanding the literature, discussing it, accepting criticisms and strong arguments even though they go against our thoughts, fact-checking, and readiness to reconstruct thoughts if needed. These are the principles I try to follow to tackle challenges. Thanks for the opportunity to discuss thoughts.”

 

Read Mohammad’s featured Materials Horizons article here:

Rationally-designed self-shaped ceramics through heterogeneous green body compositions.

Zizhen Ding, Hala Zreiqatbc and Mohammad Mirkhalaf.

Mater. Horiz., 2022,9, 2762-2772. DOI: 10.1039/D2MH00785A

 

 

 

Dr Kai Wang, Emerging Investigator 2022

Soochow University, China

 

Kai Wang received his BSc degree from the Department of Materials Science and Engineering, Beihang University in 2012, and received his PhD degree from the Technical Institute of Physics and Chemistry of Chinese Academy of Sciences in 2017. Then, he carried out postdoctoral research at the Institute of Functional Nano & Soft Materials (FUNSOM), Soochow University.  Now, he is an associate professor at Soochow University. His research interest mainly focuses on high-performance organic optoelectronic materials and their device applications.

 

How would you summarise the research which lead to your recognition as an Emerging Investigator for Materials Horizons?

“The purpose of the research is to address fundamental questions regarding the spectral broadening and concentration quenching in solid-state multiple resonance (MR) type thermally activated delayed fluorescence (TADF) systems. Previous studies often overlooked or briefly mentioned these issues as they focused primarily on developing new materials. However, these issues are crucial in understanding the behaviour of MR-TADF systems in solid states. Our research is the first to comprehensively investigate and provide answers to these general questions. We have determined that spectral broadening is caused by the formation of excimers resulting from π-π interactions, while concentration quenching is a result of triplet exciton annihilation. These findings are essential for a deeper understanding of the behaviour of MR-TADF systems.”

 

What are some of the current trends or emerging areas of research within your field that you find particularly exciting or promising?

“In my view, the emerging category of materials known as multiple resonance (MR) emitters and their associated device applications are highly promising in the realm of organic light-emitting diodes (OLEDs). These materials have the ability to achieve remarkably efficient narrowband emission, surpassing even that of inorganic systems. This challenges our existing understanding of organic systems and allows OLEDs to remain competitive in the era of ultrahigh definition displays. Moreover, they hold significant potential for use in organic laser diodes, a shared aspiration among researchers in the field of organic optoelectronics.”

 

Read Kai Wang’s featured Materials Horizons article here:

Distinguishing the respective determining factors for spectral broadening and concentration quenching in multiple resonance type TADF emitter systems.

Feng Huang, Xiao-Chun Fan, Ying-Chun Cheng, Hao Wu, Yi-Zhong Shi, Jia Yu, Kai Wang, Chun-Sing Lee and Xiao-Hong Zhang.

Mater. Horiz., 2022,9, 2226-2232.  DOI: 10.1039/D2MH00511E

 

 

We hope you enjoy reading these interviews from our Emerging Investigators. You can find all our past Emerging investigator editorials and featured articles here:

 

Emerging Investigators 2020/2021

Emerging Investigators 2022/2023

 

Or to read more of our community spotlight blog, return to the home page here

 

 

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Materials Horizons Community Spotlight – Celebrating ten years of insight and impact with our scientific collaborators

Welcome to the Materials Horizons Community Spotlight

To celebrate our wonderful community of authors, reviewers, and board members we would like to introduce you to them, their roles in the community and their current research through our Community Spotlight blog series. This special series include some of the people who have, over the past 10 years, helped to shape and transform Materials Horizons into the cutting edge, insightful and impactful journal that it is today.

This collection of blog posts started in July 2023 with the first introduction to our esteemed Advisory Board. Each month since we have followed this with introductions to some of our very first Materials Horizons Emerging Investigators from 2020 and 2021 and a selection of our nominated Outstanding Reviewers from past years.

 

Read the first of the Community spotlight series here:

Materials Horizons Advisory Board

Meet the Advisory Board Part 1

Meet the Advisory Board Part 2

Meet the Advisory Board part 3

 

 

 

 

Read the second edition of the Community spotlight series here:

Materials Horizons Emerging Investigators

Introducing our Emerging Investigators – Part 1

 

 

Introducing our Emerging Investigators – Part 2

Introducing our Emerging Investigators – Part 3

 

 

 

Finally in our third edition of the series:

Materials Horizons Outstanding Reviewers 

 

Meet some of our Outstanding Reviewers


 

 

We would like to offer a heart felt thank you to all our scientific community who play a role in shaping Materials Horizons into the successful journal that it is today. We hope you enjoy reading more about all of these fantastic people and keep your eyes peeled for more additions to the Community Spotlight series!

 

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Enhancing photodynamic therapy (PDT) with a biocompatible pure organic nanocage

By Quan Li, Community Board member.

The advantages of minimal invasiveness, excellent biocompatibility, and high spatiotemporal control manners have enabled photodynamic therapy (PDT) to be utilized as a novel alternative to conventional cancer treatment approaches. PDT relies on photosensitizers (PSs) to photochemically react with the ground-state oxygen molecules (oxygen, 3O2) or small molecules, generating highly toxic reactive oxygen species (ROS) under light irradiation in situ, to further induce tumor cell apoptosis or necrosis, vascular damage or cancer-mediated immunity, for example.

Since the first discovery of PSs based on hematoporphyrin derivatives (HpD) in 1960, the porphyrin-based PSs and their PDT performance have been extensively explored. Currently, various porphyrin-based PSs with different structures such as verteporfin, porfimer sodium, temoporfin and photocarcinosin have been approved for clinical practice. Despite great progress in clinical practice, the ROS generation of these porphyrin-based PSs is still far from satisfactory. One of the main issues is their large planar and rigid structures, which tend to form tight aggregates with strong π…π interactions at high concentrations in aqueous solutions or at tumor tissues. Such π…π stacking will cause diminished fluorescence and compromised ROS, leading to low PDT efficacy.

To weaken π…π stacking of porphyrin-based PSs, boost the generation of ROS, and enhance the PDT efficacy, work by Zhu, Zhang et al recently reported a novel biocompatible pure organic porphyrin nanocage (Py-Cage) with significantly improved ROS generation and PDT performance. Their design of the Py-Cage highlights the large cavity and long distance which effectively weaken the π…π stacking effect of porphyrins within the nanocage. Hence this Py-Cage exhibits excellent anti-ACQ features at high concentrations in aqueous solution (Figure 1a,b,c).

Fig 1. (a) and (b) Schematic comparison between traditional planar porphyrin-based photosensitizers and the porous porphyrin nanocage in attenuating the ACQ effect. (c) Schematic illustration of the enhanced ROS generation for cationic organic nanocage Py-Cage. (d) Tumor pictures of 4T1 tumor-bearing mice after different treatments (for Py-cage samples). (e) Schematic of Py-Cage NPs synthesized by a nanoprecipitation method with DSPE-PEG2000 as the encapsulation matrix. (f) Tumor pictures of 4T1 tumor-bearing mice in different groups (for Py-cage NPs samples). Reproduced from DOI: 10.1039/D3MH01263H with permission from the Royal Society of Chemistry.

A systematic comparative investigation shows that the Py-Cage can largely boost ROS generation that is superior to its PyTtDy precursor as well as widely used PSs, including Chlorin E6 (Ce6) and Rose Bengal (RB). Having established the excellent ROS generation and bright fluorescence of the Py-Cage, the team then evaluated its in vitro PDT performance using mouse breast cancer 4T1 cell. The data shows the Py-Cage can generate a large amount of ROS in cells under white light irradiations to induce cell apoptosis and death. Encouraged by the very promising in vitro results, Zhu, Zhang et al. further conducted in vivo PDT trials of the Py-Cage using a 4T1 tumor bearing mouse model. Their findings indicate that the tumors in the Py-Cage+light group showed the smallest sizes and lowest tumor weights among all the tested groups (Figure 1d), reflecting the best tumor growth inhibition performance of Py-Cage under light. The biocompatibility of the Py-Cage was also investigated by analyzing the blood routine and biochemical parameters of the rats after 48 h injection through tail veins. All the results show that the Py-Cage does not cause infection and bleeding symptoms and no damage to the liver and kidney function was observed. Other parameters such as cholesterol (CHO), triglyceride (TG), high-density lipoprotein cholesterol (HDL), low-density lipoprotein (LDL), glucose level were also not affected by Py-Cage. Moreover, the team prepared the Py-Cage nanoparticles by a nano-precipitation method to improve its water disability and biocompatibility. Similar in vitro and in vivo PDT experiments with these Py-Cage NPs were conducted and the NPs also proved to be excellent in biocompatibility and PDT efficacy (Figure 1e,f).

In summary, this work demonstrated the first porphyrin-based pure porous organic nanocage (Py-Cage) with a large cavity volume to promote both type-I and type-II ROS generation. Through comprehensive in vitro and in vivo studies, the Py-Cage proved to be extremely powerful in PDT with excellent biocompatibility and enhanced anti-tumor efficacy. The design of Py-Cage with a pure organic porous skeleton could avoid the π…π stacking to fully utilize the excited triplet state of PSs to generate ROS. This design strategy will offer enormous prospects for preparing novel and effective PSs with excellent biocompatibility for PDT and related phototheranostic applications.

 

To find out more, please read:

A biocompatible pure organic porous nanocage for enhanced photodynamic therapy
Zhong-Hong Zhu, Di Zhang, Jian Chen, Hua-Hong Zou, Zhiqiang Ni, Yutong Yang, Yating Hu, Ruiyuan Liu, Guangxue Feng, Ben Zhong Tang
Mater. Horiz. 2023, 10, 4868-4881, DOI: 10.1039/D3MH01263H

 


About the blogger


 

 

Quan Li is currently a Professor at Tianjin University of Traditional Chinese Medicine and a member of the Materials Horizons Community Board. Prof. Li’s research lab focuses on the design and preparation of soft matter materials based on light-responsive molecular machines and Chinese herbal medicine for biomedical applications, including anti-cancer, skin disease treatment, and others.

 

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Congratulations to the winners of the Materials Horizons prizes at MATSUS Fall 2023

Materials Horizons were delighted to sponsor two student prizes at the #BIOELCHEM symposium at MATSUS Fall 2023 held in Torremolinos, Spain from 16 – 20 October. Congratulations to Amrita Singh-Morgan (ETH Zurich) for being awarded the best poster presentation prize and Christopher Dreimol (ETH Zurich) for being awarded the best oral presentation. Find out more about our winners below:

Amrita Singh- Morgan

Originally from Leeds, Amrita studied Chemistry at the University of Edinburgh where she had the opportunity to do a year abroad in Switzerland. Persuaded by the alpine landscapes, she decided to do a PhD at ETH Zurich in the group of Prof. Mougel, where she now researches heterogeneous electrocatalysis.

 Using CO2 as a chemical feedstock is a promising method to produce valuable chemicals and fuels without fossil or biomass resources. Flue gas, which is formed from the combustion of fossil fuels, constitutes a major localised source from which CO2 could be captured and converted. Amrita’s research involves the electrochemical conversion of CO2 in tandem with another harmful component of flue gas, NOx, to valorise the products formed and maximise the environmental benefit.

Title of her poster: Until NOthing’s Left: Electrochemical Conversion of Nitric Oxide to Ammonia from Dilute Gas Streams

 

Christopher Dreimol

 

 

After completing an apprenticeship in the field of mechanical engineering at Kathrein SE (today Ericsson) in Rosenheim, Christopher Dreimol studied Biomimetics (B.Sc.) in the HS Bremen. He continued with a master’s in production engineering with a focus of material science at the University of Bremen that he finished with a master thesis at ETH Zürich working on bio-inspired materials together with Prof. André R. Studart. Today as a Ph.D. student, Christopher Dreimol works on sustainable wood-based electronics for smart buildings, sensors, soft electronics, and energy storage devices together with Prof. Dr. Ingo Burgert in the Wood Material Science Group at ETH Zürich and EMPA.

 

 

Title of his talk: Iron-Catalyzed Laser-Induced Graphitization: A Novel Approach to Produce Sustainable, Bio-Inspired Electrodes with Tunable Iron Phases.

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Monitoring the Evolution of Segmental Order in Conjugated Polymers During Crystallization

By Robert M. Pankow, Community Board Member.

Conjugated polymers (CPs) are transformative materials that have facilitated numerous advancements in the field of soft-matter electronics. Their low-cost, high structural tunability, and robust mechanical properties have made them desirable materials for broad range of applications, including in energy capture and storage, chemical and biological sensors, electronic skin, and electronic display devices. Recently, significant efforts have been made to develop intrinsically flexible and stretchable CPs and to understand the fundamental principles and structural characteristics that impart these elastomeric properties without impairment to charge transport. Central to this has been extensive characterization of the polymer morphology and microstructure, which yielded the discovery that local segmental order can facilitate efficient long-range charge transport in the amorphous domains of the polymer. However, directly probing the local segmental order in polymers and distinguishing the contributions of this domain towards the charge transport and physicochemical properties from that of the crystalline domains, which are defined by long-range ordering, remains challenging.

Now, a highly collaborative and extensive study by Luo et al. describes the development of a new technique for monitoring the subtle changes in the local segment order and amorphous fractions of the polymer microstructure by integrating Raman spectroscopy with fast-scanning calorimetry (FSC). The authors targeted a structurally diverse set of polymers to broadly classify their findings.

 

Figure 1. Modulating and probing microstructure of conjugated polymers by integrated ultrafast calorimetry and micro-Raman spectroscopy. Left: Schematic of this integrated technique. The time-temperature program used in this study was carried out by the chip sensor temperature controller. The growth of crystalline domain was identified by the evolution of melting peak collected through FSC. The degree of segmental order was analyzed by the Raman shift of C=C modes through resonant micro-Raman spectroscopy. Reproduced from DOI: 10.1039/D3MH00956D with permission from the Royal Society of Chemistry

Namely, analogs based on poly(3-hexylthiophene-2,5-diyl) (P3HT) and poly{2,2′-[(2,5-bis(2-hexyldecyl)-3,6-dioxo-2,3,5,6- tetrahydropyrrolo[3,4-c ]pyrrole-1,4-diyl)dithiophene]- 5,5′-diyl-alt-thiophen-2,5-diyl} (PDPP3T or PDPPT), which are prevalent throughout organic electronics. The polymers were first subjected to a carefully devised time-temperature program to erase the thermal history of the polymers by first subjecting the polymer samples to temperatures above their melting point (Tm). Following subsequent thermal quenching and annealing steps, the Raman and FSC measurements were recorded. By monitoring the evolution of the Raman spectra and tracking the shifts in C=C/C-N stretches with increasing annealing time, minute changes in the segmental order could be monitored. It was observed that the extent of segmental order saturates before maximum crystallinity is achieved and that the annealing temperature could be specifically tailored for the polymers to achieve a highly ordered microstructure with desired levels of crystallinity.

Next, polymer segmental order was correlated with the segmental dynamics and charge transport properties by using alternating current (ac) chip-calorimetry and fabricating organic field effect transistors (OFETs). It was found that the rigid amorphous fraction (RAF) plays a significant role in promoting segmental order, and that there is a strong correlation between the polymer segmental order and the OFET charge-carrier mobility. Overall, the findings, magnitude, and scope of this study makes it a pivotal work for the field of organic electronics, and it should have resounding impact throughout material science.

To find out more, read the full manuscript here:

Real-time correlation of crystallization and segmental order in conjugated polymers

Shaochuan Luo, Yukun Li, Nan Li, Zhiqiang Cao, Song Zhang, Michael U. Ocheje, Xiaodan Gu, Simon Rondeau-Gagné, Gi Xue, Sihong Wang,  Dongshan Zhou and Jie Xu

Mater. Horiz., 2023, Advance Article, DOI: 10.1039/D3MH00956D

 


About the blogger


Robert M. Pankow is an Assistant Professor at The University of Texas at El Paso and a member of the Material Horizons Community Board. Dr. Pankow’s research focuses on conjugated polymer synthesis, sustainable chemistry, and organic electronics. You can follow him on X (formerly Twitter) @RobertPankow.
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Meet our new Advisory Board member- Paulette Clancy

Materials Horizons are delighted to welcome Professor Paulette Clancy as the newest member of the Advisory Board. 

Paulette Clancy is the Edward J. Schaefer Professor of chemical and biomolecular engineering. More recently, she became the director of research for the AI-X Foundry. She is the Associate Director of the Johns Hopkins Center for Integrated Structure-Mechanical Modeling and Simulation (CISMMS), and a fellow of the Hopkins Extreme Materials Institute (HEMI) and AIChE. She spent over 30 years teaching at Cornell before moving to Johns Hopkins in 2018 to become the inaugural department Head of ChemBE.

Clancy leads one of the top groups in the country studying atomic- and molecular-scale modeling of semiconductor materials, ranging from traditional silicon-based compounds to all-organic materials. Her group’s research comprises four main areas: advanced organic materials (covalent organic frameworks, antibacterial oligomers, organic electronics); algorithm development (force field development, machine learning, and Bayesian optimization); electronic materials (particularly III-IV semiconducting materials; and nucleation and crystal growth (hybrid organic/inorganic perovskites and quantum dot nanocrystals). Her lab focuses on studies of advanced materials processing and nucleation, including understanding the links between processing, structure, and function.

Her group is at the forefront of developing new Bayesian optimization methods to encode expert knowledge and intuition, creating optimal conditions for making energy-efficient solar cells, close-to-perfect quantum dots, and discovering polymorphs of electronic materials for shape memory applications.

She is a fierce long-term advocate for the increased representation of women and those from groups under-represented in engineering and the physical sciences.  She was the founding chair of a faculty group, “Women in Science and Engineering” for Cornell University. Among her awards for that advocacy is the American Institute of Chemical Engineers (AIChE) National Women’s Initiatives Mentoring Award. She is a member of the mentoring team for Project Elevate, a DEI initiative between Hopkins in partnership with NYU and CMU.

 

Check out some of Paulette’s recent RSC publications:

A comprehensive picture of roughness evolution in organic crystalline growth: the role of molecular aspect ratio

Jordan T. Dull, Xiangyu Chen, Holly M. Johnson, Maria Clara Otani, Frank Schreiber, Paulette Clancy and  Barry P. Rand

Mater. Horiz., 2022,9, 2752-2761, DOI: 10.1039/D2MH00854H

 

A new metric to control nucleation and grain size distribution in hybrid organic–inorganic perovskites by tuning the dielectric constant of the antisolvent

Blaire A. Sorenson, Lucy U. Yoon, Eric Holmgren, Joshua J. Choi and Paulette Clancy

J. Mater. Chem. A, 2021,9, 3668-3676, DOI: 10.1039/D0TA12364A

 

A multiscale approach to uncover the self-assembly of ligand-covered palladium nanocubes

Xiangyu Chen, Thi Vo and Paulette Clancy

Soft Matter, 2023, Advance Article, DOI: 10.1039/D3SM01140B

 

Read our interview with Paulette below:

What does it mean to you to join the Advisory Board of Materials Horizons?

I feel honored to join the Advisory Board because this is such an exciting and relatively new journal. It brands itself as being “transformative” and that’s how I have found the research that it publishes. I am glad to be part of the team to keep up the wonderful momentum that it has.

What is the current biggest challenge you face in your field?

I work in the area of machine-learning guided materials discovery. The biggest challenge I currently face is to sift through the burgeoning number of new methods in this hot area and learn which ones are truly exciting and ground-breaking.

Why do you feel that researchers should choose to publish their work in Materials Horizons?

MH has it all: Thoughtful and helpful reviewers, short time to triage and review, and careful selection of strong papers.

Can you tell us about one of your latest Materials Horizons publications?

I actually have some of my most exciting new Bayesian optimization algorithm development under review with MH right now, so fingers crossed for that one. My last paper involved a joint computational (us)-experimental (Princeton) study of the thin-film growth of molecules that could be used for electronic devices. To function well in that regard, you need to create films that are as smooth as possible. Our paper looked at a few candidates for new electronic materials and showed that you need to take a holistic view of the growth process rather than relying just on the traditional step-edge energy barriers to arbitrate between rough (unwanted) and smooth growth (desirable).  We were thrilled to be recognized with an “Editor’s Choice” designation and the cover. 

 

Paulette’s last Materials Horizons article was featured on the issue front cover

Please join us in welcoming Paulette to the Materials Horizons Advisory Board!

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Materials Horizons’ New Community Board Members

Join us in welcoming our new Materials Horizons Community Board members

The Materials Horizons Community Board provide an invaluable link between the editorial office and emerging chemistry, they are our eyes and ears on the ground, allowing us to better connect with other early-career researchers. Since its inception in 2014, we have enjoyed working together with these board members to facilitate student, postdoctoral and early-career researcher engagement, through symposia support, journal clubs, webinars, special article collections and many other activities.

Over the summer, we requested nominations from the materials chemistry academic community and were thrilled with the high calibre of candidates nominated. We are delighted to share our 30 new appointees with you who, together with continuing members, make up a Materials Horizons Community Board of 50 international researchers at different stages of their early careers, ranging from PhD candidates to Professors.

From Left to right: Minah Lee, Korea Institute of Science & Technology, South Korea. • Subhajit Pal, University of California, Berkeley, United States. • Fang-Chen Liang, National University of Singapore, Singapore. • Kostas Parkatzidis, ETH Zurich, Switzerland. • Kelsey DeFrates, University of California, Berkeley, United States. • Haegyum Kim, Lawrence Berkeley National Laboratory, United States. • Jing Xie, Sichuan University, China • Raul Marquez-Montes, The University of Texas, United States. • Wen Shi, Sun Yat-sen University, China. • Valerio Piazza, Ecole Polytechnique Federale de Lausanne, Switzerland. • Shaohua Zhang, Radboud University, Netherlands • Olga Guselnikova, National Institute for Materials Science, Japan. • Qiaobao Zhang, Xiamen University, China. • Shiv Singh, CSIR - Advanced Materials and Processes Research Institute, India. • Anna Stejekalova, Harvard University, United States. • Sahid Zaman, Université du Québec à Trois-Rivières, Canada. • Felix Utama Kosasih, Nanyang Technological University, Singapore. • Xiaojuan Ni, The University of Arizona, United States. • Danila Merino, Polymat Institute, UPV/EHU, Spain. • Yunmao Zhang, Xiamen University, China. • Xianbiao Fu, Technical University of Denmark, Denmark. • Ruijuan Xu, North Carolina State University, United States. • Shyamapada Nandi, Vellore Institute of Technology Chennai, India. • Edison Ang Huixiang, Nanyang Technological University, Singapore. • Hassan Abdellatif, Cairo University, Egypt. • Guanjie He, University College London, United Kingdom • Josh Bailey, Queen's University Belfast, Northern Ireland. • Jieun Yang, Kyung Hee University, South Korea. • Raffaello Mazzaro, University of Bologna, Italy. • Ivana Qiangi Lin, University of Twente, Netherlands.

Please join us in welcoming our 30 new Community Board members:

Discover the full Community Board

You can keep up to date with the activities of our Community Board members on our blog. Our companion journal Nanoscale Horizons has also welcomed new members to their community board, and you can find out more about their new members on their blog. We will be highlighting the members of our Community Board over the coming months in a series of interviews and look forward to sharing these with you soon.

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Materials Horizons 10th Anniversary Cover

 

As part of the 10th Anniversary celebrations, a special cover image was created based on your votes for the best 10 covers from the last 10 years.

2014

Ultrasonication-switched formation of dice- and cubic-shaped fullerene crystals and their applications as catalyst supports for methanol oxidation
Ying Xu, Xiang Chen, Fupin Liu, Xi Chen, Jianhe Guo and Shangfeng Yang  

2015

Versatile third components for efficient and stable organic solar cells
Pei Cheng and Xiaowei Zhan

2016 

Mechanical meta-materials

Amir A. Zadpoor

2017

A new class of chiral semiconductors: chiral-organic-molecule-incorporating organic–inorganic hybrid perovskites
Jihoon Ahn, Eunsong Lee, Jeiwan Tan, Wooseok Yang, Bokyung Kim and Jooho Moon

2018

PLUS-M: a Porous Liquid-metal enabled Ubiquitous Soft Material

Hongzhang Wang, Bo Yuan, Shuting Liang, Rui Guo, Wei Rao, Xuelin Wang, Hao Chang, Yujie Ding, Jing Liu and Lei Wang

2019

Seamless interconnections of sp2-bonded carbon nanostructures via the crystallization of a bridging amorphous carbon joint
Longze Zhao, Yong Cheng, Qiaobao Zhang and Ming-Sheng Wang

2020

Air-stable means more: designing air-defendable lithium metals for safe and stable batteries
Jingyi Wu, Lixia Yuan, Zhen Li, Xiaolin Xie and Yunhui Huang

2021

Tilt and shift polymorphism in molecular perovskites
Stefan Burger, Shivani Grover, Keith T. Butler, Hanna L. B. Boström, Ricardo Grau-Crespo and Gregor Kieslich

image created by Dr Johannes Richers (Jo Richers Studio)

2022

Semi-paracrystallinity in semi-conducting polymers
Sara Marina, Edgar Gutierrez-Fernandez, Junkal Gutierrez, Marco Gobbi, Nicolás Ramos, Eduardo Solano, Jeromy Rech, Wei You, Luis Hueso, Agnieszka Tercjak, Harald Ade and Jaime Martin

2023

Physical crosslinked hydrogel-derived smart windows: anti-freezing and fast thermal responsive performance
Gang Li, Jiwei Chen, Zhaonan Yan, Shancheng Wang, Yujie Ke, Wei Luo, Huiru Ma, Jianguo Guan and Yi Long

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