Chemical Science Blog

New month, new HOT articles!

We are pleased to share a selection of our referee-recommended HOT articles for November 2021. We hope you enjoy reading these articles, congratulations to all the authors whose articles are featured! As always, Chemical Science is free to read & download.

You can explore our full 2021 Chemical Science HOT Article Collection here!

Browse a selection of our November HOT articles below:

Redox-active zinc thiolates for low-cost aqueous rechargeable Zn-ion batteries
Madison R. Tuttle, Christopher Walter, Emma Brackman, Curtis E. Moore, Matthew Espe, Chris Rasik, Paul Adamsb and Shiyu Zhang
Chem. Sci., 2021,12, 15253-15262

Asymmetric patterning drives the folding of a tripodal DNA nanotweezer
Daniel Saliba, Tuan Trinh, Christophe Lachance-Brais, Alexander L. Prinzen, Felix J. Rizzuto, Donatien de Rochambeaua and Hanadi F. Sleiman
Chem. Sci., 2022, Advance Article

Ligand-controlled regioselective and chemodivergent defluorinative functionalization of gem-difluorocyclopropanes with simple ketones
Leiyang Lv, Huijun Qian, Yangyang Ma, Shiqing Huang, Xiaoyu Yan and Zhiping Li
Chem. Sci., 2021,12, 15511-15518

Generation of oligonucleotide conjugates via one-pot diselenide-selenoester ligation–deselenization/alkylation
Christopher Liczner, Cameron C. Hanna, Richard J. Payne and Christopher J. Wilds
Chem. Sci., 2022, Advance Article

Synthesis of a heterobimetallic actinide nitride and an analysis of its bonding
Selena L. Staun, Guang Wu, Wayne W. Lukens and Trevor W. Hayton
Chem. Sci., 2021,12, 15519-15527

Improving the intrinsic activity of electrocatalysts for sustainable energy conversion: where are we and where can we go?
Nitish Govindarajan, Georg Kastlunger, Hendrik H. Heenen and Karen Chan
Chem. Sci., 2022, Advance Article

Submit to Chemical Science today! Check out our author guidelines for information on our article types or find out more about the advantages of publishing in a Royal Society of Chemistry journal.

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To further thank and recognise the support from our excellent reviewer community, we are highlighting reviewers who have provided exceptional support to the journal over the past year.

This month, we’ll be highlighting Christine Luscombe, Peng Yang, Shigeyoshi Inoue and Jennifer Brodbelt. We asked our reviewers a few questions about what they enjoy about reviewing, and their thoughts on how to provide a useful review.

	Christine Luscombe, Okinawa Institute of Science and Technology, Japan. Christine works on developing organic semiconducting polymers for applications including light-emitting diodes, photovoltaics, mixed ionic-electronic conduction, and stretchable electronics.
	Peng Yang, Shaanxi Normal University, China. Peng’s group develop coatings by exploiting the chemical diversity of amyloid-like protein aggregation and use them in applications including bio-interfaces, flexible electronics and adhesives.
	Shigeyoshi Inoue, Technische Universität München, Germany. Shigeyoshi’s research focus is on the synthesis, characterization and reactivity investigation of compounds containing low-valent main group elements with unusual structures and unique electronic properties.
	Jennifer Brodbelt, University of Texas at Austin, USA. Jennifer’s group develop high performance mass spectrometry strategies, such as ultraviolet photodissociation, to analyze and quantify molecules in complex mixtures, such as proteins and lipids.

What encouraged you to review for Chemical Science?

Jennifer Brodbelt: Chemical Science has a broad readership and covers a diverse range of topics. This contributes to its high impact factor and makes it a must-read journal. Serving as a reviewer is a natural part of the whole publishing process, and it is just as important to review manuscripts as it is to submit excellent manuscripts to keep the entire cycle strong.

Christine Luscombe: I am big supporter of society journals and I am also a stronger believer in trying to give back to the community. Additionally, Chemical Science is a top tier journal, so I see it as a privilege to be able to be part of the publication process.

What do you enjoy most about reviewing?

Shigeyoshi Inoue: By reviewing papers, I will always be able to read and learn from the latest results and may even be able to contribute to the paper in some way.

Peng Yang: I can learn from other scientists with a new point of view. The reviewing process is also an evaluation of myself and helps to improve my own work.

What makes a paper truly stand out for you when you are reviewing?

Shigeyoshi Inoue: Of course, the quality of the reported results and great research ideas are important. However, I personally like papers that contain a simple and readable introduction and a conclusion that reflects well on the results obtained.

Jennifer Brodbelt: I definitely appreciate good quality figures. Good figures can capture the whole story.

What would you recommend to new reviewers to ensure their report is helpful?

Peng Yang: Evaluate papers from a scientific perspective and guide authors to do more innovative research rather than simply following others. Guide the authors to do more research on basic mechanism studies and more real or close-to-real applications, instead of only proof-of-concept showcases.

What has been your biggest learning point from reviewing?

Christine Luscombe: To treat people with respect and remember that there is someone who spent months/years collecting the data that went into writing the paper. We owe it to them to be careful as possible in our reviewing process.

Tune in next month to meet our next group of #ChemSciReviewers!

If you want to learn more about how we support our reviewers, check out our Reviewer Hub.

Interested in joining our ever-growing reviewer community? Send us your CV and a completed Reviewer Application Form to becomeareviewer@rsc.org.

Recent decades have established that metal-organic frameworks (MOFs) are a pretty cool class of materials, with potential applications across a range of fields. In particular, their high porosities make them extremely attractive for storing a variety of gases, including possible fuels like methane and hydrogen. Two primary strategies have emerged to store H₂ and CH₄ in MOFs – synthesizing materials with unsaturated metals that can strongly bind to the target and synthesizing materials with small pores where multiple weak interactions combine to produce strong binding. Of course, these MOFs are designed with a single specific target in mind, making them synthetically complex and useful for storing only one type of molecule. Ideally, new MOFs with relatively straightforward syntheses that can bind multiple targets could be developed.

Figure 1. (a) Single crystal X-ray diffraction structure of 1–H2O. (b,c) View of the pores of 1–H2O showing binding pocket.

Scientists in the United States took a hybrid approach, creating MOFs with small, but flexible binding pockets. While the concept feels relatively straightforward and intuitive, it’s of course more complicated in practice. The MOF needs to hit a Goldilocks zone in terms of flexibility, where only a small number of select targets will bind rather than a wide range of gases. The researchers accomplished this by using an actinide (depleted uranium) as the metal nodes for their MOF as its tendency to adopt high coordination numbers should result in smaller pockets and limit possible rearrangements of the flexible linker. Also, the descriptor “as it is only mildly radioactive” is something I hadn’t read about a material before and rather caught my attention. The crystalline material, referred to as 1-H₂O (Figure 1), was straightforwardly synthesized in an autoclave and isolated in relatively high yields. It features pores with two pockets that are capped by the bowl-shaped linkers. As synthesized, the pockets are occupied by water molecules that can be removed by heating the MOF under a dynamic vacuum.

Figure 2. (a) Neutron powder diffraction structure of D2 adsorbed at site I in 1–D2. (b) Neutron powder diffraction structure of CD4 adsorbed at site I in 1–CD4. (c) Powder X-ray diffraction structure of DMF adsorbed inside the pore of U(bdc)2.

The MOF maintains its structural integrity after water removal, actually expanding slightly. This indicates that the MOF will contract upon binding, locking the target into place in the pocket. The researchers found that the MOF rapidly uptakes both H₂ and CH₄ at low temperatures, but the precise nature of the binding pocket adjustments can’t be determined by gas adsorption studies. To probe the structural details, the researchers turned to neutron powder diffraction to probe the binding of deuterated molecules to the MOF (Figure 2). The obtained structures show clear, cooperative effects that cause the adjustments to the binding pocket. The multiple different interactions allow the flexible structure to fit the two different adsorbates of interest, binding them both strongly. This work demonstrates the utility and versatility of flexible MOFs for adsorbing different gases with design principles that should be transferrable to non-radioactive materials.

To find out more, please read:

Self-adjusting binding pockets enhance H2 and CH4 adsorption in a uranium-based metal–organic framework

Dominik P. Halter, Ryan A. Klein, Michael A. Boreen, Benjamin A. Trump, Craig M. Brown and Jeffrey R. Long

Chem. Sci., 2020, Advance Article

About the blogger:

Dr. Beth Mundy is a recent PhD in chemistry from the Cossairt lab at the University of Washington in Seattle, Washington. Her research focused on developing new and better ways to synthesize nanomaterials for energy applications. She is often spotted knitting in seminars or with her nose in a good book. You can find her on Twitter at @BethMundySci.

We are pleased to share a selection of our referee-recommended HOT articles for March. We hope you enjoy reading these articles and congratulations to all the authors whose articles are featured! As always, Chemical Science is free to read & download. You can find our full 2020 HOT article collection here.

DP4-AI automated NMR data analysis: straight from spectrometer to structure
Alexander Howarth, Kristaps Ermanis and Jonathan M. Goodman
Chem. Sci., 2020, Advance Article
DOI: 10.1039/D0SC00442A

Completing the triad: synthesis and full characterization of homoleptic and heteroleptic carbonyl and nitrosyl complexes of the group VI metals
Jan Bohnenberger, Manuel Schmitt, Wolfram Feuerstein, Ivo Krummenacher, Burkhard Butschke, Jakub Czajka, Przemysław J. Malinowski, Frank Breher and Ingo Krossing
Chem. Sci., 2020, 11, 3592-3603
DOI: 10.1039/C9SC06445A

Recent developments in nickel-catalyzed intermolecular dicarbofunctionalization of alkenes
Joseph Derosa, Omar Apolinar, Taeho Kang, Van T. Tran and Keary M. Engle
Chem. Sci., 2020, Advance Article
DOI: 10.1039/C9SC06006E

Enhancing the selectivity of prolinamide organocatalysts using the mechanical bond in [2]rotaxanes
María Calles, Julio Puigcerver, Diego A. Alonso, Mateo Alajarin, Alberto Martinez-Cuezva and Jose Bern
Chem. Sci., 2020, 11, 3629-3635
DOI: 10.1039/D0SC00444H

Simultaneous and ultrasensitive detection of multiple microRNAs by single-molecule fluorescence imaging
Hongding Zhang, Xuedong Huang, Jianwei Liu and Baohong Liu
Chem. Sci., 2020, 11, 3812-3819
DOI: 10.1039/D0SC00580K

Submit to Chemical Science today! Check out our author guidelines for information on our article types or find out more about the advantages of publishing in a Royal Society of Chemistry journal.

Keep up to date with our latest articles, reviews, collections & more by following us on Twitter. You can also keep informed by signing up to our E-Alerts.

Have you ever heard of nonulosonic acids? As a materials chemist I hadn’t, as most of the acids I’ve dealt with are either acting as ligands or inorganic and I tend to forget that sugars are actually acids. These nine-carbon sugars are critical for a wide range of cellular functions throughout living organisms. Over 100 different members of this broad group of acids have been identified, all of which can undergo diversification at multiple positions, generating an even larger library of derivatives. What types of modifications can occur has yet to be fully realized, as novel compounds are continually discovered, particularly in prokaryotes. Even when examining a limited number of modifications, say 15, the number of possible derivatives is staggering, reaching several thousand without stereochemical considerations. Identifying these acids is key, as they have been linked to virulence in pathogenic bacteria and their previously mentioned diversity makes them challenging to genomically analyze.

Given these challenges, current detection practices rely on staining and fluorescent labeling which can be labor intensive and specific to a small number of acids. Early approaches based on mass spectroscopy were limited due to the complex backgrounds produced and the difficulties separating signal and noise. However, developments in high-resolution spectrometers and increased data processing abilities have led to successful analysis of increasing numbers of known metabolites. Researchers in the Netherlands and Russia extended this work to develop a screening approach to identify a diverse range of nonulosonic acids via small mass channel mass spectroscopy from previously unexplored environmental microbes (Figure 1).

Figure 1. Outline of the general procedure for the survey pipeline, beginning from the cells to the final structural analysis of the identified acids.

To successfully identify these unknown derivatives, the researchers identified specific ulosonic acid fragments invariant to functionalization. They used 1,2-diamino-4,5-methylene dioxybenzene, an alpha-keto-acid specific labeling reagent, to shift the double bond equivalents from the general cellular background and help conserve the core ulosonic acid structure. By screening a known range of acids with different functional group moieties, they were able to identify universal features for this category of molecules (Figure 2). From there, they created a full process for rapid-throughput studies that automated everything from initial identification of a potential acid molecule through filtering and structural analysis.

Figure 2. A) Universal fragmentation route used to identify nonulasonic acids in the screening, B) data output of various ulosonic acid derivatives identified in the study, and C) differences seen from the chemical labeling introduced in the procedure.

After the pipeline was established, the researchers used various standard cell lines, plant, animal, and algal, for a molecular level survey to confirm the validity of their approach for full-cell analysis. In general, the plants and yeast cells contained no nonulosonic acids, as expected, while the microalgae and animal cells had a range of different nonulosonic acids present. As these acids are thought to play a role in bacterial virulence, a bacteria known to display the acids was screened and several subtypes of animal and bacterial acids were identified as incorporated into the cells. With that validation, the researchers moved on to a wide range of non-pathogenic bacteria. They discovered that over half of these bacteria possess nonulosonic acids; in fact, some have only slightly lower acid abundance than mammalian cells. While much of this data was obtained from single cultures, it represents exciting validation of a broad new approach that could be used to identify potential targets for medical applications and continue to extend our understanding of the diversity of nonulosonic acids.

To find out more, please read:

Tackling the chemical diversity of microbial nonulosonic acids – a universal large-scale survey approach

Hugo B. C. Kleikamp, Yue Mei Lin, Duncan G. G. McMillan, Jeanine S. Geelhoed, Suzanne N. H. Naus-Wiezer, Peter van Baarlen, Chinmoy Saha, Rogier Louwen, Dimitry Y. Sorokin, Mark C. M. van Loosdrecht and Martin Pabst

Chem. Sci., 2020, 11, 3074-3080.

About the blogger:

Dr. Beth Mundy is a recent PhD in chemistry from the Cossairt lab at the University of Washington in Seattle, Washington. Her research focused on developing new and better ways to synthesize nanomaterials for energy applications. She is often spotted knitting in seminars or with her nose in a good book. You can find her on Twitter at @BethMundySci.