Archive for August, 2015

Coordinating nature and photochemistry to create hydrogen

When we look to our future energy resources, the need to realise new means of renewable energy is immediately obvious. Much research is being carried out around the world into the development of systems that can generate energy – from H2 to biofuels to solar fuels – all of which place great importance on high efficiency and sustainability.

Looking at the world around us for inspiration, the obvious candidate is the photosynthetic process, where visible light is employed to convert CO2 and H2O into chemical energy. This process involves the transport of electrons through a complex series of intricately aligned porphyrin-related and protein biomolecules. We can explore the development of a system that mimics the behaviour of natural systems, with respect to the relay of electrons along a series of molecules, or, alternatively, we can take the components in these systems and exploit their properties in combination with other electronically-active but non-natural molecules.

Upon photoexcitation of [Ru(bpy)3]2+, electron transfer through a ferredoxin scaffold to a cobaloxime catalyst facilitates the production of hydrogen.It is the latter approach which Lisa Utschig and her team from Argonne National Laboratory, near Chicago in the US, employed to generate a molecular system capable of photocatalysing the production of hydrogen. In their biohybrid system, the photosensitiser ruthenium(II) tris(bipyridine), ferredoxin (a water-soluble electron transfer protein), and cobaloxime (a cobalt(II)-based catalyst), were combined to generate a miniature reaction center that mimics those which occur in biological systems. However, the Utschig group’s system has a smaller molecular weight, which allows for characterisation of the electronic processes that occur in the system.

Lisa and her colleagues found that the presence of ferredoxin in the catalytic system acted as a scaffold to stabilise the charge-separated state necessary for electron transfer and the desired production of H2. They also observed that the catalytic behaviour of the Ru(II)–Co(II) pair was only possible in the presence of ferredoxin, which acted to extend the lifetime of the otherwise transient Co(I), allowing the desired reaction to occur.

In order to fully understand and enhance the properties of the molecular systems developed to fulfil the increasing need for energy alternatives, we need to be able to probe the structure and processes that occur in the molecule; the use of smaller analogs to those that exist in nature offers a means by which to achieve this goal. The photoactivated catalyst discussed in this work is an important step forward in the development of an optimized system for use in solar fuel production.

Read this hot ChemComm article in full:
Aqueous light driven hydrogen production by a Ru–ferredoxin–Co biohybrid
S. R. Soltau, J. Niklas, P. D. Dahlberg, O. G. Poluektov, D. M. Tiede, K. L. Lulfort and L. M. Utschig
Chem. Commun., 2015, 51, 10628–10631
DOI: 10.1039/C5CC03006D

Biography

Anthea Blackburn is a guest web writer for Chemical Science. She hails originally from New Zealand, and is a recent graduate student of Northwestern University in the US, where she studied under the tutelage of Prof. Fraser Stoddart (a Scot. There, she exploited supramolecular chemistry to develop multidimensional systems and study the emergent properties that arise in these superstructures. When time and money allow, she is ambitiously attempting to visit all 50 US states.

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How could a tree make tramadol?

Researchers in France, Switzerland and Cameroon are convinced that the African pin-cushion tree produces the well-known painkiller Tramadol and are determined to prove it. Back in 2013, a team led by neuroscientist Michel de Waard, of the Joseph Fourier University, claimed that significant quantities of the drug were present in the root bark extract of Nauclea latifolia, which has long been used by locals in West and Central Africa to treat pain and disease.

Last year another team, led by Michael Spiteller who is based at the Technical University of Dortmund, Germany, ran some tests of their own and cast doubt on these findings. Read the full article in Chemistry World»

N. latifol grows widely in Cameroon and is used by traditional healers to treat a wide variety of complaints. Image courtesy of Scott Zona / Wikipedia Commons (CC BY 2.0)


 

Read the original journal article in ChemComm – it’s free to read until 7th October:
Biomimetic synthesis of Tramadol
Florine Lecerf-Schmidt, Romain Haudecoeur, Basile Peres, Marcos Marçal Ferreira Queiroz, Laurence Marcourt, Soura Challal, Emerson Ferreira Queiroz, Germain Sotoing Taiwe, Thierry Lomberget, Marc Le Borgne, Jean-Luc Wolfender, Michel De Waard, Richard J. Robins and Ahcène Boumendjel 
DOI: 10.1039/C5CC05948H, Communication

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Molecular Sierpinski triangles get stability upgrade

Metal–nitrile coordination bonds hold the structures together

Earlier this year we reported that scientists in China had built molecular Sierpiński triangles from small aromatic building blocks. Now, another team in China has constructed fractal triangles on the molecular scale and this time, they’re much more robust. Read more in Chemistry World»

You can read the original journal article in ChemComm – it’s free to access until 28th September:
On-surface construction of a metal–organic Sierpiński triangle
Qiang Sun, Liangliang Cai, Honghong Ma, Chunxue Yuan and Wei Xu 
Chem. Commun., 2015, Advance Article
DOI: 10.1039/C5CC05554G, Communication

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Top 25 ChemComm articles April–June 2015

The 25 most-downloaded ChemComm articles in the second quarter of 2015 were as follows: 

A power-free microfluidic chip for SNP genotyping using graphene oxide and a DNA intercalating dye
Jing Li, Yan Huang, Dongfang Wang, Bo Song, Zhenhua Li, Shiping Song, Lihua Wang, Bowei Jiang, Xingchun Zhao, Juan Yan, Rui Liu, Dannong He and Chunhai Fan
DOI: 10.1039/C3CC40680F, Communication

A novel one-pot method for the synthesis of substituted furopyridines: iodine-mediated oxidation of enaminones by tandem metal-free cyclization
Rulong Yan, Xiaoni Li, Xiaodong Yang, Xing Kang, Likui Xiang and Guosheng Huang
DOI: 10.1039/C4CC08834D, Communication

Perovskite solar cells prepared by flash evaporation
Giulia Longo, Lidón Gil-Escrig, Maarten J. Degen, Michele Sessolo and Henk J. Bolink
DOI: 10.1039/C5CC01103E, Communication

Bio-inspired CO2 conversion by iron sulfide catalysts under sustainable conditions
A. Roldan, N. Hollingsworth, A. Roffey, H.-U. Islam, J. B. M. Goodall, C. R. A. Catlow, J. A. Darr, W. Bras, G. Sankar, K. B. Holt, G. Hogarth and N. H. de Leeuw
DOI: 10.1039/C5CC02078F, Communication

Heterostructured magnetic nanoparticles: their versatility and high performance capabilities
Young-wook Jun, Jin-sil Choi and Jinwoo Cheon
DOI: 10.1039/B614735F, Feature Article

Multifunctional catalysis by Pd-polyoxometalate: one-step conversion of acetone to methyl isobutyl ketone
Robert D. Hetterley, Elena F. Kozhevnikova and Ivan V. Kozhevnikov
DOI: 10.1039/B515325E, Communication

Selective guest sorption in an interdigitated porous framework with hydrophobic pore surfaces
Satoshi Horike, Daisuke Tanaka, Keiji Nakagawa and Susumu Kitagawa
DOI: 10.1039/B703502K, Communication

Layer-by-layer assembly of graphene and gold nanoparticles by vacuum filtration and spontaneous reduction of gold ions
Byung-Seon Kong, Jianxin Geng and Hee-Tae Jung
DOI: 10.1039/B821920F, Communication

Asymmetric catalysis activated by visible light
Eric Meggers
DOI: 10.1039/C4CC09268F, Feature Article

The surface chemistry of metal–organic frameworks
Christina V. McGuire and Ross S. Forgan
DOI: 10.1039/C4CC04458D, Feature Article
From themed collection 2015 Emerging Investigators

Graphene quantum dots: emergent nanolights for bioimaging, sensors, catalysis and photovoltaic devices
Jianhua Shen, Yihua Zhu, Xiaoling Yang and Chunzhong Li
DOI: 10.1039/C2CC00110A, Feature Article

Nanostructured electrochromic smart windows: traditional materials and NIR-selective plasmonic nanocrystals
Evan L. Runnerstrom, Anna Llordés, Sebastien D. Lounis and Delia J. Milliron
DOI: 10.1039/C4CC03109A, Feature Article

The rechargeable aluminum-ion battery
N. Jayaprakash, S. K. Das and L. A. Archer
DOI: 10.1039/C1CC15779E, Communication

Aggregation-induced emission: phenomenon, mechanism and applications
Yuning Hong, Jacky W. Y. Lam and Ben Zhong Tang
DOI: 10.1039/B904665H, Feature Article

Smart surface of water-induced superhydrophobicity
Xing Wang, Guangyan Qing, Lei Jiang, Harald Fuchs and Taolei Sun
DOI: 10.1039/B902360G, Communication

A highly selective fluorescent sensor for glucosamine
Tam Minh Tran, Yuksel Alan and Timothy Edward Glass
DOI: 10.1039/C5CC00415B, Communication

Reduction of graphene oxide viaL-ascorbic acid
Jiali Zhang, Haijun Yang, Guangxia Shen, Ping Cheng, Jingyan Zhang and Shouwu Guo
DOI: 10.1039/B917705A, Communication

Self-assembled sorbitol-derived supramolecular hydrogels for the controlled encapsulation and release of active pharmaceutical ingredients
Edward J. Howe, Babatunde O. Okesola and David K. Smith
DOI: 10.1039/C5CC01868D, Communication

Pro-fragrant ionic liquids with stable hemiacetal motifs: water-triggered release of fragrances
H. Q. Nimal Gunaratne, Peter Nockemann and Kenneth R. Seddon
DOI: 10.1039/C5CC00099H, Communication

Aromatic donor–acceptor interactions in non-polar environments
Giles M. Prentice, Sofia I. Pascu, Sorin V. Filip, Kevin R. West and G. Dan Pantos
DOI: 10.1039/C5CC00507H, Communication

Wet chemical synthesis of silver nanorods and nanowires of controllable aspect ratio
Nikhil R. Jana, Latha Gearheart and Catherine J. Murphy
DOI: 10.1039/B100521I, Communication

Palladium-catalyzed ring opening of norbornene: efficient synthesis of methylenecyclopentane derivatives
Xin-Xing Wu, Yi Shen, Wen-Long Chen, Si Chen, Xin-Hua Hao, Yu Xia, Peng-Fei Xu and Yong-Min Liang
DOI: 10.1039/C5CC02246K, Communication

A facile solvothermal growth of single crystal mixed halide perovskite CH3NH3Pb(Br1-xClx)3
Taiyang Zhang, Mengjin Yang, Eric E. Benson, Zijian Li, Jao van de Lagemaat, Joseph M. Luther, Yanfa Yan, Kai Zhu and Yixin Zhao
DOI: 10.1039/C5CC01835H, Communication

Microfluidic synthesis of chitosan-based nanoparticles for fuel cell applications
Fatemeh Sadat Majedi, Mohammad Mahdi Hasani-Sadrabadi, Shahriar Hojjati Emami, Mojtaba Taghipoor, Erfan Dashtimoghadam, Arnaud Bertsch, Homayoun Moaddel and Philippe Renaud
DOI: 10.1039/C2CC33253A, Communication

Conversion of a metal–organic framework to N-doped porous carbon incorporating Co and CoO nanoparticles: direct oxidation of alcohols to esters
Yu-Xiao Zhou, Yu-Zhen Chen, Lina Cao, Junling Lu and Hai-Long Jiang
DOI: 10.1039/C5CC01588J, Communication 


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