Chemical Science Blog

Bristol Synthesis Meeting 2019

08 Jan 2019

The Bristol Synthesis Meeting will be taking place this year on Tuesday 9th April at the University of Bristol. Chemical Science are proud to sponsor this meeting, and one of our Assistant Editors Sarah Sharp will be attending. We look forward to seeing you there.

With an inspiring line-up of speakers including Professor Craig Townsend, Professor Michinori Suginome, Professor Helma Wennemers, Professor Dean Toste and Professor Ilan Marek, this is not one to miss. Registration is now open at the Bristol Synthesis Meeting webpage.

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Andrei Yudin joins Chemical Science as an Associate Editor

20 Dec 2018

By Sarah Rainford, Deputy Editor.

We are delighted to introduce Professor Andrei Yudin as Chemical Science Associate Editor, handling submissions in the area of organic chemistry.

Andrei is a Professor of Chemistry at the University of Toronto, where his group specialise in chemical synthesis with a focus on the preparation of novel biologically active molecules. Andrei and his group pioneered work on the preparation of amphoteric reagents, developing structurally distinct intermediates that were viewed as impossible to prepare prior to their studies. The group have been highlighted for the preparation of a library of difficult-to-prepare azridine aldehydes and α-boryl aldehydes that can be applied in the preparation of medically relevant peptidomimetics.

Andrei is the current Editor-in-Chief of the Royal Society of Chemistry journal, Organic & Biomolecular Chemistry, and runs a blog series providing regular updates on the progress within his group, found at https://amphoteros.com/.

Andrei has now joined the team at Chemical Science and looks forward to receiving submissions in the areas of organic synthesis, transition metal catalysis, peptide preparation and macrocyclisation.

Below is a selection of articles published in Chemical Science that Andrei would like to highlight:

Oxygen transfer in electrophilic epoxidation probed by ¹⁷O NMR: differentiating between oxidants and role of spectator metal oxo
Christian Ehinger, Christopher P. Gordon and Christophe Coperet
Chem. Sci., 2019, Advance Article
DOI: 10.1039/C8SC04868A, Edge Article

A divergent synthetic pathway for pyrimidine-embedded medium-sized azacycles through an N-quaternizing strategy
Yoona Choi, Heejun Kim and Seung Bum Park
Chem. Sci., 2019, Advance Article
DOI: 10.1039/C8SC04061C, Edge Article

We also highlight a few of Andrei’s contributions to Chemical Science from the last few years:

3-Cyanoallyl boronates are versatile building blocks in the synthesis of polysubstituted thiophenes
Wenjie Shao, Sherif J. Kaldas and Andrei K. Yudin
Chem. Sci., 2017, 8, 4431-4436
DOI: 10.1039/C7SC00831G, Edge Article

The reactivity and conformational control of cyclic tetrapeptides derived from aziridine-containing amino acids
Benjamin K. W. Chung, Christopher J. White, Conor C. G. Scully and Andrei K. Yudin
Chem. Sci., 2016, 7, 6662-6668
DOI: 10.1039/C6SC01687A, Edge Article

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Andrew Cooper – our new Editor-in-Chief of Chemical Science

18 Dec 2018

By William King.

We are delighted to announce Professor Andrew Cooper as the new Editor-in-Chief of Chemical Science.

Andrew Cooper is Professor of Chemistry, Director of the Centre for Materials Discovery and Director of the Materials Innovation Factory at the University of Liverpool. He is a Fellow of the Royal Society and has won several prizes and awards for his research.

Professor Cooper’s research interests lie in polymeric materials, supercritical fluids, microporous materials, hydrogen storage, metal nanoparticles, organometallics, emulsion-templated materials, and high-throughput materials methodology.

As we thank Professor Daniel Nocera for his valuable contributions to the journal during his term as Editor-in-Chief of Chemical Science over the past four years, we warmly welcome Professor Cooper as he leads the journal to continued success.

As the Royal Society of Chemistry’s flagship journal, Chemical Science publishes findings of exceptional significance from across the chemical sciences. Chemical Science is free to read, and free to publish in – with all publication charges currently waived.

Professor Cooper joins us in inviting you to submit your most exceptional research to Chemical Science today!

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Carbon Coating Promotes CO2 Reduction on Nickel Surfaces

18 Dec 2018

By Tianyu Liu.

Reducing CO₂ into fuels such as CO or hydrocarbons is a promising strategy to reduce the net emission of greenhouse gases and mitigate climate change. The CO₂ reduction reaction, however, is an energy-costly process. Therefore, CO₂ reduction catalysts are necessary to enhance the CO₂ conversion efficiency and minimize the overall energy demand.

Researchers are developing high-performance yet inexpensive CO₂ reduction catalysts. Noble metals such as Au, Ag and Pd exhibit high CO₂-to-CO conversion efficiency, but their scarcity restricts their large-scale practicability. Metallic Fe, Co and Ni are active in reducing CO₂ and therefore, have been identified as alternatives to the noble metal catalysts.

Recently in Chem. Sci., a group of scientists led by Zhenyu Sun from Beijing University of Chemical Technology and Yousung Jung from Korea Advanced Institute of Science and Technology (KAIST) pushed the CO₂-reduction activity of Ni metal to a new height. The researchers synthesized carbon-supported Ni nanocrystals via pyrolysis of Ni-based metal organic frameworks (MOFs) in argon. The resultant Ni nanoparticles had an average diameter of ~30 nm and were embedded in N-doped carbon scaffolds (Fig. 1a). Each nanoparticle was uniformly coated with a thin layer of amorphous carbon (Fig. 1b).

Figure 1. (a) The elemental mapping of the carbon-supported Ni nanoparticles. Green dots and blue regions are Ni nanoparticles and carbon matrices, respectively. (b) The scanning transmission electron microscope image showing the thin carbon coating on a Ni nanoparticle surface. (c) The CO2-to-CO conversion efficiencies at different applied potentials. Ni-NC_ATPA@C and Ni-NC_TPA@C are carbon-supported Ni nanoparticles derived from MOFs with 2-amino-terephthalic acid and terephthalic acid organic linkers, respectively. NC_ATPA@C is the Ni-free carbon powder derived from ATPA.

The CO₂-to-CO conversion efficiencies of these Ni-C nanocomposites were the highest among all the reported carbon-supported Ni nanoparticles. The best Ni catalyst achieved a maximal efficiency of ~94% at an overpotential of 0.59 V, while previously reported Ni-C catalysts typically exhibited efficiencies lower than 25%. The significantly improved conversion efficiency was associated with the thin carbon coating. This coating prevented the Ni nanoparticles from directly contacting with aqueous electrolytes, and thus minimized hydrogen evolution reaction, a side reaction that decreased the conversion efficiency.

This work highlights the instrumental role of the surface carbon layers in promoting the CO₂-reduction activity of Ni nanoparticles. The carbon-coating strategy could be extended to other low-cost transition metals, which may lead to a variety of cost-effective CO₂-reduction catalysts.

To find out more please read:

Carbon-Supported Ni Nanoparticles for Efficient CO₂ Electroreduction

Mingwen Jia, Changhyeok Choi, Tai-Sing Wu, Chen Ma, Peng Kang, Hengcong Tao, Qun Fan, Song Hong, Shizhen Liu, Yun-Liang Soo, Yousung Jung, Jieshan Qiu and Zhenyu Sun

Chem. Sci., 2018, 9, 8775-8780

About the blogger:

Tianyu Liu obtained his Ph.D. (2017) in Chemistry from University of California, Santa Cruz in the United States. He is passionate about scientific communication to introduce cutting-edge research to both the general public and scientists with diverse research expertise. He is a blog writer for Chem. Commun. and Chem. Sci. More information about him can be found at http://liutianyuresearch.weebly.com/.

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Serena DeBeer joins Chemical Science as an Associate Editor

11 Dec 2018

By William King.

We are delighted to announce that Professor Serena DeBeer has joined Chemical Science as an Associate Editor.

Serena is a Professor and Director at the Max Planck Institute for Chemical Energy Conversion in Mülheim an der Ruhr, Germany. She is also an Adjunct Professor in the Department of Chemistry and Chemical Biology at Cornell University, an honorary faculty member at Ruhr University in Bochum, and the group leader of the PINK Beamline at the Energy Materials In‐Situ Laboratory at Helmholtz Zentrum in Berlin. She received her B.S. in Chemistry at Southwestern University in 1995 and her Ph.D. from Stanford University in 2002. From 2002-2009, she was a staff scientist at the Stanford Synchrotron Radiation Laboratory, before moving to her faculty position at Cornell.

Serena’s research interests lie in the development and application of advanced X-ray spectroscopic tools for understanding processes in biological, heterogeneous and homogeneous catalysis. This includes advances to X-ray spectroscopy techniques as well as applications focused on understanding electronic structural changes in catalytic processes such as N₂ reduction, CH₄ oxidation, H₂O oxidation and H₂ production.

Serena looks forward to receiving submissions in the areas of (bio)inorganic chemistry, heterogeneous and homogeneous catalysis and spectroscopy.

Below is a selection of articles published in Chemical Science which Serena would like to highlight – all free to read! We hope you enjoy them.

Excited state electron and energy relays in supramolecular dinuclear complexes revealed by ultrafast optical and X-ray transient absorption spectroscopy
Dugan Hayes, Lars Kohler, Ryan G. Hadt, Xiaoyi Zhang, Cunming Liu, Karen L. Mulfort and Lin X. Chen
Chem. Sci., 2018, 9, 860-875
DOI: 10.1039/C7SC04055E, Edge Article

Infrared spectroscopy of the nitrogenase MoFe protein under electrochemical control: potential-triggered CO binding
P. Paengnakorn, P. A. Ash, S. Shaw, K. Danyal, T. Chen, D. R. Dean, L. C. Seefeldt and K. A. Vincent
Chem. Sci., 2017, 8, 1500-1505
DOI: 10.1039/C6SC02860H, Edge Article

Metal oxidation states in biological water splitting
Vera Krewald, Marius Retegan, Nicholas Cox, Johannes Messinger, Wolfgang Lubitz, Serena DeBeer, Frank Neese and Dimitrios A. Pantazis
Chem. Sci., 2015, 6, 1676-1695
DOI: 10.1039/C4SC03720K, Edge Article

Structurally characterized terminal manganese(IV) oxo tris(alkoxide) complex
Robert L. Halbach, David Gygi, Eric D. Bloch, Bryce L. Anderson and Daniel G. Nocera
Chem. Sci., 2018, 9, 4524-4528
DOI: 10.1039/C8SC01164H, Edge Article

Magnetic circular dichroism and computational study of mononuclear and dinuclear iron(IV) complexes
Shengfa Ye, Genqiang Xue, Itana Krivokapic, Taras Petrenko, Eckhard Bill, Lawrence Que Jr and Frank Neese
Chem. Sci., 2015, 6, 2909-2921
DOI: 10.1039/C4SC03268C, Edge Article

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HOT Chemical Science articles for November

05 Dec 2018

By Carri Cotton.

We are happy to present a selection of our HOT articles over the past month. To see all of our HOT referee-recommended articles from 2018, please find the collection here.

As always, Chemical Science articles are free to access.

Carbon-supported Ni nanoparticles for efficient CO2 electroreduction

Mingwen Jia, Changhyeok Choi, Tai-Sing Wu, Chen Ma, Peng Kang, Hengcong Tao, Qun Fan, Song Hong, Shizhen Liu, Yun-Liang Soo, Yousung Jung, Jieshan Qiu and Zhenyu Sun

Chem. Sci., 2018, Advance Article

DOI: 10.1039/C8SC03732A, Edge Article

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Rare “Janus”-Faced {FeII7} Single-Molecule Magnet Exhibiting Intramolecular Ferromagnetic Interactions

Dimitris I Alexandropoulos, Kuduva R. Vignesh, Theocharis Stamatatos and Kim R. Dunbar

Chem. Sci., 2019, Accepted Manuscript

DOI: 10.1039/C8SC04384A, Edge Article

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Lytic Reactions of Drugs with Lipid Membranes

Hannah Mary Britt, Clara Antia García-Herrero, Paul W Denny, Jackie A. Mosely and John M Sanderson

Chem. Sci., 2019, Accepted Manuscript

DOI: 10.1039/C8SC04831B, Edge Article

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A Catalytic Antioxidant for Limiting Amyloid-Beta Peptide Aggregation and Reactive Oxygen Species Generation

Luiza M. F. Gomes, Atif Mahammed, Kathleen E Prosser, Jason R. Smith, Michael A. Silverman, Charles John Walsby, Zeev Gross and Tim Storr

Chem. Sci., 2019, Accepted Manuscript

DOI: 10.1039/C8SC04660C, Edge Article

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A bio-inspired approach to ligand design: folding single-chain peptoids to chelate a multimetallic cluster

Andy I. Nguyen, Ryan K. Spencer, Christopher L. Anderson and Ronald N. Zuckermann

Chem. Sci., 2018, Advance Article

DOI: 10.1039/C8SC04240C, Edge Article

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Single Ru atoms with precise coordination on a monolayer layered double hydroxide for efficient electrooxidation catalysis

Zelin Wang, Si-Min Xu, Yanqi Xu, Ling Tan, Xian Wang, Yufei Zhao, Haohong Duan and Yu-Fei Song

Chem. Sci., 2019, Advance Article

DOI: 10.1039/C8SC04480E, Edge Article

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HOT Chemical Science articles for October

07 Nov 2018

By Rebecca Withers.

We are happy to present a selection of our HOT articles over the past month. To see all of our HOT referee-recommended articles from 2018, please find the collection here.

As always, Chemical Science articles are free to access.

Enhanced annihilation electrochemiluminescence by nanofluidic confinement
Hanan Al-Kutubi, Silvia Voci, Liza Rassaei, Neso Sojic and Klaus Mathwig
Chem. Sci., 2018, Advance Article
DOI: 10.1039/C8SC03209B, Edge Article

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Mechanistic investigation into the C(sp3)–H acetoxylation of morpholinones
Cornelia S. Buettner, Darren Willcox, Ben. G. N. Chappell and Matthew J. Gaunt
Chem. Sci., 2018, Advance Article
DOI: 10.1039/C8SC03434F, Edge Article

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Ir(III)-catalyzed ortho C–H alkylations of (hetero)aromatic aldehydes using alkyl boron reagents
Xiao-Yang Chen and Erik J. Sorensen
Chem. Sci., 2018, Advance Article
DOI: 10.1039/C8SC03606C, Edge Article

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Direct observation of the intermediate in an ultrafast isomerization
Tyler M. Porter, Jiaxi Wang, Yingmin Li, Bo Xiang, Catherine Salsman, Joel S. Miller, Wei Xiong and Clifford P. Kubiak
Chem. Sci., 2018, Advance Article
DOI: 10.1039/C8SC03258K, Edge Article

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Structural control of polyelectrolyte/microemulsion droplet complexes (PEMECs) with different polyacrylates
Miriam Simon, Patrick Krause, Leonardo Chiappisi, Laurence Noirez and Michael Gradzielski
Chem. Sci., 2019, Advance Article
DOI: 10.1039/C8SC04013C, Edge Article

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Reversibility and reactivity in an acid catalyzed cyclocondensation to give furanochromanes – a reaction at the ‘oxonium-Prins’ vs. ‘ortho-quinone methide cycloaddition’ mechanistic nexus
Christian D.-T. Nielsen, Wouter J. Mooij, David Sale, Henry S. Rzepa, Jordi Burés and Alan C. Spivey
Chem. Sci., 2018, Advance Article
DOI: 10.1039/C8SC04302G, Edge Article

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Chemical Science symposia on sustainable energy

19 Oct 2018

By Carri Cotton.

Registration is now open for our Chemical Science symposia, which are to be held in two locations in China (Harbin and Xiamen) in December.

The NSFC-RSC International Symposium on Energy Chemistry will be held in Harbin, China from 7th-9th of December, you can register now here.

The Chemical Science Symposium on Sustainable Energy will be held in Xiamen, China on 10th of December, you can register now here.

The theme of the Chemical Science Symposium will be renewable energy and sustainability, bringing together leading researchers in the field of energy science and related subjects. The primary focus will be on recent advances in sustainable and renewable energy including solar energy conversion, artificial photosynthesis, photocatalysts, water splitting, gas capture, separation and storage and fuel cells. The symposia will also cover interdisciplinary studies at the energy interface with other subjects such as the properties and applications of materials for energy and sustainability, nanotechnology, photocatalysis, photonics and biotechnology.

Chemical Science Associate Editors Vincent Artero, Kazunari Domen, James McCusker and Jihong Yu will be speaking at both symposia, and Executive Editor May Copsey will be attending.

We look forward to seeing you there!

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Mutant Enzymes and Frankenstein Catalysts

04 Oct 2018

By Zoë Hearne.

I know what you’re thinking: “Autumn is here! Who needs sunny weather and optimism? Sign me up for grey skies and vitamin D supplements!”. Oh you weren’t thinking that? Me neither. Well perhaps Halloween gives you more joy, along with the chance to see one of your colleagues dressed up like Freddy Mercury (‘Hg’ emblazoned on their chest, classic) at the departmental party?

In the spirit of Halloween, Simone Morra and Anca Pordea at the University of Nottingham have synthesized a mutant alcohol dehydrogenase enzyme turned Frankenstein catalyst, by replacing the zinc catalytic site with a covalently-bound rhodium(III) complex. The resulting mutant/transition-metal composite was used in combination with the wild-type enzyme to synthesize the chiral alcohol (S)-4-phenyl-2-butanol.

Like many hybrid systems, the purpose of combining enzymatic with transition metal catalysis is to take advantage of the benefits of each. Millions of years of evolution have produced enzymatic catalysts that function under mild conditions, in aqueous solvents, with impressive selectivity and high catalytic efficiency. But the narrow range of conditions that enzymes operate under can be disadvantageous in a synthetic setting. On the other hand, transition metal catalysts are versatile and can be easily customised, reacting with a liberty that would make the most promiscuous of enzymes blush.

Unfortunately, developing multi-component systems that utilise both transition metal and enzymatic catalysis is not as simple as combining them in a single mixture, as mutual deactivation often results. The authors found that encasing the transition metal complex in an enzyme provided a physical shield against inhibition, and preserved the activity of both the wild type enzyme and the rhodium(III) complex.

Synthesis of chiral alcohols via two interconnected cycles: the wild type enzyme (native ADH) reduces the ketone to the alcohol using NADPH as a reducing agent. NADPH is regenerated using the mutant enzyme containing a rhodium active site (chemically modified ADH) with formic acid as the terminal reductant. Alcohol dehydrogenase

Synthesis of chiral alcohols via two interconnected cycles: the wild type enzyme (native ADH) reduces the ketone using NADPH as a reducing agent. NADPH is regenerated by the mutant enzyme containing a catalytically-active rhodium complex (chemically modified ADH) with formic acid as the terminal reductant.

Two interconnected catalytic cycles were responsible for synthesis of the chiral alcohol. In the first, the wild type enzyme effected reduction of 4-phenyl-2-butanol, a process that relies on the biological reductant nicotinamide adenine dinucleotide phosphate (NADPH). In the second cycle, NADPH was recycled using the composite rhodium(III) complex/mutant enzyme, with formic acid as the stoichiometric reductant. The rate of alcohol formation was slow (turnover frequency of 0.02 s^-1) and the transition-metal catalysed process was deemed to be rate limiting (compare to turnover frequencies of 4.8 s^-1for enzymatic systems). However, near perfect enantioselectivity was obtained (>99% ee).

This research demonstrates one way that transition metal catalysts can augment the scope of co-factor-dependent enzymes. Furthermore, devising strategies to prepare metal-complex/enzyme bioconjugates might have value for small molecule synthesis due to the second coordination sphere that enzymes offer; an encased steric environment to guide the reaction outcome is a valuable approach to improving selectivity in catalytic reactions.

To find out more please read:

Biocatalyst-artifical metalloenzyme cascade based on alcohol dehydrogenase

Simone Morra, Anca Pordea.
Chem. Sci., 2018, 9, 7447-7454
DOI: 10.1039/c8sc02371a

About the author

Zoë Hearne is a PhD candidate in chemistry at McGill University in Montréal, Canada, under the supervision of Professor Chao-Jun Li. She hails from Canberra, Australia, where she completed her undergraduate degree. Her current research focuses on transition metal catalysis to effect novel transformations, and out of the lab she is an enthusiastic chemistry tutor and science communicator.

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HOT Chemical Science articles for September

04 Oct 2018

By Rebecca Withers.

We are happy to present a selection of our HOT articles over the past month. To see all of our HOT referee-recommended articles from 2018, please find the collection here.

As always, Chemical Science articles are free to access.

Selective and catalytic carbon dioxide and heteroallene activation mediated by cerium N-heterocyclic carbene complexes
Polly Louise Arnold, Ryan Kerr, Catherine Weetman, Scott Doherty, Julia Rieb, Kai Wang, Christian Jandl, Max McMullon, Alexander Pöthig, Fritz Elmar Kühn and Andrew D Smith
Chem. Sci., 2018, Accepted Manuscript
DOI: 10.1039/C8SC03312A, Edge Article

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Ratiometric fluorescent probes for capturing endogenous hypochlorous acid in the lungs of mice
Xinfu Zhang, Weiyu Zhao, Bin Li, Wenqing Li, Chengxiang Zhang, Xucheng Hou, Justin Jiang and Yizhou Dong
Chem. Sci., 2018, Advance Article
DOI: 10.1039/C8SC03226B, Edge Article

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Surprising solvent-induced structural rearrangements in large [N⋯I+⋯N] halogen-bonded supramolecular capsules: an ion mobility-mass spectrometry study
Ulrike Warzok, Mateusz Marianski, Waldemar Hoffmann, Lotta Turunen, Kari Rissanen, Kevin Pagel and Christoph A. Schalley
Chem. Sci., 2018, Advance Article
DOI: 10.1039/C8SC03040E, Edge Article

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Advanced microRNA-based cancer diagnostics using amplified time-gated FRET
Xue Qiu, Jingyue Xu, Jiajia Guo, Akram Yahia-Ammar, Nikiforos-Ioannis Kapetanakis, Isabelle Duroux-Richard, Julia J. Unterluggauer, Nicole Golob-Schwarzl, Christophe Regeard, Catherine Uzan, Sébastien Gouy, Michael DuBow, Johannes Haybaeck, Florence Apparailly, Pierre Busson and Niko Hildebrandt
Chem. Sci., 2018, Advance Article
DOI: 10.1039/C8SC03121E, Edge Article

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Atomic structure of boron resolved using machine learning and global sampling
Si-Da Huang, Cheng Shang, Pei-Lin Kang and Zhi-Pan Liu
Chem. Sci., 2018, Advance Article
DOI: 10.1039/C8SC03427C, Edge Article

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Spontaneous growth of 2D coordination polymers on functionalized ferromagnetic surfaces
Michele Mattera, Víctor Rubio-Giménez, Sophie Delprat, Richard Mattana, Pierre Seneor, Sergio Tatay, Alicia Forment-Aliaga and Eugenio Coronado
Chem. Sci., 2018, Advance Article
DOI: 10.1039/C8SC03067G, Edge Article

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Chemical Science Blog

Bristol Synthesis Meeting 2019

Andrei Yudin joins Chemical Science as an Associate Editor

Andrew Cooper – our new Editor-in-Chief of Chemical Science

Carbon Coating Promotes CO2 Reduction on Nickel Surfaces

Serena DeBeer joins Chemical Science as an Associate Editor

HOT Chemical Science articles for November

HOT Chemical Science articles for October

Chemical Science symposia on sustainable energy

Mutant Enzymes and Frankenstein Catalysts

HOT Chemical Science articles for September

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