Article
Chemistry, Inorganic & Nuclear
Zhou-Yan Lv, Gang Yang, Bao-Ping Ren, Zheng-Yan Liu, Hao Zhang, Li-Ping Si, Hai-Yang Liu, Chi-Kwong Chang
Summary: Three isomeric A(2)B-type new cobalt triaryl corroles with hydroxyphenyl substituents were synthesized and characterized. The hydroxyl position of the phenyl group significantly influenced the electrocatalytic hydrogen evolution reaction (HER). The ortho-hydroxyphenyl substituted cobalt corrole showed the best HER activity with a turnover frequency (TOF) and catalytic efficiency (C.E) of 318.68 s(-1) and 1.13, respectively. The o- and p-hydroxyl isomers exhibited higher efficiency in proton relay.
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Gang Yang, Jing-He Cen, Jian Lan, Meng-Yuan Li, Xuan Zhan, Gao-Qing Yuan, Hai-Yang Liu
Summary: A new phosphorus(V) complex [(TPFC)P-V(OH)(2)] was reported as an electrocatalyst for the hydrogen evolution reaction (HER), showing excellent activity and stability. It can serve as a sustainable alternative to precious metal catalysts.
Article
Chemistry, Applied
John Daniel McCool, Shiyuan Zhang, Inen Cheng, Xuan Zhao
Summary: This review article introduces the rational design of molecular metal complexes based on earth-abundant metals for electrocatalytic hydrogen production. It emphasizes providing insight into structure-function relationships in catalytic properties for future ligand and catalyst design.
CHINESE JOURNAL OF CATALYSIS
(2022)
Article
Chemistry, Multidisciplinary
Louise Ponsard, Emmanuel Nicolas, Ngoc Huan Tran, Sarah Lamaison, David Wakerley, Thibault Cantat, Marc Fontecave
Summary: A system coupling high-pressure CO2 electrolysis with thermal catalysis using high-pressure CO has been developed to convert CO2 into beta-butyrolactone, achieving a high reaction yield. This strategy enables the production of lactones from CO2 for polyester synthesis, expanding the range of chemicals derived from CO2.
Article
Chemistry, Physical
Daan den Boer, Quentin Siberie, Maxime A. Siegler, Thimo H. Ferber, Dominik C. Moritz, Jan P. Hofmann, Dennis G. H. Hetterscheid
Summary: This study demonstrates through experimental results that not all molecular Co-based water oxidation catalysts necessarily form CoOx under operating conditions, and the deposition of catalytic material is not necessarily linked to the decomposition of the catalyst.
Article
Chemistry, Multidisciplinary
Shize Geng, Yujin Ji, Jiaqi Su, Zhiwei Hu, Miaomiao Fang, Dan Wang, Shangheng Liu, Ling Li, Youyong Li, Jin-Ming Chen, Jyh-Fu Lee, Xiaoqing Huang, Qi Shao
Summary: Catalytic reactions are surface-sensitive processes. Homogeneous metastable hexagonal close-packed (hcp) Ir is grown onto metastable phase hcp Ni, demonstrating high intrinsic activity for the alkaline hydrogen evolution reaction (HER) with low overpotential and high specific activity. The stable structure of epitaxially grown metastable hcp Ir contributes to its remarkable HER activity, making it a potential catalyst for fundamental catalytic applications.
Article
Chemistry, Applied
Zheng-Mei Zhu, Wei-Yu Peng, Wu Yang, Chen Ling, Hao Zhang, Li-Ping Si, Hai-Yang Liu
Summary: Four cobalt corrole complexes with substituents of methoxy or hydroxyl groups were synthesized and showed high electrocatalytic activity for hydrogen evolution reaction in both organic and aqueous phases. Cobalt corrole 4 exhibited the best hydrogen evolution performance.
APPLIED ORGANOMETALLIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Soumyadeep Chakrabortty, Katharina Konieczny, Felix J. de Zwart, Eduard. O. Bobylev, Eszter Barath, Sergey Tin, Bernd H. Mueller, Joost N. H. Reek, Bas de Bruin, Johannes G. de Vries
Summary: Researchers achieved enantioselective hydrogenation of cyclic enamides using an earth-abundant cobalt-bisphosphine catalyst. The catalytic system, CoCl2/(S,S)-Ph-BPE, reduced trisubstituted carbocyclic enamides to saturated amides with high activity and excellent enantioselectivity (up to 99%). The methodology can be extended to the synthesis of chiral amines by base hydrolysis of the hydrogenation products. Preliminary mechanistic investigations suggested a sigma-bond-metathesis pathway for the hydrogenation of the carbon-carbon double bond, involving a high spin cobalt (II) species.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Silvia Gutierrez-Tarrino, Sergio Rojas-Buzo, Manuel A. Ortuno, Pascual Ona-Burgos
Summary: The development of a circular economy plays a crucial role in reducing dependence on fossil fuels and promoting sustainable processes. This study introduces a sustainable methodology using a stable cobalt-based catalyst to produce value-added silicon precursors and hydrogen via dehydrogenative coupling. The reaction conditions are mild and the selectivity of hydrosilylation/hydroalkoxysilylation reactions can be controlled by adjusting the alcohol/water ratio.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2022)
Article
Chemistry, Physical
Cassandre C. Bories, Marion Barbazanges, Etienne Derat, Marc Petit
Summary: This study describes the use of silyl cobalt (III) dihydride complexes as catalysts for hydrosilylation reactions, which are efficient for a variety of imines with different protecting groups, as well as aliphatic ketimines and quinoline. Kinetic, DFT calculations, NMR spectroscopy, deuteration experiments, and X-ray diffraction analyses were used to propose a catalytic cycle based on silyl dihydrocobalt (III) complexes performing hydrocobaltation.
Article
Chemistry, Multidisciplinary
Hikaru Iwami, Masaya Okamura, Mio Kondo, Shigeyuki Masaoka
Summary: This study presents a strategy to integrate catalytic centers and hole transporters in one system, demonstrating the efficient catalytic activity of Poly-1 in water oxidation.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Emir Al-Sayed, Sreejith P. Nandan, Elias Tanuhadi, Gerald Giester, Marco Arrigoni, Georg K. H. Madsen, Alexey Cherevan, Dominik Eder, Annette Rompel
Summary: In this study, three abundant-metal-based germanotungstate clusters were synthesized using a PO43- template. These clusters showed activity as molecular water oxidation catalysts, with Co-9 and Co-20 outperforming a well-known catalyst by a factor of 2. Among them, Co-9 currently represents the fastest Co-GT-based water oxidation catalyst, with a turnover frequency of 0.608 s(-1) and a turnover numbers (TONs) up to 159.9.
Article
Chemistry, Multidisciplinary
Wence Xu, Guilan Fan, Shengli Zhu, Yanqin Liang, Zhenduo Cui, Zhaoyang Li, Hui Jiang, Shuilin Wu, Fangyi Cheng
Summary: This study introduces carbon-doped nanoporous cobalt phosphide as an electrocatalyst for hydrogen evolution reaction in seawater electrolysis, showing excellent catalytic activity and stability. Carbon atoms can tailor the electronic structure, reducing the energy barrier of water dissociation and promoting the kinetics of HER.
ADVANCED FUNCTIONAL MATERIALS
(2021)
Article
Chemistry, Physical
Fan Yang, Yi-Chen Nie, Han-Yuan Liu, Lei Zhang, Fanyang Mo, Rong Zhu
Summary: A general Co(II/III/IV) electrocatalytic platform for alkene functionalization is proposed, enabling a set of oxidative hydrofunctionalization reactions via hydrogen atom transfer without stoichiometric chemical oxidants. The study demonstrates an expansion in reactivity space in electrocatalysis by going beyond the common oxidation states of Co(I/II/III) in the VB12 system.
Article
Chemistry, Physical
Michael Benjamin, Devaraj Manoj, K. Theyagarajan, Kathavarayan Thenmozhi, Duraisamy Saravanakumar, Sellappan Senthilkumar
Summary: Electrocatalytic hydrogen production in a neutral aqueous medium is a promising technology to obtain clean and carbon-free fuel. The use of cobalt terpyridine complexes as catalysts showed superior electrocatalytic activity and high faradaic efficiency in generating hydrogen.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Engineering, Chemical
Amina Amarray, Sanae El Ghachtouli, Youssef Samih, Mouad Dahbi, Mohammed Azzi
Summary: A clean, sustainable, and efficient method using electrodeposited Na-MnO2/SnO2 for Cd(II) ions removal was proposed and analyzed. The results showed that films with the lowest charge quantity and highest oxidation state had the highest electrosorption capacity. Comparative study demonstrated that electrosorption was more effective in treatment kinetics and elimination capacity of Cd(II) compared to adsorption.
Article
Chemistry, Physical
Jennifer Dupont, Regis Guillotb, Valeria Lepere, Anne Zehnacker
Summary: The structures of diastereomer diketopiperazine dipeptides cyclo(LTyr-LPhe) and cyclo-(DTyr-LPhe) were studied in the gas phase using resonance-enhanced two-photon ionization, IR/UV double resonance spectroscopy, and quantum chemical calculation. Both diastereomers exhibit two conformations with slight differences in weak CH···ir and NH···ir interactions. The crystal structure and vibrational circular dichroism spectrum were determined, with quantum chemical calculation shedding light on structural modifications between the gas phase and the solid state.
JOURNAL OF MOLECULAR STRUCTURE
(2022)
Article
Chemistry, Multidisciplinary
Sascha Jahnigen, Katia Le Barbu-Debus, Regis Guillot, Rodolphe Vuilleumier, Anne Zehnacker
Summary: In this study, the effect of a twofold screw axis on the solid-state VCD spectrum was investigated using both experimental and theoretical analysis. It was found that the VCD spectrum can reflect the supramolecular chirality of the crystal.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Chanjuan Zhang, Philipp Gotico, Regis Guillot, Diana Dragoe, Winfried Leibl, Zakaria Halime, Ally Aukauloo
Summary: At the core of carbon monoxide dehydrogenase (CODH) active site, two metal ions and hydrogen bonding from amino acids facilitate the interconversion between CO2 and CO. A designed molecular catalyst with a bimetallic iron complex and hydrogen bonding interactions showed improved selectivity and stability in heterogeneous CO2 reduction to CO. X-ray structures revealed the compromise between rigidity and flexibility of the catalyst in accommodating CO2 capture, activation, and reduction.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Audrey Mauger, Maxime Jarret, Aurelien Tap, Remi Perrin, Regis Guillot, Cyrille Kouklovsky, Vincent Gandon, Guillaume Vincent
Summary: We synthesized highly strained pentacyclic caged framework of mavacuran alkaloids and successfully achieved the concise total synthesis of C-fluorocurine, C-profluorocurine, C-mavacurine, normavacurine, 16-epi-pleiocarpamine and taberdivarine H. A strategy involving late-stage Michael addition and intermolecular 1,4-addition reactions was designed. The first total syntheses of C-profluorocurine and C-fluorocurine were achieved through dihydroxylation of C-mavacurine and a pinacol rearrangement, respectively.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Yuna Kim, Clemence Allain, Regis Guillot, Pierre Audebert
Summary: This article describes a tetrazine derivative that exhibits color-tunable crystals upon external stimuli. By heating and cooling processes, Bis(4-methylphenoxy)tetrazine (1) forms crystalline phases with photoluminescence color transitions ranging from green to red. These thermoresponsive polymorphisms and colors can be reversibly recovered by solvent vapor annealing. Additionally, the unique T-shape arrangement of the tetrazine rings and the phenyl rings leads to the formation of flexible crystals.
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
(2023)
Article
Chemistry, Organic
Dayi Liu, Zeynab Imani, Catherine Gourson, Regis Guillot, Sylvie Robin, David J. J. Aitken
Summary: Post-synthetic modification is a powerful technique for accessing noncanonical peptide derivatives selectively, but it has not been used for installing multiple arrays of modified side chains. In this study, we applied this approach in solution phase to prepare short N- and C-capped homooligomers of 3-amino-1-methylazetidine-3-carboxylic acid with all azetidine side chain functions in the free amine form. The key step involved multiple reductive amination reactions of the corresponding post-synthetically deprotected secondary amines.
Article
Chemistry, Multidisciplinary
Mehdi Salmi, Amina Amarray, Youssef Samih, Mohammed Azzi, Sanae EL Ghachtouli
Summary: In this study, nickel sulfide thin film incorporated with carbon nanofibers (Ni4S3-CNF/ITO) was successfully electrodeposited on indium tin oxide. The electrocatalytic activity of Ni4S3-CNF/ITO towards methanol oxidation reaction (MOR) was investigated and showed high activity and stability in an alkaline medium. The addition of carbon nanofibers increased the surface area and improved the tolerance to catalyst-poising species, making it a promising low-cost and efficient fuel cell electrocatalyst.
Article
Energy & Fuels
M. Ait Himi, A. Sghiouri, B. Youbi, Y. Lghazi, A. Amarray, M. Aqil, A. Ouedrhiri, J. Bahar, C. El Haimer, A. Aynaou, L. Hdidou, I. Bimaghra, M. Dahbi, S. El Ghachtouli
Summary: The effect of applied potential on the crystallography, morphology, optical properties, and electrochemical performances of manganese oxide electrodeposited on ITO substrate was investigated. Lamellar structure was observed in all electrodeposited materials regardless of the applied potential, but the crystallite size, crystallinity, and sheets diameter were affected. Increase in applied potential resulted in higher bandgap energy for all the materials. The electrodeposited material at a potential of 1 V/SCE showed higher specific capacitance and the effect of electrodeposition potential on diffusion and capacitive contributions was analyzed.
JOURNAL OF ENERGY STORAGE
(2023)
Article
Engineering, Chemical
Amina Amarray, Mehdi Salmi, M'hamed Oubla, El-Kebir Hlil, Mouad Dahbi, Khaoula Khaless, Mohammed Azzi, Sanae Elghachtouli
Summary: This study presents a new approach for the purification of cadmium-contaminated phosphoric acid using synthesized lamellar material based on manganese (Na-MnO2). The removal efficiencies of cadmium ions were 35% and 31% for 54% and 29% P2O5 phosphoric acid, respectively. Kinetic and isotherm studies were conducted, and the Na-MnO2 material was characterized using various techniques. The results confirmed the potential of Na-MnO2 as an efficient sorbent for heavy metal removal from phosphoric acid solutions.
Article
Chemistry, Inorganic & Nuclear
Roxanne Bercy, Jean-Noel Rebilly, Christian Herrero, Regis Guillot, Helene Maisonneuve, Frederic Banse
Summary: In this study, three new iron complexes with amine/pyridine ligands were designed and used as catalysts for the oxidation of small organic molecules by hydrogen peroxide. The addition of acetic acid was found to significantly enhance the efficiency of these catalytic systems. Acetic acid promoted the protonation/dissociation of the ligands and the formation of more efficient intermediates.
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Organic
Dayi Liu, Regis Guillot, Sylvie Robin, David J. Aitken
Summary: In this study, trans-3-benzyloxycarbonylamino-1-methyl-3-(methylcarbamoyl)azetidine-1-oxide was successfully synthesized by stereoselective oxidation. The stable molecule was characterized in solution and solid state, revealing different intramolecular and intermolecular hydrogen bonding patterns.
Article
Chemistry, Inorganic & Nuclear
Diana Cebotari, Sergiu Calancea, Jerome Marrot, Regis Guillot, Clement Falaise, Vincent Guerineau, David Touboul, Mohamed Haouas, Aurelian Gulea, Sebastien Floquet
Summary: This paper reports the synthesis and characterization of six coordination complexes obtained by reacting [MoV2 O2S(2)](2+) clusters with bisthiosemicarbazone ligands containing flexible or rigid spacers. The nuclearity of the complexes was found to be controlled by the nature of the spacer between the thiosemicarbazone units, as revealed by structural characterization techniques. Flexible spacers resulted in binuclear complexes [MoV2 O2S2(L1-3)], while rigid spacers led to tetranuclear complexes [(MoV2 O2S2)(2)(L4-6)(2)].
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Inorganic & Nuclear
Jean-Noel Rebilly, Christian Herrero, Katell Senechal-David, Regis Guillot, Frederic Banse
Summary: The catalytic properties of an iron complex with a pentadentate cross-bridged ligand backbone were investigated. It exhibited moderate conversions in epoxidation and alkane hydroxylation with H2O2 as the oxidant, and satisfactory conversions in aromatic hydroxylation. However, the addition of acid to the reaction medium significantly enhanced the oxidation of aromatics and alkenes. Spectroscopic analysis revealed that the accumulation of the expected Fe-III(OOH) intermediate was limited under these conditions, unless an acid was present, which was attributed to the inertness induced by the cross-bridged ligand backbone that was partly reduced under acidic conditions.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Organic
Nabila Braia, Mounia Merabet-Khelassi, Martial Toffano, Regis Guillot, Louisa Aribi-Zouioueche
Summary: In this paper, we report the highly selective ring opening of a biobased itaconic anhydride catalyzed by Pseudomonas cepacia lipase at room temperature. This method is efficient and environmentally friendly, allowing for the synthesis of valuable itaconate esters using a variety of alcohols as nucleophiles. The reaction yields novel itaconate products when achiral primary alcohols are used as substrates.
ORGANIC & BIOMOLECULAR CHEMISTRY
(2022)
