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Structural determinants of oxygen resistance and Zn-mediated stability of the [FeFe]-hydrogenase from .
Proc Natl Acad Sci U S A
January 2025
Laboratory for Protein Crystallography, Institute for Protein Research, Osaka University, Suita, Osaka 565-0871, Japan.
[FeFe]-hydrogenases catalyze the reversible two-electron reduction of two protons to molecular hydrogen. Although these enzymes are among the most efficient H-converting biocatalysts in nature, their catalytic cofactor (termed H-cluster) is irreversibly destroyed upon contact with dioxygen. The [FeFe]-hydrogenase CbA5H from has a unique mechanism to protect the H-cluster from oxygen-induced degradation.
View Article and Find Full Text PDFRedox-Active Water-Soluble Low-Weight and Polymer-Based Anolytes Containing Tetrazine Groups: Synthesis and Electrochemical Characterization.
Polymers (Basel)
December 2024
Chemistry Department, Lomonosov Moscow State University, Moscow 119991, Russia.
Polymer-based aqueous redox flow batteries (RFBs) are attracting increasing attention as a promising next-generation energy storage technology due to their potential for low cost and environmental friendliness. The search for new redox-active organic compounds for incorporation into polymer materials is ongoing, with anolyte-type compounds in high demand. In response to this need, we have synthesized and tested a range of new water-soluble redox-active s-tetrazine derivatives, including both low molecular weight compounds and polymers with different architectures.
View Article and Find Full Text PDFNatural Densitals.
J Phys Chem Lett
January 2025
Faculty of Chemistry, Department of Physical and Quantum Chemistry, Wrocław University of Science and Technology, Wybrzeże Wyspiańskiego 27, 50-370 Wrocław, Poland.
The concept of natural densitals (NDs) and their amplitudes is introduced. These quantities provide the spectral decomposition of the cumulant of the two-electron density that, by definition, quantifies the extent of electron correlation. Consequently, they are ideally suited for a rigorous description of electron correlation effects in Coulombic systems.
View Article and Find Full Text PDFVacancy-Activated B-Doping for Efficient 2e- Oxygen Reduction through Suppressing H2O2 Decomposition at High Overpotential.
Angew Chem Int Ed Engl
January 2025
China University of Petroleum East China, State Key Laboratory of Heavy Oil Processing, 66 The Yangtze River West Road, 266580, Qingdao, CHINA.
The production of hydrogen peroxide (H2O2) through two-electron oxygen reduction reaction (2e- ORR) has emerged as a more environmentally friendly alternative to the traditional anthraquinone method. Although oxidized carbon catalysts have intensive developed due to their high selectivity and activity, the yield and conversion rate of H2O2 under high overpotential still limited. The produced H2O2 was rapidly consumed by the increased intensity of H2O2 reduction, which could ascribe to decomposition of peroxide radicals under high voltage in the carbon catalyst.
View Article and Find Full Text PDFEfficient Electrosynthesis of Hydrogen Peroxide Enabled by a Hierarchical Hollow RE-P-O (RE = Sm, La, Gd) Architecture with Open Channels.
Adv Mater
January 2025
Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, 199 Ren'ai Road, Suzhou, Jiangsu, 215123, China.
The electrochemical two-electron oxygen reduction reaction (2e ORR) offers a sustainable pathway for the production of HO; however, the development of electrocatalysts with exceptional activity, selectivity, and long-term stability remains a challenging task. Herein, a novel approach is presented to addressing this challenge by synthesizing hierarchical hollow SmPO nanospheres with open channels via a two-step hydrothermal treatment. The produced compound demonstrates remarkable 2e selectivity, exceeding 93% across a wide potential range of 0.
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