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1.
J Am Chem Soc ; 146(13): 9434-9443, 2024 Apr 03.
Artigo em Inglês | MEDLINE | ID: mdl-38507716

RESUMO

Electrocatalytic synthesis of hydrogen peroxide (H2O2) in acidic media is an efficient and eco-friendly approach to produce inherently stable H2O2, but limited by the lack of selective and stable catalysts under industrial-relevant current densities. Herein, we report a diatomic cobalt catalyst for two-electron oxygen reduction to efficiently produce H2O2 at 50-400 mA cm-2 in acid. Electrode kinetics study shows a >95% selectivity for two-electron oxygen reduction on the diatomic cobalt sites. In a flow cell device, a record-high production rate of 11.72 mol gcat-1 h-1 and exceptional long-term stability (100 h) are realized under high current densities. In situ spectroscopic studies and theoretical calculations reveal that introducing a second metal into the coordination sphere of the cobalt site can optimize the binding strength of key H2O2 intermediates due to the downshifted d-band center of cobalt. We also demonstrate the feasibility of processing municipal plastic wastes through decentralized H2O2 production.

2.
JACS Au ; 4(5): 1975-1985, 2024 May 27.
Artigo em Inglês | MEDLINE | ID: mdl-38818058

RESUMO

Chemical looping ammonia synthesis (CLAS) is a promising technology for reducing the high energy consumption of the conventional ammonia synthesis process. However, the comprehensive understanding of reaction mechanisms and rational design of novel nitrogen carriers has not been achieved due to the high complexity of catalyst structures and the unrevealed relationship between electronic structure and intrinsic activity. Herein, we propose a multistage strategy to establish the connection between catalyst intrinsic activity and microscopic electronic structure fingerprints using density functional theory computational energetics as bridges and apply it to the rational design of metal nitride catalysts for lattice nitrogen-mediated ammonia production. Molybdenum-based nitride catalysts with well-defined structures are employed as prototypes to elucidate the decoupled effects of electronic and geometrical features. The electron-transfer and spin polarization characteristics of the magnetic metals are constructed as descriptors to disclose the atomic-scale causes of intrinsic activity. Based on this design strategy, it is demonstrated that Ni3Mo3N catalysts possess the highest lattice nitrogen-mediated ammonia synthesis activity. This work reveals the structure-activity relationship of metal nitrides for CLAS and provides a multistage perspective on catalyst rational design.

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