High‐Efficiency Oxygen Reduction to Hydrogen Peroxide Catalyzed by Nickel Single‐Atom Catalysts with Tetradentate N2O2 Coordination in a Three‐Phase Flow Cell DOI
Yulin Wang, Run Shi, Lu Shang

et al.

Angewandte Chemie International Edition, Journal Year: 2020, Volume and Issue: 59(31), P. 13057 - 13062

Published: April 28, 2020

Carbon-supported NiII single-atom catalysts with a tetradentate Ni-N2 O2 coordination formed by Schiff base ligand-mediated pyrolysis strategy are presented. A complex of the ligand (R,R)-(-)-N,N'-bis(3,5-di-tert-butylsalicylidene)-1,2-cyclohexanediamine was adsorbed onto carbon black support, followed modified material at 300 °C in Ar. The /C catalyst showed excellent performance for electrocatalytic reduction to H2 through two-electron transfer process alkaline conditions, selectivity 96 %. At current density 70 mA cm-2 , production rate 5.9 mol gcat.-1 h-1 achieved using three-phase flow cell, good stability maintained over 8 h testing. could electrocatalytically reduce air high density, still affording (>90 %). precise key performance.

Language: Английский

Identification of the Highly Active Co–N4 Coordination Motif for Selective Oxygen Reduction to Hydrogen Peroxide DOI
Shanyong Chen, Tao Luo, Xiaoqing Li

et al.

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(32), P. 14505 - 14516

Published: Aug. 3, 2022

Electrosynthesis of hydrogen peroxide (H

Language: Английский

Citations

332
Oxygen Evolution/Reduction Reaction Catalysts: From In Situ Monitoring and Reaction Mechanisms to Rational Design DOI
Yonggui Zhao, Devi Prasad Adiyeri Saseendran, Chong Huang

et al.

Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(9), P. 6257 - 6358

Published: March 21, 2023

The oxygen evolution reaction (OER) and reduction (ORR) are core steps of various energy conversion storage systems. However, their sluggish kinetics, i.e., the demanding multielectron transfer processes, still render OER/ORR catalysts less efficient for practical applications. Moreover, complexity catalyst–electrolyte interface makes a comprehensive understanding intrinsic mechanisms challenging. Fortunately, recent advances in situ/operando characterization techniques have facilitated kinetic monitoring under conditions. Here we provide selected highlights mechanistic studies with main emphasis placed on heterogeneous systems (primarily discussing first-row transition metals which operate basic conditions), followed by brief outlook molecular catalysts. Key sections this review focused determination true active species, identification sites, reactive intermediates. For in-depth insights into above factors, short overview metrics accurate characterizations is provided. A combination obtained time-resolved information reliable activity data will then guide rational design new Strategies such as optimizing restructuring process well overcoming adsorption-energy scaling relations be discussed. Finally, pending current challenges prospects toward development homogeneous presented.

Language: Английский

Citations

331
Single-atom alloy catalysts: structural analysis, electronic properties and catalytic activities DOI
Tianjun Zhang,

Andrew G. Walsh,

Jihong Yu

et al.

Chemical Society Reviews, Journal Year: 2020, Volume and Issue: 50(1), P. 569 - 588

Published: Nov. 10, 2020

The structure–property relationship of single-atom alloy catalysts is reviewed from the perspective atomic structure analysis, electronic properties, and catalytic activities.

Language: Английский

Citations

327
Fe/Cu diatomic catalysts for electrochemical nitrate reduction to ammonia DOI Creative Commons
Shuo Zhang,

WU Jiang-hua,

Mengting Zheng

et al.

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: June 19, 2023

Electrochemical conversion of nitrate to ammonia offers an efficient approach reducing pollutants and a potential technology for low-temperature low-pressure synthesis. However, the process is limited by multiple competing reactions NO3- adsorption on cathode surfaces. Here, we report Fe/Cu diatomic catalyst holey nitrogen-doped graphene which exhibits high catalytic activities selectivity production. The enables maximum Faradaic efficiency 92.51% (-0.3 V(RHE)) NH3 yield rate 1.08 mmol h-1 mg-1 (at - 0.5 V(RHE)). Computational theoretical analysis reveals that relatively strong interaction between promotes discharge anions. Nitrogen-oxygen bonds are also shown be weakened due existence hetero-atomic dual sites lowers overall reaction barriers. dual-site hetero-atom strategy in this work provides flexible design further development expands electrocatalytic techniques reduction

Language: Английский

Citations

322
High‐Efficiency Oxygen Reduction to Hydrogen Peroxide Catalyzed by Nickel Single‐Atom Catalysts with Tetradentate N2O2 Coordination in a Three‐Phase Flow Cell DOI
Yulin Wang, Run Shi, Lu Shang

et al.

Angewandte Chemie International Edition, Journal Year: 2020, Volume and Issue: 59(31), P. 13057 - 13062

Published: April 28, 2020

Carbon-supported NiII single-atom catalysts with a tetradentate Ni-N2 O2 coordination formed by Schiff base ligand-mediated pyrolysis strategy are presented. A complex of the ligand (R,R)-(-)-N,N'-bis(3,5-di-tert-butylsalicylidene)-1,2-cyclohexanediamine was adsorbed onto carbon black support, followed modified material at 300 °C in Ar. The /C catalyst showed excellent performance for electrocatalytic reduction to H2 through two-electron transfer process alkaline conditions, selectivity 96 %. At current density 70 mA cm-2 , production rate 5.9 mol gcat.-1 h-1 achieved using three-phase flow cell, good stability maintained over 8 h testing. could electrocatalytically reduce air high density, still affording (>90 %). precise key performance.

Language: Английский

Citations

307