Atomically Dispersed Co/Mo Sites Anchored on Mesoporous Carbon Hollow Spheres for Highly Selective Oxygen Reduction to Hydrogen Peroxide in Acidic Media DOI Open Access
Min Yang,

Weihao Song,

Chengjin Chen

et al.

Advanced Materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 14, 2025

Abstract Two‐electron oxygen reduction reaction (2e − ORR) in acidic media is a promising route for the decentralized and on‐site hydrogen peroxide (H 2 O ) generation. Nevertheless, strong interaction between active sites * OOH intermediates usually induces O─O bond cleavage to convert 2e pathway into sluggish 4e ORR. Therefore, it highly necessary optimize electronic structure of ORR electrocatalysts regulation adsorption energy. Herein, we propose utilization atomically dispersed Co/Mo anchored on mesoporous carbon hollow spheres (Co/Mo‐MCHS) via template‐engaged strategy selective H acid. Benefitting from electron‐donating effect Mo atoms, an enriched electron density around Co center Co/Mo‐MCHS observed, resulting optimal key approach apex volcano plot. Moreover, introduction species simultaneously suppresses electroreduction as‐obtained sites. As consequence, delivers high selectivity 90–95% The flow cell based catalyst achieves remarkable yield 2102 mg 150 h. this can be extended other early transition metal elements with similar modifier effects.

Language: Английский

Selective oxygen reduction reaction: mechanism understanding, catalyst design and practical application DOI Creative Commons
Shilong Li, Lei Shi, Yingjie Guo

et al.

Chemical Science, Journal Year: 2024, Volume and Issue: 15(29), P. 11188 - 11228

Published: Jan. 1, 2024

The oxygen reduction reaction (ORR) is a key component for many clean energy technologies and other industrial processes. However, the low selectivity sluggish kinetics of ORR catalysts have hampered conversion efficiency real application these new mentioned before. Recently, tremendous efforts been made in mechanism understanding, electrocatalyst development system design. Here, comprehensive critical review provided to present recent advances field electrocatalytic ORR. two-electron four-electron transfer catalytic mechanisms evaluation parameters are discussed first. Then, up-to-date synthetic strategies

Language: Английский

Citations

22
Advancing H2O2 electrosynthesis: enhancing electrochemical systems, unveiling emerging applications, and seizing opportunities DOI
Zhiping Deng, Seung Joon Choi, Ge Li

et al.

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(16), P. 8137 - 8181

Published: Jan. 1, 2024

Hydrogen peroxide (H

Language: Английский

Citations

21
Site-designed dual-active-center catalysts for co-catalysis in advanced oxidation processes DOI Creative Commons
Wenxin Sun, Guoshuai Liu,

Hua Zou

et al.

npj Materials Sustainability, Journal Year: 2025, Volume and Issue: 3(1)

Published: Jan. 7, 2025

Abstract Advanced Oxidation Processes (AOPs) are promising for treating persistent pollutants, yet challenges arise due to the step-wise oxidants activation process, which traditional single-active-center catalysts struggle facilitate effectively. Recently, dual-active-center have emerged as a solution by enabling synergistic reactions. This review covers advances in these catalysts, their co-catalytic mechanisms, and applications electro-Fenton, photocatalytic, peroxymonosulfate-, pollutant-as-electron-donor based Fenton-like processes, along with active site design considerations future challenges.

Language: Английский

Citations

4
Accelerated O2 adsorption and stabilized *OOH for electrocatalytic H2O2 production DOI

Danni Deng,

Jinxian Wang, Meng Wang

et al.

Journal of Material Science and Technology, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

Language: Английский

Citations

4
Recent advances and challenges of double-atom catalysts in diverse environmental applications: A state-of-the-art review DOI
Tong Hu, Wenjun Zhou,

Wangwang Tang

et al.

Coordination Chemistry Reviews, Journal Year: 2025, Volume and Issue: 532, P. 216545 - 216545

Published: Feb. 19, 2025

Language: Английский

Citations

2
Metal–Organic Frameworks Derived Carbon‐Supported Metal Electrocatalysts for Energy‐Related Reduction Reactions DOI Creative Commons
Jiawei Zhu, Xue Feng Lu, Deyan Luan

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(38)

Published: June 21, 2024

Electrochemical reduction reactions, as cathodic processes in many energy-related devices, significantly impact the overall efficiency determined mainly by performance of electrocatalysts. Metal-organic frameworks (MOFs) derived carbon-supported metal materials have become one star electrocatalysts due to their tunable structure and composition through ligand design screening. However, for different electroreduction required active species vary phase component, electronic state, catalytic center configuration, hence requiring effective customization. From this perspective, review comprehensively analyzes structural principles, loading strategies, practical performance, complex mechanisms, thereby providing insights guidance future rational such catalysts.

Language: Английский

Citations

15
Recent advances in electrosynthesis of H2O2via two-electron oxygen reduction reaction DOI Creative Commons
Ao Yu, Shengwen Liu, Yang Yang

et al.

Chemical Communications, Journal Year: 2024, Volume and Issue: 60(40), P. 5232 - 5244

Published: Jan. 1, 2024

This review provides an electrosynthesis strategy of H 2 O via the 2e − ORR, covering aspects reaction mechanisms, performance assessment, catalyst engineering, and setups for scaling up production.

Language: Английский

Citations

11
Efficient Photocatalytic Two-Electron Halide Oxidation over p-Block Metal Bi- and Sb-Based Catalysts DOI
Ruofan Li, Ling Zhang, Qin Xin

et al.

ACS Catalysis, Journal Year: 2025, Volume and Issue: 15(3), P. 2171 - 2179

Published: Jan. 22, 2025

Halide (X–, X = Cl, Br) oxidation provides a promising alternative to water reaction (WOR) due the feasibility of reaction, richness reactants, and extensive application products (X2, HOX, OX–) for photocatalysis. Bismuth oxyhalide (BiOX) is still most efficient photocatalyst applied halide ever reported, but relative mechanisms remain understudied, reactivity needs be optimized. Herein, Sb(III) introduced into BiOX (Sb-BiOX), by involving itself in cycle reactive oxygen species, was significantly boosted, affording HClO up 482.5 μM within 30 min. Endowed favorable 2e– redox couple their unique s2 electron configuration Bi(III) Sb(III), X– performed manner over Sb-BiOX. Because introduction high-valent metal (M(V), M Sb, Bi) peroxide (M-OOH) could generated more expeditiously easily situ under light irradiation, which are revealed key oxidizing species oxidation. This work an in-depth understanding promoting photocatalytic offer inspiring paradigms energy-related small-molecule conversion reactions that rely on WOR half-reaction.

Language: Английский

Citations

1
Engineering Asymmetric Electronic Structure of Co─N─C Single‐Atomic Sites Toward Excellent Electrochemical H2O2 Production and Biomass Upgrading DOI Open Access
Kun Yu, Shiyou Guan, Wenbiao Zhang

et al.

Angewandte Chemie International Edition, Journal Year: 2025, Volume and Issue: unknown

Published: March 11, 2025

Abstract To advance electrochemical H 2 O production and unravel catalytic mechanisms, the precise structural coordination of single‐atomic M‐N‐C electrocatalysts is urgently required. Herein, Co─N 5 site with an asymmetric electronic configuration constructed to boost two‐electron oxygen reduction reaction (2e − ORR) compared symmetric 4 , effectively overcoming trade‐off between activity selectivity in production. Both experimental theoretical analyses demonstrate that breaking symmetry sites promotes activation molecules moderates adsorption key *OOH intermediate by disrupting linear scaling relationship for intermediates adsorption. This modulation enables efficient H₂O₂ its effective retention subsequent applications. As a proof concept, achieves rate as high 16.1 mol g cat −1 h flow cell, outperforming most recently reported counterparts. Furthermore, coupling 2e ORR oxidation cellulose‐derived carbohydrates accomplishes formic acid yields (84.1% from glucose 62.0%–92.1% other substrates), underpinning sustainable electro‐refinery biomass valorization at ambient conditions. By elucidating intrinsic 2e⁻ asymmetry sites, this work paves way high‐performance electrosynthesis.

Language: Английский

Citations

1
Balancing Electronic Spin State via Atomically-Dispersed Heteronuclear Fe–Co Pairs for High-Performance Sodium–Sulfur Batteries DOI
Canhuang Li, Jing Yu, Dawei Yang

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 27, 2025

Room-temperature sodium–sulfur (Na–S) batteries are emerging as a promising next-generation energy storage technology, offering high densities at low cost and utilizing abundant elements. However, their practical application is hindered by the shuttle effect of sodium-polysulfides sluggish kinetics sulfur redox reactions. In this study, we demonstrate heteronuclear diatomic catalyst featuring Fe Co bimetallic sites embedded in nitrogen-doped hollow carbon nanospheres (Fe–Co/NC) an effective host cathode Na–S batteries. Aberration-corrected high-angle annular dark field scanning transmission electron microscopy demonstrates presence isolated Fe–Co atomic pairs, while synchrotron radiation X-ray absorption fine structure analysis confirms (Fe–Co–N6) coordination structure. Density functional theory calculations show that introduction atoms induces delocalization Co(II), shifting electronic configuration from low-spin to higher-spin state. This shift enhances hybridization dz2 orbitals with antibonding π within sodium sulfide species accelerates catalytic conversion. As result, Fe–Co/NC-based cathodes exhibit excellent cycling stability (378 mAh g–1 after 2000 cycles) impressive rate performance (341.1 under 5 A g–1).

Language: Английский

Citations

1