Host-Guest-Induced Electronic State Triggers Two-Electron Oxygen Reduction Electrocatalysis DOI Creative Commons
Xiaojing Long,

Hongni Chen,

Chao Wang

et al.

Research Square (Research Square), Journal Year: 2024, Volume and Issue: unknown

Published: May 21, 2024

Abstract Supramolecular polymers hold promising application prospects in catalysis due to their distinctive molecular recognition and dynamic crosslinking features. However, investigating supramolecular organic electrocatalysts with high efficiency oxygen reduction reaction (ORR) hydrogen peroxide (ORHP) remains an unexplored frontier. Herein, we present for ORHP by introducing cyclodextrin-containing noncovalent building blocks, the skeleton electronic environment is further regulated via a host-guest chemistry strategy, affording HG-CD-Ph HG-CD-TPB abundant bonds. The intermediate desorption states are well-modulated through decoration, resulting appropriate regional electron binding force controllable chemical activity. Notably, introduction of units into polymer model P-CN-Ph achieves ultra-high production rate 9.14 mol g−1 cat h−1, demonstrates excellent Faraday 98.01%, surpassing most reported metal-free electrocatalysts. Supported theory calculation in situ FT-IR experiment, it revealed that C atoms (site–1) adjacent –C=N (N) group potential active sites. Moreover, bonds catalysts can effectively regulate ability its intermediates, leading reactivity selectivity 2e− ORR. This work pioneers strategy provides inspiring ideas process.

Language: Английский

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
Host-guest-induced electronic state triggers two-electron oxygen reduction electrocatalysis DOI Creative Commons

Hongni Chen,

Chao Wang,

Han Wu

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Oct. 25, 2024

Supramolecular polymers possess great potential in catalysis owing to their distinctive molecular recognition and dynamic crosslinking features. However, investigating supramolecular electrocatalysts with high efficiency oxygen reduction reaction hydrogen peroxide (ORHP) remains an unexplored frontier. Herein, we present organic for ORHP by introducing cyclodextrin-containing noncovalent building blocks, affording these supramolecules abundant bonds. The electronic states kinetics are further well-modulated via a host-guest strategy, resulting appropriate regional electron binding force controllable chemical activity. Notably, integrating units into phenyl group-containing model covalent polymer achieves production rate of 9.14 mol g

Language: Английский

Citations

17
Water Spillover to Expedite Two‐Electron Oxygen Reduction DOI Open Access

Qianyi Li,

Zhihao Nie,

Wenqiang Wu

et al.

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

Published: Jan. 5, 2025

Abstract Limited by the activity‐selectivity trade‐off relationship, electrochemical activation of small molecules (like O 2 , N 2, and CO ) rapidly diminishes Faradaic efficiencies with elevated current densities (particularly at ampere levels). Nevertheless, some catalysts can circumvent this restriction in a two‐electron oxygen reduction reaction (2e − ORR), sustainable pathway for activating to hydrogen peroxide (H ). Here we report 2e ORR expedited fluorine‐bridged copper metal–organic framework catalyst, arising from water spillover effect. Through operando spectroscopies, kinetic theoretical characterizations, it demonstrates that under neutral conditions, plays dual role accelerating dissociation stabilizing key * OOH intermediate. Benefiting spillover, catalyst expedite density range 0.1–2.0 A cm −2 both high (99–84.9%) H yield rates (63.17–1082.26 mg h −1 Further, feasibility present system has been demonstrated scaling up unit module cell 25 combination techno‐economics simulations showing production cost strongly dependent on densities, giving lowest price $0.50 kg 2.0 . This work is expected provide an additional dimension leverage systems independent oftraditional rules.

Language: Английский

Citations

2
Recent strategies to improve the electroactivity of metal–organic frameworks for advanced electrocatalysis DOI Creative Commons

Runzhi Wei,

Xiao Li, Aziz B. Ibragimov

et al.

Deleted Journal, Journal Year: 2024, Volume and Issue: 1(2), P. 181 - 206

Published: Aug. 4, 2024

Abstract Metal–organic frameworks (MOFs) have emerged as promising materials in the realm of electrocatalysis due to their high surface area, tunable porosity, and versatile chemical functionality. However, practical application has been hampered by inherent limitations such low electrical conductivity a limited number active metal sites. Researchers addressed these challenges through various strategies, including enhancing incorporating conductive nanoparticles, modifying structure composition MOFs replacing nodes functionalizing linkers, preparing catalysts thermal processes decarburization conversion into oxides, phosphides (MPs), sulfides (MSs). This review provided comprehensive summary strategies that were employed enhance electroactivity for improved electrocatalytic performance recent years. It also explored future directions potential innovations design synthesis MOF‐based electrocatalysts, offering valuable insights advancing sustainable energy technologies.

Language: Английский

Citations

11
Stability challenges of transition metal-modified cathodes for electro-Fenton process: A mini-review DOI
Chao Wang,

Tao Li,

Qianyin Deng

et al.

Chemosphere, Journal Year: 2025, Volume and Issue: 373, P. 144159 - 144159

Published: Jan. 30, 2025

Language: Английский

Citations

1
Carbon powder from sugarcane bagasse: controlled synthesis for on-demand H2O2 electrogeneration DOI
Daniel Couto Sperandio, Júlio César Lourenço, Bruno M. Nogueira

et al.

Renewable Energy, Journal Year: 2025, Volume and Issue: unknown, P. 122715 - 122715

Published: Feb. 1, 2025

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
Metal Atom–Support Interaction in Single Atom Catalysts toward Hydrogen Peroxide Electrosynthesis DOI
Hao Zhang, Haitao Xu, Canglang Yao

et al.

ACS Nano, Journal Year: 2024, Volume and Issue: 18(33), P. 21836 - 21854

Published: Aug. 7, 2024

Single metal atom catalysts (SACs) have garnered considerable attention as promising agents for catalyzing important industrial reactions, particularly the electrochemical synthesis of hydrogen peroxide (H

Language: Английский

Citations

7
Periodic Single‐Metal Site Catalysts: Creating Homogeneous and Ordered Atomic‐Precision Structures DOI
Tianyu Zhang, Dingsheng Wang, Junfeng Liu

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(41)

Published: Aug. 16, 2024

Abstract Heterogeneous single‐metal‐site catalysts (SMSCs), often referred to as single‐atom (SACs), demonstrate promising catalytic activity, selectivity, and stability across a wide spectrum of reactions due their rationally designed microenvironments encompassing coordination geometry, binding ligands, electronic configurations. However, the inherent disorderliness SMSCs at both atomic scale nanoscale poses challenges in deciphering working principles establishing correlations between performances SMSCs. The rearrangement randomly dispersed single metals into homogeneous atomic‐precisely structured periodic single‐metal site (PSMSCs) not only simplifies chaos systems but also unveils new opportunities for manipulating performance gaining profound insights reaction mechanisms. Moreover, synergistic effects adjacent integration arrangement further broaden industrial application scope This perspective offers comprehensive overview recent advancements outlines prospective avenues research design characterizations PSMSCs, while acknowledging formidable encountered prospects that lie ahead.

Language: Английский

Citations

6
Review of H2O2 generation from O2 electroreduction by gas diffusion electrodes: From homogeneous to heterogeneous electrocatalysis DOI
Xuewei Zhang, Xiaoxiao Meng, Yuwei Zhao

et al.

Journal of Electroanalytical Chemistry, Journal Year: 2024, Volume and Issue: 974, P. 118700 - 118700

Published: Oct. 5, 2024

Language: Английский

Citations

5