Contact‐electro‐catalysis for Direct Synthesis of H2O2 under Ambient Conditions DOI
J. W. Zhao, Xiaotong Zhang, Jiajia Xu

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(21)

Published: March 23, 2023

Hydrogen peroxide (H2 O2 ) is an indispensable basic reagent in various industries, such as textile bleach, chemical synthesis, and environmental protection. However, it challenging to prepare H2 a green, safe, simple efficient way under ambient conditions. Here, we found that could be synthesized using catalytic pathway only by contact charging two-phase interface at room temperature normal pressure. Particularly, the action of mechanical force, electron transfer occurs during physical between polytetrafluoroethylene particles deionized water/O2 interfaces, inducing generation reactive free radicals (⋅OH ⋅O2- ), react form , yielding high 313 μmol L-1 h-1 . In addition, new reaction device show long-term stable production. This work provides novel method for preparation which may also stimulate further explorations on contact-electrification-induced chemistry process.

Language: Английский

Electrocatalytic Refinery for Sustainable Production of Fuels and Chemicals DOI Creative Commons
Cheng Tang, Yao Zheng, Mietek Jaroniec

et al.

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(36), P. 19572 - 19590

Published: Feb. 19, 2021

Abstract Compared to modern fossil‐fuel‐based refineries, the emerging electrocatalytic refinery (e‐refinery) is a more sustainable and environmentally benign strategy convert renewable feedstocks energy sources into transportable fuels value‐added chemicals. A crucial step in conducting e‐refinery processes development of appropriate reactions optimal electrocatalysts for efficient cleavage formation chemical bonds. However, compared well‐studied primary (e.g., O 2 reduction, water splitting), mechanistic aspects materials design complex are yet be settled. To address this challenge, herein, we first present fundamentals heterogeneous electrocatalysis some reactions, then implement these establish framework by coupling situ generated intermediates (integrated reactions) or products (tandem reactions). We also set principles strategies efficiently manipulate reaction pathways.

Language: Английский

Citations

514

Carbon‐Based Electrocatalysts for Efficient Hydrogen Peroxide Production DOI
Yunfei Bu, Yaobin Wang, Gao‐Feng Han

et al.

Advanced Materials, Journal Year: 2021, Volume and Issue: 33(49)

Published: Sept. 24, 2021

Abstract Hydrogen peroxide (H 2 O ) is an environment‐friendly and efficient oxidant with a wide range of applications in different industries. Recently, the production hydrogen through direct electrosynthesis has attracted widespread research attention, emerged as most promising method to replace traditional energy‐intensive multi‐step anthraquinone process. In ongoing efforts achieve highly large‐scale H , carbon‐based materials have been developed 2e − oxygen reduction reaction catalysts, benefits low cost, abundant availability, optimal performance. This review comprehensively introduces strategies for optimizing toward production, latest advances hybrid catalysts. The active sites influence coordination heteroatom doping on selectivity are extensively analyzed. particular, appropriate design functional groups understanding effect electrolyte pH expected further improve selective efficiency producing via reaction. Methods improving catalytic activity by interface engineering kinetics summarized. Finally, challenges catalysts face before they can be employed commercial‐scale identified, prospects designing novel electrochemical reactors proposed.

Language: Английский

Citations

256

Electrocatalytic Oxygen Reduction to Hydrogen Peroxide: From Homogeneous to Heterogeneous Electrocatalysis DOI
Yulin Wang, Geoffrey I. N. Waterhouse, Lu Shang

et al.

Advanced Energy Materials, Journal Year: 2020, Volume and Issue: 11(15)

Published: Dec. 18, 2020

Abstract Hydrogen peroxide (H 2 O ) is an environmentally friendly oxidant, finding widespread use across the chemical industry, in sanitation and environmental remediation. Currently, H manufactured via anthraquinone process which has a number of disadvantages including nondistributed production, high‐energy consumption, substantial organic by‐product waste, need to transport obtained point‐of‐use. Accordingly, electrochemical synthesis now attracting lot interest as alternative, cost‐effective, small‐scale, distributed technology for manufacture. This review summarizes recent advancements development Homogeneous Heterogeneous catalysts electrocatalytic reduction reaction (ORR) . The basic principles ORR, methodologies investigating ORR are first introduced. Next, production over discussed, with focus on mechanisms factors that influence activity, selectivity, kinetics. Subsequently, breakthroughs catalysts, nonnoble metal‐based nanomaterials, carbon materials, single‐atom described. latter given special attention, since they serve bridge between catalysis catalysis, while also offering excellent performance. Finally, challenges opportunities critically discussed.

Language: Английский

Citations

251

Electrochemical and Photoelectrochemical Water Oxidation for Hydrogen Peroxide Production DOI
Yudong Xue, Yunting Wang, Zhenhua Pan

et al.

Angewandte Chemie International Edition, Journal Year: 2020, Volume and Issue: 60(19), P. 10469 - 10480

Published: Sept. 16, 2020

Abstract Hydrogen peroxide (H 2 O ), as a green fuel and oxidant, has drawn increasing attention in the energy environmental research. Compared with traditional anthraquinone process, electrochemical (EC) photoelectrochemical (PEC) syntheses of H are cost‐effective environmentally friendly. In order to construct membraneless EC/PEC devices for full synthesis, anodic production by water oxidation, which is less developed than cathodic generation, highly desirable. Here, we review recent developments including fundamental aspects, benchmarking activity evaluation, material/catalyst selection, strategies selectivity, efficiency, accumulation. Furthermore, discuss challenges outlook oxidation production, especially device‐level development, accumulation stability, industrial applications. Our intended stimulate studies further improving production.

Language: Английский

Citations

245

Engineering the Local Atomic Environments of Indium Single‐Atom Catalysts for Efficient Electrochemical Production of Hydrogen Peroxide DOI
Erhuan Zhang,

Lei Tao,

Jingkun An

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(12)

Published: Jan. 19, 2022

The in-depth understanding of local atomic environment-property relationships p-block metal single-atom catalysts toward the 2 e- oxygen reduction reaction (ORR) has rarely been reported. Here, guided by first-principles calculations, we develop a heteroatom-modified In-based metal-organic framework-assisted approach to accurately synthesize an optimal catalyst, in which single In atoms are anchored combined N,S-dual first coordination and B second supported hollow carbon rods (In SAs/NSBC). SAs/NSBC catalyst exhibits high H2 O2 selectivity above 95 % wide range pH. Furthermore, SAs/NSBC-modified natural air diffusion electrode unprecedented production rate 6.49 mol peroxide gcatalyst-1 h-1 0.1 M KOH electrolyte 6.71 PBS electrolyte. This strategy enables design next-generation high-performance materials, provides practical guidance for electrosynthesis.

Language: Английский

Citations

218

Selective hydrogen peroxide conversion tailored by surface, interface, and device engineering DOI Creative Commons
Junying Tang, Tianshuo Zhao, Devan Solanki

et al.

Joule, Journal Year: 2021, Volume and Issue: 5(6), P. 1432 - 1461

Published: May 21, 2021

Language: Английский

Citations

173

Designing highly active nanoporous carbon H2O2 production electrocatalysts through active site identification DOI Creative Commons
June Sung Lim, Jae Hyung Kim, Jinwoo Woo

et al.

Chem, Journal Year: 2021, Volume and Issue: 7(11), P. 3114 - 3130

Published: Aug. 30, 2021

Language: Английский

Citations

173

Metal single-site catalyst design for electrocatalytic production of hydrogen peroxide at industrial-relevant currents DOI Creative Commons
Peike Cao, Xie Quan, Xiaowa Nie

et al.

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

Published: Jan. 12, 2023

Direct hydrogen peroxide (H2O2) electrosynthesis via the two-electron oxygen reduction reaction is a sustainable alternative to traditional energy-intensive anthraquinone technology. However, high-performance and scalable electrocatalysts with industrial-relevant production rates remain be challenging, partially due insufficient atomic level understanding in catalyst design. Here we utilize theoretical approaches identify transition-metal single-site catalysts for using *OOH binding energy as descriptor. The predictions are then used guidance synthesize desired cobalt O-modified Co-(pyrrolic N)4 configuration that can achieve current densities up 300 mA cm-2 96-100% Faradaic efficiencies H2O2 at record rate of 11,527 mmol h-1 gcat-1. Here, show feasibility versatility metal design various commercial carbon phthalocyanine starting materials high applicability acidic, neutral alkaline electrolytes.

Language: Английский

Citations

172

Hydroxyl radicals in anodic oxidation systems: generation, identification and quantification DOI
Jiangzhou Xie, Changyong Zhang, T. David Waite

et al.

Water Research, Journal Year: 2022, Volume and Issue: 217, P. 118425 - 118425

Published: April 8, 2022

Language: Английский

Citations

169

Manipulating the oxygen reduction reaction pathway on Pt-coordinated motifs DOI Creative Commons
Jiajun Zhao, Cehuang Fu, Ke Ye

et al.

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: Feb. 3, 2022

Electrochemical oxygen reduction could proceed via either 4e

Language: Английский

Citations

157