Metallic W/WO2 solid-acid catalyst boosts hydrogen evolution reaction in alkaline electrolyte DOI Creative Commons
Zhigang Chen, Wenbin Gong, Juan Wang

et al.

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

Published: Sept. 2, 2023

The lack of available protons severely lowers the activity alkaline hydrogen evolution reaction process than that in acids, which can be efficiently accelerated by tuning coverage and chemical environment on catalyst surface. However, cycling active sites proton transfer is largely dependent utilization noble metal catalysts because appealing electronic interaction between atoms protons. Herein, an all-non-noble W/WO2 metallic heterostructure serving as efficient solid-acid exhibits remarkable performance with ultra-low overpotential -35 mV at -10 mA/cm2 a small Tafel slope (-34 mV/dec), well long-term durability production (>50 h) current densities -50 electrolyte. Multiple situ ex spectroscopy characterizations combining first-principle density functional theory calculations discover dynamic proton-concentrated surface constructed under overpotentials, enables catalyzing to follow kinetically fast Volmer-Tafel pathway two neighboring recombining into molecule. Our strategy multiple may provide interesting route for designing advanced catalytic system towards boosting

Language: Английский

Design concept for electrocatalysts DOI
Yao Wang, Xiaobo Zheng, Dingsheng Wang

et al.

Nano Research, Journal Year: 2021, Volume and Issue: 15(3), P. 1730 - 1752

Published: Sept. 4, 2021

Language: Английский

Citations

489
Activity Trends and Mechanisms in Peroxymonosulfate‐Assisted Catalytic Production of Singlet Oxygen over Atomic Metal‐N‐C Catalysts DOI
Yun Gao, Tongwei Wu, Chengdong Yang

et al.

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(41), P. 22513 - 22521

Published: Aug. 13, 2021

Abstract We synthesized a series of carbon‐supported atomic metal‐N‐C catalysts (M‐SACs: M=Mn, Fe, Co, Ni, Cu) with similar structural and physicochemical properties to uncover their catalytic activity trends mechanisms. The peroxymonosulfate (PMS) are Fe‐SAC>Co‐SAC>Mn‐SAC>Ni‐SAC>Cu‐SAC, Fe‐SAC displays the best single‐site kinetic value (1.65×10 5 min −1 mol ) compared other species. First‐principles calculations indicate that most reasonable reaction pathway for 1 O 2 production is PMS→OH*→O*→ ; M‐SACs exhibit moderate near‐average Gibbs free energies in each step have better activity, which key outstanding performance Fe‐SACs. This study gives atomic‐scale understanding fundamental mechanisms PMS‐assisted reactive oxygen species via M‐SACs, thus providing guidance developing organic pollutant degradation.

Language: Английский

Citations

388
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

347
Emerging low-nuclearity supported metal catalysts with atomic level precision for efficient heterogeneous catalysis DOI Open Access
Xiaobo Zheng, Beibei Li, Qishun Wang

et al.

Nano Research, Journal Year: 2022, Volume and Issue: 15(9), P. 7806 - 7839

Published: June 2, 2022

Language: Английский

Citations

266
Anion-exchange membrane water electrolyzers and fuel cells DOI

Yaxiong Yang,

Peng Li, Xiaobo Zheng

et al.

Chemical Society Reviews, Journal Year: 2022, Volume and Issue: 51(23), P. 9620 - 9693

Published: Jan. 1, 2022

The key components, working management, and operating techniques of anion-exchange membrane water electrolyzers fuel cells are reviewed for the first time.

Language: Английский

Citations

262
Recent advances in proton exchange membrane water electrolysis DOI
Ruiting Liu, Zheng‐Long Xu, Fumin Li

et al.

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(16), P. 5652 - 5683

Published: Jan. 1, 2023

This review scrutinizes recent progress in PEMWE system including mechanisms, the correlation among structure-composition–performance, manufacturing, design and operation protocols. The challenges perspectives for applications are proposed.

Language: Английский

Citations

260
Ru–Co Pair Sites Catalyst Boosts the Energetics for the Oxygen Evolution Reaction DOI
Xiaobo Zheng, Jiarui Yang,

Zhongfei Xu

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(32)

Published: May 31, 2022

Abstract Manipulating the coordination environment of active center via anion modulation to reveal tailored activity and selectivity has been widely achieved, especially for carbon‐based single‐atom site catalysts (SACs). However, tuning ligand fields by single‐site metal cation regulation identifying effects on resulting electronic configuration is seldom explored. Herein, we propose a Ru strategy engineer properties constructing Ru/LiCoO 2 SAC with atomically dispersed Ru−Co pair sites. Benefitting from strong coupling between Co sites, catalyst possesses an enhanced electrical conductivity achieves near‐optimal oxygen adsorption energies. Therefore, optimized delivers superior evolution reaction (OER) low overpotential, high mass 1000 A g oxide −1 at small overpotential 335 mV, excellent long‐term stability. It also exhibits rapid kinetics rate capability outstanding durability in zinc–air battery.

Language: Английский

Citations

251
Promoting Surface Reconstruction of NiFe Layered Double Hydroxide for Enhanced Oxygen Evolution DOI
Hang Lei, Liang Ma,

Qixiang Wan

et al.

Advanced Energy Materials, Journal Year: 2022, Volume and Issue: 12(48)

Published: Oct. 30, 2022

A dynamic surface reconstruction of oxide electrocatalysts in alkaline media is widely observed especially for layered double hydroxide (LDH), but little known about how to promote the toward desired surfaces improved oxygen evolution reaction (OER). Here, NiFe LDH nanosheets successfully induced a higher degree via situ sulfur doping than that by natural electrochemical activation. Theoretical calculations, operando Raman, and various ex characterizations reveal S anion-induced effect can lower energy barrier facilitate phase transformation into highly active S-doped oxyhydroxides. The generated S-NixFeyOOH optimize intermediate adsorption OER kinetics. reconstructed S-oxyhydroxides catalyst presents superior activity long-term durability compared undoped ones. This work provides structure–composition–activity relationship during restructuring pre-catalysts.

Language: Английский

Citations

250
Atomically dispersed materials: Ideal catalysts in atomic era DOI
Tao Gan, Dingsheng Wang

Nano Research, Journal Year: 2023, Volume and Issue: 17(1), P. 18 - 38

Published: May 25, 2023

Language: Английский

Citations

214
Single-Atom Engineering to Ignite 2D Transition Metal Dichalcogenide Based Catalysis: Fundamentals, Progress, and Beyond DOI
Xin Wang, Yuwei Zhang, Jing Wu

et al.

Chemical Reviews, Journal Year: 2021, Volume and Issue: 122(1), P. 1273 - 1348

Published: Nov. 17, 2021

Single-atom catalysis has been recognized as a pivotal milestone in the development history of heterogeneous by virtue its superior catalytic performance, ultrahigh atomic utilization, and well-defined structure. Beyond single-atom protrusions, two more motifs substitutions vacancies along with synergistic motif assemblies have progressively developed to enrich family. On other hand, besides traditional carbon material based substrates, wide variety 2D transitional metal dichalcogenides (TMDs) emerging promising platform for owing their diverse elemental compositions, variable crystal structures, flexible electronic intrinsic activities toward many reactions. Such substantial expansion both substrates provides an enriched toolbox further optimize geometric structures pushing performance limit. Concomitantly, higher requirements put forward synthetic characterization techniques related technical bottlenecks being continuously conquered. Furthermore, this burgeoning catalyst (SAC) system triggered serial scientific issues about changeable single atom-2D substrate interaction, ambiguous effects various assemblies, well dynamic structure-performance correlations, all which necessitate clarification comprehensive summary. In context, Review aims summarize critically discuss engineering whole field TMD covering evolution history, methodologies, techniques, applications, correlations. situ are highlighted regarding critical roles real-time detection SAC reconstruction reaction pathway evolution, thus shedding light on lifetime correlations lay solid theoretical foundation field, especially SACs.

Language: Английский

Citations

182