Metal Alloys‐Structured Electrocatalysts: Metal–Metal Interactions, Coordination Microenvironments, and Structural Property–Reactivity Relationships DOI
Chengdong Yang, Yun Gao, Tian Ma

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(51)

Published: April 24, 2023

Metal alloys-structured electrocatalysts (MAECs) have made essential contributions to accelerating the practical applications of electrocatalytic devices in renewable energy systems. However, due complex atomic structures, varied electronic states, and abundant supports, precisely decoding metal-metal interactions structure-activity relationships MAECs still confronts great challenges, which is critical direct future engineering optimization MAECs. Here, this timely review comprehensively summarizes latest advances creating MAECs, including interactions, coordination microenvironments, relationships. First, fundamental classification, design, characterization, structural reconstruction are outlined. Then, merits modulation strategies recent breakthroughs for noble non-noble metal-structured thoroughly discussed, such as solid solution alloys, intermetallic single-atom alloys. Particularly, unique insights into bond theoretical understanding, operando techniques mechanism disclosure given. Thereafter, current states diverse with a focus on property-reactivity relationships, reaction pathways, performance comparisons discussed. Finally, challenges perspectives systematically It believed that comprehensive can offer substantial impact stimulating widespread utilization metal materials electrocatalysis.

Language: Английский

Ten concerns of Zn metal anode for rechargeable aqueous zinc batteries DOI Creative Commons

Xiaoyu Yu,

Zhengang Li, Xiaohong Wu

et al.

Joule, Journal Year: 2023, Volume and Issue: 7(6), P. 1145 - 1175

Published: June 1, 2023

Language: Английский

Citations

408
Boosting Oxygen Electrocatalytic Activity of Fe–N–C Catalysts by Phosphorus Incorporation DOI Creative Commons
Yazhou Zhou, Ruihu Lu, Xiafang Tao

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(6), P. 3647 - 3655

Published: Feb. 6, 2023

Nitrogen-doped graphitic carbon materials hosting single-atom iron (Fe-N-C) are major non-precious metal catalysts for the oxygen reduction reaction (ORR). The nitrogen-coordinated Fe sites described as first coordination sphere. As opposed to good performance in ORR, that evolution (OER) is extremely poor due sluggish O-O coupling process, thus hampering practical applications of rechargeable zinc (Zn)-air batteries. Herein, we succeed boosting OER activity Fe-N-C by additionally incorporating phosphorus atoms into second sphere, here denoted P/Fe-N-C. resulting material exhibits excellent 0.1 M KOH with an overpotential low 304 mV at a current density 10 mA cm-2. Even more importantly, they exhibit remarkably small ORR/OER potential gap 0.63 V. Theoretical calculations using first-principles functional theory suggest enhances electrocatalytic balancing *OOH/*O adsorption FeN4 sites. When used air cathode Zn-air battery, P/Fe-N-C delivers charge-discharge high peak power 269 mW cm-2, highlighting its role state-of-the-art bifunctional electrocatalyst.

Language: Английский

Citations

282
Long‐Range Interactions in Diatomic Catalysts Boosting Electrocatalysis DOI
Wenhao Li, Jiarui Yang, Dingsheng Wang

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(52)

Published: Oct. 6, 2022

Abstract The simultaneous presence of two active metal centres in diatomic catalysts (DACs) leads to the occurrence specific interactions between sites. Such interactions, referred as long‐range (LRIs), play an important role determining rate and selectivity a reaction. optimal combination must be determined achieve targeted efficiency. To date, various types DACs have been synthesised applied electrochemistry. However, LRIs not systematically summarised. Herein, regulation, mechanism, electrocatalytic applications are comprehensively summarised discussed. In addition basic information above, challenges, opportunities, future development proposed order present overall view reference for research.

Language: Английский

Citations

213
High-Density Cobalt Single-Atom Catalysts for Enhanced Oxygen Evolution Reaction DOI
Pawan Kumar, Kannimuthu Karthick, Ali Shayesteh Zeraati

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(14), P. 8052 - 8063

Published: March 30, 2023

Single atom catalysts (SACs) possess unique catalytic properties due to low-coordination and unsaturated active sites. However, the demonstrated performance of SACs is limited by low SAC loading, poor metal-support interactions, nonstable performance. Herein, we report a macromolecule-assisted synthesis approach that enabled us demonstrate high-density Co single atoms (10.6 wt % SAC) in pyridinic N-rich graphenic network. The highly porous carbon network (surface area ∼186 m2 g-1) with increased conjugation vicinal site decoration significantly enhanced electrocatalytic oxygen evolution reaction (OER) 1 M KOH (η10 at 351 mV; mass activity 2209 mA mgCo-1 1.65 V) more than 300 h stability. Operando X-ray absorption near-edge structure demonstrates formation electron-deficient Co-O coordination intermediates, accelerating OER kinetics. Density functional theory (DFT) calculations reveal facile electron transfer from cobalt species-accelerated OER.

Language: Английский

Citations

197
Tuning the spin state of Fe single atoms by Pd nanoclusters enables robust oxygen reduction with dissociative pathway DOI Creative Commons
Xiaoqian Wei, Shaojia Song, Weiwei Cai

et al.

Chem, Journal Year: 2022, Volume and Issue: 9(1), P. 181 - 197

Published: Oct. 27, 2022

Language: Английский

Citations

195
Microenvironment Engineering of Single/Dual‐Atom Catalysts for Electrocatalytic Application DOI Open Access
Yun Gao, Baozhong Liu, Dingsheng Wang

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(31)

Published: Feb. 23, 2023

Single/dual-metal atoms supported on carbon matrix can be modulated by coordination structure and neighboring active sites. Precisely designing the geometric electronic uncovering structure-property relationships of single/dual-metal confront with grand challenges. Herein, this review summarizes latest progress in microenvironment engineering single/dual-atom sites via a comprehensive comparison single-atom catalyst (SACs) dual-atom catalysts (DACs) term design principles, modulation strategy, theoretical understanding structure-performance correlations. Subsequently, recent advances several typical electrocatalysis process are discussed to get general reaction mechanisms finely-tuned SACs DACs. Finally, full-scaled summaries challenges prospects given for This will provide new inspiration development atomically dispersed electrocatalytic application.

Language: Английский

Citations

181
Geminal-atom catalysis for cross-coupling DOI
Xiao Hai, Yang Zheng, Qi Yu

et al.

Nature, Journal Year: 2023, Volume and Issue: 622(7984), P. 754 - 760

Published: Sept. 20, 2023

Language: Английский

Citations

149
Multi-atom cluster catalysts for efficient electrocatalysis DOI Creative Commons
Libo Sun, Vikas Reddu, Xin Wang

et al.

Chemical Society Reviews, Journal Year: 2022, Volume and Issue: 51(21), P. 8923 - 8956

Published: Jan. 1, 2022

This review presents recent developments in the synthesis, modulation and characterization of multi-atom cluster catalysts for electrochemical energy applications.

Language: Английский

Citations

138
Challenges and Opportunities in Engineering the Electronic Structure of Single-Atom Catalysts DOI Creative Commons
Vera Giulimondi, Sharon Mitchell, Javier Pérez‐Ramírez

et al.

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(5), P. 2981 - 2997

Published: Feb. 14, 2023

Controlling the electronic structure of transition-metal single-atom heterogeneous catalysts (SACs) is crucial to unlocking their full potential. The ability do this with increasing precision offers a rational strategy optimize processes associated adsorption and activation reactive intermediates, charge transfer dynamics, light absorption. While several methods have been proposed alter characteristics SACs, such as oxidation state, band structure, orbital occupancy, spin, lack systematic approach application makes it difficult control effects. In Perspective, we examine how configuration SACs can be engineered for thermochemical, electrochemical, photochemical applications, exploring relationship activity, selectivity, stability. We discuss synthetic analytical challenges in controlling discriminating possible directions toward closing gap between computational experimental efforts. By bringing topic center, hope stimulate research understand, control, exploit effects ultimately spur technological developments.

Language: Английский

Citations

130
Inter‐Metal Interaction with a Threshold Effect in NiCu Dual‐Atom Catalysts for CO2 Electroreduction DOI Creative Commons
Dazhi Yao, Cheng Tang, Xing Zhi

et al.

Advanced Materials, Journal Year: 2022, Volume and Issue: 35(11)

Published: Nov. 26, 2022

Dual-atom catalysts (DACs) have become an emerging platform to provide more flexible active sites for electrocatalytic reactions with multi-electron/proton transfer, such as the CO2 reduction reaction (CRR). However, introduction of asymmetric dual-atom causes complexity in structure, leaving incomprehensive understanding inter-metal interaction and catalytic mechanism. Taking NiCu DACs example, herein, a rational structural model is proposed, distance-dependent investigated by combining theoretical simulations experiments, including density functional theory computation, aberration-corrected transmission electron microscopy, synchrotron-based X-ray absorption fine Monte Carlo experiments. A distance threshold around 5.3 Å between adjacent NiN4 CuN4 moieties revealed trigger effective electronic regulation boost CRR performance on both selectivity activity. universal macro-descriptor rigorously correlating intrinsic material features (e.g., metal loading thickness) established guide design synthesis advanced DACs. This study highlights significance identifying DACs, helps bridge gap experimental atomically dispersed highly correlated sites.

Language: Английский

Citations

124