First-Principles Insights into the Selectivity of CO2 Electroreduction over Heterogeneous Single-Atom Catalysts DOI
Tianyang Liu, Yu Jing, Yafei Li

et al.

The Journal of Physical Chemistry Letters, Journal Year: 2024, Volume and Issue: 15(23), P. 6216 - 6221

Published: June 5, 2024

Heterogeneous metal-nitrogen-carbon (M-N-C) single-atom catalysts (SACs) have garnered considerable attention in the two-electron CO

Language: Английский

Structural engineering of atomic catalysts for electrocatalysis DOI Creative Commons

Tianmi Tang,

Xue Bai, Zhenlü Wang

et al.

Chemical Science, Journal Year: 2024, Volume and Issue: 15(14), P. 5082 - 5112

Published: Jan. 1, 2024

This review systematically introduces how to regulate the electronic structure and geometric configuration of atomic catalysts achieve high-efficiency electrocatalysis performances by analyzing detailed electrocatalytic applications mechanisms.

Language: Английский

Citations

62
Electronic Structure Design of Transition Metal-Based Catalysts for Electrochemical Carbon Dioxide Reduction DOI Creative Commons
Liang Guo, Jingwen Zhou, Fu Liu

et al.

ACS Nano, Journal Year: 2024, Volume and Issue: 18(14), P. 9823 - 9851

Published: March 28, 2024

With the increasingly serious greenhouse effect, electrochemical carbon dioxide reduction reaction (CO2RR) has garnered widespread attention as it is capable of leveraging renewable energy to convert CO2 into value-added chemicals and fuels. However, performance CO2RR can hardly meet expectations because diverse intermediates complicated processes, necessitating exploitation highly efficient catalysts. In recent years, with advanced characterization technologies theoretical simulations, exploration catalytic mechanisms gradually deepened electronic structure catalysts their interactions intermediates, which serve a bridge facilitate deeper comprehension structure-performance relationships. Transition metal-based (TMCs), extensively applied in CO2RR, demonstrate substantial potential for further modulation, given abundance d electrons. Herein, we discuss representative feasible strategies modulate catalysts, including doping, vacancy, alloying, heterostructure, strain, phase engineering. These approaches profoundly alter inherent properties TMCs interaction thereby greatly affecting rate pathway CO2RR. It believed that rational design modulation fundamentally provide viable directions development toward conversion many other small molecules.

Language: Английский

Citations

34
Not One, Not Two, But at Least Three: Activity Origin of Copper Single-Atom Catalysts toward CO2/CO Electroreduction to C2+ Products DOI
Juan Zhang, Yu Wang, Yafei Li

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(22), P. 14954 - 14958

Published: May 28, 2024

Copper (Cu) single-atom catalysts (SACs) exhibit great potential for generating multicarbon (C2+) products, but the intrinsic activity of Cu (Cu1) under realistic conditions remains controversial. Herein, we perform extensive calculations with explicit solvation to investigate underlying mechanism SACs, disclosing absence C2+ in Cu1 sites regardless different substrates. The original (first taking stably anchored on carbon nitride as an example) cannot facilitate *CO hydrogenation and CO–CO coupling due lack active nearby, they are unstable operation, causing leaching aggregation form small clusters. derived clusters composed at least three atoms can efficiently promote coupling, revealed by kinetic analyses. We extend modeling other typical SACs reveal that all inactive, while performance Cu-cluster is substrate-dependent. This study offers mechanistic insights into provides practical guidance their rational optimization.

Language: Английский

Citations

32
Strategies for robust electrocatalytic activity of 2D materials: ORR, OER, HER, and CO2RR DOI Creative Commons
Ali Raza, Jahan Zeb Hassan, Usman Qumar

et al.

Materials Today Advances, Journal Year: 2024, Volume and Issue: 22, P. 100488 - 100488

Published: May 8, 2024

Electrocatalysis utilizing 2D materials is an encouraging approach for advancing sustainable energy conversion technologies. This review explores the strategies employed to achieve robust electrocatalytic activity of in key reactions, namely, OER, HER, and CO2RR. The distinct structural electrical characteristics offer opportunities rapid catalytic performance, indicating significant efficiency selectivity. We systematically discuss factors governing two-dimensional materials, including their intrinsic properties, surface modification techniques, heterostructure engineering, role defects. Furthermore, we summarize recent advances experimental theoretical studies understand fundamental mechanisms with respect behavior. For ORR, defect phase interface heteroatom doping techniques have been explored. In addition, case CO2RR, modification, surface-structure tuning, electrolyte electrolyzer optimization were examined. emphasizes prospective as efficient electrocatalysts processes. Moreover, it provides future insights into this rapidly evolving field highlights possible challenges. conclusion, aims serve a remarkable resource researchers seeking harness potential response applications.

Language: Английский

Citations

27
Spin effect in dual-atom catalysts for electrocatalysis DOI Creative Commons

Xiaoqin Xu,

Jingqi Guan

Chemical Science, Journal Year: 2024, Volume and Issue: 15(36), P. 14585 - 14607

Published: Jan. 1, 2024

The development of high-efficiency atomic-level catalysts for energy-conversion and -storage technologies is crucial to address energy shortages. spin states diatomic (DACs) are closely tied their catalytic activity. Adjusting the DACs' active centers can directly modify occupancy d-orbitals, thereby influencing bonding strength between metal sites intermediates as well transfer during electro reactions. Herein, we discuss various techniques characterizing atomic strategies modulating center states. Next, outline recent progress in study effects DACs oxygen reduction reaction (ORR), evolution (OER), hydrogen (HER), electrocatalytic nitrogen/nitrate (eNRR/NO

Language: Английский

Citations

27
Materials Containing Single‐, Di‐, Tri‐, and Multi‐Metal Atoms Bonded to C, N, S, P, B, and O Species as Advanced Catalysts for Energy, Sensor, and Biomedical Applications DOI Creative Commons
Jitendra N. Tiwari, Krishan Kumar, Moein Safarkhani

et al.

Advanced Science, Journal Year: 2024, Volume and Issue: 11(33)

Published: July 1, 2024

Abstract Modifying the coordination or local environments of single‐, di‐, tri‐, and multi‐metal atom (SMA/DMA/TMA/MMA)‐based materials is one best strategies for increasing catalytic activities, selectivity, long‐term durability these materials. Advanced sheet supported by metal atom‐based have become a critical topic in fields renewable energy conversion systems, storage devices, sensors, biomedicine owing to maximum utilization efficiency, precisely located centers, specific electron configurations, unique reactivity, precise chemical tunability. Several offer excellent support are attractive applications energy, medical research, such as oxygen reduction, production, hydrogen generation, fuel selective detection, enzymatic reactions. The strong metal–metal metal–carbon with metal–heteroatom (i.e., N, S, P, B, O) bonds stabilize optimize electronic structures atoms due interfacial interactions, yielding activities. These provide models understanding fundamental problems multistep This review summarizes substrate structure‐activity relationship different active sites based on experimental theoretical data. Additionally, new synthesis procedures, physicochemical characterizations, biomedical discussed. Finally, remaining challenges developing efficient SMA/DMA/TMA/MMA‐based presented.

Language: Английский

Citations

24
An Overview of Metal Density Effects in Single-Atom Catalysts for Thermal Catalysis DOI
Hongqiang Jin, Weiguo Song, Changyan Cao

et al.

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(22), P. 15126 - 15142

Published: Nov. 8, 2023

With the development of synthetic methodology, recent breakthroughs have been achieved to prepare metal single-atom catalysts (SACs) with high loadings, leading an emerging class SACs called densely populated or high-density SACs. This type provides not only higher mass-specific activity but also additional interaction among single sites, which can further influence local geometric and electronic structures individual centers thus affect intrinsic active sites. Review examines research progress atomic regulation engineering density how it affects catalytic performance in specific thermal catalysis. Last, we outline challenges prospects for future work design

Language: Английский

Citations

23
Catalytic reactivity descriptors of metal‐nitrogen‐doped carbon catalysts for electrocatalysis DOI Creative Commons
Hong Liu, Jiejie Li, Jordi Arbiol

et al.

EcoEnergy, Journal Year: 2023, Volume and Issue: 1(1), P. 154 - 185

Published: Sept. 1, 2023

Abstract Metal‐nitrogen‐doped carbon material have sparked enormous attentions as they show excellent electrocatalytic performance and provide a prototype for mechanistic understandings of reactions. Researchers spare no effort to find catalytic reactivity “descriptor”, which is correlated with catalytical properties could be utilized guiding the rational design high‐performance catalysts. In recent years, benefited from development computational technology, theoretical calculation came into being powerful tool understand mechanisms an atomic level well accelerate process finding descriptor promoting effective present review, we latest research toward energetic electronic descriptors metal‐nitrogen‐doped (M‐N‐C) materials, shown understanding This review uses density functional theory most advanced machine learning method describe exploration four kinds reaction descriptors, namely oxygen reduction reaction, dioxide hydrogen evolution nitrogen reaction. The aim this inspire future high‐efficiency M‐N‐C catalysts by providing in‐depth insights activity these materials.

Language: Английский

Citations

23
Carbon Catalysts Empowering Sustainable Chemical Synthesis via Electrochemical CO2 Conversion and Two‐Electron Oxygen Reduction Reaction DOI Creative Commons
Yuying Zhao, Jithu Raj, Xiang Xu

et al.

Small, Journal Year: 2024, Volume and Issue: unknown

Published: Feb. 2, 2024

Abstract Carbon materials hold significant promise in electrocatalysis, particularly electrochemical CO 2 reduction reaction (eCO RR) and two‐electron oxygen (2e − ORR). The pivotal factor achieving exceptional overall catalytic performance carbon catalysts is the strategic design of specific active sites nanostructures. This work presents a comprehensive overview recent developments electrocatalysts for eCO RR 2e ORR. creation through single/dual heteroatom doping, functional group decoration, topological defect, micro‐nano structuring, along with their synergistic effects, thoroughly examined. Elaboration on mechanisms structure‐activity relationships these provided. In addition to directly serving as electrocatalysts, this review explores role matrix support finely adjusting reactivity single‐atom molecular catalysts. Finally, addresses challenges prospects associated designing fabricating providing valuable insights into future trajectory dynamic field.

Language: Английский

Citations

15
A molecular view of single-atom catalysis toward carbon dioxide conversion DOI Creative Commons
Xin Shang,

Xiaofeng Yang,

Ye Liu

et al.

Chemical Science, Journal Year: 2024, Volume and Issue: 15(13), P. 4631 - 4708

Published: Jan. 1, 2024

We present critical advances in single-atom catalysis toward CO 2 transformation and address crucial issues about SACs from a molecular point of view.

Language: Английский

Citations

14