Understanding the structure-performance relationship of active sites at atomic scale

Nano Research, Год журнала: 2022, Номер 15(8), С. 6888 - 6923

Опубликована: Июнь 14, 2022

Язык: Английский

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Identifying and tailoring C–N coupling site for efficient urea synthesis over diatomic Fe–Ni catalyst

Nature Communications, Год журнала: 2022, Номер 13(1)

Опубликована: Сен. 10, 2022

Electrocatalytic urea synthesis emerged as the promising alternative of Haber-Bosch process and industrial synthetic protocol. Here, we report that a diatomic catalyst with bonded Fe-Ni pairs can significantly improve efficiency electrochemical synthesis. Compared isolated single-atom catalysts, act efficient sites for coordinated adsorption activation multiple reactants, enhancing crucial C-N coupling thermodynamically kinetically. The performance up to an order magnitude higher than those electrocatalysts, high yield rate 20.2 mmol h-1 g-1 corresponding Faradaic 17.8% has been successfully achieved. A total about 100% formation value-added urea, CO, NH3 was realized. This work presents insight into synergistic catalysis towards sustainable via identifying tailoring atomic site configurations.

Язык: Английский

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Emerging low-nuclearity supported metal catalysts with atomic level precision for efficient heterogeneous catalysis

Nano Research, Год журнала: 2022, Номер 15(9), С. 7806 - 7839

Опубликована: Июнь 2, 2022

Язык: Английский

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Metal-metal interactions in correlated single-atom catalysts

Science Advances, Год журнала: 2022, Номер 8(17)

Опубликована: Апрель 29, 2022

Single-atom catalysts (SACs) include a promising family of electrocatalysts with unique geometric structures. Beyond conventional ones fully isolated metal sites, an emerging class the adjacent single atoms exhibiting intersite metal-metal interactions appear in recent years and can be denoted as correlated SACs (C-SACs). This type provides more opportunities to achieve substantial structural modification performance enhancement toward wider range electrocatalytic applications. On basis clear identification interactions, this review critically examines research progress C-SACs. It shows that control enables regulation atomic structure, local coordination, electronic properties atoms, which facilitate modulation behavior Last, we outline directions for future work design development C-SACs, is indispensable creating high-performing new SAC architectures.

Язык: Английский

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Atomically dispersed materials: Ideal catalysts in atomic era

Nano Research, Год журнала: 2023, Номер 17(1), С. 18 - 38

Опубликована: Май 25, 2023

Язык: Английский

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Microenvironment Engineering of Single/Dual‐Atom Catalysts for Electrocatalytic Application

Advanced Materials, Год журнала: 2023, Номер 35(31)

Опубликована: Фев. 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.

Язык: Английский

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Bioinspired Framework Catalysts: From Enzyme Immobilization to Biomimetic Catalysis

Chemical Reviews, Год журнала: 2023, Номер 123(9), С. 5347 - 5420

Опубликована: Апрель 12, 2023

Enzymatic catalysis has fueled considerable interest from chemists due to its high efficiency and selectivity. However, the structural complexity vulnerability hamper application potentials of enzymes. Driven by practical demand for chemical conversion, there is a long-sought quest bioinspired catalysts reproducing even surpassing functions natural As nanoporous materials with surface areas crystallinity, metal-organic frameworks (MOFs) represent an exquisite case how enzymes their active sites are integrated into porous solids, affording heterogeneous superior stability customizable structures. In this review, we comprehensively summarize advances MOFs catalysis, discuss design principle various MOF-based catalysts, such as MOF-enzyme composites embedded sites, explore utility these in different reactions. The advantages enzyme mimetics also highlighted, including confinement, templating effects, functionality, comparison homogeneous supramolecular catalysts. A perspective provided potential solutions addressing current challenges MOF catalysis.

Язык: Английский

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Proximity Electronic Effect of Ni/Co Diatomic Sites for Synergistic Promotion of Electrocatalytic Oxygen Reduction and Hydrogen Evolution

Advanced Functional Materials, Год журнала: 2022, Номер 33(4)

Опубликована: Ноя. 13, 2022

Abstract The modulation effect manifests an encouraging potential to enhance the performance of single‐atom catalysts; however, in‐depth study about this for isolated diatomic sites (DASs) remains a great challenge. Herein, proximity electronic (PEE) Ni/Co DASs is proposed that anchored in N‐doped carbon (N‐C) substrate (NiCo DASs/N‐C) synergistic promoting electrocatalytic oxygen reduction reaction (ORR) and hydrogen evolution (HER). Benefiting from PEE adjacent Ni by four nitrogen (Ni‐N 4 ) moiety, NiCo DASs/N‐C catalyst exhibits superior ORR HER activity. In situ characterization results suggest Co (Co‐N as main active site O 2 adsorption‐activation process, which promotes formation key *OOH desorption *OH intermediate accelerate multielectron kinetics. Theoretical calculation reveals Ni‐N modulator can effectively adjust localization Co‐N site, *H adsorption on thereby boosting process significantly. This opens new opportunity rationally regulating catalytic centers well provides guidance designing high‐efficiency bifunctional electrocatalysts promising applications.

Язык: Английский

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Breaking the symmetry of single-atom catalysts enables an extremely low energy barrier and high stability for large-current-density water splitting

Energy & Environmental Science, Год журнала: 2022, Номер 15(10), С. 4048 - 4057

Опубликована: Янв. 1, 2022

The single-atomic-site doping of oxophilic-metal (Ru) species in FeCo-LDH leads to the active atom reconstruction at symmetry-breaking interfaces and then excellent catalytic performance for OER/HER overall water splitting large current densities.

Язык: Английский

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Design of Co‐Cu Diatomic Site Catalysts for High‐efficiency Synergistic CO₂ Electroreduction at Industrial‐level Current Density

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(47)

Опубликована: Сен. 13, 2022

Single atom catalysts (SACs) have been widely studied in the field of CO2 electroreduction, but industrial-level current density and near-unity product selectivity are still difficult to achieve. Herein, a diatomic site (DASCs) consisting Co-Cu hetero-diatomic pairs is synthesized. The CoCu DASC exhibits excellent with maximum CO Faradaic efficiency 99.1 %. can maintain above 95 % over wide range from 100 mA cm-2 500 . partial reach 483 flow cell, far exceed requirements (>200 ). Theoretical calculation reveals that synergistic catalysis bimetallic sites reduce activation energy promote formation intermediate *COOH. This work shows introduction another metal into SACs significantly affect electronic structure then enhance catalytic activity SACs.

Язык: Английский

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