A high-entropy atomic environment converts inactive to active sites for electrocatalysis

Energy & Environmental Science, Год журнала: 2023, Номер 16(2), С. 619 - 628

Опубликована: Янв. 1, 2023

An electronegativity-dominant high-entropy atomic environment regulation strategy was developed to manipulate the electrocatalytic properties by tailoring competitive adsorption sites in HEA NPs.

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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Multi-atom cluster catalysts for efficient electrocatalysis

Chemical Society Reviews, Год журнала: 2022, Номер 51(21), С. 8923 - 8956

Опубликована: Янв. 1, 2022

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

Язык: Английский

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Atomically Dispersed Ni–Cu Catalysts for pH‐Universal CO₂ Electroreduction

Advanced Materials, Год журнала: 2023, Номер 35(13)

Опубликована: Янв. 10, 2023

CO2 electroreduction is of great significance to reduce emissions and complete the carbon cycle. However, unavoidable carbonate formation low utilization efficiency in neutral or alkaline electrolytes hinder its application at commercial scale. The development reduction under acidic conditions provides a promising strategy, but inhibition hydrogen evolution reaction difficult. Herein, first work design Ni-Cu dual atom catalyst supported on hollow nitrogen-doped reported for pH-universal CO. shows high CO Faradaic ≈99% acidic, neutral, electrolytes, partial current densities reach 190 ± 11, 225 10, 489 14 mA cm-2 , respectively. In particular, reaches 64.3%, which twice as that conditions. Detailed study indicates existence electronic interaction between Ni Cu atoms. atoms push d-band center further toward Fermi level, thereby accelerating *COOH. addition, operando characterizations density functional theory calculation are used elucidate possible mechanism electrolytes.

Язык: Английский

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Structural optimization of carbon-based diatomic catalysts towards advanced electrocatalysis

Coordination Chemistry Reviews, Год журнала: 2023, Номер 492, С. 215288 - 215288

Опубликована: Июнь 12, 2023

Язык: Английский

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N‐Coordinated Cu–Ni Dual‐Single‐Atom Catalyst for Highly Selective Electrocatalytic Reduction of Nitrate to Ammonia

Small, Год журнала: 2023, Номер 19(20)

Опубликована: Фев. 15, 2023

As a traditional method of ammonia (NH3 ) synthesis, Haber-Bosch expends vast amount energy. An alternative route for NH3 synthesis is proposed from nitrate (NO3- via electrocatalysis. However, the structure-activity relationship remains challenging and requires in-depth research both experimentally theoretically. Here an N-coordinated Cu-Ni dual-single-atom catalyst anchored in N-doped carbon (Cu/Ni-NC) reported, which has competitive activity with maximal Faradaic efficiency 97.28%. Detailed characterizations demonstrate that high Cu/Ni-NC mainly comes contribution dual active sites. That is, (1) electron transfer (Ni → Cu) reveals strong interaction dual-single-atom; (2) hybridizations Cu 3d-and Ni 3d-O 2p orbitals NO3- can accelerate dual-site to ; (3) effectively decrease rate-limiting step barriers, suppress N-N coupling N2 O formation hydrogen production.

Язык: Английский

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Dinuclear metal synergistic catalysis for energy conversion

Chemical Society Reviews, Год журнала: 2023, Номер 52(9), С. 3170 - 3214

Опубликована: Янв. 1, 2023

An exclusive review focusing on catalysts exhibiting the dinuclear metal synergistic catalysis (DMSC) effect for energy conversion reactions is presented.

Язык: Английский

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Confined interface engineering of self-supported Cu@N-doped graphene for electrocatalytic CO2 reduction with enhanced selectivity towards ethanol

Nano Research, Год журнала: 2022, Номер 15(10), С. 8872 - 8879

Опубликована: Июль 27, 2022

Язык: Английский

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In Situ Construction of Metal–Organic Frameworks as Smart Channels for the Effective Electrocatalytic Reduction of Nitrate at Ultralow Concentrations to Ammonia

ACS Catalysis, Год журнала: 2023, Номер 13(13), С. 9125 - 9135

Опубликована: Июнь 26, 2023

Electrochemical conversion of nitrate, a widespread water pollutant, into high-value-added ammonia is renewable and delocalized route to restore the globally perturbed nitrogen cycle. However, premature desorption catalytic intermediates competitive reaction hydrogen evolution make current performance still far from suitable for practical applications. In this work, Zr-based metal–organic framework (MOF) in situ constructed at interface serve as smart channel highly selective electrocatalytic reduction nitrate ammonia. The secondary coordination interaction introduced by pendant Brønsted acidic groups MOF not only effectively stabilize facilitate overall process but also certainly increase proton activation barrier suppress competing reaction. When coupled with nanocluster active center, proof-of-concept system achieves simultaneous improvement three critical parameters, rate 97.6%, an selectivity 95.2%, Faradaic efficiency 91.4% −1.0 V (vs RHE) under ultralow concentration conditions. This strategy provides interesting application MOFs paves way removal its

Язык: Английский

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Confinement Engineering of Electrocatalyst Surfaces and Interfaces

Advanced Functional Materials, Год журнала: 2022, Номер 32(46)

Опубликована: Сен. 9, 2022

Abstract The electrocatalytic performance of nanomaterials can be enhanced by fine‐tuning the coordination environment and number low‐coordination atoms. Confinement engineering is most effective strategy for precise chemical synthesis electrocatalysts through modulation electron transfer properties, atomic arrangement, molecular structure in a confined region. It not only alters environments to adjust formation mechanism active centers, but also regulates physicochemical properties electrocatalysts. Consequently, nucleation, transportation, stabilization intermediate species electrocatalysis are optimized, then improve covering activity, stability, selectivity. In this review, confinement introduced terms definition, classification, construction, basic principles. Then, latest advances oxygen reduction reaction, hydrogen evolution nitrogen carbon dioxide reaction systematically evaluated. Furthermore, using representative experimental results theoretical calculations, structure‐activity relationships between illustrated. Finally, potential challenges future development prospects highlighted, with focus on controlling construction environments, investigating uncommon catalytic regions, practical applications.

Язык: Английский

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