Construction of C–N bonds from small-molecule precursors through heterogeneous electrocatalysis

Nature Reviews Chemistry, Journal Year: 2022, Volume and Issue: 6(5), P. 303 - 319

Published: April 25, 2022

Language: Английский

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

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

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Water electrolysis for hydrogen production: from hybrid systems to self-powered/catalyzed devices

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 17(1), P. 49 - 113

Published: Nov. 7, 2023

This perspective highlights recent advancements in innovative strategies to provide valuable insights into the potential for energy-saving hydrogen production through water electrolysis.

Language: Английский

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Theoretically Revealed and Experimentally Demonstrated Synergistic Electronic Interaction of CoFe Dual-Metal Sites on N-doped Carbon for Boosting Both Oxygen Reduction and Evolution Reactions

Nano Letters, Journal Year: 2022, Volume and Issue: 22(8), P. 3392 - 3399

Published: April 18, 2022

Heteronuclear double-atom catalysts, unlike single atom may change the charge density of active metal sites by introducing another atom, thereby modifying adsorption energies reaction intermediates and increasing catalytic activities. First, functional theory calculations are used to figure out best combination modeling two transition-metal atoms from Fe, Co, Ni onto N-doped graphene. Generally, Fe Co highly for oxygen reduction (ORR) evolution (OER), respectively. The form CoFe-N-C not only further improves Fe's ORR Co's OER activities but also greatly enhances site's Then, we synthesize a two-step pyrolysis process find that exhibits exceptional electrocatalytic in alkaline media, significantly superior Fe-N-C Co-N-C even commercial catalysts.

Language: Английский

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Multi-atom cluster catalysts for efficient electrocatalysis

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

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Challenges and Opportunities in Engineering the Electronic Structure of Single-Atom Catalysts

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

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Inter‐Metal Interaction with a Threshold Effect in NiCu Dual‐Atom Catalysts for CO₂ Electroreduction

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

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Catalytic Activity Enhancement on Alcohol Dehydrogenation via Directing Reaction Pathways from Single- to Double-Atom Catalysis

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(11), P. 4913 - 4924

Published: March 9, 2022

To further improve the intrinsic reactivity of single-atom catalysts (SACs), controllable modification a single site by coordinating with second neighboring metal atom, developing double-atom (DACs), affords new opportunities. Here we report catalyst that features two bonded Fe-Co double atoms, which is well represented an FeCoN6(OH) ensemble 100% dispersion, work together to switch reaction mechanism in alcohol dehydrogenation under oxidant-free conditions. Compared Fe-SAC and Co-SAC, FeCo-DAC displays higher activity performance, yielding desired products up 98% yields. Moreover, broad diversity benzyl alcohols aliphatic convert into corresponding dehydrogenated excellent yields high selectivity. The kinetic results show lower activation energy obtained than Co-SAC. computational studies demonstrate path DACs different from SACs, providing rationale for observed enhancements.

Language: Английский

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Tailoring of Active Sites from Single to Dual Atom Sites for Highly Efficient Electrocatalysis

ACS Nano, Journal Year: 2022, Volume and Issue: 16(11), P. 17572 - 17592

Published: Nov. 4, 2022

Single atom catalysts (SACs) have been attracting extensive attention in electrocatalysis because of their unusual structure and extreme utilization, but the low metal loading unified single site induced scaling relations may limit activity practical application. Tailoring active sites at atomic level is a sensible approach to break existing limits SACs. In this review, SACs were first discussed regarding carbon or non-carbon supports. Then, five tailoring strategies elaborated toward improving electrocatalytic SACs, namely strain engineering, spin-state tuning axial functionalization ligand porosity so as optimize electronic state sites, tune d orbitals transition metals, adjust adsorption strength intermediates, enhance electron transfer, elevate mass transport efficiency. Afterward, from angle inducing redistribution optimizing nature centers, synergistic effect adjacent atoms recent advances on with binuclear configuration which include simple, homonuclear, heteronuclear dual (DACs) summarized. Finally, summary some perspectives for achieving efficient sustainable presented based strategies, design situ characterization.

Language: Английский

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Atomically Site Synergistic Effects of Dual-Atom Nanozyme Enhances Peroxidase-like Properties

Nano Letters, Journal Year: 2023, Volume and Issue: 23(13), P. 6073 - 6080

Published: June 26, 2023

Pursuing effective and generalized strategies for modulating the electronic structures of atomically dispersed nanozymes with remarkable catalytic performance is exceptionally attractive yet challenging. Herein, we developed a facile "formamide condensation carbonization" strategy to fabricate library single-atom (M1-NC; 6 types) dual-atom (M1/M2-NC; 13 metal-nitrogen-carbon (M = Fe, Co, Ni, Mn, Ru, Cu) reveal peroxidase- (POD-) like activities. The Fe1Co1-NC nanozyme Fe1-N4/Co1-N4 coordination displayed highest POD-like activity. Density functional theory (DFT) calculations revealed that Co atom site synergistically affects d-band center position Fe served as second reaction center, which contributes better Finally, Fe1Co1 NC was shown be in inhibiting tumor growth both vitro vivo, suggesting diatomic synergy an developing artificial novel nanocatalytic therapeutics.

Language: Английский

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