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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Tailoring acidic microenvironments for carbon-efficient CO₂electrolysis over a Ni–N–C catalyst in a membrane electrode assembly electrolyzer

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(4), P. 1502 - 1510

Published: Jan. 1, 2023

By tailoring the microenvironments of a Ni–N–C catalyst in an acidic MEA electrolyzer, we achieve CO faradaic efficiency 95% at 500 mA cm −2 , and 2 loss is reduced by 86% 300 pH 0.5, compared to alkaline electrolysis.

Language: Английский

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Electron‐Rich Bi Nanosheets Promote CO₂⋅⁻ Formation for High‐Performance and pH‐Universal Electrocatalytic CO₂ Reduction

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(11)

Published: Jan. 20, 2023

Electrochemical CO2 reduction reaction (CO2 RR) to chemical fuels such as formate offers a promising pathway carbon-neutral future, but its practical application is largely inhibited by the lack of effective activation molecules and pH-universal feasibility. Here, we report an electronic structure manipulation strategy electron-rich Bi nanosheets, where electrons transfer from Cu donor acceptor in bimetallic Cu-Bi, enabling RR towards with concurrent high activity, selectivity stability (acidic, neutral alkaline) electrolytes. Combined situ Raman spectra computational calculations unravel that promotes ⋅- formation activate molecules, enhance adsorption strength *OCHO intermediate up-shifted p-band center, thus leading superior activity formate. Further integration robust nanosheets into III-V-based photovoltaic solar cell results unassisted artificial leaf solar-to-formate (STF) efficiency 13.7 %.

Language: Английский

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Dopant- and Surfactant-Tuned Electrode–Electrolyte Interface Enabling Efficient Alkynol Semi-Hydrogenation

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(11), P. 6516 - 6525

Published: March 13, 2023

Electrochemical alkynol semi-hydrogenation has emerged as a sustainable and environmentally benign route for the production of high-value alkenols, featuring water hydrogen source instead H2. It is highly challenging to design electrode-electrolyte interface with efficient electrocatalysts their matched electrolytes break selectivity-activity stereotype. Here, boron-doped Pd catalysts (PdB) surfactant-modified are proposed enable simultaneous increase in alkenol selectivity conversion. Typically, compared pure commercial Pd/C catalysts, PdB catalyst achieves both higher turnover frequency (139.8 h-1) specific (above 90%) 2-methyl-3-butyn-2-ol (MBY). Quaternary ammonium cationic surfactants that employed electrolyte additives assembled at electrified response applied bias potential, establishing an interfacial microenvironment can facilitate transfer hinder suitably. Eventually evolution reaction inhibited promoted, without inducing decrease selectivity. This work offers distinct perspective on creating suitable electrosynthesis.

Language: Английский

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Boosting Hydrogen Peroxide Electrosynthesis via Modulating the Interfacial Hydrogen‐Bond Environment

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(27)

Published: May 10, 2023

Abstract Designing highly efficient and stable electrode‐electrolyte interface for hydrogen peroxide (H 2 O ) electrosynthesis remains challenging. Inhibiting the competitive side reaction, 4 e − oxygen reduction to H O, is essential selective electrosynthesis. Instead of hindering excessive hydrogenation via catalyst modification, we discover that adding a hydrogen‐bond acceptor, dimethyl sulfoxide (DMSO), KOH electrolyte enables simultaneous improvement selectivity activity Spectral characterization molecular simulation confirm formation bonds between DMSO water molecules at can reduce dissociation into active H* species. The suitable supply environment hinders reaction (ORR), thus improving ORR achieving over 90 % . This work highlights importance regulating interfacial by organic as means boosting electrochemical performance in aqueous beyond.

Language: Английский

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Reaction Environment Regulation for Electrocatalytic CO₂ Reduction in Acids

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(26)

Published: April 19, 2024

The electrocatalytic CO

Language: Английский

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Electrochemical CO2 reduction catalyzed by organic/inorganic hybrids

eScience, Journal Year: 2023, Volume and Issue: 3(2), P. 100097 - 100097

Published: Jan. 18, 2023

Electroreduction of CO2 into value-added chemicals and fuels utilizing renewable electricity offers a sustainable way to meet the carbon-neutral goal viable solution for storage intermittent green energy sources. At core this technology is development electrocatalysts accelerate redox kinetics reduction reactions (CO2RR) toward high targeted-product yield at minimal input. This perspective focuses on unique category CO2RR embodying both inorganic organic components synergistically promote reaction activity, selectivity stability. First, we summarize recent progress design fabrication organic/inorganic hybrids electrocatalysts, with special attention assembly protocols structural configurations. We then carry out comprehensive discussion mechanistic understanding processes tackled jointly by phases, respect regulation mass charge transport, modification double-layer configuration, tailoring intermediates adsorption, establishment tandem pathways. end, outline future challenges in rational further extend scope device level. hope work could incentivize more research interests construct mobilizing electrocatalytic towards industrialization.

Language: Английский

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Confinement of an alkaline environment for electrocatalytic CO₂ reduction in acidic electrolytes

Chemical Science, Journal Year: 2023, Volume and Issue: 14(21), P. 5602 - 5607

Published: Jan. 1, 2023

Acidic electrochemical CO2 reduction reaction (CO2RR) can minimize carbonate formation and eliminate crossover, thereby improving long-term stability enhancing single-pass carbon efficiency (SPCE). However, the kinetically favored hydrogen evolution (HER) is generally predominant under acidic conditions. This paper describes confinement of a local alkaline environment for efficient CO2RR in strongly electrolyte through manipulation mass transfer processes well-designed hollow-structured Ag@C electrocatalysts. A high faradaic over 95% at current density 300 mA cm-2 an SPCE 46.2% flow rate 2 standard cubic centimeters per minute are achieved electrolyte, with enhanced compared to that Computational modeling results reveal unique structure could regulate diffusion process OH- H+, confining high-pH promoted activity. work presents promising route engineer microenvironment regulation transport permits electrolytes performance.

Language: Английский

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Nanocurvature-induced field effects enable control over the activity of single-atom electrocatalysts

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Feb. 26, 2024

Tuning interfacial electric fields provides a powerful means to control electrocatalyst activity. Importantly, can modify adsorbate binding energies based on their polarizability and dipole moment, hence operate independently of scaling relations that fundamentally limit performance. However, implementation such strategy remains challenging because typical methods the field non-uniformly affects only minority active sites. Here we discover uniformly tunable modulation be achieved using model system single-atom catalysts (SACs). These consist M-N

Language: Английский

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Tuning the Interfacial Reaction Environment for CO₂ Electroreduction to CO in Mildly Acidic Media

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(8), P. 5242 - 5251

Published: Feb. 13, 2024

A considerable carbon loss of CO2 electroreduction in neutral and alkaline media severely limits its industrial viability as a result the homogeneous reaction OH– under interfacial alkalinity. Here, to mitigate reactions, we conducted mildly acidic media. By modulating environment via multiple electrolyte effects, parasitic hydrogen evolution is suppressed, leading faradaic efficiency over 80% for CO on planar Au electrode. Using rotating ring-disk electrode technique, ring constitutes an situ collector pH sensor, enabling recording Faradaic monitoring while reduction takes place disk. The dominant branch switches from proton water changes alkaline. comparison, starts within region approaches near-neutral conditions. Thereafter, decays, place, protons are increasingly consumed by electrogenerated reduction. reaches maximum just before initiates. Slowing mass transport lowers current, hardly influenced. In contrast, appropriate protic anion, e.g., HSO4– our case, weakly hydrated cations, K+, accelerate reduction, with former providing extra flux but higher local pH, latter stabilizing *CO2– intermediate.

Language: Английский

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