Structural engineering of atomic catalysts for electrocatalysis

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

---

Steering the Site Distance of Atomic Cu‐Cu Pairs by First‐Shell Halogen Coordination Boosts CO2‐to‐C2 Selectivity

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(46)

Published: Aug. 6, 2024

Electrocatalytic reduction of CO

Language: Английский

---

Addressing the Carbonate Issue: Electrocatalysts for Acidic CO₂ Reduction Reaction

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: May 9, 2024

Abstract Electrochemical CO 2 reduction reaction (CO RR) powered by renewable energy provides a promising route to conversion and utilization. However, the widely used neutral/alkaline electrolyte consumes large amount of produce (bi)carbonate byproducts, leading significant challenges at device level, thereby impeding further deployment this reaction. Conducting RR in acidic electrolytes offers solution address “carbonate issue”; however, it presents inherent difficulties due competitive hydrogen evolution reaction, necessitating concerted efforts toward advanced catalyst electrode designs achieve high selectivity activity. This review encompasses recent developments RR, from mechanism elucidation design engineering. begins discussing mechanistic understanding pathway, laying foundation for RR. Subsequently, an in‐depth analysis advancements catalysts is provided, highlighting heterogeneous catalysts, surface immobilized molecular enhancement. Furthermore, progress made device‐level applications summarized, aiming develop high‐performance systems. Finally, existing future directions are outlined, emphasizing need improved selectivity, activity, stability, scalability.

Language: Английский

---

Efficient acidic CO2 electroreduction to formic acid by modulating electrode structure at industrial-level current

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 489, P. 151238 - 151238

Published: April 14, 2024

Language: Английский

---

Experimental and Theoretical Insights into Single Atoms, Dual Atoms, and Sub‐Nanocluster Catalysts for Electrochemical CO₂ Reduction (CO₂RR) to High‐Value Products

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(52)

Published: Nov. 26, 2024

Abstract Electrocatalytic carbon dioxide (CO 2 ) conversion into valuable chemicals paves the way for realization of recycling. Downsizing catalysts to single‐atom (SACs), dual‐atom (DACs), and sub‐nanocluster (SNCCs) has generated highly active selective CO transformation reduced products. This is due introduction numerous sites, unsaturated coordination environments, efficient atom utilization, confinement effect compared their nanoparticle counterparts. Herein, recent Cu‐based SACs are first reviewed newly emerged DACs SNCCs expanding catalysis electrocatalytic reduction RR) high‐value products discussed. Tandem SAC–nanocatalysts (NCs) (SAC–NCs) also discussed RR Then, non‐Cu‐based SACs, DACs, SAC–NCs, theoretical calculations various transition‐metal summarized. Compared previous achievements less‐reduced products, this review focuses on double objective achieving full increasing selectivity formation rate toward C–C coupled with additional emphasis stability catalysts. Finally, through combined experimental research, future outlooks offered further develop over isolated atoms sub‐nanometal clusters.

Language: Английский

---

Highly Selective Acidic CO₂ Electroreduction with Large Current on Polypyrrole‐Modified Ag Catalyst by Local Microenvironment Modulation

Advanced Energy Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 2, 2025

Abstract Electrocatalytic carbon dioxide reduction (CO 2 RR) holds great promise for capture and utilization. In acidic media, CO RR enables efficient conversion, but with low selectivity due to the competitive hydrogen evolution reaction (HER) catalyst corrosion. Herein, conductive polymer polypyrrole (PPy) coated Ag nanoparticles (NPs) catalysts (Ag@PPy) different thicknesses are designed synthesized, which could create a hydrophobic environment that reduces accessibility of H O NPs thereby inhibiting HER. The coating PPy layer also protects from corrosion improves stability system. Among them, Ag@PPy‐2 appropriate thickness showed up 91.7% electrocatalytic high durability in electrolyte at −300 mA cm −2 . Density functional theory (DFT) calculation shows not only inhibit HER, reduce energy barrier, improve efficiency CO. This study may provide some new ideas design advanced selective by local microenvironmental engineering.

Language: Английский

---

Polymeric ionic liquid promotes acidic electrocatalytic CO2 conversion to multicarbon products with ampere level current on Cu

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: Feb. 21, 2025

The acidic electroreduction of CO2 into multicarbon (C2+) products is much attractive for the improved carbon utilization than alkaline or neutral electroreduction. How to improve efficiency C2+ generation by CO2, important, especially at high current density and in electrolyte with low K+ concentration. Herein, we propose a strategy capping Cu surface polymeric ionic liquid (PIL) adlayer boosting electrocatalytic conversion densities (ampere-level) In relatively concentration (1.0 M), Faradaic (FE) reaches 82.2% under 1.0 A·cm−2 environment (pH=1.8). Particularly, when as 1.5 A·cm−2, FE still keeps 75.8%. Experimental theoretical studies reveal that presence PIL on catalyst can well inhibit H+ diffusion surface, enrich more facilitate C-C coupling reaction. Acidic reduction promising way utilization, which selectivity activity need improvement. Here, authors report boost ampere level density.

Language: Английский

---

Progress in Cu‐Based Catalyst Design for Sustained Electrocatalytic CO₂ to C₂₊ Conversion

Advanced Science, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 27, 2025

Abstract The electrocatalytic conversion of CO 2 into valuable multi‐carbon (C 2+ ) products using Cu‐based catalysts has attracted significant attention. This review provides a comprehensive overview recent advances in catalyst design to improve C selectivity and operational stability. It begins with an analysis the fundamental reaction pathways for formation, encompassing both established emerging mechanisms, which offer critical insights design. In situ techniques, essential validating these by real‐time observation intermediates material evolution, are also introduced. A key focus this is placed on how enhance through manipulation, particularly emphasizing catalytic site construction promote C─C coupling via increasing * coverage optimizing protonation. Additionally, challenge maintaining activity under conditions discussed, highlighting reduction active charged Cu species materials reconstruction as major obstacles. To address these, describes strategies preserve sites control including novel utilization mitigation reconstruction. By presenting developments challenges ahead, aims guide future conversion.

Language: Английский

---

Fundamental Insights into Photoelectrochemical Carbon Dioxide Reduction: Elucidating the Reaction Pathways

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(22), P. 16795 - 16833

Published: Oct. 31, 2024

The photoelectrochemical (PEC) reduction of carbon dioxide (CO2) to produce solar fuels presents a sustainable strategy mitigate CO2 emissions and alleviate the global energy crisis. While significant research efforts have been dedicated optimizing cell system configurations designing efficient photoelectrocatalysts, there remains lack in-depth understanding pathway. This review provides comprehensive overview fundamental insights PEC with focus on pathways from perspectives final products adsorption modes. First, key challenges are identified analyzed, including initial activation CO2, competitive hydrogen evolution reaction (HER), complex carbon–carbon (C–C) coupling process. then examines aspects process, covering state-of-the-art devices, their operational principles, methodologies for capturing intermediates. through concerted or sequential proton–electron transfer mechanisms is discussed in detail. Furthermore, potential systematically categorized basis distinct modes that drive insertion, carbon-coordinated oxygen-coordinated monodentate adsorption, bidentate oxygen vacancies. Detailed leading formation C1, C2, C3 compounds elucidated, an emphasis strategies enhance selectivity toward C1 C2+ products. In particular, aids catalyst design. For production, design focuses promoting activation, as rate-determining step (RDS) activation. contrast, formation, aim increase intermediate concentration, thereby enhancing lateral interaction intermediates, which crucial C–C coupling. Finally, summarizes future breakthroughs electron, interfacial, ionic pathways, offering into ongoing technologies.

Language: Английский

---

Polyoxometalate Functionalized Cyclic Trinuclear Copper Compounds for Bifunctional Electrochemical Detection and Photocatalytic Reduction of Cr(VI)

Inorganic Chemistry, Journal Year: 2024, Volume and Issue: 63(27), P. 12564 - 12571

Published: June 26, 2024

The design and intentional construction of crystalline materials containing two clusters with redox properties in one framework still remains challenging. Linking oxidative polyoxometalate (POM) a reductive cyclic trinuclear copper complex (Cu-CTC) to prepare stable catalysts is rarely reported. Herein, we successfully obtained new polyoxometalate-based metal-organic compounds (POMOCs) [Cu

Language: Английский

---