Urea Electrosynthesis from Nitrate and CO₂ on Diatomic Alloys

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(30)

Published: June 14, 2024

Abstract Urea electrosynthesis from co–electrolysis of NO 3 − and CO 2 (UENC) offers a promising technology for achieving sustainable efficient urea production. Herein, diatomic alloy catalyst (CuPd 1 Rh –DAA), with mutually isolated Pd atoms alloyed on Cu substrate, is theoretically designed experimentally confirmed to be highly active selective UENC catalyst. Combining theoretical computations operando spectroscopic characterizations reveals the synergistic effect –Cu sites promote via tandem catalysis mechanism, where site triggers early C–N coupling promotes *CO –to–*CO NH steps, while facilitates subsequent protonation step *COOHNH toward formation. Impressively, CuPd –DAA assembled in flow cell presents highest Faradaic efficiency 72.1% yield rate 53.2 mmol h −1 g cat at −0.5 V versus RHE, representing nearly performance among all reported catalysts.

Language: Английский

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Metal–organic framework-derived single-atom catalysts for electrocatalytic energy conversion applications

Journal of Materials Chemistry A, Journal Year: 2024, Volume and Issue: 12(30), P. 18921 - 18947

Published: Jan. 1, 2024

Single-atom catalysts (SACs) derived from metal–organic frameworks (MOFs) are revolutionizing electrocatalytic energy conversion.

Language: Английский

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Atomically dispersed metal cocatalysts for solar energy conversion

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(20), P. 7649 - 7680

Published: Jan. 1, 2024

This review explores the role of atomic metal site cocatalysts in photocatalysis for solar energy conversion, focusing on recent advances single-atom and cluster cocatalysts, their structure–activity relationships, key applications.

Language: Английский

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Isolated Tin Enhanced CO Coverage‐Regulation on Sn₁Cu Alloy for Selective CO₂ Electroreduction to C₂₊ Products

Small, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 15, 2025

Electricity-powered C─C coupling of CO2 represents an attractive strategy for producing valuable commodity chemicals with renewable energy, but it is still challenging to gain high C2+ selectivity at current density. Here, a Sn1Cu single-atom alloy (SAA) reported isolated Sn atom embedded into the Cu lattice, as efficient ectrocatalyst reduction. The prepared Sn1Cu-SAA catalyst shows maximal Faradaic efficiency 79.3% 800 mA cm-2, which can be kept stable least 16 h. combination in situ spectroscopy and DFT calculation reveal that introduced promote activation *CO, enhance CO coverage on Sn1Cu-SAA. As results, reaction barrier pathway significantly reduced, boosting generation products. These findings offer novel sight fabricating multicarbon products from via regulation concentration intermediates catalytic interface.

Language: Английский

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Gold Single Atom Doped Defective Nanoporous Copper Octahedrons for Electrocatalytic Reduction of Carbon Dioxide to Ethylene

ACS Nano, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 24, 2025

Electrocatalytic CO2 reduction into high-value multicarbon products offers a sustainable approach to closing the anthropogenic carbon cycle and contributing neutrality, particularly when renewable electricity is used power reaction. However, lack of efficient durable electrocatalysts with high selectivity for multicarbons severely hinders practical application this promising technology. Herein, nanoporous defective Au1Cu single-atom alloy (De-Au1Cu SAA) catalyst developed through facile low-temperature thermal in hydrogen subsequent dealloying process, which shows toward ethylene (C2H4), Faradaic efficiency 52% at current density 252 mA cm–2 under potential −1.1 V versus reversible electrode (RHE). In situ spectroscopy measurements functional theory (DFT) calculations reveal that C2H4 product results from synergistic effect between Au single atoms Cu sites on surface catalysts, where promote *CO generation defects stabilize key intermediate *OCCO, altogether enhances C–C coupling kinetics. This work provides important insights design electrochemical products.

Language: Английский

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Isolated Metal Centers Activate Small Molecule Electrooxidation: Mechanisms and Applications

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

Published: Jan. 26, 2025

Abstract Electrochemical oxidation of small molecules shows great promise to substitute oxygen evolution reaction (OER) or hydrogen (HOR) enhance kinetics and reduce energy consumption, as well produce high‐valued chemicals serve fuels. For these reactions, high‐valence metal sites generated at oxidative potentials are typically considered active trigger the process molecules. Isolated atom site catalysts (IASCs) have been developed an ideal system precisely regulate state coordination environment single‐metal centers, thus optimize their catalytic property. The isolated in IASCs inherently possess a positive state, can be more readily homogeneous under than nanoparticle counterparts. Meanwhile, merely centers but lack ensemble sites, which alter adsorption configurations compared with counterparts, induce various pathways mechanisms change product selectivity. More importantly, construction is discovered limit d‐electron back donation CO 2p * orbital overly strong on resolve poisoning problems most electro‐oxidation reactions improve stability. Based advantages fields electrochemical molecules, this review summarizes recent developments advancements focusing anodic HOR fuel cells OER electrolytic alternative such formic acid/methanol/ethanol/glycerol/urea/5‐hydroxymethylfurfural (HMF) key reactions. merits different decoding structure–activity relationships specifically discussed guide precise design structural regulation from perspective comprehensive mechanism. Finally, future prospects challenges put forward, aiming motivate application possibilities for diverse functional IASCs.

Language: Английский

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Single-Atom-Alloy Catalysts for Enhanced Hydrogenation Reaction Process: Mechanism, Regulation Strategy, and Design Principle

ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 3674 - 3698

Published: Feb. 14, 2025

Language: Английский

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Radiocatalytic synthesis of acetic acid from CH4 and CO2

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(44)

Published: July 26, 2024

Abstract The C−C coupling of methane (CH 4 ) and carbon dioxide (CO 2 to generate acetic acid 3 COOH) represents a highly atom‐efficient chemical conversion, fostering the comprehensive utilization greenhouse gases. However, inherent thermodynamic stability kinetic inertness CH CO present obstacles achieving efficient selective conversion at room temperature. Our study reveals that hydroxyl radicals (⋅OH) hydrated electrons (e aq − produced by water radiolysis can effectively activate , yielding methyl (⋅CH radical anions(⋅CO facilitate production COOH ambient introduction radiation‐synthesized CuO‐anchored TiO bifunctional catalyst could further enhance reaction efficiency selectivity remarkably boosting radiation absorption stability, resulting in concentration 7.1 mmol ⋅ L −1 with near‐unity (>95 %). These findings offer valuable insights for design implementation radiation‐induced conversion.

Language: Английский

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When Electrocatalytic Nitrate Reduction Meets Copper-based Atomic Site Catalysts

Journal of Materials Chemistry A, Journal Year: 2024, Volume and Issue: unknown

Published: Jan. 1, 2024

This manuscript comprehensively reviews the recent advancements in Cu-based atomic site catalysts NO 3 RR, following a sequential order with six sections: Introduction, Mechanism, SACs, SAAs, DACs, and Perspectives.

Language: Английский

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Regulation of Metal‐Support Interaction in Single‐Atom Catalysis

Small, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 24, 2024

Abstract In recent years, single‐atom catalysts (SACs) with separated active centers and high atom utilization have grown significantly as a significant area of catalytic research. applications, SACs various kinds demonstrated exceptional performance, so the study mechanism provides clearer direction for preparation performance. Strong linkages between single atoms support are necessary to overcome tendency aggregate into clusters, which is called metal‐support interaction (MSI). MSI affects not only stability individual atoms, but also nature binding site applicable reactions. Therefore, investigating connection crucial. This work describes latest developments in means activity modulation catalysis. First, synthesis strategies presented, including ALD, co‐deposition, impregnation, on. Second, mechanisms realized by using loading different types supports highlighted. Third, discussed, heterojunction strategy, ligand environment dual‐single‐atom strategy. Finally, possible directions future development catalysis suggested.

Language: Английский

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