Asymmetric CO–CHO Coupling over Pr Single-Atom Alloy Enables Industrial-Level Electrosynthesis of Ethylene DOI
Yanteng Xiao, Fuqing Yu,

Chenfeng Xia

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: April 24, 2025

The electrocatalytic conversion of carbon dioxide (CO2) to ethylene (C2H4) holds great promise for sustainable chemical synthesis, yet achieving industrially relevant production rates remains a significant challenge. Through computational screening, we have identified praseodymium (Pr) single-atom alloy embedded in copper (Cu) catalyst (Pr@Cu) that exhibits superior CO2 activation and remarkably low energy barrier asymmetric *CO-*CHO coupling, primarily by facilitating the *CHO intermediate formation. Our optimized catalyst, Pr@Cu-2 (6 wt % Pr), achieves C2H4 Faradaic efficiency (FE) 64.2% at -1.6 V versus reversible hydrogen electrode (RHE) under high current density 1200 mA cm-2 reduction reaction (CO2RR). Furthermore, when integrated into 100 cm2 membrane assembly (MEA) electrolyzer, demonstrates robust performance, maintaining continuous rate 21.3 mL min-1 20 A over 200 h. This work provides fundamental insights role Pr alloys CO2RR highlights their potential scalable electrosynthesis.

Language: Английский

Low-coordinated copper facilitates the *CH2CO affinity at enhanced rectifying interface of Cu/Cu2O for efficient CO2-to-multicarbon alcohols conversion DOI Creative Commons
Yangyang Zhang, Yanxu Chen, Xiaowen Wang

et al.

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

Published: June 18, 2024

Abstract The carbon−carbon coupling at the Cu/Cu 2 O Schottky interface has been widely recognized as a promising approach for electrocatalytic CO conversion into value-added alcohols. However, limited selectivity of C 2+ alcohols persists due to insufficient control over rectifying characteristics required precise bonding oxyhydrocarbons. Herein, we present an investigation manipulation coordination environment Cu sites through in-situ electrochemical reconstruction strategy, which indicates that construction low-coordinated facilitates enhanced interfaces, and induces asymmetric electronic perturbation faster electron exchange, thereby boosting C-C oxyhydrocarbons towards nucleophilic reaction process *H CCO-CO. Impressively, exhibit superior faradic efficiency 64.15 ± 1.92% energy ~39.32% production, while maintaining stability 50 h (faradic >50%, total current density = 200 mA cm −2 ) in flow-cell electrolyzer. Theoretical calculations, operando synchrotron radiation Fourier transform infrared spectroscopy, Raman experiments decipher can enhance coverage *CO adsorption *CH CH CHO, facilitating formation

Language: Английский

Citations

29
Doping engineering of Cu-based catalysts for electrocatalytic CO2 reduction to multi-carbon products DOI

Shiya You,

Jiewen Xiao, Shuyu Liang

et al.

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(16), P. 5795 - 5818

Published: Jan. 1, 2024

Recent developments in heteroatom-doped Cu-based catalysts for CO 2 electroreduction into C 2+ products are highlighted. The design strategies doped and situ technologies discussed.

Language: Английский

Citations

29
Bottom‐up Growth of Convex Sphere with Adjustable Cu(0)/Cu(I) Interfaces for Effective C2 Production from CO2 Electroreduction DOI
Huan Liu, Cheng‐Han Yang,

Tong Bian

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(28)

Published: May 4, 2024

Abstract One challenge confronting the Cu 2 O catalysts in electrocatalysis of carbon dioxide reduction reaction (CO RR) is active Cu(I) species, resulting low selectivity and quick deactivation. In this study, we for first time introduce a bottom‐up growth convex sphere with adjustable Cu(0)/Cu(I) interfaces (Cu x @Cu spheres). Interestingly, are dynamically modulated by varying hydrothermal time, thus regulating conversion C 1 products. particular, 4 h treatment applied to 0.25 favorable interface results highest products (90.5 %). situ Fourier‐transform infrared spectroscopy measurements density functional theory calculations reveal that lowers energy barrier production ethylene ethanol while increasing coverage localized *CO adsorbate increased dimerization. This work establishes novel approach transforming state valence‐sensitive electrocatalysts into high‐value energy‐related engineering

Language: Английский

Citations

26
Selective Increase in CO2 Electroreduction to Ethanol Activity at Nanograin‐Boundary‐Rich Mixed Cu(I)/Cu(0) Sites via Enriching Co‐Adsorbed CO and Hydroxyl Species DOI
Ting Zhang,

Shenglin Xu,

De‐Li Chen

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: May 31, 2024

Selective producing ethanol from CO

Language: Английский

Citations

24
Unlocking high-current-density nitrate reduction and formaldehyde oxidation synergy for scalable ammonia production and fixation DOI
Linjie Zhang, Yimeng Cai, Yanghua Li

et al.

Energy & Environmental Science, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

Single atom Ag-decorated Cu 2 O nanowires achieve two-ampere-level nitrate-to-ammonia conversion, facilitating further ammonia fixation into ammonium formate at 10 g-scale.

Language: Английский

Citations

3
Electrosynthesis of ethylene glycol from biomass glycerol DOI Creative Commons
Haoyuan Chi,

Zhanpeng Liang,

Siyu Kuang

et al.

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

Published: Jan. 24, 2025

Ethylene glycol, a widely used chemical, has large global capacity exceeding 40 million tons per year. Nevertheless, its production is heavily reliant on fossil fuels, resulting in substantial CO2 emissions. Herein, we report an approach for electrochemically producing ethylene glycol from biomass glycerol. This process involves glycerol electrooxidation to glycolaldehyde at anode, which subsequently electro-reduced cathode. While the anode reaction been reported, cathode remains challenge. An electrodeposited electrode with metallic Cu catalyst enables us achieve glycolaldehyde-to-ethylene conversion exceptional faradaic efficiency of about 80%. Experimental and theoretical studies reveal that facilitates C=O activation, promoting hydrogenation into glycol. We further assemble zero-gap electrolyzer demonstrate electrosynthesis give decent rate 1.32 mmol cm–2 h–1 under 3.48 V cell voltage. The carbon intensity assessment based valid assumption reveals our strategy may reduce emissions by over 80 annually compared conventional fuel routes. utilized produced annually, typically made high Here, authors electrochemical method produce glycerol, offering more sustainable, low-emission alternative.

Language: Английский

Citations

2
Transient pulsed discharge preparation of graphene aerogel supports asymmetric Cu cluster catalysts promote CO2 electroreduction DOI Creative Commons
Kaiyuan Liu, H. F. Shen,

Zhiyi Sun

et al.

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

Published: Jan. 31, 2025

Designing asymmetrical structures is an effective strategy to optimize metallic catalysts for electrochemical carbon dioxide reduction reactions. Herein, we demonstrate a transient pulsed discharge method instantaneously constructing graphene-aerogel supports asymmetric copper nanocluster catalysts. This process induces the convergence of atoms decomposed by chloride onto graphene originating from intense current pulse and high temperature. The exhibit atomic electronic due lattice distortion oxygen doping clusters. In reaction, selectivity activity ethanol production are enhanced structure abundance active sites on catalysts, achieving Faradaic efficiency 75.3% 90.5% multicarbon products at −1.1 V vs. reversible hydrogen electrode. Moreover, strong interactions between nanoclusters support confer notable long-term stability. We elucidate key reaction intermediates mechanisms Cu4O-Cu/C2O1 moieties through in situ testing density functional theory calculations. study provides innovative approach balancing stability asymmetric-structure energy conversion. Asymmetric show promise CO2 catalytic reduction. Here, authors develop prepare graphene-aerogel-supported Cu that enhance conversion into products.

Language: Английский

Citations

2
Brass Phase Determining Selectivity in Urea Electrosynthesis from CO2 and Nitrate DOI

Shengliang Zhai,

Zheng Peng,

Xiaokang Chen

et al.

ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 3276 - 3283

Published: Feb. 7, 2025

Language: Английский

Citations

2
Enhancing C-C Coupling in CO2 Electroreduction by Engineering Pore Size of Porous Carbon-Supported Cu Catalysts DOI Open Access

Aiming Huang,

Jian Yu,

Junjun Zhang

et al.

Catalysts, Journal Year: 2025, Volume and Issue: 15(3), P. 199 - 199

Published: Feb. 20, 2025

The electroreduction of CO2 (CO2RR) is a promising and environmentally sustainable approach to closing the carbon cycle. However, achieving high activity selectivity for multicarbon (C2₊) products remains significant challenge due complexity reaction pathways. In this study, porous carbon-supported copper catalysts (CuHCS) with pore sizes 120 nm (CuHCS120) 500 (CuHCS500) were synthesized tailor microenvironment at electrode–electrolyte interface enhance product selectivity. CuHCS120 achieved maximum faradaic efficiency (FE) C2₊ 46%, double that CuHCS500 (23%). contrast, showed higher FE CO (36%) compared (14%) same potential. In-depth ex situ in investigations revealed smaller pores promote enrichment adsorption *CO intermediates, thereby enhancing C–C coupling formation products. These findings underscore critical role structural confinement modulating catalytic provide valuable insights rational design advanced CO2RR.

Language: Английский

Citations

2
Electrocatalytic CO2 hydrogenation to C2+ alcohols catalysed by Pr–Cu oxide heterointerfaces DOI

J Liu,

Pengsong Li, Shuaiqiang Jia

et al.

Nature Synthesis, Journal Year: 2025, Volume and Issue: unknown

Published: March 13, 2025

Language: Английский

Citations

2