Trace Iodine Modified Copper Catalyst Drives Asymmetric C─C Coupling in Stable CO2 Electroreduction DOI Open Access
Zijun Yan, Min Liu,

Zeyu Guo

et al.

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

Published: Jan. 23, 2025

Abstract Cu‐based catalysts efficiently catalyze the electrochemical conversion of CO 2 into high‐value multicarbon (C 2+ ) products. However, it remains a challenge to achieve optimal structural stability, product selectivity, and long‐term catalytic durability. In this study, well‐active oxide‐derived Cu surface consisting predominantly O(111) facets is developed, which contains trace amounts iodine (I). The enhances hydrogenation *CO facilitates asymmetric coupling *CHO, while intercalated boosts adsorption CO. During reaction, release excess I increases roughness, remaining controls chemical state Cu. These effects together lead Faradaic efficiency 79.0% cathodic energy 43.5% for C products at current density 300 mA cm −2 . Moreover, found that periodic electrode treatment with iodide prevents agglomeration preserves sufficient active sites, ensuring improved stability production. This study provides new insights synergistic interactions between Cu─O compounds offers promising route development highly durable systems electroreduction.

Language: Английский

Enhancing CO2 Electroreduction Performance through Si-Doped CuO: Stabilization of Cu+/Cu0 Sites and Improved C2 Product Selectivity DOI
Feng Long, Rong Wang, Wenzhe Si

et al.

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(13), P. 10324 - 10333

Published: June 25, 2024

Language: Английский

Citations

14
Dynamic transformation of active sites in energy and environmental catalysis DOI Creative Commons
Hao Zhang, Lei Chen, Feng Dong

et al.

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(18), P. 6435 - 6481

Published: Jan. 1, 2024

Active sites play a pivotal role in photo/electrocatalysis, particularly the transition from fossil fuels to clean, efficient and renewable energy sources.

Language: Английский

Citations

13
Strong d‐p Orbital Hybridization of Os‐P via Ultrafast Microwave Plasma Assistance for Anion Exchange Membrane Electrolysis DOI Open Access
Qichang Li, Xiaowei Fu, Hongdong Li

et al.

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

Published: Aug. 2, 2024

Abstract Orbital hybridization is a promising approach to modulating the electronic structure of designed electrocatalysts boost reaction kinetics. In contrast d‐d hybridization, p‐d orbital between p‐block elements and d‐block metals can provide new opportunities modulate properties thus promote catalytic performance. Herein, phosphorus‐doped osmium (P‐Os) catalyst through ultrafast (20 s) microwave plasma engineering. Theoretical calculations verify d‐p P Os, leading modulation d‐band center Os active site. Specifically, neighboring exhibit highest activity, facilitating crucial processes such as H 2 O/H* adsorption dissociation. The overpotential P‐Os in alkaline seawater only 152 mV at 1 A cm −2 , which superior reported electrocatalysts. Moreover, synthesized catalysts are integrated into an anion exchange membrane (AEM) electrolyzer, demonstrating remarkable AEM electrolyzer requires 1.86/2.02 V achieve 500/1000 mA current densities. Then, achieved have great potential for practical electrocatalytic water‐splitting applications.

Language: Английский

Citations

12
Revolutionizing electrochemical CO2 reduction to deeply reduced products on non-Cu-based electrocatalysts DOI

Haoming Yu,

Hsiwen Wu,

Yuen Leong Chow

et al.

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(15), P. 5336 - 5364

Published: Jan. 1, 2024

Producing deeply reduced (>2 e − per carbon atom) products from the electrochemical CO 2 reduction reaction on non-Cu-based catalysts is an attractive and sustainable approach for utilization.

Language: Английский

Citations

10
Asymmetrically Coordinated Cu Dual‐Atom‐Sites Enables Selective CO2 Electroreduction to Ethanol DOI
Changli Chen,

Zhiyi Sun,

Gangzhi Qin

et al.

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

Published: Oct. 6, 2024

Abstract Electrochemical reduction of CO 2 (CO RR) to value‐added liquid fuels is a highly attractive solution for carbon‐neutral recycling, especially C 2+ products. However, the selectivity control preferable products great challenge due complex multi‐electron proton transfer process. In this work, series Cu atomic dispersed catalysts are synthesized by regulating coordination structures optimize RR selectivity. ‐SNC catalyst with uniquely asymmetrical coordinated CuN ‐CuNS site shows high ethanol selective FE 62.6% at −0.8 V versus RHE and 60.2% 0.9 in H‐Cell Flow‐Cell test, respectively. Besides, nest‐like structure beneficial mass process selection catalytic situ experiments theory calculations reveal reaction mechanisms such ethanol. The S atoms weaken bonding ability adjacent carbon atom, which accelerates from *CHCOH generate *CHCHOH, resulting This work indicates promising strategy rational design asymmetrically single, dual, or tri‐atom provides candidate material produce

Language: Английский

Citations

9
Establishment of Gas–Liquid–Solid Interface on Multilevel Porous Cu2O for Potential-Driven Selective CO2 Electroreduction toward C1 or C2 Products DOI
Changjiang Liu,

Hu Zang,

Xin Liu

et al.

ACS Applied Materials & Interfaces, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 20, 2025

Copper-based catalysts demonstrate distinctive multicarbon product activity in the CO2 electroreduction reaction (CO2RR); however, their low selectivity presents significant challenges for practical applications. Herein, we have developed a multilevel porous spherical Cu2O structure, wherein mesopores are enriched with catalytic active sites and effectively stabilize Cu+, while macropores facilitate formation of "gas–liquid–solid" three-phase interface, thereby creating microenvironment an increasing water concentration gradient from interior to exterior. Potential-driven phase engineering protonation synergistically optimize pathway, facilitating switch between CO C2H4. At current density 100 mA cm–2, faradaic efficiency (FE) reaches impressive 96.97%. When increases 1000 FEC2H4 attains 53.05%. Experiments theoretical calculations indicate that at lower potentials, pure diminishes adsorption *CO intermediates, weak inhibits hydrogen evolution reactions, promoting production. Conversely, more negative Cu0/Cu+ interface strong generate locally elevated concentrations *COOH which enhance C–C coupling deep hydrogenation, ultimately improving toward C2+ products. This study provides novel insights into rational design copper-based customizable

Language: Английский

Citations

1
Adjustable Selectivity for CO2 Electroreduction to Ethylene or Ethanol by Regulating Interphases Between Copper and Tin Oxides DOI Open Access
Huan Liu, Cheng‐Han Yang,

Tong Bian

et al.

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

Published: Feb. 10, 2025

Abstract Enhancing the selectivity of C 2 products and revealing reaction mechanisms in CO electroreduction (CO RR) remain challenging. Regulating interphases catalysts is one most promising pathways. Herein, between copper (Cu) tin (Sn) oxides are regulated by controlling degree reduction during self‐assembly process, which exhibits obvious different to ethylene ethanol, respectively. The interphase Cu‐SnO ethanol as high 74.6%, while Cu O‐SnO shows 71.4% at –0.6 V versus RHE. In situ Fourier‐transform infrared spectroscopy measurements density functional theory calculations demonstrate that strong electron interaction, preferentially forming key *COH intermediates for asymmetrical C─C coupling produce ethanol. contrast, possesses oxygen vacancies both sites, thus enriching *CO symmetrical interphase. findings this work offer an advanced strategy regulating adjust RR.

Language: Английский

Citations

1
Modulating Water Dissociation for Ampere-Level CO2-to-Ethanol Conversion over La(OH)3@Cu Hollow-fiber Penetration Electrode DOI

Jiayu Xia,

Shoujie Li, Xiaohu Liu

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2025, Volume and Issue: unknown, P. 125202 - 125202

Published: Feb. 1, 2025

Language: Английский

Citations

1
Pulsed electrosynthesis of glycolic acid through polyethylene terephthalate upcycling over a mesoporous PdCu catalyst DOI Creative Commons

Shu Han,

Lizhi Sun,

Dongping Fan

et al.

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

Published: April 10, 2025

Electrocatalytic upcycling of polyethylene terephthalate (PET) plastics offers a promising and sustainable route that not only addresses serious waste pollution but also produces high value-added chemicals. Despite some important achievements, their activity selectivity have been slower than needed. In this work, pulsed electrocatalysis is employed to engineer chemisorption properties on lamellar mesoporous PdCu (LM-PdCu) catalyst, which delivers stability for selective electrosynthesis glycolic acid (GA) from PET under ambient conditions. LM-PdCu synthesized by in situ nucleation attachment strategy along assembled templates, whose stacked morphology structure kinetically accelerate desorption GA expose fresh active sites metal catalysts continuous at mode. This thus Faraday efficiency >92% wide potential windows, yield rate reaching 0.475 mmol cm-2 h-1, cycling exceeding 20 cycles electrocatalytic upcycling. Moreover, discloses good performance scaled-up real bottle plastics. work presents chemicals through various feedstocks.

Language: Английский

Citations

1
Pulse Manipulation on Cu-Based Catalysts for Electrochemical Reduction of CO2 DOI

Wanlong Xi,

Hexin Zhou,

Peng Yang

et al.

ACS Catalysis, Journal Year: 2024, Volume and Issue: unknown, P. 13697 - 13722

Published: Aug. 30, 2024

Electrocatalytic carbon dioxide reduction (CO2RR) over Cu-based catalysts has emerged as a promising strategy for value-added artificial cycling, addressing the current climate and energy challenges. However, product selectivity long-term stability of are limited by their instability at constant potential. Recent advancements in pulsed techniques aim to overcome these limitations, enhancing industrial feasibility CO2RR systems. This review critically examines recent research progress catalysts, offering comprehensive synthesis findings. Key pulse parameters characterization strategies explored uncover mechanisms behind enhanced performance. The focus is on surface reconstruction, encompassing regeneration stabilization Cu oxidation states alongside morphological evolution, while also discussing microenvironment changes, including local CO2 concentration, pH, ionic arrangement. intricate modulation mode, potential, duration performance elucidated, highlighting interconnections. Finally, we identify prevailing challenges propose future directions achieving environmentally friendly economically viable cycling. By providing insightful perspectives optimizing CO2RR, this paves way developing more efficient robust catalytic

Language: Английский

Citations

8