Dual‐Metal Sites Drive Tandem Electrocatalytic CO2 to C2+ Products DOI Open Access

Guixian Xie,

Weiwei Guo,

Zijian Fang

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(47)

Published: Aug. 14, 2024

Abstract The electrochemical conversion of CO 2 into valuable chemicals is a promising route for renowable energy storage and the mitigation greenhouse gas emission, production multicarbon (C 2+ ) products highly desired. Here, we report 1.4 %Pd−Cu@CuPz comprising dispersive CuO x PdO dual nanoclusters embedded in MOF CuPz (Pz=Pyrazole), which achieves high C Faradaic efficiency (FE C2+ 81.9 % alcohol FE 47.5 with remarkable stability when using 0.1 M KCl aqueous solution as electrolyte typical H‐cell. Particularly, obviously improved on compared to Cu@CuPz . Theoretical calculations have revealed that enhanced interfacial electron transfer facilitates adsorption *CO intermediate *CO−*CO dimerization Cu−Pd sites bridged by Cu nodes Additionally, oxophilicity Pd can stabilize key *CH CHO promote subsequent proton‐coupled more efficiently, confirming formation pathway skew towards *C H 5 OH. Consequently, play synergistic tandem role cooperatively improving selectivity accelerating reductive

Language: Английский

Metal-organic-framework-based materials as platforms for energy applications DOI Creative Commons
Wenjuan Wang, Di Chen,

Fayan Li

et al.

Chem, Journal Year: 2023, Volume and Issue: 10(1), P. 86 - 133

Published: Oct. 10, 2023

Language: Английский

Citations

124
Selective CO2 Reduction to Ethylene Mediated by Adaptive Small‐molecule Engineering of Copper‐based Electrocatalysts DOI
Shenghua Chen,

Chengliang Ye,

Ziwei Wang

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(50)

Published: Oct. 30, 2023

Electrochemical CO2 reduction reaction (CO2 RR) over Cu catalysts exhibits enormous potential for efficiently converting to ethylene (C2 H4 ). However, achieving high C2 selectivity remains a considerable challenge due the propensity of undergo structural reconstruction during RR. Herein, we report an in situ molecule modification strategy that involves tannic acid (TA) molecules adaptive regulating Cu-based material pathway facilitates products. An excellent Faraday efficiency (FE) 63.6 % on with current density 497.2 mA cm-2 flow cell was achieved, about 6.5 times higher than pristine catalyst which mainly produce CH4 . The X-ray absorption spectroscopy and Raman studies reveal hydroxyl group TA stabilizes Cuδ+ Furthermore, theoretical calculations demonstrate /Cu0 interfaces lower activation energy barrier *CO dimerization, species stabilize *COH intermediate via hydrogen bonding, thereby promoting production. Such engineering modulated electronic structure provides promising achieve highly selective value-added chemicals.

Language: Английский

Citations

89
Boosting CO2 Electroreduction to C2H4 via Unconventional Hybridization: High-Order Ce4+ 4f and O 2p Interaction in Ce-Cu2O for Stabilizing Cu+ DOI

Yanfei Sun,

Jiangzhou Xie, Zhenzhen Fu

et al.

ACS Nano, Journal Year: 2023, Volume and Issue: 17(14), P. 13974 - 13984

Published: July 6, 2023

Efficient conversion of carbon dioxide (CO2) into value-added materials and feedstocks, powered by renewable electricity, presents a promising strategy to reduce greenhouse gas emissions close the anthropogenic loop. Recently, there has been intense interest in Cu2O-based catalysts for CO2 reduction reaction (CO2RR), owing their capabilities enhancing C–C coupling. However, electrochemical instability Cu+ Cu2O leads its inevitable Cu0, resulting poor selectivity C2+ products. Herein, we propose an unconventional feasible stabilizing through construction Ce4+ 4f–O 2p–Cu+ 3d network structure Ce-Cu2O. Experimental results theoretical calculations confirm that orbital hybridization near Ef based on high-order 4f 2p can more effectively inhibit leaching lattice oxygen, thereby Ce-Cu2O, compared with traditional d–p hybridization. Compared pure Cu2O, Ce-Cu2O catalyst increased ratio C2H4/CO 1.69-fold during CO2RR at −1.3 V. Furthermore, situ ex spectroscopic techniques were utilized track oxidation valency copper under conditions time resolution, identifying well-maintained species catalyst. This work not only avenue design involving but also provides deep insights metal-oxidation-state-dependent catalysts.

Language: Английский

Citations

78
Grain boundary-abundant copper nanoribbons on balanced gas-liquid diffusion electrodes for efficient CO2 electroreduction to C2H4 DOI
Lei Bian, Ziyang Zhang, Hao Tian

et al.

CHINESE JOURNAL OF CATALYSIS (CHINESE VERSION), Journal Year: 2023, Volume and Issue: 54, P. 199 - 211

Published: Nov. 1, 2023

Language: Английский

Citations

78
Cascade Dual Sites Modulate Local CO Coverage and Hydrogen-Binding Strength to Boost CO2 Electroreduction to Ethylene DOI
Junjun Li, Yu Chen, Bingqing Yao

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(8), P. 5693 - 5701

Published: Feb. 9, 2024

Rationally modulating the binding strength of reaction intermediates on surface sites copper-based catalysts could facilitate C–C coupling to generate multicarbon products in an electrochemical CO2 reduction reaction. Herein, theoretical calculations reveal that cascade Ag–Cu dual synergistically increase local CO coverage and lower kinetic barrier for protonation, leading enhanced asymmetric C2H4. As a proof concept, Cu3N-Ag nanocubes (NCs) with Ag located partial Cu Cu3N unit center are successfully synthesized. The Faraday efficiency current density C2H4 over NCs 7.8 9.0 times those NCs, respectively. In situ spectroscopies combined confirm produce promote *COCHO, significantly enhancing generation Our work provides new insights into catalysis strategy at atomic scale boosting products.

Language: Английский

Citations

60
Steering CO2 Electroreduction Selectivity U-Turn to Ethylene by Cu–Si Bonded Interface DOI
Wanfeng Xiong, Duan‐Hui Si, Hong-Fang Li

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 146(1), P. 289 - 297

Published: Dec. 22, 2023

Copper (Cu), with the advantage of producing a deep reduction product, is unique catalyst for electrochemical CO2 (CO2RR). Designing Cu-based to trigger CO2RR multicarbon product and understanding accurate structure–activity relationship elucidating reaction mechanisms still remain challenge. Herein, we demonstrate rational design core–shell structured silica-copper (p-Cu@m-SiO2) through Cu–Si direct bonding efficient selective CO2RR. The interface fulfills inversion in selectivity. ratio C2H4/CH4 changes from 0.6 14.4 after silica modification, current density reaches high up 450 mA cm–2. kinetic isotopic effect, situ attenuated total reflection Fourier-transform infrared spectra, functional theory were applied elucidate mechanism. SiO2 shell stabilizes *H intermediate by forming Si–O–H inhibits hydrogen evolution effectively. Moreover, direct-bonded makes bare Cu sites larger charge density. Such stabilized *CHO activated *CO, promoting coupling *CO intermediates form C2H4. This work provides promising strategy designing catalysts C2H4 catalytic activity.

Language: Английский

Citations

56
Advances and challenges in the electrochemical reduction of carbon dioxide DOI Creative Commons

Jingyi Han,

Xue Bai,

Xiaoqin Xu

et al.

Chemical Science, Journal Year: 2024, Volume and Issue: 15(21), P. 7870 - 7907

Published: Jan. 1, 2024

This review highlights the structure–activity relationship of ECO 2 RR, provides a detailed summary advanced materials by analyzing electrocatalytic applications and reaction mechanisms, discusses challenges in both devices.

Language: Английский

Citations

52
MOF-based materials for electrochemical reduction of carbon dioxide DOI

Jian-Mei Huang,

Xiang‐Da Zhang,

Jiayi Huang

et al.

Coordination Chemistry Reviews, Journal Year: 2023, Volume and Issue: 494, P. 215333 - 215333

Published: July 28, 2023

Language: Английский

Citations

45
Atomic-Scale Tailoring C–N Coupling Sites for Efficient Acetamide Electrosynthesis over Cu-Anchored Boron Nitride Nanosheets DOI
Yan Wang,

Shuai Xia,

Kui Chen

et al.

ACS Nano, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 4, 2024

Electrochemical conversion of carbon and nitrogen sources into valuable chemicals provides a promising strategy for mitigating CO

Language: Английский

Citations

36
Challenges and opportunities of atomic-scales reactive sites in thriving electrochemical CO2 reduction reaction DOI
Pengliang Sun, Sailin Liu, Xiong Zheng

et al.

Nano Today, Journal Year: 2024, Volume and Issue: 55, P. 102152 - 102152

Published: Jan. 13, 2024

Language: Английский

Citations

25