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Enhanced Carbon‐Carbon Coupling at Interfaces with Abrupt Coordination Number Changes
Abstract
Abstract Cu‐catalyzed electrochemical CO 2 reduction reaction (CO 2 RR) produces multi‐carbon (C 2+ ) chemicals with considerable selectivities and activities, yet required high overpotentials impede its practical application. Here, we design interfaces with abrupt coordination number (CN) changes that greatly reduce the applied potential for achieving high C 2+ Faradaic efficiency (FE). Encouraged by the mechanistic finding that the coupling between *CO and *CO(H) is the most probable C−C bond formation path, we use Cu 2 O‐ and Cu‐phthalocyanine‐derived Cu (OD−Cu and PD−Cu) to build the interface. Using operando X‐ray absorption spectroscopy (XAS), we find that the Cu CN of OD−Cu is ~11, favoring CO* adsorption, while the PD−Cu has a COH*‐favorable CN of ~4. Operando Raman spectroscopy revealed that the interfaces with abrupt CN changes promote *OCCOH formation. As a result, the designed catalyst achieves a C 2+ FE of 85±2 % at 220 mA cm −2 in a zero‐gap CO 2 electrolyzer. An improvement of C 2+ FE by 3 times is confirmed at the low potential regime where the current density is 60–140 mA cm −2 , compared to bare OD−Cu. We report a 45‐h stable CO 2 RR operation at 220 mA cm −2 , producing a C 2+ product FE of ~80 %.
- Authors:
-
[1]
- Institute of Functional Nano &, Soft Materials (FUNSOM) Jiangsu Key Laboratory for Advanced Negative Carbon Technologies Soochow University Suzhou 215123 China
- School of Chemical Sciences University of Auckland Auckland 1010 New Zealand
- Laboratory of Advanced Materials Department of Chemistry Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Fudan University Shanghai 200438 China
- Frontiers Science Center for Transformative Molecules Shanghai Jiao Tong University Shanghai 200240 China
- Department of Mechanical and Industrial Engineering University of Toronto 5 King's College Road Toronto ON M5S 3G8 Canada
- Department of Applied Chemistry National Yang Ming Chiao Tung University Hsinchu 300 Taiwan
- Publication Date:
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 2333708
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Publisher's Accepted Manuscript
- Journal Name:
- ChemSusChem
- Additional Journal Information:
- Journal Name: ChemSusChem; Journal ID: ISSN 1864-5631
- Publisher:
- Wiley Blackwell (John Wiley & Sons)
- Country of Publication:
- Germany
- Language:
- English
Citation Formats
Wang, Xuan, Lu, Ruihu, Pan, Binbin, Yang, Chao, Zhuansun, Mengjiao, Li, Jun, Xu, Yi, Hung, Sung‐Fu, Zheng, Gengfeng, Li, Yanguang, Wang, Ziyun, and Wang, Yuhang. Enhanced Carbon‐Carbon Coupling at Interfaces with Abrupt Coordination Number Changes. Germany: N. p., 2024.
Web. doi:10.1002/cssc.202400150.
Wang, Xuan, Lu, Ruihu, Pan, Binbin, Yang, Chao, Zhuansun, Mengjiao, Li, Jun, Xu, Yi, Hung, Sung‐Fu, Zheng, Gengfeng, Li, Yanguang, Wang, Ziyun, & Wang, Yuhang. Enhanced Carbon‐Carbon Coupling at Interfaces with Abrupt Coordination Number Changes. Germany. https://doi.org/10.1002/cssc.202400150
Wang, Xuan, Lu, Ruihu, Pan, Binbin, Yang, Chao, Zhuansun, Mengjiao, Li, Jun, Xu, Yi, Hung, Sung‐Fu, Zheng, Gengfeng, Li, Yanguang, Wang, Ziyun, and Wang, Yuhang. Thu .
"Enhanced Carbon‐Carbon Coupling at Interfaces with Abrupt Coordination Number Changes". Germany. https://doi.org/10.1002/cssc.202400150.
@article{osti_2333708,
title = {Enhanced Carbon‐Carbon Coupling at Interfaces with Abrupt Coordination Number Changes},
author = {Wang, Xuan and Lu, Ruihu and Pan, Binbin and Yang, Chao and Zhuansun, Mengjiao and Li, Jun and Xu, Yi and Hung, Sung‐Fu and Zheng, Gengfeng and Li, Yanguang and Wang, Ziyun and Wang, Yuhang},
abstractNote = {Abstract Cu‐catalyzed electrochemical CO 2 reduction reaction (CO 2 RR) produces multi‐carbon (C 2+ ) chemicals with considerable selectivities and activities, yet required high overpotentials impede its practical application. Here, we design interfaces with abrupt coordination number (CN) changes that greatly reduce the applied potential for achieving high C 2+ Faradaic efficiency (FE). Encouraged by the mechanistic finding that the coupling between *CO and *CO(H) is the most probable C−C bond formation path, we use Cu 2 O‐ and Cu‐phthalocyanine‐derived Cu (OD−Cu and PD−Cu) to build the interface. Using operando X‐ray absorption spectroscopy (XAS), we find that the Cu CN of OD−Cu is ~11, favoring CO* adsorption, while the PD−Cu has a COH*‐favorable CN of ~4. Operando Raman spectroscopy revealed that the interfaces with abrupt CN changes promote *OCCOH formation. As a result, the designed catalyst achieves a C 2+ FE of 85±2 % at 220 mA cm −2 in a zero‐gap CO 2 electrolyzer. An improvement of C 2+ FE by 3 times is confirmed at the low potential regime where the current density is 60–140 mA cm −2 , compared to bare OD−Cu. We report a 45‐h stable CO 2 RR operation at 220 mA cm −2 , producing a C 2+ product FE of ~80 %.},
doi = {10.1002/cssc.202400150},
journal = {ChemSusChem},
number = ,
volume = ,
place = {Germany},
year = {Thu Apr 04 00:00:00 EDT 2024},
month = {Thu Apr 04 00:00:00 EDT 2024}
}
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