单分散Cu-TCPP/Cu2O杂化微球:一种具有优异电还原CO2产C2性能的级联电催化剂

doi:10.13208/j.electrochem.2303271

电化学（中英文） ›› 2024, Vol. 30 ›› Issue (1): 2303271. doi: 10.13208/j.electrochem.2303271

单分散Cu-TCPP/Cu₂O杂化微球:一种具有优异电还原CO₂产C₂性能的级联电催化剂

万紫轩^a, Aidar Kuchkaev^b, Dmitry Yakhvarov^b^,^c^,^*(), 康雄武^a^,^*()

^a华南理工大学环境与能源学院新能源研究所，广东广州 510006
^b阿尔布佐夫有机与物理化学研究所，俄罗斯联邦，喀山， 420088
^c喀山联邦大学亚历山大·巴特列罗夫化学研究所，俄罗斯联邦，喀山， 420008

收稿日期:2023-04-07 修回日期:2023-05-15 接受日期:2023-06-07 出版日期:2024-01-28 发布日期:2023-06-14

Monodispersed Cu-TCPP/Cu₂O Hybrid Microspheres: A Superior Cascade Electrocatalyst toward CO₂ Reduction to C₂ Products

Zi-Xuan Wan^a, Aidar Kuchkaev^b, Dmitry Yakhvarov^b^,^c^,^*(), Xiong-Wu Kang^a^,^*()

^aNew Energy Research Institute, School of Environment and Energy, South China University of Technology, Higher Education Mega Center, Guangzhou 510006, Guangdong, China
^bArbuzov Institute of Organic and Physical Chemistry, FRC Kazan Scientific Center of RAS, Arbuzov Street 8, Kazan, 420088, Russian Federation
^cAlexander Butlerov Institute of Chemistry, Kazan Federal University, Kremlyovskaya Street 18, Kazan, 420008, Russian Federation

Received:2023-04-07 Revised:2023-05-15 Accepted:2023-06-07 Published:2024-01-28 Online:2023-06-14
Contact: *Xiong-Wu Kang, Tel: (86-20)39381206, E-mail address: esxkang@scut.edu.cn; Dmitry Yakhvarov, E-mail address: yakhvar@iopc.ru

1. S1.pdf(1690KB)

摘要/Abstract

摘要：

高效电还原CO₂（ECR）为有价值的多碳产物是解决CO₂排放问题的有效解决方案。基于卟啉的金属有机框架（MOFs）具有多孔结构和有序的活性位点，有望提高ECR生成多碳产物的选择性。本文制备了由铜-四（4-羧基）卟啉（Cu-TCPP）和Cu₂O组成的有机/无机杂化Cu-TCPP@Cu₂O电催化剂，其中TCPP在调控形貌方面起着重要作用。ECR过程中原位形成的Cu与Cu-TCPP（Cu-TCPP@Cu）结合可以抑制析氢，富集CO中间体，促进C-C偶联生成C₂产物。多孔碳（PC）负载的Cu-TCPP@Cu在PC上被还原为Cu纳米簇，同时对C₂产物具有较高的ECR活性和选择性。催化剂在-1.0 V时（相对于可逆氢电极），C₂产物法拉第效率为62.3%，部分电流密度为83.4 mA·cm^-2，是纯Cu₂O和TCPP的7.6倍和13.1倍。本论文研究了催化剂形貌和杂化结构如何提高ECR生C₂产物的选择性，为高性能ECR催化剂的设计提供了新思路。

关键词: 有机/无机杂化电催化剂, 四（4-羧基）卟啉, 氧化亚铜, 级联电催化剂

Abstract:

The electrochemical conversion of carbon dioxide (CO₂) into valuable chemicals is a feasible way to mitigate the negative impacts of overmuch CO₂ emissions. Porphyrin-based metal organic frameworks (MOFs) are expected to be used for selective and efficient electrochemical CO₂ reduction (ECR) with porous structure and ordered active sites. Herein, we report the synthesis of a monodispersed and spherical organic/inorganic hybrid Cu-TCPP@Cu₂O electrocatalyst composed of Cu-TCPP (TCPP=tetrakis (4-carboxyphenyl) porphyrin) and Cu₂O, where TCPP plays significant roles in regulating the morphology. In-situ formed Cu during ECR process in combination with Cu-TCPP (Cu-TCPP@Cu) can suppress hydrogen evolution, enrich CO intermediate and promote C-C coupling toward C₂ products. The Cu-TCPP@Cu supported on porous carbon (PC) showed ultrafine Cu nanoclusters on PC, and displayed high ECR activity and selectivity toward C₂ products, with a C₂ faradaic efficiency of 62.3% at -1.0 V versus the reversible hydrogen electrode and a C₂ partial current density of 83.4 mA·cm^-2, which is 7.6 times and 13.1 times those of pure Cu₂O and TCPP, respectively. The morphology and hybrid structure of the catalyst were studied to improve the selectivity of ECR to produce C₂ products, which provides a new idea for the design of high-performance ECR catalyst.

Key words: Organic/inorganic hybrid electrocatalysts, TCPP, Cuprous oxide, Cascade electrocatalysts

万紫轩, Aidar Kuchkaev, Dmitry Yakhvarov, 康雄武. 单分散Cu-TCPP/Cu₂O杂化微球:一种具有优异电还原CO₂产C₂性能的级联电催化剂[J]. 电化学（中英文）, 2024, 30(1): 2303271.

Zi-Xuan Wan, Aidar Kuchkaev, Dmitry Yakhvarov, Xiong-Wu Kang. Monodispersed Cu-TCPP/Cu₂O Hybrid Microspheres: A Superior Cascade Electrocatalyst toward CO₂ Reduction to C₂ Products[J]. Journal of Electrochemistry, 2024, 30(1): 2303271.

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链接本文: https://electrochem.xmu.edu.cn/CN/10.13208/j.electrochem.2303271

https://electrochem.xmu.edu.cn/CN/Y2024/V30/I1/2303271

图/表 4

参考文献 61

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单分散Cu-TCPP/Cu₂O杂化微球:一种具有优异电还原CO₂产C₂性能的级联电催化剂

Monodispersed Cu-TCPP/Cu₂O Hybrid Microspheres: A Superior Cascade Electrocatalyst toward CO₂ Reduction to C₂ Products

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