Zinc Hollow-Fiber Penetration Electrode Promotes Ampere-Level CO2 Electroreduction for Viable Applications

IF 13.1 1区 化学 Q1 CHEMISTRY, PHYSICAL ACS Catalysis Pub Date : 2025-02-25 DOI:10.1021/acscatal.4c07490
Xiaohu Liu, Shoujie Li, Aohui Chen, Xiao Dong, Jianing Mao, Chang Zhu, Gangfeng Wu, Yiheng Wei, Jiayu Xia, Huanyi Zhu, Xiaotong Wang, Ziran Xu, Guihua Li, Yanfang Song, Wei Wei, Wei Chen
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Abstract

CO2 conversion into value-added chemicals via the electrochemical CO2 reduction reaction (eCO2RR) offers substantial environmental and economic benefits. Among all eCO2RR products, CO shows vital significance due to its extensive application in chemical industrial synthesis, yet its production via eCO2RR is hindered by the requirements of noble metal catalysts. Zinc-based catalysts are potential cost-effective alternatives while still confronting the inadequacy of eCO2RR activity and CO selectivity. This study introduces an architecturally optimized zinc hollow-fiber penetration electrode (Zn HPE) that achieves a CO Faradaic efficiency exceeding 90% while sustaining stable operation for 110 h at 800 mA cm–2. In situ X-ray absorption analysis along with operando Raman spectroscopy confirms the maintenance of metallic Zn0 during eCO2RR. Transmission Fourier transform infrared spectroscopy confirmed that the superior performance of Zn HPE is attributed to its unique penetration effect, ensuring the local enrichment and rapid replenishment of CO2 at the surface active sites. Besides, the effect of local CO2 enrichment with high coverage on lowering the energy barrier for forming the *COOH intermediate and subsequent CO2-to-CO conversion enhancement was also elucidated via density functional theory calculations. The techno-economic analysis further suggests the prominent cost advantage of Zn HPE. This work presents a promising approach for designing efficient CO2 electroreduction electrodes for viable applications.

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锌中空纤维渗透电极促进安培级CO2电还原可行的应用
通过电化学CO2还原反应(eCO2RR)将CO2转化为增值化学品具有巨大的环境和经济效益。在所有eCO2RR产品中,CO因其在化工合成中的广泛应用而具有重要意义,但通过eCO2RR生产CO受到贵金属催化剂要求的阻碍。锌基催化剂是具有成本效益的潜在替代品,但仍面临着eCO2RR活性和CO选择性不足的问题。本研究介绍了一种结构优化的锌空心纤维渗透电极(Zn HPE),其CO法拉第效率超过90%,同时在800 mA cm-2下保持稳定运行110小时。原位x射线吸收分析和operando拉曼光谱证实了eCO2RR期间金属Zn0的维持。透射傅里叶变换红外光谱证实,Zn HPE的优越性能归功于其独特的穿透效应,保证了CO2在表面活性位点的局部富集和快速补充。此外,通过密度泛函理论计算,还阐明了高覆盖率的局部CO2富集对降低*COOH中间体形成的能垒和随后的CO2-to- co转化增强的作用。技术经济分析进一步表明,锌HPE具有突出的成本优势。这项工作为设计有效的二氧化碳电还原电极提供了一种有前途的方法。
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来源期刊
ACS Catalysis
ACS Catalysis CHEMISTRY, PHYSICAL-
CiteScore
20.80
自引率
6.20%
发文量
1253
审稿时长
1.5 months
期刊介绍: ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.
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