دورية أكاديمية
Stabilizing highly active atomically dispersed NiN4Cl sites by Cl‐doping for CO2 electroreduction
| العنوان: | Stabilizing highly active atomically dispersed NiN4Cl sites by Cl‐doping for CO2 electroreduction |
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| المؤلفون: | Zhao Li, Xueqiang Qi, Junjie Wang, Zhaozhao Zhu, Jinxia Jiang, Xiaobin Niu, Andreu Cabot, Jun Song Chen, Rui Wu |
| المصدر: | SusMat, Vol 3, Iss 4, Pp 498-509 (2023) |
| بيانات النشر: | Wiley, 2023. |
| سنة النشر: | 2023 |
| المجموعة: | LCC:Materials of engineering and construction. Mechanics of materials LCC:Environmental engineering |
| مصطلحات موضوعية: | atomically dispersed catalyst, chlorine‐doped carbon, electrocatalytic CO2 reduction, NiN4Cl sites, zinc‐CO2 battery, Materials of engineering and construction. Mechanics of materials, TA401-492, Environmental engineering, TA170-171 |
| الوصف: | Abstract Nickel‐nitrogen‐carbon single‐atom catalysts have attracted widespread interest for CO2 electroreduction but they suffer from poor stability. Herein, we report on the preparation of Cl‐ and N‐doped porous carbon nanosheets with atomically dispersed NiN4Cl active sites (NiN4Cl‐ClNC) through a molten‐salt‐assisted pyrolysis strategy. The optimized NiN4Cl‐ClNC catalyst delivers exceptional CO2 conversion activity with outstanding stability for over 220 h at −0.7 V versus RHE and a high CO Faradaic efficiency of 98.7% at a CO partial current density of 12.4 mA cm‒2. Moreover, NiN4Cl‐ClNC displays a remarkable CO partial current density of approximately 349.4 mA cm−2 in flow‐cell, meeting the requirements of industrial applications. Operando attenuated total reflectance surface‐enhanced infrared absorption spectroscopy and density functional theory calculations are used to understand the outstanding activity and stability. Results reveal that the introduced axial Ni‐Cl bond on the Ni center and Cl─C bond on the carbon support synergetically induce electronic delocalization, which not only stabilizes Ni against leaching but also facilitates the formation of the COOH* intermediate that is found to be the rate‐determining step. |
| نوع الوثيقة: | article |
| وصف الملف: | electronic resource |
| اللغة: | English |
| تدمد: | 2692-4552 |
| العلاقة: | https://doaj.org/toc/2692-4552Test |
| DOI: | 10.1002/sus2.148 |
| الوصول الحر: | https://doaj.org/article/ee25ed4283d8451799523c5676ddc4e2Test |
| رقم الانضمام: | edsdoj.25ed4283d8451799523c5676ddc4e2 |
| قاعدة البيانات: | Directory of Open Access Journals |
Full Text Finder | تدمد: | 26924552 |
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| DOI: | 10.1002/sus2.148 |