过电位
共价键
催化作用
材料科学
密度泛函理论
X射线吸收光谱法
共价有机骨架
碳纤维
单体
化学工程
纳米技术
吸收光谱法
化学
电化学
有机化学
聚合物
物理化学
电极
计算化学
物理
量子力学
工程类
复合材料
复合数
作者
Lipeng Zhai,Shuai Yang,Chenbao Lu,Cheng‐Xing Cui,Qing Xu,Jing Liu,Xiubei Yang,Xutong Meng,Siyu Lu,Xiaodong Zhuang,Gaofeng Zeng,Zheng Jiang
出处
期刊:Small
[Wiley]
日期:2022-07-10
卷期号:18 (32)
被引量:18
标识
DOI:10.1002/smll.202200736
摘要
Developing effective electrocatalysts for CO2 reduction (CO2 RR) is of critical importance for producing carbon-neutral fuels. Covalent organic frameworks (COFs) are an ideal platform for constructing catalysts toward CO2 RR, because of their controllable skeletons and ordered pores. However, most of these COFs are synthesized from Co-porphyrins or phthalocyanines-based monomers, and the available building units and resulting catalytic centers in COFs are still limited. Herein, Co-N5 sites are first developed through anchoring Co porphyrins on an olefin-linked COF, where the Co active sites are uniformly distributed in the hexagonal networks. The strong electronic coupling between Co porphyrins and COF is disclosed by various characterizations such as X-ray absorption spectroscopy (XAS) and density functional theory calculation (DFT). Thanks to the CoN5 sites, the catalytic COF shows remarkable catalytic activity with Faraday efficiencies (FECO ) of 84.2-94.3% at applied potentials between -0.50 and -0.80 V (vs RHE), and achieves a turnover frequency of 4578 h-1 at -1.0 V. Moreover, the theoretical calculation further reveals that the CoN5 sites enable a decrease in the overpotential for the formation COOH*. This work provides a design strategy to employ COFs as scaffold for fabricating efficient CO2 electrocatalysts.
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