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Highly Selective and Active Electrochemical Reduction of CO2 to CO on a Polymeric Co(II) Phthalocyanine@Graphitic Carbon Nitride Nanosheet-Carbon Nanotube Composite.
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2020-09-16 , DOI: 10.1021/acs.inorgchem.0c01977
Ting-Ting Li 1 , Yan Mei 1 , Hongwei Li 1 , Jinjie Qian 2 , Miao Wu 1 , Yue-Qing Zheng 1
Affiliation  

The electrochemical reduction of CO2 using intermittent renewable electricity is an attractive strategy for producing value-added fuels and chemicals, but until now, it has been greatly hindered by the shortage of high-performance electrocatalysts. In this study, we have demonstrated a type of molecular-catalyst-based hybrid material by the polymerization of cobalt phthalocyanine (CoPc) on a three-dimensional (3D) g-C3N4 nanosheet–carbon nanotube support for the aqueous electrochemical reduction of CO2. The electrocatalytic results show that the obtained composite can selectively transform CO2 to CO with considerable Faradaic efficiency (FE) of 95 ± 1.8%, a turnover frequency of 4.9 ± 0.2 s–1, and excellent long-term stability over 24 h at −0.8 V vs the reversible hydrogen electrode (RHE). In comparison to the analogous hybrid electrocatalysts prepared by the drop-drying or dip-coating method, the polymeric form of the molecular catalyst immobilized on 3D carbonaceous materials with an interconnected network enlarges the electrochemically active surface area and enhances the structural and operational robustness.

中文翻译:

在聚合钴(II)酞菁@石墨氮化碳纳米片-碳纳米管复合材料上将CO2选择性高效地电化学还原为CO。

使用间歇性可再生电力对CO 2进行电化学还原是生产增值燃料和化学品的有吸引力的策略,但直到现在,由于高性能电催化剂的短缺,它一直受到很大的阻碍。在这项研究中,我们通过在三维(3D)gC 3 N 4纳米片–碳纳米管载体上聚合钴酞菁(CoPc)来证明一种基于分子催化剂的杂化材料,用于CO的水性电化学还原2。电催化结果表明,所获得的复合材料可以选择性地将CO 2转化为CO,具有相当高的法拉第效率(FE),为95±1.8%,周转频率为4.9±0.2 s –1与可逆氢电极(RHE)相比,在-0.8 V电压下24小时内具有出色的长期稳定性。与通过滴干或浸涂法制备的类似杂化电催化剂相比,固定在具有互连网络的3D碳质材料上的分子催化剂的聚合形式扩大了电化学活性表面积,并增强了结构和操作的坚固性。
更新日期:2020-09-16
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