镍
酞菁
电化学
材料科学
超分子化学
可逆氢电极
电解质
催化作用
法拉第效率
纳米技术
电流密度
碳纳米管
无机化学
分子
化学工程
电极
化学
冶金
有机化学
工作电极
物理化学
物理
量子力学
工程类
作者
Yucheng Jin,Xiaoning Zhan,Yingting Zheng,Hailong Wang,Xiaolin Liu,Baoqiu Yu,Dongdong Xu,Tianyu Zheng,Kang Wang,Dongdong Qi,Jianzhuang Jiang
标识
DOI:10.1016/j.apcatb.2023.122446
摘要
Heterogeneous catalysts made up of molecule-based catalysts on conductive substrates enable the large current density, high selectivity, and easy operation for carbon dioxide reduction reaction towards the practical use. Herein, we report a hydrogen-bonded supramolecular structure (1) assembled from asymmetric A3B-type nickel phthalocyanine NiPc(OH)6(DCNFO), which is afforded via solvothermal reaction of 2,3,9,10,16,17,23,24-octahydroxyl-phthalocyaninato nickel with tetrafluoroterephthalene. Single crystal X-ray diffraction analysis reveals the one-dimensional supramolecular ribbons of 1 formed from individual modules via hydrogen-bond between the hydroxyl groups, showing good solution resistance due mainly to the additional strong π-π interactions. Nevertheless, in-situ growing 1 on carbon nanotubes generates a phthalocyanine-based composite for gas diffusion electrode, displaying the highly selective conversion of CO2 to CO with Faradaic efficiency > 98% at a wide voltage range from − 0.5 to − 1.2 V versus reversible hydrogen electrode, a high current density of 353 mA cm−2 at − 1.2 V, and stable cycling at 150 mA cm−2 for 40 h in 0.5 M KHCO3 electrolyte. Employment of 1.0 M KOH results in a further improved current density of 620 mA cm−2 at − 1.2 V and higher stable cycling current density of 230 mA cm−2 for 40 h.
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