酞菁
电催化剂
镍
金属有机骨架
材料科学
法拉第效率
催化作用
密度泛函理论
无机化学
化学工程
吸附
电极
电化学
化学
纳米技术
物理化学
电解质
有机化学
计算化学
冶金
工程类
作者
Meng‐Di Zhang,Duan‐Hui Si,Jun‐Dong Yi,Qi Yin,Yuan−Biao Huang,Rong Cao
标识
DOI:10.1007/s11426-021-1022-3
摘要
Porous crystalline metal-organic frameworks (MOFs) are one class of promising electrode materials for CO2 electroreduction reaction (CO2RR) by virtue of their large CO2 adsorption capacities and abundant tunable active sites, but their insulating nature usually leads to low current density. Herein, a two-dimensional (2D) Ni-phthalocyanine-based MOF (NiPc-Ni(NH)4) constructed by 2,3,9,10,16,17,23,24-octaaminophthalocyaninato nickel(II) (NiPc-(NH2)8) and nickel(II) ions attained high electrical conductivity due to the high overlap of d-π conjugation orbitals between the nickel node and the Ni-phthalocyanine-substituted o-phenylenediamine. During CO2RR, the NiPc-Ni(NH)4 nanosheets achieved a high CO Faradaic efficiency of 96.4% at −0.7 V and a large CO partial current density of 24.8 mA cm−2 at −1.1 V, which surpassed all the reported two-dimensional MOF electrocatalysts evaluated in an H-cell. The control experiments and density functional theory (DFT) calculations suggested that the Ni-N4 units of the phthalocyanine ring are the catalytic active sites. This work provides a new route to the design of highly efficient porous framework materials for the enhanced electrocatalysis via improving electrical conductivity.
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