材料科学
纳米笼
铜
电解质
催化作用
电化学
法拉第效率
可逆氢电极
金属
无机化学
电极
冶金
物理化学
有机化学
工作电极
化学
作者
Jin‐Meng Heng,Haolin Zhu,Zhen‐Hua Zhao,Pei‐Qin Liao,Xiao‐Ming Chen
标识
DOI:10.1002/adma.202415101
摘要
Synthesis of high-loading atomic-level dispersed catalysts for highly efficient electrochemical CO2 reduction reaction (eCO2RR) to ethylene (C2H4) in neutral electrolyte remain challenging tasks. To address common aggregation issues, a host-guest strategy is employed, by using a metal-azolate framework (MAF-4) with nanocages as the host and a dinuclear Cu(I) complex as the guest, to form precursors for pyrolysis into a series of nitrogen-doped porous carbons (NPCs) with varying loadings of dual copper sites, namely NPCMAF-4-Cu2-21 (21.2 wt%), NPCMAF-4-Cu2-11 (10.6 wt%), and NPCMAF-4-Cu2-7 (6.9 wt%). Interestingly, as the loading of dual copper sites increased from 6.9 to 21.2 wt%, the partial current density for eCO2RR to yield C2H4 also gradually increased from 38.7 to 93.6 mA cm-2. In a 0.1 m KHCO3 electrolyte, at -1.4 V versus reversible hydrogen electrode (vs. RHE), NPCMAF-4-Cu2-21 exhibits the excellent performance with a Faradaic efficiency of 52% and a current density of 180 mA cm-2. Such performance can be attributed to the presence of ultrahigh-loading dual copper sites, which promotes C─C coupling and the formation of C2 products. The findings demonstrate the confinement effect of MAF-4 with nanocages is conducive to the preparation of high-loading atomic-level catalysts.
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