Mediating Heterogenized Nickel Phthalocyanine into Isolated Ni-N3 Moiety for Improving Activity and Stability of Electrocatalytic CO2 Reduction
Social Science Research Network(2022)
摘要
The poor stability of heterogenized nickel phthalocyanine (NiPc) has hindered its application as a desirable catalyst for electrocatalytic carbon dioxide reduction. Herein, the electrocatalytic stability of heterogenized NiPc on nitrogen-doped hollow carbon nanospheres (NiPc@NHCSs) can be optimized via mediating NiPc into Ni-NC moiety (Ni-NC/NHCSs-Y) to construct a stable Ni catalytic unit. Different from the poor activity of NiPc@NHCSs (CO Faradaic efficiency, FECO< 80%, stability < 1200 s), the optimal catalyst (Ni-NC/NHCSs-600) with unsat-urated Ni-N3 nitrogen-vacancy structure, displays FECO of 98.57% and CO turnover frequency of 3.75 s-1 at -0.87 V vs. RHE, and stable operation over 14 h (-0.82 V vs. RHE). The stabilization mechanism and the temperature effect on the structure-activity relationship are systematically explored, which successfully steers the design of stable Ni-NC catalytic unit on different carbon substrate, while a zinc-CO2 rechargeable battery is constructed, displaying a peak power density of 0.64 mW cm-2 and FECO of 91.45%.
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关键词
Electrocatalytic CO < sub > 2 <,sub > reduction,Nickel phthalocyanine,Monoatomic Ni catalyst,Zn-CO < sub > 2 <,sub > battery,UnsaturatedNi-N < sub > 3 <,sub > moiety
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