nl9b03324_si_001.pdf (790.81 kB)
Cu3N Nanocubes for Selective Electrochemical Reduction of CO2 to Ethylene
journal contribution
posted on 2019-11-08, 14:44 authored by Zhouyang Yin, Chao Yu, Zhonglong Zhao, Xuefeng Guo, Mengqi Shen, Na Li, Michelle Muzzio, Junrui Li, Hu Liu, Honghong Lin, Jie Yin, Gang Lu, Dong Su, Shouheng SunUnderstanding
the Cu-catalyzed electrochemical CO2 reduction
reaction (CO2RR) under ambient conditions is both fundamentally
interesting and technologically important for selective CO2RR to hydrocarbons. Current Cu catalysts studied for the CO2RR can show high activity but tend to yield a mixture of different
hydrocarbons, posing a serious challenge on using any of these catalysts
for selective CO2RR. Here, we report a new perovskite-type
copper(I) nitride (Cu3N) nanocube (NC) catalyst for selective
CO2RR. The 25 nm Cu3N NCs show high CO2RR selectivity and stability to ethylene (C2H4) at −1.6 V (vs reversible hydrogen electrode (RHE)) with
the Faradaic efficiency of 60%, mass activity of 34 A/g, and C2H4/CH4 molar ratio of >2000. More
detailed
electrochemical characterization, X-ray photon spectroscopy,
and density functional theory calculations suggest that the high CO2RR selectivity is likely a result of (100) Cu(I) stabilization
by the Cu3N structure, which favors CO–CHO coupling
on the (100) Cu3N surface, leading to selective formation
of C2H4. Our study presents a good example of
utilizing metal nitrides as highly efficient nanocatalysts for selective
CO2RR to hydrocarbons that will be important for sustainable
chemistry/energy applications.
History
Usage metrics
Categories
Keywords
Cu 3 N structure25 nm Cu 3 N NCs showambient conditionsRHEC 2 H 4CO 2electrochemical characterization X-ray photon spectroscopyCu 3 N Nanocubeshydrogen electrodeCu 3 NCO 2 RRCHtheory calculationsCurrent Cu catalystsCO 2 RR selectivityFaradaic efficiencymetal nitridesCu-catalyzed electrochemical CO 2 reduction reactionSelective Electrochemical Reduction
Licence
Exports
RefWorks
BibTeX
Ref. manager
Endnote
DataCite
NLM
DC