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Molecular engineering of dispersed nickel phthalocyanines on carbon nanotubes for selective CO2 reduction

Journal Article · · Nature Energy
 [1];  [2];  [2];  [3];  [2];  [2];  [2];  [2];  [3];  [4];  [5];  [6];  [2];  [3];  [7];  [8];  [2]
  1. Southern University of Science and Technology, Shenzhen, Guangdong (China); Stanford Univ., CA (United States)
  2. Southern University of Science and Technology, Shenzhen, Guangdong (China)
  3. Oregon State Univ., Corvallis, OR (United States)
  4. Yale Univ., New Haven, CT (United States)
  5. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  6. Northwestern Univ., Evanston, IL (United States)
  7. Southern University of Science and Technology, Shenzhen, Guangdong (China); Tsinghua Univ., Beijing (China)
  8. Stanford Univ., CA (United States)
+ Show Author Affiliations
Electrochemical reduction of CO2 is a promising route for sustainable production of fuels. A grand challenge is developing low-cost and efficient electrocatalysts that can enable rapid conversion with high product selectivity. Here we design a series of nickel phthalocyanine molecules supported on carbon nanotubes as molecularly dispersed electrocatalysts (MDEs), achieving CO2 reduction performances that are superior to aggregated molecular catalysts in terms of stability, activity and selectivity. The optimized MDE with methoxy group functionalization solves the stability issue of the original nickel phthalocyanine catalyst and catalyses the conversion of CO2 to CO with >99.5% selectivity at high current densities of up to -300 mA cm-2 in a gas diffusion electrode device with stable operation at -150 mA cm-2 for 40 h. The well-defined active sites of MDEs also facilitate the in-depth mechanistic understandings from in situ/operando X-ray absorption spectroscopy and theoretical calculations on structural factors that affect electrocatalytic performance.
Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
National Natural Science Foundation of China (NSFC); National Science Foundation (NSF); USDOE Office of Science (SC)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1774346
Journal Information:
Nature Energy, Journal Name: Nature Energy Journal Issue: 9 Vol. 5; ISSN 2058-7546
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

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