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

Xiao Zhang, Yang Wang, Meng Gu, Maoyu Wang, Zisheng Zhang, Weiying Pan, Zhan Jiang, Hongzhi Zheng, Marcos Lucero, Hailiang Wang, George E. Sterbinsky, Qing Ma, Yang-Gang Wang (), Zhenxing Feng (), Jun Li, Hongjie Dai and Yongye Liang ()
Additional contact information
Xiao Zhang: Southern University of Science and Technology
Yang Wang: Southern University of Science and Technology
Meng Gu: Southern University of Science and Technology
Maoyu Wang: Oregon State University
Zisheng Zhang: Southern University of Science and Technology
Weiying Pan: Southern University of Science and Technology
Zhan Jiang: Southern University of Science and Technology
Hongzhi Zheng: Southern University of Science and Technology
Marcos Lucero: Oregon State University
Hailiang Wang: Yale University
George E. Sterbinsky: Argonne National Laboratory
Qing Ma: Northwestern University
Yang-Gang Wang: Southern University of Science and Technology
Zhenxing Feng: Oregon State University
Jun Li: Southern University of Science and Technology
Hongjie Dai: Stanford University
Yongye Liang: Southern University of Science and Technology

Nature Energy, 2020, vol. 5, issue 9, 684-692

Abstract: Abstract 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.

Date: 2020
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DOI: 10.1038/s41560-020-0667-9

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