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

Zhang, Xiao; Wang, Yang; Gu, Meng; Wang, Maoyu; Zhang, Zisheng; Pan, Weiying; Jiang, Zhan; Zheng, Hongzhi; Lucero, Marcos; Wang, Hailiang; Sterbinsky, George E.; Ma, Qing; Wang, Yang-Gang; Feng, Zhenxing; Li, Jun; Dai, Hongjie; Liang, Yongye

doi:10.1038/s41560-020-0667-9

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

Journal Article · Mon Aug 10 00:00:00 EDT 2020 · Nature Energy

DOI:https://doi.org/10.1038/s41560-020-0667-9· OSTI ID:1774346

Zhang, Xiao ^[1]; Wang, Yang ^[2];

^[2]; Wang, Maoyu ^[3]; Zhang, Zisheng ^[2]; Pan, Weiying ^[2]; Jiang, Zhan ^[2]; Zheng, Hongzhi ^[2];

^[3];

^[4]; Sterbinsky, George E. ^[5]; Ma, Qing ^[6];

^[2];

^[3]; Li, Jun ^[7];

^[8];

^[2]

Southern University of Science and Technology, Shenzhen, Guangdong (China); Stanford Univ., CA (United States)
Southern University of Science and Technology, Shenzhen, Guangdong (China)
Oregon State Univ., Corvallis, OR (United States)
Yale Univ., New Haven, CT (United States)
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Northwestern Univ., Evanston, IL (United States)
Southern University of Science and Technology, Shenzhen, Guangdong (China); Tsinghua Univ., Beijing (China)
Stanford Univ., CA (United States)

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.

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC); National Natural Science Foundation of China (NSFC); National Science Foundation (NSF)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1774346

Journal Information:: Nature Energy, Vol. 5, Issue 9; ISSN 2058-7546

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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