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

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.

Authors:
 [1];  [2]; ORCiD logo [2];  [3];  [2];  [2];  [2];  [2]; ORCiD logo [3]; ORCiD logo [4];  [5];  [6]; ORCiD logo [2]; ORCiD logo [3];  [7]; ORCiD logo [8]; ORCiD logo [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)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC); National Natural Science Foundation of China (NSFC); National Science Foundation (NSF)
OSTI Identifier:
1774346
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Energy
Additional Journal Information:
Journal Volume: 5; Journal Issue: 9; Journal ID: ISSN 2058-7546
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
42 ENGINEERING

Citation Formats

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, and Liang, Yongye. Molecular engineering of dispersed nickel phthalocyanines on carbon nanotubes for selective CO2 reduction. United States: N. p., 2020. Web. doi:10.1038/s41560-020-0667-9.
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. Molecular engineering of dispersed nickel phthalocyanines on carbon nanotubes for selective CO2 reduction. United States. https://doi.org/10.1038/s41560-020-0667-9
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, and Liang, Yongye. 2020. "Molecular engineering of dispersed nickel phthalocyanines on carbon nanotubes for selective CO2 reduction". United States. https://doi.org/10.1038/s41560-020-0667-9. https://www.osti.gov/servlets/purl/1774346.
@article{osti_1774346,
title = {Molecular engineering of dispersed nickel phthalocyanines on carbon nanotubes for selective CO2 reduction},
author = {Zhang, Xiao and Wang, Yang and Gu, Meng and Wang, Maoyu and Zhang, Zisheng and Pan, Weiying and Jiang, Zhan and Zheng, Hongzhi and Lucero, Marcos and Wang, Hailiang and Sterbinsky, George E. and Ma, Qing and Wang, Yang-Gang and Feng, Zhenxing and Li, Jun and Dai, Hongjie and Liang, Yongye},
abstractNote = {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.},
doi = {10.1038/s41560-020-0667-9},
url = {https://www.osti.gov/biblio/1774346}, journal = {Nature Energy},
issn = {2058-7546},
number = 9,
volume = 5,
place = {United States},
year = {Mon Aug 10 00:00:00 EDT 2020},
month = {Mon Aug 10 00:00:00 EDT 2020}
}

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