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Title: Active sites of copper-complex catalytic materials for electrochemical carbon dioxide reduction

Abstract

Restructuring-induced catalytic activity is an intriguing phenomenon of fundamental importance to rational design of high-performance catalyst materials. We study three coppercomplex materials for electrocatalytic carbon dioxide reduction. Among them, the copper(II) phthalocyanine exhibits by far the highest activity for yielding methane with a Faradaic efficiency of 66% and a partial current density of 13 mA cm-2 at the potential of – 1.06 V versus the reversible hydrogen electrode. Utilizing in-situ and operando X-ray absorption spectroscopy, we find that under the working conditions copper(II) phthalocyanine undergoes reversible structural and oxidation state changes to form ~ 2 nm metallic copper clusters, which catalyzes the carbon dioxide-to-methane conversion. Density functional calculations rationalize the restructuring behavior and attribute the reversibility to the strong divalent metal ion–ligand coordination in the copper(II) phthalocyanine molecular structure and the small size of the generated copper clusters under the reaction conditions.

Authors:
ORCiD logo [1];  [2];  [3];  [2];  [2];  [4];  [5];  [6];  [2];  [2];  [7];  [3]; ORCiD logo [2]
  1. South University of Science and Technology of China, Shenzhen (China); Yale Univ., New Haven, CT (United States)
  2. Yale Univ., New Haven, CT (United States)
  3. Oregon State Univ., Corvallis, OR (United States)
  4. Yale Univ., New Haven, CT (United States); Shanghai University (China)
  5. University of South China, Hengyang, Hunan (China)
  6. Northwestern Univ., Evanston, IL (United States)
  7. South University of Science and Technology of China, Shenzhen (China)
Publication Date:
Research Org.:
Yale Univ., New Haven, CT (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; National Science Foundation (NSF)
OSTI Identifier:
1419868
Grant/Contract Number:  
FG02-07ER15909; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
ENGLISH
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE

Citation Formats

Weng, Zhe, Wu, Yueshen, Wang, Maoyu, Jiang, Jianbing, Yang, Ke, Huo, Shengjuan, Wang, Xiao-Feng, Ma, Qing, Brudvig, Gary W., Batista, Victor S., Liang, Yongye, Feng, Zhenxing, and Wang, Hailiang. Active sites of copper-complex catalytic materials for electrochemical carbon dioxide reduction. United States: N. p., 2018. Web. https://doi.org/10.1038/s41467-018-02819-7.
Weng, Zhe, Wu, Yueshen, Wang, Maoyu, Jiang, Jianbing, Yang, Ke, Huo, Shengjuan, Wang, Xiao-Feng, Ma, Qing, Brudvig, Gary W., Batista, Victor S., Liang, Yongye, Feng, Zhenxing, & Wang, Hailiang. Active sites of copper-complex catalytic materials for electrochemical carbon dioxide reduction. United States. https://doi.org/10.1038/s41467-018-02819-7
Weng, Zhe, Wu, Yueshen, Wang, Maoyu, Jiang, Jianbing, Yang, Ke, Huo, Shengjuan, Wang, Xiao-Feng, Ma, Qing, Brudvig, Gary W., Batista, Victor S., Liang, Yongye, Feng, Zhenxing, and Wang, Hailiang. Mon . "Active sites of copper-complex catalytic materials for electrochemical carbon dioxide reduction". United States. https://doi.org/10.1038/s41467-018-02819-7. https://www.osti.gov/servlets/purl/1419868.
@article{osti_1419868,
title = {Active sites of copper-complex catalytic materials for electrochemical carbon dioxide reduction},
author = {Weng, Zhe and Wu, Yueshen and Wang, Maoyu and Jiang, Jianbing and Yang, Ke and Huo, Shengjuan and Wang, Xiao-Feng and Ma, Qing and Brudvig, Gary W. and Batista, Victor S. and Liang, Yongye and Feng, Zhenxing and Wang, Hailiang},
abstractNote = {Restructuring-induced catalytic activity is an intriguing phenomenon of fundamental importance to rational design of high-performance catalyst materials. We study three coppercomplex materials for electrocatalytic carbon dioxide reduction. Among them, the copper(II) phthalocyanine exhibits by far the highest activity for yielding methane with a Faradaic efficiency of 66% and a partial current density of 13 mA cm-2 at the potential of – 1.06 V versus the reversible hydrogen electrode. Utilizing in-situ and operando X-ray absorption spectroscopy, we find that under the working conditions copper(II) phthalocyanine undergoes reversible structural and oxidation state changes to form ~ 2 nm metallic copper clusters, which catalyzes the carbon dioxide-to-methane conversion. Density functional calculations rationalize the restructuring behavior and attribute the reversibility to the strong divalent metal ion–ligand coordination in the copper(II) phthalocyanine molecular structure and the small size of the generated copper clusters under the reaction conditions.},
doi = {10.1038/s41467-018-02819-7},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {2018},
month = {1}
}

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Cited by: 137 works
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Figures / Tables:

Fig. 1 Fig. 1: Molecular structures of three Cu-complex materials and their electrocatalytic performance for CO2 reduction. Molecular structures of a CuPc, b HKUST-1, and c [Cu(cyclam)]Cl2. Potential-dependent d Faradaic efficiencies and e partial current densities of products for CO2 electroreduction reaction catalyzed by CuPc. Comparison of f Faradaic efficiency and gmore » partial current density distributions among CO2 electroreduction reactions catalyzed by the three materials at – 1.06 V vs RHE. Error bars represent the SD from multiple measurements« less

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    • Energy & Environmental Science, Vol. 12, Issue 9
    • DOI: 10.1039/c9ee01899a

    Electrocatalytic reduction of carbon dioxide: opportunities with heterogeneous molecular catalysts
    journal, January 2020

    • Sun, Libo; Reddu, Vikas; Fisher, Adrian C.
    • Energy & Environmental Science, Vol. 13, Issue 2
    • DOI: 10.1039/c9ee03660a

    Facile synthesis of polymerized cobalt phthalocyanines for highly efficient CO 2 reduction
    journal, January 2019

    • Chen, Jiacheng; Li, Jiayu; Liu, Weiliang
    • Green Chemistry, Vol. 21, Issue 22
    • DOI: 10.1039/c9gc02705j

    Engineering ultrasmall metal nanoclusters for photocatalytic and electrocatalytic applications
    journal, January 2019

    • Chai, Osburg Jin Huang; Liu, Zhihe; Chen, Tiankai
    • Nanoscale, Vol. 11, Issue 43
    • DOI: 10.1039/c9nr07272a

    Accelerated proton transmission in metal–organic frameworks for the efficient reduction of CO 2 in aqueous solutions
    journal, January 2019

    • Mao, Fangxin; Jin, Yan-Huan; Liu, Peng Fei
    • Journal of Materials Chemistry A, Vol. 7, Issue 40
    • DOI: 10.1039/c9ta07967j

    Current progress in electrocatalytic carbon dioxide reduction to fuels on heterogeneous catalysts
    journal, January 2020

    • Liu, Anmin; Gao, Mengfan; Ren, Xuefeng
    • Journal of Materials Chemistry A, Vol. 8, Issue 7
    • DOI: 10.1039/c9ta11966c

    The Impact of Different Si Surface Terminations in the (100) p-Si | n + -Si | Cu Junction with Respect to the Photo Electrochemical Performance
    journal, January 2019

    • Steinert, Céline; Tengeler, Sven; Kaiser, Bernhard
    • Journal of The Electrochemical Society, Vol. 166, Issue 5
    • DOI: 10.1149/2.0291905jes

    Emerging Carbon‐Based Heterogeneous Catalysts for Electrochemical Reduction of Carbon Dioxide into Value‐Added Chemicals
    journal, December 2018


    Copper and Copper-Based Bimetallic Catalysts for Carbon Dioxide Electroreduction
    journal, October 2018

    • Birhanu, Mulatu Kassie; Tsai, Meng-Che; Kahsay, Amaha Woldu
    • Advanced Materials Interfaces, Vol. 5, Issue 24
    • DOI: 10.1002/admi.201800919

    Molecular Evidence for Metallic Cobalt Boosting CO 2 Electroreduction on Pyridinic Nitrogen
    journal, February 2020


    Introducing Fe 2+ into Nickel-Iron Layered Double Hydroxide: Local Structure Modulated Water Oxidation Activity
    journal, June 2018

    • Cai, Zhao; Zhou, Daojin; Wang, Maoyu
    • Angewandte Chemie International Edition, Vol. 57, Issue 30
    • DOI: 10.1002/anie.201804881

    Identification of single-atom active sites in carbon-based cobalt catalysts during electrocatalytic hydrogen evolution
    journal, December 2018


    From CO 2 methanation to ambitious long-chain hydrocarbons: alternative fuels paving the path to sustainability
    journal, January 2019

    • Marques Mota, Filipe; Kim, Dong Ha
    • Chemical Society Reviews, Vol. 48, Issue 1
    • DOI: 10.1039/c8cs00527c

    Highly efficient electroconversion of carbon dioxide into hydrocarbons by cathodized copper–organic frameworks
    journal, January 2019

    • Yang, Fan; Chen, Aling; Deng, Pei Lin
    • Chemical Science, Vol. 10, Issue 34
    • DOI: 10.1039/c9sc02605c

    Ultrafast X-ray Absorption Studies of the Structural Dynamics of Molecular and Biological Systems in Solution
    journal, May 2011

    • Milne, Christopher J.; Van der Veen, Renske M.; Pham, Van-Thai
    • CHIMIA International Journal for Chemistry, Vol. 65, Issue 5
    • DOI: 10.2533/chimia.2011.303

      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.