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Title: A Molecular Surface Functionalization Approach to Tuning Nanoparticle Electrocatalysts for Carbon Dioxide Reduction

Abstract

Conversion of the greenhouse gas carbon dioxide (CO2) to value-added products is an important challenge for sustainable energy research, and nanomaterials offer a broad class of heterogeneous catalysts for such transformations. Here we report a molecular surface functionalization approach to tuning gold nanoparticle (Au NP) electrocatalysts for reduction of CO2 to CO. The N-heterocyclic (NHC) carbene-functionalized Au NP catalyst exhibits improved faradaic efficiency (FE = 83%) for reduction of CO2 to CO in water at neutral pH at an overpotential of 0.46 V with a 7.6-fold increase in current density compared to that of the parent Au NP (FE = 53%). Tafel plots of the NHC carbene-functionalized Au NP (72 mV/decade) vs parent Au NP (138 mV/decade) systems further show that the molecular ligand influences mechanistic pathways for CO2 reduction. The results establish molecular surface functionalization as a complementary approach to size, shape, composition, and defect control for nanoparticle catalyst design.

Authors:
 [1];  [1];  [1];  [2];  [1];  [2];  [3];  [2];  [1];  [1];  [4];  [2]
  1. Univ. of California, Berkeley, CA (United States)
  2. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  3. Chinese Academy of Sciences, Shanxi (China); Synfuels China, Beijing (China)
  4. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Kavli Energy Nanosciences Institute, Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1466697
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 138; Journal Issue: 26; Related Information: © 2016 American Chemical Society.; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Cao, Zhi, Kim, Dohyung, Hong, Dachao, Yu, Yi, Xu, Jun, Lin, Song, Wen, Xiaodong, Nichols, Eva M., Jeong, Keunhong, Reimer, Jeffrey A., Yang, Peidong, and Chang, Christopher J.. A Molecular Surface Functionalization Approach to Tuning Nanoparticle Electrocatalysts for Carbon Dioxide Reduction. United States: N. p., 2016. Web. https://doi.org/10.1021/jacs.6b02878.
Cao, Zhi, Kim, Dohyung, Hong, Dachao, Yu, Yi, Xu, Jun, Lin, Song, Wen, Xiaodong, Nichols, Eva M., Jeong, Keunhong, Reimer, Jeffrey A., Yang, Peidong, & Chang, Christopher J.. A Molecular Surface Functionalization Approach to Tuning Nanoparticle Electrocatalysts for Carbon Dioxide Reduction. United States. https://doi.org/10.1021/jacs.6b02878
Cao, Zhi, Kim, Dohyung, Hong, Dachao, Yu, Yi, Xu, Jun, Lin, Song, Wen, Xiaodong, Nichols, Eva M., Jeong, Keunhong, Reimer, Jeffrey A., Yang, Peidong, and Chang, Christopher J.. Mon . "A Molecular Surface Functionalization Approach to Tuning Nanoparticle Electrocatalysts for Carbon Dioxide Reduction". United States. https://doi.org/10.1021/jacs.6b02878. https://www.osti.gov/servlets/purl/1466697.
@article{osti_1466697,
title = {A Molecular Surface Functionalization Approach to Tuning Nanoparticle Electrocatalysts for Carbon Dioxide Reduction},
author = {Cao, Zhi and Kim, Dohyung and Hong, Dachao and Yu, Yi and Xu, Jun and Lin, Song and Wen, Xiaodong and Nichols, Eva M. and Jeong, Keunhong and Reimer, Jeffrey A. and Yang, Peidong and Chang, Christopher J.},
abstractNote = {Conversion of the greenhouse gas carbon dioxide (CO2) to value-added products is an important challenge for sustainable energy research, and nanomaterials offer a broad class of heterogeneous catalysts for such transformations. Here we report a molecular surface functionalization approach to tuning gold nanoparticle (Au NP) electrocatalysts for reduction of CO2 to CO. The N-heterocyclic (NHC) carbene-functionalized Au NP catalyst exhibits improved faradaic efficiency (FE = 83%) for reduction of CO2 to CO in water at neutral pH at an overpotential of 0.46 V with a 7.6-fold increase in current density compared to that of the parent Au NP (FE = 53%). Tafel plots of the NHC carbene-functionalized Au NP (72 mV/decade) vs parent Au NP (138 mV/decade) systems further show that the molecular ligand influences mechanistic pathways for CO2 reduction. The results establish molecular surface functionalization as a complementary approach to size, shape, composition, and defect control for nanoparticle catalyst design.},
doi = {10.1021/jacs.6b02878},
journal = {Journal of the American Chemical Society},
number = 26,
volume = 138,
place = {United States},
year = {2016},
month = {6}
}

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    Electrochemical CO 2 reduction in confined space: Enhanced activity of metal catalysts by graphene overlayer
    journal, November 2019

    • Lin, Zheng‐Zhe; Chen, Xi; Yin, Cong
    • International Journal of Energy Research, Vol. 44, Issue 2
    • DOI: 10.1002/er.4888

    New challenges of electrokinetic studies in investigating the reaction mechanism of electrochemical CO 2 reduction
    journal, January 2018

    • Lee, Chan Woo; Cho, Nam Heon; Im, Sang Won
    • Journal of Materials Chemistry A, Vol. 6, Issue 29
    • DOI: 10.1039/c8ta03480j

    The role of reticular chemistry in the design of CO2 reduction catalysts
    journal, February 2018


    Recent advances in the nanoengineering of electrocatalysts for CO 2 reduction
    journal, January 2018

    • Li, Fengwang; MacFarlane, Douglas R.; Zhang, Jie
    • Nanoscale, Vol. 10, Issue 14
    • DOI: 10.1039/c7nr09620h

    Water-soluble platinum nanoparticles stabilized by sulfonated N-heterocyclic carbenes: influence of the synthetic approach
    journal, January 2018

    • Baquero, Edwin A.; Tricard, Simon; Coppel, Yannick
    • Dalton Transactions, Vol. 47, Issue 12
    • DOI: 10.1039/c8dt00240a

    Current progress of metallic and carbon-based nanostructure catalysts towards the electrochemical reduction of CO 2
    journal, January 2019

    • Hou, Liang; Yan, Jingze; Takele, Leta
    • Inorganic Chemistry Frontiers, Vol. 6, Issue 12
    • DOI: 10.1039/c9qi00484j

    Recent Advances in Electrochemical CO 2 -to-CO Conversion on Heterogeneous Catalysts
    journal, August 2018

    • Zheng, Tingting; Jiang, Kun; Wang, Haotian
    • Advanced Materials, Vol. 30, Issue 48
    • DOI: 10.1002/adma.201802066

    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

    Highly Dispersive Gold Nanoparticles on Carbon Black for Oxygen and Carbon Dioxide Reduction
    journal, September 2018


    Ligand-mediated bifunctional catalysis for enhanced oxygen reduction and methanol oxidation tolerance in fuel cells
    journal, January 2018

    • Lu, Linfang; Wang, Zhiqiang; Zou, Shihui
    • Journal of Materials Chemistry A, Vol. 6, Issue 39
    • DOI: 10.1039/c8ta06071a

    Highly Efficient CO 2 Electroreduction on ZnN 4 -based Single-Atom Catalyst
    journal, August 2018


    Systematically Tuning the Electronic Structure of Gold Nanoclusters through Ligand Derivatization
    journal, July 2019

    • Cirri, Anthony; Morales Hernández, Hanna; Kmiotek, Christina
    • Angewandte Chemie, Vol. 131, Issue 39
    • DOI: 10.1002/ange.201907586

    Recent Advances in the Chemistry of N ‐Heterocyclic‐Carbene‐Functionalized Metal‐Nanoparticles and Their Applications
    journal, December 2018

    • An, Yuan‐Yuan; Yu, Jian‐Gang; Han, Ying‐Feng
    • Chinese Journal of Chemistry, Vol. 37, Issue 1
    • DOI: 10.1002/cjoc.201800450

    Robust gold nanorods stabilized by bidentate N-heterocyclic-carbene–thiolate ligands
    journal, November 2018


    Progress in catalyst exploration for heterogeneous CO 2 reduction and utilization: a critical review
    journal, January 2017

    • Zhao, Guixia; Huang, Xiubing; Wang, Xiangxue
    • J. Mater. Chem. A, Vol. 5, Issue 41
    • DOI: 10.1039/c7ta07290b

    Oxygen vacancy associated single-electron transfer for photofixation of CO2 to long-chain chemicals
    journal, February 2019


    Regulation of Coordination Number over Single Co Sites: Triggering the Efficient Electroreduction of CO 2
    journal, January 2018

    • Wang, Xiaoqian; Chen, Zhao; Zhao, Xuyan
    • Angewandte Chemie International Edition, Vol. 57, Issue 7
    • DOI: 10.1002/anie.201712451

    Reduced SnO 2 Porous Nanowires with a High Density of Grain Boundaries as Catalysts for Efficient Electrochemical CO 2 -into-HCOOH Conversion
    journal, February 2017

    • Kumar, Bijandra; Atla, Veerendra; Brian, J. Patrick
    • Angewandte Chemie, Vol. 129, Issue 13
    • DOI: 10.1002/ange.201612194

    Selective Electrochemical Reduction of Carbon Dioxide to Ethanol on a Boron- and Nitrogen-Co-doped Nanodiamond
    journal, October 2017


    Nanocrystal/Metal–Organic Framework Hybrids as Electrocatalytic Platforms for CO 2 Conversion
    journal, July 2019

    • Guntern, Yannick T.; Pankhurst, James R.; Vávra, Jan
    • Angewandte Chemie, Vol. 131, Issue 36
    • DOI: 10.1002/ange.201905172

    A Polymer Solution To Prevent Nanoclustering and Improve the Selectivity of Metal Nanoparticles for Electrocatalytic CO 2 Reduction
    journal, September 2019

    • Zhang, Lei; Wei, Zichao; Thanneeru, Srinivas
    • Angewandte Chemie, Vol. 131, Issue 44
    • DOI: 10.1002/ange.201909069

    A Benchtop Method for Appending Protic Functional Groups to N‐Heterocyclic Carbene Protected Gold Nanoparticles
    journal, March 2020

    • DeJesus, Joseph F.; Sherman, Lindy M.; Yohannan, Darius J.
    • Angewandte Chemie, Vol. 132, Issue 19
    • DOI: 10.1002/ange.202001440

    Tuning Gold Nanoparticles with Chelating Ligands for Highly Efficient Electrocatalytic CO 2 Reduction
    journal, August 2018

    • Cao, Zhi; Zacate, Samson B.; Sun, Xiaodong
    • Angewandte Chemie International Edition, Vol. 57, Issue 39
    • DOI: 10.1002/anie.201805696

    Systematically Tuning the Electronic Structure of Gold Nanoclusters through Ligand Derivatization
    journal, August 2019

    • Cirri, Anthony; Morales Hernández, Hanna; Kmiotek, Christina
    • Angewandte Chemie International Edition, Vol. 58, Issue 39
    • DOI: 10.1002/anie.201907586