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Title: Synergistic enhancement of electrocatalytic CO2 reduction to C2 oxygenates at nitrogen-doped nanodiamonds/Cu interface

Abstract

To date, effective control over the electrochemical reduction of CO2 to multicarbon products (C ≥ 2) has been very challenging. Here, we report a design principle for the creation of a selective yet robust catalytic interface for heterogeneous electrocatalysts in the reduction of CO2 to C2 oxygenates, demonstrated by rational tuning of an assembly of nitrogen-doped nanodiamonds and copper nanoparticles. The catalyst exhibits a Faradaic efficiency of ~63% towards C2 oxygenates at applied potentials of only -0.5 V versus reversible hydrogen electrode. Moreover, this catalyst shows an unprecedented persistent catalytic performance up to 120 h, with steady current and only 19% activity decay. Density functional theory calculations show that CO binding is strengthened at the copper/nanodiamond interface, suppressing CO desorption and promoting C2 production by lowering the apparent barrier for CO dimerization. The inherent compositional and electronic tunability of the catalyst assembly offers an unrivalled degree of control over the catalytic interface, and thereby the reaction energetics and kinetics.

Authors:
ORCiD logo [1];  [2];  [3];  [4];  [4]; ORCiD logo [4]; ORCiD logo [4]; ORCiD logo [4];  [4];  [4]; ORCiD logo [4];  [4];  [4];  [4];  [2]; ORCiD logo [5]; ORCiD logo [6]; ORCiD logo [3];  [7];  [8] more »; ORCiD logo [9] « less
  1. Stanford Univ., CA (United States). Dept. of Materials Science and Engineering; Beijing Univ. of Chemical Technology (China)
  2. Stanford Univ., CA (United States). Dept. of Physics
  3. Stanford Univ., CA (United States). SUNCAT Center for Interface Science and Catalysis
  4. Stanford Univ., CA (United States). Dept. of Materials Science and Engineering
  5. Stanford Univ., CA (United States). Dept. of Materials Science and Engineering; SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)
  6. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)
  7. Beijing Univ. of Chemical Technology (China). Beijing Advanced Innovation Center for Soft Matter Science and Engineering; Beijing Univ. of Chemical Technology (China). National Energy R&D Center for Biorefinery
  8. Stanford Univ., CA (United States). Dept. of Physics and Dept. of Molecular and Cellular Physiology
  9. SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., CA (United States). Dept. of Materials Science and Engineering
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1605382
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Nature Nanotechnology
Additional Journal Information:
Journal Volume: 15; Journal Issue: 2; Journal ID: ISSN 1748-3387
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Wang, Hongxia, Tzeng, Yan-Kai, Ji, Yongfei, Li, Yanbin, Li, Jun, Zheng, Xueli, Yang, Ankun, Liu, Yayuan, Gong, Yongji, Cai, Lili, Li, Yuzhang, Zhang, Xiaokun, Chen, Wei, Liu, Bofei, Lu, Haiyu, Melosh, Nicholas A., Shen, Zhi-Xun, Chan, Karen, Tan, Tianwei, Chu, Steven, and Cui, Yi. Synergistic enhancement of electrocatalytic CO2 reduction to C2 oxygenates at nitrogen-doped nanodiamonds/Cu interface. United States: N. p., 2020. Web. doi:10.1038/s41565-019-0603-y.
Wang, Hongxia, Tzeng, Yan-Kai, Ji, Yongfei, Li, Yanbin, Li, Jun, Zheng, Xueli, Yang, Ankun, Liu, Yayuan, Gong, Yongji, Cai, Lili, Li, Yuzhang, Zhang, Xiaokun, Chen, Wei, Liu, Bofei, Lu, Haiyu, Melosh, Nicholas A., Shen, Zhi-Xun, Chan, Karen, Tan, Tianwei, Chu, Steven, & Cui, Yi. Synergistic enhancement of electrocatalytic CO2 reduction to C2 oxygenates at nitrogen-doped nanodiamonds/Cu interface. United States. https://doi.org/10.1038/s41565-019-0603-y
Wang, Hongxia, Tzeng, Yan-Kai, Ji, Yongfei, Li, Yanbin, Li, Jun, Zheng, Xueli, Yang, Ankun, Liu, Yayuan, Gong, Yongji, Cai, Lili, Li, Yuzhang, Zhang, Xiaokun, Chen, Wei, Liu, Bofei, Lu, Haiyu, Melosh, Nicholas A., Shen, Zhi-Xun, Chan, Karen, Tan, Tianwei, Chu, Steven, and Cui, Yi. Mon . "Synergistic enhancement of electrocatalytic CO2 reduction to C2 oxygenates at nitrogen-doped nanodiamonds/Cu interface". United States. https://doi.org/10.1038/s41565-019-0603-y. https://www.osti.gov/servlets/purl/1605382.
@article{osti_1605382,
title = {Synergistic enhancement of electrocatalytic CO2 reduction to C2 oxygenates at nitrogen-doped nanodiamonds/Cu interface},
author = {Wang, Hongxia and Tzeng, Yan-Kai and Ji, Yongfei and Li, Yanbin and Li, Jun and Zheng, Xueli and Yang, Ankun and Liu, Yayuan and Gong, Yongji and Cai, Lili and Li, Yuzhang and Zhang, Xiaokun and Chen, Wei and Liu, Bofei and Lu, Haiyu and Melosh, Nicholas A. and Shen, Zhi-Xun and Chan, Karen and Tan, Tianwei and Chu, Steven and Cui, Yi},
abstractNote = {To date, effective control over the electrochemical reduction of CO2 to multicarbon products (C ≥ 2) has been very challenging. Here, we report a design principle for the creation of a selective yet robust catalytic interface for heterogeneous electrocatalysts in the reduction of CO2 to C2 oxygenates, demonstrated by rational tuning of an assembly of nitrogen-doped nanodiamonds and copper nanoparticles. The catalyst exhibits a Faradaic efficiency of ~63% towards C2 oxygenates at applied potentials of only -0.5 V versus reversible hydrogen electrode. Moreover, this catalyst shows an unprecedented persistent catalytic performance up to 120 h, with steady current and only 19% activity decay. Density functional theory calculations show that CO binding is strengthened at the copper/nanodiamond interface, suppressing CO desorption and promoting C2 production by lowering the apparent barrier for CO dimerization. The inherent compositional and electronic tunability of the catalyst assembly offers an unrivalled degree of control over the catalytic interface, and thereby the reaction energetics and kinetics.},
doi = {10.1038/s41565-019-0603-y},
journal = {Nature Nanotechnology},
number = 2,
volume = 15,
place = {United States},
year = {Mon Jan 06 00:00:00 EST 2020},
month = {Mon Jan 06 00:00:00 EST 2020}
}

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