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

Hongxia Wang^#^{1

2}, Yan-Kai Tzeng^#³, Yongfei Ji^#⁴, Yanbin Li¹, Jun Li¹, Xueli Zheng¹, Ankun Yang¹, Yayuan Liu¹, Yongji Gong¹, Lili Cai¹, Yuzhang Li¹, Xiaokun Zhang¹, Wei Chen¹, Bofei Liu¹, Haiyu Lu³, Nicholas A Melosh^{1

5}, Zhi-Xun Shen^{3

5}, Karen Chan⁶, Tianwei Tan^{7

8}, Steven Chu^{9

10}, Yi Cui^{11

12}

Affiliations

¹ Department of Materials Science and Engineering, Stanford University, Stanford, CA, USA.
² Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, China.
³ Department of Physics, Stanford University, Stanford, CA, USA.
⁴ SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, CA, USA.
⁵ Stanford Institute for Materials and Energy Science, SLAC National Accelerator Laboratory, Menlo Park, CA, USA.
⁶ SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, CA, USA. kchan@fysik.dtu.dk.
⁷ Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, China. twtan@mail.buct.edu.cn.
⁸ National Energy R&D Center for Biorefinery, Beijing University of Chemical Technology, Beijing, China. twtan@mail.buct.edu.cn.
⁹ Department of Physics, Stanford University, Stanford, CA, USA. schu@stanford.edu.
¹⁰ Department of Molecular and Cellular Physiology, Stanford University, Stanford, CA, USA. schu@stanford.edu.
¹¹ Department of Materials Science and Engineering, Stanford University, Stanford, CA, USA. yicui@stanford.edu.
¹² Stanford Institute for Materials and Energy Science, SLAC National Accelerator Laboratory, Menlo Park, CA, USA. yicui@stanford.edu.

^# Contributed equally.

PMID: 31907442
DOI: 10.1038/s41565-019-0603-y

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

Hongxia Wang et al. Nat Nanotechnol. 2020 Feb.

. 2020 Feb;15(2):131-137.

doi: 10.1038/s41565-019-0603-y. Epub 2020 Jan 6.

Authors

Affiliations

¹ Department of Materials Science and Engineering, Stanford University, Stanford, CA, USA.
² Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, China.
³ Department of Physics, Stanford University, Stanford, CA, USA.
⁴ SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, CA, USA.
⁵ Stanford Institute for Materials and Energy Science, SLAC National Accelerator Laboratory, Menlo Park, CA, USA.
⁶ SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, CA, USA. kchan@fysik.dtu.dk.
⁷ Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, China. twtan@mail.buct.edu.cn.
⁸ National Energy R&D Center for Biorefinery, Beijing University of Chemical Technology, Beijing, China. twtan@mail.buct.edu.cn.
⁹ Department of Physics, Stanford University, Stanford, CA, USA. schu@stanford.edu.
¹⁰ Department of Molecular and Cellular Physiology, Stanford University, Stanford, CA, USA. schu@stanford.edu.
¹¹ Department of Materials Science and Engineering, Stanford University, Stanford, CA, USA. yicui@stanford.edu.
¹² Stanford Institute for Materials and Energy Science, SLAC National Accelerator Laboratory, Menlo Park, CA, USA. yicui@stanford.edu.

^# Contributed equally.

PMID: 31907442
DOI: 10.1038/s41565-019-0603-y

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.

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References

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

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

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Abstract

References

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