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

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

doi:10.1038/s41565-019-0603-y

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

Journal Article · 06 January 2020 · Nature Nanotechnology

DOI: https://doi.org/10.1038/s41565-019-0603-y · OSTI ID:1605382

^[1]; Tzeng, Yan-Kai ^[2]; Ji, Yongfei ^[3]; Li, Yanbin ^[4]; Li, Jun ^[4];

^[4];

^[4]; Gong, Yongji ^[4]; Cai, Lili ^[4];

^[4]; Zhang, Xiaokun ^[4]; Chen, Wei ^[4]; Liu, Bofei ^[4]; Lu, Haiyu ^[2];

^[5];

^[6];

^[3]; Tan, Tianwei ^[7]; Chu, Steven ^[8] more »

Stanford Univ., CA (United States). Dept. of Materials Science and Engineering; Beijing Univ. of Chemical Technology (China)
Stanford Univ., CA (United States). Dept. of Physics
Stanford Univ., CA (United States). SUNCAT Center for Interface Science and Catalysis
Stanford Univ., CA (United States). Dept. of Materials Science and Engineering
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)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)
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
Stanford Univ., CA (United States). Dept. of Physics and Dept. of Molecular and Cellular Physiology
SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., CA (United States). Dept. of Materials Science and Engineering

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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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1605382

Journal Information:: Nature Nanotechnology, Journal Name: Nature Nanotechnology Journal Issue: 2 Vol. 15; ISSN 1748-3387

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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