Structural defects on converted bismuth oxide nanotubes enable highly active electrocatalysis of carbon dioxide reduction

Gong, Qiufang; Ding, Pan; Xu, Mingquan; Zhu, Xiaorong; Wang, Maoyu; Deng, Jun; Ma, Qing; Han, Na; Zhu, Yong; Lu, Jun; Feng, Zhenxing; Li, Yafei; Zhou, Wu; Li, Yanguang

doi:10.1038/s41467-019-10819-4

Title: Structural defects on converted bismuth oxide nanotubes enable highly active electrocatalysis of carbon dioxide reduction

Journal Article · Wed Jun 26 00:00:00 EDT 2019 · Nature Communications

DOI:https://doi.org/10.1038/s41467-019-10819-4· OSTI ID:1559554

Gong, Qiufang ^[1]; Ding, Pan ^[1]; Xu, Mingquan ^[2]; Zhu, Xiaorong ^[3]; Wang, Maoyu ^[4]; Deng, Jun ^[1]; Ma, Qing ^[5]; Han, Na ^[1]; Zhu, Yong ^[2];

^[6];

^[4]; Li, Yafei ^[3]; Zhou, Wu ^[2]; Li, Yanguang ^[1]

Soochow Univ., Suzhou (China)
Chinese Academy of Sciences (CAS), Beijing (China)
Nanjing Univ. (China)
Oregon State Univ., Corvallis, OR (United States)
Northwestern Univ., Evanston, IL (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)

Formic acid (or formate) is suggested to be one of the most economically viable products from electrochemical carbon dioxide reduction. However, its commercial viability hinges on the development of highly active and selective electrocatalysts. Here we report that structural defects have a profound positive impact on the electrocatalytic performance of bismuth. Bismuth oxide double-walled nanotubes with fragmented surface are prepared as a template, and are cathodically converted to defective bismuth nanotubes. This converted electrocatalyst enables carbon dioxide reduction to formate with excellent activity, selectivity and stability. Most significantly, its current density reaches ~288 mA cm^-2 at -0.61 V versus reversible hydrogen electrode within a flow cell reactor under ambient conditions. Using density functional theory calculations, the excellent activity and selectivity are rationalized as the outcome of abundant defective bismuth sites that stabilize the *OCHO intermediate. Furthermore, this electrocatalyst is coupled with silicon photocathodes and achieves high-performance photoelectrochemical carbon dioxide reduction.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: Ministry of Science and Technology of the People's Republic of China; National Natural Science Foundation of China (NSFC); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1559554

Journal Information:: Nature Communications, Vol. 10, Issue 1; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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