Transition-Metal Single Atoms in a Graphene Shell as Active Centers for Highly Efficient Artificial Photosynthesis

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Transition-Metal Single Atoms in a Graphene Shell as Active Centers for Highly Efficient Artificial Photosynthesis

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Title: Transition-Metal Single Atoms in a Graphene Shell as Active Centers for Highly Efficient Artificial Photosynthesis
Author: Jiang, Kun; Siahrostami, Samira; Akey, Austin; Li, Yanbin; Lu, Zhiyi; Lattimer, Judith; Hu, Yongfeng; Stokes, Richard C.; Gangishetty, Mahesh; Chen, Guangxu; Zhou, Yawei; Hill, I. Winfield; Cai, Wen-Bin; Bell, David C.; Chan, Karen; Nørskov, Jens K.; Cui, Yi; Wang, Haotian

Note: Order does not necessarily reflect citation order of authors.

Citation: Jiang, Kun, Samira Siahrostami, Austin J. Akey, Yanbin Li, Zhiyi Lu, Judith Lattimer, Yongfeng Hu, et al. 2017. “Transition-Metal Single Atoms in a Graphene Shell as Active Centers for Highly Efficient Artificial Photosynthesis.” Chem (October). doi:10.1016/j.chempr.2017.09.014.
Access Status: This work is under embargo until 2018-10-20
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Abstract: Utilizing solar energy to fix carbon dioxide (CO2) with water into chemical fuels and oxygen, a mimic process of photosynthesis in nature, is becoming increasingly important but still challenged by the low selectivity and activity, especially in CO2 electrocatalytic reduction. Here
we report transition metal atoms coordinated in graphene shell as active centers for aqueous CO2 reduction to carbon monoxide (CO), with high Faradaic efficiencies over 90 % under significant currents up to ~ 60 mA/mg (12 mA/cm2). Three-dimensional atom probe tomography was employed to directly identify the single Ni atomic sites in graphene vacancies. Theoretical simulations suggest that compared to metallic Ni, the Ni atomic sites present significantly different electronic structures which facilitate CO2 to CO conversion and suppress the competing hydrogen evolution reaction dramatically.
Published Version: doi:10.1016/j.chempr.2017.09.014
Terms of Use: This article is made available under the terms and conditions applicable to Other Posted Material, as set forth at http://nrs.harvard.edu/urn-3:HUL.InstRepos:dash.current.terms-of-use#LAA
Citable link to this page: http://nrs.harvard.edu/urn-3:HUL.InstRepos:34306112
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