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Nitrogen fixation by Ru single-atom electrocatalytic reduction
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Tao, Hengcong, Choi, Changhyeok, Ding, Liang-Xin, Jiang, Zheng, Han, Zishan, Jia, Mingwen, Fan, Qun, Gao, Yunnan, Wang, Haihui, Robertson, Alex W., Hong, Song, Jung, Yousung, Liu, Shizhen and Sun, Zhenyu (2019) Nitrogen fixation by Ru single-atom electrocatalytic reduction. Chem, 5 (1). pp. 204-214. doi:10.1016/j.chempr.2018.10.007 ISSN 24519294.
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Official URL: http://dx.doi.org/10.1016/j.chempr.2018.10.007
Abstract
Nitrogen fixation under ambient conditions remains a significant challenge. Here, we report nitrogen fixation by Ru single-atom electrocatalytic reduction at room temperature and pressure. In contrast to Ru nanoparticles, single Ru sites supported on N-doped porous carbon greatly promoted electroreduction of aqueous N2 selectively to NH3, affording an NH3 formation rate of 3.665 mgNH3h−1mg−1Ru at −0.21 V versus the reversible hydrogen electrode. Importantly, the addition of ZrO2 was found to significantly suppress the competitive hydrogen evolution reaction. An NH3 faradic efficiency of about 21% was achieved at a low overpotential (0.17 V), surpassing many other reported catalysts. Experiments combined with density functional theory calculations showed that the Ru sites with oxygen vacancies were major active centers that permitted stabilization of *NNH, destabilization of *H, and enhanced N2 adsorption. We envision that optimization of ZrO2 loading could further facilitate electroreduction of N2 at both high NH3 synthesis rate and faradic efficiency.
Item Type: | Journal Article | ||||||||||
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Divisions: | Faculty of Science, Engineering and Medicine > Science > Physics | ||||||||||
Journal or Publication Title: | Chem | ||||||||||
Publisher: | CellPress | ||||||||||
ISSN: | 24519294 | ||||||||||
Official Date: | 10 January 2019 | ||||||||||
Dates: |
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Volume: | 5 | ||||||||||
Number: | 1 | ||||||||||
Page Range: | pp. 204-214 | ||||||||||
DOI: | 10.1016/j.chempr.2018.10.007 | ||||||||||
Status: | Peer Reviewed | ||||||||||
Publication Status: | Published | ||||||||||
Access rights to Published version: | Restricted or Subscription Access | ||||||||||
Copyright Holders: | Elsevier Inc. | ||||||||||
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