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Engineering vacancy and hydrophobicity of two-dimensional TaTe2 for efficient and stable electrocatalytic N2 reduction
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Zhao, Zhenqing, Park, Jongseo, Choi, Changhyeok, Hong, Song, Hui, Xiangchao, Zhang, Hao, Benedict Lo, Tsz Woon, Robertson, Alex W., Lv, Zengxiang, Jung, Yousung and Sun, Zhenyu (2022) Engineering vacancy and hydrophobicity of two-dimensional TaTe2 for efficient and stable electrocatalytic N2 reduction. The Innovation, 3 (1). 100190. doi:10.1016/j.xinn.2021.100190 ISSN 2666-6758.
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Official URL: http://dx.doi.org/10.1016/j.xinn.2021.100190
Abstract
Demand for ammonia continues to increase to sustain the growing global population. The direct electrochemical N2 reduction reaction (NRR) powered by renewable electricity offers a promising carbon-neutral and sustainable strategy for manufacturing NH3, yet achieving this remains a grand challenge. Here, we report a synergistic strategy to promote ambient NRR for ammonia production by tuning the Te vacancies (VTe) and surface hydrophobicity of two-dimensional TaTe2 nanosheets. Remarkable NH3 faradic efficiency of up to 32.2% is attained at a mild overpotential, which is largely maintained even after 100 h of consecutive electrolysis. Isotopic labeling validates that the N atoms of formed NH4+ originate from N2. In situ X-ray diffraction indicates preservation of the crystalline structure of TaTe2 during NRR. Further density functional theory calculations reveal that the potential-determining step (PDS) is ∗NH2 + (H+ + e–) → NH3 on VTe-TaTe2 compared with that of ∗ + N2 + (H+ + e–) → ∗N–NH on TaTe2. We identify that the edge plane of TaTe2 and VTe serve as the main active sites for NRR. The free energy change at PDS on VTe-TaTe2 is comparable with the values at the top of the NRR volcano plots on various transition metal surfaces.
Item Type: | Journal Article | |||||||||||||||||||||
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Subjects: | Q Science > QD Chemistry | |||||||||||||||||||||
Divisions: | Faculty of Science, Engineering and Medicine > Science > Physics | |||||||||||||||||||||
Library of Congress Subject Headings (LCSH): | Transition metals, Transition metals -- Surfaces, Ammonia -- Synthesis | |||||||||||||||||||||
Journal or Publication Title: | The Innovation | |||||||||||||||||||||
Publisher: | Elsevier | |||||||||||||||||||||
ISSN: | 2666-6758 | |||||||||||||||||||||
Official Date: | 25 January 2022 | |||||||||||||||||||||
Dates: |
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Volume: | 3 | |||||||||||||||||||||
Number: | 1 | |||||||||||||||||||||
Article Number: | 100190 | |||||||||||||||||||||
DOI: | 10.1016/j.xinn.2021.100190 | |||||||||||||||||||||
Status: | Peer Reviewed | |||||||||||||||||||||
Publication Status: | Published | |||||||||||||||||||||
Access rights to Published version: | Open Access (Creative Commons) | |||||||||||||||||||||
Date of first compliant deposit: | 13 April 2022 | |||||||||||||||||||||
Date of first compliant Open Access: | 14 April 2022 | |||||||||||||||||||||
RIOXX Funder/Project Grant: |
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