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Substrate strain engineering: An efficient strategy to enhance the catalytic activity of SACs on waved graphene for e-NRR
Di Liu1; Haoqiang Ai2; Wan Tong Lou3; Feifei Li1; Kin Ho Lo2; Shuangpeng Wang1,4; Hui Pan1,4
2020-07-01
Source PublicationSustainable Energy and Fuels
ISSN2398-4902
Volume4Issue:7Pages:3773-3779
Other Abstract

Ammonia is an important chemical in both industry and agriculture. The production of ammonia in a green way is challenging. The electrochemical nitrogen reduction reaction (e-NRR) has been proposed for this purpose. However, this technology is still far from practical applications due to low production, which is mainly because of inefficient electrocatalysts. In this work, we have designed a series of single-atom catalysts (SACs) anchored on waved graphene (wG) for efficient e-NRR and systematically investigated the effect of curvature on the catalytic performance based on first-principles calculations. Eight SACs (V, Cr, Mn, Fe, Co, Ni, Cu, and Pt) anchored on waved graphene with various curvatures (0-50%) have been studied. We found that the curvature strongly affected the formation, catalytic activity, and selectivity of SACs for e-NRR: (1) the formation possibility of SACs on wG was considerably enhanced on increasing the curvature. (2) The free energies for the rate-determining steps of SAC-V-wG, SAC-Mn-wG, and SAC-Cr-wG were less than 1.0 eV, leading to high catalytic activity for e-NRR. In particular, SAC-Mn-wG exhibited higher activity for e-NRR than SAC-Mn on flat graphene. (3) The three systems had higher selectivity for e-NRR than for HER, which could be further improved by compression. Thus, we conclude that SAC-Mn-wG is the best SAC on wG for e-NRR because of its easy fabrication, good catalytic performance and high selectivity. We believe that our findings can provide new insights in reported experimental results and guidance for the design of novel SACs with high performance for e-NRR.

DOI10.1039/d0se00518e
URLView the original
Indexed BySCIE
Language英語English
WOS Research AreaChemistry ; Energy & Fuels ; Materials Science
WOS SubjectChemistry, Physical ; Energy & Fuels ; Materials Science, Multidisciplinary
WOS IDWOS:000544657200055
Scopus ID2-s2.0-85087548648
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Document TypeJournal article
CollectionDEPARTMENT OF ELECTROMECHANICAL ENGINEERING
INSTITUTE OF APPLIED PHYSICS AND MATERIALS ENGINEERING
Corresponding AuthorShuangpeng Wang
Affiliation1.Institute of Applied Physics and Materials Engineering,University of Macau,Macao SAR,Macao
2.Department of Electromechanical Engineering,Faculty of Science and Technology,University of Macau,Macao SAR,Macao
3.Department of Physics,University of Oxford,Oxford,United Kingdom
4.Department of Physics and Chemistry,Faculty of Science and Technology,University of Macau,Macao SAR,Macao
First Author AffilicationINSTITUTE OF APPLIED PHYSICS AND MATERIALS ENGINEERING
Corresponding Author AffilicationINSTITUTE OF APPLIED PHYSICS AND MATERIALS ENGINEERING;  Faculty of Science and Technology
Recommended Citation
GB/T 7714
Di Liu,Haoqiang Ai,Wan Tong Lou,et al. Substrate strain engineering: An efficient strategy to enhance the catalytic activity of SACs on waved graphene for e-NRR[J]. Sustainable Energy and Fuels, 2020, 4(7), 3773-3779.
APA Di Liu., Haoqiang Ai., Wan Tong Lou., Feifei Li., Kin Ho Lo., Shuangpeng Wang., & Hui Pan (2020). Substrate strain engineering: An efficient strategy to enhance the catalytic activity of SACs on waved graphene for e-NRR. Sustainable Energy and Fuels, 4(7), 3773-3779.
MLA Di Liu,et al."Substrate strain engineering: An efficient strategy to enhance the catalytic activity of SACs on waved graphene for e-NRR".Sustainable Energy and Fuels 4.7(2020):3773-3779.
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