CAS OpenIR  > 中科院上海应用物理研究所2011-2020年
An oxygen vacancy-rich two-dimensional Au/TiO2 hybrid for synergistically enhanced electrochemical N2 activation and reduction
Zhao, Sen1; Liu, Han-Xuan2; Qiu, Yu1; Liu, Shuang-Quan1; Diao, Jin-Xiang1; Chang, Chun-Ran2; Si, Rui3; Guo, Xiao-Hui1
2020
Source PublicationJournal of Materials Chemistry A
ISSN2050-7488
Volume8Issue:14Pages:6586-6596
Subtype期刊论文
AbstractThe electrochemical nitrogen reduction reaction (NRR) is emerging as a promising sustainable technique that can convert nitrogen (N2) to ammonia (NH3) under ambient conditions. However, the selectivity and electrocatalytic activity of the NRR obtained experimentally to date are still unsatisfactory. As a consequence, it remains a technical challenge to develop scalable, low-cost, and efficient NRR electrocatalysts. Herein, we present an oxygen vacancy (VO)-rich two-dimensional gold (Au)/titanium dioxide (TiO2) hybrid that acts as an advanced NRR electrocatalyst under ambient conditions. Electrocatalytic testing demonstrated that the Au/TiO2 hybrid catalyst delivered a promising NH3 yield of 64.6 μg h-1 mg-1 cat and a high faradaic efficiency of 29.5% at -0.40 V versus the reversible hydrogen electrode in acidic media. Experimental findings and theoretical calculations demonstrate that the strong electron-donating effect of VO in TiO2 was essential for N2 activation. Meanwhile, the introduction of Au promotes both the electrochemical and thermodynamic rate-limiting steps by adjusting the electronic structure of the active sites. Together, these effects greatly facilitate the activation and reduction of N2 under ambient conditions. The specific catalyst design strategy in our work represents an alternative avenue to produce other two-dimensional electrocatalysts with high NRR activity and selectivity through rational structural engineering. © 2020 The Royal Society of Chemistry.
KeywordGold compounds Ammonia Catalyst selectivity Chemical activation Electrocatalysts Electronic structure Nitrogen Oxide minerals Oxygen Oxygen vacancies Reduction Titanium dioxide Electrocatalytic activity Electron donating effects Faradaic efficiencies Nitrogen reduction Rate limiting steps Reversible hydrogen electrodes Technical challenges Theoretical calculations
DOI10.1039/d0ta00658k
Indexed ByEI
Language英语
Citation statistics
Document Type期刊论文
Identifierhttp://ir.sinap.ac.cn/handle/331007/32703
Collection中科院上海应用物理研究所2011-2020年
Affiliation1.Key Lab of Synthetic and Natural Functional Molecule Chemistry, Ministry of Education, College of Chemistry and Materials Science, Northwest University, Xi'an; 710069, China;
2.Shaanxi Key Laboratory of Energy Chemical Process Intensification, School of Chemical Engineering and Technology, Xi'An Jiaotong University, Xi'an; 710049, China;
3.Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai; 201800, China
Recommended Citation
GB/T 7714
Zhao, Sen,Liu, Han-Xuan,Qiu, Yu,et al. An oxygen vacancy-rich two-dimensional Au/TiO2 hybrid for synergistically enhanced electrochemical N2 activation and reduction[J]. Journal of Materials Chemistry A,2020,8(14):6586-6596.
APA Zhao, Sen.,Liu, Han-Xuan.,Qiu, Yu.,Liu, Shuang-Quan.,Diao, Jin-Xiang.,...&Guo, Xiao-Hui.(2020).An oxygen vacancy-rich two-dimensional Au/TiO2 hybrid for synergistically enhanced electrochemical N2 activation and reduction.Journal of Materials Chemistry A,8(14),6586-6596.
MLA Zhao, Sen,et al."An oxygen vacancy-rich two-dimensional Au/TiO2 hybrid for synergistically enhanced electrochemical N2 activation and reduction".Journal of Materials Chemistry A 8.14(2020):6586-6596.
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