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Electrochemical nitrogen fixation via bimetallic Sn-Ti sites on defective titanium oxide catalysts.

Authors
  • Cao, Na1
  • Wei, Zengxi2
  • Xu, Jie3
  • Luo, Jun3
  • Guan, Anxiang1
  • Al-Enizi, Abdullah M4
  • Ma, Jianmin2
  • Zheng, Gengfeng5
  • 1 Laboratory of Advanced Materials, Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200438, China. , (China)
  • 2 School of Physics and Electronics, Hunan University, Changsha 410082, China. , (China)
  • 3 Center for Electron Microscopy and Tianjin Key Lab of Advanced Functional Porous Materials, Institute for New Energy Materials, School of Materials, Tianjin University of Technology, Tianjin 300384, China. , (China)
  • 4 Department of Chemistry, College of Science, King Saud University, Riyadh 11451, Saudi Arabia. , (Saudi Arabia)
  • 5 Laboratory of Advanced Materials, Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200438, China. Electronic address: [email protected] , (China)
Type
Published Article
Journal
Journal of Colloid and Interface Science
Publisher
Elsevier
Publication Date
Apr 15, 2021
Volume
588
Pages
242–247
Identifiers
DOI: 10.1016/j.jcis.2020.12.061
PMID: 33388584
Source
Medline
Keywords
Language
English
License
Unknown

Abstract

The efficient adsorption and activation of inert N2 molecules on a heterogeneous electrocatalyst surface are critical toward electrochemical N2 fixation. Inspired by the bimetallic sites in nitrogenase, herein, we developed a bi-metallic tin-titanium (Sn-Ti) structure in Sn-doped anatase TiO2 via an oxygen vacancy induced engineering approach. Density functional theory (DFT) calculations indicated that Sn atoms were introduced in the oxygen vacancy sites in anatase TiO2 (101) to form Sn-Ti bonds. These Sn-Ti bonds provided both strong σ-electron accepting and strong π-electron donating capabilities, thus serving as both N2 adsorption and catalytic N2 reduction sites. In 0.1 M KOH aqueous solution, the Sn-TiO2 electrocatalyst achieved a NH3 production rate of 10.5 μgh-1cm-2 and a corresponding Faradaic efficiency (FENH3) of 8.36% at -0.45 V vs. reversible hydrogen electrode (RHE). Our work suggests the potential of atomic-scale designing and constructing bimetallic active sites for efficient electrocatalytic N2 fixation. Copyright © 2020 Elsevier Inc. All rights reserved.

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