Journal
JOURNAL OF COLLOID AND INTERFACE SCIENCE
Volume 588, Issue -, Pages 242-247Publisher
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcis.2020.12.061
Keywords
Electrocatalysis; Nitrogen reduction; Adsorption; Oxygen vacancy; Faradaic efficiency
Categories
Funding
- National Key Research and Development Program of China [2017YFA0206901, 2018YFA0209401]
- Natural Science Foundation of China [22025502, 21975051, 21773036]
- Science and Technology Commission of Shanghai Municipality [19XD1420400]
- Innovation Program of Shanghai Municipal Education Commission [2019-01-07-00-07-E00045]
- King Saud University, Riyadh, Saudi Arabia [RSP-2020/55]
- Shanghai Synchrotron Radiation Facility (SSRF)
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The study demonstrated the successful development of a bi-metallic Sn-Ti structure in TiO2 for efficient electrocatalytic N-2 fixation, highlighting the potential of atomic-scale designing and constructing bimetallic active sites.
The efficient adsorption and activation of inert N-2 molecules on a heterogeneous electrocatalyst surface are critical toward electrochemical N-2 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 sigma-electron accepting and strong pi-electron donating capabilities, thus serving as both N-2 adsorption and catalytic N-2 reduction sites. In 0.1 M KOH aqueous solution, the Sn-TiO2 electrocatalyst achieved a NH3 production rate of 10.5 mu g h(-1) cm(-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 N-2 fixation. (C) 2020 Elsevier Inc. All rights reserved.
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