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Efficient Electrochemical Nitrogen Fixation over Isolated Pt Sites
Author(s) -
Hao Ran,
Sun Wenming,
Liu Qian,
Liu Xiaolu,
Chen Jialiang,
Lv Xianwei,
Li Wei,
Liu Yuping,
Shen Zhurui
Publication year - 2020
Publication title -
small
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 3.785
H-Index - 236
eISSN - 1613-6829
pISSN - 1613-6810
DOI - 10.1002/smll.202000015
Subject(s) - faraday efficiency , electrochemistry , electrocatalyst , nitrogen , nitrogen fixation , reversible hydrogen electrode , materials science , yield (engineering) , nanoparticle , chemical engineering , nanotechnology , electrode , chemistry , organic chemistry , working electrode , engineering , metallurgy
Recently, ambient electrochemical N 2 fixation has gained great attention. However, the commercial Pt‐based electrocatalyst hardly shows its potential in this field. Herein, it is found that the isolated Pt sites anchored on WO 3 nanoplates exhibit the optimum electrochemical NH 3 yield rate (342.4 µg h −1 mg −1 Pt ) and Faradaic efficiency (31.1%) in 0.1 m K 2 SO 4 at −0.2 V versus RHE, which are about 11 and 15 times higher than their nanoparticle counterparts, respectively. The mechanistic analysis indicates that N 2 conversion to NH 3 follows an alternating hydrogenation pathway, and positively charged isolated Pt sites with special Pt−3O structure can favorably chemisorb and activate the N 2 . Furthermore, the hydrogen evolution reaction can be greatly suppressed on isolated Pt sites decorated WO 3 nanoplates, which guarantees the efficient going‐on of nitrogen reduction reaction.