Efficient Electrochemical Nitrogen Fixation over Isolated Pt Sites

Recently, ambient electrochemical N2 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 WO3 nanoplates exhibit the optimum electrochemical NH3 yield rate (342.4 µg...

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Veröffentlicht in:Small (Weinheim an der Bergstrasse, Germany) Jg. 16; H. 22; S. e2000015 - n/a
Hauptverfasser: Hao, Ran, Sun, Wenming, Liu, Qian, Liu, Xiaolu, Chen, Jialiang, Lv, Xianwei, Li, Wei, Liu, Yu‐ping, Shen, Zhurui
Format: Journal Article
Sprache:Englisch
Veröffentlicht: Germany Wiley Subscription Services, Inc 01.06.2020
Schlagworte:
Ammonia
Chemical reduction
density functional theory calculations
electrocatalysis
electrochemical in situ Fourier transform infrared spectroscopy
Hydrogen evolution reactions
Hydrogen storage
isolated Pt sites
Nanoparticles
Nanotechnology
nitrogen reduction reaction
Nitrogenation
Potassium sulfate
Tungsten oxides
isolated Pt sites
density functional theory calculations
electrocatalysis
nitrogen reduction reaction
electrochemical in situ Fourier transform infrared spectroscopy
ISSN:1613-6810, 1613-6829, 1613-6829
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Zusammenfassung:Recently, ambient electrochemical N2 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 WO3 nanoplates exhibit the optimum electrochemical NH3 yield rate (342.4 µg h−1 mg−1Pt) and Faradaic efficiency (31.1%) in 0.1 m K2SO4 at −0.2 V versus RHE, which are about 11 and 15 times higher than their nanoparticle counterparts, respectively. The mechanistic analysis indicates that N2 conversion to NH3 follows an alternating hydrogenation pathway, and positively charged isolated Pt sites with special Pt−3O structure can favorably chemisorb and activate the N2. Furthermore, the hydrogen evolution reaction can be greatly suppressed on isolated Pt sites decorated WO3 nanoplates, which guarantees the efficient going‐on of nitrogen reduction reaction. Isolated Pt atoms anchored on WO3 nanoplates exhibit highly active for ambient ammonia electrosynthesis, which is ascribed to facilitated chemisorption and activation of nitrogen and effective suppression for hydrogen evolution reaction (HER), immensely enhancing NH3 yield rate and Faradic efficiency. This groundbreaking research presents Pt‐based nanocatalysts for electroreduction of nitrogen and provides an idea for the HER depression.
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ISSN:1613-6810
1613-6829
1613-6829
DOI:10.1002/smll.202000015