Journal
SMALL
Volume 16, Issue 22, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202000015
Keywords
density functional theory calculations; electrocatalysis; electrochemical in situ Fourier transform infrared spectroscopy; isolated Pt sites; nitrogen reduction reaction
Categories
Funding
- National Natural Science Foundation of China [21872102, 21703219, 21878162, 21978137]
- Natural Science Foundation of Tianjin [17JCYBJC17100]
- Science and Technology Commissioner of Tianjin [18JCTPJC55900]
- Fundamental Research Funds for the Central Universities
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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 WO3 nanoplates exhibit the optimum electrochemical NH3 yield rate (342.4 mu g h(-1) mg(Pt)(-1)) 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 N-2 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 N-2. 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.
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