MoS2 Polymorphic Engineering Enhances Selectivity in the Electrochemical Reduction of Nitrogen to Ammonia

被引：280

作者：

Surrnto, Bryan H. R. ^{[1
]}

Wang, Dabin ^{[1
]}

Azofra, Luis Miguel ^{[2
]}

Harb, Moussab ^{[2
]}

Cavallo, Luigi ^{[2
]}

Jalili, Rouhollah ^{[3
]}

Mitchell, David R. G. ^{[4
]}

Chatti, Manjunath ^{[1
]}

MacFarlane, Douglas R. ^{[1
]}

机构：

[1] Monash Univ, Australian Ctr Electromat Sci, Sch Chem, Clayton, Vic 3800, Australia

[2] KAUST, KAUST Catalysis Ctr KCC, Thuwal 239556900, Saudi Arabia

[3] RMIT Univ, Sch Sci, Melbourne, Vic 3001, Australia

[4] Univ Wollongong, UOW Electron Microscopy Ctr, Wollongong, NSW 2522, Australia

来源：

ACS ENERGY LETTERS | 2019年 / 4卷 / 02期

基金：

澳大利亚研究理事会;

关键词：

ATMOSPHERIC-PRESSURE; AMBIENT CONDITIONS; SULFUR VACANCIES; N-2; CARBON; TEMPERATURE; ELECTROSYNTHESIS; NANOSHEETS; MECHANISM; CATALYSTS;

D O I：

10.1021/acsenergylett.8b02257

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

The electrochemical N-2 reduction reaction (NRR) offers a direct pathway to produce NH3 from renewable energy. However, aqueous NRR suffers from both low Faradaic efficiency (FE) and low yield rate. The main reason is the more favored H+ reduction to H-2 in aqueous electrolytes. Here we demonstrate a highly selective Ru/MoS2NRR catalyst on which the MoS2 polymorphs can be controlled to suppress H+ reduction. A NRR FE as high as 17.6% and NH3 yield rate of 1.14 X 10(-10) mol cm(-2) s(-1) are demonstrated at 50 degrees C. Theoretical evidence supports a hypothesis that the high NRR activity originates from the synergistic interplay between the Ru clusters as N-2 binding sites and nearby isolated S-vacancies on the 2H-MoS2 as centers for hydrogenation; this supports formation of NH3 at the Ru/2H-MoS2 interface.

引用

页码：430 / 435

页数：11

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