Mo-doped SnS2 with enriched S-vacancies for highly efficient electrocatalytic N2 reduction: the critical role of the Mo-Sn-Sn trimer

被引:180
作者
Chu, Ke [1 ]
Wang, Jing [1 ]
Liu, Ya-ping [1 ]
Li, Qing-qing [1 ]
Guo, Ya-li [1 ]
机构
[1] Lanzhou Jiaotong Univ, Sch Mat Sci & Engn, Lanzhou 730070, Peoples R China
基金
中国国家自然科学基金;
关键词
NITROGEN REDUCTION; GRAPHENE/COPPER COMPOSITES; OXYGEN VACANCIES; INTERFACE; FIXATION; AMMONIA; NANOSHEETS; NANOPARTICLES; MONOLAYER; CATALYSTS;
D O I
10.1039/d0ta01688h
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
Vacancy engineering and heteroatom doping are two effective approaches to tailor the electronic structures of catalysts for improved electrocatalytic activity. Herein, these two approaches were rationally combined to modulate the structure of SnS2 toward the N-2 reduction reaction (NRR) by means of Mo-doping, which simultaneously induced the generation of enriched S-vacancies (V-s). The developed Mo-doped SnS2 nanosheets with enriched V-s presented a conspicuously enhanced NRR activity with an NH3 yield of 41.3 mu g h(-1) mg(-1) (-0.5 V) and a faradaic efficiency of 20.8% (-0.4 V) and are among the best SnS2-based NRR catalysts to date. Mechanistic studies revealed that the co-presence of the Mo dopant and V-s enabled the creation of Mo-Sn-Sn trimer catalytic sites, capable of strongly activating N-2 even for the cleavage of the N N triple bond to the N N double bond at the N-2 adsorption stage, consequently leading to a downhill process of the first hydrogenation step and a largely reduced energy barrier.
引用
收藏
页码:7117 / 7124
页数:8
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