Mo-doped SnS2 with enriched S-vacancies for highly efficient electrocatalytic N2 reduction: the critical role of the Mo–Sn–Sn trimer,Journal of Materials Chemistry A

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Mo-doped SnS2 with enriched S-vacancies for highly efficient electrocatalytic N2 reduction: the critical role of the Mo–Sn–Sn trimer
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2020/03/24 , DOI: 10.1039/d0ta01688h
Ke Chu _{1,

2,

3,

4} , Jing Wang _{1,

2,

3,

4} , Ya-ping Liu _{1,

2,

3,

4} , Qing-qing Li _{1,

2,

3,

4} , Ya-li Guo _{1,

2,

3,

4}

Affiliation

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 N₂ 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 μg 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 N₂ even for the cleavage of the N [triple bond, length as m-dash]

N triple bond to the N [double bond, length as m-dash]

N double bond at the N₂ adsorption stage, consequently leading to a downhill process of the first hydrogenation step and a largely reduced energy barrier.

中文翻译：

Mo掺杂的SnS2具有丰富的S空位，可以高效地电催化还原N2：Mo–Sn–Sn三聚体的关键作用

空位工程和杂原子掺杂是两种定制催化剂的电子结构以提高电催化活性的有效方法。在此，将这两种方法合理地组合以通过Mo掺杂来向N ₂还原反应（NRR）调节SnS ₂的结构，其同时诱导了富集的S-空位（V _s）的产生。具有富集的V _s的已开发的Mo掺杂SnS ₂纳米片呈现出显着增强的NRR活性，NH ₃产率为41.3μgh ^-1 mg ^-1（-0.5 V），法拉第效率为20.8％（-0.4 V），并且是最好的SnS _2之一迄今为止的基于NRR的催化剂。机制研究表明，莫掺杂剂的共同存在和V_小号启用的Mo-Sn系的Sn的创建三聚体的催化位点，能够强烈激活Ñ ₂甚至对于N的裂解 [三重键，长度为m-破折号]