Our official English website, www.x-mol.net, welcomes your
feedback! (Note: you will need to create a separate account there.)
Role of Sulfur Vacancies and Undercoordinated Mo Regions in MoS2 Nanosheets toward the Evolution of Hydrogen
ACS Nano ( IF 15.8 ) Pub Date : 2019-05-28 00:00:00 , DOI: 10.1021/acsnano.9b01583 Lei Li 1, 2 , Zhaodan Qin 1 , Lucie Ries 1 , Song Hong 3 , Thierry Michel 4 , Jieun Yang 5 , Chrystelle Salameh 1 , Mikhael Bechelany 1 , Philippe Miele 1, 6 , Daniel Kaplan 7 , Manish Chhowalla 5 , Damien Voiry 1
ACS Nano ( IF 15.8 ) Pub Date : 2019-05-28 00:00:00 , DOI: 10.1021/acsnano.9b01583 Lei Li 1, 2 , Zhaodan Qin 1 , Lucie Ries 1 , Song Hong 3 , Thierry Michel 4 , Jieun Yang 5 , Chrystelle Salameh 1 , Mikhael Bechelany 1 , Philippe Miele 1, 6 , Daniel Kaplan 7 , Manish Chhowalla 5 , Damien Voiry 1
Affiliation
|
Low-dimensional materials have been examined as electrocatalysts for the hydrogen evolution reaction (HER). Among them, two-dimensional transition metal dichalcogenides (2D-TMDs) such as MoS2 have been identified as potential candidates. However, the performance of TMDs toward HER in both acidic and basic media remains inferior to that of noble metals such as Pt and its alloys. This calls for investigating the influence of controlled defect engineering of 2D TMDs on their performance toward hydrogen production. Here, we explored the HER activity from defective multilayered MoS2 over a large range of surface S vacancy concentrations up to 90%. Amorphous MoS2 and 2H MoS2 with ultrarich S vacancies demonstrated the highest HER performance in acid and basic electrolytes, respectively. We also report that the HER performance from multilayered MoS2 can be divided into two domains corresponding to “point defects” at low concentrations of surface S vacancies (Stage 1) and large regions of undercoordinated Mo atoms for high concentrations of surface S vacancies (Stage 2). The highest performance is obtained for Stage 2 in the presence of undercoordinated Mo atoms with a TOF of ∼2 s–1 at an overpotential of 160 mV in 0.1 M KOH which compares favorably to the best results in the literature. Overall, our work provides deeper insight on the HER mechanism from defected MoS2 and provides guidance for the development of defect-engineered TMD-based electrocatalysts.
中文翻译：
MoS 2纳米片中硫空位和钼配位不足对氢演化的作用
低尺寸材料已作为氢析出反应（HER）的电催化剂进行了研究。其中，诸如MoS 2之类的二维过渡金属二卤化物（2D-TMDs）已被确定为潜在的候选物质。但是，TMDs在酸性和碱性介质中对HER的性能仍然不如Pt及其合金等贵金属。这就要求调查2D TMD的受控缺陷工程对其对制氢性能的影响。在这里，我们探索了缺陷的多层MoS 2在高达90％的表面S空位浓度范围内的HER活性。非晶MoS 2和2H MoS 2具有超富集S的空位分别在酸性和碱性电解质中显示出最高的HER性能。我们还报告说，多层MoS 2的HER性能可以分为两个区域，分别对应于低浓度的表面S空位（阶段1）和高浓度的表面S空位（阶段）的配位不足的Mo原子的“点缺陷” 2）。在未配位的Mo原子下，TOF为〜2 s –1，在0.1 M KOH中的过电势为160 mV时，可获得最高的性能，优于文献中的最佳结果。总体而言，我们的工作从缺陷MoS 2的角度对HER机制提供了更深入的了解 并为开发基于缺陷的TMD基电催化剂提供指导。
更新日期：2019-05-28
中文翻译：
MoS 2纳米片中硫空位和钼配位不足对氢演化的作用
低尺寸材料已作为氢析出反应（HER）的电催化剂进行了研究。其中，诸如MoS 2之类的二维过渡金属二卤化物（2D-TMDs）已被确定为潜在的候选物质。但是，TMDs在酸性和碱性介质中对HER的性能仍然不如Pt及其合金等贵金属。这就要求调查2D TMD的受控缺陷工程对其对制氢性能的影响。在这里，我们探索了缺陷的多层MoS 2在高达90％的表面S空位浓度范围内的HER活性。非晶MoS 2和2H MoS 2具有超富集S的空位分别在酸性和碱性电解质中显示出最高的HER性能。我们还报告说，多层MoS 2的HER性能可以分为两个区域，分别对应于低浓度的表面S空位（阶段1）和高浓度的表面S空位（阶段）的配位不足的Mo原子的“点缺陷” 2）。在未配位的Mo原子下，TOF为〜2 s –1，在0.1 M KOH中的过电势为160 mV时，可获得最高的性能，优于文献中的最佳结果。总体而言，我们的工作从缺陷MoS 2的角度对HER机制提供了更深入的了解 并为开发基于缺陷的TMD基电催化剂提供指导。
京公网安备 11010802027423号