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Unveiling Active Sites for the Hydrogen Evolution Reaction on Monolayer MoS2
Advanced Materials ( IF 27.4 ) Pub Date : 2017-09-22 , DOI: 10.1002/adma.201701955 Jing Zhang 1 , Jingjie Wu 1 , Hua Guo 1 , Weibing Chen 1 , Jiangtan Yuan 1 , Ulises Martinez 2 , Gautam Gupta 2 , Aditya Mohite 2 , Pulickel M. Ajayan 1 , Jun Lou 1
Advanced Materials ( IF 27.4 ) Pub Date : 2017-09-22 , DOI: 10.1002/adma.201701955 Jing Zhang 1 , Jingjie Wu 1 , Hua Guo 1 , Weibing Chen 1 , Jiangtan Yuan 1 , Ulises Martinez 2 , Gautam Gupta 2 , Aditya Mohite 2 , Pulickel M. Ajayan 1 , Jun Lou 1
Affiliation
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Here, the hydrogen evolution reaction (HER) activities at the edge and basal‐plane sites of monolayer molybdenum disulfide (MoS2) synthesized by chemical vapor deposition (CVD) are studied using a local probe method enabled by selected‐area lithography. Reaction windows are opened by e‐beam lithography at sites of interest on poly(methyl methacrylate) (PMMA)‐covered monolayer MoS2 triangles. The HER properties of MoS2 edge sites are obtained by subtraction of the activity of the basal‐plane sites from results containing both basal‐plane and edge sites. The catalytic performances in terms of turnover frequencies (TOFs) are calculated based on the estimated number of active sites on the selected areas. The TOFs follow a descending order of 3.8 ± 1.6, 1.6 ± 1.2, 0.008 ± 0.002, and 1.9 ± 0.8 × 10−4 s−1, found for 1T′‐, 2H‐MoS2 edges, and 1T′‐, 2H‐MoS2 basal planes, respectively. Edge sites of both 2H‐ and 1T′‐MoS2 are proved to have comparable activities to platinum (≈1–10 s−1). When fitted into the HER volcano plot, the MoS2 active sites follow a trend distinct from conventional metals, implying a possible difference in the reaction mechanism between transition‐metal dichalcogenides (TMDs) and metal catalysts.
中文翻译：
在单层MoS2上揭示氢发生反应的活性位点
在此，使用局部区域光刻技术，通过局部探针法研究了通过化学气相沉积（CVD）合成的单层二硫化钼（MoS 2）的边缘和基平面位处的放氢反应（HER）活性。通过电子束光刻在聚甲基丙烯酸甲酯（PMMA）覆盖的单层MoS 2三角形上感兴趣的位置打开反应窗口。MoS 2的HER特性边缘位点是通过从同时包含基底位点和边缘位点的结果中减去基底位点的活性而获得的。基于周转频率（TOF）的催化性能是基于所选区域上活性位点的估计数量来计算的。TOF的降序依次为3.8± 1.6、1.6 ± 1.2、0.008 ±0.002和1.9±0.8×10 -4 s -1，适用于1T'-，2H-MoS 2边缘和1T'-，2H- MoS 2基础平面。事实证明，2H-和1T'-MoS 2的边缘部位都具有与铂相当的活性（≈1-10s -1）。当安装到HER火山区中时，MoS 2 活性位点的趋势不同于传统金属，这意味着过渡金属二卤化碳（TMD）与金属催化剂之间的反应机理可能存在差异。
更新日期：2017-09-22
中文翻译：
在单层MoS2上揭示氢发生反应的活性位点
在此，使用局部区域光刻技术，通过局部探针法研究了通过化学气相沉积（CVD）合成的单层二硫化钼（MoS 2）的边缘和基平面位处的放氢反应（HER）活性。通过电子束光刻在聚甲基丙烯酸甲酯（PMMA）覆盖的单层MoS 2三角形上感兴趣的位置打开反应窗口。MoS 2的HER特性边缘位点是通过从同时包含基底位点和边缘位点的结果中减去基底位点的活性而获得的。基于周转频率（TOF）的催化性能是基于所选区域上活性位点的估计数量来计算的。TOF的降序依次为3.8± 1.6、1.6 ± 1.2、0.008 ±0.002和1.9±0.8×10 -4 s -1，适用于1T'-，2H-MoS 2边缘和1T'-，2H- MoS 2基础平面。事实证明，2H-和1T'-MoS 2的边缘部位都具有与铂相当的活性（≈1-10s -1）。当安装到HER火山区中时，MoS 2 活性位点的趋势不同于传统金属，这意味着过渡金属二卤化碳（TMD）与金属催化剂之间的反应机理可能存在差异。
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