A Synthetic Route to MoS2 Catalysts Supported on a Metal-Organic Framework for Electrochemical Hydrogen Evolution Reaction Utilizing Chemical Vapor Deposition
A Synthetic Route to MoS2 Catalysts Supported on a Metal-Organic Framework for Electrochemical Hydrogen Evolution Reaction Utilizing Chemical Vapor Deposition
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金属有机骨架负载的 MoS2 催化剂的合成路线，用于利用化学气相沉积的电化学析氢反应
DOI：
10.1021/acs.energyfuels.1c03454
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发表时间：
2021
期刊：
影响因子：
5.3
通讯作者：
Horiuchi Yu
中科院分区：
文献类型：
--
作者：
Nishigaki Kenichi;Katagiri Makoto;Matsuoka Masaya;Horiuchi Yu
采用两步化学气相沉积(CVD)新方法，在锆基金属有机骨架UIO-66中合成了用于电化学析氢反应的MoS2催化剂。第一步，以Mo(CO)6为前驱体，在UIO-66骨架的苯基上合成了芳基三羰基钼络合物。随后，用二甲基硫(CH3S2CH3)进行第二次CVD过程，将钼络合物转化为MoS2。傅立叶变换红外光谱和拉曼光谱分别证实了钼络合物和MoS2在UIO-66中的成功形成。此外，X射线衍射仪和氮气吸附-脱附测试表明，两步CVD方法后的UIO-66骨架保持不变。由此合成的MoS_2固定化UIO-66具有比块体MoS_2更高的HER电化学活性。电化学阻抗谱表明，在UIO-66空腔中生长的MoS2粒子在电极界面具有较低的电荷转移电阻，这是导致HER活性较高的原因。
MoS2catalysts for electrochemical hydrogen evolution reaction (HER) have been synthesized in a Zr-based metal–organic framework, UiO-66, by a new two-step chemical vapor deposition (CVD) method. The first CVD process was performed to construct the arenetricarbonyl Mo complex on the phenylene moiety of the UiO-66 framework by using Mo(CO)6as a precursor. Subsequently, the Mo complex was converted to MoS2by the second CVD process with dimethyl sulfide (CH3S2CH3). The successful formation of the Mo complex and MoS2in UiO-66 was confirmed by using FT-IR and Raman spectroscopy, respectively. In addition, XRD and N2adsorption–desorption measurements revealed the preservation of the UiO-66 framework after the two-step CVD method. The thus-synthesized MoS2-immobilized UiO-66 exhibited a higher activity for electrochemical HER than bulk MoS2. Electrochemical impedance spectroscopy suggested that a low charge transfer resistance at the electrode interface for MoS2particles grown in the cavity of UiO-66 was responsible for the high electrochemical HER activity.