Kagkoura Antonia, Canton-Vitoria Ruben, Vallan Lorenzo, Hernandez-Ferrer Javier, Benito Ana M, Maser Wolfgang K, Arenal Raul, Tagmatarchis Nikos
Theoretical and Physical Chemistry Institute, National Hellenic Research Foundation, 48 Vassileos Constantinou Avenue, Athens, 11635, Greece.
Instituto de Carboquimica (ICB-CSIC), C/Miguel Luesma Castan 4, 50018, Zaragoza, Spain.
Chemistry. 2020 May 20;26(29):6635-6642. doi: 10.1002/chem.202000125. Epub 2020 Mar 31.
The preparation of an MoS -polymer carbon nanodot (MoS -PCND) hybrid material was accomplished by employing an easy and fast bottom-up synthetic approach. Specifically, MoS -PCND was realized by the thermal decomposition of ammonium tetrathiomolybdate and the in situ complexation of Mo with carboxylic acid units present on the surface of PCNDs. The newly prepared hybrid material was comprehensively characterized by spectroscopy, thermal means, and electron microscopy. The electrocatalytic activity of MoS -PCND was examined in the hydrogen evolution reaction (HER) and compared with that of the corresponding hybrid material prepared by a top-down approach, namely MoS -PCND(exf-fun), in which MoS was firstly exfoliated and then covalently functionalized with PCNDs. The MoS -PCND hybrid material showed superior electrocatalytic activity toward the HER with low Tafel slope, excellent electrocatalytic stability, and an onset potential of -0.16 V versus RHE. The superior catalytic performance of MoS -PCND was rationalized by considering the catalytically active sites of MoS , the effective charge/energy-transfer phenomena from PCNDs to MoS , and the synergetic effect between MoS and PCNDs in the hybrid material.
通过采用一种简便快速的自下而上合成方法制备了一种二硫化钼-聚合物碳纳米点（MoS -PCND）杂化材料。具体而言，MoS -PCND是通过四硫代钼酸铵的热分解以及Mo与PCNDs表面存在的羧酸单元的原位络合实现的。通过光谱学、热分析方法和电子显微镜对新制备的杂化材料进行了全面表征。在析氢反应（HER）中考察了MoS -PCND的电催化活性，并与通过自上而下方法制备的相应杂化材料MoS -PCND(exf-fun)进行了比较，在MoS -PCND(exf-fun)中，MoS首先被剥离，然后与PCNDs进行共价功能化。MoS -PCND杂化材料对HER表现出优异的电催化活性，具有低塔菲尔斜率、出色的电催化稳定性以及相对于可逆氢电极（RHE）为-0.16 V的起始电位。通过考虑MoS的催化活性位点、从PCNDs到MoS的有效电荷/能量转移现象以及杂化材料中MoS与PCNDs之间的协同效应，合理解释了MoS -PCND的优异催化性能。
