[硫化钼]作为硫化钼析氢催化的模型体系：通过红外多光子解离光谱探测气相中的质子化位点。

Baloglou Aristeidis, Plattner Manuel, Ončák Milan, Grutza Marie-Luise, Kurz Philipp, Beyer Martin K

Institut für Ionenphysik und Angewandte Physik, Universität Innsbruck, Technikerstraße 25, 6020, Innsbruck, Austria.

Institut für Anorganische und Analytische Chemie und Freiburger Materialforschungszentrum (FMF), Albert-Ludwigs-Universität Freiburg, Albertstraße 21, 79104, Freiburg, Germany.

Angew Chem Int Ed Engl. 2021 Mar 1;60(10):5074-5077. doi: 10.1002/anie.202014449. Epub 2021 Jan 26.

Materials based on molybdenum sulfide are known as efficient hydrogen evolution reaction (HER) catalysts. As the binding site for H atoms on molybdenum sulfides for the catalytic process is under debate, [HMo S ] is an interesting molecular model system to address this question. Herein, we probe the [HMo S ] cluster in the gas phase by coupling Fourier-transform ion-cyclotron-resonance mass spectrometry (FT-ICR MS) with infrared multiple photon dissociation (IRMPD) spectroscopy. Our investigations show one distinct S-H stretching vibration at 2450 cm . Thermochemical arguments based on DFT calculations strongly suggest a terminal disulfide unit as the H adsorption site.

基于硫化钼的材料是已知的高效析氢反应（HER）催化剂。由于催化过程中硫化钼上氢原子的结合位点存在争议，[HMoS]是解决这个问题的一个有趣的分子模型系统。在此，我们通过将傅里叶变换离子回旋共振质谱（FT-ICR MS）与红外多光子解离（IRMPD）光谱相结合，在气相中探测[HMoS]簇。我们的研究表明在2450 cm处有一个明显的S-H伸缩振动。基于密度泛函理论（DFT）计算的热化学论据有力地表明末端二硫单元是氢吸附位点。