Jagminas Arunas, Gaigalas Paulius, Bittencourt Carla, Klimas Vaclovas
The Department of Electrochemical Materials Science, State Research Institute Center for Physical Sciences and Technology, Sauletekio ave. 3, LT-01257 Vilnius, Lithuania.
Chemie des Interactions Plasma-Surface, University of Mons, Place du Parc 22, 7000 Mons, Belgium.
Materials (Basel). 2021 Mar 2;14(5):1165. doi: 10.3390/ma14051165.
The noble, metal-free materials capable of efficiently catalyzing water splitting reactions currently hold a great deal of promise. In this study, we reported the structure and electrochemical performance of new MoS-based material synthesized with L-cysteine. For this, a facile one-pot hydrothermal process was developed and an array of densely packed nanoplatelet-shaped hybrid species directly on a conductive substrate were obtained. The crucial role of L-cysteine was determined by numerous methods on the structure and composition of the synthesized material and its activity and stability for hydrogen evolution reaction (HER) from the acidic water. A low Tafel slope of 32.6 mV dec, close to a Pt cathode, was registered for the first time. The unique HER performance at the surface of this hybrid material in comparison with recently reported MoS-based electrocatalysts was attributed to the formation of more defective 1T, 2H-MoS/MoO, C nanostructures with the dominant 1T-MoS phase and thermally degraded cysteine residues entrapped. Numerous stacks of metallic (1T-MoS and MoO) and semiconducting (2H-MoS and MoO) fragments relayed the formation of highly active layered nanosheets possessing a low hydrogen adsorption free energy and much greater durability, whereas intercalated cysteine fragments had a low Tafel slope of the HER reaction. X-ray photoelectron spectroscopy, scanning electron microscopy, thermography with mass spectrometry, high-resolution transmission electron microscopy, Raman spectroscopy techniques, and linear sweep voltammetry were applied to verify our findings.
目前,能够有效催化水分解反应的贵金属无材料具有很大的前景。在本研究中,我们报道了用L-半胱氨酸合成的新型MoS基材料的结构和电化学性能。为此,开发了一种简便的一锅水热法,并在导电基底上直接获得了一系列紧密堆积的纳米片状混合物种。通过多种方法确定了L-半胱氨酸对合成材料的结构和组成及其从酸性水中析氢反应(HER)的活性和稳定性的关键作用。首次记录到低至32.6 mV dec的塔菲尔斜率,接近铂阴极。与最近报道的基于MoS的电催化剂相比,这种混合材料表面独特的HER性能归因于形成了更多缺陷的1T、2H-MoS/MoO、C纳米结构,其中以1T-MoS相为主,并包裹有热降解的半胱氨酸残基。大量的金属(1T-MoS和MoO)和半导体(2H-MoS和MoO)片段堆叠形成了具有低氢吸附自由能和更高耐久性的高活性层状纳米片,而插层的半胱氨酸片段具有较低的HER反应塔菲尔斜率。应用X射线光电子能谱、扫描电子显微镜、热重质谱联用、高分辨率透射电子显微镜、拉曼光谱技术和线性扫描伏安法来验证我们的发现。