以硫脲为固体硫化剂、相应过渡金属磷酸盐为前驱体,采用程序升温还原的方法制备了Co₂P、MoP和WP的磷硫化物。结果表明,添加硫脲后制备的催化剂结晶度和粒度都有所降低。在酸性条件下电催化析氢反应(HER)中,磷硫化物活性随前驱体中硫脲质量分数的增加呈先增加后降低的趋势。制备Co₂P、MoP和WP的磷硫化物时前驱体中最佳的硫脲质量分数分别为26%、33%和33%。过渡金属磷化物催化HER、杂环含氮化合物加氢以及二苯并噻吩(DBT)加氢脱硫(HDS)活性顺序均为MoP>WP>Co₂P,说明这些反应之间存在内在联系。

The phosphosulfide phases of Co₂P,MoP,and WP are prepared via temperature-programmed reduction by using the corresponding transition metals phosphate as precursors and thiourea as solid sulfiding agent.Both the crystallinities and particle sizes of the catalysts prepared by adding thiourea decrease.In the catalytic hydrogen evolution reaction (HER) under acidic conditions,the activities of the phosphosulfide catalysts firstly increases and then decreases with the increasing content of thiourea in the phosphate precursors.The optimal content of thiourea in the precursors of Co₂P,MoP,and WP for the preparation of phosphosulfides are 26%,33%,and 33%,respectively.MoP phosphides exhibits the biggest activity in the hydrogen evolution reaction,the hydrogenation of heterocyclic nitrogen-containing compounds,and the hydrodesulfurization of dibenzothiophene,followed by WP phosphides and then Co₂P phosphides,suggesting a correlation among these reactions.

胡洋(1997-),男,硕士生,研究方向为加氢精制及电催化析氢,13622133326@163.com。