摘要
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Co_(2)P、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Co_(2)P、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>Co_(2)P,说明这些反应之间存在内在联系。
The phosphosulfide phases of Co_(2)P,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 Co_(2)P,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 Co_(2)P phosphides,suggesting a correlation among these reactions.
作者
胡洋
李翔
盛强
尚森森
张晨曦
邹洁
HU Yang;LI Xiang;SHENG Qiang;SHANG Sen-sen;ZHANG Chen-xi;ZOU Jie(College of Chemical Engineering and Materials Science,Tianjin University of Science and Technology,Tianjin 300457,China;Yinchuan University of Energy,Yinchuan 750105,China)
出处
《现代化工》
CAS
CSCD
北大核心
2023年第S02期129-135,共7页
Modern Chemical Industry
基金
国家自然科学基金(21673029,22108207)
天津市自然科学基金重点项目(19JCZDJC31700)
重质油国家重点实验室开放基金(SKLOP202002003,SKLHOP202202005)
宁夏自然科学基金(2021AAC03253)
关键词
加氢脱硫
加氢脱氮
电催化析氢反应
过渡金属磷化物
过渡金属磷硫化物
硫脲
hydrodesulfurization
hydrodenitrogenation
hydrogen evolution reaction
transition-metal phosphide
transition-metal phosphosulfide
thiourea
作者简介
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;通讯联系人:李翔(1973-),男,博士,教授,研究方向为加氢、加氢精制和多孔催化材料等,lixiang@tust.edu.cn。