Pd-P/g-C_(3)N_(4)催化剂的优化制备及在甲酸分解制氢中的应用  

Preparation of Pd-P/g-C_(3)N_(4) catalyst and its application in hydrogen production by formic acid decomposition

作　　者：夏媛玉 王雨生 裴瑜洁 解品红 李其明[1] 李芳[1] Xia Yuanyu;Wang Yusheng;Pei Yujie;Xie Pinhong;Li Qiming;Li Fang(School of Petrochemical Engineering,Liaoning Petrochemical University,Fushun 113001)

机构地区：[1]辽宁石油化工大学石油化工学院,抚顺113001

出　　处：《化工新型材料》2023年第6期186-190,198,共6页New Chemical Materials

基　　金：国家自然科学基金(21703091,21201096);辽宁省教育厅资助项目(L2019009);辽宁科技厅计划指导项目(2019-ZD-0058)。

摘　　要：以氮化碳(g-C_(3)N_(4))为载体,采用液相还原法制备了一系列Pd-P/g-C_(3)N_(4)催化剂用于甲酸分解制氢,通过优化还原温度和活性组分负载量可以显著提高催化剂性能。采用X射线衍射仪、透射电子显微镜和X射线光电子能谱仪对催化剂的晶相结构、微观形貌、活性组分分布以及价态进行分析,并通过甲酸分解制氢实验测试了催化剂的甲酸分解制氢活性。结果表明:使用次磷酸钠还原剂需要在较高还原温度(90℃)才能实现Pd-P活性组分在g-C_(3)N_(4)载体表面的高度分散,获得较小的纳米粒子,过高或过低的还原温度都不利于制备高性能催化剂。当Pd负载量为8.0%(质量分数)时,2-Pd-P/g-C_(3)N_(4)催化剂表现出最佳催化性能,通过动力学研究和Arrhenius方程计算得到该催化剂的甲酸分解活化能为33.83kJ/mol。A series of Pd-P/C_(3)N_(4) catalysts for hydrogen production from formic acid were prepared by liquid-phase reduction method using carbon nitride(g-C_(3)N_(4))as the carrier.Here the catalytic activity of the catalysts was significantly improved by optimizing the reduction temperature and loading amounts of active components.The crystal structure,microstructure,active component distribution and valence state of the catalysts were analyzed by X-ray diffractometry(XRD),transmission electron microscopy(TEM)and X-ray photoelectron spectroscopy(XPS).The activity of the catalyst for hydrogen production from formic acid decomposition was tested by formic acid decomposition experiment.The results showed that the reducing agent based on sodium hypophosphite needed a high reduction temperature(90℃)to achieve the high dispersion of the Pd-P active component on the surface of carbon nitride carrier,and to obtain small nanoparticles.Too high or too low reduction temperature was not conducive to the preparation of high-performance catalysts.When the Pd loading was 8.0%(mass fraction),the 2-Pd-P/g-C_(3)N_(4) catalyst showed the best catalytic performance,and the activation energy of the catalyst for formic acid decomposition was 33.83kJ/mol calculated by the kinetic study and the Arrhenius equation.

关 键 词：甲酸 还原 催化剂 制氢 

分 类 号：TQ028.8[化学工程]