PdM/g-C_(3)N_(4)(M=Cu、Co、Ir)催化剂制备及其可见光驱动光解水制氢反应性能  

Study of the visible-light photocatalytic water splitting for hydrogen evolution on PdM/g-C_(3)N_(4)(M=Cu,Co,Ir)

作　　者：石冰清 李玉凡 陈冲 邹伟欣 仝庆 杨珊[5] 孙传智 万海勤[1,4] 汤常金[2,4] 董林[1,3,4] SHI Bingqing;LI Yufan;CHEN Chong;ZOU Weixin;TONG Qing;YANG Shan;SUN Chuanzhi;WANHaiqin;TANG Changjin;DONG Lin(School of Environment,Nanjing University,Nanjing,210023,China;School of Chemistry and Chemical Engineering,Nanjing University,Nanjing,210023,China;Center of Moden Analysis,Nanjing,210023,China;Jiangsu Key Laboratory of Vehicle Emissions Control,Nanjing University,Nanjing,210023,China;College of Chemistry,Chemical Engineering and Materials Science,Shandong Normal University,Jinan,250014,China)

机构地区：[1]南京大学环境学院,南京210023 [2]南京大学化学化工学院,南京210023 [3]南京大学现代分析中心,南京210023 [4]江苏省机动车尾气污染控制重点实验室,南京大学,南京210023 [5]山东师范大学化学化工与材料科学学院,济南250014

出　　处：《环境化学》2021年第10期3112-3121,共10页Environmental Chemistry

基　　金：国家自然科学基金(21976082)资助。

摘　　要：贵金属基光催化剂在可见光驱动分解水产氢反应中具有十分优异的性能,却面临价格贵、利用率较低的问题.本文采用乙二醇还原法,将金属Cu、Co、Ir分别引入到贵金属Pd粒子中形成二元PdM金属粒子,负载到g-C_(3)N_(4)表面制得催化剂.在可见光驱动下分解水产氢性能测试结果表明,二元金属Co、Ir的引入相较于0.05 g单金属负载催化剂的4 h产氢量都有明显提升,而Cu则稍微有所降低,最高产氢量是215μmol.并且使得Pd原子的平均产氢量增至1.4—4.4倍.光催化性能提升的主要原因是由于PdM粒子负载增强了样品对光的吸收,促进了光生电子与空穴的分离,增加了样品的亲水性降低了水分子吸附能.另外,二元金属的引入可显著提升Pd原子的平均产氢量.尤其是与过渡金属Co形成PdCo粒子,其4 h产氢性能与PdIr接近,但其价格远低于Ir.因而PdCo/g-C_(3)N_(4)催化剂具有很好的经济性.Noble metal based photocatalysts have excellent performance toward the hydrogen evolution by water splitting under visible light irradiation, but some disadvantages are present, such as expensive, low utilization, etc. In this study, by the polyol reduction method, the elements of copper(Cu), cobalt(Co) and iridium(Ir) were introduced into Pd nanoparticles to prepare PdM bimetallic nanoparticles, which were loaded on the surface of g-C_(3)N_(4). The results of hydrogen evolution indicated that compared to pristine Pd/g-C_(3)N_(4), the hydrogen amounts of 0.05 g Pd(Co,Ir)/g-C_(3)N_(4) catalysts have significant hydrogen evolution increase in 4 h, while Cu has a slight decrease, the highest one achieved 215 μmol. And the introduction of Cu, Co, Ir increases the hydrogen evolution of average Pd atoms by 1.4 —4.4 times. The improvement of catalytic performance is attributed to the increased light absorption, the separation of electron and hole, the hydrophilic property, and the decreased adsorption energy with water reactant of the PdM/g-C_(3)N_(4) catalysts. Furthermore, the average produced hydrogen amount of Pd atom was increased by introducing of M, PdCo/g-C_(3)N_(4) displayed a similar catalytic performance with PdIr/g-C_(3)N_(4). On the basis of that cobalt is cheaper than iridium, PdCo/g-C_(3)N_(4) is very economical.

关 键 词：PdM二元金属 g-C_(3)N_(4) 可见光 光催化 分解水产氢 

分 类 号：TQ116.2[化学工程—无机化工] TQ426