不同直链二胺对敏化石墨烯制氢光催化剂性能的影响  

Effects of Different Linear Diamines on the Performance of Photocatalysts for Hydrogen Production of Sensitized Graphene

作　　者：王玉营 陈建彪[1] 张旭强[1,2] 吕功煊[2] WANG Yu-ying;CHEN Jian-biao;ZHANG Xu-qiang;LU Gong-xuan(Key Laboratory of Atomic and Molecular Physics&Functional Materials of Gansu Province,College of Physics and Electronic Engineering,Northwest Normal University,Lanzhou 730070,China;National Key Laboratory of Carbonyl Synthesis and Selective Oxygenation,Lanzhou Institute of Chemical Physics,Chinese Academy of Sciences,Lanzhou 73000,China)

机构地区：[1]甘肃省原子分子物理与功能材料重点实验室,西北师范大学物理与电子工程学院,甘肃兰州730070 [2]中国科学院兰州化学物理研究所羰基合成与选择氧化国家重点实验室,甘肃兰州730000

出　　处：《分子催化》2020年第1期1-7,I0001,共8页Journal of Molecular Catalysis(China)

基　　金：国家自然科学基金(11864035,11364036,11474231,11464041,21433007,21673262)。

摘　　要：采用一步水热法合成方法,分别利用乙二胺(1,2-EDA),1,3-丙二胺(1,3-PDA),1,4-丁二胺(1,4-BDA)和1,5-二胺基戊烷(1,5-PDA)4种不同碳链长度的直链二胺与氧化石墨烯(GO)进行胺缩合反应(ACR),在GO表面构筑了链接基团,再利用这些经过化学修饰的GO为载体,构筑了染料敏化的光催化剂,研究了它们在可见光辐照下的产氢性能.结果表明,用乙二胺经ACR反应处理的GO呈现出皱褶结构,所制备的催化剂较未处理催化剂的产氢活性高出1.9倍,反应2 h产生1308.6μmol的氢气,而用其它二胺处理过的GO活性并没有明显变化.多种表征方法的结果表明,乙二胺通过ACR反应在GO上形成了具有共轭特性的皱褶官能团,这些官能团缩短了在GO表面电荷传输路径,提高了催化剂的电荷传导能力,催化剂表现出更高的电导率、更长的激子寿命,制氢催化活性也更高.相反,其它二胺不能形成具有共轭特性的官能团,因此催化活性变化不明显,甚至还有降低.结果表明,在GO上修饰适当的官能团是一种构筑高效太阳能光催化制氢催化剂的新策略.The amine condensation reaction(ACR)of graphite oxide(GO)with Ethylenediamine(1,2-EDA),1,3-propanediamine(1,3-PDA),1,4-ethylenediamine(1,4-BDA)and 1,5-diaminopentane(1,5-PDA)were used to synthesize catalyst carriers with linking groups by a one-step hydrothermal synthesis method.Then these chemically modified GOs were used to construct dye-sensitized photocatalysts.Their photocatalytic hydrogen production performances under on visible light irradiation were investigated.The results showed that GO treated with ethylenediamine by ACR reaction showed a wrinkled structure and a 1.9-fold higher hydrogen production activity than the untreated catalyst.The catalyst produced 1308.6μmol of hydrogen in 2 hours.The activity of GO treated with other diamines did not present significant enhanced activities.The characterization results showed that ethylenediamine formed wrinled-like functional groups with conjugate properties on GO through the ACR reaction.These functional groups shorten the charge transfer path on the surface of GO,increased the charge transfer ability,making catalyst exhibiting higher conductivity,longer exciton life and higher hydrogen catalytic activity.The results in this paper indicate that GO with a suitable functional group modification is a new strategy for constructing efficient solar photocatalytic hydrogen production catalysts.

关 键 词：直链二胺 胺缩合 敏化光催化制氢 高导电性 

分 类 号：O643.32[理学—物理化学]