石墨烯助剂与Ni(Ⅱ)活性位点协同增强TiO2制氢性能
Synergistic Effect of Graphene as Electron-Transfer Mediator and Ni (Ⅱ) as Interfacial Catalytic Active Site for Enhanced H2-Production Performance of TiO2
作者单位E-mail
张超颖 武汉理工大学化学化工与生命科学学院应用化学系, 武汉 430070  
王苹 武汉理工大学化学化工与生命科学学院应用化学系, 武汉 430070 wangping0904@whut.edu.cn 
刘岩岩 武汉理工大学化学化工与生命科学学院应用化学系, 武汉 430070  
胡灵娜 武汉理工大学化学化工与生命科学学院应用化学系, 武汉 430070  
摘要: 采用水热法和低温浸渍法制备了电子助剂还原石墨烯(rGO)和界面活性位点Ni(Ⅱ)共修饰的高效TiO2光催化剂(简称Ni(Ⅱ)/TiO2-rGO)。制氢性能测试结果表明:相比于TiO2和单独还原石墨烯复合的TiO2,经还原石墨烯与Ni(Ⅱ)协同修饰后的TiO2表现出更高的光催化制氢性能。其中,Ni(Ⅱ)/TiO2-rGO(0.1 mol·L-1)具有最高制氢性能,制氢速率达到77.0 μmol·h-1,分别是TiO2(16.4 μmol·h-1)和TiO2-rGO(28.0 μmol·h-1)的4.70倍和2.75倍。还原石墨烯助剂与Ni(Ⅱ)活性位点协同增强制氢性能的原理是:还原石墨烯作为电子助剂可以快速捕获和传输电子,Ni(Ⅱ)作为界面活性位点可以从溶液中捕获H+,提高界面反应速率,2种助剂协同作用加快了TiO2上的光生电子-空穴对的有效分离。
关键词: TiO2  协同效应  还原石墨烯  电子助剂  Ni(Ⅱ)  界面活性位点
基金项目: 国家自然科学基金(No.21477094)和国家级大学生创新创业训练计划项目(No.20161049720001)资助
Abstract: Highly efficient TiO2 photocatalysts co-modified by reduced graphene oxide (rGO) as electron-transfer mediator and Ni (Ⅱ) as interfacial catalytic active-sites (referred to as Ni (Ⅱ)/TiO2-rGO) were synthesized via a two-step process including the initial hydrothermal method of rGO on the TiO2 surface and the following low-temperature impregnation method of Ni (Ⅱ) on the rGO.Photocatalytic experimental results indicated that all resulted Ni (Ⅱ)/TiO2- rGO photocatalysts exhibited obviously high H2-production performance.The highest H2-production rate of the resultant Ni (Ⅱ)/TiO2-rGO (0.1 mol·L-1) reached 77.0 μmol·h-1,while this value was higher than that of the TiO2(16.4 μmol·h-1) and TiO2-rGO (28.0 μmol·h-1) by a factor of 4.70 and 2.75,respectively.On the basis of the experimental results,a synergistic effect mechanism of rGO and Ni (Ⅱ) bi-cocatalysts was proposed to account for its enhanced H2-production performance,namely,rGO functions as an electron-transfer mediator to rapidly capture and transfer the photogenerated electron from TiO2 surface,while the Ni (Ⅱ) cocatalyst serves as an effectively active site for the following reduction.
Keywords: TiO2  synergistic effect  reduced graphene oxide (rGO)  electron-transfer mediator  Ni(Ⅱ)  interfacial catalytic active-site
投稿时间:2017-03-21 修订日期:2017-06-15
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张超颖,王苹,刘岩岩,胡灵娜.石墨烯助剂与Ni(Ⅱ)活性位点协同增强TiO2制氢性能[J].无机化学学报,2017,33(7):1132-1138.
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