王玉营,陈建彪,张旭强,吕功煊.不同直链二胺对敏化石墨烯制氢光催化剂性能的影响[J].分子催化编辑部,2020,34(1):1-7
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
投稿时间:2019-12-10  修订日期:2020-01-12
DOI:
中文关键词:  直链二胺  胺缩合  敏化光催化制氢  高导电性
英文关键词:linear diamine  amine condensation reaction  sensitized photocatalytic hydrogen production  high conductivity
基金项目:国家自然科学基金(11864035,11364036,11474231,11464041,21433007,21673262).
作者单位E-mail
王玉营 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  
陈建彪 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 jbchen@nwnu.edu.cn 
张旭强 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
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 
 
吕功煊 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 gxlu@lzb.ac.cn 
摘要点击次数: 232
全文下载次数: 200
中文摘要:
      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1308.6 μmol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.
英文摘要:
      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 1308.6 μmol 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.
HTML  查看全文  查看/发表评论  下载PDF阅读器