| 表面稳定单质铜的介孔二氧化钛的光催化产氢性能 |
| Stabilizing Metallic Cu0 on the Surface of m-TiO2 for Photocatalytic H2 Production |
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| 摘要: 采用十二烷基硫醇作为保护剂有效地稳定住了光催化过程中介孔二氧化钛(m-TiO2)表面原位生成的Cu0物种。通过X射线衍射,X射线光电子能谱,高分辨透射电镜,高角环形暗场扫描透射电镜等手段对催化剂的组成结构进行了表征,发现催化剂中仅有Cu0物种存在。在紫外光照射下,以甲醛水溶液为牺牲试剂测试了Cu0物种对介孔二氧化钛产氢性能的影响,发现适量的Cu0纳米颗粒能够极大地提高介孔二氧化钛的产氢性能。当Cu0的物质的量分数为1.0%时,Cu0/m-TiO2表现出最高的产氢速率,为725μmol·h-1·g-1。该样品中Cu0纳米颗粒的尺寸为(4.2±0.9)nm。此外,通过气相色谱检测到产生的H2和CO2的物质的量之比为2:1,表明部分氢气来自于水分解。 |
| 关键词: 单质铜 介孔二氧化钛 光催化产氢 甲醛 |
| 基金项目: 国家自然科学基金(No.21271153,21373181,21222307,U1402233),国家自然科学基金重大研究计划(No.91545113)资助项目。 |
| Abstract: Dodecanethiol was introduced as a protective agent to stabilize the in situ generated Cu0 species on the surface of mesoporous TiO2 (m-TiO2). The as-produced samples were characterized by XRD, XPS, HRTEMand HADDF-STEM. It is noteworthy that only Cu0 species were detected in these samples. The system thus served as an excellent model to investigate Cu0-incorporated m-TiO2. Photocatalytic measurements suggested that the Cu0 species could greatly enhance the photocatalytic H2-evolution activity of m-TiO2 in formaldehyde solution. Moreover, we found that the activity depends on the concentration of Cu0. The maximum H2 evolution rate of 725 μmol·h-1·g-1 is obtained on1.0% Cu/m-TiO2, with average Cu0 particle size of (4.2±0.9) nm. It is interesting to find that in our case, the molar ratio of produced H2 to CO2 is 2:1, which indicates the involvement of H2Oas hydrogen source. |
| Keywords: Cu0 species mesoporous TiO2 photocatalytic H2 evolution formaldehyde |
| 投稿时间：2016-03-03 修订日期：2016-03-26 |
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| 刘娟娟,乔培胜,过军芳,邹世辉,肖丽萍,范杰.表面稳定单质铜的介孔二氧化钛的光催化产氢性能[J].无机化学学报,2016,32(6):1063-1070. |
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