多孔二维单层氧化物负载低含量Au水气变换催化剂的设计制备及稳定性研究

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中文摘要
水气变换(WGS)反应是制氢的经典途径,被认为是连接碳氢燃料和氢燃料电池的纽带,关键是开发高性能的催化剂。Au系WGS催化剂被认为是氢燃料电池体系最有商业化前景的催化剂之一,但Au是贵金属,降低其用量并保持高性能是难题。本项目提出利用二维超薄材料的单层超薄结构和多孔特性,解决传统载体对金属分散能力差、内部“热电子”迁移路径长、传质阻力大等缺点,利用二维载体层间限域效应、表面缺陷效应解决Au纳米粒子易团聚的难题。拟通过水热法和液相剥离法,设计制备多孔二维单层氧化物载体(TiO2、Co3O4、CeO2),负载高分散、低含量Au,调控制备出高性能“单层载体”Au系WGS催化剂。发展二维载体、Au系催化剂的调控制备方法,揭示催化剂微结构—表面性质—热电流—活性—稳定性之间的构效关系,阐明二维超薄载体效应和热电流反应机理,期望为适用于燃料电池体系的高性能Au系催化剂开发提供新思路和研究基础。
英文摘要
The water-gas shift (WGS, CO + H2O = CO2 + H2) reaction is a classical industrial reaction to economically get large-scale pure hydrogen, since the WGS reaction is considered as the key link between hydrocarbon fuel and hydrogen fuel cell. The highly efficient catalysts play a key role in the hydrogen production process from WGS reaction. The supported gold catalysts have been considered as the most likely candidate of commercialization. However, due to the high price of gold, the significant challenges are the decreasing of gold loading and the remaining of highly catalytic performance. In the present project, with the help of single-layered ultrathin structures and porous properties of ultrathin two-dimensional (2D) materials, the shortages of the classical supports will be solved, such as the poor dispersive capacity of supports for active metals, long path of inner hot-electrons migration and slow mass-transfer. The agglomeration problem of Au nanoparticles will be overcame by taking advantages of interlayer confinement effect and surface defect engineering. A series of 2D single-layered oxides (TiO2, Co3O4, CeO2) as the supports will be controllably synthesized by hydrothermal methods or exfoliation in solution. After less loading of highly dispersed gold as active composition, the highly efficient gold supported on “single-layered supported” WGS catalysts will be controllably synthesized. Finally, the controllable synthesis methods of the ultrathin 2D supports and the supported gold catalysts will be developed. Their structure-performance relationships between catalyst’s microstructures, surface properties, activities, hot-electron flow efficiencies and stabilities will be discussed and uncovered. The 2D ultrathin support effect and “hot-electron flow” mechanism will be clarified. The results will open avenues for the development of the highly efficient supported gold WGS catalysts for the application of fuel cell systems.
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Role of percentage of {001} crystal facets in TiO2 supports toward the water-gas shift reaction over Au-TiO2 catalysts
TiO2 载体中 {001} 晶面的百分比对 Au-TiO2 催化剂上水煤气变换反应的作用
DOI:10.1016/j.cej.2022.137010
发表时间:2022-05
期刊:Chemical Engineering Journal
影响因子:15.1
作者:Pang Qianqian;Zhong Xiaohong;Yan Wensi;Ma Hui;Ren Hongju;Song Li;Lv Zhenguo;Li Lei;Chen Chen;Wang Haidong;Lin Xingyi;Zhang Qiaohong
通讯作者:Zhang Qiaohong
DOI:10.1016/j.surfin.2023.103729
发表时间:2024-01
期刊:Surfaces and Interfaces
影响因子:6.2
作者:Yan Sang;Guohong Li;Jingwei Xue;Junjie Hu;Yaxin Tong;Biao Liang;Lei Li
通讯作者:Yan Sang;Guohong Li;Jingwei Xue;Junjie Hu;Yaxin Tong;Biao Liang;Lei Li
DOI:10.1016/j.cej.2023.146084
发表时间:2023-09
期刊:Chemical Engineering Journal
影响因子:15.1
作者:Tianji Ma;Shuqi Tan;Rongyao Yuan;Xuan Kang;Peixian Guo;Yaxin Tong;Tingting Zhao;Zhongliang Xiao;Zhong Cao;Lei Li;Sebastien Balme
通讯作者:Tianji Ma;Shuqi Tan;Rongyao Yuan;Xuan Kang;Peixian Guo;Yaxin Tong;Tingting Zhao;Zhongliang Xiao;Zhong Cao;Lei Li;Sebastien Balme
DOI:--
发表时间:2023
期刊:化学试剂
影响因子:--
作者:马惠;宋利;于彦龙;李雷
通讯作者:李雷
DOI:10.1016/j.cej.2023.145650
发表时间:2023-08-28
期刊:CHEMICAL ENGINEERING JOURNAL
影响因子:15.1
作者:Hong,Zhe;Xiong,Chuanfang;Zhu,Zhirong
通讯作者:Zhu,Zhirong
基于 MoS2 仿生性的管式一体化电极及其电催
化氧化硫醚
- 批准号:Z24B060001
- 项目类别:省市级项目
- 资助金额:0.0万元
- 批准年份:2024
- 负责人:李雷
- 依托单位:
高性能氧化锆基二氧化碳加氢催化剂的氧空位稳定性与毗邻界面精准调控
- 批准号:--
- 项目类别:面上项目
- 资助金额:54万元
- 批准年份:2022
- 负责人:李雷
- 依托单位:
多孔二维单层TiO2基水煤气变换催化剂及其热电流增强机理
- 批准号:LY19B030005
- 项目类别:省市级项目
- 资助金额:0.0万元
- 批准年份:2018
- 负责人:李雷
- 依托单位:
“黑”TiO2基水气变换催化剂的制备及其热电流传输行为的改性研究
- 批准号:21503092
- 项目类别:青年科学基金项目
- 资助金额:21.0万元
- 批准年份:2015
- 负责人:李雷
- 依托单位:
国内基金
海外基金
