单位接TiO2,具有可见光生产的多种协调环境
Pu Zhang1, Haihua Zeng1, Decai Wen2
1State Key Lab of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, P. R. China.
ChemSusChem
|September 28, 2023
概括
为高效的太阳能气生产开发了单站式接种的二氧化 (TiO2) 光催化剂. 最佳催化剂表明演化反应 (HER) 速率增加了260倍,突显了定制活点的重要性.
科学领域:
- 材料科学 材料科学 材料科学
- 光催化作用的光催化
- 可再生能源可再生能源是可再生能源.
背景情况:
- 高效的太阳能气生产对于解决能源危机至关重要.
- 在光催化剂上操纵活性位点的微环境显著提高了催化性能.
- 单站式催化剂可以精确控制活动站点协调和电子属性.
研究的目的:
- 构建精确定义的单位Ni-移植TiO2光催化剂,具有可见光诱导的光催化演化反应 (HER) 的特定协调环境.
- 调查 Ni 活跃站点的协调环境与 HER 性能之间的结构-活动关系.
- 阐明对增强光催化活性负责的潜在机制.
主要方法:
- 表面有机金属化学与表面连接物交换相结合,合成T-Ni Bpy和T-Ni Phpy光催化剂.
- 可见光诱导的光催化演化反应 (HER) 测量.
- 电子偏磁共振 (EPR) 和秒瞬态红外吸收光谱分析电荷载体动态和缺陷状态.
主要成果:
- 最优的催化剂2.2'-双二-Ni-O-TiO2 (T-Ni Bpy) 实现了显著的HER速率33.82 μmol·g−1·h−1和0.451 h−1的Ni的周转频率.
- 与Ni-O-TiO2.2.相比,T-Ni Bpy催化剂的HER活性是Ni-O-TiO2.2的260倍.
- 鉴定结果显示,T-Ni Bpy中电子捕获氧空缺较少,长寿命光生成电子 (>3 ns,~52.9%) 的比例较大,与增强的HER活性相关.
结论:
- 精确定义的单位Ni-移植TiO2光催化剂,具有特定的协调环境,可以显著增强可见光驱动的HER.
- 由于优化电子特性和减少电荷载体重组,T-Ni Bpy催化剂表现出卓越的性能.
- 从Ni光吸收器注入到TiO2导电带的长寿命自由电子的数量是决定优秀HER活性的一个关键因素.
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