论文标题
用单位Ti催化剂在石墨烯上氢溢出和储存
Hydrogen spillover and storage on graphene with single-site Ti catalysts
论文作者
论文摘要
单位金属催化剂的氢溢出和储存，包括单原子催化剂（SAC）和单纳米簇催化剂，已被阐明用于各种载体，但对惰性碳载体的理解仍然不足。在这里，我们使用基于同步加速器辐射的方法研究单位Ti催化剂在石墨烯中在氢溢出和存储中的作用。我们的原位角度分辨光发射光谱的结果表明带隙开口，X射线吸收光谱揭示了C-H键的形成，这都表明部分石墨烯氢化。随着Ti沉积和H2暴露的增加，Ti原子倾向于聚集形成纳米簇催化剂，并产生13.5％SP3杂交碳原子，对应于1.11 wt％的氢储存能力（不包括Ti纳米升温器的重量[1]）。我们的结果表明，TI SAC的简单溢出过程如何导致石墨烯上的共价氢键，从而为碳支持的单位催化剂的合理设计提供了策略。
Hydrogen spillover and storage for single-site metal catalysts, including single-atom catalysts (SACs) and single nanocluster catalysts, have been elucidated for various supports but remain poorly understood for inert carbon supports. Here, we use synchrotron radiation-based methods to investigate the role of single-site Ti catalysts on graphene for hydrogen spillover and storage. Our in-situ angle-resolved photoemission spectra results demonstrate a bandgap opening and the X-ray absorption spectra reveal the formation of C-H bonds, both indicating the partial graphene hydrogenation. With increasing Ti deposition and H2 exposure, the Ti atoms tend to aggregate to form nanocluster catalysts and yield 13.5% sp3-hybridized carbon atoms corresponding to a hydrogen-storage capacity of 1.11 wt% (excluding the weight of the Ti nanoclusters [1]). Our results demonstrate how a simple spillover process at Ti SACs can lead to covalent hydrogen bonding on graphene, thereby providing a strategy for a rational design of carbon-supported single-site catalysts.
