Wang Zhaohua, Dong Chunyang, Tang Xuan, Qin Xuetao, Liu Xingwu, Peng Mi, Xu Yao, Song Chuqiao, Zhang Jie, Liang Xuan, Dai Sheng, Ma Ding
Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, P. R. China.
UCCS-Unité de Catalyse et Chimie du Solide, Université de Lille, CNRS, Centrale Lille, ENSCL, Université d'Artois, UMR, 8181, Lille, France.
Nat Commun. 2022 Jul 29;13(1):4404. doi: 10.1038/s41467-022-32100-x.
Hydrogen storage by means of catalytic hydrogenation of suitable organic substrates helps to elevate the volumetric density of hydrogen energy. In this regard, utilizing cheaper industrial crude hydrogen to fulfill the goal of hydrogen storage would show economic attraction. However, because CO impurities in crude hydrogen can easily deactivate metal active sites even in trace amounts such a process has not yet been realized. Here, we develop a robust RuNi/TiO catalyst that enables the efficient hydrogenation of toluene to methyl-cyclohexane under simulated crude hydrogen feeds with 1000-5000 ppm CO impurity at around 180 °C under atmospheric pressure. We show that the co-localization of Ru and Ni species during reduction facilitated the formation of tightly coupled metallic Ru-Ni clusters. During the catalytic hydrogenation process, due to the distinct bonding properties, Ru and Ni served as the active sites for CO methanation and toluene hydrogenation respectively. Our work provides fresh insight into the effective utilization and purification of crude hydrogen for the future hydrogen economy.
通过对合适的有机底物进行催化氢化来储存氢气，有助于提高氢能的体积密度。在这方面，利用成本较低的工业粗氢来实现储氢目标将具有经济吸引力。然而，由于粗氢中的CO杂质即使含量极少也能轻易使金属活性位点失活，这样的过程尚未实现。在此，我们开发了一种稳健的RuNi/TiO催化剂，该催化剂能够在约180°C的大气压下，在含有1000 - 5000 ppm CO杂质的模拟粗氢进料条件下，将甲苯高效氢化为甲基环己烷。我们表明，还原过程中Ru和Ni物种的共定位促进了紧密耦合的金属Ru - Ni簇的形成。在催化氢化过程中，由于键合性质不同，Ru和Ni分别作为CO甲烷化和甲苯氢化的活性位点。我们的工作为未来氢能经济中粗氢的有效利用和提纯提供了新的见解。
