State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029, P. R. China.
Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang, 110016, P. R. China.
Nat Commun. 2023 Jun 2;14(1):3189. doi: 10.1038/s41467-023-38883-x.
The metal-support interaction (MSI) in heterogeneous catalysts plays a crucial role in reforming reaction to produce renewable hydrogen, but conventional objects are limited to single metal and support. Herein, we report a type of RhNi/TiO catalysts with tunable RhNi-TiO strong bimetal-support interaction (SBMSI) derived from structure topological transformation of RhNiTi-layered double hydroxides (RhNiTi-LDHs) precursors. The resulting 0.5RhNi/TiO catalyst (with 0.5 wt.% Rh) exhibits extraordinary catalytic performance toward ethanol steam reforming (ESR) reaction with a H yield of 61.7%, a H production rate of 12.2 L h g and a high operational stability (300 h), which is preponderant to the state-of-the-art catalysts. By virtue of synergistic catalysis of multifunctional interface structure (Rh-Ni-O-Ti; O denotes oxygen vacancy), the generation of formate intermediate (the rate-determining step in ESR reaction) from steam reforming of CO and CH is significantly promoted on 0.5RhNi/TiO catalyst, accounting for its ultra-high H production.
在多相催化剂中，金属-载体相互作用（MSI）在重整反应中生成可再生氢气方面起着至关重要的作用，但传统的研究对象仅限于单一金属和载体。在此，我们报告了一种 RhNi/TiO 催化剂，其具有可调的 RhNi-TiO 强双金属-载体相互作用（SBMSI），源自 RhNiTi 层状双氢氧化物（RhNiTi-LDHs）前体的结构拓扑转变。所得的 0.5RhNi/TiO 催化剂（负载 0.5wt.% Rh）在乙醇蒸汽重整（ESR）反应中表现出非凡的催化性能，H 产率为 61.7%，H 生成速率为 12.2 L h g，且具有高的操作稳定性（300 h），优于最先进的催化剂。凭借多功能界面结构（Rh-Ni-O-Ti；O 表示氧空位）的协同催化作用，0.5RhNi/TiO 催化剂上显著促进了来自 CO 和 CH 蒸汽重整的甲酸盐中间产物（ESR 反应中的速率决定步骤）的生成，这解释了其超高的 H 生成率。
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