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Title: Zeolite‐Encaged Pd‐Mn Nanocatalysts for CO2 Hydrogenation and Formic Acid Dehydrogenation
Authors: SUN QIMING 
Chen, Benjamin WJ
Wang, Ning
Chang, Albert
Yang, Chia-Min
Asakura, Hiroyuki
Tanaka, Tsunehiro
Hülsey, Max J
Yu, Jihong
Yan Ning 
Issue Date: 7-Aug-2020
Publisher: Wiley
Citation: SUN QIMING, Chen, Benjamin WJ, Wang, Ning, HE QIAN, Chang, Albert, Yang, Chia-Min, Asakura, Hiroyuki, Tanaka, Tsunehiro, Hülsey, Max J, WANG CHI-HWA, Yu, Jihong, Yan Ning (2020-08-07). Zeolite‐Encaged Pd‐Mn Nanocatalysts for CO2 Hydrogenation and Formic Acid Dehydrogenation. Angewandte Chemie International Edition. ScholarBank@NUS Repository.
Abstract: CO2-mediated hydrogen storage energy cycle is a promising way to implement the hydrogen economy, but the exploration of efficient catalysts to achieve this process remains challenging. Herein, sub-nanometer Pd-Mn clusters were encaged within silicalite-1 (S-1) zeolites by a ligand-protected method under direct hydrothermal conditions. The obtained zeolite-encaged metallic nanocatalysts exhibited extraordinary catalytic activity and durability in both CO2 hydrogenation into formate and formic acid (FA) dehydrogenation back to CO2 and hydrogen. Thanks to the formation of ultrasmall metal clusters and the synergic effect of bi-metallic components, the PdMn0.6@S-1 catalyst afforded a formate generation rate of 2151 molformate molPd-1 h-1 at 353 K, and an initial turnover frequency of 6860 molH2 molPd-1 h-1 for CO-free FA decomposition at 333 K without any additive. Both values represent the top levels among the state-of-the-art heterogeneous catalysts under similar conditions. This work demonstrates that zeolite-encaged metallic catalysts hold great promise to realize CO2-mediated hydrogen energy cycles in the future featuring fast charging and releasing kinetics. Introduction Hydrogen (H2) is an environmental-friendly and high energy density fuel,[1] yet developing reliable and efficient H2 storage systems remains a challenge.[2] Among various strategies for H2
Source Title: Angewandte Chemie International Edition
ISSN: 1433-7851
DOI: 10.1002/anie.202008962
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