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Figure 4. Subnanometric Hybrid Pd-M(OH)2 (M = Ni, Co) Clusters in Zeolite Silicalite-1 as Highly Efficient Nanocatalysts for Hydrogen Generation from Formic Acid Subnanometric hybrid Pd-M(OH)2 clusters were encapsulated within silicalite-1 under direct hydrothermal conditions. The hybrid bimetallic nanocatalysts exhibited shape-selective catalytic performance, superior thermal stability, and exceedingly high dehydrogenation efficiency toward complete formic acid decomposition. Reprinted from Sun et al.21 further reduced Pd cluster size and basic sites introduced in silicalite-1. In addition, the as-synthesized catalysts possessed superior thermal stabilities as well as excellent recycling stabilities as a result of the suitable confinement of Pd clusters within the silicalite-1 matrix. Furthermore, Sun et al.21 prepared a series of subnano- metric hybrid bimetallic clusters Pd-M(OH)2 (M = Ni, Co) within silicalite-1 (Figure 4). The hybrid bimetallic nanocatalysts exhibited excellent shape-selective catalytic performance and thermal stability at 600C–700C because of the stabilization ef- fect from the confinement of zeolite and the bimetallic synergistic effect. In partic- ular, the 0.8Pd0.2Ni(OH)2@silicalite-1 catalyst afforded the highest initial turnover frequency up to 5,803 hr1 toward the decomposition of formic acid without any ad- ditives at 60C. Assuming an operation efficiency of 60%, 1.0 g of the 0.8Pd0.2Ni(OH)2@silicalite-1 catalyst was capable of producing H2 for 4–14 small (0.5–2.0 Wh) proton exchange membrane fuel cell devices. These metal/zeolite composite catalysts are opening new prospects for practical hydrogen storage for fuel cells. Methanol is another important fuel for fuel cells. Traditional methanol production from methane, an abundant greenhouse gas, is an indirect, expensive, and en- ergy-intensive process that needs to overoxidize methane to syngas at extremely high temperature.22 The direct conversion of methane to methanol is a promising alternative for methanol production, but quite challenging because methanol is easier to oxidize than methane. Transition-metal-exchanged zeolites have shown great potential in this process because of their unique metal active sites confined in zeolite pores. For instance, the trinuclear [Cu3(m-O)3]2+ clusters well confined in Cu-exchanged zeolite mordenite (MOR type) could serve as the single-site active centers for the efficient activation of C–H bonds in methane and its subsequent transformation into methanol;23 the exceptional catalytic activity for low-tempera- ture methane-to-methanol conversion over Fe-exchanged beta came from the two Chem 3, 928–949, December 14, 2017 935PDF Image | Applications of Zeolites in Sustainable Chemistry
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