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silicalite-1 crystals.18 A broad range of mesopores were incorporated into the crystals of silicalite-1 via a recrystallization approach to enhance the mass transfer in the composite catalyst and the accessibility of Au. Because of the confinement effect and shape selectivity of silicalite-1, the encapsulated Au nanoparticles ex- hibited excellent stability and resulted in 50% conversion of bioethanol with 98% selectivity toward acetaldehyde formation. In a different study, a core-shell struc- tured Pd@silicalite-1 composite catalyst with Pd nanoparticles (the core) encapsu- lated by a crystal of zeolite silicalite-1 (the shell) was prepared from a solvent-free crystallization.19 Combining the highly activity of Pd nanoparticles and the selectivity of silicalite-1, this composite catalyst exhibited a high furan selectively (98.7%) and furfural conversion (91.3%) for the hydrogenation of furfural at 250C. In contrast, the furan selectivity over conventional silicalite-1-supported Pd nanoparticles (Pd/ silicalite-1) was only 5.6%. Such extraordinary furan selectivity was attributed to the distinguishable mass transfer of the hydrogenated products in zeolite micropores. In summary, zeolites have exhibited outstanding potential for future industrial biomass utilization by taking advantage of their unique Brønsted/Lewis acidic and multifunctional active sites. However, their stability, re-generatability, and product selectivity need to be further improved for these emerging applications. In partic- ular, the catalytic capability of zeolites should be evaluated not only in batch reaction systems but also in scale-up reactors. Different from petroleum-derived chemicals, biomass-derived molecules usually contain a large amount of oxygen, making their catalytic conversions even more challenging. In addition, the reaction mechanisms of many biomass conversions over zeolite catalysts are still unclear. Therefore, comprehensive experimental and theoretical studies toward the biomass conversion mechanisms are needed in the future with the aid of operando characterization and high-level computer modeling. Meanwhile, the product distribution of biomass conversion is rather complex, which requires judicious utilization of the shape selec- tivity of different zeolites. Once their complex structure-activity relationship is revealed, new zeolite catalysts with particular structural features will be rationally designed toward specific catalytic reactions of interest in the future. FUEL CELLS A fuel cell is an electrochemical device that converts chemical energy released by fuel oxidation into electrical energy, being an excellent power source for automobile applications. The working of fuel cells involves many electrochemical processes and component materials. Because of their superior catalytic, adsorption, and separa- tion capabilities, zeolites can be used not only as catalysts for efficient production of fuels (such as hydrogen and methanol) but also as cell component materials (such as electrodes and membranes). Hydrogen is one of the most important fuels for fuel cells. Traditional hydrogen gen- eration methods, such as steam reforming of natural gas, produce a notable amount of impurities along with H2, such as CO, which can poison the electrodes in fuel cells. Developing green methods to efficiently generate pure H2 has attracted much attention. Wang et al.20 developed a facile strategy to synthesize ultrasmall Pd clusters encapsulated within the intersectional channels of nanosized silicalite-1 for highly efficient H2 generation from the complete decomposition of formic acid under mild conditions without generating CO. Notably, the Pd/silicalite-1 catalyst prepared with the introduction of KOH afforded the highest turnover frequency values, reaching up to 856 hr1 at 25C and 3,027 hr1 at 50C, as a result of the 934 Chem 3, 928–949, December 14, 2017PDF Image | Applications of Zeolites in Sustainable Chemistry
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