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Figure 5. Two-Step Methane-to-Methanol Conversion Using Water as Oxidant over Cu-Mordenite Schematic representation of the reaction conditions of the partial oxidation of methane by water, involving the reduction of the mono(m-oxo)di-copper site of mordenite and providing two electrons to stoichiometrically oxidize methane into methanol. Subsequent reduction of water into hydrogen returns two electrons for the rejuvenation of the mono(m-oxo)di-copper active site. Reprinted with permission from Sushkevich et al.26 Copyright 2017 AAAS. consecutively formed mononuclear high-spin active sites, FeII and FeIV=O, which were well confined in the distorted 6-rings in beta;24 the Pd-exchanged ZSM-5 with singly dispersed Pd1O4 active sites anchored in the micropores of ZSM-5 exhibited high selectivity and activity in methane-to-methanol conversion through partial oxidation with H2O2.25 Very recently, Sushkevich et al.26 developed an anaerobic direct stepwise method that uses water as the source of oxygen for methane-to-methanol conversion with high selectivity ($97%) over Cu-exchanged mordenite. The whole process consisted of two consecutive steps over the mono(m-oxo)di-copper active sites, i.e., methane oxidation and water reduction, consistently producing 0.2 mol of CH3OH per mol of Cu in Cu-mordenite (Figure 5). Here, water molecules not only acted as a cheap and abundant source of oxygen to partially oxidize methane and regenerate the active sites in Cu-mordenite but also facilitated the desorption of methanol and stabilized the reaction intermediates. With water acting as the oxidant, no molecular oxygen was needed. In comparison with direct oxidation with oxygen leading to high operation temperatures and low yields, such stepped methane-to-methanol conversion routes are expected to receive increasing attention in the near future. Besides being the catalysts for fuel production, zeolites can also be used for building fuel cells. For instance, CeO2-decorated ZSM-5 nanocatalysts could be used to make CeO2/ZSM-5-modified glassy-carbon electrodes for electrochemical oxidation of methanol.27 CeO2/ZSM-5 exhibited approximately three times higher electrocata- lytic activity than commercial Pt(20%)/C catalyst as a result of the good dispersion of CeO2 nanocrystals on the large surface areas of ZSM-5. Moreover, the current density of CeO2(30%)/ZSM-5 remained above 96% even after cycling 1,000 times, whereas commercial Pt(20%)/C could retain only 9% of its original activity. Such a good cycling life was attributed to the catalytic capability of CeO2(30%)/ZSM-5 to convert CO, a reaction intermediate that was poisonous to the Pt electrodes, into CO2. Zeolites can also be used for preparing composite electrolyte membranes to improve the performance of fuel cells because of their high thermal and mechanical stability and tunable hydrophilicity. For instance, perfluorosulfonic acid/zeolite composite membranes could be fabricated for self-humidifying fuel cells that were operable at high temperature in the absence of external humidification.28 In particular, Nafion-117/silicalite-1, Nafion-117/H-ZSM-5, and Nafion-117/H-ZSM-5/ silicalite-1 composite membranes exhibited a much improved glass transition 936 Chem 3, 928–949, December 14, 2017PDF Image | Applications of Zeolites in Sustainable Chemistry
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