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reported the direction conversion of CO2 into C5+ hydrocarbons with a selectivity of 78.6% and a very low CH4 production (1%) over In2O3/H-ZSM-5 composite catalyst under industrially relevant conditions. The oxygen vacancies on the In2O3 surfaces activated CO2 and H2 to form methanol, and the pores of H-ZSM-5 facilitated the formation of gasoline-range hydrocarbons with a high octane number via CC coupling. The proximity of the two components was believed to be crucial to suppress the undesired reverse water-gas shift reaction. Besides direct hydrogenation, CO2 can transform with CH4 over metal-modified zeolite catalysts into high-value chemicals, representing a promising direction toward the utilization of greenhouse gases. For instance, the direct formation of acetic acid from CO2 and CH4 over Zn/H-ZSM-5 bifunctional catalyst at tempera- tures ranging from 250 to 500C was reported.47 During this reaction, the extra- framework Zn efficiently activated CH4 to form ZnCH3 species, which further formed ZnOOCCH3 species via CO2 insertion, and the Brønsted acid sites in H-ZSM-5 facilitated the final formation of acetic acid by transferring protons to the surface acetate species. Despite all the success, developing composite catalysts with cheap metals that are active for CO2 conversion under mild conditions is still a big challenge. Meanwhile, the exact reaction mechanisms for many CO2 conver- sion processes are still under debate, and require more efforts in the future with the aid of operando characterization and computer modeling techniques. AIR-POLLUTION REMEDIATION With global industrialization, air pollution has become a severe issue that harms human health and the environment. Currently, the main air pollutants include NOx, NH3, and nonmethane volatile organic compounds (VOCs), etc. With their superior adsorption and catalytic capabilities, zeolites are playing an important role in air-pollution remediation. NOx and NH3 NOx (mainly NO and NO2) are produced from combustion of fossil fuels in automo- biles or coal-fired power plants, which can induce acid rain, photochemical smog, and direct damage to the respiratory systems of humans. Among various ‘‘deNOx’’ technologies, the selective catalytic reduction of NOx with NH3 (NH3-SCR: NO + NH3 + O2 / N2 + H2O) is currently the most widely applied. Metal-exchanged zeolite catalysts have played a key role in the development of NH3-SCR technology, such as ZSM-5, Y, mordenite, and beta.53 In comparison with previous NH3-SCR catalysts, zeolites have the advantages of high activity, easy availability, and high stability at different operational temperatures.54 In 2010, Kwak et al.55 synthesized Cu-exchanged zeolite SSZ-13 by using N,N,N-tri- methyl-1-adamantanamine iodide as the template and studied its catalytic performance on NH3-SCR reactions. In comparison with Cu-ZSM-5 and Cu-beta, Cu-SSZ-13 was not only more active over a wide temperature range (160C– 550C) but also more selective toward nitrogen formation, significantly lowering the formation of undesired NO2 and N2O byproducts. Since then, Cu-exchanged CHA-type zeolites have been extensively studied for NH3-SCR reactions. Note that Cu-SSZ-13 has already been commercialized for NOx emission control, and is today’s most common choice in automobile NH3-SCR systems.54 Although the exact mechanisms for NH3-SCR reactions over Cu-exchanged CHA-type zeolites are still not clear, it is generally accepted that this process should involve a reduction half-cycle (CuII / CuI) and an oxidation half-cycle (CuI / CuII) (Figure 8).56 Recent Chem 3, 928–949, December 14, 2017 941PDF Image | Applications of Zeolites in Sustainable Chemistry
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