The cycloaddition reaction of CO2 with epoxide not only effectively reduces the concentration of CO2 in the atmosphere, but also has excellent industrial application value and up to 100% atom utilization, but there are difficulties in separation and recovery of traditional homogeneous catalysts, harsh reaction conditions of traditional heterogeneous catalysts, and activation of CO2 molecules. In this paper, an easily synthesized heterogeneous catalyst CeNCl/C was used to catalyze the cycloaddition reaction of CO2 with styrene oxide, with a high yield of 92.7%, a high selectivity of 96.7%, a TON value of 349, and a good stability demonstrated in six cycle tests (equivalent to 216 hours of testing). Through comprehensive studies, it was shown that CeNCl/C contains Lewis acid-base centers as active centers, which can effectively reduce the energy barrier required for ring opening of the reaction substrate, enhance the adsorption and activation of CO2, and promote the formation of intermediates, which led to the acquisition of excellent catalytic activity.
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Zeolite-based catalyst hydrocracking of plastics is a potential strategy for mitigating the environmental impacts of plastic wastes and recycling valuable resources, but difficult mass transfer, low concentration of acid sites, and high cost are still barriers to their practical applications. In this paper, we report an excellent hydrocracking catalyst of ZSM-5 nanosheets (Ce/b-ZSM-5) modified by Ce species with high conversion up to 96.3%, C3−C5 selectivity up to 80.9%, and good stability during the hydrogenation of low-density polyethylene. Through comprehensive studies, b-ZSM-5 shows higher molecular diffusion efficiency and acid site concentrations compared with normal ZSM-5 (n-ZSM-5) and hollow ZSM-5 (h-ZSM-5). The introduction of Ce species into b-ZSM-5 further increases the density of Brønsted (B) and Lewis (L) acid sites as active sites, which enhances the adsorption of substrates and facilitates the formation of intermediates and desorption of products. As a result, the hydrocracking activity of Ce/b-ZSM-5 is significantly improved.
One-pot tandem catalysis has been regarded as one of the most atomic economic ways to produce secondary amines, the important platform molecules for chemical synthesis and pharmaceutical manufacture, but it is facing serious issues in overall efficiency. New promotional effects are highly desired for boosting the activity and regulating the selectivity of conventional tandem catalysts. In this work, we report a high-performance tandem catalyst with maximized synergistic effect among each counterpart by preciously manipulating the spatial structure, which involves the active CeO2/Pt component as kernel, the densely-coated N-doped C (NC) layer as selectivity controller, and the differentially-grown Co species as catalytic performance regulators. Through comprehensive investigations, the unique growth mechanism and the promotion effect of Co regulators are clarified. Specifically, the surface-landed Co clusters (Cocs) are crucial to selectivity by altering the adsorption configuration of benzylideneaniline intermediates. Meanwhile, the inner Co particles (Cops) are essential for activity by denoting their electrons to neighboring Ptps. Benefiting from the unique promotion effect, a remarkably-improved catalytic efficiency (100% nitrobenzene conversion with 94% N-benzylaniline selectivity) is achieved at a relatively low temperature of 80 °C, which is much better than that of CeO2/Pt (100% nitrobenzene conversion with 12% N-benzylaniline selectivity) and CeO2/Pt/NC (35% nitrobenzene conversion with 94% benzylideneaniline selectivity).
Electrochemical nitrogen reduction reaction (NRR) paves a new way to cost-efficient production of ammonia, but is still challenging in the sluggish kinetics caused by hydrogen evolution reaction competition and chemical inertness of N≡N bond. Herein, we report a “dual-site” strategy for boosting NRR performance. A high-performance catalyst is successfully constructed by anchoring isolated Fe and Mo atoms on hierarchical N doped carbon nanotubes through a facile self-sacrificing template route, which exhibits a remarkably improved NH3 yield rate of 26.8 μg·h−1·mg