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Revamping SiO_2 Spheres by Core-Shell Porosity Endowment to Construct a Mazelike Nanoreactor for Enhanced Catalysis in CO_2 Hydrogenation to Methanol

机译:Revamping SiO_2 Spheres by Core-Shell Porosity Endowment to Construct a Mazelike Nanoreactor for Enhanced Catalysis in CO_2 Hydrogenation to Methanol

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摘要

Beyond the catalytic activity of nanocatalysts, the support with architectural design and explicit boundary could also promote the overall performance through improving the diffusion process, highlighting additional support for the morphology-dependent activity. To delineate this, herein, a novel mazelike-reactor framework, namely multi-voids mesoporous silica sphere (MVmSiO(2)), is carved through a top-down approach by endowing core-shell porosity premade Stober SiO2 spheres. The precisely-engineered MVmSiO(2) with peripheral one-dimensional pores in the shell and interconnecting compartmented voids in the core region is simulated to prove combined hierarchical and structural superiority over its analogous counterparts. Supported with CuZn-based alloys, mazelike MVmSiO(2) nanoreactor experimentally demonstrated its expected workability in model gas-phase CO2 hydrogenation reaction where enhanced CO2 activity, good methanol yield, and more importantly, a prolonged stable performance are realized. While tuning the nanoreactor composition besides morphology optimization could further increase the catalytic performance, it is accentuated that the morphological architecture of support further boosts the reaction performance apart from comprehensive compositional optimization. In addition to the found morphological restraints and size-confinement effects imposed by MVmSiO(2), active sites of catalysts are also investigated by exploring the size difference of the confined CuZn alloy nanoparticles in CO2 hydrogenation employing both in-situ experimental characterizations and density functional theory calculations.

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