Product Selectivity Controlled by Nanoporous Environments in Zeolite Crystals Enveloping Rhodium Nanoparticle Catalysts for CO2 Hydrogenation
Product Selectivity Controlled by Nanoporous Environments in Zeolite Crystals Enveloping Rhodium Nanoparticle Catalysts for CO2 Hydrogenation
复制标题
包覆铑纳米粒子催化剂的沸石晶体中的纳米孔环境控制二氧化碳加氢的产物选择性
DOI：
10.1021/jacs.9b01555
复制
发表时间：
2019-05-29
影响因子：
15
通讯作者：
Xiao, Feng-Shou
中科院分区：
文献类型：
--
作者：
Wang, Chengtao;Guan, Erjia;Xiao, Feng-Shou
负载铑纳米颗粒（NPs）是众所周知的催化甲烷化CO，氢化。现在我们证明，选择分子筛晶体作为载体，可以优化该过程的选择性。NPs被包裹在晶体中，具有可控的纳米孔环境，可以调节催化选择性，以最大限度地减少甲烷化，并有利于逆向水气转换反应。纯硅MFI （S-1）固定的铑NPs在高CO2转化率下表现出最大的CO选择性，而铝硅酸盐MFI沸石负载的铑NPs在同等条件下表现出较高的甲烷选择性。纳米孔环境与催化选择性之间存在很强的相关性，表明S-1能最大限度地减少氢溢出，有利于CO的快速解吸，从而限制深度加氢。本课程的材料似乎为各种反应提供了有吸引力的机会来定制选择性负载催化剂。
Supported rhodium nanoparticles (NPs) are well-known for catalyzing methanation in CO, hydrogenation. Now we demonstrate that the selectivity in this process can be optimized for CO production by choice of molecular sieve crystals as supports. The NPs are enveloped within the crystals with controlled nanopore environments that allow tuning of the catalytic selectivity to minimize methanation and favor the reverse water-gas shift reaction. Pure silica MFI (S-1)-fixed rhodium NPs exhibited maximized CO selectivity at high CO2 conversions, whereas aluminosilicate MFI zeolite-supported rhodium NPs displayed high methane selectivity under the equivalent conditions. Strong correlations were observed between the nanoporous environment and catalytic selectivity, indicating that S-1 minimizes hydrogen spillover and favors fast desorption of CO to limit deep hydrogenation. Materials in this class appear to offer appealing opportunities for tailoring selective supported catalysts for a variety of reactions.