Combining shell confinement and outside decoration to boost the selectivity of Pt nanocatalysts in hollow-flower like Zr-MOFs double shell micro-reactor for hydrogenation cinnamaldehyde to unsaturated alcohol

纳米材料基催化剂 肉桂醛 壳体(结构) 选择性 肉桂醇 材料科学 纳米技术 化学工程 化学 纳米颗粒 催化作用 复合材料 有机化学 工程类
作者
Bingzhen Zhang,Meiyan Li,Huijin Lei,Jialiang Chen,Shuhua Wang,Chao Chen
出处
期刊:Applied Surface Science [Elsevier BV]
卷期号:599: 153899-153899 被引量:39
标识
DOI:10.1016/j.apsusc.2022.153899
摘要

A fabulous hollow flower-like heterogeneous catalysis of Void@UiO-66-NH 2 @Pt@UiO-66- NO 2 utilizing UiO-66-NH 2 as the core, evenly anchoring the Pt NPs (ca. 1.74 nm), and growing the UiO-66-NH 2 , matching the channel size of the reactant molecule, as the outer shell was fabricated, and effectively displayed marvelous selectivity and conversion in the hydrogenation of CAL. • A hollow flower-like Pt/Zr-MOF nanosphere has been fabricated by MHT approach. • The flower-like and hollow structure can accelerate the reaction mass transfer rate. • UiO-66-NH 2 enables Pt NPs (ca. 1.74 nm) evenly dispersed within the matrix of the inner shell. • UiO-66 shell possesses the matching channel window with the size of cinnamaldehyde reactant. • The catalyst delivered the efficient catalytic performance in the hydrogenation of cinnamaldehyde. Rational design of the heterogeneous micro-environment with subtle engineering in catalyst preparation is crucial for inorganic materials to boost catalytic efficiency. Here, we designed a hollow-flower like Zr-MOF double-shell nanosphere to confine Pt nanocatalysts, decorating with functional groups such as -H, -NH 2 , -Br and NO 2 on shell, and employed as catalytic micro-reactors for hydrogenation of cinnamaldehyde. They were featured as Void@UiO-66-NH 2 @Pt@UiO-66-X (X = H, NH 2 , Br, NO 2 ) with ultra-fine Pt nanocatalysts (ca. 1.7 nm) arched on inner UiO-66-NH 2 shell. By comparing the catalytic efficiency of the samples with different groups, it was demonstrated that the double-shell with outside decoration is not only functional as stabilizer to confine Pt nanoparticles in high dispersion, also as the sieve to control the access direction of cinnamaldehyde to Pt site in view of the channel in moderate size formed on the outer shell; by changing the decoration groups on the outer shell, above advances could be further intensified with the enhanced mass-transformation. The Void@UiO-66-NH 2 @Pt@UiO-66-NO 2 greatly boost the yield of unsaturated alcohol in outstanding selectivity (95%). Therefore, the combination of shell confinement and outside decoration present on the Pt-embedded Zr-MOFs could be an attractive design for advanced applications.
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