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层状孔限域的超小铜纳米粒子用于高效氧化 5-羟甲基糠醛。

Hierarchical Pores-Confined Ultrasmall Cu Nanoparticles for Efficient Oxidation of 5-Hydroxymethylfurfural.

机构信息

State Key Laboratory of Pulp and Paper Engineering, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, 510640, P. R. China.

South China University of Technology, Zhuhai Institute of Modern Industrial Innovation, Zhuhai, 519175, P. R. China.

出版信息

ChemSusChem. 2022 Jul 7;15(13):e202200210. doi: 10.1002/cssc.202200210. Epub 2022 Mar 30.

Abstract

Pyrolysis is one of the most widely utilized protocols for the preparation of nanoconfined metal species for heterogeneous catalysis, but it still suffers from the uncontrollable composition evolution process with undesired metal sintering and porous structure collapse. Herein, a novel and versatile molten salt-assisted pyrolysis strategy was demonstrated for the preparation of ultrasmall transition-metal nanoparticles embedded in hollow hierarchical carbon skeletons. The preparation only involved the fabrication of metal-organic framework templates and subsequent pyrolysis with the addition of KCl-KBr molten salt, which played a crucial role in pore size extending and metal sintering inhibiting. Benefitting from the encapsulation effect, the as-synthesized Cu@HHC materials exhibited remarkable catalytic performance and recycling stability in the selective oxidation of biomass-derived 5-hydroxymethylfurfural into 2,5-diformylfuran under mild reaction conditions.

摘要

热解是制备用于多相催化的纳米受限金属物种最广泛应用的方法之一,但它仍然存在组成演变过程不可控的问题,导致金属烧结和多孔结构塌陷。在此,本文提出了一种新颖且通用的熔融盐辅助热解策略,用于制备嵌入中空分级碳骨架中的超小过渡金属纳米颗粒。该制备方法仅涉及金属有机骨架模板的制备,以及添加 KCl-KBr 熔融盐后的后续热解,这在孔径扩展和抑制金属烧结方面发挥了关键作用。得益于封装效应,所合成的 Cu@HHC 材料在温和反应条件下,将生物质衍生的 5-羟甲基糠醛选择性氧化为 2,5-二糠醛的反应中表现出优异的催化性能和回收稳定性。

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