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将氧化铜纳米颗粒封装在硅沸石-1中作为糠醛转移加氢的可再生催化剂。

Encapsulation of CuO nanoparticles within silicalite-1 as a regenerative catalyst for transfer hydrogenation of furfural.

作者信息

Weng Mingwei, Zhang Zihao, Okejiri Francis, Yan Yue, Lu Yubing, Tian Jinshu, Lu Xiuyang, Yao Siyu, Fu Jie

机构信息

Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, China.

Institute of Zhejiang University - Quzhou, 78 Jiuhua Boulevard North, Quzhou 324000, China.

出版信息

iScience. 2021 Jul 17;24(8):102884. doi: 10.1016/j.isci.2021.102884. eCollection 2021 Aug 20.

Abstract

Catalytic transfer hydrogenation (CTH) of biomass-derived furfural (FAL) to furfuryl alcohol is recognized as one of the most versatile techniques for biomass valorization. However, the irreversible sintering of metal sites under the high-temperature reaction or during the coke removal regeneration process poses a serious concern. Herein, we present a silicalite-1-confined ultrasmall CuO structure (CuO@silicalite-1) and then compared its catalytic efficiency against conventional surface-supported CuO structure (CuO/silicalite-1) toward CTF of FAL with alcohols. Characterization results revealed that CuO nanoparticles encapsulated within the silicalite-1 matrix are ∼1.3 nm in size in CuO@silicalite-1, exhibiting better dispersion as compared to that in the CuO/silicalite-1. The CuO@silicalite-1, as a result, exhibited nearly 100-fold higher Cu-mass-based activity than the CuO/silicalite-1 counterpart. More importantly, the activity of the CuO@silicalite-1 catalyst can be regenerated via facile calcination to remove the surface-bound carbon deposits, unlike the CuO/silicalite-1 that suffered severe deactivation after use and cannot be effectively regenerated.

摘要

生物质衍生的糠醛(FAL)催化转移加氢制糠醇被认为是生物质增值最具通用性的技术之一。然而,高温反应过程中或焦炭去除再生过程中金属位点的不可逆烧结是一个严重问题。在此,我们展示了一种硅沸石-1限制的超小CuO结构(CuO@硅沸石-1),然后将其对FAL与醇的催化转移加氢(CTF)的催化效率与传统表面负载的CuO结构(CuO/硅沸石-1)进行了比较。表征结果表明,封装在硅沸石-1基质中的CuO纳米颗粒在CuO@硅沸石-1中的尺寸约为1.3纳米,与CuO/硅沸石-1相比表现出更好的分散性。因此,CuO@硅沸石-1的基于铜质量的活性比CuO/硅沸石-1对应物高出近100倍。更重要的是,CuO@硅沸石-1催化剂的活性可以通过简单的煅烧再生以去除表面结合的碳沉积物,这与使用后严重失活且无法有效再生的CuO/硅沸石-1不同。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/48fa/8355926/08da2e212951/fx1.jpg

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