Hollow Zeolites Encapsulating Ultra-Low Noble Metal Nanoparticles for HMF Oxidation
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Hollow Zeolites Encapsulating Ultra‑Low Noble Metal Nanoparticles for HMF Oxidation Shilpi Saxena1 · Dhyananand Yadaw1 · Kajal Tiwari2 · V. Venkatesh3 · Sandeep Verma3,5 · Raj Ganesh S. Pala1,4 · Sri Sivakumar1,4,5 Received: 14 May 2020 / Accepted: 18 August 2020 © Springer Science+Business Media, LLC, part of Springer Nature 2020
Abstract We report the development of zeolite nanocapsules (MCM-22 and ZSM-5) encapsulating ultra-low amount (0.01 wt%) of noble metal nanoparticles (Gold, Platinum and Palladium) for the oxidation of HMF. These catalysts showed enhanced HMF conversion (> 95%) with higher yield (> 90%) of FDCA under mild conditions (60 °C, 0.3 MPa oxygen) in an organic solvent-free medium in 6 h. We also investigated the effect of size and amount of gold nanoparticles encapsulated inside zeolite capsules for the oxidation of HMF. We found that Au cluster loaded MCM-22 showed enhanced HMF conversion and yield of FDCA (91%). Graphic Abstract
Keywords Nanoparticles · Zeolites · Encapsulation · Ultra low loading · HMF oxidation · High activity
Electronic supplementary material The online version of this article (https://doi.org/10.1007/s10562-020-03361-2) contains supplementary material, which is available to authorized users. * Sri Sivakumar [email protected] 1
Department of Chemical Engineering, Indian Institute of Technology, Kanpur, UP 208016, India
Department of Chemical Engineering, Banasthali University, Rajasthan 304022, India
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Department of Chemistry, Indian Institute of Technology, Kanpur, UP 208016, India
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Materials Science Program, Indian Institute of Technology Kanpur, Kanpur, UP 208016, India
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Thematic Unit of Excellence on Soft Nanofabrication, Indian Institute of Technology, Kanpur, UP 208016, India
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1 Introduction The catalytic conversion of biomass has gained huge popularity as it provides an alternative route for producing non-fossil-feed-based chemicals or liquid fuels and thus potentially reducing the dependence on petroleumbased resources [1–3]. One such example is oxidation of 5-Hydroxymethylfurfural (HMF), which is synthesized by dehydration of fructose or glucose [4, 5]. The catalytic oxidation produces two potential bio- renewable chemicals, 2,5-furandicarboxylic acid (FDCA) and 2,5-diformylfuran (DFF) [6, 7]. FDCA is listed as one of the most important biomass-derived chemical, as declared by the U.S. Department of Energy, as it is an alternative for terephthalic acid (derived from petroleum fractions), in the production of polyesters [8, 9]. In the past decades, strong oxidants (e.g. permanganate, chromate and dichromate) were employed for oxidation of HMF [10]. However, such oxidants are not expensive but also toxic and leaving behind a lot of by-products after usage and also give a low yield of FDCA (Scheme 1). Alternatively, homogeneous catalysts (e.g., Co(OAc)2/ Zn(OAc)2/Br−, Co/Mn/Zr/Br) have been used in the aerobic oxidation of HMF to FDCA at high temperatures (373–498 K) [10, 11]. However, it yielded DFF rather
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