Stable copper-based metal–organic framework-supported Pt–Bi nanoparticles for selective oxidation of glycerol into dihydroxyacetone†

IF 4.2 3区 化学 Q2 CHEMISTRY, PHYSICAL
Liang Lv, Tao Chen, Chaohui Guan, Jing Yu, Yijing Pian, Zihan Ma, Junfeng Du, Shuai Zhang, Hang Wei and Haibin Chu
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Abstract

The selective oxidation of glycerol into high-value-added products (e.g., dihydroxyacetone, DHA) has attracted much attention. However, it is still constrained by low DHA selectivity (≤60%) under high glycerol conversion. Herein, we report a Pt–Bi nanoparticle catalyst supported on Cu-based metal–organic frameworks (Cu-MOFs, HKUST-1). Cu-MOF as a support promotes electron transfer from the support to Pt–Bi and inhibits the decomposition of DHA. In situ FTIR, O2-TPD, kinetic experiments, EPR experiments, and fluorescence spectroscopy techniques show that Cu-MOF with rich microporous structure can promote oxygen adsorption and water dissociation and enhance the strong adsorption capacity of glycerol and the ability to generate abundant OH*, which is conducive to accelerating the conversion of glycerol to DHA. Consequently, Pt–Bi/Cu-MOF maintains considerable DHA selectivity (68.8%) even at a high glycerol conversion (94.2%), gaining a high yield of DHA (62.9%). Importantly, the stability of the Cu-MOF support as well as the intense metal–support interaction ensures the stability of the catalyst, which keeps superior glycerol oxidation performance after 10 reaction cycles.

Abstract Image

稳定的铜基金属-有机框架-支持Pt-Bi纳米颗粒选择性氧化甘油成二羟基丙酮†
甘油选择性氧化成高附加值产品(如二羟基丙酮、DHA)引起了人们的广泛关注。然而,在高甘油转化率下,它仍然受到低DHA选择性(≤60%)的限制。本文报道了一种基于cu基金属有机骨架(Cu-MOFs, HKUST-1)的Pt-Bi纳米颗粒催化剂。Cu-MOF作为载体促进电子从载体转移到Pt-Bi,抑制DHA的分解。原位FTIR、O2-TPD、动力学实验、EPR实验和荧光光谱技术表明,Cu-MOF具有丰富的微孔结构,可以促进氧吸附和水解离,增强了对甘油的强吸附能力和生成丰富OH*的能力,有利于加速甘油向DHA的转化。因此,Pt-Bi /Cu-MOF即使在高甘油转化率(94.2%)下也能保持相当高的DHA选择性(68.8%),从而获得高DHA收率(62.9%)。重要的是,Cu-MOF载体的稳定性以及强烈的金属-载体相互作用确保了催化剂的稳定性,在10个反应循环后仍保持优越的甘油氧化性能。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Catalysis Science & Technology
Catalysis Science & Technology CHEMISTRY, PHYSICAL-
CiteScore
8.70
自引率
6.00%
发文量
587
审稿时长
1.5 months
期刊介绍: A multidisciplinary journal focusing on cutting edge research across all fundamental science and technological aspects of catalysis. Editor-in-chief: Bert Weckhuysen Impact factor: 5.0 Time to first decision (peer reviewed only): 31 days
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