Bifunctional Pd-Pt Supported Nanoparticles for the Mild Hydrodeoxygenation and Oxidation of Biomass-Derived Compounds.

IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY ChemSusChem Pub Date : 2025-01-02 DOI:10.1002/cssc.202402641
Vincenzo Ruta, Luis A Cipriano, Giovanni Di Liberto, Robert Wojcieszak, Gianvito Vilé
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Abstract

The conversion of bio-based molecules into valuable chemicals is essential for advancing sustainable processes and addressing global resource challenges. However, conventional catalytic methods often demand harsh conditions and suffer from low product selectivity. This study introduces a series of bifunctional PdxPty catalysts supported on TiO2, designed for achieving selective and mild-temperature catalysis in biomass conversion. Synthesized via a sol immobilization method and characterized by XRF, N2 physisorption, HRTEM, HAADF-STEM, and XPS, these catalysts demonstrate superior selectivity and activity over monometallic counterparts. In fact, at 20 bar H2, Pt/TiO2 show a low selectivity in benzophenone hydrodeoxygenation, favoring the benzhydrol hydrogenation product; similarly, Pd/TiO2 preferentially form the diphenylmethane hydrodeoxygenation (HDO) product, but with slow conversion rates. The synergistic combination of the two metals in Pd4Pt1/TiO2 drastically improve performance, with 100 % benzophenone conversion and 73 % diphenylmethane selectivity. DFT calculations confirm the synergy between Pd and Pt as the key to drive the activity and selectivity. Additionally, the catalysts also demonstrate high recyclability with minimal performance loss, and have been generalized for the HDO of vanillin and furfural, and in HMF oxidation. Overall, this work highlights the potential of bimetallic catalysts in enabling efficient and selective bio-based molecule conversion under mild conditions.

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双功能Pd-Pt负载纳米颗粒用于生物质衍生化合物的轻度加氢脱氧和氧化。
将生物基分子转化为有价值的化学品对于推进可持续工艺和应对全球资源挑战至关重要。然而,传统的催化方法往往需要苛刻的条件,而且产品选择性低。本研究介绍了一系列以 TiO2 为载体的双功能 PdxPty 催化剂,旨在实现生物质转化过程中的选择性和低温催化。这些催化剂是通过溶胶固定法合成的,并通过 XRF、N2 物理吸附、HRTEM、HAADF-STEM 和 XPS 进行表征。在 20 bar H2 条件下,Pt/TiO2 在二苯甲酮加氢脱氧反应中的选择性较差,更倾向于加氢产物苯海醇的形成;事实上,Pd/TiO2 更倾向于生成 HDO 产物二苯基甲烷,但转化率较慢。然而,Pd4Pt1/TiO2 中两种金属的协同组合大大提高了性能,二苯甲酮转化率达到 100%,二苯甲烷选择性达到 73%。DFT 计算证实了双金属体系在推动选择性方面的作用。此外,催化剂还具有很高的可回收性,性能损失极小,对香兰素和糠醛的 HDO 以及 HMF 氧化有效。总之,这项工作凸显了双金属催化剂在更温和、更高效的生物基分子转化方面的潜力。
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
ChemSusChem
ChemSusChem 化学-化学综合
CiteScore
15.80
自引率
4.80%
发文量
555
审稿时长
1.8 months
期刊介绍: ChemSusChem Impact Factor (2016): 7.226 Scope: Interdisciplinary journal Focuses on research at the interface of chemistry and sustainability Features the best research on sustainability and energy Areas Covered: Chemistry Materials Science Chemical Engineering Biotechnology
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