Manganese-Biochar Catalyst for Sustainable Glycolic Acid Production from Biomass-Derived Glucose and Oligosaccharides

IF 7.1 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Sustainable Chemistry & Engineering Pub Date : 2024-10-23 DOI:10.1021/acssuschemeng.4c06938

Qiaozhi Zhang, Yang Cao, Zibo Xu, Hanwu Lei, Xiaoguang Duan, James H. Clark, Daniel C. W. Tsang

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Abstract

Production of glycolic acid from renewable resources is a significant challenge considering its extensive market and the depletion of fossil resources. This study accomplished sustainable glycolic acid production from biomass-derived saccharides using a microwave-assisted aerobic oxidation system. Various Mn-biochar catalysts were synthesized using different precursors (MnCl₂ and KMnO₄) and synthesis temperatures (400–850 °C). Glycolic acid yield from glucose could reach 62.8 Cmol % within 20 min at 180 °C over MnBC-VII-700 (i.e., catalyst derived from Mn(VII) precursor and synthesized at 700 °C). Mn(III) was identified as the catalytically active state by correlation with the catalytic performance. Biochar support is vital for reactant adsorption, electron transfer, and microwave absorption. Transformation from glucose to glycolic acid would experience retro-aldol and oxidation reactions, while oxidation-hydrolysis of the glycosidic bond could be achieved for one-pot oligosaccharide conversion. The yields of glycolic acid reached 43.1, 29.2, and 33.3 Cmol % within 30 min, when the substrates were cellobiose, maltose, and maltotriose, respectively. This study developed a low-cost Mn-biochar catalyst for biomass valorization. The study presents valuable mechanistic insights that can serve as a critical reference for the sustainable production of chemical building blocks in heterogeneous catalysis.

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利用生物质提取的葡萄糖和低聚糖生产可持续乙醇酸的锰-生物炭催化剂

考虑到乙醇酸的广泛市场和化石资源的枯竭，利用可再生资源生产乙醇酸是一项重大挑战。本研究利用微波辅助有氧氧化系统，从生物质衍生糖类中实现了乙醇酸的可持续生产。使用不同的前驱体（MnCl2 和 KMnO4）和合成温度（400-850 ℃）合成了各种锰生物炭催化剂。在 MnBC-VII-700（即由 Mn（VII）前体衍生并在 700 °C 下合成的催化剂）上，葡萄糖在 180 °C 下 20 分钟内的乙醇酸产量可达 62.8 Cmol %。通过与催化性能的相关性，确定锰（III）为催化活性状态。生物炭支持对反应物吸附、电子转移和微波吸收至关重要。从葡萄糖到乙醇酸的转化过程会经历逆醛醇反应和氧化反应，而糖苷键的氧化-水解则可实现寡糖的一锅转化。当底物为纤维生物糖、麦芽糖和麦芽三糖时，糖醛酸的产率在 30 分钟内分别达到 43.1、29.2 和 33.3 Cmol %。本研究开发了一种用于生物质增值的低成本锰生物炭催化剂。该研究提出了宝贵的机理见解，可作为在异相催化中可持续生产化学构件的重要参考。

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来源期刊

ACS Sustainable Chemistry & Engineering CHEMISTRY, MULTIDISCIPLINARY-ENGINEERING, CHEMICAL

CiteScore

13.80

自引率

4.80%

发文量

1470

审稿时长

1.7 months

期刊介绍： ACS Sustainable Chemistry & Engineering is a prestigious weekly peer-reviewed scientific journal published by the American Chemical Society. Dedicated to advancing the principles of green chemistry and green engineering, it covers a wide array of research topics including green chemistry, green engineering, biomass, alternative energy, and life cycle assessment. The journal welcomes submissions in various formats, including Letters, Articles, Features, and Perspectives (Reviews), that address the challenges of sustainability in the chemical enterprise and contribute to the advancement of sustainable practices. Join us in shaping the future of sustainable chemistry and engineering.