Enhanced glucose conversion to formic acid with deep eutectic solvents-mediated bimetallic oxides: Morphology and valence state regulation

IF 5.8 2区 生物学 Q1 AGRICULTURAL ENGINEERING Biomass & Bioenergy Pub Date : 2025-03-01 Epub Date: 2025-02-12 DOI:10.1016/j.biombioe.2025.107698
Hejuan Wu , Hongrui Guo , Boxiong Shen , Xiao Zhang , Feng Shen
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Abstract

The valorization of biomass into chemicals has emerged as an appealing approach for utilizing biomass as a renewable feedstock. In this study, a deep eutectic solvent (DES)-mediated solvothermal strategy was employed to synthesize a bimetallic nanoparticle catalyst for the conversion of glucose to formic acid. The impact of DES-based solvent systems on the morphology, valence states, and catalytic performance of the catalyst were systematically examined. Experimental results demonstrated that at the same reaction conditions (150 °C, 3 h), the catalyst prepared using DES achieved a formic acid yield of 63.63 %, significantly surpassing the 50.37 % yield obtained with catalysts synthesized through conventional hydrothermal methods. Under optimal conditions of reacting at 150 °C for 5 h, maximum formic acid yield of 65.17 % was attained with DES-mediated catalyst. Characterization underscored the crucial role of DES in promoting the construction of uniform nanospheres and in reducing the manganese valence state from +2.69 to +2.30, which serves as the primary active site. Mechanistic studies identified two main pathways governing the glucose-to-formic acid conversion: (i) a direct conversion route from glucose to formic acid and (ii) an initial isomerization of glucose to fructose, followed by the conversion of fructose into formic acid.

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用深度共晶溶剂介导的双金属氧化物增强葡萄糖转化为甲酸:形态和价态调节
将生物质转化为化学品已成为利用生物质作为可再生原料的一种有吸引力的方法。在本研究中,采用深度共晶溶剂(DES)介导的溶剂热策略合成了葡萄糖转化为甲酸的双金属纳米颗粒催化剂。系统考察了des基溶剂体系对催化剂形态、价态和催化性能的影响。实验结果表明,在相同的反应条件下(150℃,3 h),用DES制备的催化剂甲酸收率为63.63%,明显优于传统水热法合成的催化剂的50.37%。在最佳条件下,在150℃下反应5 h, des催化的甲酸收率最高可达65.17%。表征强调了DES在促进均匀纳米球的构建和将锰价态从+2.69降低到+2.30(作为主要活性位点)方面的关键作用。机制研究确定了控制葡萄糖到甲酸转化的两个主要途径:(i)葡萄糖到甲酸的直接转化途径;(ii)葡萄糖到果糖的初始异构化,随后果糖转化为甲酸。
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来源期刊
Biomass & Bioenergy
Biomass & Bioenergy 工程技术-能源与燃料
CiteScore
11.50
自引率
3.30%
发文量
258
审稿时长
60 days
期刊介绍: Biomass & Bioenergy is an international journal publishing original research papers and short communications, review articles and case studies on biological resources, chemical and biological processes, and biomass products for new renewable sources of energy and materials. The scope of the journal extends to the environmental, management and economic aspects of biomass and bioenergy. Key areas covered by the journal: • Biomass: sources, energy crop production processes, genetic improvements, composition. Please note that research on these biomass subjects must be linked directly to bioenergy generation. • Biological Residues: residues/rests from agricultural production, forestry and plantations (palm, sugar etc), processing industries, and municipal sources (MSW). Papers on the use of biomass residues through innovative processes/technological novelty and/or consideration of feedstock/system sustainability (or unsustainability) are welcomed. However waste treatment processes and pollution control or mitigation which are only tangentially related to bioenergy are not in the scope of the journal, as they are more suited to publications in the environmental arena. Papers that describe conventional waste streams (ie well described in existing literature) that do not empirically address ''new'' added value from the process are not suitable for submission to the journal. • Bioenergy Processes: fermentations, thermochemical conversions, liquid and gaseous fuels, and petrochemical substitutes • Bioenergy Utilization: direct combustion, gasification, electricity production, chemical processes, and by-product remediation • Biomass and the Environment: carbon cycle, the net energy efficiency of bioenergy systems, assessment of sustainability, and biodiversity issues.
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