Promoting 5-hydroxymethylfurfural production from cellulose and wheat straw via sulfonic acid group-grafted SBA-15 mesoporous silica embedded with iron phosphate

IF 6.2 1区 农林科学 Q1 AGRICULTURAL ENGINEERING
Siyu Zhou , Wanni Liu , Dongqi Liu , Xian Shi , Kai Huang , Feng Jiang , Hui Gao , Haian Xia , Ying Guan , Siquan Xu
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Abstract

Efficient catalytic conversion of cellulose into 5-hydroxymethylfurfural (HMF) remains challenging and arouses concern. In this study, iron phosphate (FePO4) was embedded into the SBA-15 mesoporous silica matrix as an available active phase via ultrasound-assisted implantation, and then the abundant silanol nests were utilized to graft sulfonic acid groups to construct an innovative FeP@SBA-15-S catalyst. Through a systematic analysis of the characteristics of crystal, texture, element valence, acidity, hydrophilicity, etc., it was reflected that FeP@SBA-15-S catalyst gave the active FePO4 component porosity and exhibited bifunctional acidity. Without pretreatment and other acid additives, FeP@SBA-15-S catalyzed cellulose under optimal conditions provided a desired HMF yield of 52 %. More meaningfully, the cellulose and hemicellulose components in native wheat straw could be catalyzed simultaneously by FeP@SBA-15-S catalyst, yielding 61 % HMF and 60 % furfural in one-pot. The cyclability evaluation showed that the FeP@SBA-15-S catalyst still had considerable activity after six continuous runs, with a slight loss in activity attributed to the leaching of active components and pore coverage. A clear catalytic pathway was summarized by GC-MS and 13C NMR spectrum as cellulose undergoing glucose monomer ring opening, isomerization to fructose, fructose ring closure and final dehydration, and the by-products were also detected as mainly C3-C23 fragments and oligomers.

Abstract Image

磷酸铁包埋SBA-15介孔二氧化硅磺酸基接枝促进纤维素和麦秸生产5-羟甲基糠醛
纤维素高效催化转化为5-羟甲基糠醛(HMF)仍然具有挑战性,引起了人们的关注。本研究通过超声辅助植入,将磷酸铁(FePO4)作为有效的活性相嵌入SBA-15介孔二氧化硅基体中,然后利用丰富的硅醇巢接枝磺酸基,构建创新的FeP@SBA-15-S催化剂。通过对晶体、结构、元素价态、酸度、亲水性等特征的系统分析,反映FeP@SBA-15-S催化剂给予活性FePO4组分孔隙,呈现双功能酸性。在没有预处理和其他酸添加剂的情况下,FeP@SBA-15-S催化纤维素在最佳条件下的HMF产率为52% %。更有意义的是,在FeP@SBA-15-S催化剂下,天然麦秸中的纤维素和半纤维素组分可以同时催化,在一锅中得到61 %的HMF和60 %的糠醛。循环性评估表明,FeP@SBA-15-S催化剂在连续运行六次后仍具有相当大的活性,活性略有下降,原因是活性组分的浸出和孔隙覆盖。通过GC-MS和13C NMR谱分析,纤维素经过葡萄糖单体开环、异构化成果糖、果糖环闭合并最终脱水的催化途径较为明确,副产物主要为C3-C23片段和低聚物。
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来源期刊
Industrial Crops and Products
Industrial Crops and Products 农林科学-农业工程
CiteScore
9.50
自引率
8.50%
发文量
1518
审稿时长
43 days
期刊介绍: Industrial Crops and Products is an International Journal publishing academic and industrial research on industrial (defined as non-food/non-feed) crops and products. Papers concern both crop-oriented and bio-based materials from crops-oriented research, and should be of interest to an international audience, hypothesis driven, and where comparisons are made statistics performed.
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