Research on highly efficient photocatalytic selective oxidation of HMF to DFF using CdS@MXene Composites: Construction of Schottky junctions and mechanistic investigation

IF 13.2 1区 工程技术 Q1 ENGINEERING, CHEMICAL Chemical Engineering Journal Pub Date : 2025-01-31 DOI:10.1016/j.cej.2025.159946
Chenxi Zhang, Peng Zhan, Houchao Shan, Wenqiang Ren, Yicheng Liu, Xiangshi Liu, Shize Zheng, Zihao Liao, Di Cai, Peiyong Qin
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Abstract

Highly-effective photocatalytic selective oxidative valorization of renewable 5-hydroxymethylfurfural (HMF) into 2,5-diformylfuran (DFF), a biomass-derived platform chemical, remains a challenging task for chemists. In this work, uniformly distributed CdS nanospheres were synthesized using the deep eutectic solvent method and subsequently loaded onto monolayer MXene nanosheets. This method successfully yielded CdS@MXene Schottky junction photocatalysts. The outstanding electron-trapping capability of MXene significantly improves the selectivity and long-term stability of CdS@MXene, which is capable of being used for photocatalysis DFF production from HMF. Up to 91.63 % of DFF selectivity can be obtained from 1 mM of HMF by CdS@MXene-11 % under visible light irradiation using water as solvent. Density functional theory was further adopted to investigate electron transfer between CdS and MXene, confirming the presence of a Schottky junction for the enhanced separation and interfacial transfer efficiency of photogenerated carriers. The mechanism for the photocatalysis production of DFF from HMF was proposed by employing electron paramagnetic resonance, which suggests ·O2– as the main radical, and plays a decisive role in the selective oxidation process. This work provides new insights into construction of MXene-based Schottky junction as a promising approach for the photocatalytic valorization of biomass under mild conditions.

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CdS@MXene复合材料高效光催化氧化HMF制备DFF的研究:肖特基结的构建及其机理研究
可再生5-羟甲基糠醛(HMF)高效的光催化选择性氧化价化反应生成2,5-二甲酰呋喃(DFF)是一种生物质衍生的平台化学品,对化学家来说仍然是一个具有挑战性的任务。本文采用深共晶溶剂法合成了均匀分布的CdS纳米球,并将其加载到单层MXene纳米片上。该方法成功制备了CdS@MXene肖特基结光催化剂。MXene优异的电子俘获能力显著提高了CdS@MXene的选择性和长期稳定性,可用于光催化HMF制备DFF。以水为溶剂,在可见光照射下,以CdS@MXene-11 %的浓度对1 mM的HMF的DFF选择性可达91.63 %。采用密度泛函理论进一步研究了CdS和MXene之间的电子转移,证实了肖特基结的存在,提高了光生载流子的分离和界面转移效率。利用电子顺磁共振技术对羟甲基糠醛光催化制备DFF的机理进行了研究,结果表明·O2 -为主要自由基,在选择性氧化过程中起决定性作用。这项工作为构建基于mxeni的肖特基结提供了新的见解,该结是一种在温和条件下光催化生物质增值的有前途的方法。
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来源期刊
Chemical Engineering Journal
Chemical Engineering Journal 工程技术-工程:化工
CiteScore
21.70
自引率
9.30%
发文量
6781
审稿时长
2.4 months
期刊介绍: The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.
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