多功能co3o4修饰ZnIn2S4光催化剂选择性氧化生物质衍生5-羟甲基糠醛的研制

IF 14.9 1区 化学 Q1 Energy
Shan Jiang , Zhenpan Chen , Shaofeng Xiong , Hongxin Zhao , Xishun Xiao , Zhigang Shen
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引用次数: 0

摘要

生物质衍生的5-羟甲基糠醛(HMF)的光催化选择性氧化为热催化提供了一种可持续的替代方法。然而,该工艺的效率受到传统光催化剂中光产生的载流子的快速重组和光吸收效率不足的限制。在此,我们开发了一种Co3O4/ZnIn2S4 (Co3O4/ZIS)光催化剂,其中Co3O4作为多功能助催化剂。该光催化剂通过界面氧-羟基相互作用显著增强HMF分子的化学吸附和活化。此外,窄带隙Co3O4的加入拓宽了复合光催化剂的光吸收范围。此外,将Co3O4与ZnIn2S4集成后,电荷分离效率比原始ZnIn2S4提高了5.9倍。优化后的Co3O4/ZIS-3光催化剂(Co3O4负载3 wt%)在可见光下对2,5-二甲酰基呋喃(DFF)表现出优异的选择性和产率,与原始ZnIn2S4相比,DFF的选择性达到70.4%,提高了5.4倍。清除剂实验和电子自旋共振(ESR)谱分析表明,超氧自由基(⋅O2−)和h+是驱动HMF光催化氧化的主要活性物质。分子模拟结果表明,与ZnIn2S4相比,Co3O4/ZIS复合材料具有较低的活化障碍,更有利于HMF的活化和中间*MF向*DFF的转化。通过这项工作,我们的目标是设计高效和负担得起的生物质增值光催化剂,并为光催化氧化HMF的机制提供有价值的见解。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Development of multifunctional Co3O4-modified ZnIn2S4 photocatalyst for the selective oxidation of biomass-derived 5-hydroxymethylfurfural

Development of multifunctional Co3O4-modified ZnIn2S4 photocatalyst for the selective oxidation of biomass-derived 5-hydroxymethylfurfural
The photocatalytic selective oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) offers a sustainable alternative to thermal catalysis. However, the efficiency of this process is significantly limited by inadequate light absorption efficiency and the rapid recombination of photogenerated charge carriers in conventional photocatalysts. Herein, we developed a Co3O4/ZnIn2S4 (Co3O4/ZIS) photocatalyst, in which Co3O4 functions as a multifunctional cocatalyst. This photocatalyst significantly enhances the chemisorption and activation of HMF molecules through interfacial oxygen-hydroxyl interactions. Additionally, the incorporation of narrow-band gap Co3O4 broadens the optical absorption range of the composite photocatalyst. Besides, integrating Co3O4 with ZnIn2S4 leads to a 5.9-fold increase in charge separation efficiency compared to pristine ZnIn2S4. The optimized Co3O4/ZIS-3 photocatalyst (3 wt% Co3O4 loading) exhibits exceptional selectivity and yield for 2,5-diformylfuran (DFF) under visible light irradiation, achieving 70.4% DFF selectivity with a 5.4-fold enhancement compared to pristine ZnIn2S4. Scavenger experiments and electron spin resonance (ESR) spectroscopy indicate that superoxide radicals (⋅O2) and h+ are the main active species driving the photocatalytic oxidation of HMF. Molecular simulations reveal that the activation of HMF and the transformation of the intermediate *MF to *DFF are more favorable over the Co3O4/ZIS composite due to lower activation barriers compared to those over ZnIn2S4. Through this work, we aim to design highly efficient and affordable photocatalysts for biomass valorization and contribute valuable insights into the mechanisms of photocatalytic oxidation of HMF.
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来源期刊
Journal of Energy Chemistry
Journal of Energy Chemistry CHEMISTRY, APPLIED-CHEMISTRY, PHYSICAL
CiteScore
19.10
自引率
8.40%
发文量
3631
审稿时长
15 days
期刊介绍: The Journal of Energy Chemistry, the official publication of Science Press and the Dalian Institute of Chemical Physics, Chinese Academy of Sciences, serves as a platform for reporting creative research and innovative applications in energy chemistry. It mainly reports on creative researches and innovative applications of chemical conversions of fossil energy, carbon dioxide, electrochemical energy and hydrogen energy, as well as the conversions of biomass and solar energy related with chemical issues to promote academic exchanges in the field of energy chemistry and to accelerate the exploration, research and development of energy science and technologies. This journal focuses on original research papers covering various topics within energy chemistry worldwide, including: Optimized utilization of fossil energy Hydrogen energy Conversion and storage of electrochemical energy Capture, storage, and chemical conversion of carbon dioxide Materials and nanotechnologies for energy conversion and storage Chemistry in biomass conversion Chemistry in the utilization of solar energy
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