CdS quantum dots with sulfur defects for photoreforming plastics into valuable chemicals coupled with hydrogen production

IF 4.9 2区 化学 Q2 CHEMISTRY, PHYSICAL Molecular Catalysis Pub Date : 2025-03-24 DOI:10.1016/j.mcat.2025.115049
Jiaxin Song , Cheng Rao , Zeshu Zhang , Xiangguang Yang , Yibo Zhang
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Abstract

Photocatalytic reforming of plastics, involving converting plastics into valuable chemicals while producing hydrogen from water, is a promising green technology with sustainability potential. However, designing catalysts with optimized structures to further enhance efficiency remained a major challenge. In this study, a series of CdS Quantum dots (QDs) with different sulfur defect concentrations were synthesized by a one-step solvothermal method by adjusting the type of sulfur precursors. In the absence of co-catalysts, the optimal CdS-NS photocatalyst achieved reforming of polyethylene terephthalate (PET) into formate with 870 μmol g−1 h−1 and acetate esters with 90 μmol g−1 h−1, while the hydrogen production rate reached 1771 μmol g−1 h−1. EPR spectra and other analyses confirmed the presence of abundant sulfur defects in the prepared CdS QDs and further demonstrated that the concentration of sulfur defects was closely related to photocatalytic performance. Suitable sulfur defects effectively modulated the electronic and band structure of CdS QDs, enhanced the oxidation capacity of photogenerated holes, reduced the recombination rate of charge carriers, and ultimately improved photocatalytic activity. This work provided an effective approach for designing efficient photocatalysts for the high-value recycling of plastic waste to achieve carbon neutrality.

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含硫缺陷的CdS量子点用于光重整塑料,使其转化为有价值的化学品,并伴有氢气的产生
塑料的光催化重整,包括将塑料转化为有价值的化学品,同时从水中产生氢,是一项具有可持续发展潜力的有前途的绿色技术。然而,设计具有优化结构的催化剂以进一步提高效率仍然是一个主要挑战。本研究通过调整硫前驱体的类型,采用一步溶剂热法合成了一系列具有不同硫缺陷浓度的CdS量子点。在无助催化剂的情况下,最佳的CdS-NS光催化剂可将聚对苯二甲酸乙二醇酯(PET)转化为甲酸酯(870 μmol g−1 h−1)和乙酸酯(90 μmol g−1 h−1),产氢率可达1771 μmol g−1 h−1。EPR光谱等分析证实了所制备的CdS量子点中存在丰富的硫缺陷,并进一步证明了硫缺陷的浓度与光催化性能密切相关。适当的硫缺陷可以有效地调节CdS量子点的电子和能带结构,增强光生空穴的氧化能力,降低载流子的重组速率,最终提高光催化活性。本研究为设计高效的光催化剂,实现高价值塑料废物的回收利用,实现碳中和提供了有效途径。
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麦克林
Polylactic acid
麦克林
3-Mercaptopropionic acid
麦克林
Cadmium chloride
麦克林
Polylactic acid
麦克林
3-Mercaptopropionic acid
麦克林
Cadmium chloride
阿拉丁
NaOD
阿拉丁
D2O
阿拉丁
Thioacetamide
阿拉丁
NaOD
阿拉丁
D2O
阿拉丁
Thioacetamide
来源期刊
Molecular Catalysis
Molecular Catalysis Chemical Engineering-Process Chemistry and Technology
CiteScore
6.90
自引率
10.90%
发文量
700
审稿时长
40 days
期刊介绍: Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are: Heterogeneous catalysis including immobilized molecular catalysts Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis Photo- and electrochemistry Theoretical aspects of catalysis analyzed by computational methods
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