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含硫空位的超薄ZnInS纳米片中硫原子的调制异质重构协同增强了CO光还原性能。

Te modulated heterogeneous remodeling of S atoms in ultrathin ZnInS nanosheets containing S vacancies synergistically enhances CO photoreduction.

作者信息

Liu Xing, Yuan Meng, Li Yudong, Sun Bowen, Yang Xiaohui, Su Yuchen, Luo Juhua

机构信息

School of Materials Science and Engineering, Yancheng Institute of Technology, Yancheng 224051, China.

Key Laboratory of Bio-based Material Science & Technology, Ministry of Education, Northeast Forestry University, Harbin 150040, China.

出版信息

J Colloid Interface Sci. 2025 Feb;679(Pt A):772-784. doi: 10.1016/j.jcis.2024.10.013. Epub 2024 Oct 5.

Abstract

Reconfiguration of in situ heterojunction composites without interfacial resistance by substitution of homologous anions for the formation of gradient work function differences inducing the formation of built-in electric field is an effective strategy to enhance the charge separation efficiency. Herein, Te/ZnInS-V (Te/ZIS-V) in situ heterojunction was synthesized by substitution of Te ions for S in ultrathin ZIS containing S vacancies, which can significantly promote photogenerated charge separation, surface electron enrichment, and CO adsorption/activation. The presence of S vacancies and adjacent Te/S double anions, the double active sites constructed by defect engineering promote the desorption of *CO molecules while inhibiting the protonation toward *CHO, which was more favorable for selective CO photoreduction to CO. The experimental results showed that the CO yield of Te/ZIS-V was significantly increased to 672.1 μmol g h compared with pristine ZIS (54.3 μmol g h) and the CO selectivity was close to 83 %. Notably, the life cycle assessment (LCA) of Te/ZnlnS nanosheets with S-vacancy was performed. The evaluation results showed that most of the 17 impact categories showed low overall impact values and were environmentally friendly. Based on the results of this LCA, suggestions were put forward to further optimize the product to reduce carbon emissions.

摘要

通过用同源阴离子取代来形成梯度功函数差以诱导内建电场的形成,从而重构无界面电阻的原位异质结复合材料,是提高电荷分离效率的有效策略。在此,通过在含硫空位的超薄ZIS中用碲离子取代硫,合成了Te/ZnInS-V(Te/ZIS-V)原位异质结,其可显著促进光生电荷分离、表面电子富集以及CO吸附/活化。硫空位和相邻的Te/S双阴离子的存在,即通过缺陷工程构建的双活性位点,促进了CO分子的解吸,同时抑制了向CHO的质子化,这更有利于将CO选择性光还原为CO。实验结果表明,与原始ZIS(54.3 μmol g h)相比,Te/ZIS-V的CO产率显著提高至672.1 μmol g h,且CO选择性接近83%。值得注意的是,对具有硫空位的Te/ZnlnS纳米片进行了生命周期评估(LCA)。评估结果表明,17个影响类别中的大多数显示出较低的总体影响值,且对环境友好。基于该LCA的结果,提出了进一步优化产品以减少碳排放的建议。

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