Synergistically Regulating D-Band Centers of Cd0.5Zn0.5S/LaCoO3 Heterojunction by Dual Electric Fields for Enhanced Photocatalytic Hydrogen Evolution

IF 7 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Chemistry of Materials Pub Date : 2025-03-20 DOI:10.1021/acs.chemmater.5c0045210.1021/acs.chemmater.5c00452

Jieyuan Du, Fei Jin, Guoping Jiang* and Zhiliang Jin*,

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Abstract

The rapid recombination of charges severely limits the activity of photocatalysis. In this article, a polarized electric field and an internal electric field are formed between catalysts by constructing an interface engineering strategy. Through the synergistic effect of double electric fields, the above problems have been effectively resolved . The granular Cd_0.5Zn_0.5S was attached to the LaCoO₃ network structure by electrostatics, and the composite catalyst Cd_0.5Zn_0.5S/LaCoO₃ (CL) was formed. In situ characterization by XPS, EPR, and KFAM confirmed the formation of an S-scheme heterojunction between the composite catalysts. At the same time, electrochemical and fluorescence characterization confirmed that the photogenerated carrier separation efficiency of the CL-25 composite catalyst was significantly improved. This is because the built-in electric field at the interface of the composite catalyst exerts the polarizing electric field between the individual catalysts to an extreme degree, greatly reducing the recombination rate of photogenerated carriers and effectively improving the hydrogen evolution efficiency of the composite photocatalyst. DFT theoretical calculations prove that the existence of a double electric field can greatly reduce the Gibbs free energy of hydrogen adsorption.

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双电场协同调节Cd0.5Zn0.5S/LaCoO3异质结d带中心增强光催化析氢

电荷的快速重组严重地限制了光催化的活性。本文通过构建界面工程策略，在催化剂之间形成极化电场和内电场。通过双电场的协同作用，有效地解决了上述问题。将颗粒状的Cd0.5Zn0.5S通过静电吸附在LaCoO3网络结构上，形成Cd0.5Zn0.5S/LaCoO3 （CL）复合催化剂。通过XPS， EPR和KFAM原位表征证实复合催化剂之间形成了s型异质结。同时，电化学和荧光表征证实了CL-25复合催化剂的光生载流子分离效率得到了显著提高。这是因为复合催化剂界面处的内置电场将单个催化剂之间的极化电场发挥到极致，大大降低了光生载流子的复合速率，有效提高了复合光催化剂的析氢效率。DFT理论计算证明了双电场的存在可以大大降低吸附氢的吉布斯自由能。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Chemistry of Materials 工程技术-材料科学：综合

CiteScore

14.10

自引率

5.80%

发文量

929

审稿时长

1.5 months

期刊介绍： The journal Chemistry of Materials focuses on publishing original research at the intersection of materials science and chemistry. The studies published in the journal involve chemistry as a prominent component and explore topics such as the design, synthesis, characterization, processing, understanding, and application of functional or potentially functional materials. The journal covers various areas of interest, including inorganic and organic solid-state chemistry, nanomaterials, biomaterials, thin films and polymers, and composite/hybrid materials. The journal particularly seeks papers that highlight the creation or development of innovative materials with novel optical, electrical, magnetic, catalytic, or mechanical properties. It is essential that manuscripts on these topics have a primary focus on the chemistry of materials and represent a significant advancement compared to prior research. Before external reviews are sought, submitted manuscripts undergo a review process by a minimum of two editors to ensure their appropriateness for the journal and the presence of sufficient evidence of a significant advance that will be of broad interest to the materials chemistry community.