Anion Effect on the CuII–Neocuproine Mediator and Its Electrocatalysts for Dye-Sensitized Solar Cells: Polymeric Chalcogenides of PEDOT–PEDTT and [Ag2(SePh)2]n

IF 8.3 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY ACS Applied Materials & Interfaces Pub Date : 2024-09-20 DOI:10.1021/acsami.4c08861

Xin-Bei Lin, Chih-Ya Wu, Bo-Yu Han, Yu-Chien Lee, Yin-Fan Lin, Sie-Rong Li, Shih-Sheng Sun, Chun-Ting Li

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Abstract

The synthetical methodology for the [Cu(dmp)₂]^2+/1+ (dmp = 2,9-dimethyl-1,10-phenanthroline; neocuproine) complexes has been systematically investigated by using various copper precursors, including CuCl₂, Cu(NO₃)₂, and Cu(ClO₄)₂. After an anion exchange to trifluoromethanesulfonimide (TFSI), the tetra-coordinated Cu^II(dmp)₂(TFSI)₂-Cu(ClO₄)₂ (7.43%) outperformed the penta-coordinated Cu^II(dmp)₂(TFSI)(NO₃)-Cu(NO₃)₂ (4.30%) and Cu^II(dmp)₂(TFSI)(Cl)-CuCl₂. Polymeric chalcogenides, including a conducting copolymeric electrode of PEDOT–PEDTT [PEDOT = poly(3,4-ethylenedioxythiophene); PEDTT = poly(3,4-ethylenedithiothiophene)] and a coordination polymeric electrode of silver bezeneselenolate ([Ag₂(SePh)₂]_n; mithrene), are introduced as the electrocatalysts for [Cu(dmp)₂]^2+/1+ for the first time. After optimization, dye-sensitized solar cells (DSSCs) based on carbon cloth (CC)/AgSePh-30 (10.18%) showed superior electrocatalytic ability compared to the benchmark CC/Pt (7.43%) due to numerous active sites provided by electron-donating Se atoms, high film roughness, and bottom-up 2D charge transfer routes. The DSSC based on CC/PEDTT-50 (10.38%) also outperformed CC/Pt due to numerous active sites provided by electron-donating S atoms and proper energy band structure. This work sheds light on the future design and synthesis in Cu-complex mediators and functional polymeric chalcogenides for high-performance DSSCs.

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阴离子对 CuII-Neocuproine 中介体及其用于染料敏化太阳能电池的电催化剂的影响：PEDOT-PEDTT 和 [Ag2(SePh)2]n 的聚合物卤化物

通过使用各种铜前体，包括 CuCl2、Cu(NO3)2 和 Cu(ClO4)2，系统地研究了[Cu(dmp)2]2+/1+（dmp = 2,9-二甲基-1,10-菲罗啉；新乌头原碱）配合物的合成方法。在与三氟甲磺酰亚胺（TFSI）进行阴离子交换后，四配位的 CuII(dmp)2(TFSI)2-Cu(ClO4)2 (7.43%) 优于五配位的 CuII(dmp)2(TFSI)(NO3)-Cu(NO3)2 (4.30%) 和 CuII(dmp)2(TFSI)(Cl)-CuCl2 。聚合卤化物，包括 PEDOT-PEDTT [PEDOT = 聚(3,4-亚乙二氧基噻吩)；PEDTT = 聚(3,4-亚乙二硫基噻吩)] 的导电共聚物电极和倍苯硒酸银（[Ag2(SePh)2]n；mithrene）的配位聚合物电极，首次被引入作为 [Cu(dmp)2]2+/1+ 的电催化剂。经过优化，基于碳布（CC）/AgSePh-30（10.18%）的染料敏化太阳能电池（DSSC）的电催化能力优于基准的 CC/Pt（7.43%），这是由于电子捐赠 Se 原子提供了大量的活性位点、高薄膜粗糙度以及自下而上的二维电荷转移路线。基于 CC/PEDTT-50 的 DSSC（10.38%）的性能也优于 CC/Pt，这是由于电子捐赠的 S 原子提供了大量的活性位点和适当的能带结构。这项研究为未来设计和合成用于高性能 DSSC 的铜络合物介质和功能性聚合物掺杂物提供了启示。

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来源期刊

ACS Applied Materials & Interfaces 工程技术-材料科学：综合

CiteScore

16.00

自引率

6.30%

发文量

4978

审稿时长

1.8 months

期刊介绍： ACS Applied Materials & Interfaces is a leading interdisciplinary journal that brings together chemists, engineers, physicists, and biologists to explore the development and utilization of newly-discovered materials and interfacial processes for specific applications. Our journal has experienced remarkable growth since its establishment in 2009, both in terms of the number of articles published and the impact of the research showcased. We are proud to foster a truly global community, with the majority of published articles originating from outside the United States, reflecting the rapid growth of applied research worldwide.