Bi-metallic [Cu/Co(6mna)2]n metal organic chalcogenolate frameworks as high-performance electro-catalysts for dye-sensitized solar cells: a ligand-assisted bottom-up synthesis

Chun Wei Lai, Yu Chien Lee, Yi Zhen Jiang, Chia Her Lin, Gautam Kumar, Michael H. Huang, Chun Ting Li*

*此作品的通信作者

研究成果: 雜誌貢獻期刊論文同行評審

摘要

Mercaptonicotinate-based metal organic chalcogenolate frameworks (MOFs), including [Cu2(6mna)(6mn)NH4]n-NO3, [Co2(6mna)2]n-NO3, [Co2(6mna)2]n-Cl, [Cu/Co(6mna)2]n-NO3, and [Cu/Co(6mna)2]n-Cl (6mna = 6-mercaptonicotinic acid; 6mn = 6-mercaptonicotinate), were newly introduced as the electro-catalytic counter electrodes in dye-sensitized solar cells (DSSCs). By using a ligand-assisted bottom-up synthesis, these five types of MOF films were covalently bonded to a conducting substrate to deliver their intrinsic electro-catalytic ability without any additives. The DSSCs coupled with all the carbon cloth/MOF electrodes showed a superior solar-to-electricity conversion efficiency (9.4%-10.0%) to the cell with a traditional carbon cloth/Pt electrode (9.3%), demonstrating their outstanding electrochemical activities. Heterogeneous bi-metallic MOFs, [Cu/Co(6mna)2]n-NO3 and [Cu/Co(6mna)2]n-Cl, outperformed their mono-metallic counterparts by increasing film roughness/porosity and decreasing the activation energy for I/I3. Their remarkable electrochemical performance was attributed to the successful synergistic effect, where [Cu2(6mna)(6mn)NH4]n-NO3 provided facile charge transfer via its 2D (-Cu-S-)n planes, while [Co2(6mna)2]n supplied large surface area and multiple electro-catalytic active sites through its helical (-Co-S-)n chains. With the use of different redox mediators (iodide, Co-phenanthroline, and Cu-neocuproine), the optimal carbon cloth/[Cu/Co(6mna)2]n-Cl electrode also showed better electro-catalytic ability and long-term stability than carbon cloth/Pt. Under room light illumination, higher cell efficiencies were obtained at 1.0 klux (19.5% for an office), 3.0 klux (23.3% for a shopping window), and 6.0 klux (26.4% for a lampshade), revealing the potential of mercaptonicotinate-based bi-metallic MOFs to be applied in various electrochemical devices.

原文英語
頁(從 - 到)1595-1608
頁數14
期刊Journal of Materials Chemistry A
12
發行號3
DOIs
出版狀態已發佈 - 2023 12月 4

ASJC Scopus subject areas

  • 一般化學
  • 可再生能源、永續發展與環境
  • 一般材料科學

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