Tong, S. W., Chai, J., Ng, M.-F., Fu, W., Goh, W. P., & Jiang, C. (2024). Interfacial Engineering of Metal-Organic Framework-Based Electrode for High-Performance Smart Glass. ACS Applied Optical Materials, 2(4), 539–548. https://doi.org/10.1021/acsaom.3c00437
Abstract:
Prussian blue (PB), a representative metal-organic framework, holds great promise as an electrode material for optical applications. However, the preparation of cycle-stable PB with minimal defects/vacancies and coordinated water have been limited by the uncontrollable growth kinetics. Here, we report on the electrodeposition of cycle-stable PB film via pre-silanization on the growth substrate. By self-assembling an aminosilane layer on the indium-tin-oxide (a-ITO) substrate before the PB growth, we demonstrate the a-ITO/PB film with minimal defects/vacancies and water (~ 5 %), as validated by a combination of XPS, Raman and TGA studies. In addition, SEM measurements indicate that the conventional delamination and cracking issue of PB film can be effectively impeded in our a-ITO/PB film over 1,000 cycles. The cyclic tests also indicate that the a-ITO/PB film attains a remarkably higher charge density of 17.4 mC/cm2 with better stability (charge density retention ~ 87 % over 1,000 cycles) than the state-of-the-art PB benchmark. The crucial role of the aminosilane treatment in increasing the a-ITO/PB interaction/binding is elucidated by the Density functional theory (DFT) simulations. DFT results suggest that there is a substantial charge redistribution localized around the interface of a-ITO/PB, leading to the six times increment in binding energy as compared to non-treated ITO/PB. As an exemplified application, the cycle-stable a-ITO/PB film is applied as an efficient counter electrode in a smart glass. This study paves an effective interfacial engineering means for increasing the binding at PB- substrate interface and structural integrity of PB itself for long-term electrochemical and optical applications.
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Funding Info:
This research / project is supported by the Agency for Science, Technology, and Research - Career Development Fund
Grant Reference no. : C210112032
This research / project is supported by the Agency for Science, Technology, and Research - Sustainable Hybrid Lighting System for Controlled Environment Agriculture
Grant Reference no. : A19D9a0096
This research / project is supported by the Agency for Science, Technology, and Research - MTC programmatic fund
Grant Reference no. : M23L9b0052