Direct Construction of Isomeric Benzobisoxazole-Vinylene-Linked Covalent Organic Frameworks with Distinct Photocatalytic Properties

Li S, Ma R, Xu S, Zheng T, Fu G, Wu Y, Liao Z, Kuang Y, Hou Y, Wang D, Petkov PS, Simeonova K, Feng X, Wu LZ, Li XB, Zhang T (2022)

Publication Type: Journal article

Publication year: 2022

Journal

Journal of the American Chemical Society American Chemical Society

Book Volume: 144

Pages Range: 13953-13960

Journal Issue: 30

DOI: 10.1021/jacs.2c06042

Abstract

Vinylene/olefin-linked two-dimensional covalent organic frameworks (v-2D-COFs) have emerged as advanced semiconducting materials with excellent in-plane conjugation, high chemical stabilities, and precisely tunable electronic structures. Exploring new linkage chemistry for the reticular construction of v-2D-COFs remains in infancy and challenging. Herein, we present a solid-state benzobisoxazole-mediated aldol polycondensation reaction for the construction of two novel isomeric benzobisoxazole-bridged v-2D-COFs (v-2D-COF-NO1 and v-2D-COF-NO2) with trans and cis configurations of benzobisoxazole. Interestingly, the isomeric benzobisoxazole linkers endow the two v-2D-COFs with distinct optoelectronic and electrochemical properties, ranging from light absorption and emission to charge-transfer properties. When employed as the photocathode, v-2D-COF-NO1 exhibits a photocurrent of up to ∼18 μA/cm2under AM 1.5G irradiation at -0.3 V vs reversible hydrogen electrode (RHE), which is twice the value of v-2D-COF-NO2 (∼9.1 μA/cm2). With Pt as a cocatalyst, v-2D-COF-NO1 demonstrates a photocatalytic hydrogen evolution rate of ∼1.97 mmol h-1g-1, also in clear contrast to that of v-2D-COF-NO2 (∼0.86 mmol h-1g-1) under identical conditions. This work demonstrates the synthesis of v-2D-COFs via benzobisoxazole-mediated aldol polycondensation with isomeric structures and distinct photocatalytic properties.

Involved external institutions

Chinese Academy of Sciences (CAS) / 中国科学院 CN China (CN) Technische Universität Dresden DE Germany (DE) Fraunhofer-Institut für Keramische Technologien und Systeme (IKTS) DE Germany (DE) Zhejiang University CN China (CN) Sofia University "St. Kliment Ohridski" / Софийски университет "Св. Климент Охридски" BG Bulgaria (BG) Quzhou University / 衢州学院 CN China (CN)

How to cite

APA:

Li, S., Ma, R., Xu, S., Zheng, T., Fu, G., Wu, Y.,... Zhang, T. (2022). Direct Construction of Isomeric Benzobisoxazole-Vinylene-Linked Covalent Organic Frameworks with Distinct Photocatalytic Properties. Journal of the American Chemical Society, 144(30), 13953-13960. https://doi.org/10.1021/jacs.2c06042

MLA:

Li, Shengxu, et al. "Direct Construction of Isomeric Benzobisoxazole-Vinylene-Linked Covalent Organic Frameworks with Distinct Photocatalytic Properties." Journal of the American Chemical Society 144.30 (2022): 13953-13960.

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