Topologically Isomeric Effects on the Photocatalytic H2O2 Production Performance of Two-dimensional Covalent Organic Frameworks
摘要
Two-dimensional covalent organic frameworks (2D COFs), characterized by tunable optoelectronic properties and well-defined porous architectures, have emerged as promising photocatalysts for solar-driven H2O2 production. Although network topology exerts a profound impact on the optoelectronic characteristics of 2D materials, achieving precise regulation of their topology remains a significant challenge. In this study, we report two topologically isomeric 2D COFs constructed from the same building blocks, namely ETBA-kgm-COF with a kgm topology and ETBA-sql-COF with a sql topology. Particularly, the isomeric COFs with same chemical compositions provide an ideal platform to isolate and elucidate intrinsic topological effects in 2D COFs. Comprehensive characterizations reveal that the sql topology facilitates efficient charge separation and transfer, thereby enhancing photocatalytic performance. Moreover, without any sacrificial agents, ETBA-sql-COF exhibits a superior photocatalytic H2O2 production rate up to 2042 µmol·g−1·h−1, which is 1.57 times that of ETBA-kgm-COF (1303 µmol·g−1·h−1). This work provides an in-depth investigation into topology-property relationships in COFs and offers a rational strategy for the design and synthesis of high-performance photocatalysts.