Abstract
Heterogeneous catalysts offer a cyclable platform for exploring efficient transformation systems, and their promising applications underpin a broad research interest. Covalent organic frameworks (COFs) are a class of crystalline porous networks that can integrate organic units into ordered skeletons and pores, offering an insoluble and robust platform for exploring heterogeneous catalysts. In this Outlook, we describe a conceptual scheme for designing catalytic COFs to promote various transformations. We summarize the general strategy for designing COFs to construct tailor-made skeletons and pores by emphasizing their structural uniqueness. We introduce different approaches to develop catalytic functions by sampling COFs into four regimes, i.e., skeletons, walls, pores, and systematically organized systems. We scrutinize their catalytic features and elucidate interplays with electrons, holes, and molecules by highlighting the key role of interface design in exploring catalytic COFs. We further envisage the key issues to be challenged, future research directions, and perspectives to show a full picture of designer heterogeneous catalysis based on COFs.