As covalent organic frameworks (COFs) are coming of age, the lack of effective approaches to achieve crystalline and centimeter-scale-homogeneous COF films remains a significant bottleneck toward advancing the application of COFs in optoelectronic devices. Here, we present the synthesis of colloidal COF nanoplates, with lateral sizes of ∼200 nm and average heights of 35 nm, and their utilization as photocathodes for solar hydrogen evolution. The resulting COF nanoplate colloid exhibits a unimodal particle-size distribution and an exceptional colloidal stability without showing agglomeration after storage for 10 months and enables smooth, homogeneous, and thickness-tunable COF nanofilms via spin coating. Photoelectrodes comprising COF nanofilms were fabricated for photoelectrochemical (PEC) solar-to-hydrogen conversion. By rationally designing multicomponent photoelectrode architectures including a polymer donor/COF heterojunction and a hole-transport layer, charge recombination in COFs is mitigated, resulting in a significantly increased photocurrent density and an extremely positive onset potential for PEC hydrogen evolution (over +1 V against the reversible hydrogen electrode), among the best of classical semiconductor-based photocathodes. This work thus paves the way toward fabricating solution-processed large-scale COF nanofilms and heterojunction architectures and their use in solar-energy-conversion devices.

All primary data files of measurements and processed data of the journal article mentioned under related publications from Lotsch group can be found here.

The data is structured according to figures and schemes in the research article and contains the following data types: XRD patterns (.raw), AFM images (.ibw), Nitrogen isotherm profiles (.qps), dynamic light scattering data (.dts), TEM images (.dm3), ChemDraw files (.cdxml), NMR data (.jdf, .mnova), python jupyter files (.ipynb), CorelDraw files (.cdr), SEM images (.tif), electrochemistry data (.paax), origin files (.opju), COF structure models (.cif), and FT-IR spectra (*.sp).

View data by "tree" to understand the file structure and file names according to the designations used in the original publication.