Cargando…

Covalent Organic Framework Nanoplates Enable Solution-Processed Crystalline Nanofilms for Photoelectrochemical Hydrogen Evolution

[Image: see text] 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 synt...

Descripción completa

Detalles Bibliográficos
Autores principales: Yao, Liang, Rodríguez-Camargo, Andrés, Xia, Meng, Mücke, David, Guntermann, Roman, Liu, Yongpeng, Grunenberg, Lars, Jiménez-Solano, Alberto, Emmerling, Sebastian T., Duppel, Viola, Sivula, Kevin, Bein, Thomas, Qi, Haoyuan, Kaiser, Ute, Grätzel, Michael, Lotsch, Bettina V.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2022
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9204765/
https://www.ncbi.nlm.nih.gov/pubmed/35657204
http://dx.doi.org/10.1021/jacs.2c01433
Descripción
Sumario:[Image: see text] 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.