Just Accepted
Yuting Wu, Haifeng Lv*, Xiaojun Wu*
https://doi.org/10.1016/j.cjsc.2024.100375
Covalent organic frameworks; Photocatalytic water splitting; The first-principles calculations; Molecular design; Machine learning
ABSTRACT
Utilizing
sunlight to split water into H2 and O2 is a highly promising approach in renewable
energy production approaches. Recently, significant efforts have been devoted
to develop innovative photocatalysts for splitting water. Metal-free
two-dimensional (2D) covalent organic frameworks (COFs) are emerging as ideal
catalytic platforms for this purpose. However, the rational design of these
materials requires appropriate band alignment and active sites capable of
catalyzing both hydrogen and oxygen evolution reactions, which depends on the
judicious selection of molecular precursors. To address these requirements,
first-principles calculations have proven to be an efficient method for
designing and screening potential photocatalysts. Here, we provide a concise
overview of recent advancements in the development of 2D COFs photocatalysts
for overall water splitting (OWS), examining it from a theoretical perspective.
This includes outlining the design principles, exploring the data-driven
discovery of potential candidates using a COFs database, and applying machine
learning techniques to predict the electronic structure of COFs based on the
molecular orbitals of their precursors. Furthermore, we discuss the accuracy of
current computational methods and address future challenges and potential of 2D
COFs in practical applications for OWS.