Controlling crystallization in covalent organic frameworks to facilitate photocatalytic hydrogen production

Bibliographic Details
Title: Controlling crystallization in covalent organic frameworks to facilitate photocatalytic hydrogen production
Authors: Zheng Lin, Xiangkun Yu, Zijian Zhao, Ning Ding, Changchun Wang, Ke Hu, Youliang Zhu, Jia Guo
Source: Nature Communications, Vol 16, Iss 1, Pp 1-11 (2025)
Publisher Information: Nature Portfolio, 2025.
Publication Year: 2025
Collection: LCC:Science
Subject Terms: Science
More Details: Abstract The catalytic performance, depending on the surface nature, is ubiquitous in photocatalysis. However, surface engineering for organic photocatalysts through structural modulation has long been neglected. Here, we propose a zone crystallization strategy for covalent organic frameworks (COFs) that enhances surface ordering through regulator-induced amorphous-to-crystalline transformation. Dynamic simulations show that attaching monofunctional regulators to the surface of spherical amorphous precursor improves surface dynamic reversibility, increasing crystallinity from the inside out. The resulting COF microspheres display surface-enhanced crystallinity and uniform spherical morphology. The visible photocatalytic hydrogen evolution rate reaches 126 mmol g–1 h–1 for the simplest β-ketoenamine-linked COF and 350 mmol gCOF –1 h–1 for SiO2@COF with minimal Pt cocatalysts. Mechanism studies indicate that surface crystalline domains build the surface electrical fields to accumulate photogenerated electrons and diminish electron transfer barriers between the COF and Pt interface. This work bridges the gap between microscopic molecules and macroscopic properties, allowing tailored design of crystalline organic photocatalysts.
Document Type: article
File Description: electronic resource
Language: English
ISSN: 2041-1723
Relation: https://doaj.org/toc/2041-1723
DOI: 10.1038/s41467-025-57166-1
Access URL: https://doaj.org/article/767bcd2215974164bb461d93ee8c0d52
Accession Number: edsdoj.767bcd2215974164bb461d93ee8c0d52
Database: Directory of Open Access Journals
More Details
ISSN:20411723
DOI:10.1038/s41467-025-57166-1
Published in:Nature Communications
Language:English