Three-Dimensional Covalent Organic Frameworks with Ultra-Large Pores for Highly Efficient Photocatalysis

Benefiting from their unique structural merits, three-dimensional (3D) large-pore COF materials demonstrate high surface areas and interconnected large channels, which makes these materials promising in practical applications. Unfortunately, functionalization strategies and application research are still absent in these structures. To this end, a series of functional 3D stp-topologized COFs are designed based on porphyrin or metalloporphyrin moieties, named JUC-640-M (M = Co, Ni, or H). Interestingly, JUC-640-H exhibits a record-breaking low crystal density (0.106 cm3 g-1) among all crystalline materials, along with the largest interconnected pore size (4.6 nm) in 3D COFs, high surface area (2204 m2 g-1), and abundant exposed porphyrin moieties (0.845 mmol g-1). Inspired by the unique structural characteristics and photoelectrical performance, JUC-640-Co is utilized for the photoreduction of CO2 to CO and demonstrates a high CO production rate (15.1 mmol g-1 h-1), selectivity (94.4%), and stability. It should be noted that the CO production rate of JUC-640-Co has exceeded those of all reported COF-based materials. This work not only produces a series of novel 3D COFs with large channels but also provides a new guidance for the functionalization and applications of COFs.

Medienart:

E-Artikel

Erscheinungsjahr:

2023

Erschienen:

2023

Enthalten in:

Zur Gesamtaufnahme - volume:145

Enthalten in:

Journal of the American Chemical Society - 145(2023), 5 vom: 08. Feb., Seite 3248-3254

Sprache:

Englisch

Beteiligte Personen:

Ding, Jiehua [VerfasserIn]
Guan, Xinyu [VerfasserIn]
Lv, Jia [VerfasserIn]
Chen, Xiaohong [VerfasserIn]
Zhang, Yi [VerfasserIn]
Li, Hui [VerfasserIn]
Zhang, Daliang [VerfasserIn]
Qiu, Shilun [VerfasserIn]
Jiang, Hai-Long [VerfasserIn]
Fang, Qianrong [VerfasserIn]

Links:

Volltext

Themen:

Journal Article

Anmerkungen:

Date Completed 08.02.2023

Date Revised 08.02.2023

published: Print-Electronic

Citation Status PubMed-not-MEDLINE

doi:

10.1021/jacs.2c13817

funding:

Förderinstitution / Projekttitel:

PPN (Katalog-ID):

NLM352293705