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1.
Adv Mater ; 35(40): e2304170, 2023 Oct.
Article in English | MEDLINE | ID: mdl-37363880

ABSTRACT

Artificial photosynthetic diluted CO2 reduction directly driven by natural sunlight is a challenging, but promising way to realize carbon-resources recycling utilization. Herein, a three-in-one photocatalytic system of CO2 enrichment, CO2 reduction and H2 O oxidation sites is designed for diluted CO2 reduction. A Zn-Salen-based covalent organic framework (Zn-S-COF) with oxidation and reductive sites is synthesized; then, ionic liquids (ILs) are loaded into the pores. As a result, [Emim]BF4 @Zn-S-COF shows a visible-light-driven CO2 -to-CO conversion rate of 105.88 µmol g-1 h-1 under diluted CO2 (15%) atmosphere, even superior than most photocatalysts in high concentrations CO2 . Moreover, natural sunlight driven diluted CO2 reduction rate also reaches 126.51 µmol g-1 in 5 h. Further experiments and theoretical calculations reveal that the triazine ring in the Zn-S-COF promotes the activity of H2 O oxidation and CO2 reduction sites, and the loaded ILs provide an enriched CO2 atmosphere, realizing the efficient photocatalytic activity in diluted CO2 reduction.

2.
J Colloid Interface Sci ; 633: 233-242, 2023 Mar.
Article in English | MEDLINE | ID: mdl-36446216

ABSTRACT

The construction of tightly integrated heterostructures with metal-organic frameworks (MOFs) and covalent organic frameworks (COFs) has been confirmed to be an effective way for improved hydrogen evolution. However, the reported tightly integrated MOF/COF hybrids were usually limited to the covalent connection of COFs with aldehyde groups and NH2-MOF via Schiff base reaction, restricting the development of MOF/COF hybrids. Herein, a covalent triazine framework (CTF-1), a subtype of crystalline COFs, was integrated with a conductive two-dimensional (2D) MOF (Ni-CAT-1) by a novel coordinating connection mode for significantly enhanced visible-light-driven hydrogen evolution. The terminal amidine groups in the CTF-1 layers offer dual N sites for the coordination of metal ions, which provides the potential of coordinating connection between CTF-1 and Ni-CAT-1. The conductive 2D Ni-CAT-1 in Ni-CAT-1/CTF-1 hybrids effectively facilitates the separation of photogenerated carriers of CTF-1 component, and the resultant hybrid materials show significantly enhanced photocatalytic hydrogen evolution activity. In particular, the Ni-CAT-1/CTF-1 (1:19) sample exhibits the maximum hydrogen evolution rate of 8.03 mmol g-1h-1, which is about four times higher than that of the parent CTF-1 (1.96 mmol g-1h-1). The enhanced photocatalytic activity of Ni-CAT-1/CTF-1 is mainly attributed to the incorporation of conductive MOF which leads to the formation of a Z-Scheme heterostructure, promoting the electron transfer in hybrid materials. The coordinating combination mode of Ni-CAT-1 and CTF-1 in this work provides a novel strategy for constructing tightly integrated MOF/COF hybrid materials.

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