2D Copper–Porphyrin Metal–Organic Framework Nanosheet‐Photosensitized TiO2 for Efficiently Broadband Light‐Driven Conversion of CO2 to CH4

Author:

Xu Xiaoqian1,Wang Hui1,Gao Ting1,Luo Tian1,Zvereva Irina2,Orudzhev Farid3,Wang Chuanyi1ORCID,Bahnemann Detlef Wemer145ORCID

Affiliation:

1. School of Environmental Science and Engineering Shaanxi University of Science and Technology Xi'an 710021 P. R. China

2. Institute of Chemistry Department of Chemical Thermodynamics and Kinetics Center for Thermal Analysis and Calorimetry St. Petersburg State University Universitetskiy Pr. 26 Peterhof 198504 Russia

3. Geothermal and Renewal Energy Institute of the Russian Academy of Sciences I. Shamil Ave. 39a Makhachkala Dagestan 367030 Russian

4. Institute for Technical Chemistry Leibniz University Hannover 30167 Hannover Germany

5. Laboratory of Photoactive Nanocomposite Materials Saint Petersburg State University Saint‐Petersburg 198504 Russia

Abstract

The effective utilization of light is crucial in the use of the solar energy for CO2 conversion into valuable fuels and chemicals, in which improving the photocatalytic materials’ capacity to absorb light is a key. Herein, a 2D copper–porphyrin metal−organic framework (MOF)‐photosensitized titania, TiO2/Zn–CuTCPP, is reported, which can absorb wide range of light and photoreduce CO2 with high efficiency under full spectrum irradiation. Fluorescence spectral analysis elucidates the relationship between the photocatalytic activity and the electron–hole separation efficiency. In addition, mechanistic information obtained from electron paramagnetic resonance and in situ infrared analyses demonstrates that the presence of Cu–N4 site in the MOF structure is conducive to the generation of hydrogen free radicals (•H), which plays a key role in the formation of intermediates, thus facilitating the hydrogenation in the reaction process. Consequently, TiO2/Zn–CuTCPP significantly enhances the photocatalytic conversion of CO2 into CH4 with a yield 14 times higher than that of P25.

Funder

Shaanxi Administration of Foreign Expert Affairs

Publisher

Wiley

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