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Novel benzimidazole-linked microporous conjugated polymers for highly selective adsorption and photocatalytic reduction of diluted CO2

Integrated capture and photoreduction of diluted CO2 into energy-rich fuels represents an important challenge in renewable energy research and is attracting remarkable attention. In this study, two new benzimidazole-linked conjugated microporous polymers (CMPs), namely TFPA-DAB and TFPT-DAB, have be...

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Published in:Green chemistry : an international journal and green chemistry resource : GC 2023-11, Vol.25 (22), p.9335-9342
Main Authors: Wu, Wei, Feng, Chunyuan, Chen, Mantao, Tan, Qin, Deng, Yue, Zeng, Chao, Zhong, Lixiang, Dai, Chunhui
Format: Article
Language:English
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Summary:Integrated capture and photoreduction of diluted CO2 into energy-rich fuels represents an important challenge in renewable energy research and is attracting remarkable attention. In this study, two new benzimidazole-linked conjugated microporous polymers (CMPs), namely TFPA-DAB and TFPT-DAB, have been constructed by the condensation of 3,3′-diaminobenzidine (DAB) with tris(4-formylphenyl)amine (TFPA) and 2,4,6-tris(4-formylphenyl)-1,3,5-triazine (TFPT), respectively. The abundant basic N sites within the polymer network endow both TFPA-DAB (44.82 cm3 g−1) and TFPT-DAB (53.21 cm3 g−1) with high CO2 uptake at 273 K and 1 bar. Initial slope selectivity calculations demonstrated that TFPT-DAB possessed excellent CO2/N2 selectivity of 103 in comparison with TPFA-DAB (85) at 273 K as a result of changing the polymer core from 2,4,6-triphenyl-1,3,5-triazine to triphenylamine. Moreover, TFPT-DAB showed a narrower band gap down to 2.35 eV and better interface charge transfer than TFPA-DAB. Accordingly, under a 1% CO2/N2 atmosphere with water vapor as the electron donor, TFPT-DAB without a cocatalyst exhibited a superior CO production rate (CPR) of up to 178.45 μmol h−1 g−1 with almost 100% reaction selectivity (>420 nm), which is 5 times that of TFPA-DAB (35.31 μmol h−1 g−1) and ranks among the highest of known photocatalysts for gas–solid-phase CO2 reduction to date. This contribution indicates the bright prospect of benzimidazole-linked CMPs for highly efficient photoreduction of low-content CO2 in industrial exhaust.
ISSN:1463-9262
1463-9270
DOI:10.1039/d3gc02966b