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Achieving an unprecedented hydrogen evolution rate by solvent-exfoliated CPP-based photocatalysts

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Abstract

How to prompt higher photocatalytic hydrogen production (PHP) efficiency from water to achieve practical applications still remains a big challenge with conjugated porous polymers (CPP)-based photocatalysts. Herein, we developed a simple and efficient cosolvent-assisted strategy to significantly improve the photocatalytic efficiency of CPP-based photocatalysts by introducing water-soluble aprotic bipolar co-solvents, including N,N-dimethylformamide (DMF), N,N-dimethylacetamide (DMAc), and N-methyl pyrrolidone (NMP). The PHP activity of the pyrene–bithiophene-based CPP (named CP-St) using ascorbic acid (AA) as a sacrificial electron donor could be excellently accelerated in the presence of an aprotic bipolar NMP solvent. CP-St dispersed in an NMP/H2O/AA mixed solution under visible-light (λ > 420 nm) irradiation without the aid of a Pt cocatalyst achieved an unprecedented hydrogen evolution rate (HER) of 190.7 mmol h−1 g−1. As a result, 6 mg CP-St amazingly produced 128.1 mL H2 (∼5.72 mmol) under visible-light irradiation for only 5 h. Excitingly, by introducing 0.5 wt% Pt cocatalyst into the NMP/H2O/AA system, the HER of CP-St could be further boosted to 303.7 mmol h−1 g−1 (1.82 mmol h−1/6 mg), which represents the highest photocatalytic HER ever reported. This outstanding photocatalytic performance is mainly ascribed to the enhanced dispersity, strong hydrogen-bond interactions, and exfoliation effect by the NMP solvent. This study provides us with some new design ideas and opportunities for effectively catering to the actual hydrogen production demand.

Graphical abstract: Achieving an unprecedented hydrogen evolution rate by solvent-exfoliated CPP-based photocatalysts

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Supplementary files

Article information


Submitted
10 Dec 2019
Accepted
30 Jan 2020
First published
31 Jan 2020

J. Mater. Chem. A, 2020, Advance Article
Article type
Paper

Achieving an unprecedented hydrogen evolution rate by solvent-exfoliated CPP-based photocatalysts

J. Cheng, L. Liu, G. Liao, Z. Shen, Z. Tan, Y. Xing, X. Li, K. Yang, L. Chen and S. Liu, J. Mater. Chem. A, 2020, Advance Article , DOI: 10.1039/C9TA13514F

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