期刊
ACS APPLIED MATERIALS & INTERFACES
卷 15, 期 21, 页码 25173-25183出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.2c14533
关键词
coordination polymer gel (CPG); porphyrin; iron hydrogenase; photocatalysis; visible light driven hydrogen evolution
资金
- Council of Scientific and Industrial Research (CSIR) , Govt. of India
- SERB, Dept. of Science and Technology (DST) , Govt. of India [12-RD-TFR-5.10-0100]
- Sheik Saqr senior fellowship
- Department of Atomic Energy (DAE) , Government of India
- [t CRG/2019/005951]
Self-assembled porphyrin-based coordination polymer gel has been developed as a soft photocatalyst material for hydrogen production from water under visible light, showing a significant enhancement in catalytic activity through the coassembly of a cocatalyst [Fe2(bdt)(CO)6]. The study supported a cascade electron transfer process for H2 production.
There has been a widespread interest in developing self-assembled porphyrin nanostructures to mimic nature's light-harvesting processes. Herein, porphyrin-based coordination polymer gel (CPG) has been developed as a soft photocatalyst material for hydrogen (H2) production from water under visible light. The CPG offers a hierarchical nanofibrous network structure obtained through self-assembly of a terpyridine alkyl-amide appended porphyrin (TPY-POR)-based low molecular weight gelator with ruthenium ions (RuII) and produces H2 with a rate of 5.7 mmol g-1 h-1 in the presence of triethylamine (TEA) as a sacrificial electron donor. Further, the [Fe2(bdt)(CO)6] (dbt = 1,2-benzenedithiol) cocatalyst, which can mimic the activity of iron hydrogenase, is coassembled in the CPG and shows remarkable improvement in H2 evolution (catalytic activity; rate similar to 10.6 mmol g-1 h-1 and turnover number similar to 1287). The significant enhancement in catalytic activity was supported by several controlled experiments, including femtosecond transient absorption (TA) spectroscopy and also DFT calculation. The TA study supported the cascade electron transfer process from porphyrin core to [Ru(TPY)2]2+ center, and subsequently, the electron transfers to the cocatalyst [Fe2(bdt)(CO)6] for H2 production.
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