Charge-transfer regulated visible light driven photocatalytic H2 production and CO2 reduction in tetrathiafulvalene based coordination polymer gel

Parul Verma, Ashish Singh, Faruk Ahamed Rahimi, Pallavi Sarkar, Sukhendu Nath, Swapan Kumar Pati and Tapas Kumar Maji ()
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Parul Verma: Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur
Ashish Singh: Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur
Faruk Ahamed Rahimi: Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur
Pallavi Sarkar: Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur
Sukhendu Nath: Bhabha Atomic Research Centre
Swapan Kumar Pati: Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur
Tapas Kumar Maji: Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur

Nature Communications, 2021, vol. 12, issue 1, 1-14

Abstract: Abstract The much-needed renewable alternatives to fossil fuel can be achieved efficiently and sustainably by converting solar energy to fuels via hydrogen generation from water or CO2 reduction. Herein, a soft processable metal-organic hybrid material is developed and studied for photocatalytic activity towards H2 production and CO2 reduction to CO and CH4 under visible light as well as direct sunlight irradiation. A tetrapodal low molecular weight gelator (LMWG) is synthesized by integrating tetrathiafulvalene (TTF) and terpyridine (TPY) derivatives through amide linkages and results in TPY-TTF LMWG. The TPY-TTF LMWG acts as a linker, and self-assembly of this gelator molecules with ZnII ions results in a coordination polymer gel (CPG); Zn-TPY-TTF. The Zn-TPY-TTF CPG shows high photocatalytic activity towards H2 production (530 μmol g−1h−1) and CO2 reduction to CO (438 μmol g−1h−1, selectivity > 99%) regulated by charge-transfer interactions. Furthermore, in situ stabilization of Pt nanoparticles on CPG (Pt@Zn-TPY-TTF) enhances H2 evolution (14727 μmol g−1h−1). Importantly, Pt@Zn-TPY-TTF CPG produces CH4 (292 μmol g−1h−1, selectivity > 97%) as CO2 reduction product instead of CO. The real-time CO2 reduction reaction is monitored by in situ DRIFT study, and the plausible mechanism is derived computationally.

Date: 2021
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DOI: 10.1038/s41467-021-27457-4

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