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Synthesis of water-soluble Ni(II) complexes and their role in photo-induced electron transfer with MPA-CdTe quantum dots

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Abstract

Photocatalytic water splitting using solar energy for hydrogen production offers a promising alternative form of storable and clean energy for the future. To design an artificial photosynthesis system that is cost-effective and scalable, earth abundant elements must be used to develop each of the components of the assembly. To develop artificial photosynthetic systems, we need to couple a catalyst for proton reduction to a photosensitizer and understand the mechanism of photo-induced electron transfer from the photosensitizer to the catalyst that serves as the fundamental step for photocatalysis. Therefore, our work is focused on the study of light driven electron transfer kinetics from the quantum dot systems made with inorganic chalcogenides in the presence of Ni-based reduction catalysts. Herein, we report the synthesis and characterization of four Ni(II) complexes of tetradentate ligands with amine and pyridine functionalities (N2/Py2) and their interactions with CdTe quantum dots stabilized by 3-mercaptopropionic acid. The lifetime of the quantum dots was investigated in the presence of the Ni complexes and absorbance, emission and electrochemical measurements were performed to gain a deeper understanding of the photo-induced electron transfer process.

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Abbreviations

AP:

Artificial photosynthesis

QDs:

Quantum dots

MPA:

3-Mercaptopropionic acid

UV–Vis:

Ultraviolet-Visible

Ksv :

Stern–Volmer quenching constant

kq :

Bimolecular quenching rate constant

TCSPC:

Time-correlated single-photon counting

Eg :

Bandgap

Evb :

Valence band energy level

Ecb :

Conduction band energy level

NHE:

Normal hydrogen electrode

NMR:

Nuclear magnetic resonance

ESI–MS:

Electrospray ionization mass spectrometry

RT:

Room temperature

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Acknowledgements

This work was funded by the University of Alabama in Huntsville, Individual Investigator Distinguished Research (IIDR) awards to Anusree Mukherjee and Seyed M. Sadeghi.

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Correspondence to Anusree Mukherjee.

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The authors declare no competing financial interest.

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Botcha, N.K., Gutha, R.R., Sadeghi, S.M. et al. Synthesis of water-soluble Ni(II) complexes and their role in photo-induced electron transfer with MPA-CdTe quantum dots. Photosynth Res 143, 143–153 (2020). https://doi.org/10.1007/s11120-019-00668-z

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  • DOI: https://doi.org/10.1007/s11120-019-00668-z

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