An Efficient Copper-Based Redox Shuttle Bearing a Hexadentate Polypyridyl Ligand for DSCs under Low-Light Conditions

Devdass, Anthony; Watson, Jonathon; Firestone, Eric; Hamann, Thomas W.; Delcamp, Jared H.; Jurss, Jonah W.

doi:10.1021/acsaem.2c00344

Title: An Efficient Copper-Based Redox Shuttle Bearing a Hexadentate Polypyridyl Ligand for DSCs under Low-Light Conditions

Journal Article · 03 May 2022 · ACS Applied Energy Materials

DOI: https://doi.org/10.1021/acsaem.2c00344 · OSTI ID:2341748

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^[2]; Firestone, Eric ^[3];

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Univ. of Mississippi, University, MS (United States); Michigan State University
Univ. of Mississippi, University, MS (United States)
Michigan State Univ., East Lansing, MI (United States)

A Cu complex featuring a hexadentate ligand was synthesized and evaluated as a redox shuttle in dye-sensitized solar cell (DSC) devices, which exhibited excellent performance under low-light conditions. Cu-based redox shuttles (RSs) have been shown to perform remarkably well under low-light conditions; however, most of the known Cu-based RSs employ bidentate pyridyl ligands and often require bulky flanking groups adjacent to the nitrogen donors of these ligands to prevent distortion and binding of exogenous Lewis bases such as 4-tert-butylpyridine (TBP) that are added to enhance cell performance. Without the bulky substituents, the bidentate ligands are susceptible to ligand exchange with TBP. In this context, we have developed a Cu-based RS with a preorganized multidentate ligand designed to facilitate efficient electron transfer kinetics and high stability via the chelate effect. The Cu system, [Cu(bpyPY4)]^2+/+, reported here is supported by the hexadentate polypyridyl ligand bpyPY4 (6,6'-bis(1,1-di(pyridine-2-yl)ethyl)-2,2'-bipyridine) and examined as a RS in DSCs. From X-ray crystallography and variable-temperature ¹H NMR studies, bpyPY4 provides a dynamic coordination environment around the metal center. Cyclic voltammetry and UV–visible and NMR spectroscopy indicate that noncoordinated pyridyl donors block binding of TBP to copper. DSC devices using [Cu(bpyPY4)]^2+/+ as the redox electrolyte gave a power conversion efficiency (PCE) value of 4.9% under 1 sun illumination (100 mW/cm²). Strikingly, the device performance increased to 11.11% when irradiated with 2400 lux (0.5 mW/cm²) via a fluorescent lamp light source and improved further to 15.2% PCE at 13500 lux (2.10 mW/cm²). In conclusion, the Cu redox shuttle is an intriguing candidate for implementation with narrow band gap sensitizers with low oxidation potentials, which are important for high photocurrent DSC devices.

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Research Organization:: Michigan State Univ., East Lansing, MI (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); National Science Foundation (NSF)

Grant/Contract Number:: SC0017342

OSTI ID:: 2341748

Alternate ID(s):: OSTI ID: 1978225

Journal Information:: ACS Applied Energy Materials, Journal Name: ACS Applied Energy Materials Journal Issue: 5 Vol. 5; ISSN 2574-0962

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Structure determination of nitrito- and thiocyanato-copper(II) complexes: X-ray structures of [Cu(Medpt)(ONO)(H2O)]ClO4 (1), [Cu(dien)(ONO)]ClO4 (2) and [Cu2(Medpt)2(μN,S-NCS)2](ClO4)2 (3) (Medpt=3,3′-diamino-N-methyldipropylamine and dien=diethylenetriamine) Mautner, Franz A.; Vicente, Ramon; Massoud, Salah S. Polyhedron, Vol. 25, Issue 7 https://doi.org/10.1016/j.poly.2005.11.008	journal	May 2006
Role of Electrolytes on Charge Recombination in Dye-Sensitized TiO₂ Solar Cell (1): The Case of Solar Cells Using the I^-/I₃^- Redox Couple Nakade, Shogo; Kanzaki, Taisuke; Kubo, Wataru The Journal of Physical Chemistry B, Vol. 109, Issue 8 https://doi.org/10.1021/jp0460036	journal	January 2005
A low-cost, high-efficiency solar cell based on dye-sensitized colloidal TiO₂ films O'Regan, Brian; Grätzel, Michael Nature, Vol. 353, Issue 6346, p. 737-740 https://doi.org/10.1038/353737a0	journal	October 1991
Parameters Influencing the Efficiency of Electron Injection in Dye-Sensitized Solar Cells Koops, Sara E.; O’Regan, Brian C.; Barnes, Piers R. F. Journal of the American Chemical Society, Vol. 131, Issue 13 https://doi.org/10.1021/ja8091278	journal	April 2009
Probing Dye-Correlated Interplay of Energetics and Kinetics in Mesoscopic Titania Solar Cells with 4-tert-Butylpyridine Long, Huijin; Zhou, Difei; Zhang, Min The Journal of Physical Chemistry C, Vol. 115, Issue 29 https://doi.org/10.1021/jp202826m	journal	July 2011
Influence of alkylpyridine additives in electrolyte solution on the performance of dye-sensitized solar cell Kusama, Hitoshi; Konishi, Yoshinari; Sugihara, Hideki Solar Energy Materials and Solar Cells, Vol. 80, Issue 2 https://doi.org/10.1016/j.solmat.2003.08.001	journal	October 2003
Exploration on the Combination of Push-Pull Porphyrin Dyes and Copper(I/II) Redox Shuttles toward High-performance Dye-sensitized Solar Cells Higashino, Tomohiro; Iiyama, Hitomi; Nishimura, Issei Chemistry Letters, Vol. 49, Issue 8 https://doi.org/10.1246/cl.200317	journal	August 2020
A review of solar photovoltaic technologies Parida, Bhubaneswari; Iniyan, S.; Goic, Ranko Renewable and Sustainable Energy Reviews, Vol. 15, Issue 3 https://doi.org/10.1016/j.rser.2010.11.032	journal	April 2011

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37
hexadentate polypyridyl ligand
low-light conditions
copper-based redox shuttle
dye-sensitized solar cells
dynamic
fluxional coordination behavior
electron transfer kinetics

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