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There Is a Future for N-Heterocyclic Carbene Iron(II) Dyes in Dye-Sensitized Solar Cells: Improving Performance through Changes in the Electrolyte.

ABSTRACT: By systematic tuning of the components of the electrolyte, the performances of dye-sensitized solar cells (DSCs) with an N-heterocyclic carbene iron(II) dye have been significantly improved. The beneficial effects of an increased Li+ ion concentration in the electrolyte lead to photoconversion efficiencies (PCEs) up to 0.66% for fully masked cells (representing 11.8% relative to 100% set for N719) and an external quantum efficiency maximum (EQEmax) up to approximately 25% due to an increased short-circuit current density (JSC). A study of the effects of varying the length of the alkyl chain in 1-alkyl-3-methylimidazolium iodide ionic liquids (ILs) shows that a longer chain results in an increase in JSC with an overall efficiency up to 0.61% (10.9% relative to N719 set at 100%) on going from n-methyl to n-butyl chain, although an n-hexyl chain leads to no further gain in PCE. The results of electrochemical impedance spectroscopy (EIS) support the trends in JSC and open-circuit voltage (VOC) parameters. A change in the counterion from I- to [BF4]- for 1-propyl-3-methylimidazolium iodide ionic liquid leads to DSCs with a remarkably high JSC value for an N-heterocyclic carbene iron(II) dye of 4.90 mA cm-2, but a low VOC of 244 mV. Our investigations have shown that an increased concentration of Li+ in combination with an optimized alkyl chain length in the 1-alkyl-3-methylimidazolium iodide IL in the electrolyte leads to iron(II)-sensitized DSC performances comparable with those of containing some copper(I)-based dyes.

SUBMITTER: Karpacheva M

PROVIDER: S-EPMC6947502 | biostudies-literature | 2019 Dec

REPOSITORIES: biostudies-literature

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Project description:A new generation of octahedral iron(ii)-N-heterocyclic carbene (NHC) complexes, employing different tridentate C^N^C ligands, has been designed and synthesized as earth-abundant photosensitizers for dye sensitized solar cells (DSSCs) and related solar energy conversion applications. This work introduces a linearly aligned push-pull design principle that reaches from the ligand having nitrogen-based electron donors, over the Fe(ii) centre, to the ligand having an electron withdrawing carboxylic acid anchor group. A combination of spectroscopy, electrochemistry, and quantum chemical calculations demonstrate the improved molecular excited state properties in terms of a broader absorption spectrum compared to the reference complex, as well as directional charge-transfer displacement of the lowest excited state towards the semiconductor substrate in accordance with the push-pull design. Prototype DSSCs based on one of the new Fe NHC photosensitizers demonstrate a power conversion efficiency exceeding 1% already for a basic DSSC set-up using only the I-/I3 - redox mediator and standard operating conditions, outcompeting the corresponding DSSC based on the homoleptic reference complex. Transient photovoltage measurements confirmed that adding the co-sensitizer chenodeoxycholic acid helped in improving the efficiency by increasing the electron lifetime in TiO2. Time-resolved spectroscopy revealed spectral signatures for successful ultrafast (<100 fs) interfacial electron injection from the heteroleptic dyes to TiO2. However, an ultrafast recombination process results in undesirable fast charge recombination from TiO2 back to the oxidized dye, leaving only 5-10% of the initially excited dyes available to contribute to a current in the DSSC. On slower timescales, time-resolved spectroscopy also found that the recombination dynamics (longer than 40 μs) were significantly slower than the regeneration of the oxidized dye by the redox mediator (6-8 μs). Therefore it is the ultrafast recombination down to fs-timescales, between the oxidized dye and the injected electron, that remains as one of the main bottlenecks to be targeted for achieving further improved solar energy conversion efficiencies in future work.

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There Is a Future for N-Heterocyclic Carbene Iron(II) Dyes in Dye-Sensitized Solar Cells: Improving Performance through Changes in the Electrolyte.

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