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Dye-sensitized solar cells based on Fe N-heterocyclic carbene photosensitizers with improved rod-like push-pull functionality

Lindh, Linnea (author)
Lund University,Lunds universitet,NanoLund: Centre for Nanoscience,Annan verksamhet, LTH,Lunds Tekniska Högskola,Kemisk fysik,Enheten för fysikalisk och teoretisk kemi,Kemiska institutionen,Institutioner vid LTH,Beräkningskemi,Other operations, LTH,Faculty of Engineering, LTH,Chemical Physics,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,Computational Chemistry,Faculty of Engineering, LTH,Lund Univ, Dept Chem, Chem Phys Div, Box 124, SE-22100 Lund, Sweden.;Lund Univ, Dept Chem, Theoret Chem Div, Box 124, SE-22100 Lund, Sweden.
Gordivska, Olga (author)
Lund University,Lunds universitet,Centrum för analys och syntes,Kemiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Centre for Analysis and Synthesis,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,Lund Univ, Ctr Anal & Synth, Dept Chem, Box 124, SE-22100 Lund, Sweden.
Persson, Samuel (author)
Lund University,Lunds universitet,Centrum för analys och syntes,Kemiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Centre for Analysis and Synthesis,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,Lund Univ, Ctr Anal & Synth, Dept Chem, Box 124, SE-22100 Lund, Sweden.
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Michaels, Hannes (author)
Uppsala universitet,Uppsala University,University of Newcastle upon Tyne,Fysikalisk kemi,Uppsala Univ, Dept Chem, Angstrom Lab, Box 523, SE-75120 Uppsala, Sweden.;Newcastle Univ, Sch Nat & Environm Sci, Bedson Bldg, Newcastle Upon Tyne NE1 7RU, Tyne & Wear, England.
Fan, Hao (author)
Lund University,Lunds universitet,Centrum för analys och syntes,Kemiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Centre for Analysis and Synthesis,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,Lund Univ, Ctr Anal & Synth, Dept Chem, Box 124, SE-22100 Lund, Sweden.
Chábera, Pavel (author)
Lund University,Lunds universitet,NanoLund: Centre for Nanoscience,Annan verksamhet, LTH,Lunds Tekniska Högskola,Kemisk fysik,Enheten för fysikalisk och teoretisk kemi,Kemiska institutionen,Institutioner vid LTH,Other operations, LTH,Faculty of Engineering, LTH,Chemical Physics,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,Lund Univ, Dept Chem, Chem Phys Div, Box 124, SE-22100 Lund, Sweden.
Rosemann, Nils W. (author)
Lund University,Lunds universitet,NanoLund: Centre for Nanoscience,Annan verksamhet, LTH,Lunds Tekniska Högskola,Centrum för analys och syntes,Kemiska institutionen,Institutioner vid LTH,Kemisk fysik,Enheten för fysikalisk och teoretisk kemi,Other operations, LTH,Faculty of Engineering, LTH,Centre for Analysis and Synthesis,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,Chemical Physics,Physical and theoretical chemistry,Faculty of Engineering, LTH,Lund Univ, Dept Chem, Chem Phys Div, Box 124, SE-22100 Lund, Sweden.;Lund Univ, Ctr Anal & Synth, Dept Chem, Box 124, SE-22100 Lund, Sweden.
Gupta, Arvind Kumar (author)
Lund University,Lunds universitet,Centrum för analys och syntes,Kemiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Centre for Analysis and Synthesis,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,Lund Univ, Ctr Anal & Synth, Dept Chem, Box 124, SE-22100 Lund, Sweden.
Benesperi, Iacopo (author)
University of Newcastle upon Tyne,Lund University,Lund Univ, Ctr Anal & Synth, Dept Chem, Box 124, SE-22100 Lund, Sweden.;Newcastle Univ, Sch Nat & Environm Sci, Bedson Bldg, Newcastle Upon Tyne NE1 7RU, Tyne & Wear, England.
Uhlig, Jens (author)
Lund University,Lunds universitet,NanoLund: Centre for Nanoscience,Annan verksamhet, LTH,Lunds Tekniska Högskola,Kemisk fysik,Enheten för fysikalisk och teoretisk kemi,Kemiska institutionen,Institutioner vid LTH,Other operations, LTH,Faculty of Engineering, LTH,Chemical Physics,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,Lund Univ, Dept Chem, Chem Phys Div, Box 124, SE-22100 Lund, Sweden.
Prakash, Om (author)
Lund University,Lunds universitet,Centrum för analys och syntes,Kemiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Centre for Analysis and Synthesis,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,Lund Univ, Ctr Anal & Synth, Dept Chem, Box 124, SE-22100 Lund, Sweden.
Sheibani, Esmaeil (author)
Lund University,Lunds universitet,Centrum för analys och syntes,Kemiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Centre for Analysis and Synthesis,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,Lund Univ, Ctr Anal & Synth, Dept Chem, Box 124, SE-22100 Lund, Sweden.
Kjaer, Kasper S. (author)
Lund University,Lund Univ, Dept Chem, Chem Phys Div, Box 124, SE-22100 Lund, Sweden.
Boschloo, Gerrit (author)
Uppsala universitet,Uppsala University,Fysikalisk kemi
Yartsev, Arkady (author)
Lund University,Lunds universitet,NanoLund: Centre for Nanoscience,Annan verksamhet, LTH,Lunds Tekniska Högskola,Kemisk fysik,Enheten för fysikalisk och teoretisk kemi,Kemiska institutionen,Institutioner vid LTH,Other operations, LTH,Faculty of Engineering, LTH,Chemical Physics,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,Lund Univ, Dept Chem, Chem Phys Div, Box 124, SE-22100 Lund, Sweden.
Freitag, Marina (author)
Uppsala universitet,Uppsala University,University of Newcastle upon Tyne,Fysikalisk kemi,Newcastle Univ, Sch Nat & Environm Sci, Bedson Bldg, Newcastle Upon Tyne NE1 7RU, Tyne & Wear, England.
Lomoth, Reiner (author)
Uppsala universitet,Uppsala University,Fysikalisk kemi
Persson, Petter (author)
Lund University,Lunds universitet,NanoLund: Centre for Nanoscience,Annan verksamhet, LTH,Lunds Tekniska Högskola,Beräkningskemi,Enheten för fysikalisk och teoretisk kemi,Kemiska institutionen,Institutioner vid LTH,Other operations, LTH,Faculty of Engineering, LTH,Computational Chemistry,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,Theoretical Chemistry Division, Department of Chemistry, Lund University, Box 124, SE-22100 Lund, Sweden
Wärnmark, Kenneth (author)
Lund University,Lunds universitet,NanoLund: Centre for Nanoscience,Annan verksamhet, LTH,Lunds Tekniska Högskola,Centrum för analys och syntes,Kemiska institutionen,Institutioner vid LTH,Other operations, LTH,Faculty of Engineering, LTH,Centre for Analysis and Synthesis,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,Lund Univ, Ctr Anal & Synth, Dept Chem, Box 124, SE-22100 Lund, Sweden.
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 (creator_code:org_t)
2021
2021
English 19 s.
In: Chemical Science. - : Royal Society of Chemistry (RSC). - 2041-6520 .- 2041-6539. ; 12:48, s. 16035-16053
Related links:
http://dx.doi.org/10... (free)
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https://pubs.rsc.org...
https://doi.org/10.1...
https://lup.lub.lu.s...
https://doi.org/10.1...
https://urn.kb.se/re...
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  • Journal article (peer-reviewed)
Abstract Subject headings
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  • 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 TiO2back 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.

Subject headings

NATURVETENSKAP  -- Kemi -- Fysikalisk kemi (hsv//swe)
NATURAL SCIENCES  -- Chemical Sciences -- Physical Chemistry (hsv//eng)
NATURVETENSKAP  -- Fysik -- Atom- och molekylfysik och optik (hsv//swe)
NATURAL SCIENCES  -- Physical Sciences -- Atom and Molecular Physics and Optics (hsv//eng)

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