@article{2e213b31ce60441d8ea83ef9857022ee,
title = "A photoelectrochemical-thermoelectric device for semi-artificial CO2 fixation employing full solar spectrum utilization",
abstract = "Natural and most artificial photosynthesis systems utilize a pair of light absorbers to convert CO2 into sugar and fuels. However, much of the solar energy is lost as unabsorbed (mainly infrared [IR]) irradiation and thermalization heat, limiting efficiency. Here, we show that a thermoelectric (TE) generator can harvest this waste heat toward unassisted CO2 reduction with a water-oxidizing BiVO4 photoanode upon irradiation by concentrated sunlight. We employ the enzyme formate dehydrogenase (FDh) as a model catalyst to achieve selective CO2-to-formate conversion with minimal overpotential. The catalytic activity of the FDh cathode and BiVO4 photoanode benefits from solar heating, enabling the bias-free semi-artificial FDh-TE-BiVO4 device to attain a 97% faradic yield for formate production under 3-sun irradiation. This work demonstrates unassisted CO2 reduction coupled to water oxidation using only a single semiconductor light absorber through effective waste heat utilization, overcoming the challenges of (non-)complementary light absorption and IR losses in both natural and artificial photosynthesis.",
keywords = "BiVO, continuum modelling, DTI-2: Explore, enzyme electrochemistry, heat management CO reduction, photoelectrocatalysis, photoelectrochemistry, solar fuels, solar thermal conversion, thermoelectric generator",
author = "Cobb, {Samuel J.} and Chanon Pornrungroj and Virgil Andrei and Badiani, {Vivek M.} and Lin Su and Manuel, {Rita R.} and Pereira, {In{\^e}s A.C.} and Erwin Reisner",
note = "Funding Information: We acknowledge support from the Leverhulme Trust for an Early Career Fellowship ( ECF-2021-072 to S.J.C. and ECF-2022-392 to L.S.), the Isaac Newton Trust (20.08(r) to S.J.C. and 22.08(c) to L.S.), the Cambridge Trust ( Cambridge Thai Foundation Award to C.P.), a Trinity-Henry Barlow Scholarship (to C.P.), the Cambridge Philosophical Society (to C.P.), the Program Management Unit for Human Resources and Institutional Development, Research, and Innovation ( B16F640166 to C.P.), the EPSRC Graphene CDT ( EP/L016087/1 to V.M.B.), St John\u2019s College Cambridge ( Title A Research Fellowship to V.A.), the European Research Council (ERC) for a Consolidator Grant (MatEnSAP, 682833 to E.R.) and a UKRI/ERC Advanced Grant ( EP/X030563/1 to E.R.), the Funda\u00E7\u00E3o para a Ci\u00EAncia e a Tecnologia (FCT, Portugal) for fellowship DFA/BD/7897/2020 (to R.R.M.), grant PTDC/BII-BBF/2050/2020 (to I.A.C.P.) and MOSTMICRO-ITQB unit ( UIDB/04612/2020 and UIDP/04612/2020 ), and Associated Laboratory LS4FUTURE ( LA/P/0087/2020 ). Funding Information: We acknowledge support from the Leverhulme Trust for an Early Career Fellowship (ECF-2021-072 to S.J.C. and ECF-2022-392 to L.S.), the Isaac Newton Trust (20.08(r) to S.J.C. and 22.08(c) to L.S.), the Cambridge Trust (Cambridge Thai Foundation Award to C.P.), a Trinity-Henry Barlow Scholarship (to C.P.), the Cambridge Philosophical Society (to C.P.), the Program Management Unit for Human Resources and Institutional Development, Research, and Innovation (B16F640166 to C.P.), the EPSRC Graphene CDT (EP/L016087/1 to V.M.B.), St John's College Cambridge (Title A Research Fellowship to V.A.), the European Research Council (ERC) for a Consolidator Grant (MatEnSAP, 682833 to E.R.) and a UKRI/ERC Advanced Grant (EP/X030563/1 to E.R.), the Funda\u00E7\u00E3o para a Ci\u00EAncia e a Tecnologia (FCT, Portugal) for fellowship DFA/BD/7897/2020 (to R.R.M.), grant PTDC/BII-BBF/2050/2020 (to I.A.C.P.) and MOSTMICRO-ITQB unit (UIDB/04612/2020 and UIDP/04612/2020), and Associated Laboratory LS4FUTURE (LA/P/0087/2020). Conceptualization, S.J.C. C.P. and E.R; investigation, S.J.C. C.P. V.M.B. L.S. and R.R.M.; resources, R.R.M. and I.A.C.P.; formal analysis, S.J.C. C.P. V.M.B. L.S. R.R.M.; writing \u2013 original draft, S.J.C. C.P. and E.R.; writing \u2013 review & editing, V.A. L.S. R.R.M. and I.A.C.P.; visualization, S.J.C. C.P. V.A. and L.S.; supervision, E.R.; funding acquisition, S.J.C. I.A.C.P. and E.R. The authors declare no competing interests. Publisher Copyright: {\textcopyright} 2024 The Author(s)",
year = "2024",
doi = "10.1016/j.device.2024.100505",
language = "English",
journal = "Device",
issn = "2666-9986",
publisher = "Cell Press",
}