Aim 1 aims to establish the toolbox needed to interface the biotic with the abiotic components:
i) We expanded current state-of-the-art ITO electrode design to TiO2 and graphene and allowed for the incorporation of live cells [J. Am. Chem. Soc., 2018, 140, 6-9; Nano Lett., 2019, 19, 1844-1850; Angew. Chem. Int. Ed., 2019, 58, 4601-1605; Proc. Natl. Acad. Sci, 2020, 117, 5074-5080].
ii) We integrated state-of-the-art photovoltaic componements (p-Si and lead halide perovskites) with enzymes [Angew. Chem. Int. Ed., 2018, 57, 10595-10599; ACS Energy Lett., 2020, 12, 8176-8282; ACS Catal., 2021, 11, 1868-1876].
Aim 2 develops new approaches to understand the biotic-abiotic interface:
i) A Mo-containing formate dehydrogenase was characterised using a combination of inhibition studies, electrochemistry, QCM and ATR-IR spectroscopy and modelling [J. Am. Chem. Soc., 2017, 139, 29, 9927-9936; J. Am. Chem. Soc., 2020, 142, 12226-12236; Angew. Chem. Int. Ed., 2019, 58, 4601-1605]. Some of those techniques were also used to investigate the whole cell-electrode interface [J. Am. Chem. Soc., 2020, 142, 5194-5203]
ii) The protein conduit, MtrC, was identified for high performance H2O2 reduction when developing Raman spectroscopy [J. Am. Chem. Soc., 2017, 139, 9, 3324-3327].
iii) Rotating ring disk electrodes were established to study photo-induced charge conversion events by protein-films [J. Am. Chem. Soc., 2018, 140, 17923-17931].
iv) We have contributed to the development of protein film electrochemical EPR spectroscopy [Chem. Commun., 2019, 55, 8840-8843]
v) A carboxysome-inspired CO2 reduction system [Angew. Chem. Int. Ed., 2023, 62, e202218782] and a carbon dot biohybrid system [ J. Am. Chem. Soc. 2022, 144, 14207−14216] have been characterised.
vi) The orientation of enzymes on electrodes [ACS Catal., 2022, 12, 1886−1897] as well as the local environment in bioelectrochemistry has been unraveled [Proc. Natl. Acad. Sci USA, 2022, 119, e2114097119 and Nature Chem., 2022, 14, 417–424];
vii) We have contributed to the understanding of enzyme mechanisms [J. Am. Chem. Soc., 2022, 144, 18296−18304] and identification of ultra-fast quenching of Photosystem II [Nature, 2023, 615, 836-840].
Aim 3 establishes novel proof-of-concept solar fuel generation pathways via semi-artificial photosynthesis:
i) We have accomplished the wiring of enzymes for solar-driven overall bias-free water splitting and CO2 reduction [Nature Energy, 2018, 3, 944-951; J. Am. Chem. Soc., 2018, 140, 16418-16422].
ii) Reversible interconversion of formate into H2/CO2 has been accomplished with a pair of wired redox enzymes (J. Am. Chem. Soc., 2019, 141, 17498-17502]
iii) Semi-artificial devices and systems have been assembled: simultaneous CO2 and cellulose to formate conversion [Angew. Chem. Int. Ed., 2023, 62, e2022158]; simultaneous CO2 and plastic upcycling [Nature Synth., 2023, 2, 182–192]; microbial plastic fermentation [Angew. Chem. Int. Ed. 2022, 61, e202211057]; bacteria photocatalyst sheets for CO2 utilisation [Nature Catal. 2022, 5, 633–641], solar CO2 utilisation coupled to alcohol oxidation [Nature Synth., 2022, 1, 77–86]; and a semi-artificial leave for CO2-to-formate conversion [Angew. Chem. Int. Ed., 2022, 60, 26303 –26307].
iv) The development of the semi-artificial devices has been translated into synthetic prototypes for bias-free solar fuel production: Thermoelectric-photoelectrochemical water splitting devices [J. Am. Chem. Soc., 2023, 145, 13709−13714] and the floating artificial leave [Nature, 2022, 608, 518–522].
vi) The insights from this ERC project have resulted in a bio-electrocatalytic platform for food waste upcycling [ACS Catal., 2023, 12, 13360−13371] as well as synthetic ligand tuning on quantum dots for CO2 reduction [Chem. Sci, 2022, 13, 5988–5998 and Chem. Sci., 2021, 12, 9078–9087].
Reviews: Acc. Chem. Res., 2019, 52, 1439-1448; Nat. Rev. Chem., 2020, 4, 6-21; Nature Nanotechn., 2018, 13, 890-899; Chem. Soc. Rev., 2020, 49, 4926-4952; Acc. Chem. Res., 2022, 55, 3376−3386; Nature Catal., 2023, 6, 657–665; Nature Rev. Methods Primers, 2023, 3, 61.
