Abstract
Photosynthetic reaction centers catalyze the majority of solar energy conversion on the Earth. Under low-intensity illumination, this is achieved with a near-unity quantum efficiency, almost every absorbed photon producing a photochemical charge separation. Biohybrid technologies seek to capture the high efficiency of natural photoproteins by combining them with man-made electrodes. However, the transfer of photoproteins from their membrane environment into an abiotic architecture invariably results in efficiency losses. Here, we combined spectroscopy and analytical electrochemistry to identify the loss processes in a reaction-center-based biophotoelectrode. While over 90% efficient under low-intensity illumination, the biophotoelectrode efficiency dropped to ∼11% under high-intensity illumination. This loss stemmed from bottlenecks in electron transfer that rendered 60% of reaction centers inactive, as well as a short-circuiting of 73% of the separated charge from active reaction centers. The quantitative insights into loss processes presented in this work will be instrumental in shaping future rational design of biophotoelectrode devices.
| Original language | English |
|---|---|
| Pages (from-to) | 529-544 |
| Number of pages | 16 |
| Journal | Joule |
| Volume | 7 |
| Issue number | 3 |
| DOIs | |
| Publication status | Published - 15 Mar 2023 |
Bibliographical note
Funding Information:This work was supported by the Netherlands Organization for Scientific Research (NWO) TTW Veni Project No. 16866 (V.M.F.), the NWO-Vici Project No. 86510013 (R.C.), the NWO-TTW Project No. 14595 (R.N.F.), the European Union's Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement No. 799083 (W.J.N.) and No. 101068908 (V.M.F.), the Biotechnology and Biological Sciences Research Council and Engineering and Physical Sciences Research Council of the UK Grant BB/L01386X/1 (M.R.J.), and the BrisSynBio Synthetic Biology Research Centre at the University of Bristol (M.R.J.). Molecular graphics were performed with the UCSF Chimera package. Chimera is developed by the Resource for Biocomputing, Visualization, and Informatics at the University of California, San Francisco (supported by NIGMS P41-GM103311). M.R.J. provided purified RC-LH1 complexes. V.M.F. and W.J.N. conceived the research project. V.M.F. constructed the IO-mITO RC-LH1 biophotoelectrode. V.M.F. and W.J.N. designed the experiments and performed the investigation. Supervision was provided by W.J.N. R.C. and V.M.F. All authors discussed the results, wrote, and commented on, the manuscript. The authors declare no competing interests. We support inclusive, diverse, and equitable conduct of research.
Funding Information:
This work was supported by the Netherlands Organization for Scientific Research (NWO) TTW Veni Project No. 16866 (V.M.F.), the NWO -Vici Project No. 86510013 (R.C.), the NWO -TTW Project No. 14595 (R.N.F.), the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement No. 799083 (W.J.N.) and No. 101068908 (V.M.F.), the Biotechnology and Biological Sciences Research Council and Engineering and Physical Sciences Research Council of the UK Grant BB/L01386X/1 (M.R.J.), and the BrisSynBio Synthetic Biology Research Centre at the University of Bristol (M.R.J.). Molecular graphics were performed with the UCSF Chimera package. Chimera is developed by the Resource for Biocomputing, Visualization, and Informatics at the University of California, San Francisco (supported by NIGMS P41-GM103311 ).
Publisher Copyright:
© 2023 Elsevier Inc.
Research Groups and Themes
- Bristol BioDesign Institute
- BrisSynBio