{"entity": "publication", "iuid": "24eb7e2ba42842ca989bb4daf4614833", "timestamp": "2026-07-20T16:39:45.133Z", "links": {"self": {"href": "https://publications.scilifelab.se/publication/24eb7e2ba42842ca989bb4daf4614833.json"}, "display": {"href": "https://publications.scilifelab.se/publication/24eb7e2ba42842ca989bb4daf4614833"}}, "title": "Polymer Dots as Photoactive Membrane Vesicles for [FeFe]-Hydrogenase Self-Assembly and Solar-Driven Hydrogen Evolution.", "authors": [{"family": "Pavliuk", "given": "Mariia V", "initials": "MV"}, {"family": "Lorenzi", "given": "Marco", "initials": "M"}, {"family": "Morado", "given": "Dustin R", "initials": "DR", "orcid": "0000-0003-4693-3220", "researcher": {"href": "https://publications.scilifelab.se/researcher/eef09b7a95b64a699900bae6a5390e31.json"}}, {"family": "Gedda", "given": "Lars", "initials": "L"}, {"family": "Wrede", "given": "Sina", "initials": "S"}, {"family": "Mejias", "given": "Sara H", "initials": "SH", "orcid": "0000-0002-7440-2657", "researcher": {"href": "https://publications.scilifelab.se/researcher/454bc4ffb8f841a3a2118e74fa06ed02.json"}}, {"family": "Liu", "given": "Aijie", "initials": "A"}, {"family": "Senger", "given": "Moritz", "initials": "M", "orcid": "0000-0001-9225-4910", "researcher": {"href": "https://publications.scilifelab.se/researcher/da88e9696aa94341a7654e52a30604a2.json"}}, {"family": "Glover", "given": "Starla", "initials": "S", "orcid": "0000-0003-0318-7790", "researcher": {"href": "https://publications.scilifelab.se/researcher/db3c293a478a4a8092270494b902460e.json"}}, {"family": "Edwards", "given": "Katarina", "initials": "K"}, {"family": "Berggren", "given": "Gustav", "initials": "G", "orcid": "0000-0002-6717-6612", "researcher": {"href": "https://publications.scilifelab.se/researcher/2645e83be0d74ee184b47a2fd4d74976.json"}}, {"family": "Tian", "given": "Haining", "initials": "H", "orcid": "0000-0001-6897-2808", "researcher": {"href": "https://publications.scilifelab.se/researcher/cad36aa1812b4287bc2bf54f5b714ff1.json"}}], "type": "journal article", "published": "2022-08-03", "journal": {"title": "J. Am. Chem. Soc.", "issn": "1520-5126", "issn-l": "0002-7863", "volume": "144", "issue": "30", "pages": "13600-13611"}, "abstract": "A semiartificial photosynthesis approach that utilizes enzymes for solar fuel production relies on efficient photosensitizers that should match the enzyme activity and enable long-term stability. Polymer dots (Pdots) are biocompatible photosensitizers that are stable at pH 7 and have a readily modifiable surface morphology. Therefore, Pdots can be considered potential photosensitizers to drive such enzyme-based systems for solar fuel formation. This work introduces and unveils in detail the interaction within the biohybrid assembly composed of binary Pdots and the HydA1 [FeFe]-hydrogenase from Chlamydomonas reinhardtii. The direct attachment of hydrogenase on the surface of toroid-shaped Pdots was confirmed by agarose gel electrophoresis, cryogenic transmission electron microscopy (Cryo-TEM), and cryogenic electron tomography (Cryo-ET). Ultrafast transient spectroscopic techniques were used to characterize photoinduced excitation and dissociation into charges within Pdots. The study reveals that implementation of a donor-acceptor architecture for heterojunction Pdots leads to efficient subpicosecond charge separation and thus enhances hydrogen evolution (88 460 \u03bcmolH2\u00b7gH2ase-1\u00b7h-1). Adsorption of [FeFe]-hydrogenase onto Pdots resulted in a stable biohybrid assembly, where hydrogen production persisted for days, reaching a TON of 37 500 \u00b1 1290 in the presence of a redox mediator. This work represents an example of a homogeneous biohybrid system combining polymer nanoparticles and an enzyme. Detailed spectroscopic studies provide a mechanistic understanding of light harvesting, charge separation, and transport studied, which is essential for building semiartificial photosynthetic systems with efficiencies beyond natural and artificial systems.", "doi": "10.1021/jacs.2c03882", "pmid": "35863067", "labels": {"Cryo-EM": "Collaborative"}, "xrefs": [{"db": "pmc", "key": "PMC9354254"}], "notes": [], "created": "2022-07-25T12:24:29.139Z", "modified": "2023-12-04T10:19:40.478Z"}