Publicação
Solar Fuel Synthesis Using a Semiartificial Colloidal Z-Scheme
| Resumo: | The integration of enzymes with semiconductor light absorbers in semiartificial photosynthetic assemblies offers an emerging strategy for solar fuel production. However, such colloidal biohybrid systems rely currently on sacrificial reagents, and semiconductor-enzyme powder systems that couple fuel production to water oxidation are therefore needed to mimic an overall photosynthetic reaction. Here, we present a Z-scheme colloidal enzyme system that produces fuel with electrons sourced from water. This “closed-cycle” semiartificial approach utilizes particulate SrTiO3:La,Rh and BiVO4:Mo (light absorbers), hydrogenase or formate dehydrogenase (cocatalyst), and a molecular cobalt complex (a redox mediator). Under simulated solar irradiation, this system continuously generates molecular hydrogen or formate, while co-producing molecular oxygen for 10 h using only sunlight, water, and carbon dioxide as inputs. In-depth analysis using quartz crystal microbalance, photoelectrochemical impedance spectroscopy, transient photocurrent spectroscopy, and intensity-modulated photovoltage spectroscopy provides mechanistic understanding and characterization of the semiconductor-enzyme hybrid interface. This study provides a rational platform to assemble functional semiartificial colloidal Z-scheme systems for solar fuel synthesis. |
|---|---|
| Autores principais: | Liu, Yongpeng |
| Outros Autores: | Bin Mohamad Annuar, Ariffin; Rodríguez-Jiménez, Santiago; Yeung, Celine Wing See; Wang, Qian; Coito, Ana M.; Manuel, Rita R.; Pereira, Inês A.C.; Reisner, Erwin |
| Assunto: | Catalysis General Chemistry Biochemistry Colloid and Surface Chemistry |
| Ano: | 2024 |
| País: | Portugal |
| Tipo de documento: | artigo |
| Tipo de acesso: | acesso aberto |
| Instituição associada: | Universidade Nova de Lisboa |
| Idioma: | inglês |
| Origem: | Repositório Institucional da UNL |
| _version_ | 1868983137048985600 |
|---|---|
| author | Liu, Yongpeng |
| author2 | Bin Mohamad Annuar, Ariffin Rodríguez-Jiménez, Santiago Yeung, Celine Wing See Wang, Qian Coito, Ana M. Manuel, Rita R. Pereira, Inês A.C. Reisner, Erwin |
| author2_role | author author author author author author author author |
| author_facet | Liu, Yongpeng Bin Mohamad Annuar, Ariffin Rodríguez-Jiménez, Santiago Yeung, Celine Wing See Wang, Qian Coito, Ana M. Manuel, Rita R. Pereira, Inês A.C. Reisner, Erwin |
| author_role | author |
| contributor_name_str_mv | Instituto de Tecnologia Química e Biológica António Xavier (ITQB) ACS - American Chemical Society RUN |
| country_str | PT |
| creators_json_txt | [{\"Person.name\":\"Liu, Yongpeng\"},{\"Person.name\":\"Bin Mohamad Annuar, Ariffin\"},{\"Person.name\":\"Rodríguez-Jiménez, Santiago\"},{\"Person.name\":\"Yeung, Celine Wing See\"},{\"Person.name\":\"Wang, Qian\"},{\"Person.name\":\"Coito, Ana M.\"},{\"Person.name\":\"Manuel, Rita R.\"},{\"Person.name\":\"Pereira, Inês A.C.\"},{\"Person.name\":\"Reisner, Erwin\"}] |
| datacite.contributors.contributor.contributorName.fl_str_mv | Instituto de Tecnologia Química e Biológica António Xavier (ITQB) ACS - American Chemical Society RUN |
| datacite.creators.creator.creatorName.fl_str_mv | Liu, Yongpeng Bin Mohamad Annuar, Ariffin Rodríguez-Jiménez, Santiago Yeung, Celine Wing See Wang, Qian Coito, Ana M. Manuel, Rita R. Pereira, Inês A.C. Reisner, Erwin |
| datacite.date.Accepted.fl_str_mv | 2024-10-16T00:00:00Z |
| datacite.date.available.fl_str_mv | 2025-05-07T21:24:18Z |
| datacite.date.embargoed.fl_str_mv | 2025-05-07T21:24:18Z |
| datacite.rights.fl_str_mv | http://purl.org/coar/access_right/c_abf2 |
| datacite.subjects.subject.fl_str_mv | Catalysis General Chemistry Biochemistry Colloid and Surface Chemistry |
| datacite.titles.title.fl_str_mv | Solar Fuel Synthesis Using a Semiartificial Colloidal Z-Scheme |
| dc.contributor.none.fl_str_mv | Instituto de Tecnologia Química e Biológica António Xavier (ITQB) ACS - American Chemical Society RUN |
| dc.creator.none.fl_str_mv | Liu, Yongpeng Bin Mohamad Annuar, Ariffin Rodríguez-Jiménez, Santiago Yeung, Celine Wing See Wang, Qian Coito, Ana M. Manuel, Rita R. Pereira, Inês A.C. Reisner, Erwin |
| dc.date.Accepted.fl_str_mv | 2024-10-16T00:00:00Z |
| dc.date.available.fl_str_mv | 2025-05-07T21:24:18Z |
| dc.date.embargoed.fl_str_mv | 2025-05-07T21:24:18Z |
| dc.format.none.fl_str_mv | application/pdf |
| dc.identifier.none.fl_str_mv | http://hdl.handle.net/10362/182778 |
| dc.language.none.fl_str_mv | eng |
| dc.rights.none.fl_str_mv | http://purl.org/coar/access_right/c_abf2 |
| dc.subject.none.fl_str_mv | Catalysis General Chemistry Biochemistry Colloid and Surface Chemistry |
| dc.title.fl_str_mv | Solar Fuel Synthesis Using a Semiartificial Colloidal Z-Scheme |
| dc.type.none.fl_str_mv | http://purl.org/coar/resource_type/c_6501 |
| description | The integration of enzymes with semiconductor light absorbers in semiartificial photosynthetic assemblies offers an emerging strategy for solar fuel production. However, such colloidal biohybrid systems rely currently on sacrificial reagents, and semiconductor-enzyme powder systems that couple fuel production to water oxidation are therefore needed to mimic an overall photosynthetic reaction. Here, we present a Z-scheme colloidal enzyme system that produces fuel with electrons sourced from water. This “closed-cycle” semiartificial approach utilizes particulate SrTiO3:La,Rh and BiVO4:Mo (light absorbers), hydrogenase or formate dehydrogenase (cocatalyst), and a molecular cobalt complex (a redox mediator). Under simulated solar irradiation, this system continuously generates molecular hydrogen or formate, while co-producing molecular oxygen for 10 h using only sunlight, water, and carbon dioxide as inputs. In-depth analysis using quartz crystal microbalance, photoelectrochemical impedance spectroscopy, transient photocurrent spectroscopy, and intensity-modulated photovoltage spectroscopy provides mechanistic understanding and characterization of the semiconductor-enzyme hybrid interface. This study provides a rational platform to assemble functional semiartificial colloidal Z-scheme systems for solar fuel synthesis. |
| dirty | 0 |
| eu_rights_str_mv | openAccess |
| format | article |
| fulltext.url.fl_str_mv | https://run.unl.pt/bitstreams/09e85dfa-bf89-45bf-855e-fb23ec20d130/download |
| id | run_ded1942e4504e4c7bc531f9ca1144cdf |
| identifier.url.fl_str_mv | http://hdl.handle.net/10362/182778 |
| inst_facet_str | urn:organizationAcronym:unl{{{_:::_}}}Universidade Nova de Lisboa |
| instacron_str | unl |
| institution | Universidade Nova de Lisboa |
| instname_str | Universidade Nova de Lisboa |
| language | eng |
| network_acronym_str | run |
| network_name_str | Repositório Institucional da UNL |
| oai_identifier_str | oai:run.unl.pt:10362/182778 |
| organization_str_mv | urn:organizationAcronym:unl |
| person_str_mv | Liu, Yongpeng Bin Mohamad Annuar, Ariffin Rodríguez-Jiménez, Santiago Yeung, Celine Wing See Wang, Qian Coito, Ana M. Manuel, Rita R. Pereira, Inês A.C. Reisner, Erwin |
| publishDate | 2024 |
| repo_facet_str | urn:repositoryAcronym:run{{{_:::_}}}Repositório Institucional da UNL |
| reponame_str | Repositório Institucional da UNL |
| repository_id_str | urn:repositoryAcronym:run |
| service_str_mv | urn:repositoryAcronym:run |
| spelling | engenThe integration of enzymes with semiconductor light absorbers in semiartificial photosynthetic assemblies offers an emerging strategy for solar fuel production. However, such colloidal biohybrid systems rely currently on sacrificial reagents, and semiconductor-enzyme powder systems that couple fuel production to water oxidation are therefore needed to mimic an overall photosynthetic reaction. Here, we present a Z-scheme colloidal enzyme system that produces fuel with electrons sourced from water. This “closed-cycle” semiartificial approach utilizes particulate SrTiO3:La,Rh and BiVO4:Mo (light absorbers), hydrogenase or formate dehydrogenase (cocatalyst), and a molecular cobalt complex (a redox mediator). Under simulated solar irradiation, this system continuously generates molecular hydrogen or formate, while co-producing molecular oxygen for 10 h using only sunlight, water, and carbon dioxide as inputs. In-depth analysis using quartz crystal microbalance, photoelectrochemical impedance spectroscopy, transient photocurrent spectroscopy, and intensity-modulated photovoltage spectroscopy provides mechanistic understanding and characterization of the semiconductor-enzyme hybrid interface. This study provides a rational platform to assemble functional semiartificial colloidal Z-scheme systems for solar fuel synthesis.application/pdfenSolar Fuel Synthesis Using a Semiartificial Colloidal Z-SchemeLiu, YongpengBin Mohamad Annuar, AriffinRodríguez-Jiménez, SantiagoYeung, Celine Wing SeeWang, QianCoito, Ana M.Manuel, Rita R.Pereira, Inês A.C.Reisner, ErwinInstituto de Tecnologia Química e Biológica António Xavier (ITQB)ACS - American Chemical SocietyHostingInstitutionOrganizationalRUNe-mailmailto:run@unl.ptrun@unl.ptISSNIsPartOf0002-7863URNIsPartOfPURE: 111148056URNIsPartOfPURE UUID: feada21d-8402-4f62-9dd1-e5710ec614a0URNIsPartOfScopus: 85207154942URNIsPartOfPubMed: 39413284DOIIsPartOf10.1021/jacs.4c118272025-05-07T21:24:18Z2024-10-162024-10-16T00:00:00ZHandlehttp://hdl.handle.net/10362/182778http://purl.org/coar/access_right/c_abf2open accessCatalysisGeneral ChemistryBiochemistryColloid and Surface Chemistry4402879 bytesliteraturehttp://purl.org/coar/resource_type/c_6501journal articlehttp://purl.org/coar/access_right/c_abf2application/pdffulltexthttps://run.unl.pt/bitstreams/09e85dfa-bf89-45bf-855e-fb23ec20d130/download |
| spellingShingle | Solar Fuel Synthesis Using a Semiartificial Colloidal Z-Scheme Liu, Yongpeng Catalysis General Chemistry Biochemistry Colloid and Surface Chemistry |
| status | SINGLETON |
| subject.fl_str_mv | Catalysis General Chemistry Biochemistry Colloid and Surface Chemistry |
| title | Solar Fuel Synthesis Using a Semiartificial Colloidal Z-Scheme |
| title_full | Solar Fuel Synthesis Using a Semiartificial Colloidal Z-Scheme |
| title_fullStr | Solar Fuel Synthesis Using a Semiartificial Colloidal Z-Scheme |
| title_full_unstemmed | Solar Fuel Synthesis Using a Semiartificial Colloidal Z-Scheme |
| title_short | Solar Fuel Synthesis Using a Semiartificial Colloidal Z-Scheme |
| title_sort | Solar Fuel Synthesis Using a Semiartificial Colloidal Z-Scheme |
| topic | Catalysis General Chemistry Biochemistry Colloid and Surface Chemistry |
| topic_facet | Catalysis General Chemistry Biochemistry Colloid and Surface Chemistry |
| url | http://hdl.handle.net/10362/182778 |
| visible | 1 |