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dc.contributor.authorBau, Jeremy A.
dc.contributor.authorTakanabe, Kazuhiro
dc.date.accessioned2017-10-30T07:55:31Z
dc.date.available2017-10-30T07:55:31Z
dc.date.issued2017-10-17
dc.identifier.citationBau JA, Takanabe K (2017) Ultrathin Microporous SiO2 Membranes Photodeposited on Hydrogen Evolving Catalysts Enabling Overall Water Splitting. ACS Catalysis: 7931–7940. Available: http://dx.doi.org/10.1021/acscatal.7b03017.
dc.identifier.issn2155-5435
dc.identifier.issn2155-5435
dc.identifier.doi10.1021/acscatal.7b03017
dc.identifier.urihttp://hdl.handle.net/10754/625978
dc.description.abstractSemiconductor systems for photocatalytic overall water splitting into H2 and O2 gases typically require metal cocatalyst particles, such as Pt, to efficiently catalyze H2 evolution. However, such metal catalyst surfaces also serve as recombination sites for H2 and O2, forming H2O. We herein report the photon-induced fabrication of microporous SiO2 membranes that can selectively restrict passage of O2 and larger hydrated ions while allowing penetration of protons, water, and H2. The SiO2 layers were selectively photodeposited on Pt nanoparticles on SrTiO3 photocatalyst by using tetramethylammonium (TMA) as a structure-directing agent (SDA), resulting in the formation of core–shell Pt@SiO2 cocatalysts. The resulting photocatalyst exhibited both improved overall water splitting performance under irradiation and with no H2/O2 recombination in the dark. The function of the SiO2 layers was investigated electrochemically by fabricating the SiO2 layers on a Pt electrode via an analogous cathodic deposition protocol. The uniform, dense, yet amorphous layers possess microporosity originating from ring structures formed during the hydrolysis of the silicate precursor in the presence of TMA, suggesting a double-role for TMA in coordinating silicate to cathodic surfaces and in creating a microporous material. The resulting layers were able to function as a molecular sieve, allowing for exclusive H2 generation while excluding unwanted side reactions by O2 or ferricyanide. The SiO2 layer is stable for extended periods of time in photocatalytic conditions, demonstrating promise as a nontoxic material for selective H2 evolution.
dc.description.sponsorshipThis research in this work was supported by the King Abdullah University of Science and Technology (KAUST). We thank Drs. Nini Wei, Dalaver H. Anjum, and Sergey Lopatin for their assistance with electron microscopy. We thank Dr. Nimer Wehbe for performing SIMS measurements. We thank Muhammad Qureshi for his assistance with photocatalysis.
dc.publisherAmerican Chemical Society (ACS)
dc.relation.urlhttp://pubs.acs.org/doi/10.1021/acscatal.7b03017
dc.rightsThis is an open access article published under a Creative Commons Non-Commercial No Derivative Works (CC-BY-NC-ND) Attribution License, which permits copying and redistribution of the article, and creation of adaptations, all for non-commercial purposes.
dc.rights.urihttp://pubs.acs.org/page/policy/authorchoice_ccbyncnd_termsofuse.html
dc.subjectelectrocatalysis
dc.subjecthydrogen
dc.subjectmembrane
dc.subjectoverall water splitting
dc.subjectphotocatalysis
dc.subjectSiO2
dc.subjectstructure directing agent
dc.titleUltrathin Microporous SiO2 Membranes Photodeposited on Hydrogen Evolving Catalysts Enabling Overall Water Splitting
dc.typeArticle
dc.contributor.departmentKAUST Catalysis Center (KCC)
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Division
dc.identifier.journalACS Catalysis
dc.eprint.versionPublisher's Version/PDF
kaust.personBau, Jeremy A.
kaust.personTakanabe, Kazuhiro
refterms.dateFOA2018-06-14T03:37:19Z


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