Simon Falkner, Carina B Maliakkal, Mareike Liebertseder, Joachim Czechowsky, Maria Casapu, Jan-Dierk Grunwaldt, Christian Kübel, Claus Feldmann
{"title":"High-porosity Pt-CeO<sub>2</sub> nanosponges as oxidation catalyst.","authors":"Simon Falkner, Carina B Maliakkal, Mareike Liebertseder, Joachim Czechowsky, Maria Casapu, Jan-Dierk Grunwaldt, Christian Kübel, Claus Feldmann","doi":"10.1039/d4na00525b","DOIUrl":null,"url":null,"abstract":"<p><p>Pt-CeO<sub>2</sub> nanosponges (1 wt% Pt) with high surface area (113 m<sup>2</sup> g<sup>-1</sup>), high pore volume (0.08 cm<sup>3</sup> g<sup>-1</sup>) and small-sized Pt nanoparticles (1.8 ± 0.4 nm) are prepared by thermal decomposition of a cerium oxalate precursor and examined for catalytic oxidation of CO, volatile organic compounds (VOCs), and NH<sub>3</sub>. The cerium oxalate precursor Ce<sub>2</sub>(C<sub>2</sub>O<sub>4</sub>)<sub>3</sub>·10H<sub>2</sub>O is prepared by aqueous precipitation from Ce(NO<sub>3</sub>)<sub>3</sub>·6H<sub>2</sub>O and K<sub>2</sub>C<sub>2</sub>O<sub>4</sub>·H<sub>2</sub>O and thermally converted to CeO<sub>2</sub> nanosponges by heating in air. Optimal conditions for decomposition in terms of surface area and porosity are observed at 350 °C for 20 min. Finally, the CeO<sub>2</sub> nanosponges are decorated with small-sized Pt nanoparticles, using a wet-chemical impregnation with Pt(ac)<sub>2</sub> in methanol. Electron microscopy with tomography, electron spectroscopy and further methods (TG, XRD, FT-IR, sorption analysis) are used to characterize the catalyst composition and especially the structure and porosity of the Pt-CeO<sub>2</sub> nanosponges as well as the uniform distribution of the Pt nanoparticles. The Pt-CeO<sub>2</sub> nanosponges show good thermal stability (up to 400 °C) and, already as a new, non-optimized catalyst, promising activity for catalytic oxidation of CO, VOCs, NH<sub>3</sub> as indicated by high activities in terms of low and stable light-out and light-off temperatures as well as a high selectivity to N<sub>2</sub> (for NH<sub>3</sub> oxidation) with >80% at 170-250 °C.</p>","PeriodicalId":18806,"journal":{"name":"Nanoscale Advances","volume":" ","pages":""},"PeriodicalIF":4.6000,"publicationDate":"2024-12-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11705977/pdf/","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nanoscale Advances","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1039/d4na00525b","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
Pt-CeO2 nanosponges (1 wt% Pt) with high surface area (113 m2 g-1), high pore volume (0.08 cm3 g-1) and small-sized Pt nanoparticles (1.8 ± 0.4 nm) are prepared by thermal decomposition of a cerium oxalate precursor and examined for catalytic oxidation of CO, volatile organic compounds (VOCs), and NH3. The cerium oxalate precursor Ce2(C2O4)3·10H2O is prepared by aqueous precipitation from Ce(NO3)3·6H2O and K2C2O4·H2O and thermally converted to CeO2 nanosponges by heating in air. Optimal conditions for decomposition in terms of surface area and porosity are observed at 350 °C for 20 min. Finally, the CeO2 nanosponges are decorated with small-sized Pt nanoparticles, using a wet-chemical impregnation with Pt(ac)2 in methanol. Electron microscopy with tomography, electron spectroscopy and further methods (TG, XRD, FT-IR, sorption analysis) are used to characterize the catalyst composition and especially the structure and porosity of the Pt-CeO2 nanosponges as well as the uniform distribution of the Pt nanoparticles. The Pt-CeO2 nanosponges show good thermal stability (up to 400 °C) and, already as a new, non-optimized catalyst, promising activity for catalytic oxidation of CO, VOCs, NH3 as indicated by high activities in terms of low and stable light-out and light-off temperatures as well as a high selectivity to N2 (for NH3 oxidation) with >80% at 170-250 °C.