Deposited PtGe clusters as active and durable catalysts for CO oxidation
Ugartemendia, A., Mercero, J. M., de Cózar, A., Melander, M. M., Akola, J., & Jimenez-Izal, E. (2024). Deposited PtGe clusters as active and durable catalysts for CO oxidation. ChemCatChem, 16(3), Article e202301137. https://doi.org/10.1002/cctc.202301137
Julkaistu sarjassa
ChemCatChemTekijät
Päivämäärä
2024Oppiaine
Nanoscience CenterKemiaResurssiviisausyhteisöFysikaalinen kemiaNanoscience CenterChemistrySchool of Resource WisdomPhysical ChemistryTekijänoikeudet
© 2023 Wiley-VCH GmbH
Control of CO emissions raises serious environmental concerns in the current chemical industry, as well as in nascent technologies based on hydrogen such as electrolyzers and fuel cells. Pt remains one of the state-of-art catalysts for the CO oxidation reaction, but suffers from CO self–poisoning. Recently, PtGe alloys were proposed as an excellent alternative to reduce CO poisoning. In this work we investigate the impact of Ge content on the CO oxidation kinetics of P4Gen subnanoclusters supported on MgO. Pt−Ge nanoalloys act as a bifunctional catalyst by displaying dual adsorption sites; i.e., CO is adsorbed on Pt whereas oxygen binds to Ge, forming an alternative oxygen source GeOx. Besides, Ge alloying modifies the electronic structure of Pt (ligand effects) and reduces the affinity to CO. In this way, the competition between CO and O2 adsorption and the overbinding of CO is alleviated, achieving a CO poisoning−free kinetic regime. Our calculations suggest that Pt4Ge3 is the optimal catalyst, evidencing that alloying composition is a parameter of extreme importance in nanocatalyst design. The work relies on global optimization search techniques to determine the accessibility of multiple structures at different conditions, mechanistic studies and microkinetic modelling.
...
Julkaisija
Wiley-VCH VerlagISSN Hae Julkaisufoorumista
1867-3880Asiasanat
Julkaisu tutkimustietojärjestelmässä
https://converis.jyu.fi/converis/portal/detail/Publication/194237377
Metadata
Näytä kaikki kuvailutiedotKokoelmat
Rahoittaja(t)
Suomen AkatemiaRahoitusohjelmat(t)
Akatemiatutkija, SALisätietoja rahoituksesta
A.U. gratefully thanks Eusko Jaurlaritza for his predoctoral grant and for his mobility grant EGONLABUR for short term stays. This work was supported by Grant No. PID2020-114754GA-I00 was funded by MCIN/AEI/10.13039/501100011033, and funding was provided by Gobierno Vasco-Eusko Jaurlaritza (GrantNo.IT1254-19,IT1553-22). M.M.M. was supported by the Research Council of Finland (grant number 338228). DIPCandSGI-IZO-SGIker(UPV/EHU) are acknowledged for their technical support and the generous allocation of computational resources. The authors thankfully acknowledge also the computer resources at Mare Nostrum and the technical support provided by the Barcelona Supercomputing Center (Grant No.QHS-2022-2-002 and QHS-2022-3-0015). ...Lisenssi
Samankaltainen aineisto
Näytetään aineistoja, joilla on samankaltainen nimeke tai asiasanat.
-
The role of polaronic states in the enhancement of CO oxidation by single-atom Pt/CeO2
Kauppinen, Minttu M.; Daelman, Nathan; López, Núria; Honkala, Karoliina (Elsevier BV, 2023)Single Atom Catalysts (SACs) have shown that the miniaturization of the active site implies new phenomena like dynamic charge transfer between isolated metal atoms and the oxide. To obtain direct proof of this character ... -
Towards atomically precise supported catalysts from monolayer‐protected clusters : the critical role of the support
Häkkinen, Hannu; Longo, Alessandro; de Boed, Ewoud; Mammen, Nisha; van der Linden, Marte; Honkala, Karoliina; de Jongh, Petra; Donoeva, Baira (Wiley-VCH Verlag, 2020)Controlling the size and uniformity of metal clusters with atomic precision is essential for fine‐tuning their catalytic properties, however for clusters deposited on supports such control is challenging. Here, by combining ... -
A Self-Consistent Charge Density-Functional Tight-Binding Parameterization for Pt-Ru Alloys
Shi, Hongbo; Koskinen, Pekka; Ramasubramaniam, Ashwin (American Chemical Society, 2017)We present a self-consistent charge density-functional tight-binding (SCC-DFTB) parametrization for PtRu alloys, which is developed by employing a training set of alloy cluster energies and forces obtained from Kohn–Sham ... -
Oxidovanadium(V) complexes with tridentate hydrazone ligands as oxygen atom transfer catalysts
Hossain, Md Kamal; Haukka, Matti; Lisensky, George C.; Richmond, Michael G.; Nordlander, Ebbe (Elsevier, 2024)Four isostructural oxovanadium(V) complexes with hydrazone ligands have been synthesised, characterised, and evaluated as epoxidation and sulfoxidation catalysts. The reactions between [VO(acac)2] (acac– = acetylacetonate) ... -
Effect of atomic layer deposited zinc promoter on the activity of copper-on-zirconia catalysts in the hydrogenation of carbon dioxide to methanol
Arandia, Aitor; Yim, Jihong; Warraich, Hassaan; Leppäkangas, Emilia; Bes, René; Lempelto, Aku; Gell, Lars; Jiang, Hua; Meinander, Kristoffer; Viinikainen, Tiia; Huotari, Simo; Honkala, Karoliina; Puurunen, Riikka L. (Elsevier, 2023)The development of active catalysts for carbon dioxide (CO2) hydrogenation to methanol is intimately related to the creation of effective metal-oxide interfaces. In this work, we investigated how the order of addition of ...
Ellei toisin mainittu, julkisesti saatavilla olevia JYX-metatietoja (poislukien tiivistelmät) saa vapaasti uudelleenkäyttää CC0-lisenssillä.