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2. Appendix A. Supplementary material for The promoter effect of Nb species on the catalytic performance of Ir-based catalysts for VOCs total oxidation [Dataset]

Author

Gobierno de Aragón, Agencia Estatal de Investigación (España), Ministerio de Ciencia e Innovación (España), European Commission, Ministerio de Economía y Competitividad (España), Chávez Sifontes, Marvin [0000-0001-8264-291X], García Moreno, Adrián [0000-0002-9530-1230], Furgeaud, Clarisse [0000-0002-6654-396X], Mayoral, Álvaro [0000-0002-5229-2717], Arenal, Raúl [0000-0002-2071-9093], Morgan, David J. [0000-0002-1611-9263], Taylor, Stuart H. [0000-0002-1933-4874], López Sebastián, José Manuel [0000-0002-6203-8835], García Martínez, Tomás [0000-0003-4255-5998], Solsona, Benjamín [0000-0001-7235-2038], García Martínez, Tomás; Solsona, Benjamín, García Moreno, Adrián, Chávez Sifontes, Marvin, Sanchis, Rut, Furgeaud, Clarisse, Mayoral, Álvaro, Arenal, Raúl, Morgan, David J., Taylor, Stuart H., López Sebastián, José Manuel, García Martínez, Tomás, Solsona, Benjamín, Gobierno de Aragón, Agencia Estatal de Investigación (España), Ministerio de Ciencia e Innovación (España), European Commission, Ministerio de Economía y Competitividad (España), Chávez Sifontes, Marvin [0000-0001-8264-291X], García Moreno, Adrián [0000-0002-9530-1230], Furgeaud, Clarisse [0000-0002-6654-396X], Mayoral, Álvaro [0000-0002-5229-2717], Arenal, Raúl [0000-0002-2071-9093], Morgan, David J. [0000-0002-1611-9263], Taylor, Stuart H. [0000-0002-1933-4874], López Sebastián, José Manuel [0000-0002-6203-8835], García Martínez, Tomás [0000-0003-4255-5998], Solsona, Benjamín [0000-0001-7235-2038], García Martínez, Tomás; Solsona, Benjamín, García Moreno, Adrián, Chávez Sifontes, Marvin, Sanchis, Rut, Furgeaud, Clarisse, Mayoral, Álvaro, Arenal, Raúl, Morgan, David J., Taylor, Stuart H., López Sebastián, José Manuel, García Martínez, Tomás, and Solsona, Benjamín

Abstract

Figure S1. XRD patterns of fresh Ir/Nb/Ti catalysts. Figure S2. Figure S3. Cs-corrected STEM-HAADF. Figure S4. O(1s) XPS core-level spectra.

Published
2022

3. Formamidinium halide salts as precursors of carbon nitrides

Author

Ministerio de Ciencia e Innovación (España), European Commission, Gobierno de Aragón, Ministerio de Ciencia, Innovación y Universidades (España), Agencia Estatal de Investigación (España), Diputación General de Aragón, Ciria Ramos, Isabel [0000-0002-9162-9829], Navascués, Nuria [0000-0003-3363-2912], Diaw, Fatou [0000-0002-3640-0802], Furgeaud, Clarisse [0000-0002-6654-396X], Ansón Casaos, Alejandro [0000-0002-3134-8566], Haro Remón, Marta [0000-0001-7246-2149], Juárez Pérez, Emilio J. [0000-0001-6040-1920], Ciria-Ramos, Isabel, Navascués, Nuria, Diaw, Fatou, Furgeaud, Clarisse, Ansón Casaos, Alejandro, Haro Remón, Marta, Juárez-Pérez, Emilio J., Ministerio de Ciencia e Innovación (España), European Commission, Gobierno de Aragón, Ministerio de Ciencia, Innovación y Universidades (España), Agencia Estatal de Investigación (España), Diputación General de Aragón, Ciria Ramos, Isabel [0000-0002-9162-9829], Navascués, Nuria [0000-0003-3363-2912], Diaw, Fatou [0000-0002-3640-0802], Furgeaud, Clarisse [0000-0002-6654-396X], Ansón Casaos, Alejandro [0000-0002-3134-8566], Haro Remón, Marta [0000-0001-7246-2149], Juárez Pérez, Emilio J. [0000-0001-6040-1920], Ciria-Ramos, Isabel, Navascués, Nuria, Diaw, Fatou, Furgeaud, Clarisse, Ansón Casaos, Alejandro, Haro Remón, Marta, and Juárez-Pérez, Emilio J.

Abstract

Pyrolysis of formamidinium halide salts (FAI, FABr) results in a new type of amorphous carbon nitride materials with a mass fraction of 40–50% nitrogen content. Pyrolysis temperature drives final chemical composition, morphology, optical and electrical properties of the material independently of the halide precursor and identifying triazine ring, instead of typical heptazine unit, as the main building block of this material. We elaborated a temperature dependent mechanism of formation for these materials and foresee its potential value as native passivation layer in the field of perovskite solar cells.

Published
2022

4. The promoter effect of Nb species on the catalytic performance of Ir-based catalysts for VOCs total oxidation

Author

Gobierno de Aragón, Ministerio de Ciencia, Innovación y Universidades (España), European Commission, Diputación General de Aragón, Agencia Estatal de Investigación (España), Ministerio de Economía y Competitividad (España), Chávez Sifontes, Marvin [0000-0001-8264-291X], García Moreno, Adrián [0000-0002-9530-1230], Furgeaud, Clarisse [0000-0002-6654-396X], Mayoral, Álvaro [0000-0002-5229-2717], Arenal, Raúl [0000-0002-2071-9093], Morgan, David J. [0000-0002-1611-9263], Taylor, Stuart H. [0000-0002-1933-4874], López Sebastián, José Manuel [0000-0002-6203-8835], García Martínez, Tomás [0000-0003-4255-5998], Solsona, Benjamín [0000-0001-7235-2038], Chávez Sifontes, Marvin, García Moreno, Adrián, Sanchis, Rut, Furgeaud, Clarisse, Mayoral, Álvaro, Arenal, Raúl, Morgan, David J., Taylor, Stuart H., López Sebastián, José Manuel, García Martínez, Tomás, Solsona, Benjamín, Gobierno de Aragón, Ministerio de Ciencia, Innovación y Universidades (España), European Commission, Diputación General de Aragón, Agencia Estatal de Investigación (España), Ministerio de Economía y Competitividad (España), Chávez Sifontes, Marvin [0000-0001-8264-291X], García Moreno, Adrián [0000-0002-9530-1230], Furgeaud, Clarisse [0000-0002-6654-396X], Mayoral, Álvaro [0000-0002-5229-2717], Arenal, Raúl [0000-0002-2071-9093], Morgan, David J. [0000-0002-1611-9263], Taylor, Stuart H. [0000-0002-1933-4874], López Sebastián, José Manuel [0000-0002-6203-8835], García Martínez, Tomás [0000-0003-4255-5998], Solsona, Benjamín [0000-0001-7235-2038], Chávez Sifontes, Marvin, García Moreno, Adrián, Sanchis, Rut, Furgeaud, Clarisse, Mayoral, Álvaro, Arenal, Raúl, Morgan, David J., Taylor, Stuart H., López Sebastián, José Manuel, García Martínez, Tomás, and Solsona, Benjamín

Abstract

Ir/TiO2 catalysts promoted by niobium have been synthesized, characterized by different complementary techniques and tested for the total oxidation of a set of alkanes and their mixtures. The addition of appropriate amounts of niobium to Ir/TiO2 catalysts resulted in a remarkable increase in the catalytic activity compared to the Nb-free Ir/TiO2 catalysts. The promotion caused by the presence of niobium has been related to the massive presence of isolated IrOx surface species which, interestingly, present remarkable reducibility and, consequently, excellent catalytic activity. Conversely, the IrOx species formed in the catalyst in the absence of niobium also include IrO2 clusters with lower intrinsic reactivity. Similarly, Nb-loadings exceeding the theoretical monolayer tends to the formation of bulk Nb2O5 species on the titania surface that provokes the formation of IrO2 nanoclusters. A positive influence on the reactivity of non-stoichiometric surface non- Ti3+ species that generates oxygen vacancies is also observed.

Published
2022

5. Photocatalytic hydrogen generation from a methanol-water mixture in the presence of g-C3N4 and graphene/g-C3N4

Author

Ministère de l'Enseignement Supérieur et de la Recherche Scientifique (Algerie), Universidade de Aveiro, Ministerio de Ciencia, Innovación y Universidades (España), Agencia Estatal de Investigación (España), European Commission, Gobierno de Aragón, Diputación General de Aragón, Touati, Wassila, Karmaoui, Mohamed, Bekka, Ahmed, Edelmannová, Miroslava Filip, Furgeaud, Clarisse, Chakib, Alaoui, Allah, Imene kadi, Figueiredo, Bruno, Labrincha, J. A., Arenal, Raúl, Koci, Kamila, Tobaldi, David Maria, Ministère de l'Enseignement Supérieur et de la Recherche Scientifique (Algerie), Universidade de Aveiro, Ministerio de Ciencia, Innovación y Universidades (España), Agencia Estatal de Investigación (España), European Commission, Gobierno de Aragón, Diputación General de Aragón, Touati, Wassila, Karmaoui, Mohamed, Bekka, Ahmed, Edelmannová, Miroslava Filip, Furgeaud, Clarisse, Chakib, Alaoui, Allah, Imene kadi, Figueiredo, Bruno, Labrincha, J. A., Arenal, Raúl, Koci, Kamila, and Tobaldi, David Maria

Abstract

Graphitic carbon nitride (g-C3N4), possessing high thermal and chemical stability, non-toxicity, facile synthesis, and low band gap energy is a promising candidate for photocatalytic applications. In this study, bulk and exfoliated g-C3N4 were synthesised from different precursors (melamine and urea). Moreover, the surface of bulk g-C3N4 and exfoliated g-C3N4 was modified with graphene (0.5 wt% and 1 wt%) aiming to obtain a prolonged carrier lifetime. The effect of g-C3N4 synthesis from various precursors and the influence of graphene content on the photocatalytic activity during the degradation of a water–methanol mixture under UVC irradiation were examined, in comparison to commercial P25. Hydrogen, methane and carbon monoxide were the decomposition products; hydrogen was the main product of decomposition, whereas CH4 and CO resulting from the reduction of CO2 were generated in a significantly smaller amount. All the produced photocatalysts, whether pure or modified with graphene, exhibited higher activity than the commercial photocatalyst P25.

Published
2022

6. In Situ and Real-Time Nanoscale Monitoring of Ultra-Thin Metal Film Growth Using Optical and Electrical Diagnostic Tools

Author

Colin, Jonathan, Jamnig, Andreas, Furgeaud, Clarisse, Michel, Anny, Pliatsikas, Nikolaos, Sarakinos, Kostas, Abadias, Gregory, Colin, Jonathan, Jamnig, Andreas, Furgeaud, Clarisse, Michel, Anny, Pliatsikas, Nikolaos, Sarakinos, Kostas, and Abadias, Gregory

Abstract

Continued downscaling of functional layers for key enabling devices has prompted the development of characterization tools to probe and dynamically control thin film formation stages and ensure the desired film morphology and functionalities in terms of, e.g., layer surface smoothness or electrical properties. In this work, we review the combined use of in situ and real-time optical (wafer curvature, spectroscopic ellipsometry) and electrical probes for gaining insights into the early growth stages of magnetron-sputter-deposited films. Data are reported for a large variety of metals characterized by different atomic mobilities and interface reactivities. For fcc noble-metal films (Ag, Cu, Pd) exhibiting a pronounced three-dimensional growth on weakly-interacting substrates (SiO2, amorphous carbon (a-C)), wafer curvature, spectroscopic ellipsometry, and resistivity techniques are shown to be complementary in studying the morphological evolution of discontinuous layers, and determining the percolation threshold and the onset of continuous film formation. The influence of growth kinetics (in terms of intrinsic atomic mobility, substrate temperature, deposition rate, deposition flux temporal profile) and the effect of deposited energy (through changes in working pressure or bias voltage) on the various morphological transition thicknesses is critically examined. For bcc transition metals, like Fe and Mo deposited on a-Si, in situ and real-time growth monitoring data exhibit transient features at a critical layer thickness of similar to 2 nm, which is a fingerprint of an interface-mediated crystalline-to-amorphous phase transition, while such behavior is not observed for Ta films that crystallize into their metastable tetragonal beta-Ta allotropic phase. The potential of optical and electrical diagnostic tools is also explored to reveal complex interfacial reactions and their effect on growth of Pd films on a-Si or a-Ge interlayers. For all case studies presented in the, Funding Agencies|French Government program "Investissements dAvenir" (LABEX INTERACTIFS)French National Research Agency (ANR) [ANR-11-LABX-0017-01]; French Government program "Investissements dAvenir" (EUR INTREE)French National Research Agency (ANR) [ANR-18-EURE-0010]; Linkoping University ("LiU Career Contract) [Dnr-LiU-2015-01510]; Swedish research councilSwedish Research Council [VR-2015-04630]; AForsk foundation [AF 19-137, AF 19-746]; Olle Engkvist foundation [SOEB 190-312]; Wenner-Gren foundations [UPD2018-0071, UPD2019-0007]

Published
2020
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9. Formamidinium halide salts as precursors of carbon nitrides

Author

Isabel Ciria-Ramos, Nuria Navascués, Fatou Diaw, Clarisse Furgeaud, Raul Arenal, Alejandro Ansón-Casaos, Marta Haro, Emilio J. Juarez-Perez, Ministerio de Ciencia e Innovación (España), European Commission, Gobierno de Aragón, Ministerio de Ciencia, Innovación y Universidades (España), Agencia Estatal de Investigación (España), Diputación General de Aragón, Ciria Ramos, Isabel, Navascués, Nuria, Diaw, Fatou, Furgeaud, Clarisse, Ansón Casaos, Alejandro, Haro Remón, Marta, Juárez Pérez, Emilio J., Ciria Ramos, Isabel [0000-0002-9162-9829], Navascués, Nuria [0000-0003-3363-2912], Diaw, Fatou [0000-0002-3640-0802], Furgeaud, Clarisse [0000-0002-6654-396X], Ansón Casaos, Alejandro [0000-0002-3134-8566], Haro Remón, Marta [0000-0001-7246-2149], and Juárez Pérez, Emilio J. [0000-0001-6040-1920]

Subjects
Formamidinium cation, Perovskite solar cells, General Materials Science, General Chemistry, Carbon nitrides, Pyrolysis
Abstract

13 figures, 6 tables.-- Supplementary information available., Pyrolysis of formamidinium halide salts (FAI, FABr) results in a new type of amorphous carbon nitride materials with a mass fraction of 40–50% nitrogen content. Pyrolysis temperature drives final chemical composition, morphology, optical and electrical properties of the material independently of the halide precursor and identifying triazine ring, instead of typical heptazine unit, as the main building block of this material. We elaborated a temperature dependent mechanism of formation for these materials and foresee its potential value as native passivation layer in the field of perovskite solar cells., E.J.J-P acknowledges the funding support from MCIN/AEI/10.13039/501100011033 and European Union NextGenerationEU/PRTR (project grants PID2019-107893RB-I00 and EIN2020-112315, respectively). M.H. acknowledges the funding support from MCIN/AEI/10.13039/501100011033 for the Ramón y Cajal fellowship (RYC-2018-025222-I) and the project PID2019-108247RA-I00. R.A. acknowledges funding from the Spanish MICINN (project grant PID2019-104739 GB-100/AEI/10.13039/501100011033). RA also acknowledge to Government of Aragon (project DGA E13-20R (FEDER, EU)) and European Union H2020 program “ESTEEM3” (823717). A.A-C acknowledges financial support from Spanish MCIN/AEI/10.13039/501100011033 under project PID2019-104272RB-C51/AEI/10.13039/501100011033 and the Diputación General de Aragón under project T03_20R (Grupo Reconocido).

Published
2022

10. The promoter effect of Nb species on the catalytic performance of Ir-based catalysts for VOCs total oxidation

Author

Marvin Chávez-Sifontes, Adrián García, Rut Sanchis, Clarisse Furgeaud, Alvaro Mayoral, Raul Arenal, David J. Morgan, Stuart H. Taylor, Jose Manuel López, Tomás García, Benjamín Solsona, Gobierno de Aragón, Ministerio de Ciencia, Innovación y Universidades (España), European Commission, Diputación General de Aragón, Agencia Estatal de Investigación (España), Ministerio de Economía y Competitividad (España), Chávez Sifontes, Marvin [0000-0001-8264-291X], García Moreno, Adrián [0000-0002-9530-1230], Furgeaud, Clarisse [0000-0002-6654-396X], Mayoral, Álvaro [0000-0002-5229-2717], Arenal, Raúl [0000-0002-2071-9093], Morgan, David J. [0000-0002-1611-9263], Taylor, Stuart H. [0000-0002-1933-4874], López Sebastián, José Manuel [0000-0002-6203-8835], García Martínez, Tomás [0000-0003-4255-5998], Solsona, Benjamín [0000-0001-7235-2038], Chávez Sifontes, Marvin, García Moreno, Adrián, Furgeaud, Clarisse, Mayoral, Álvaro, Arenal, Raúl, Morgan, David J., Taylor, Stuart H., López Sebastián, José Manuel, García Martínez, Tomás, and Solsona, Benjamín

Subjects
Titania, Niobium, Process Chemistry and Technology, Total oxidation, Alkane, VOCs, Chemical Engineering (miscellaneous), Iridium, Pollution, Waste Management and Disposal
Abstract

12 figures, 2 tables.-- Supporting information available., Ir/TiO2 catalysts promoted by niobium have been synthesized, characterized by different complementary techniques and tested for the total oxidation of a set of alkanes and their mixtures. The addition of appropriate amounts of niobium to Ir/TiO2 catalysts resulted in a remarkable increase in the catalytic activity compared to the Nb-free Ir/TiO2 catalysts. The promotion caused by the presence of niobium has been related to the massive presence of isolated IrOx surface species which, interestingly, present remarkable reducibility and, consequently, excellent catalytic activity. Conversely, the IrOx species formed in the catalyst in the absence of niobium also include IrO2 clusters with lower intrinsic reactivity. Similarly, Nb-loadings exceeding the theoretical monolayer tends to the formation of bulk Nb2O5 species on the titania surface that provokes the formation of IrO2 nanoclusters. A positive influence on the reactivity of non-stoichiometric surface non- Ti3+ species that generates oxygen vacancies is also observed., This work was supported by the Regional Government of Aragon (DGA) under the research groups support programme. We also thank the MAT2017-84118-C2-1-R MCIN/AEI/10.13039/501100011033/ project and FEDER “Una manera de hacer Europa”. This research was also funded by MINECO-Spain, grant number PRE2018-085211.

Published
2022

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