All Outputs (44)

Monitoring dynamics of defects and single Fe atoms in N-functionalized few-layer graphene by in situ temperature programmed scanning transmission electron microscopy (2021)
Journal Article
Arrigo, R., Sasaki, T., Callison, J., Gianolio, D., & Schuster, M. (2022). Monitoring dynamics of defects and single Fe atoms in N-functionalized few-layer graphene by in situ temperature programmed scanning transmission electron microscopy. Journal of Energy Chemistry, 64, 520-530. https://doi.org/10.1016/j.jechem.2021.05.005

In this study, we aim to contribute an understanding of the pathway of formation of Fe species during top-down synthesis of dispersed Fe on N-functionalized few layer graphene. We use X-ray absorption spectroscopy to determine the electronic structur... Read More about Monitoring dynamics of defects and single Fe atoms in N-functionalized few-layer graphene by in situ temperature programmed scanning transmission electron microscopy.

Structural insight into [Fe–S2–Mo] motif in electrochemical reduction of N2 over Fe1-supported molecular MoS2 (2020)
Journal Article
Zheng, J., Wu, S., Lu, L., Huang, C., Ho, P., Kirkland, A., …Edman Tsang, S. (2021). Structural insight into [Fe–S2–Mo] motif in electrochemical reduction of N2 over Fe1-supported molecular MoS2. Chemical Science, 12(2), 688-695. https://doi.org/10.1039/d0sc04575f

The catalytic synthesis of NH3 from the thermodynamically challenging N2 reduction reaction under mild conditions is currently a significant problem for scientists. Accordingly, herein, we report the development of a nitrogenase-inspired inorganic-ba... Read More about Structural insight into [Fe–S2–Mo] motif in electrochemical reduction of N2 over Fe1-supported molecular MoS2.

Investigations of carbon nitride-supported Mn3 O4 oxide nanoparticles for ORR (2020)
Journal Article
Large, A., Wahl, S., Abate, S., da Silva, I., Delgado Jaen, J., Pinna, N., …Arrigo, R. (2020). Investigations of carbon nitride-supported Mn3 O4 oxide nanoparticles for ORR. Catalysts, 10(11), e1289. https://doi.org/10.3390/catal10111289

Earth-abundant Mn-based oxide nanoparticles are supported on carbon nitride using two different immobilization methods and tested for the oxygen reduction reaction. Compared to the metal free CN, the immobilization of Mn oxide enhances not only the e... Read More about Investigations of carbon nitride-supported Mn3 O4 oxide nanoparticles for ORR.

On the activity/selectivity and phase stability of thermally grown copper oxides during the electrocatalytic reduction of CO2 (2020)
Journal Article
Velasco-Vélez, J., Chuang, C., Gao, D., Zhu, Q., Ivanov, D., Jeon, H., …Schlögl, R. (2020). On the activity/selectivity and phase stability of thermally grown copper oxides during the electrocatalytic reduction of CO2. ACS catalysis, 10(19), 11510-11518. https://doi.org/10.1021/acscatal.0c03484

Revealing the active nature of oxide-derived copper is of key importance to understand its remarkable catalytic performance during the cathodic CO2 reduction reaction (CO2RR) to produce valuable hydrocarbons. Using advanced spectroscopy, electron mic... Read More about On the activity/selectivity and phase stability of thermally grown copper oxides during the electrocatalytic reduction of CO2.

Ambient-pressure endstation of the Versatile Soft X-ray (VerSoX) beamline at Diamond Light Source (2020)
Journal Article
Held, G., Venturini, F., Grinter, D., Ferrer, P., Arrigo, R., Deacon, L., …Scott, S. (2020). Ambient-pressure endstation of the Versatile Soft X-ray (VerSoX) beamline at Diamond Light Source. Journal of Synchrotron Radiation, 27(5), 1153-1166. https://doi.org/10.1107/S1600577520009157

The ambient-pressure endstation and branchline of the Versatile Soft X-ray (VerSoX) beamline B07 at Diamond Light Source serves a very diverse user community studying heterogeneous catalysts, pharmaceuticals and biomaterials under realistic condition... Read More about Ambient-pressure endstation of the Versatile Soft X-ray (VerSoX) beamline at Diamond Light Source.

The electronic structure, surface properties, and in situ N2O decomposition of mechanochemically synthesised LaMnO3 (2020)
Journal Article
Blackmore, R., Rivas, M., Tierney, G., Mohammed, K., Decarolis, D., Hayama, S., …Wells, P. (2020). The electronic structure, surface properties, and in situ N2O decomposition of mechanochemically synthesised LaMnO3. Physical Chemistry Chemical Physics, 22(34), 18774-18787. https://doi.org/10.1039/d0cp00793e

The use of mechanochemistry to prepare catalytic materials is of significant interest; it offers an environmentally beneficial, solvent-free, route and produces highly complex structures of mixed amorphous and crystalline phases. This study reports o... Read More about The electronic structure, surface properties, and in situ N2O decomposition of mechanochemically synthesised LaMnO3.

Revealing the active phase of copper during the electroreduction of CO2 in aqueous electrolyte by correlating in situ x-ray spectroscopy and in situ electron microscopy (2020)
Journal Article
Velasco-Velez, J., Mom, R., Sandoval-Diaz, L., Falling, L., Chuang, C., Gao, D., …Schlögl, R. (2020). Revealing the active phase of copper during the electroreduction of CO2 in aqueous electrolyte by correlating in situ x-ray spectroscopy and in situ electron microscopy. ACS Energy Letters, 5(6), 2106-2111. https://doi.org/10.1021/acsenergylett.0c00802

The variation in the morphology and electronic structure of copper during the electroreduction of CO2 into valuable hydrocarbons and alcohols was revealed by combining in situ surface- and bulk-sensitive X-ray spectroscopies with electrochemical scan... Read More about Revealing the active phase of copper during the electroreduction of CO2 in aqueous electrolyte by correlating in situ x-ray spectroscopy and in situ electron microscopy.

Elucidating the mechanism of the CO2 methanation reaction over Ni–Fe hydrotalcite-derived catalysts via surface-sensitive in situ XPS and NEXAFS (2020)
Journal Article
Giorgianni, G., Mebrahtu, C., Schuster, M., Large, A., Held, G., Ferrer, P., …Arrigo, R. (2020). Elucidating the mechanism of the CO2 methanation reaction over Ni–Fe hydrotalcite-derived catalysts via surface-sensitive in situ XPS and NEXAFS. Physical Chemistry Chemical Physics, 22(34), 18788-18797. https://doi.org/10.1039/d0cp00622j

Hydrotalcite-derived Ni and Fe-promoted hydrotalcite-derived Ni catalysts were found to outperform industrial catalysts in the CO2 methanation reaction, however the origin of the improved activity and selectivity of these catalysts is not clear. Here... Read More about Elucidating the mechanism of the CO2 methanation reaction over Ni–Fe hydrotalcite-derived catalysts via surface-sensitive in situ XPS and NEXAFS.

Influence of synthesis conditions on the structure of nickel nanoparticles and their reactivity in selective asymmetric hydrogenation (2019)
Journal Article
Arrigo, R., Gallarati, S., Schuster, M., Seymour, J., Gianolio, D., da Silva, I., …Held, G. (2020). Influence of synthesis conditions on the structure of nickel nanoparticles and their reactivity in selective asymmetric hydrogenation. ChemCatChem, 12(5), 1491-1503. https://doi.org/10.1002/cctc.201901955

Unsupported and SiO2-supported Ni nanoparticles (NPs), were synthesised via hot-injection colloidal route using oleylamine (OAm) and trioctylphosphine (TOP) as reducing and protective agents, respectively. By adopting a multi-length scale structural... Read More about Influence of synthesis conditions on the structure of nickel nanoparticles and their reactivity in selective asymmetric hydrogenation.

On the high structural heterogeneity of Fe impregnated graphite-carbon catalysts from Fe nitrate precursor (2019)
Journal Article
Arrigo, R., & Schuster, M. (2019). On the high structural heterogeneity of Fe impregnated graphite-carbon catalysts from Fe nitrate precursor. Catalysts, 9(4), 303. https://doi.org/10.3390/catal9040303

Wet impregnation is broadly applied for the synthesis of carbon supported metal/metal oxide nanostructures because of its high flexibility, simplicity and low cost. By contrast, impregnated catalysts are typified by a usually undesired nanostructural... Read More about On the high structural heterogeneity of Fe impregnated graphite-carbon catalysts from Fe nitrate precursor.

The role of the copper oxidation state in the electrocatalytic reduction of CO2 into valuable hydrocarbons (2018)
Journal Article
Velasco-Vélez, J., Jones, T., Gao, D., Carbonio, E., Arrigo, R., Hsu, C., …Chuang, C. (2018). The role of the copper oxidation state in the electrocatalytic reduction of CO2 into valuable hydrocarbons. ACS sustainable chemistry & engineering, 7(1), 1485-1492. https://doi.org/10.1021/acssuschemeng.8b05106

Redox-active copper catalysts with accurately prepared oxidation states (Cu0, Cu+ and Cu2+) and high selectivity to C2 hydrocarbon formation, from electrocatalytic cathodic reduction of CO2, were fabricated and characterized. The electrochemically pr... Read More about The role of the copper oxidation state in the electrocatalytic reduction of CO2 into valuable hydrocarbons.

Electrochemically active Ir NPs on graphene for OER in acidic aqueous electrolyte investigated by in situ and ex situ spectroscopies (2018)
Journal Article
Velasco-Vélez, J., Jones, T., Streibel, V., Hävecker, M., Chuang, C., Frevel, L., …Knop-Gericke, A. (2018). Electrochemically active Ir NPs on graphene for OER in acidic aqueous electrolyte investigated by in situ and ex situ spectroscopies. Surface Science, 681(Mar 19), 1-8. https://doi.org/10.1016/j.susc.2018.10.021

An electrode for the oxygen evolution reaction based on a conductive bi-layered free standing graphene support functionalized with iridium nanoparticles was fabricated and characterized by means of potentiometric and advanced X-ray spectroscopic tech... Read More about Electrochemically active Ir NPs on graphene for OER in acidic aqueous electrolyte investigated by in situ and ex situ spectroscopies.

In situ electrochemical cells to study the oxygen evolution reaction by near ambient pressure x-ray photoelectron spectroscopy (2018)
Journal Article
Streibel, V., Hävecker, M., Yi, Y., Velasco Vélez, J., Skorupska, K., Stotz, E., …Arrigo, R. (2018). In situ electrochemical cells to study the oxygen evolution reaction by near ambient pressure x-ray photoelectron spectroscopy. Topics in Catalysis, 61(20), 2064-2084. https://doi.org/10.1007/s11244-018-1061-8

In this contribution, we report the development of in situ electrochemical cells based on proton exchange membranes suitable for studying interfacial structural dynamics of energy materials under operation by near ambient pressure X-ray photoelectron... Read More about In situ electrochemical cells to study the oxygen evolution reaction by near ambient pressure x-ray photoelectron spectroscopy.

Operando spectroscopy study of the carbon dioxide electro-reduction by iron species on nitrogen-doped carbon (2018)
Journal Article
Genovese, C., Schuster, M., Gibson, E., Gianolio, D., Posligua, V., Grau-Crespo, R., …Arrigo, R. (2018). Operando spectroscopy study of the carbon dioxide electro-reduction by iron species on nitrogen-doped carbon. Nature communications, 9, 935. https://doi.org/10.1038/s41467-018-03138-7

The carbon–carbon coupling via electrochemical reduction of carbon dioxide represents the biggest challenge for using this route as platform for chemicals synthesis. Here we show that nanostructured iron (III) oxyhydroxide on nitrogen-doped carbon en... Read More about Operando spectroscopy study of the carbon dioxide electro-reduction by iron species on nitrogen-doped carbon.

In situ observation of reactive oxygen species forming on oxygen-evolving iridium surfaces (2016)
Journal Article
Pfeifer, V., Jones, T., Velasco Vélez, J., Arrigo, R., Piccinin, S., Hävecker, M., …Schlögl, R. (2017). In situ observation of reactive oxygen species forming on oxygen-evolving iridium surfaces. Chemical Science, 8(3), 2143-2149. https://doi.org/10.1039/c6sc04622c

Water splitting performed in acidic media relies on the exceptional performance of iridium-based materials to catalyze the oxygen evolution reaction (OER). In the present work, we use in situ X-ray photoemission and absorption spectroscopy to resolve... Read More about In situ observation of reactive oxygen species forming on oxygen-evolving iridium surfaces.

Acid-base properties of N-doped carbon nanotubes : a combined temperature-programmed desorption, X-ray photoelectron spectroscopy, and 2-propanol reaction investigation (2016)
Journal Article
Ortega, K., Arrigo, R., Frank, B., Schlögl, R., & Trunschke, A. (2016). Acid-base properties of N-doped carbon nanotubes : a combined temperature-programmed desorption, X-ray photoelectron spectroscopy, and 2-propanol reaction investigation. Chemistry of Materials, 28(19), 6826-6839. https://doi.org/10.1021/acs.chemmater.6b01594

Chemical and electronic properties of N-doped multiwalled carbon nanotubes (NCNTs) synthesized by NH3 treatment of preoxidized CNTs at 300, 500, and 700°C have been investigated by a set of surface sensitive techniques. Temperature-programmed desorpt... Read More about Acid-base properties of N-doped carbon nanotubes : a combined temperature-programmed desorption, X-ray photoelectron spectroscopy, and 2-propanol reaction investigation.

Pd supported on carbon nitride boosts the direct hydrogen peroxide synthesis (2016)
Journal Article
Arrigo, R., Schuster, M., Abate, S., Giorgianni, G., Centi, G., Perathoner, S., …Schlögl, R. (2016). Pd supported on carbon nitride boosts the direct hydrogen peroxide synthesis. ACS catalysis, 6(10), 6959-6966. https://doi.org/10.1021/acscatal.6b01889

Herein, the development of an improved Pd on
carbon nitride catalyst for direct H2O2 synthesis from the
elements is reported. Microcalorimetric CO chemisorption is used to characterize the chemical speciation of the Pd-selective and -unselective si... Read More about Pd supported on carbon nitride boosts the direct hydrogen peroxide synthesis.

Reactive oxygen species in iridium-based OER catalysts (2016)
Journal Article
Arrigo, R. (2016). Reactive oxygen species in iridium-based OER catalysts. Chemical Science, 2016(7), 6791-6795. https://doi.org/10.1039/c6sc01860b

Tremendous effort has been devoted towards elucidating the fundamental reasons for the higher activity of
hydrated amorphous IrIII/IV oxyhydroxides (IrOx) in the oxygen evolution reaction (OER) in comparison with
their crystalline counterpart, ruti... Read More about Reactive oxygen species in iridium-based OER catalysts.

Characterization of platinum and iridium oxyhydrate surface layers from platinum and iridium foils (2016)
Journal Article
Johnson, B., Ranjan, C., Greiner, M., Arrigo, R., Schuster, M., Höpfner, B., …Schlögl, R. (2016). Characterization of platinum and iridium oxyhydrate surface layers from platinum and iridium foils. ChemSusChem, 9(13), 1634-1646. https://doi.org/10.1002/cssc.201600143

Platinum and iridium polycrystalline foils were oxidized electrochemically through anodization to create thin platinum and iridium hydrous oxide layers, which were analyzed through laboratory photoelectron spectroscopy during heating and time series... Read More about Characterization of platinum and iridium oxyhydrate surface layers from platinum and iridium foils.

The electronic structure of iridium oxide electrodes active in water splitting (2015)
Journal Article
Pfeifer, V., Jones, T., Velasco Vélez, J., Massué, C., Greiner, M., Arrigo, R., …Schlögl, R. (2015). The electronic structure of iridium oxide electrodes active in water splitting. Physical Chemistry Chemical Physics, 2016(18), 2292-2296. https://doi.org/10.1039/c5cp06997a

Iridium oxide based electrodes are among the most promising candidates for electrocatalyzing the oxygen evolution reaction, making it imperative to understand their chemical/electronic structure. However, the complexity of iridium oxide's electronic... Read More about The electronic structure of iridium oxide electrodes active in water splitting.