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Alkali Containing Layered Metal Oxides as Catalysts for the Oxygen Evolution Reaction (2024)
Journal Article
Falsaperna, M., Arrigo, R., Marken, F., & Freakley, S. J. (in press). Alkali Containing Layered Metal Oxides as Catalysts for the Oxygen Evolution Reaction. ChemElectroChem, e202300761. https://doi.org/10.1002/celc.202300761

Improving the efficiency of the oxygen evolution reaction (OER) is essential to realise energy systems based on water electrolysis. Many catalysts have been developed for the OER to date, with iridium‐based oxides being the most promising due to thei... Read More about Alkali Containing Layered Metal Oxides as Catalysts for the Oxygen Evolution Reaction.

Advanced (photo)electrocatalytic approaches to substitute the use of fossil fuels in chemical production (2023)
Journal Article
Centi, G., Perathoner, S., Genovese, C., & Arrigo, R. (in press). Advanced (photo)electrocatalytic approaches to substitute the use of fossil fuels in chemical production. Chemical Communications, 59(21), 3005-3023. https://doi.org/10.1039/d2cc05132j

Electrification of the chemical industry for carbon-neutral production requires innovative (photo)electrocatalysis. This study highlights the contribution and discusses recent research projects in this area, which are relevant case examples to explor... Read More about Advanced (photo)electrocatalytic approaches to substitute the use of fossil fuels in chemical production.

Assessment of the Degradation Mechanisms of Cu Electrodes during the CO (2023)
Journal Article
Mom, R. V., Sandoval-Diaz, L., Gao, D., Chuang, C., Carbonio, E. A., Jones, T. E., …Velasco-Vélez, J. (in press). Assessment of the Degradation Mechanisms of Cu Electrodes during the CO. ACS applied materials & interfaces, 15(25), https://doi.org/10.1021/acsami.2c23007

Catalyst degradation and product selectivity changes are two of the key challenges in the electrochemical reduction of CO on copper electrodes. Yet, these aspects are often overlooked. Here, we combine X-ray spectroscopy, electron microscopy, an... Read More about Assessment of the Degradation Mechanisms of Cu Electrodes during the CO.

Interfacial chemistry in the electrocatalytic hydrogenation of CO2 over C-Supported Cu-Based systems (2023)
Journal Article
Gianolio, D., Higham, M., Quesne, M., Aramini, M., Xu, R., Large, A., …Arrigo, R. (2023). Interfacial chemistry in the electrocatalytic hydrogenation of CO2 over C-Supported Cu-Based systems. ACS catalysis, 13,

Operando soft and hard X-ray spectroscopic techniques were used in combination with plane-wave density functional theory (DFT) simulations to rationalize the enhanced activities of Zn-containing Cu nanostructured electrocatalysts in the electrocataly... Read More about Interfacial chemistry in the electrocatalytic hydrogenation of CO2 over C-Supported Cu-Based systems.

Orange peel biomass‐derived carbon supported Cu electrocatalysts active in the CO2 ‐ reduction to formic acid (2023)
Journal Article
Miah, T., Demoro, P., Nduka, I., De Luca, F., Abate, S., & Arrigo, R. (2023). Orange peel biomass‐derived carbon supported Cu electrocatalysts active in the CO2 ‐ reduction to formic acid. ChemPhysChem, https://doi.org/10.1002/cphc.202200589

We report a green, wet chemistry approach towards the production of C‐supported Cu electrocatalysts active in the CO2 reduction to formic acid. We use citrus peels as a C support precursor and as a source of reducing agents for the Cu cations. We sho... Read More about Orange peel biomass‐derived carbon supported Cu electrocatalysts active in the CO2 ‐ reduction to formic acid.

Enhanced stability of sub-nanometric iridium decorated graphitic carbon nitride for H 2 production upon hydrous hydrazine decomposition (2022)
Journal Article
Bellomi, S., Barlocco, I., Chen, X., Delgado, J., Arrigo, R., Dimitratos, N., …Villa, A. (2022). Enhanced stability of sub-nanometric iridium decorated graphitic carbon nitride for H 2 production upon hydrous hydrazine decomposition. Physical Chemistry Chemical Physics, 2, 1081-1095. https://doi.org/10.1039/d2cp04387d

Stabilizing metal nanoparticles is vital for large scale implementations of supported metal catalysts, particularly for a sustainable transition to clean energy, e.g., H2 production. In this work, iridium sub-nanometric particles were deposited on co... Read More about Enhanced stability of sub-nanometric iridium decorated graphitic carbon nitride for H 2 production upon hydrous hydrazine decomposition.

In situ dynamics of carbon supported metal systems for carbon dioxide electroreduction (2022)
Presentation / Conference
Arrigo, R. (2022, November). In situ dynamics of carbon supported metal systems for carbon dioxide electroreduction. Presented at Proceedings of International Conference on Frontiers in Electrocatalytic Transformations (INTERECT22), València, Spain

Graphitic materials are largely explored as redox-active supports for metal species in acid/base catalysis, redox catalysis and electrocatalysis. [1] Edge terminations and in-plane point defects, such non 6-membered rings and vacancies on the basal p... Read More about In situ dynamics of carbon supported metal systems for carbon dioxide electroreduction.

The rise of electrochemical NAPXPS operated in the soft X-ray regime exemplified by the oxygen evolution reaction on IrO (2022)
Journal Article
Velasco Vélez, J., Bernsmeier, D., Jones, T., Zeller, P., Carbonio, E., Chuang, C., …Schlögl, R. (2022). The rise of electrochemical NAPXPS operated in the soft X-ray regime exemplified by the oxygen evolution reaction on IrO. Faraday Discussions, https://doi.org/10.1039/d1fd00114k

Photoelectron spectroscopy offers detailed information about the electronic structure and chemical composition of surfaces, owing to the short distance that the photoelectrons can escape from a dense medium. Unfortunately, photoelectron based spectro... Read More about The rise of electrochemical NAPXPS operated in the soft X-ray regime exemplified by the oxygen evolution reaction on IrO.

On the stability of isolated iridium sites in N-rich frameworks against agglomeration under reducing conditions (2022)
Journal Article
Iemhoff, A., Vennewald, M., Artz, J., Mebrahtu, C., Meledin, A., Weirich, T. E., …Palkovits, R. (2022). On the stability of isolated iridium sites in N-rich frameworks against agglomeration under reducing conditions. ChemCatChem, 14(9), https://doi.org/10.1002/cctc.202200179

Stabilization of single metal atoms is a persistent challenge in heterogeneous catalysis. Especially supported late transitions metals are prone to undergo agglomeration to nanoparticles under reducing conditions. In this study, nitrogen-rich covalen... Read More about On the stability of isolated iridium sites in N-rich frameworks against agglomeration under reducing conditions.

Elucidating the formation and structural evolution of platinum single-site catalysts for the hydrogen evolution reaction (2022)
Journal Article
Tang, P., Lee, H., Hurlbutt, K., Huang, P., Narayanan, S., Wang, C., …Pasta, M. (2022). Elucidating the formation and structural evolution of platinum single-site catalysts for the hydrogen evolution reaction. ACS catalysis, 12(5), 3173-3180. https://doi.org/10.1021/acscatal.1c05958

Platinum single-site catalysts (SSCs) are a promising technology for the production of hydrogen from clean energy sources. They have high activity and maximal platinum-atom utilization. However, the bonding environment of platinum during operation... Read More about Elucidating the formation and structural evolution of platinum single-site catalysts for the hydrogen evolution reaction.

Dynamics over a Cu–graphite electrode during the gas-phase CO2 reduction investigated by APXPS (2022)
Journal Article
Arrigo, R., Blume, R., Large, A., Velasco-Vélez, J., Hävecker, M., Knop-Gericke, A., & Held, G. (2022). Dynamics over a Cu–graphite electrode during the gas-phase CO2 reduction investigated by APXPS. Faraday Discussions, https://doi.org/10.1039/d1fd00121c

The electrocatalytic conversion of CO2 to fuels and chemicals using renewable energy is a key decarbonization technology. From a technological viewpoint, the realization of such process in the gas phase and at room temperature is considered advantage... Read More about Dynamics over a Cu–graphite electrode during the gas-phase CO2 reduction investigated by APXPS.

Dynamics at polarized, carbon dioxide-iron oxyhydroxide interfaces unveil the origin of multicarbon product formation (2021)
Journal Article
Arrigo, R., Blume, R., Streibel, V., Genovese, C., Roldan, A., Schuster, M., …Centi, G. (2022). Dynamics at polarized, carbon dioxide-iron oxyhydroxide interfaces unveil the origin of multicarbon product formation. ACS catalysis, 12(1), 411-430. https://doi.org/10.1021/acscatal.1c04296

Surface-sensitive ambient pressure X-ray photoelectron spectroscopy and near edge X-ray absorption fine structure spectroscopy combined with an electrocatalytic reactivity study, multilength scale electron microscopy and theo-retical modelling provid... Read More about Dynamics at polarized, carbon dioxide-iron oxyhydroxide interfaces unveil the origin of multicarbon product formation.

Surface electron-hole rich species active in the electrocatalytic water oxidation (2021)
Journal Article
Velasco-Vélez, J., Carbonio, E., Chuang, C., Hsu, C., Lee, J., Arrigo, R., …Jones, T. (2021). Surface electron-hole rich species active in the electrocatalytic water oxidation. Abstracts of papers / American Chemical Society, 143(32), 12524-12534. https://doi.org/10.1021/jacs.1c01655

Iridium and ruthenium and their oxides/hydroxides are the best candidates for the oxygen evolution reaction under harsh acidic conditions owing to the low overpotentials observed for Ru- and Ir-based anodes and the high corrosion resistance of Ir-oxi... Read More about Surface electron-hole rich species active in the electrocatalytic water oxidation.

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.