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Preparation of Alkali Metal Iridates as Oxygen Evolution Catalysts Via Thermal Transformation of Amorphous Iridium (oxy)hydroxides. (2024)
Journal Article
Falsaperna, M., Arrigo, R., Marken, F., & Freakley, S. (in press). Preparation of Alkali Metal Iridates as Oxygen Evolution Catalysts Via Thermal Transformation of Amorphous Iridium (oxy)hydroxides. ChemCatChem, Article e202401326. https://doi.org/10.1002/cctc.202401326

Achieving efficient water‐splitting under acidic conditions for hydrogen production is severely limited by the anodic oxygen evolution reaction (OER). Overcoming this obstacle is vital to realise effective electrolysers and deliver a hydrogen‐driven... Read More about Preparation of Alkali Metal Iridates as Oxygen Evolution Catalysts Via Thermal Transformation of Amorphous Iridium (oxy)hydroxides..

Investigation on the structure and performance of supported Ni nanoparticles for the hydrogenation of furfural (2024)
Journal Article
Chen, X., Alijani, S., Gallarati, S., Tessore, F., Jaen, J. J. D., Gianolio, D., …Arrigo, R. (2024). Investigation on the structure and performance of supported Ni nanoparticles for the hydrogenation of furfural. ChemCatChem, Article e202400229. https://doi.org/10.1002/cctc.202400229

In this study, nickel nanoparticles were successfully synthesized using two methods: the hot‐injection method and a room temperature colloidal synthesis using dioctyl tartrate as a capping agent. Each approach yielded Ni nanoparticles with unique mor... Read More about Investigation on the structure and performance of supported Ni nanoparticles for the hydrogenation of furfural.

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.-E., Gao, D., Chuang, C.-H., Carbonio, E. A., Jones, T. E., …Velasco-Vélez, J.-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.

Cationic Copper Species Stabilized by Zinc during the Electrocatalytic Reduction of CO2 Revealed by In Situ X‐Ray Spectroscopy (2023)
Journal Article
Velasco‐Vélez, J., Poon, J., Gao, D., Chuang, C., Bergmann, A., Jones, T. E., …Schlögl, R. (2023). Cationic Copper Species Stabilized by Zinc during the Electrocatalytic Reduction of CO2 Revealed by In Situ X‐Ray Spectroscopy. Advanced Sustainable Systems, 7(5), Article 2200453. https://doi.org/10.1002/adsu.202200453

Advanced in situ X-ray absorption spectroscopy characterization of electrochemically co-electrodeposited bi-element copper alloy electrodes shows that zinc yields the formation of a stable cationic Cu species during the electroreduction of CO2 at hig... Read More about Cationic Copper Species Stabilized by Zinc during the Electrocatalytic Reduction of CO2 Revealed by In Situ X‐Ray Spectroscopy.

Insights by in-situ studies on the nature of highly-active hydrotalcite-based Ni-Fe catalysts for CO2 methanation (2023)
Journal Article
Mebrahtu, C., Krebs, F., Giorgianni, G., Abate, S., Perathoner, S., Centi, G., …Palkovits, R. (2023). Insights by in-situ studies on the nature of highly-active hydrotalcite-based Ni-Fe catalysts for CO2 methanation. Chemical Engineering Research and Design, 193, 320-339. https://doi.org/10.1016/j.cherd.2023.03.026

Designing CO2 methanation catalysts that meet industrial requirements is still challenging. We report Ni-Fe hydrotalcite-derived catalysts with a wide range of Ni and Mg loadings showing that an optimised composition with Ni0.4 gives a very high CO2... Read More about Insights by in-situ studies on the nature of highly-active hydrotalcite-based Ni-Fe catalysts for CO2 methanation.

Lithium-Directed Transformation of Amorphous Iridium (Oxy)hydroxides To Produce Active Water Oxidation Catalysts (2023)
Journal Article
Ruiz Esquius, J., Morgan, D. J., Algara Siller, G., Gianolio, D., Aramini, M., Lahn, L., …Freakley, S. J. (2023). Lithium-Directed Transformation of Amorphous Iridium (Oxy)hydroxides To Produce Active Water Oxidation Catalysts. Journal of the American Chemical Society, 145(11), 6398-6409. https://doi.org/10.1021/jacs.2c13567

The oxygen evolution reaction (OER) is crucial to future energy systems based on water electrolysis. Iridium oxides are promising catalysts due to their resistance to corrosion under acidic and oxidizing conditions. Highly active iridium (oxy)hydroxi... Read More about Lithium-Directed Transformation of Amorphous Iridium (Oxy)hydroxides To Produce Active Water Oxidation Catalysts.

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.

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. J., Bernsmeier, D., Jones, T. E., 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, 236, 103-125. https://doi.org/10.1039/d1fd00114k

Different operando approaches based in PES were used and compared under OER conditions on IrOx. ResPES indicates that single coordinated oxygen atoms (μ1-O) are the active species yielding the formation of peroxo (μ1-OO) and finally O2 as product.

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. I., Velasco-Vélez, J. 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, 236, 126-140. https://doi.org/10.1039/d1fd00121c

We use ambient pressure X-ray photoelectron and absorption spectroscopies coupled with on-line gas detection to investigate in situ performance and interface chemistry of an electrodeposited Cu on a carbon support under conditions of CO2 reduction.

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.