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30 items found (0 items not approved), displaying 1 to 10.[First/Prev] 1, 2, 3 [Next/Last]

Instruments / Technical Area	Publication Details	Published
B18-Core EXAFS	Active and durable R2MnRuO7 pyrochlores with low Ru content for acidic oxygen evolution Dmitry Galyamin , Jorge Torrero , Isabel Rodríguez , Manuel J. Kolb , Pilar Ferrer , Laura Pascual , Mohamed Abdel Salam , Diego Gianolio , Veronica Celorrio , Mohamed Mokhtar , Daniel Garcia Sanchez , Aldo Saul Gago , Kaspar Andreas Friedrich , Miguel A. Peña , José Antonio Alonso , Federico Calle-Vallejo , Maria Retuerto , Sergio Rojas Nature Communications 14 DOI: 10.1038/s41467-023-37665-9 Open Access Show Abstract ▼ Abstract: The production of green hydrogen in water electrolyzers is limited by the oxygen evolution reaction (OER). State-of-the-art electrocatalysts are based on Ir. Ru electrocatalysts are a suitable alternative provided their performance is improved. Here we show that low-Ru-content pyrochlores (R2MnRuO7, R = Y, Tb and Dy) display high activity and durability for the OER in acidic media. Y2MnRuO7 is the most stable catalyst, displaying 1.5 V at 10 mA cm−2 for 40 h, or 5000 cycles up to 1.7 V. Computational and experimental results show that the high performance is owed to Ru sites embedded in RuMnOx surface layers. A water electrolyser with Y2MnRuO7 (with only 0.2 mgRu cm−2) reaches 1 A cm−2 at 1.75 V, remaining stable at 200 mA cm−2 for more than 24 h. These results encourage further investigation on Ru catalysts in which a partial replacement of Ru by inexpensive cations can enhance the OER performance.	Apr 2023
	Cathodes for electrochemical carbon dioxide reduction to multi-carbon products: Part I : A focused review of recent highlights Harry Macpherson , Toby Hodges , Moyahabo Hellen Chuma , Connor Sherwin , Ursa Podbevsek , Katie Rigg , Veronica Celorrio , Andrea Russell , Elena C. Corbos Johnson Matthey Technology Review 67, 97 - 109 DOI: 10.1595/205651323X16672291226135 Show Abstract ▼ Abstract: This is a focused review of recent highlights in the literature in cathode development for low temperature electrochemical carbon dioxide and carbon monoxide reduction to multi-carbon (C2+) products. The major goals for the field are to increase Faradaic efficiency (FE) for specific C2+ products, lower cell voltage for industrially relevant current densities and increase cell lifetime. A key to achieving these goals is the rational design of cathodes through increased understanding of structure-selectivity and structure-activity relationships for catalysts and the influence of catalyst binders and gas diffusion layers (GDLs) on the catalyst microenvironment and subsequent performance.	Jan 2023
	Cathodes for electrochemical carbon dioxide reduction to multi-carbon products: part II : rapid improvement in cathode performance Harry Macpherson , Toby Hodges , Moyahabo Hellen Chuma , Connor Sherwin , Urša Podbevšek , Katie Rigg , Veronica Celorrio , Andrea Russell , Elena C. Corbos Johnson Matthey Technology Review 67, 110 - 123 DOI: 10.1595/205651323X16703459968311 Show Abstract ▼ Abstract: This is Part II of a focused review of recent highlights in the literature in cathode development for low temperature electrochemical carbon dioxide and carbon monoxide reduction to multi-carbon (C2+) products. Part I (1) introduced the role of CO2 reduction in decarbonising the chemical industry and described the catalysts and modelling approaches. Part II describes in situ characterisation to improve the understanding and development of catalysts, the catalyst layer and the gas diffusion layer.	Jan 2023
B18-Core EXAFS	Highly active and stable OER electrocatalysts derived from Sr2MIrO6 for proton exchange membrane water electrolyzers Maria Retuerto , Laura Pascual , Jorge Torrero , Mohamed Abdel Salam , Alvaro Tolosana-Moranchel , Diego Gianolio , Pilar Ferrer , Paula Kayser , Vincent Wilke , Svenja Stiber , Veronica Celorrio , Mohamed Mokthar , Daniel García Sanchez , Aldo Saul Gago , Kaspar Andreas Friedrich , Miguel Antonio Peña , José Antonio Alonso , Sergio Rojas Nature Communications 13 DOI: 10.1038/s41467-022-35631-5 Diamond Proposal Number(s): [27733] Open Access Show Abstract ▼ Abstract: Proton exchange membrane water electrolysis is a promising technology to produce green hydrogen from renewables, as it can efficiently achieve high current densities. Lowering iridium amount in oxygen evolution reaction electrocatalysts is critical for achieving cost-effective production of green hydrogen. In this work, we develop catalysts from Ir double perovskites. Sr2CaIrO6 achieves 10 mA cm−2 at only 1.48 V. The surface of the perovskite reconstructs when immersed in an acidic electrolyte and during the first catalytic cycles, resulting in a stable surface conformed by short-range order edge-sharing IrO6 octahedra arranged in an open structure responsible for the high performance. A proton exchange membrane water electrolysis cell is developed with Sr2CaIrO6 as anode and low Ir loading (0.4 mgIr cm−2). The cell achieves 2.40 V at 6 A cm−2 (overload) and no loss in performance at a constant 2 A cm−2 (nominal load). Thus, reducing Ir use without compromising efficiency and lifetime.	Dec 2022
B18-Core EXAFS	Correlating orbital composition and activity of LaMnxNi1–xO3 nanostructures toward oxygen electrocatalysis Mohammed A. Alkhalifah , Benjamin Howchen , Joseph Staddon , Veronica Celorrio , Devendra Tiwari , David J. Fermin Journal Of The American Chemical Society DOI: 10.1021/jacs.1c11757 Diamond Proposal Number(s): [10306] Show Abstract ▼ Abstract: The atomistic rationalization of the activity of transition metal oxides toward oxygen electrocatalysis is one of the most complex challenges in the field of electrochemical energy conversion. Transition metal oxides exhibit a wide range of structural and electronic properties, which are acutely dependent on composition and crystal structure. So far, identifying one or several properties of transition metal oxides as descriptors for oxygen electrocatalysis remains elusive. In this work, we performed a detailed experimental and computational study of LaMnxNi1–xO3 perovskite nanostructures, establishing an unprecedented correlation between electrocatalytic activity and orbital composition. The composition and structure of the single-phase rhombohedral oxide nanostructures are characterized by a variety of techniques, including X-ray diffraction, X-ray absorption spectroscopy, X-ray photoelectron spectroscopy, and electron microscopy. Systematic electrochemical analysis of pseudocapacitive responses in the potential region relevant to oxygen electrocatalysis shows the evolution of Mn and Ni d-orbitals as a function of the perovskite composition. We rationalize these observations on the basis of electronic structure calculations employing DFT with HSE06 hybrid functional. Our analysis clearly shows a linear correlation between the OER kinetics and the integrated density of states (DOS) associated with Ni and Mn 3d states in the energy range relevant to operational conditions. In contrast, the ORR kinetics exhibits a second-order reaction with respect to the electron density in Mn and Ni 3d states. For the first time, our study identifies the relevant DOS dominating both reactions and the importance of understanding orbital occupancy under operational conditions.	Mar 2022
B18-Core EXAFS E01-JEM ARM 200CF E02-JEM ARM 300CF	Identification and manipulation of dynamic active site deficiency-induced competing reactions in electrocatalytic oxidation processes Runjia Lin , Liqun Kang , Tianqi Zhao , Jianrui Feng , Veronica Celorrio , Guohui Zhang , Giannantonio Cibin , Anthony Kucernak , Dan Brett , Furio Cora , Ivan P. Parkin , Guanjie He Energy & Environmental Science DOI: 10.1039/D1EE03522C Diamond Proposal Number(s): [25410, 29207] Open Access Show Abstract ▼ Abstract: Electrocatalytic organic compound oxidation reactions (OCORs) have been intensively studied for energy and environmentally benign applications. However, relatively little effort has been devoted to developing a fundamental understanding of OCOR, including the detailed competition with side reactions and activity limitations, thus inhibiting the rational design of high-performance electrocatalysts. Herein, by taking NiWO4-catalysed urea oxidation reaction (UOR) in aqueous media as an example, the competition between the OCOR and the oxygen evolution reaction (OER) within a wide potential range is examined. It is shown that the root of the competition can be ascribed to insufficient surface concentration of dynamic Ni3+, an active site shared by both UOR and OER. Similar phenomenon are observed in other OCOR electrocatalysts and systems. To address the issue, a “controllable reconstruction of pseudo-crystalline bimetal oxides” design strategy is proposed to maximise the dynamic Ni3+ population and manipulate the competition between UOR and OER. The optimised electrocatalyst delivers best-in-class performance and a ~10-fold increase in current density at 1.6 V versus the reversible hydrogen electrode for alkaline urea electrolysis compared to that of the pristine materials.	Mar 2022
B18-Core EXAFS	Insight into the activity and selectivity of nanostructured copper titanates during electrochemical conversion of CO2 at neutral pH via in situ X-ray Absorption Spectroscopy Matthew J. Lawrence , Veronica Celorrio , Elizabeth Sargeant , Haoliang Huang , Joaquín Rodríguez-López , Yuanmin Zhu , Meng Gu , Andrea E. Russell , Paramaconi Rodriguez Acs Applied Materials & Interfaces DOI: 10.1021/acsami.1c19298 Diamond Proposal Number(s): [21533] Open Access Show Abstract ▼ Abstract: The electrochemical conversion of carbon dioxide (CO2) to useful chemical fuels is a promising route toward the achievement of carbon neutral and carbon negative energy technologies. Copper (Cu)- and Cu oxide-derived surfaces are known to electrochemically convert CO2 to high-value and energy-dense products. However, the nature and stability of oxidized Cu species under reaction conditions are the subject of much debate in the literature. Herein, we present the synthesis and characterization of copper-titanate nanocatalysts, with discrete Cu–O coordination environments, for the electrochemical CO2 reduction reaction (CO2RR). We employ real-time in situ X-ray absorption spectroscopy (XAS) to monitor Cu species under neutral-pH CO2RR conditions. Combination of voltammetry and on-line electrochemical mass spectrometry with XAS results demonstrates that the titanate motif promotes the retention of oxidized Cu species under reducing conditions for extended periods, without itself possessing any CO2RR activity. Additionally, we demonstrate that the specific nature of the Cu–O environment and the size of the catalyst dictate the long-term stability of the oxidized Cu species and, subsequently, the product selectivity.	Jan 2022
B18-Core EXAFS E01-JEM ARM 200CF	Structure-activity relationships in highly active platinum-tin MFI-type zeolite catalysts for propane dehydrogenation Andrew Beale , Ines Lezcano-Gonzalez , Peixi Cong , Emma Campbell , Monik Panchal , Miren Agote-Aran , Veronica Celorrio , Qian He , Ramon Oord , Bert M. Weckhuysen Chemcatchem DOI: 10.1002/cctc.202101828 Show Abstract ▼ Abstract: Pt/Sn-containing MFI zeolites prepared by one-pot hydrothermal methods are highly active and selective catalysts for propane dehydrogenation. An alternative preparation method is reported alongside an in-depth characterization of Pt and Sn before and after reaction. Pt species dispersed on highly-defective Silicalite-1 show a significantly long catalytic lifetime with an improved coke resistance, but increased Pt-Sn alloying and the (eventual) build-up of carbon leads to deactivation.	Jan 2022
B18-Core EXAFS	Na2.4Al0.4Mn2.6O7 anionic redox cathode material for sodium ion batteries - a combined experimental and theoretical approach to elucidate its charge storage mechanism Cindy Soares , Begoña Silvan , Yong-Seok Choi , Veronica Celorrio , Giannantonio Cibin , David O. Scanlon , Nuria Tapia-Ruiz Journal Of Materials Chemistry A DOI: 10.1039/D1TA05137G Diamond Proposal Number(s): [21847] Open Access Show Abstract ▼ Abstract: Here we report the synthesis via ceramic methods of the high-performance Mn-rich Na2.4Al0.4Mn2.6O7 oxygen-redox cathode material for Na-ion batteries which we use as a testbed material to study the effects of Al substitution and subsequent Na excess in the high-capacity, anionic redox-based cathode material Na2Mn3O7. The material shows a stable electrochemical performance, with a specific capacity of 200 mAh g-1 in the 1.5 - 4.7 voltage window at C/20 and capacity retention of 90 % after 40 cycles. Using a combination of electrochemical and structural analysis together with hybrid density functional theory calculations we explain the behaviour of this material with changes in Mn/anionic redox reactions and associated O2 release reactions occurring in the material during electrochemical cycling (Na insertion/extraction) and compare these findings to Na2Mn3O7. We expect that these results will advance understanding of the effect of dopants in Mn-rich cathode materials with oxygen redox activity to pave their way towards real applications in high-performing sodium-ion battery applications.	Dec 2021
B18-Core EXAFS	Isolating the contributions of surface Sn atoms in the bifunctional behaviour of PtSn CO oxidation electrocatalysts Haoliang Huang , Oliver F. Blackman , Veronica Celorrio , Andrea E. Russell Electrochimica Acta 52 DOI: 10.1016/j.electacta.2021.138811 Diamond Proposal Number(s): [19850] Show Abstract ▼ Abstract: The bifunctional mechanism is well-acknowledged for the promoted CO oxidation on Pt-based bimetallic electrocatalysts. However, the direct identification of the active oxygenated species and the nature and electrochemistry of the second component are still a matter of debate. Herein, Snad-Pt/C catalysts, where Sn ad-atoms are exclusively on the surface of Pt nanoparticles at low coverages ranging from 0.0033 to 0.2 monolayers to avoid sub-surface Sn and alloy formation, were prepared as a model system to resolve these issues using a surface organometallic chemistry approach. Effects of the Sn ad-atoms on CO oxidation were studied by CO stripping voltammograms as a function of Sn coverage. Using in situ XAS measurements, the Sn average oxidation state is estimated to increase from +0.2 to +3.1 as the potential increases from 0 to 0.8 VRHE, with the number of the oxygen neighbours increasing stepwise. Pt4.5-Sn-(OH)1.5 is revealed as the active species responsible for the bifunctional mechanism at low overpotentials and is generated via a redox couple corresponding to Pt4.5-Sn*/Pt4.5-Sn-(OH)1.5.	Jun 2021

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