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Название: First virtual Bilateral Conference on Functional Materials (BiC-FM)

Автор: Сборник статей

Издательство: Aegitas

Жанр: Техническая литература

Серия:

isbn: 9780369404497

isbn:

СКАЧАТЬ style="font-size:15px;">      [1] D. Duan et al., Sci. Rep. 4, 6968 (2018)

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      Enhanced Electrocatalytic Activities by Substitutional Tuning of Nickel-based Ruddlesden-Popper Catalysts for the Oxidation of Urea and Small Alcohols

      Stevenson, K. J.1

      1 – Skolkovo Institute of Science and Technology, Moscow, Russia

      [email protected]

      The electrooxidation of urea continues to attract considerable interest as an alternative to the oxygen evolution reaction (OER) as the anodic reaction in the electrochemical generation of hydrogen due to the lower potential required to drive the reaction and the abundance of urea available in waste streams. In this talk the effect of Sr substitution in a series of La2-xSrxNiO4+δRuddlesden-Popper catalysts on the electrooxidations of urea, methanol, and ethanol are presented. We demonstrate that activities toward the urea oxidation reaction increase with increasing Ni oxidation state. The 75 % Sr-substituted La0.5Sr1.5NiO4+δ catalyst exhibits a mass activity of 588 mA and 7.85 A for the electrooxidation of urea in 1 M KOH containing 0.33 M urea, demonstrating the potential applications of Ni-based Ruddlesden-Popper materials for direct urea fuel cells and low-cost hydrogen production.[1] Additionally, we find the same correlations between Ni oxidation state and activities for the electrooxidations of methanol and ethanol, as well as identify processes that result in catalyst deactivation for all three oxidations. This demonstration of how systematically increasing Ni – O bond covalency by raising the formal oxidation state of Ni above +3 serves to increase catalyst activity for these reactions acts as a governing principle for the rational design of catalysts for the electrooxidation of urea and other small molecules going forward [2]

      References:

      [1] Forslund, R. P.; Alexander, C. T.; Abakumov, A. M.; Johnston, K. P.; Stevenson, K. J. “Enhanced Electrocatalytic Activities of Nickel-based Ruddlesden-Popper Catalysts for the Oxidation of Urea and Small Alcohols By Active Site Variation,” ACS Catal. 2019,9(3), 2664–2673.

      [2] Forslund, R. P.; Hardin, W. G.; Rong, X; Abakumov, A. M.; Filimonov, D.; Alexander, C. T.; Mefford, J. T.; Iyer, H.; Kolpak, A. M.; Johnston, K. P; Stevenson, K. J. “Exceptional Electrocatalytic Oxygen Evolution Via Tunable Charge Transfer Interactions in La0.5Sr1.5Ni1-xFexO4+δ Ruddlesden-Popper Oxides,” Nature Comm. 2018,9(1)3150.

      Professor Stevenson is Full Professor and Provost at the Skolkovo Institute for Science and Technology in Moscow, Russia. His interests are aimed at elucidating and controlling chemistry at interfaces vital to many energy storage and energy conversion technologies. He has published over 280 papers, six patents, and six book chapters. He is the founding director of Skoltech’s Center for Energy Science and Technology. In 2019, Skoltech became the youngest university in the world and only university in the Russian Federation to be ranked in top 100 Nature Index of Top Young Universities.

      Electrochemical synthesis of copolymers containing porphyrine derivatives and their activity towards CO2

      Sachin Kochrekar,1,2 Ajit Kalekar,2 Shweta Mehta,3,4 Pia Damlin,2 Mikko Salomäki,2 Sari Granroth,5 Niko Meltola,6 Kavita Joshi,3,4Carita Kvarnström2

      1Turku University Graduate School (UTUGS) Doctoral Programme in Physical and Chemical Sciences, FI-20014 Turku, Finland

      2Turku University Centre for Materials and Surfaces (MatSurf), Department of Chemistry, University of Turku, Vatselankatu 2, FI-20014 Turku, Finland.

      3Physical and Materials Chemistry Division, CSIR-National Chemical Laboratory, Pune 411008 India.

      4Academy of Scientific and Innovative Research (AcSIR), Ghaziabad-200112, UP, India.

      5Laboratory of Materials Science, University of Turku, FI-20014, Turku, Finland.

      6ArcDia International Oy Ltd, Lemminkäisenkatu 32, FI-20521-Turku, Finland.

      [email protected]

      This study reports the electropolymerization of novel keto functionalized octaethyl metal porphyrins (Zn+2 and Ni+2) in presence of 4,4 bipyridine (4,4´ BPy) as bridging nucleophile on FTO surface. The polymer films were characterized by electrochemical, spectroscopic (UV–Vis, XPS, FT-IR and Raman spectroscopy) and microscopic (AFM and SEM) techniques. The absorption and electronic spectra establish the binding of monomer units in the polymer film, retaining most of the spectroscopic properties of the monomer with slight shift and peak broadening. The surface morphology reveals heterogeneous polymerization. Through computational studies, we aim to get insight into the effect of metal center (Zn+2 and Ni+2) and presence of the keto group on the porphyrin unit. The first 4,4´ BPy prefers meso position next to β-keto group in ZnOEPK whereas it prefers opposite meso position in NiOEPK further leading to linear and branched orientation with the introduction of second 4,4´ BPy, respectively. The interaction between the polymer films in the absence and presence of CO2 suggests a similar mechanism for both the polymers. The role of the 4,4´ BPy in the polymer unit in association with the activity with CO2 is emphasized.

      Acknowledgement. The authors acknowledge the Magnus Ehrnrooth foundation and Business Finland for financial support.

      Carita Kvarnström

      Professor of Materials Chemistry

      Department of Chemistry

      University of Turku

      Finland

      1996 PhD, Åbo Akademi University, Åbo-Turku Finland

      1996–2008 Assistant and Associate Professor, Åbo Akademi University, Åbo-Turku Finland

      2009- Full Professor in Materials Chemistry University of Turku, СКАЧАТЬ