Читать книгу First virtual Bilateral Conference on Functional Materials (BiC-FM) - Сборник статей, Андрей Владимрович Быстров, Анна Владимировна Климович - Страница 13
Oral Sessions
Thursday, October 8
Enhanced Electrocatalytic Activities by Substitutional Tuning of Nickel-based Ruddlesden-Popper Catalysts for the Oxidation of Urea and Small Alcohols
ОглавлениеStevenson, K. J.1
1 – Skolkovo Institute of Science and Technology, Moscow, Russia
k.stevenson@skoltech.ru
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.
