Chakraborty Biswarup, Kalra Shweta, Beltrán-Suito Rodrigo, Das Chittaranjan, Hellmann Tim, Menezes Prashanth W, Driess Matthias
Department of Chemistry Metalorganics and Inorganic Materials, Technische Universität Berlin, Straße des 17 Juni 135, Sekr. C2, 10623, Berlin, Germany.
Karlsruhe Institute of Technology (KIT), Institute for Applied Materials (IAM-ESS), Hermann-von-Helmholtz-Platz 1, D-76344, Eggenstein-Leopoldshafen, Germany.
Chem Asian J. 2020 Mar 16;15(6):852-859. doi: 10.1002/asia.202000022. Epub 2020 Feb 20.
In the urge of designing noble metal-free and sustainable electrocatalysts for oxygen evolution reaction (OER), herein, a mineral Digenite Cu S has been prepared from a molecular copper(I) precursor, {(PyHS) Cu (PyHS)} (1), and utilized as an anode material in electrocatalytic OER for the first time. A hot injection of 1 yielded a pure phase and highly crystalline Cu S , which was then electrophoretically deposited (EPD) on a highly conducting nickel foam (NF) substrate. When assessed as an electrode for OER, the Cu S /NF displayed an overpotential of merely 298±3 mV at a current density of 10 mA cm in alkaline media. The overpotential recorded here supersedes the value obtained for the best reported Cu-based as well as the benchmark precious-metal-based RuO and IrO electrocatalysts. In addition, the choronoamperometric OER indicated the superior stability of Cu S /NF, rendering its suitability as the sustainable anode material for practical feasibility. The excellent catalytic activity of Cu S can be attributed to the formation of a crystalline CuO overlayer on the conductive Cu S that behaves as active species to facilitate OER. This study delivers a distinct molecular precursor approach to produce highly active copper-based catalysts that could be used as an efficient and durable OER electro(pre)catalysts relying on non-precious metals.
在设计用于析氧反应(OER)的无贵金属且可持续的电催化剂的迫切需求下,本文首次从分子铜(I)前体{(PyHS)Cu(PyHS)}(1)制备了矿物辉铜矿Cu₂S,并将其用作电催化OER的阳极材料。对1进行热注射得到了纯相且高度结晶的Cu₂S,然后将其电泳沉积(EPD)在高导电性泡沫镍(NF)基底上。当评估其作为OER电极时,Cu₂S/NF在碱性介质中电流密度为10 mA cm⁻²时的过电位仅为298±3 mV。此处记录的过电位超过了报道的最佳铜基以及基准贵金属基RuO₂和IrO₂电催化剂所获得的值。此外,计时电流法OER表明Cu₂S/NF具有优异的稳定性,使其适合作为实际可行性的可持续阳极材料。Cu₂S优异的催化活性可归因于在导电的Cu₂S上形成了结晶CuO覆盖层,该覆盖层作为活性物种促进OER。这项研究提供了一种独特的分子前体方法来制备高活性铜基催化剂,该催化剂可用作依赖非贵金属的高效且耐用的OER电(预)催化剂。