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用于碱性析氧反应(OER)的MOF-碳复合材料原位合成与合成后形成的比较作为电催化剂

Comparison of In Situ and Postsynthetic Formation of MOF-Carbon Composites as Electrocatalysts for the Alkaline Oxygen Evolution Reaction (OER).

作者信息

Sondermann Linda, Voggenauer Laura Maria, Vollrath Annette, Strothmann Till, Janiak Christoph

机构信息

Institut für Anorganische Chemie und Strukturchemie, Heinrich-Heine-Universität Düsseldorf, 40225 Düsseldorf, Germany.

出版信息

Molecules. 2025 Jan 7;30(2):208. doi: 10.3390/molecules30020208.

Abstract

Mixed-metal nickel-iron, NiFe materials draw attention as affordable earth-abundant electrocatalysts for the oxygen evolution reaction (OER). Here, nickel and mixed-metal nickel-iron metal-organic framework (MOF) composites with the carbon materials ketjenblack (KB) or carbon nanotubes (CNT) were synthesized in situ in a one-pot solvothermal reaction. As a direct comparison to these in situ synthesized composites, the neat MOFs were postsynthetically mixed by grinding with KB or CNT, to generate physical mixture composites. The in situ and postsynthetic MOF/carbon samples were comparatively tested as (pre-)catalysts for the OER, and most of them outperformed the RuO benchmark. Depending on the carbon material and metal ratio, the in situ or postsynthetic composites performed better, showing that the method to generate the composite can influence the OER activity. The best material NiFe-CNT was synthesized in situ and achieved an overpotential () of 301 mV (RuO = 354 mV), a Tafel slope () of 58 mV/dec (RuO = 91 mV/dec), a charge transfer resistance (R) of 7 Ω (RuO R = 39 Ω), and a faradaic efficiency (FE) of 95% (RuO FE = 91%). Structural changes in the materials could be seen through a stability test in the alkaline electrolyte, and chronopotentiometry over 12 h showed that the derived electrocatalysts and RuO have good stability.

摘要

混合金属镍铁(NiFe)材料作为一种价格低廉且储量丰富的析氧反应(OER)电催化剂备受关注。在此,通过一锅法溶剂热反应原位合成了镍以及镍铁混合金属有机框架(MOF)与碳材料科琴黑(KB)或碳纳米管(CNT)的复合材料。作为对这些原位合成复合材料的直接对比,将纯净的MOF通过与KB或CNT研磨进行后合成混合,以生成物理混合复合材料。对原位和后合成的MOF/碳样品作为OER的(预)催化剂进行了对比测试,其中大多数表现优于RuO基准。根据碳材料和金属比例,原位或后合成复合材料表现更佳,这表明生成复合材料的方法会影响OER活性。最佳材料NiFe-CNT是原位合成的,其过电位(η)为301 mV(RuO₂为354 mV),塔菲尔斜率(b)为58 mV/dec(RuO₂为91 mV/dec),电荷转移电阻(Rct)为7 Ω(RuO₂的Rct = 39 Ω),法拉第效率(FE)为95%(RuO₂的FE = 91%)。通过在碱性电解质中的稳定性测试可以观察到材料的结构变化,12小时的计时电位法表明衍生的电催化剂和RuO₂具有良好的稳定性。

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