[Ru(tmphen)3]2[Fe(CN)6] 和 [Ru(phen)3][Fe(CN)5(NO)] 配合物形成异质结构的 RuO2-Fe2O3 纳米复合材料作为高效的碱性 HER 和 OER电催化剂,Dalton Transactions

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[Ru(tmphen)3]2[Fe(CN)6] 和 [Ru(phen)3][Fe(CN)5(NO)] 配合物形成异质结构的 RuO2-Fe2O3 纳米复合材料作为高效的碱性 HER 和 OER电催化剂
Dalton Transactions ( IF 3.5 ) Pub Date : 2022-03-31 , DOI: 10.1039/d2dt00398h
Hamta Mosallaei ₁ , Hassan Hadadzadeh ₁ , Annette Foelske ₂ , Markus Sauer ₂ , Hadi Amiri Rudbari ₃ , Olivier Blacque ₄

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水电解是提供清洁燃料的最有效工艺之一。在此，两种新型离子型Ru( II )-Fe( II )配合物[Ru(tmphen) ₃ ] ₂ [Fe(CN) ₆ ]和[Ru(phen) ₃ ][Fe(CN) ₅ (NO)]，其中 tmphen = 3,4,7,8-tetramethyl-1,10-phenanthroline 和 phen = 1,10-phenanthroline，合成并通过紫外-可见光谱、元素分析、FT-IR 和单晶 X-射线结构分析。通过将 [Ru(tmphen) ₃ ] ₂ [Fe(CN) ₆ ] 配合物在 600 °C 下热分解 4 h，得到异质结构的 RuO ₂ –Fe ₂ O ₃通过简单的一锅法处理制备纳米复合材料，然后通过 FT-IR、XRD、FT-Raman、UV-Vis (DRS)、ICP-OES、FE-SEM、TEM、TGA/DTG、BET 和 XPS 分析对其进行表征，这表明形成了平均尺寸为 8-12 nm的高度结晶的 RuO ₂ -Fe ₂ O _{3纳米颗粒。}制备的纳米复合材料是一种高效的异质结构电催化剂，用于在碱性溶液中进行水分解氧化还原反应过程，包括析氢和析氧反应（HER 和 OER）。在这方面，还通过[Ru(tmphen) ₃ ](NO ₃ ) _{2的热分解制备了RuO}₂和Fe ₂ O _3样品。和 K ₄ [Fe(CN) ₆ ] 前体分别作为对照实验，比较它们的 HER 和 OER 电催化活性与 RuO ₂ -Fe ₂ O ₃纳米复合材料的电催化活性。具体来说，RuO ₂ -Fe ₂ O ₃纳米复合材料表现出显着的电催化性能，在 -148 和 292 mV 过电位下产生 10 mA cm ^-2电流密度，将 LSV 曲线拟合到 Tafel 方程的 Tafel 斜率为 -43 和HER 和 OER 分别为56.08 mV dec ^{-1 。}因此，异质结构的RuO ₂ -Fe ₂ O ₃纳米复合材料可以被视为 HER 和 OER 的双功能电催化剂，因为它利用了异质结构和其界面处的活性位点的协同效应。

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[Ru(tmphen)3]2[Fe(CN)6] and [Ru(phen)3][Fe(CN)5(NO)] complexes and formation of a heterostructured RuO2–Fe2O3 nanocomposite as an efficient alkaline HER and OER electrocatalyst

Water electrolysis is one of the most capable processes for supplying clean fuel. Herein, two novel ionic Ru(II)–Fe(II) complexes, [Ru(tmphen)₃]₂[Fe(CN)₆] and [Ru(phen)₃][Fe(CN)₅(NO)], where tmphen = 3,4,7,8-tetramethyl-1,10-phenanthroline and phen = 1,10-phenanthroline, were synthesized and characterized by UV-Vis spectroscopy, elemental analysis, FT-IR, and single-crystal X-ray structural analysis. By thermally decomposing the [Ru(tmphen)₃]₂[Fe(CN)₆] complex at 600 °C for 4 h, a heterostructured RuO₂–Fe₂O₃ nanocomposite was fabricated through a facile one-pot treatment and then characterized by FT-IR, XRD, FT-Raman, UV-Vis (DRS), ICP-OES, FE-SEM, TEM, TGA/DTG, BET, and XPS analyses, which revealed the formation of highly crystalline RuO₂–Fe₂O₃ nanoparticles with an average size of 8–12 nm. The prepared nanocomposite was an efficient heterostructured electrocatalyst for performing water-splitting redox reaction processes, including hydrogen and oxygen evolution reactions (HER and OER) in alkaline solutions. In this regard, RuO₂ and Fe₂O₃ samples were also prepared through thermal decomposition of [Ru(tmphen)₃](NO₃)₂ and K₄[Fe(CN)₆] precursors, respectively, as control experiments to compare their HER and OER electrocatalytic activity with that of the RuO₂–Fe₂O₃ nanocomposite. Specifically, the RuO₂–Fe₂O₃ nanocomposite exhibited significant electrocatalytic performance, generating 10 mA cm⁻² current density at −148 and 292 mV overpotentials, and the Tafel slope results from fitting the LSV curves to the Tafel equation were −43 and 56.08 mV dec⁻¹ for the HER and OER, respectively. Therefore, the heterostructured RuO₂–Fe₂O₃ nanocomposite can be viewed as a bi-functional electrocatalyst for HER and OER because it exploits the synergistic effects of heterostructures and active sites at its interface.

更新日期：2022-03-31

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