Exploring the combustion synthesis for yttrium ruthenate pyrochlores as OER electrocatalysts†

IF 4.7 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY
Megan Heath, Elise Fosdal Closs, Svein Sunde and Frode Seland
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Abstract

Yttrium ruthenate pyrochlores have become popular as electrocatalysts for the oxygen evolution reaction in water electrolysis. However, the traditional synthesis routes used to prepare these Y2Ru2−xYxO7 electrocatalysts require calcination at temperatures higher than 1000 °C for extended periods of time, resulting in highly sintered particles. We propose an alternative synthesis route, a glycine combustion method, that reduces the calcination time to only two hours to obtain porous pyrochlores. These pyrochlores contain a small RuO2 impurity phase that is eliminated when the combusted product is calcined for nine hours instead of two. When the combustion synthesis is combined with a molten salt synthesis (MSS), there is no impurity phase, but large pyrochlore crystallites in a porous matrix are produced. The electrochemically active surface area (ECSA) is an order of magnitude lower than the other pyrochlores prepared, negatively affecting the electrocatalytic activity. In addition to altering the fuel and calcination conditions used in the synthesis, the oxidiser : fuel ratio (ϕ) has also been altered to manipulate the intensity of the combustion reaction. A ϕ = 1, an explosive reaction takes place. The intensity is reduced to a slow burn when adjusting ϕ to 0.3. The synthesised pyrochlores have been analysed with X-ray diffraction (XRD), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), X-ray absorption spectroscopy (XAS) and Raman spectroscopy. They have also been tested as OER electrocatalysts in 0.5 M H2SO4. Combustion-synthesised Y2Ru2−xYxO7 calcined for nine hours has an active-area normalised current of 1.52 mA cm−2 at 1.6 V, which is almost two times higher than that of the same pyrochlore prepared by citric acid, and three times higher than that of RuO2 and IrO2.

Abstract Image

钌酸钇焦绿石燃烧合成OER电催化剂的研究
钌酸钇焦绿石已成为水电解析氧反应的常用电催化剂。然而,用于制备这些Y2Ru2−xYxO7电催化剂的传统合成路线需要在高于1000°C的温度下长时间煅烧,从而导致高度烧结的颗粒。我们提出了一种替代的合成路线,甘氨酸燃烧法,将煅烧时间减少到只有两个小时,以获得多孔焦绿石。这些焦绿石含有少量的RuO2杂质相,当燃烧产物煅烧9小时而不是2小时时,这种杂质相就会被消除。当燃烧合成与熔盐合成(MSS)相结合时,没有杂质相,但在多孔基质中产生了大的焦绿石晶体。电化学活性表面积(ECSA)比制备的其他焦绿石低一个数量级,对电催化活性有不利影响。除了改变合成中使用的燃料和煅烧条件外,氧化剂:燃料比(ϕ)也被改变以操纵燃烧反应的强度。当φ = 1时,发生爆炸反应。当调整φ到0.3时,强度降低到缓慢燃烧。用x射线衍射(XRD)、扫描电镜(SEM)、x射线光电子能谱(XPS)、x射线吸收光谱(XAS)和拉曼光谱对合成的焦绿石进行了分析。它们还在0.5 M H2SO4中作为OER电催化剂进行了测试。燃烧合成的Y2Ru2−xYxO7在1.6 V下具有1.52 mA cm−2的活性区归一化电流,几乎是由柠檬酸制备的相同的焦绿盐的两倍,是RuO2和IrO2的三倍。
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来源期刊
Materials Advances
Materials Advances MATERIALS SCIENCE, MULTIDISCIPLINARY-
CiteScore
7.60
自引率
2.00%
发文量
665
审稿时长
5 weeks
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