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多孔LaCo1-xNixO3-δ纳米结构作为一种用于水氧化和锌空气电池的高效电催化剂

Porous LaCo1-xNixO3-δ Nanostructures as an Efficient Electrocatalyst for Water Oxidation and for a Zinc-Air Battery.

作者信息

Vignesh Ahilan, Prabu Moni, Shanmugam Sangaraju

机构信息

Department of Energy Systems Engineering, Daegu Gyeongbuk Institute of Science and Technology (DGIST) , 50-1 Sang-Ri, Hyeongpung-Myeon, Dalseong-gun, Daegu 42988, Republic of Korea.

出版信息

ACS Appl Mater Interfaces. 2016 Mar 9;8(9):6019-31. doi: 10.1021/acsami.5b11840. Epub 2016 Mar 1.

Abstract

Perovskites have emerged as promising earth-abundant alternatives to precious metals for catalyzing the oxygen evolution reaction (OER). Herein, we report the synthesis of a series of porous perovskite nanostructures, LaCo0.97O3-δ, with systematic Ni substitution in Co octahedral sites. Their electrocatalytic activity during the water oxidation reaction was studied in alkaline electrolytes. The electrocatalytic OER activity and stability of the perovskite nanostructure was evaluated using the rotating disk electrode technique. We show that the progressive replacement of Co by Ni in the LaCo0.97O3-δ perovskite structure greatly altered the electrocatalytic activity and that the La(Co0.71Ni0.25)0.96O3-δ composition exhibited the lowest OER overpotential of 324 and 265 mV at 10 mA cm(-2) in 0.1 M KOH and 1 M KOH, respectively. This value was much lower than that of the noble metal catalysts, IrO2, Ru/C, and Pt/C. Furthermore, the La(Co0.71Ni0.25)0.96O3-δ nanostructure showed outstanding electrode stability, with no observable decrease in performance up to 114th cycle in the auxiliary linear sweep voltammetry that lasted for 10 h in chronoamperometry studies. The excellent oxygen evolution activity of the La(Co0.71Ni0.25)0.96O3-δ perovskite nanostructure can be attributed to its intrinsic structure, interconnected particle arrangement, and unique redox characteristics. The enhanced intrinsic electrocatalytic activity of the La(Co0.71Ni0.25)0.96O3-δ catalyst was correlated with several parameters, such as the electrochemical surface area, the roughness factor, and the turnover frequency, with respect to variation in the transition metals of the perovskite structure. Subsequently, La(Co0.71Ni0.25)0.96O3-δ was utilized as the air cathode in a zinc-air battery application.

摘要

钙钛矿已成为一种有前景的、以地球上储量丰富的元素替代贵金属来催化析氧反应(OER)的材料。在此,我们报告了一系列多孔钙钛矿纳米结构LaCo0.97O3-δ的合成,其中在钴八面体位置进行了系统的镍取代。在碱性电解质中研究了它们在水氧化反应中的电催化活性。使用旋转圆盘电极技术评估了钙钛矿纳米结构的电催化OER活性和稳定性。我们表明,在LaCo0.97O3-δ钙钛矿结构中用镍逐步取代钴极大地改变了电催化活性,并且La(Co0.71Ni0.25)0.96O3-δ组成在0.1 M KOH和1 M KOH中于10 mA cm(-2)时分别表现出最低的OER过电位,为324和265 mV。该值远低于贵金属催化剂IrO2、Ru/C和Pt/C。此外,La(Co0.71Ni0.25)0.96O3-δ纳米结构表现出出色的电极稳定性,在计时电流法研究中持续10小时的辅助线性扫描伏安法中,直至第114个循环性能均未观察到下降。La(Co0.71Ni0.25)0.96O3-δ钙钛矿纳米结构优异的析氧活性可归因于其固有结构、相互连接的颗粒排列以及独特的氧化还原特性。La(Co0.71Ni0.25)0.96O3-δ催化剂增强的固有电催化活性与几个参数相关,例如电化学表面积、粗糙度因子和周转频率,这与钙钛矿结构中过渡金属的变化有关。随后,La(Co0.71Ni0.25)0.96O3-δ被用作锌空气电池应用中的空气阴极。

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