M3O4(M=FeCoCrMnMg)高熵氧化物粉体的简易制备及超电容性能研究

doi:10.15541/jim20200388

无机材料学报 ›› 2021, Vol. 36 ›› Issue (4): 425-430.DOI: 10.15541/jim20200388 CSTR: 32189.14.10.15541/jim20200388

所属专题：能源材料论文精选(2021)；【能源环境】超级电容器(202409)

M₃O₄(M=FeCoCrMnMg)高熵氧化物粉体的简易制备及超电容性能研究

王义良¹^,²(), 艾云龙², 杨书伟², 梁炳亮¹^,²(), 郑振环³, 欧阳晟², 何文², 陈卫华², 刘长虹¹^,², 张建军², 刘智勇²

1.南昌航空大学江西省金属材料微结构调控重点实验室, 南昌 330063
2.南昌航空大学材料科学与工程学院, 南昌 330063
3.福州大学材料科学与工程学院, 福州 350108

收稿日期:2020-07-10 修回日期:2020-09-26 出版日期:2021-04-20 网络出版日期:2020-09-20
通讯作者: 梁炳亮, 博士. E-mail: lbl@nchu.edu.cn
作者简介:王义良(1995-), 男, 硕士研究生. E-mail: 1801085204040@stu.nchu.edu.cn
基金资助:
国家自然科学基金(51664043);国家自然科学基金(51802140);江西省自然科学基金(20192BAB206007);江西省金属材料微结构调控重点实验室(南昌航空大学)开放基金(EJ201901455)(EJ201901455);国家留学基金委基金(201708360036)

Facile Synthesis and Supercapacitor Performance of M₃O₄(M=FeCoCrMnMg) High Entropy Oxide Powders

WANG Yiliang¹^,²(), AI Yunlong², YANG Shuwei², LIANG Bingliang¹^,²(), ZHENG Zhenhuan³, OUYANG Sheng², HE Wen², CHEN Weihua², LIU Changhong¹^,², ZHANG Jianjun², LIU Zhiyong²

1. Key Laboratory for Microstructural Control of Metallic Materials of Jiangxi Province, Nanchang Hangkong University, Nanchang 330063, China
2. School of Materials Science and Engineering, Nanchang Hangkong University, Nanchang 330063, China
3. College of Materials Science and Engineering, Fuzhou University, Fuzhou 350108, China

Received:2020-07-10 Revised:2020-09-26 Published:2021-04-20 Online:2020-09-20
Contact: LIANG Bingliang, PhD. E-mail: lbl@nchu.edu.cn
About author:WANG Yiliang(1995-), male, Master candidate. E-mail: 1801085204040@stu.nchu.edu.cn
Supported by:
Natural Science Foundation of China(51664043);Natural Science Foundation of China(51802140);Natural Science Foundation of Jiangxi Province(20192BAB206007);Key Laboratory for Microstructural Control of Metallic Materials of Jiangxi Province(Nanchang Hangkong University Open Fund)(EJ201901455);The China Scholarship Council(201708360036)

摘要/Abstract

摘要：

高熵氧化物以其独特的结构和潜在的应用前景引起了越来越多的关注。本工作采用简单易行的固相反应法制备了M₃O₄(M=FeCoCrMnMg)高熵氧化物粉体, 采用不同手段对粉体进行表征, 并采用涂覆法制备了 M₃O₄/泡沫镍(M₃O₄/NF)复合电极, 研究其超电容性能。结果表明, 随着煅烧温度升高, Fe₂O₃(H)/Co₃O₄(S)/Cr₂O₃(E)和Mn₂O₃(B)相继固溶进入尖晶石主晶相晶格; 在900 ℃煅烧2 h所得M₃O₄粉体的平均粒径为0.69 μm, 具有单一尖晶石结构(面心立方, Fd-3m, a=0.8376 nm), 且Fe、Co、Cr、Mn和Mg五种元素在晶粒内均匀分布, 呈典型的高熵氧化物特征。此外, M₃O₄/NF复合电极在1 mol/L KOH的电解液中, 当电流密度为1 A·g^-1时, 其质量比电容达到193.7 F·g^-1, 可见M₃O₄高熵氧化物在超级电容器电极材料领域具有良好的应用前景。

关键词: M₃O₄高熵氧化物, 固相反应法, 尖晶石结构, 超电容性能

Abstract:

High-entropy oxides have attracted more and more attention due to their unique structures and potential applications. In this work, M₃O₄(M=FeCoCrMnMg) high entropy oxide powders were synthesized by a facile solid-state reaction method. The powders were characterized by different methods. Furthermore, M₃O₄/Ni foam (M₃O₄/NF) electrode was prepared by a coating method, followed by investigation of its supercapacitor performance. The results showed that, with the increase of calcining temperature, Fe₂O₃(H)/Co₃O₄(S)/Cr₂O₃(E) and Mn₂O₃(B) dissolved successively in the crystal lattice of spinel structure. After M₃O₄ powders being calcined at 900 ℃ for 2 h, single spinel structure (FCC, Fd-3m, a=0.8376 nm) was obtained with uniform distribution of Fe, Co, Cr, Mn, and Mg elements, the typical characteristic of high entropy oxide. In addition, the mass specific capacitance of M₃O₄/NF composite electrode is 193.7 F·g^-1, with 1 mol/L KOH as electrolyte and 1 A·g^-1 as current density, which indicated that the M₃O₄ high entropy oxide can be considered as a promising candidate for the electrode material in the field of supercapacitor applications.

Key words: M₃O₄ high entropy oxide, solid state reaction method, spinel structure, supercapacitor performance

中图分类号:

TB34

王义良, 艾云龙, 杨书伟, 梁炳亮, 郑振环, 欧阳晟, 何文, 陈卫华, 刘长虹, 张建军, 刘智勇. M₃O₄(M=FeCoCrMnMg)高熵氧化物粉体的简易制备及超电容性能研究[J]. 无机材料学报, 2021, 36(4): 425-430.

WANG Yiliang, AI Yunlong, YANG Shuwei, LIANG Bingliang, ZHENG Zhenhuan, OUYANG Sheng, HE Wen, CHEN Weihua, LIU Changhong, ZHANG Jianjun, LIU Zhiyong. Facile Synthesis and Supercapacitor Performance of M₃O₄(M=FeCoCrMnMg) High Entropy Oxide Powders[J]. Journal of Inorganic Materials, 2021, 36(4): 425-430.

图/表 5

图1 不同温度煅烧得到的M3O4粉体的XRD图谱(a)、局部放大XRD图谱(2θ=28°~38°)(b)以及Rietveld精修XRD图谱(c)

Fig. 1 XRD patterns (a), enlarged XRD patterns (2θ=28°-38°) (b) and Rietveld refined XRD pattern (c) of M3O4 powders calcined at different temperatures

图2 M3O4粉体的SEM照片(a)和粒度分布图(b)

Fig. 2 SEM image(a) and particle size distribution pattern(b) of M3O4 powders

图3 M3O4的STEM图(a), O、Fe、Co、Cr、Mn、Mg的EDS面分析(b~g), HRTEM照片(h)及沿$[\bar{1}14]$晶带轴的FFT图(i)

Fig. 3 STEM image(a), EDS mapping of O, Fe, Co, Cr, Mn, Mg(b-g), HRTEM image(h) and corresponding FFT pattern aligned along the $[\bar{1}14]$ zone axis(i) of M3O4

图4 M3O4的XPS图谱

Fig. 4 XPS spectra of M3O4 (a) O1s; (b) Fe2p; (c) Co2p; (d) Cr2p; (e) Mn2p; (f) Mg1s

图5 M3O4/NF电极材料的CV曲线(a)、CP曲线(b)、比容量与库仑效率(c)、循环性能(d)和阻抗分析(e)

Fig. 5 CV curves at different scan rates (a), CP curves at different current densities (b), specific capacitance and Coulombic efficiency (c), cycle life (d) and EIS curves (e) for M3O4/NF electrode

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M₃O₄(M=FeCoCrMnMg)高熵氧化物粉体的简易制备及超电容性能研究

Facile Synthesis and Supercapacitor Performance of M₃O₄(M=FeCoCrMnMg) High Entropy Oxide Powders

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