Zr–Cu oxide heterostructures with introduced defects for efficient oxygen reduction reaction

IF 4.7 3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Materials Chemistry and Physics Pub Date : 2025-07-01 Epub Date: 2025-03-08 DOI:10.1016/j.matchemphys.2025.130688
Simin Shan , Lijian Du , Shuaishuai Cheng, Yue Yin, Jinfang Wu, Wenbo Wang
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Abstract

Creating an oxygen reduction reaction (ORR) electrocatalyst with outstanding performance is crucial for advancing green energy storage and conversion technology. In this experiment, Zr–Cu oxide heterostructure nanocomposite catalysts, ZrO2–Cu2S/C and ZrO2–Cu1.93S/C, were successfully synthesized by vulcanizing ZrO2–Cu2(OH)2CO3/C and introducing defect engineering. The catalysts were thoroughly examined using various testing methods to determine their structures, and their catalytic performance in ORR was assessed. ZrO2 forms heterostructures with Cu2S and Cu1.93S, which are evenly dispersed on the carbon carrier. In an alkaline medium, both catalysts display excellent ORR activity. The ZrO2–Cu1.93S/C catalyst exhibits the highest ORR activity, with an onset potential of 0.90 V and a half-wave potential of 0.75 V (vs. RHE) in 0.1 M KOH. The limiting diffusion current density is measured at 3.25 mA cm−2. The DFT theoretical calculation indicates that electrons are redistributed and accumulated at the heterojunction interface, presenting a stronger electron-donating ability and a faster electron conduction ability. Both vulcanization and the introduction of defects play an important role in enhancing the ORR performance of the catalyst. This study provides an ORR catalyst with excellent performance and opens up a new direction and idea for the research of Zr–Cu oxide composite electrocatalysts.

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引入缺陷的Zr-Cu氧化物异质结构用于高效氧还原反应
研制性能优异的氧还原反应(ORR)电催化剂是推进绿色能源存储与转化技术的关键。本实验通过对ZrO2-Cu2 (OH)2CO3/C进行硫化并引入缺陷工程,成功合成了Zr-Cu氧化物异质结构纳米复合催化剂ZrO2-Cu2S /C和ZrO2-Cu1.93S /C。采用各种测试方法对催化剂进行了全面的测试,以确定其结构,并评估了其在ORR中的催化性能。ZrO2与Cu2S和Cu1.93S形成异质结构,均匀分布在碳载体上。在碱性介质中,两种催化剂均表现出优异的ORR活性。ZrO2-Cu1.93S /C催化剂表现出最高的ORR活性,在0.1 M KOH条件下,起始电位为0.90 V,半波电位为0.75 V(相对于RHE)。极限扩散电流密度测量为3.25 mA cm−2。DFT理论计算表明,电子在异质结界面处被重新分配和积累,呈现出更强的给电子能力和更快的电子传导能力。硫化和缺陷的引入都是提高催化剂ORR性能的重要因素。本研究提供了一种性能优良的ORR催化剂,为Zr-Cu氧化物复合电催化剂的研究开辟了新的方向和思路。
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麦克林
Zirconium chloride
来源期刊
Materials Chemistry and Physics
Materials Chemistry and Physics 工程技术-材料科学:综合
CiteScore
8.70
自引率
4.30%
发文量
1515
审稿时长
69 days
期刊介绍: Materials Chemistry and Physics is devoted to short communications, full-length research papers and feature articles on interrelationships among structure, properties, processing and performance of materials. The Editors welcome manuscripts on thin films, surface and interface science, materials degradation and reliability, metallurgy, semiconductors and optoelectronic materials, fine ceramics, magnetics, superconductors, specialty polymers, nano-materials and composite materials.
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