Rational engineering of high-entropy oxides for Li-ion battery anodes with finely tuned combustion syntheses

IF 8.6 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Npg Asia Materials Pub Date : 2023-10-13 DOI:10.1038/s41427-023-00502-y
Dongjoon Shin, Seunghoon Chae, Seonghyun Park, Byungseok Seo, Wonjoon Choi
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Abstract

Abstract High-entropy oxides (HEOs) are promising conversion-type anode materials for Li-ion batteries (LIBs) owing to their excellent cycling stabilities and rate capabilities. However, the conventional syntheses and screening processes are time-consuming and complex and require phase and interfacial segregation of individual elements. Herein, we report a rational screening strategy for LIB anodes using precisely tunable HEOs fabricated by one-step combustion syntheses with different fuel-to-oxidizer ratios (φ). A slightly lean fuel mixture (φ-0.95) enabled a suitable temperature and non-reducing atmosphere for optimal HEO syntheses. This provided high crystallinity, perfectly homogeneous elemental distributions, and adequate pore structures without selective precipitation, whereas lower or higher fuel-to-oxidizer ratios resulted in excessively porous morphologies or elemental segregation. HEO-based anodes with φ-0.95 exhibited outstanding specific capacities (1165 mAh g −1 , 80.9% retention at 0.1 A g −1 , and 791 mAh g −1 even at 3 A g −1 ), excellent rate capabilities, and stable cycling lifetimes (1252 mAh g −1 , 80.9% retention after 100 cycles at 0.2 A g −1 ). This design strategy will provide fascinating HEO electrodes that cannot be prepared with conventional fabrication methods.

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精细调节燃烧合成的锂离子电池阳极高熵氧化物的合理工程
摘要:高熵氧化物(HEOs)具有良好的循环稳定性和倍率性能,是锂离子电池(LIBs)极有前途的转换型负极材料。然而,传统的合成和筛选过程耗时且复杂,并且需要对单个元素进行相分离和界面分离。在此,我们报告了一种合理的筛选策略,使用一步燃烧合成的具有不同燃料-氧化剂比(φ)的精确可调谐HEOs来筛选锂离子电池阳极。稍稀薄的燃料混合物(φ-0.95)为最佳的HEO合成提供了合适的温度和非还原气氛。这提供了高结晶度、完全均匀的元素分布和足够的孔隙结构,没有选择性沉淀,而较低或较高的燃料与氧化剂比会导致过度多孔形态或元素偏析。φ-0.95的heo基阳极具有出色的比容量(1165 mAh g−1,在0.1 A g−1下保持80.9%,在3 A g−1下保持791 mAh g−1),优异的倍率能力和稳定的循环寿命(1252 mAh g−1,在0.2 A g−1下循环100次后保持80.9%)。这种设计策略将提供传统制造方法无法制备的令人着迷的HEO电极。
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来源期刊
Npg Asia Materials
Npg Asia Materials MATERIALS SCIENCE, MULTIDISCIPLINARY-
CiteScore
15.40
自引率
1.00%
发文量
87
审稿时长
2 months
期刊介绍: NPG Asia Materials is an open access, international journal that publishes peer-reviewed review and primary research articles in the field of materials sciences. The journal has a global outlook and reach, with a base in the Asia-Pacific region to reflect the significant and growing output of materials research from this area. The target audience for NPG Asia Materials is scientists and researchers involved in materials research, covering a wide range of disciplines including physical and chemical sciences, biotechnology, and nanotechnology. The journal particularly welcomes high-quality articles from rapidly advancing areas that bridge the gap between materials science and engineering, as well as the classical disciplines of physics, chemistry, and biology. NPG Asia Materials is abstracted/indexed in Journal Citation Reports/Science Edition Web of Knowledge, Google Scholar, Chemical Abstract Services, Scopus, Ulrichsweb (ProQuest), and Scirus.
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