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探索钙钛矿型KVTiO（0.25≤≤2）作为钾离子电池（KIBs）的电极材料。

Exploring Hollandite-Type KVTiO (0.25 ≤ ≤ 2) as Electrode Materials in Potassium-Ion Batteries (KIBs).

作者信息

Nieto-Simón Juan Andrés, González-Barrios Marta María, Gómez-Herrero Adrián, Fernández-Díaz María Teresa, Prado-Gonjal Jesús, Castillo-Martínez Elizabeth

机构信息

Departamento de Química Inorgánica, Facultad de Ciencias Químicas, Universidad Complutense de Madrid, Madrid E-28040, Spain.

ICTS Centro Nacional de Microscopía Electrónica, Universidad Complutense de Madrid, Madrid E-28040, Spain.

出版信息

Inorg Chem. 2025 May 5;64(17):8578-8590. doi: 10.1021/acs.inorgchem.4c05579. Epub 2025 Apr 22.

DOI:10.1021/acs.inorgchem.4c05579
PMID:40261682
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12123605/
Abstract

Hollandite-type oxides, KVTiO, = 0.25, 0.5, 0.75, 1, 1.25, 1.5, and 2, are synthesized via the citrate method and evaluated as potential electrode materials for potassium-ion batteries (KIBs). Neutron powder diffraction (NPD) confirms an undistorted 4/ structure, uniform K content (1.4 ≤ ≤ 1.6), and high potassium isotropic displacement parameter (B). This decreases significantly for ≥ 1, correlating with tunnel narrowing and vanadium's stronger polarization. Transmission electron microscopy (TEM) techniques, including selected area electron diffraction (SAED), annular bright field (ABF), and high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) identify superstructure reflections assigned to potassium/vacancy short-range order along the axis with disorder between tunnels. Magnetic studies reveal paramagnetic behavior down to 2 K, with antiferromagnetic interactions at low temperature except for = 0.25 composition, which exhibits ferromagnetic interactions. The experimental magnetic moment suggests a low Ti content, with notable deviations at = 1.25. The electrochemical performance is assessed via galvanostatic cycling using 2.5 M potassium bis(fluorosulfonyl)imide (KFSI) in triethyl phosphate (TEP) as electrolyte. At a rate of C/10, 2 K are reversibly de/inserted per formula unit, comparable to KTiO. At C/5, KVTiO demonstrates a reversible de/insertion of 1 K/f.u., highlighting its potential for rechargeable KIBs.

摘要

通过柠檬酸盐法合成了K(_x)V(_2)O(_5)（(x) = 0.25、0.5、0.75、1、1.25、1.5和2）型的钙钛矿型氧化物，并将其评估为钾离子电池（KIBs）的潜在电极材料。中子粉末衍射（NPD）证实了其具有未畸变的4H结构、均匀的K含量（1.4 ≤ (x) ≤ 1.6）以及较高的钾各向同性位移参数（B）。当(x) ≥ 1时，该参数显著降低，这与隧道变窄以及钒更强的极化作用相关。包括选区电子衍射（SAED）、环形明场（ABF）和高角度环形暗场扫描透射电子显微镜（HAADF-STEM）在内的透射电子显微镜（TEM）技术，识别出了沿c轴的钾/空位短程有序的超结构反射，且隧道之间存在无序。磁性研究表明，除了(x) = 0.25组成表现出铁磁相互作用外，在低至2 K的温度下均呈现顺磁行为，在低温下存在反铁磁相互作用。实验磁矩表明Ti含量较低，在(x) = 1.25时存在显著偏差。使用2.5 M双（氟磺酰）亚胺钾（KFSI）在磷酸三乙酯（TEP）中作为电解质，通过恒电流循环评估其电化学性能。在C/10的速率下，每个化学式单元可逆地脱嵌2个K，与K(_2)TiO(3)相当。在C/5时，K({1.25})V(_2)O(_5)展示了1个K/f.u.的可逆脱嵌，突出了其在可充电KIBs中的潜力。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/aed2/12123605/4713eb625b16/ic4c05579_0009.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/aed2/12123605/137247992d7c/ic4c05579_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/aed2/12123605/5fbb3e7b1784/ic4c05579_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/aed2/12123605/42c4ac814d6b/ic4c05579_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/aed2/12123605/b5760d6f5d5b/ic4c05579_0007.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/aed2/12123605/4713eb625b16/ic4c05579_0009.jpg

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