氮空位调控晶格畸变度强化(NbMoTaW)Nx薄膜的力学性质和耐磨损性

doi:10.15541/jim20230564

无机材料学报 ›› 2024, Vol. 39 ›› Issue (6): 715-725.DOI: 10.15541/jim20230564 CSTR: 32189.14.10.15541/jim20230564

所属专题：【结构材料】高熵陶瓷(202409)

氮空位调控晶格畸变度强化(NbMoTaW)N_x薄膜的力学性质和耐磨损性

张睿(), 张侃(), 袁梦雅, 谷鑫磊, 郑伟涛

吉林大学材料科学与工程学院, 超硬材料国家重点实验室, 长春 130012

收稿日期:2023-12-07 修回日期:2024-02-26 出版日期:2024-06-20 网络出版日期:2024-05-24
通讯作者: 张侃, 教授. E-mail: kanzhang@jlu.edu.cn
作者简介:张睿(2001-), 女, 博士研究生. E-mail: zhangr22@mails.jlu.edu.cn
基金资助:
国家自然科学基金(52322206);国家自然科学基金(51972139);国家重点研发计划(2023YFF0716800);吉林省自然科学基金(20210101062JC)

Nitrogen Vacancy Regulated Lattice Distortion on Improvement of (NbMoTaW)N_x Thin Films: Mechanical Properties and Wear Resistance

ZHANG Rui(), ZHANG Kan(), YUAN Mengya, GU Xinlei, ZHENG Weitao

State Key Laboratory of Superhard Materials, College of Materials Science and Engineering, Jilin University, Changchun 130012, China

Received:2023-12-07 Revised:2024-02-26 Published:2024-06-20 Online:2024-05-24
Contact: ZHANG Kan, professor. E-mail: kanzhang@jlu.edu.cn
About author:ZHANG Rui (2001-), female, PhD candidate. E-mail: zhangr22@mails.jlu.edu.cn
Supported by:
National Natural Science Foundation of China(52322206);National Natural Science Foundation of China(51972139);National Key R&D Program of China(2023YFF0716800);Science and Technology Development Program of Jilin Province(20210101062JC)

摘要/Abstract

摘要：

高熵过渡金属氮化物(HENs)具有热稳定性, 抗腐蚀、抗氧化性以及优异的力学性质, 可用作结构部件及运动部件的表面防护薄膜。然而, 受HENs组元多样性的影响, 宽泛可调的金属组分与HENs力学性质之间的映射关系相当复杂。本工作以(NbMoTaW)N_x薄膜为研究对象, 基于磁控溅射方法调节薄膜生长过程中氮气流量, 制备了不同氮含量的(NbMoTaW)N_x (x = 0, 0.59, 0.80, 0.95)薄膜, 研究了(NbMoTaW)N_x薄膜的成分、结构、形貌与性能, 并对薄膜力学性质的主要影响机制进行了系统探究。结果表明, 通过调节氮空位, 实现了对氮原子及金属原子亚晶格畸变度的协同调控, 得益于氮原子和金属原子亚晶格的高畸变度, (NbMoTaW)N_0.80样品具有最高的硬度与最好的耐磨损性能。排除电子结构、残余应力、晶粒尺寸等力学性质影响因素后, 进一步确认了HENs薄膜晶格畸变度与力学性质之间的直接关系。本研究寻找到一条简洁的晶格畸变度调控策略, 为调节、优化氮化物薄膜性能, 进而更好地解决复杂服役环境下防护薄膜的机械损伤问题提供了新的思路。

关键词: 晶格畸变度, 氮空位, 力学性质, 高熵过渡金属氮化物, 耐磨损性

Abstract:

High-entropy transition metal nitrides (HENs) are renowned for their thermal stability, corrosion and oxidation resistance, and exceptional mechanical properties, endowing them suitable for use as surface protection films for structural and moving components. However, mapping relationship between broadly adjustable metal components and mechanical properties of HENs is quite complex due to their diversity of HENs components. Taking (NbMoTaW)N_x thin film as the research object, this study prepared (NbMoTaW)N_x (x = 0, 0.59, 0.80, 0.95) thin films with different nitrogen contents by regulating nitrogen flow velocity during the film growth process based on the magnetron sputtering technique. Following analysis of (NbMoTaW)N_x thin films' composition, structure, morphology, and performance, the primary influence mechanism that govern their mechanical properties were explored. The findings revealed that by manipulating nitrogen vacancy, coordinated regulation over the lattice distortions of the nitrogen and metal sublattices was achieved. Due to high degree of the nitrogen and metal sublattice distortions, the (NbMoTaW)N_0.80 sample demonstrated the highest hardness and best wear resistance performance. After excluding factors such as electronic structure, residual stress, and grain size that affect mechanical properties, a direct relationship between lattice distortions and mechanical properties of HENs films was confirmed. In summary, this research has unearthed a straightforward strategy for controlling the lattice distortions, offering a novel approach to adjust and optimize the performance of nitride films, and ultimately providing a more effective solution to address the mechanical damage issues that arise in the context of complex service environments.

Key words: lattice distortion, nitrogen vacancy, mechanical property, high-entropy transition metal nitride, wear resistance

中图分类号:

TQ174

张睿, 张侃, 袁梦雅, 谷鑫磊, 郑伟涛. 氮空位调控晶格畸变度强化(NbMoTaW)N_x薄膜的力学性质和耐磨损性[J]. 无机材料学报, 2024, 39(6): 715-725.

ZHANG Rui, ZHANG Kan, YUAN Mengya, GU Xinlei, ZHENG Weitao. Nitrogen Vacancy Regulated Lattice Distortion on Improvement of (NbMoTaW)N_x Thin Films: Mechanical Properties and Wear Resistance[J]. Journal of Inorganic Materials, 2024, 39(6): 715-725.

图/表 9

图1 (a) NbMoTaW, (b) (NbMoTaW)N0.59, (c) (NbMoTaW)N0.80和(d) (NbMoTaW)N0.95薄膜表面的SEM照片及相应的EDS元素分布

Fig. 1 SEM images and corresponding EDS mappings of the surfaces for (a) NbMoTaW, (b) (NbMoTaW)N0.59, (c) (NbMoTaW)N0.80, and (d) (NbMoTaW)N0.95 thin films

图2 结构变化趋势分析

Fig. 2 Analysis of the structural change trends (a) XRD patterns of (NbMoTaW)Nx thin films on Si(100) substrate; (b) Lattice constants of (NbMoTaW)Nx thin films obtained from XRD patterns and DFT calculations, and grain sizes of (NbMoTaW)Nx thin films calculated from XRD patterns; (c) HRTEM image and SAED pattern of (NbMoTaW)N0.80 sample

图3 (NbMoTaW)Nx(x = 0.59, 0.81, 1.00)的键长分布

Fig. 3 Bond-length distributions of (NbMoTaW)Nx (x = 0.59, 0.81, 1.00) (a) Schematic representation of the crystal structure after structural optimization; (b1-b3) 1NN atomic distance distribution of Me-N in the supercell and Gaussian fitting curves; (c1-c3) 1NN atomic distance distribution of Me-Me in the supercell and Gaussian fitting curves

图4 x = (a) 1.00, (b) 0.81, (c) 0.59时, (NbMoTaW)Nx化合物(001)晶面的电荷密度分布示意图

Fig. 4 Schematic diagram of charge density on the (001) plane of (NbMoTaW)Nx compounds when x = (a) 1.00, (b) 0.81, (c) 0.59 Black lines indicating atomic lattice, while dashed lines indicating empty lattice points

图5 基于两种方法评估(NbMoTaW)Nx (x = 0.59, 0.81, 1.00)中氮原子亚晶格和金属原子亚晶格畸变度随氮含量x的变化趋势

Fig. 5 Trends in lattice distortions of nitrogen and metal sublattices in (NbMoTaW)Nx (x = 0.59, 0.81, 1.00) as function of nitrogen content x evaluated by two methods (a) Method one: lattice distortions σ obtained from the peak width of Gaussian fitting results as described in Fig. 3; (b) Method two: lattice distortions δ calculated using equations

图6 (NbMoTaW)Nx薄膜的(a) H及E, (b) H/E和H3/E2, 以及(c)相应的残余应力

Fig. 6 (a) H and E values, (b) H/E and H3/E2 ratio values, and (c) corresponding residual stress values for (NbMoTaW)Nx thin films

图7 (a) NbMoTaW, (b) (NbMoTaW)N0.59, (c) (NbMoTaW)N0.80和(d) (NbMoTaW)N0.95薄膜的10000圈磨损轨迹的SEM照片和相应的EDS元素分析

Fig. 7 SEM images of wear tracks at 10000 laps and corresponding EDS mappings for (a) NbMoTaW, (b) (NbMoTaW)N0.59, (c) (NbMoTaW)N0.80, and (d) (NbMoTaW)N0.95 thin films

图8 (a) (NbMoTaW)N0.59, (b) (NbMoTaW)N0.81和(c) (NbMoTaW)N的态密度(DOS)和分波态密度(PDOS), 以及(d)三种薄膜在费米能级的DOS

Fig. 8 Density of states (DOS) and partial density of states (PDOS) for (a) (NbMoTaW)N0.59, (b) (NbMoTaW)N0.81 and (c) (NbMoTaW)N, and (d) DOS at the Fermi level for the three thin films The position of the Fermi surface is indicated by dotted lines; Colorful figures are available on website

图9 (NbMoTaW)Nx (x = 0.59, 0.81, 1.00)的硬度随晶格畸变度变化的趋势

Fig. 9 Trend in hardness of (NbMoTaW)Nx (x = 0.59, 0.81, 1.00) with respect to lattice distortion (a, b) Lattice distortions obtained through the peak width of Gaussian fitting results of (a) nitrogen sublattice (σMe-N) and (b) metal sublattice (σMe-Me); (c, d) Calculated lattice distortions using equations of (c) nitrogen sublattice (δMe-N) and (d) metal sublattice (δMe-Me); Colorful figures are available on website

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氮空位调控晶格畸变度强化(NbMoTaW)N_x薄膜的力学性质和耐磨损性

Nitrogen Vacancy Regulated Lattice Distortion on Improvement of (NbMoTaW)N_x Thin Films: Mechanical Properties and Wear Resistance

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氮空位调控晶格畸变度强化(NbMoTaW)Nx薄膜的力学性质和耐磨损性

Nitrogen Vacancy Regulated Lattice Distortion on Improvement of (NbMoTaW)Nx Thin Films: Mechanical Properties and Wear Resistance

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氮空位调控晶格畸变度强化(NbMoTaW)N_x薄膜的力学性质和耐磨损性

Nitrogen Vacancy Regulated Lattice Distortion on Improvement of (NbMoTaW)N_x Thin Films: Mechanical Properties and Wear Resistance