三元层状材料结构调控及性能研究进展

doi:10.15541/jim20230123

无机材料学报 ›› 2023, Vol. 38 ›› Issue (8): 845-884.DOI: 10.15541/jim20230123 CSTR: 32189.14.10.15541/jim20230123

所属专题：【材料计算】计算材料(202409)；【信息功能】MAX层状材料、MXene及其他二维材料(202409)；【结构材料】核用陶瓷（202409）

• 特邀综述 • 下一篇

三元层状材料结构调控及性能研究进展

丁浩明¹^,²^,³(), 李勉¹^,³, 李友兵¹^,³, 陈科¹^,³, 肖昱琨¹^,³, 周洁⁴, 陶泉争⁴, 尹航⁵, 柏跃磊⁵, 张毕堃⁶, 孙志梅⁶, 王俊杰⁷, 张一鸣¹^,³, 黄振莺⁸, 张培根⁹, 孙正明⁹, 韩美康¹⁰, 赵双¹¹, 王晨旭¹¹, 黄庆¹^,³()

1.中国科学院宁波材料技术与工程研究所, 先进能源材料工程实验室, 宁波 315201
2.中国科学院大学, 北京 101408
3.宁波杭州湾新材料研究院, 宁波 315336
4.林雪平大学物理、化学和生物学系, 瑞典林雪平 SE-58183
5.哈尔滨工业大学特种环境复合材料技术国防科技重点实验室/复合材料与结构研究所, 哈尔滨 150001
6.北京航空航天大学材料科学与工程学院, 北京 100191
7.西北工业大学材料学院, 西安 710072
8.北京交通大学机械与电子控制工程学院, 北京 100044
9.东南大学材料科学与工程学院, 南京 211189
10.复旦大学光电研究院和上海市智能光电与感知前沿科学研究基地, 上海 200433
11.北京大学核物理与核技术国家重点实验室, 北京 100871

收稿日期:2023-03-09 修回日期:2023-04-19 出版日期:2023-08-20 网络出版日期:2023-05-04
通讯作者: 黄庆, 研究员. E-mail: huangqing@nimte.ac.cn
作者简介:丁浩明(1994-), 男, 博士研究生. E-mail: dinghaoming@nimte.ac.cn
基金资助:
浙江省重点研发计划(2022C01236);国家自然科学基金(12275009);国家自然科学基金(51972080);国家自然科学基金(52171033);国家自然科学基金(52272307);国家自然科学基金(21671195);国家自然科学基金(52172254);国家自然科学基金(U2004212);国家自然科学基金(52202325);上海市浦江人才计划(22PJ1400800);浙江省领军型创新创业团队(2019R01003);浙江省万人杰出项目(2022R51007)

Progress in Structural Tailoring and Properties of Ternary Layered Ceramics

DING Haoming¹^,²^,³(), LI Mian¹^,³, LI Youbing¹^,³, CHEN Ke¹^,³, XIAO Yukun¹^,³, ZHOU Jie⁴, TAO Quanzheng⁴, Johanna Rosen⁴, YIN Hang⁵, BAI Yuelei⁵, ZHANG Bikun⁶, SUN Zhimei⁶, WANG Junjie⁷, ZHANG Yiming¹^,³, HUANG Zhenying⁸, ZHANG Peigen⁹, SUN Zhengming⁹, HAN Meikang¹⁰, ZHAO Shuang¹¹, WANG Chenxu¹¹, HUANG Qing¹^,³()

1. Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo 315201, China
2. University of Chinese Academy of Sciences, Beijing 101408, China
3. Qianwan Institute of CHiTECH, Ningbo 315336, China
4. Department of Physics, Chemistry and Biology (IFM), Linköping University, Linköping SE-58183, Sweden
5. National Key Laboratory of Science and Technology on Advanced Composites in Special Environments and Center for Composite Materials and Structures, Harbin Institute of Technology, Harbin 150001, China
6. School of Materials Science and Engineering, Beihang University, Beijing 100191, China
7. School of Materials Science and Engineering, Northwestern Polytechnic University, Xi’an 710072, China
8. School of Mechanical, Electronic and Control Engineering, Beijing Jiaotong University, Beijing 100044, China
9. School of Materials Science and Engineering, Southeast University, Nanjing 211189, China
10. Institute of Optoelectronics and Shanghai Frontiers Science Research Base of Intelligent Optoelectronics and Perception, Fudan University, Shanghai 200433, China
11. State Key Laboratory of Nuclear Physics and Technology, Peking University, Beijing 100871, China

Received:2023-03-09 Revised:2023-04-19 Published:2023-08-20 Online:2023-05-04
Contact: HUANG Qing, professor. E-mail: huangqing@nimte.ac.cn
About author:DING Haoming (1994-), male, PhD candidate. E-mail: dinghaoming@nimte.ac.cn
Supported by:
Key R&D Projects of Zhejiang Province(2022C01236);National Natural Science Foundation of China(12275009);National Natural Science Foundation of China(51972080);National Natural Science Foundation of China(52171033);National Natural Science Foundation of China(52272307);National Natural Science Foundation of China(21671195);National Natural Science Foundation of China(52172254);National Natural Science Foundation of China(U2004212);National Natural Science Foundation of China(52202325);Shanghai Pujiang Program(22PJ1400800);Leading Innovative and Entrepreneur Team Introduction Program of Zhejiang(2019R01003);Ten-Thousand Talents Plan of Zhejiang Province(2022R51007)

摘要/Abstract

摘要：

MAX/MAB相是一类非范德华三元层状材料, 具有丰富的元素组成和晶体结构, 兼具陶瓷和金属的物理性质, 在高温、强腐蚀、辐照等极端环境中极具应用潜力。近年来, 由MAX/MAB相衍生的二维(2D)材料(MXene和MBene)在材料物理与材料化学领域引起了广泛兴趣, 已经成为继石墨烯和过渡金属硫族化合物之后最受关注的二维范德华材料。MAX/MAB相材料结构调控不仅对这类非范德华层状材料本征性能产生重要影响, 而且对其衍生的二维范德华材料结构功能特性研究也具有重要价值。本文归纳和总结了MAX/MAB相层状材料在结构调控、理论计算和应用基础研究等方向的最新科研进展, 并展望了该类层状材料未来发展方向。

关键词: MAX相, MAB相, 二维过渡金属碳氮化物, 结构调控, 理论计算, 综述

Abstract:

MAX/MAB phases are a series of non-van der Waals ternary layered ceramic materials with a hexagonal structure, rich in elemental composition and crystal structure, and embody physical properties of both ceramics and metals. They exhibit great potential for applications in extreme environments such as high temperature, strong corrosion, and irradiation. In recent years, two-dimensional (2D) materials derived from the MAX/MAB phase (MXene and MBene) have attracted enormous interest in the fields of materials physics and materials chemistry and become a new 2D van der Waals material after graphene and transition metal dichalcogenides. Therefore, structural modulation of MAX/MAB phase materials is essential for understanding the intrinsic properties of this broad class of layered ceramics and for investigating the functional properties of their derived structures. In this paper, we summarize new developments in MAX/MAB phases in recent years in terms of structural modulation, theoretical calculation, and fundamental application research and provide an outlook on the key challenges and prospects for the future development of these layered materials.

Key words: MAX phase, MAB phase, MXene, structural modulation, theoretical calculation, review

中图分类号:

TB383

丁浩明, 李勉, 李友兵, 陈科, 肖昱琨, 周洁, 陶泉争, 尹航, 柏跃磊, 张毕堃, 孙志梅, 王俊杰, 张一鸣, 黄振莺, 张培根, 孙正明, 韩美康, 赵双, 王晨旭, 黄庆. 三元层状材料结构调控及性能研究进展[J]. 无机材料学报, 2023, 38(8): 845-884.

DING Haoming, LI Mian, LI Youbing, CHEN Ke, XIAO Yukun, ZHOU Jie, TAO Quanzheng, Johanna Rosen, YIN Hang, BAI Yuelei, ZHANG Bikun, SUN Zhimei, WANG Junjie, ZHANG Yiming, HUANG Zhenying, ZHANG Peigen, SUN Zhengming, HAN Meikang, ZHAO Shuang, WANG Chenxu, HUANG Qing. Progress in Structural Tailoring and Properties of Ternary Layered Ceramics[J]. Journal of Inorganic Materials, 2023, 38(8): 845-884.

图/表 28

图1 三元层状材料的发现时间轴(非完全统计)

Fig. 1 Non-exhaustive chronicle of ternary layered materials In 1960, Ti2SC was synthesized[40]; From 1960 to 1966, a large number of ternary layered carbides/nitrides (H-phases) with an M2AX formula (211 type) were synthesized[41-42]; From 1967 to 1968, Ti3SiC2 (312 type) and a set of 312 and 211 types H-phases were produced[41,43-44]; In 1969, a typical ternary layered boride Fe2AlB2 was synthesized[7]; In 1994, Ti3AlC2 was discovered[45]; In 1996, the high purity Ti3SiC2 was produced and exhibited excellent properties, thus triggering the research upsurge to these materials[46]; In 2000, Barsoum[1] renamed H-phases as Mn+1AXn phases, short for MAX phases; In 2011, the first MXene Ti3C2Tx was discovered[28]; In 2013, the discovery of magnetocaloric effect of Fe2AlB2 raised research upsurge on ternary layered borides[9]. Also, Lu2SnC was synthesized and found to be superconducting[47]; In 2014, an o-MAX (Cr2/3Ti1/3)3AlC2 was synthesized[48]; In 2015, ternary layered borides were named as MAB phases. In addition, the first Zr-based MAX phase was discovered[10,49]; In 2017, an i-MAX (Mo2/3Sc1/3)2AlC and two noble-metal MAX phases Ti3AuC2 and Ti3IrC2 were synthesized[22,50]; In 2019, a series of MAX phases containing Cu and Zn, and a hexagonal MAB phase Ti2InB2, as well as Nb2SBxC1-x (x=0-1) were synthesized[24⇓-26,51,52]; In 2020, two i-MAB phases (Mo2/3Sc1/3)2AlB2 and (Mo2/3Y1/3)2AlB2, as well as a variety of MAX phases containing Fe, Co, Ni, and Mn were synthesized[16,19]; In 2021, MAX phases having Se atoms at the A-site were produced[53]; In 2022, o-MAX phase Ti4MoSiB2, the first MBene, and Zr2Se(B1-xSex) were synthesized[20,54-55]; In 2023, a chemical scissor-mediated structural editing strategy was proposed, which extremely expands the diversity of MAX phases and MXene[56]

图1 三元层状材料的发现时间轴(非完全统计)

图2 MAX相的元素及结构调控

Fig. 2 Atomic and structural regulation of MAX phases (a) Schematic illustration of Ti3SiC2 film covered by Au film on the SiC substrate[22]; (b) STEM image of Ti3SiC2 and its corresponding atomic model[22]; (c) Schematic illustration of preparing novel MAX phases and MXene based on a Lewis-acidic-molten-salt route[24]; (d) STEM image of Ti3ZnC2 and its corresponding atomic model[24]; (e) STEM image of Ti3C2Cl2 and its corresponding atomic model[24]; (f) Schematic illustration of the conversion from non-van der Waals solids to 2D transition-metal chalcogenides[57]

图3 不同的MXene的制备方法

Fig. 3 Different methods for the synthesis of MXene (a) Schematic illustration of preparing MXene using HF solution as etchant[28]; (b) SEM image of Ti3C2Tx prepared by HF solution, showing the typical accordion-like morpholorgy of MXene particle[28]; (c) STEM image of Ti3C2Cl2 prepared by Lewis-acidic-molten-salt route, and its corresponding atomic model[24]; (d) Schematic illustration of preparing Ti3C2Tx MXene via a reaction between Ti3SiC2 and CuCl2; (e) Redox potential/Gibbs free energy between Lewis acid cations and A-site atoms in molten salts[30]; (f) Schematic illustration of the electrochemistry etching strategy for the preparation of MXene in molten salt[72]

图4 “化学剪刀”辅助的MAX相和MXene的结构编辑

Fig. 4 Structural editing of MAX phases and MXene aided by chemical scissors (a) Schematic illustration of chemical intercalation strategy aided by chemical scissors[56]; (b) Periodic table showing elements involved in the formation of MAX phases and MXenes. Light blue: M elements; Brown: A elements; Black: X elements; Green: ligand (T) elements; Circled: elements studied in the present work[56]

图5 新型硫属MAX相的晶体结构及其典型的物理性能

Fig. 5 Crystal structure and physical properties of novel chalcogenide MAX phases (a-d) First synthesized Se-containing MAX phase, Zr2SeC[53]; (e, f) First synthesized Te-containing MAX phase, Hf2TeB[93]; (h-j) First synthesized MAX phase with chalcogen at X site, Zr2Se(B1-xSex) with x at 0 (h), 0.60 (i), and 0.97 (j), respectively[20]

图6 单晶MAX相的制备

Fig. 6 Preparation of single crystal MAX phases (a) Crystal structure of V4AlC3-x[106]; (b) SEM image of single MAX phase V4AlC3-x[106]; (c) Schematic of the experimental set-up used for high temperature solution growth[107]; (d) Photograph of part of the crucible cut after growth and dipping into dilute HCl, the Cr2AlC platelets are coalescing due to an unusually long growth time[107]

图7 Cr2AlC单晶的热容和各向异性的热导率[110]

Fig. 7 Heat capacity and anisotropic thermal conductivity in Cr2AlC single crystals at high temperatures[110] (a) Atomic structure model of Cr2AlC; (b) Schematic of the in-plane resistivity measurements in Cr2AlC using a four-probe configuration with equidistant and parallel pads; (c) Temperature-dependence measurements of the in-plane resistivity for Cr2AlC single crystals (black line); (d) Predicted out-of-plane resistivity (orange line); (e) Heat capacity measurements of Cr2AlC single crystals measured experimentally (blue dots); (f) Measured in-plane (κ∥) and out-of-plane (κ⊥) thermal conductivities using various techniques

图8 i-MAX相及其衍生的二维结构i-MXene[50]

Fig. 8 i-MAX phases and its derived two-dimensional product of i-MXene[50] (a-c) i-MAX with in-plane chemical order, viewed from [100], [010] and [110] zone axes, respectively; (d) Schematic of the conversion from i-MAX to i-MXene; (e) Low-magnification STEM image of single flake of Mo1.33C i-MXene; (f) Higher magnification STEM image with the FFT result of Mo1.33C i-MXene; (g) Atomically resolved STEM image of Mo1.33C i-MXene; (h) Atomic structure model corresponding to (g)

表1 实验上已经合成的i-MAX相

Table 1 List of synthesized i-MAX phases

M′_4/3	M″_2/3	A	X	Ref.
Mo_4/3	Sc_2/3/Y_2/3	Al	C	[50,118]
W_4/3	Sc_2/3/Y_2/3	Al	C	[123]
Mn_4/3	Sc_2/3	Ga	C	[124]
Cr_4/3	Sc_2/3/Y_2/3/Zr_2/3	Al	C	[125-126]
Cr_4/3	Sc_2/3	Ga	C	[16,124]
V_4/3	Sc_2/3/Zr_2/3	Al	C	[118,127]
Mo_4/3	Sc_2/3/Y_2/3	Ga	C	[128]
Mo_4/3	Ce_2/3/Pr_2/3/Nd_2/3/Sm_2/3/Gd_2/3/Tb_2/3/Dy_2/3/Ho_2/3/Er_2/3/Tm_2/3/Lu_2/3	Al	C	[119]
Mo_4/3	Gd_2/3/Tb_2/3/Dy_2/3/Ho_2/3/Er_2/3/Tm_2/3/Yb_2/3/Lu_2/3	Ga	C	[120]
W_4/3	Gd_2/3/Tb_2/3/Dy_2/3/Ho_2/3/Er_2/3/Tm_2/3/Lu_2/3	Al	C	[121]
Cr_4/3	Gd_2/3/Tb_2/3/Dy_2/3/Ho_2/3/Er_2/3/Tm_2/3/Lu_2/3	Al	C	[122]

图9 MAB相、i-MAB相和o-MAB相

Fig. 9 MAB phases, i-MAB phases and o-MAB phases (a) SEM image of layered Ti2InB2; (b) STEM image of Ti2InB2 along the direction of [001] and corresponding FFT result in the inset image; (c) SEM image of 2D-TiB and its corresponding EDS semi-quantitative resultin inset table[52]; (d-f) STEM images of i-MAB phase (Mo2/3A1/3)2AlB2 and corresponding atomic model along the direction [0001], [$1\bar{1}00$] and [$11\bar{2}0$], respectively, and their corresponding FFT images[55]; (g-i) STEM images of o-MAB phase Ti4MoSiB2 and corresponding atomic model along the direction [100], [210] and [110], respectivly, and their corresponding FFT images[54]

图10 通过化学刻蚀得到的MAB相衍生的二维产物

Fig. 10 Two-dimensional products derived from MAB phases through chemical etching (a) Schematic of chemical etching i-MAB phase to prepare two-dimensional derivative[55]; (b) XRD patterns of prestine i-MAX (Mo2/3Y1/3)2AlB2, etched product Mo4/3B2-xTz, TBAOH intercalation product, and delamination film with SEM image (inset) showing the cross-sectional morphology of Mo4/3B2-xTz film [55]; (c) STEM image of monolayer Mo4/3B2-xTz and its FFT image (inset) [55]; (d) XRD patterns of o-MAX Ti4MoSiB2, product etched by ZnCl2 and two-dimensional TiOxCly after delamination and filtering with SEM image (inset) of cross-sectional morphology of a TiOxCly film[54]

图11 实验测量的单边缺口梁断裂韧性随部分典型三元层状化合物(MAX和MAB相)的最弱与最强化学键刚度比kmin/kmax的变化[138]

Fig. 11 Experimentally measured unilateral notched beam fracture toughness as a function of the weakest to strongest chemical bond stiffness ratio kmin/kmax for some typical ternary layered compounds (MAX and MAB phases)[138]

表2 理论预测可稳定存在的MAB相种类

Table 2 Stable MAB phases by theoretical prediction

MAB phase	M type	A type	Ref.	MAB phase	M type	A type	Ref.
Orthorhombic M₂A₂B₂	Ti	Al	[160-161]	Orthorhombic M₃AB₄	Sc	Al	[160-161]
	Hf				Ti
	V				Zr
	Nb				Hf
	Ta				V
	Tc				Nb
	Cr				Ta
	Mn				Mo
Orthorhombic M₂AB₂	Sc	Al	[160-161]		W
	Ti				Mn
	Zr				Fe
	Hf			Orthorhombic M₄AB₆	Sc	Al	[160-161]
	V				Ti
	Nb				Zr
	W				Hf
	Tc				V
	Rh				Nb
	Ni				Ta
	Co				Mo
Orthorhombic M₃A₂B₂	Sc	Al	[160-161]	Hexagonal M₂AB₂	Ti	Sn	[52]
	Ti				Hf	In	[162]
	Zr				Hf	Sn
	Hf				Zr	In
	Cr					Pb
	Mn					Tl
	Tc			Hexagonal M₃AB₄	Hf	In	[162]
	Fe					Sn
	Ni					P
					Zr	Cd
					Zr	Pb

图12 MAB相的理论计算

Fig. 12 Theoretical calculation of MAB phases (a) Structures of orthorhombic and hexagonal MAB phases[163]; (b) Bonding energy of M2AlB2-type orthorhombic MAB and M2AlC-type MAX phases; (c) Simulated exfoliation process of orthorhombic M2AlB2 using HF, where the red, green, black, cyan, and pink balls represent Mo, B, Al, F, and H atoms, respectively[146]

表3 部分MAB相的理论体积模量(B)、剪切模量(G)、杨氏模量(E)和泊松比(ν)

Table 3 Theoretical mechanical properties of several MAB-phases, including bulk modulus (B), shear modulus (G), Young’s modulus (E), and Poisson ratio (ν)

MAB phase	B/GPa	G/GPa	E/GPa	¯ν/GPa	Ref.
Mn₂AlB₂	239	169	411	0.21	[160]
Fe₂AlB₂	209	133	329	0.24
Co₂AlB₂	216	92	242	0.31
TiAlB	145	116	274	0.18
VAlB	173	133	317	0.19
NbAlB	180	130	315	0.21
TaAlB	192	138	333	0.21
CrAlB	189	140	338	0.20
MnAlB	167	101	252	0.25
TcAlB	220	114	292	0.28
Sc₂AlB₂	238	142	356	0.25
Ti₂AlB₂	170	150	347	0.16
Zr₂AlB₂	152	112	270	0.20
Hf₂AlB₂	168	132	314	0.19
V₂AlB₂	195	129	317	0.23
Nb₂AlB₂	199	110	279	0.27
Cr₂AlB₂	229	177	422	0.19
Mo₂AlB₂	238	142	356	0.25
W₂AlB₂	262	139	354	0.28
Tc₂AlB₂	260	132	339	0.28
Ni₂AlB₂	200	91	237	0.30
MoAlB	213	146	357	0.22	[164]
WAlB	232	146	362	0.24	[164]
Mn₂AlB₂	222	161	388	0.21	[165]
Fe₂AlB₂	210	132	329	0.24	[165]
Co₂AlB₂	241	101	266	0.31	[166]
Zr₃CdB₄	—	82	202	0.37	[167]
Hf₃PB₄	—	180	407	0.19	[168]

图13 MBene的种类及结构示意图[163]

Fig. 13 Members and atomic structures of all reported orth- and hex-MBenes[163]

图14 三元MAX相的发现

Fig. 14 Discovery of ternary MAX phases (a) Calculation-based approach to discovery of novel ternary phases Ti2InB2[52]; (b) High-throughput prediction of MAB phases[162]; (c) Crystal structures for the stable Nb2AB2 and Nb2AB (A: P or S)[183]

图15 四元MAB相的理论预测

Fig. 15 Theoretical study of quaternary MAB phases (a) Crystal structure of Cr3AlB4, ordered M2M'AlB4, and disordered M2M'AlB4[186]; (b) Prediction and synthesis of i-MAB phases Mo4/3Sc2/3AlB2 and Mo4/3Y2/3AlB2[16]; (c) Elemental mapping involved in this computational work; (d) Schematic illustration of the evolution of structure and electronic structure of h-MAB during the introduction of the fourth element M″[187]

图16 选取特征量为电子浓度和尺寸因素所绘制的结构映射图[36]

Fig. 16 Structure mapping based on the selected characteristic quantities of electron concentration and atomic sizes[36]

图17 MAX增强金属基复合材料

Fig. 17 MAX-reinforced metal matrix composites (a-b) Fracture morphology of MAX in Mg matrix composites undergoing microplastic deformation[213]; (c) MAX/Cu matrix composite MCC pantograph slide plate[215]; (d, e) Transformation of MAX to TiCx and Cr3C2 in Ni matrix composites and morphology of in situ authentic γ'[224]; (f) Morphology of the MAX transformation to TiCx and Ti5Si3 in Ti matrix composites[225]

图18 在空气与真空中交替生长的Sn晶须的SEM图片[259]

Fig. 18 SEM images of a Sn whisker alternately cultivated in air and vacuum[259] (a-e) For once, twice, 3 times, 4 times, and 5 times, respectively with faceted segments formed in vacuum being pointed by white arrows; (f-h) High magnification SEM images of the faceted segments indicated by arrow A in (b), arrow C in (c), and arrow C in (d), respectively

图19 Zr2InC样品端口及其表面生长的In晶须的SEM照片[243]

Fig. 19 SEM images of fractured Zr2InC surface and an In whisker[243] (a) Fractured Zr2InC surface showing In at grain boundaries (this surface being covered with thin In film); (b) An In whisker whose cross-sectional shape is determined by grain boundary geometry at the In/Zr2InC interface

图20 Sn晶须/Ti2SnC界面的微观结构[266]

Fig. 20 Microstructure of Sn whiskers/Ti2SnC interface[266] (a) TEM image of the interface; (b) Magnified view of the white rectangle area in (a); (c, d) HRTEM images of the interface

图21 不同MXene薄膜的电导率(a)及其电磁屏蔽效能与电导率间的关系(b)[282]

Fig. 21 (a) Electrical conductivity of different MXene films and (b) conductivity-dependent electromagnetic interference shielding effectiveness of different MXenes[282]

图22 辐照环境下MAX相材料中的缺陷产生和微观结构转变

Fig. 22 Defect generation and microstructural transformation in MAX phase materials under irradiation (a) STEM HAADF (high-angle annular dark-field) image along [11¯20] of Ti3AlC2 irradiated with 1 MeV Au ions, showing direct evidence of cation antisite defects. The white arrows indicate the initial Al layers, whose image contrast is altered when compared with the initial hexagonal structure[295]; (b, c) Contrast profiles along line 1 and line 2 in (a), respectively, which directly show the variation of contrast arising from the formation of TiAl-AlTi antisite defects produced by ion irradiation[295]; (d) TEM image of Ti3(Si,Al)C2 being irradiated at 0.2 dpa indicating a cluster of point defects (black dots)[296]; (e-g) Phase transformation (hcp to γ to fcc solid solution) processes with chemical disorder induced by ion irradiation in a typical MAX phase, Ti3AlC2 (hcp: hexagonal close packing; fcc: face-centered cubic)[295]

图23 MAX相的辐照温度效应

Fig. 23 MAX phase irradiation temperature effect (a) Ti3AlC2 is completely recovered to initial phase (a dose of 2×1016 cm-2) or partially recovered to initial phase and γ-Ti3AlC2 phase (a dose of 4×1016 cm-2) after irradiation with 1 MeV Au ions and then annealed at 800 ℃ for 1 h[303]; (b) Cr2AlC films showing completely amorphous after irradiation with 320 keV Xe ions up to 3.3 dpa at 300 K, but not completely amorphized after irradiation up to 90 dpa at 623 K[306]

图24 高熵MAX相的辐照相变及非晶化[302]

Fig. 24 Phase transformation and amorphization caused by irradiation of MAX phases[302] (a) Schematic of atomic structure models of Ti2SnC and (TiVNbZrHf)2SnC; (b) In-situ selective area electron diffraction (SAED) micrographs of Ti2SnC and five-component (TiVNbZrHf)2SnC recorded during 800 keV Kr2+ irradiation, showing different phase transformation process and amorphization resistance; (c) M-Sn antisite defect formation energies calculated via DFT in the corresponding single-component M2SnC and the five-component (TiVNbZrHf)2SnC supercell

图25 (Mo2/3RE1/3)2GaC i-MAX相沿 (a) [100]和 (b) [010] 方向的扫描透射电镜(STEM)图像[120]

Fig. 25 STEM micrographs of (Mo2/3RE1/3)2GaC i-MAX phase along (a) [100] and (b) [010] zone axis[120]

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三元层状材料结构调控及性能研究进展

Progress in Structural Tailoring and Properties of Ternary Layered Ceramics

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