AI Chat Paper
Note: Please note that the following content is generated by AMiner AI. SciOpen does not take any responsibility related to this content.
{{lang === 'zh_CN' ? '文章概述' : 'Summary'}}
{{lang === 'en_US' ? '中' : 'Eng'}}
Chat more with AI
PDF (17.5 MB)
Collect
Submit Manuscript AI Chat Paper
Show Outline
Outline
Show full outline
Hide outline
Outline
Show full outline
Hide outline
Research Article | Open Access

Lattice evolution, order transformation, and microwave dielectric properties of the Zn1−xLi2xTiO3 (0 ≤ x ≤ 1) system ceramics

Qianbiao Du1Longxiang Jiang1Linzhao Ma1Jianhong Duan1Zeyan Zhou2( )Hao Li1( )
College of Electrical and Information Engineering, Hunan University, Changsha 410082, China
College of Materials Science and Engineering, Hunan University, Changsha 410082, China
Show Author Information

Graphical Abstract

Abstract

Research on doping modification of ZnTiO3 ceramics to enhance microwave dielectric properties has been hindered by poor performance, unclear structure-function mechanisms. To expand the applicability of ZnTiO3 ceramics, this study explores Zn1–xLi2xTiO3 (0 ≤ x ≤ 1) ceramics using a phase engineering strategy. Our findings reveal that the introduction of Li+ into the ZnTiO3 system initiates a multiple phase transition, starting at x = 0.1. Initially, ilmenite ZnTiO3 transforms into a cubic ordered spinel phase (space group P4332). Subsequently, a transition to a disordered spinel phase (space group Fd 3¯m) occurs at x = 0.5, culminating in the formation of a monoclinic rock salt-structured Li2TiO3 phase. Significantly, two sets of ceramics with near-zero temperature coefficients of resonance frequency (τf) were obtained at x = 0.1 and 0.75. Moreover, the quality factor (Q×f) demonstrated a 4.4-fold increase compared to that of ZnTiO3 ceramics at x = 0.25 (105,013 GHz). Additionally, it was observed that the Ti4+ polarization in Zn1−xLi2xTiO3 ceramics was underestimated by 11.3%–13.3%, causing the measured dielectric constant (εr) exceeding the theoretical dielectric constant (εth). The ionic polarizability of Ti4+ was adjusted to stabilize around 3.29 Å3. Evaluation using multiple methods, including Phillips–van Vechten–Levine (P–V–L) theory, Raman vibrational mode analysis, bond valence, bond energy theory, and octahedral distortion, confirms that the Ti–O bonds within the octahedron predominantly affect εr, the increasing lattice energy (U) contributes to the enhancement of Q×f, and the strengthened Li–O bond energy effectively regulates τf.

Electronic Supplementary Material

Download File(s)
JAC0927_ESM.pdf (1.1 MB)

References

[1]

Sebastian MT, Ubic R, Jantunen H. Low-loss dielectric ceramic materials and their properties. Int Mater Rev 2015, 60: 392–412.

[2]

Hill MD, Cruickshank DB, MacFarlane IA. Perspective on ceramic materials for 5G wireless communication systems. Appl Phys Lett 2021, 118: 120501.

[3]

Zhang X, Fang ZX, Yang HY, et al. Lattice evolution, ordering transformation and microwave dielectric properties of rock-salt Li3+ x Mg2−2 x Nb1− x Ti2 x O6 solid-solution system: A newly developed pseudo ternary phase diagram. Acta Mater 2021, 206: 116636.

[4]

Bao J, Zhang YP, Kimura H, et al. Crystal structure, chemical bond characteristics, infrared reflection spectrum, and microwave dielectric properties of Nd2(Zr1− x Ti x )3(MoO4)9 ceramics. J Adv Ceram 2023, 12: 82–92.

[5]

Pan ZW, Yu XD, Wang QC, et al. Stabilization and tunable microwave dielectric properties of the rutile polymorph in α-PbO2-type GaTaO4-based ceramics. J Mater Chem C 2014, 2: 4957–4966.

[6]

Belous A, Ovchar O, Durilin D, et al. High-Q microwave dielectric materials based on the spinel Mg2TiO4. J Am Ceram Soc 2006, 89: 3441–3445.

[7]

Li L, Chen XM, Fan XC. Microwave dielectric characteristics and finite element analysis of MgTiO3–CaTiO3 layered dielectric resonators. J Eur Ceram Soc 2006, 26: 3265–3271.

[8]

Cao M, Li L, Wu SY, et al. Dominant role of ceramic connectivity in microwave dielectric properties of porous ceramics. Acta Mater 2023, 258: 119207.

[9]

Guo HH, Fu MS, Zhou D, et al. Design of a high-efficiency and -gain antenna using novel low-loss, temperature-stable Li2Ti1− x (Cu1/3Nb2/3) x O3 microwave dielectric ceramics. ACS Appl Mater Inter 2021, 13: 912–923.

[10]

Li W, Fang L, Tang Y, et al. Microwave dielectric properties in the Li4+ x Ti5O12 (0 ≤ x ≤ 12) ceramics. J Alloys Compd 2017, 701: 295–300.

[11]

George S, Sebastian MT. Synthesis and microwave dielectric properties of novel temperature stable high Q, Li2ATi3O8 (A = Mg, Zn) ceramics. J Am Ceram Soc 2010, 93: 2164–2166.

[12]

Zhang YD, Zhou D. Pseudo phase diagram and microwave dielectric properties of Li2O–MgO–TiO2 ternary system. J Am Ceram Soc 2016, 99: 3645–3650.

[13]

Nolan NT, Seery MK, Pillai SC. Crystallization and phase-transition characteristics of sol–gel-synthesized zinc titanates. Chem Mater 2011, 23: 1496–1504.

[14]

Yang HY, Li EZ, Yang YF, et al. Co2O3 substitution effects on the structure and microwave dielectric properties of low-firing (Zn0.9Mg0.1)TiO3 ceramics. Ceram Int 2018, 44: 5010–5016.

[15]

Jaramillo-Fierro X, Cuenca G, Ramón J. Comparative study of the effect of doping ZnTiO3 with rare earths (La and Ce) on the adsorption and photodegradation of cyanide in aqueous systems. Int J Mol Sci 2023, 24: 3780.

[16]

Wei SH, Chang SF, Qian J, et al. Selective cocatalyst deposition on ZnTiO3− x N y hollow nanospheres with efficient charge separation for solar-driven overall water splitting. Small 2021, 17: 2100084.

[17]

Mohammadi MR, Fray DJ. Low temperature nanostructured zinc titanate by an aqueous particulate sol-gel route: Optimisation of heat treatment condition based on Zn : Ti molar ratio. J Eur Ceram Soc 2010, 30: 947–961.

[18]

Dulin FH, Rase DE. Phase equilibria in the system ZnO–TiO2. J Am Ceram Soc 1960, 43: 125–131.

[19]

Bartram SF, Slepetys RA. Compound formation and crystal structure in the system ZnO–TiO2. J Am Ceram Soc 1961, 44: 493–499.

[20]

Lei SH, Fan HQ, Ren XH, et al. Novel sintering and band gap engineering of ZnTiO3 ceramics with excellent microwave dielectric properties. J Mater Chem C 2017, 5: 4040–4047.

[21]

Kim HT, Kim Y, Valant M, et al. Titanium incorporation in Zn2TiO4 spinel ceramics. J Am Ceram Soc 2001, 84: 1081–1086.

[22]

Kim HT, Kim SH, Nahm S, et al. Low-temperature sintering and microwave dielectric properties of zinc metatitanate-rutile mixtures using boron. J Am Ceram Soc 1999, 82: 3043–3048.

[23]

Chang YS, Chang YH, Chen IG, et al. Synthesis, formation and characterization of ZnTiO3 ceramics. Ceram Int 2004, 30: 2183–2189.

[24]

Inaguma Y, Aimi A, Shirako Y, et al. High-pressure synthesis, crystal structure, and phase stability relations of a LiNbO3-type polar titanate ZnTiO3 and its reinforced polarity by the second-order Jahn-Teller effect. J Am Chem Soc 2014, 136: 2748–2756.

[25]

Raji S, Masin B, Bhagya KM, Ashok K, Vishnuc S, Sreemoolanadhan H, Prabhakaran K, . Low-temperature sintering of ZnTiO3 using CaV2O6 as a liquid-forming additive for LTCC applications. Ceram Int 2024, 50: 9206–9213.

[26]

Wu SP, Luo JH, Cao SX. Microwave dielectric properties of B2O3–doped ZnTiO3 ceramics made with sol–gel technique. J Alloys Compd 2010, 502: 147–152.

[27]

Li EZ, Zhang P, Duan SX, et al. Low temperature sintering of low-loss ZnTiO3 microwave dielectric ceramics with Zn–B–Si glass. J Alloys Compd 2015, 647: 866–872.

[28]

Zhang JY, Li J, Sun YH, et al. Densification, microwave dielectric properties and rattling effect of LiYbO2 ceramics with low εr and anomalous positive τf. J Eur Ceram Soc 2022, 42: 7455–7460.

[29]

Liu K, Shi L, Wang XY, et al. Li+ enrichment to improve the microwave dielectric properties of Li2ZnTi3O8 ceramics and the relationship between structure and properties. J Eur Ceram Soc 2023, 43: 1483–1491.

[30]

Zuo RZ, Qi H, Qin F, et al. A new Li-based ceramic of Li4MgSn2O7: Synthesis, phase evolution and microwave dielectric properties. J Eur Ceram Soc 2018, 38: 5442–5447.

[31]

Zhang J, Zuo RZ. Effect of ordering on the microwave dielectric properties of spinel-structured (Zn1− x (Li2/3Ti1/3) x )2TiO4 ceramics. J Am Ceram Soc 2016, 99: 3343–3349.

[32]

Du QB, Wen QZ, Jiang LX, et al. A novel low-temperature sintering microwave dielectric ceramic Li4SrCaSi2O8 with low- ϵr and low loss. Ceram Int 2023, 49: 22617–22622.

[33]

Pan HL, Wu HT. Crystal structure, infrared spectra and microwave dielectric properties of new ultra low-loss Li6Mg7Ti3O16 ceramics. Ceram Int 2017, 43: 14484–14487.

[34]

Huang FY, Su H, Li YX, et al. Low-temperature sintering and microwave dielectric properties of CaMg1− x Li2 x Si2O6 ( x = 0−0.3) ceramics. J Adv Ceram 2020, 9: 471–480.

[35]

Du XY, Su H, Zhang HW, et al. Effects of Li-ion substitution on the microwave dielectric properties of low-temperature sintered ceramics with nominal composition Li2 x Mg2− x SiO4. Ceram Int 2018, 44: 2300–2303.

[36]

Xiang HC, Fang L, Fang WS, et al. A novel low-firing microwave dielectric ceramic Li2ZnGe3O8 with cubic spinel structure. J Eur Ceram Soc 2017, 37: 625–629.

[37]

Pang LX, Zhou D. A low-firing microwave dielectric material in Li2O–ZnO–Nb2O5 system. Mater Lett 2010, 64: 2413–2415.

[38]

Pang LX, Zhou D. Microwave dielectric properties of low-firing Li2MO3 (M = Ti, Zr, Sn) ceramics with B2O3–CuO addition. J Am Ceram Soc 2010, 93: 3614–3617.

[39]

Zhou HF, Liu XB, Chen XL, et al. Preparation, phase structure and microwave dielectric properties of CoLi2/3Ti4/3O4 ceramic. Mater Res Bull 2012, 47: 1278–1280.

[40]

Zhou HF, Gong JZ, Wang N, et al. A novel temperature stable microwave dielectric ceramic with low sintering temperature and high quality factor. Ceram Int 2016, 42: 8822–8825.

[41]

Fang WS, Sun YM, Fang L, et al. Temperature stable microwave dielectric ceramics in Li1.33 x Zn2−2 x Ti1+0.67 x O4 (0.75 < x < 1) cubic spinels and their chemical compatibility with silver. J Alloys Compd 2017, 722: 1002–1007.

[42]

Singh SK, Kiran SR, Murthy VRK. Structural, Raman spectroscopic and microwave dielectric studies on spinel Li2Zn(1− x )Ni x Ti3O8 compounds. Mater Chem Phys 2013, 141: 822–827.

[43]

Li B, Tang B, Zhang SR, et al. Low temperature sintering and microwave dielectric properties of (Zn0.65Mg0.35)TiO3 ceramics with BiVO4. J Mater Sci 2010, 45: 6461–6466.

[44]

Wang YJ, Zhang ZY, Li J, et al. Effect of cation occupancy on crystal structure and microwave dielectric characteristics of spinel-structured (1− x)Zn2TiO4− x Li2MgTi3O8 ceramics. Ceram Int 2024, 50: 13500–13507.

[45]

Li YX, Li H, Tang B, et al. Microwave dielectric properties of low-fired Li2ZnTi3O8–TiO2 composite ceramics with Li2WO4 addition. J Mater Sci—Mater El 2015, 26: 1181–1185.

[46]

Lei T, Chen JW, Xu ZQ, et al. Microwave dielectric properties of the low-temperature-fired Li2ZnTi3O8–Li2TiO3 ceramics for LTCC applications. J Mater Sci—Mater El 2018, 29: 14705–14709.

[47]

Mendelson MI. Average grain size in polycrystalline ceramics. J Am Ceram Soc 1969, 52: 443–446.

[48]

McClure DS. The distribution of transition metal cations in spinels. J Phys Chem Solids 1957, 3: 311–317.

[49]

Burdett JK, Price GD, Price SL. Role of the crystal-field theory in determining the structures of spinels. J Am Chem Soc 1982, 104: 92–95.

[50]

Hu W, Liu HX, Hao H, et al. Influence of TiO2 additive on the microwave dielectric properties of α-CaSiO3–Al2O3 ceramics. Ceram Int 2015, 41: S510–S514.

[51]

Chen XQ, Li H, Zhang PC, et al. SrZnV2O7: A low-firing microwave dielectric ceramic with high-quality factor. J Am Ceram Soc 2021, 104: 5110–5119.

[52]

Penn SJ, Alford NM, Templeton A, et al. Effect of porosity and grain size on the microwave dielectric properties of sintered alumina. J Am Ceram Soc 1997, 80: 1885–1888.

[53]

Shannon RD. Dielectric polarizabilities of ions in oxides and fluorides. J Appl Phys 1993, 73: 348–366.

[54]

Du K, Fan J, Zou ZY, et al. Crystal structure, phase compositions, and microwave dielectric properties of malayaite-type Ca1− x Sr x SnSiO5 ceramics. J Am Ceram Soc 2020, 103: 6369–6377.

[55]

Kim ES, Chun BS, Freer R, et al. Effects of packing fraction and bond valence on microwave dielectric properties of A2+B6+O4 (A2+: Ca, Pb, Ba; B6+: Mo, W) ceramics. J Eur Ceram Soc 2010, 30: 1731–1736.

[56]

Kim ES, Jeon CJ. Microwave dielectric properties of ATiO3 (A=Ni,Mg,Co,Mn) ceramics. J Eur Ceram Soc 2010, 30: 341–346.

[57]

Liao QW, Li LX, Ding X. Phase constitution, structure analysis and microwave dielectric properties of Zn0.5Ti1− x Zr x NbO4 ceramics. Solid State Sci 2012, 14: 1385–1391.

[58]

Li LX, Li YT, Qiao JL, et al. Developing high- Q× f value MgNb2− x Ta x O6 (0 ≤ x ≤ 08) columbite ceramics and clarifying the impact mechanism of dielectric loss: Crystal structure, Raman vibrations, microstructure, lattice defects, chemical bond characteristics, structural parameters, and microwave dielectric properties in-depth studies. J Mater Sci Technol 2023, 146: 186–199.

[59]

Brese NE, O’Keeffe M. Bond-valence parameters for solids. Acta Cryst 1991, 47: 192–197.

[60]

Shannon RD. Oxygen position, octahedral distortion, and bond-valence parameter from bond lengths in Ti1− x Sn x O2 (0 ≤ x ≤ 1). J Am Ceram Soc 2000, 83: 3205–3207.

[61]
Luo YR. Bond dissociation energies. In: CRC Handbook of Chemistry and Physics. William M. Haynes, Ed. CRC Press, 2012.
[62]

Batsanov SS. Dielectric methods of studying the chemical bond and the concept of electronegativity. Russ Chem Rev 1982, 51: 684–697.

[63]

Borbón S, Lugo S, Pineda N, et al. ZnTiO3 nanoparticles for application as photoanode in dye-sensitized solar cells (DSSC). Phys B 2022, 630: 413704.

[64]

Guo HH, Zhou D, Pang LX, et al. Influence of (Mg1/3Nb2/3) complex substitutions on crystal structures and microwave dielectric properties of Li2TiO3 ceramics with extreme low loss. J Materiomics 2018, 4: 368–382.

[65]

Xiao K, Tang Y, Tian YF, et al. Enhancement of the cation order and the microwave dielectric properties of Li2ZnTi3O8 through composition modulation. J Eur Ceram Soc 2019, 39: 3064–3069.

[66]

Huang FY, Su H, Zhang Q, et al. The structural characteristics and microwave dielectric properties of Ti4+ doped CaMgSi2O6 ceramics. Ceram Int 2022, 48: 33615–33623.

Journal of Advanced Ceramics
Pages 1178-1188
Cite this article:
Du Q, Jiang L, Ma L, et al. Lattice evolution, order transformation, and microwave dielectric properties of the Zn1−xLi2xTiO3 (0 ≤ x ≤ 1) system ceramics. Journal of Advanced Ceramics, 2024, 13(8): 1178-1188. https://doi.org/10.26599/JAC.2024.9220927

917

Views

192

Downloads

2

Crossref

1

Web of Science

3

Scopus

0

CSCD

Altmetrics

Received: 03 April 2024
Revised: 07 June 2024
Accepted: 11 June 2024
Published: 30 August 2024
© The Author(s) 2024.

This is an open access article under the terms of the Creative Commons Attribution 4.0 International License (CC BY 4.0, http://creativecommons.org/licenses/by/4.0/).

Return