Li/Ce/La Multidoping on Crystal Structure and Electric Properties of CaBi2Nb2O9 Piezoceramics

doi:10.15541/jim20180225

Abstract

Abstract:

(Li_0.5Ce_0.25La_0.25)_xCa_1-_xBi₂Nb₂O₉ Aurivillius phase ceramics were prepared via conventional solid-state sintering route. The effects of co-substitution with different types of rare-earth elements on crystal structure, microstructure and electric properties were investigated. Rietveld-refinement analysis showed that the multiple rare earth elements embedded into the lattice point and formed corresponding solid solutions. The crystal structure tended to transform to tetragonal system from pristine orthorhombic system, whereas Bi ³⁺ in A-site with 6s2 lone pair electrons suppressed this change. SEM images exhibited that the grain growth in the direction perpendicular to the c-axis was restrained, which could be attributed to the rare earth oxides’ high melting point and low diffusion during the sintering process. Morphotropic phase boundary of a glide plane between orthorhombic system and pseudo-tetragonal system vanished, which generated spontaneous polarization along a and b axis and resulted in increase of piezoelectric properties. The obtained (Li_0.5Ce_0.25La_0.25)_0.17Ca_0.83Bi₂Nb₂O₉ ceramics performed optimal piezoelectric properties (d₃₃=16.4 pC/N, T_c=913 ℃) and exhibited excellent thermal stability, remaining 85.4% of their initial d₃₃ values after annealing at 850 ℃ for 2 h. All above results demonsrated that the multidoped materials are promising candidates for ultrahigh temperature applications.

Key words: rare earth element doping, bismuth layered structure, Rietveld refinement, crystal structure, piezoelectric property

CLC Number:

TB34

Xiang-Xiong ZENG, Jin-Chao YANG, Lian ZUO, Ben-Ben YANG, Jun QIN, Zhi-Hang PENG. Li/Ce/La Multidoping on Crystal Structure and Electric Properties of CaBi₂Nb₂O₉ Piezoceramics[J]. Journal of Inorganic Materials, 2019, 34(4): 379-386.

Figures/Tables 14

References 26

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	CBN	CBNLCL-5	CBNLCL-10	CBNLCL-12	CBNLCL-15	CBNLCL-17
Space group	A2₁am	A2₁am	A2₁am	A2₁am	A2₁am	A2₁am
R_p/%	6.31	7.25	4.86	5.16	4.72	5.01
R_wp/%	8.62	9.57	6.35	6.76	6.04	6.66
R_exp/%	4.77	5.26	5.38	5.15	5.37	5.34
Chi2	3.26	3.31	1.39	1.72	1.26	1.56
a/nm	0.54778(3)	0.54802(2)	0.54778(2)	0.54761(2)	0.54725(2)	0.54704(2)
b/nm	0.54355(3)	0.54372(2)	0.54379(2)	0.54378(2)	0.54396(2)	0.54390(2)
c/nm	2.48626(8)	2.48738(7)	2.48689(6)	2.48641(7)	2.48581(8)	2.48495(7)
V/nm³	0.740273(5)	0.741164(4)	0.740778(4)	0.742398(4)	0.739980(5)	0.739362(4)
a/b	1.00778	1.00790	1.00734	1.00706	1.00606	1.00577
Occupancy of Bi³⁺ at A site	0.108	0.116	0.106	0.108	0.092	0.094

	CBN	CBNLCL-5	CBNLCL-10	CBNLCL-12	CBNLCL-15	CBNLCL-17
Space group	A2₁am	A2₁am	A2₁am	A2₁am	A2₁am	A2₁am
R_p/%	6.31	7.25	4.86	5.16	4.72	5.01
R_wp/%	8.62	9.57	6.35	6.76	6.04	6.66
R_exp/%	4.77	5.26	5.38	5.15	5.37	5.34
Chi2	3.26	3.31	1.39	1.72	1.26	1.56
a/nm	0.54778(3)	0.54802(2)	0.54778(2)	0.54761(2)	0.54725(2)	0.54704(2)
b/nm	0.54355(3)	0.54372(2)	0.54379(2)	0.54378(2)	0.54396(2)	0.54390(2)
c/nm	2.48626(8)	2.48738(7)	2.48689(6)	2.48641(7)	2.48581(8)	2.48495(7)
V/nm³	0.740273(5)	0.741164(4)	0.740778(4)	0.742398(4)	0.739980(5)	0.739362(4)
a/b	1.00778	1.00790	1.00734	1.00706	1.00606	1.00577
Occupancy of Bi³⁺ at A site	0.108	0.116	0.106	0.108	0.092	0.094

Bond type	CBN	CBNLCL-5	CBNLCL-10	CBNLCL-12	CBNLCL-15	CBNLCL-17
Nb—O
Nb—O1—Nb/(°)	158.47	151.84	153.94	152.96	158.99	152.68
O1—Nb—O2/(°)	174.11	172.79	172.99	171.85	171.33	171.81
Nb—O1/nm	0.2120	0.2159	0.2148	0.2143	0.2127	0.2151
Nb—O2/nm	0.2047	0.1888	0.1817	0.1836	0.1804	0.1805
Nb—O4 (1)/nm	0.1938	0.1846	0.1854	0.1848	0.1897	0.1872
Nb—O4 (2)/nm	0.2066	0.2180	0.2174	0.2162	0.2146	0.2127
Nb—O5 (1)/nm	0.1837	0.1968	0.1956	0.1945	0.1943	0.1955
Nb—O5 (2)/nm	0.2135	0.1979	0.1971	0.1997	0.1968	0.2002
Ca1/Bi1/Li/Ce/La—O (A—O)
A—O1(1ong bond along a axis)/nm	0.3191	0.3424	0.3233	0.3250	0.3123	0.3167
A—O1(short bond along a axis)/nm	0.2312	0.2058	0.2291	0.2277	0.2382	0.2364
A—O1(short bond along b axis)/nm	0.2365	0.2627	0.2323	0.2337	0.2315	0.2267
A—O1(1ong bond along b axis)/nm	0.3143	0.2980	0.3199	0.3191	0.3176	0.3235
A—O4 (1)/nm	0.2604×2	0.2539×2	0.2532×2	0.2546×2	0.2573×2	0.2526×2
A—O4 (2)/nm	0.2605×2	0.2549×2	0.2567×2	0.2557×2	0.2584×2	0.2585×2
A—O5 (1)/nm	0.2305×2	0.3208×2	0.3226×2	0.3269×2	0.3235×2	0.3257×2
A—O5 (2)/nm	0.2380×2	0.2422×2	0.2466×2	0.2486×2	0.2448×2	0.2477×2
Bi2/Ca2—O
Bi2/Ca2—O2 (1)/nm	0.2660	0.2553	0.2574	0.2516	0.2587	0.2599
Bi2/Ca2—O2 (2)/nm	0.2775	0.3165	0.2832	0.2827	0.2748	0.2789
Bi2/Ca2—O2 (3)/nm	0.2961	0.2733	0.3075	0.3086	0.3170	0.3111
Bi2/Ca2—O2 (4)/nm	0.3039	0.3313	0.3296	0.3356	0.3310	0.3277

Bond type	CBN	CBNLCL-5	CBNLCL-10	CBNLCL-12	CBNLCL-15	CBNLCL-17
Nb—O
Nb—O1—Nb/(°)	158.47	151.84	153.94	152.96	158.99	152.68
O1—Nb—O2/(°)	174.11	172.79	172.99	171.85	171.33	171.81
Nb—O1/nm	0.2120	0.2159	0.2148	0.2143	0.2127	0.2151
Nb—O2/nm	0.2047	0.1888	0.1817	0.1836	0.1804	0.1805
Nb—O4 (1)/nm	0.1938	0.1846	0.1854	0.1848	0.1897	0.1872
Nb—O4 (2)/nm	0.2066	0.2180	0.2174	0.2162	0.2146	0.2127
Nb—O5 (1)/nm	0.1837	0.1968	0.1956	0.1945	0.1943	0.1955
Nb—O5 (2)/nm	0.2135	0.1979	0.1971	0.1997	0.1968	0.2002
Ca1/Bi1/Li/Ce/La—O (A—O)
A—O1(1ong bond along a axis)/nm	0.3191	0.3424	0.3233	0.3250	0.3123	0.3167
A—O1(short bond along a axis)/nm	0.2312	0.2058	0.2291	0.2277	0.2382	0.2364
A—O1(short bond along b axis)/nm	0.2365	0.2627	0.2323	0.2337	0.2315	0.2267
A—O1(1ong bond along b axis)/nm	0.3143	0.2980	0.3199	0.3191	0.3176	0.3235
A—O4 (1)/nm	0.2604×2	0.2539×2	0.2532×2	0.2546×2	0.2573×2	0.2526×2
A—O4 (2)/nm	0.2605×2	0.2549×2	0.2567×2	0.2557×2	0.2584×2	0.2585×2
A—O5 (1)/nm	0.2305×2	0.3208×2	0.3226×2	0.3269×2	0.3235×2	0.3257×2
A—O5 (2)/nm	0.2380×2	0.2422×2	0.2466×2	0.2486×2	0.2448×2	0.2477×2
Bi2/Ca2—O
Bi2/Ca2—O2 (1)/nm	0.2660	0.2553	0.2574	0.2516	0.2587	0.2599
Bi2/Ca2—O2 (2)/nm	0.2775	0.3165	0.2832	0.2827	0.2748	0.2789
Bi2/Ca2—O2 (3)/nm	0.2961	0.2733	0.3075	0.3086	0.3170	0.3111
Bi2/Ca2—O2 (4)/nm	0.3039	0.3313	0.3296	0.3356	0.3310	0.3277

Li/Ce/La Multidoping on Crystal Structure and Electric Properties of CaBi₂Nb₂O₉ Piezoceramics

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