Effects of Li content on stability, electronic and Li-ion diffusion properties of Li3xLa(2/3)–x†(1/3)–2xTiO3 surface

Hua Biao; Sun Bao-Zhen; Wang Jing-Xuan; Shi Jing; Xu Bo

doi:10.7498/aps.72.20221808

Abstract

Li_3xLa_(2/3)–x†_(1/3)–2xTiO₃(LLTO) is a promising solid-state electrolyte for Li-ion batteries. We study the effect of Li content on the stability, electronic and Li-ion diffusion properties of LLTO surface based on first-principles and molecular dynamics simulations. We consider both Li-poor and Li-rich LLTO surfaces. The results show that La/O/Li-terminated LLTO (001) is the most stable crystal surface. Further, LLTO (001) surface gives better stability when Li content is 0.17, 0.29, and 0.38 for Li-poor phase, while 0.33, 0.40, and 0.45 for Li-rich phase . Electronic structure calculations infer that in both Li-poor and Li-rich LLTO(001) surfaces there occurs the transition from conductor to semiconductor with the increase of Li content. Besides, we find that Li-ion always keeps a two-dimensional diffusion path for different Li content. As Li content increases from 0.17 to 0.38 for Li-poor LLTO (001) surface, Li-ion diffusion coefficient increases gradually and Li-ion diffusion barrier decreases from 0.58 eV to 0.42 eV. Differently, when Li content increases from 0.33 to 0.45 for Li-rich LLTO(001) surface, it does not follow a monotonic trend for diffusion coefficient nor for diffusion barrier of Li-ion. In this case, Li-ion diffusion coefficient is the largest and Li-ion diffusion barrier is the lowest (0.30 eV) when Li content is 0.40. Thus, our study suggests that by varying Li content, the stability, band gap, and Li-ion diffusion performance of LLTO (001) can be changed favorably. These advantages can inhibit the formation of lithium dendrites on the LLTO (001) surface.

Keywords:

Authors and contacts

1.
College of Physics and Communication Electronics, Jiangxi Normal University, Nanchang 330022, China
2.
Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education, Jiangxi Normal University, Nanchang 330022, China

Corresponding author: Sun Bao-Zhen, bzsun@jxnu.edu.cn ; Xu Bo, bxu4@mail.ustc.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 12064015, 12164019) and the Natural Science Foundation of Jiangxi Province, China (Grant No. 20212BAB201017).

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References

[1]	Famprikis T, Canepa P, Dawson J A, Islam M S, Masquelier C 2019 Nat. Mater. 18 1278 Google Scholar
[2]	Manthiram A, Yu X W, Wang S F 2017 Nat. Rev. Mater. 2 1 Google Scholar
[3]	Zhao Q, Stalin S, Zhao C-Z, Archer L A 2020 Nat. Rev. Mater. 5 229 Google Scholar
[4]	Wu M S, Xu B, Lei X L, Huang K, Ouyang C Y 2018 J. Mater. Chem. A 6 1150 Google Scholar
[5]	Yan S, Yim C H, Pankov V, Bauer M, Baranova E, Weck A, Merati A, Abu-Lebdeh Y 2021 Batteries 7 75 Google Scholar
[6]	Sun Y D, Guan P Y, Liu Y J, Xu H L, Li S, Chu D W 2018 Crit. Rev. Solid State 44 265 Google Scholar
[7]	Hua C, Fang X, Wang Z, Chen L 2013 Electrochem. Commun. 32 5 Google Scholar
[8]	Stramare S, Thangadurai V, Weppner W 2003 Chem. Mater. 15 3974 Google Scholar
[9]	Chen C H, Amine K 2001 Solid State Ion. 144 51 Google Scholar
[10]	Inaguma o, Liquan C, Itoh M, Nakamura T 1993 Solid State Commun. 86 689 Google Scholar
[11]	Han F D, Westover A S, Yue J, Fan X L, Wang F, Chi M F, Leonard D N, Dudney N, Wang H, Wang C S 2019 Nat. Energy 4 187 Google Scholar
[12]	Wu B B, Wang S Y, Lochala J S, Desrochers D, Liu B, Zhang W Q, Yang J H, Xiao J 2018 Energy Environ. Sci. 11 1803 Google Scholar
[13]	Cervantes J M, Pilo J, Rosas-Huerta J L, Antonio J E, Muñoz H, Oviedo-Roa R, Carvajal E 2021 J. Electrochem. Soc. 168 080516 Google Scholar
[14]	Zhao Q S, Xue H T, Tang F L, Wei C D 2021 Solid State Ion. 373 115797 Google Scholar
[15]	Cheng L, Chen W, Kunz M, Persson K, Tamura N, Chen G Y, Doeff M 2015 ACS Appl. Mater. Interface 7 2073 Google Scholar
[16]	Belousov V V 2007 Russ. J. Phys. Chem. A 81 441 Google Scholar
[17]	Wu M S, Xu B, Luo W W, Sun B Z, Shi J, Ouyang C Y 2020 Appl. Surf. Sci. 510 145394 Google Scholar
[18]	Jung S C, Han Y K 2011 Phys. Chem. Chem. Phys. 13 21282 Google Scholar
[19]	Nakayama M, Usui T, Uchimoto Y, Wakihara M, Yamamoto M 2005 J. Phys. Chem. B 109 4135 Google Scholar
[20]	Inaguma Y, Itoh M 1996 Solid State Ion. 86-88 257
[21]	Maruyama Y, Ogawa H, Kamimura M, Kobayashi M 2006 J. Phys. Soc. Jpn. 75 064602 Google Scholar
[22]	Ren Y Y, Shen Y, Lin Y H, Nan C W 2019 ACS Appl. Mater. Interface 11 5928 Google Scholar
[23]	Catti M 2008 J. Phys. Chem. C 112 11068 Google Scholar
[24]	Qian D N, Xu B, Cho H M, Hatsukade T, Carroll K J, Meng Y S 2012 Chem. Mater. 24 2744 Google Scholar
[25]	Kresse G, Furthmuller J 1996 Phys. Rev. B 54 11169 Google Scholar
[26]	Kresse G, Hafner J 1994 Phys. Rev. B 49 14251 Google Scholar
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图 1 未优化的LLTO体相结构　(a) Li_0.125La_0.625TiO₃; (b) Li_0.35La_0.55TiO₃

Figure 1. Unrelaxed bulk structures of LLTO: (a) Li_0.125La_0.625TiO₃; (b) Li_0.35La_0.55TiO₃.

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图 2 具有La/O/Li-终端的LLTO(001)表面结构图　(a), (b)分别为贫锂相和富锂相的侧视图; (c), (d) 分别为贫锂相和富锂相的俯视图

Figure 2. La/O/Li-terminated LLTO(001) surfaces: (a), (b) The side views of Li-poor and Li-rich phases, respectively; (c), (d) the top views of Li-poor and Li-rich phases, respectively.

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图 3 不同Li含量下贫锂相和富锂相LLTO (001)面的表面能 (E_surf)

Figure 3. Surface energy (E_surf) of Li-poor and Li-rich LLTO (001) surfaces at different Li contents.

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图 4 贫锂相和富锂相LLTO (001)面在极值点附近的总态密度

Figure 4. Total density state (TDOS) of Li-poor and Li-rich LLTO (001) surfaces near the minimum point.

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图 5 Li在贫锂相和富锂相LLTO(001)表面的顺序吸附能(E_ads). 蓝色字体代表Li吸附能

Figure 5. The adsorption energies (E_ads) per Li on the poor-Li and rich-Li LLTO(001) surfaces. The blue texts denote the values of E_ads

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图 6 LLTO(001)表面的总态密度和投影态密度　(a) 贫锂相; (b)富锂相

Figure 6. TDOS and PDOS of LLTO(001) surfaces: (a) Li-poor phase; (b) Li-rich phase.

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图 7 800 K温度下Li⁺沿不同轴向的MSD随时间的变化曲线图　(a1)—(a4)贫锂相; (b1)—(b4)富锂相. 插图代表Li⁺的运动轨迹

Figure 7. The time dependence of MSDs for Li ions in a, b, and c directions: (a1)–(a4) Li-poor phase; (b1)–(b4)Li-rich phase. The inset shows the corresponding trajectories of Li⁺.

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图 8 LLTO体相及不同Li含量的LLTO(001)表面结构中Li⁺的扩散系数与温度关系

Figure 8. Arrhenius plot of Li⁺ diffusion coefficient for the LLTO bulk and its (001) surface with different lithium contents.

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表 1 不同泛函计算所得贫锂相LLTO体相的晶格参数(a, b, c)及带隙 (E_g)

Table 1. The calculated lattice parameters (a, b, c) and band gap (E_g) of Li-poor LLTO bulk with different functional.

Functional	a	b	c	E_g
GGA+PBE	7.842	7.771	7.843	1.630
GGA+PW91	7.835	7.768	7.838	1.585
LDA	7.705	7.638	7.697	1.624
PBE+U (U_Ti = 2.3 eV)	7.892	7.822	7.871	1.861
PBE+U (U_Ti = 2.5 eV)	7.897	7.827	7.834	1.851
PBE+U (U_Ti = 4.0 eV)	7.935	7.852	7.899	1.853
B3LYP^[23]	7.828	7.812	7.902	—
PBE+U (U_La = 7.5 eV)^[24]	7.828	7.754	7.871	—

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表 2 富锂相LLTO不同表面终端的表面能(E_surf)和化学式(SFs), 括号中的值对应贫锂相

Table 2. Surface energy (E_surf) and structural formulas (SFs) of Li-rich LLTO surfaces with different terminations. The data of Li-poor LLTO (001) is shown in parentheses.

Facets	Termination	SFs	E_surf/(J·m^–2)
(001)	La/O-	Li₃La₁₁Ti₁₀O₃₅ (Li₂La₁₄Ti₁₆O₅₂)	2.89 (1.95)
	Ti/O-	Li₃La₆Ti₁₅O₄₀ (LiLa₉Ti₁₆O₄₄)	1.40 (1.33)
	La/O/Li-	Li₁₀La₁₂Ti₂₀O₆₅ (Li₃La₁₁Ti₁₆O₅₂)	0.69 (0.78)
	Li/O-	Li₁₁La₁₁Ti₂₀O₆₅	0.78
(010)	La/O-	Li₇La₁₃Ti₂₀O₆₄	0.93
	Ti/O-	Li₇La₁₁Ti₂₄O₆₈	0.87
	La/O/Li-	Li₉La₁₃Ti₂₀O₆₄	0.82
(100)	La/O-	Li₇La₁₃Ti₂₀O₆₄	1.05
	Ti/O-	Li₇La₁₁Ti₂₄O₆₈	0.90
	La/O/Li-	Li₉La₁₃Ti₂₀O₆₄	0.83
(110)	O-	Li₇La₁₁Ti₂₀O₆₈	0.98
	Ti/La/O-	Li₇La₁₃Ti₂₄O₆₄	3.40
	Ti/O/La/Li-	Li₉La₁₄Ti₂₄O₇₂	1.21
(111)	La/O-	Li₉La₁₃Ti₂₄O₇₂	2.21
	Ti/O-	Li₇La₁₁Ti₂₀O₆₀	0.85
	Ti/O/La/Li-	Li₇La₁₁Ti₂₀O₆₀	0.93

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表 3 不同温度下贫锂相和富锂相LLTO(001)表面结构中全部Li⁺的最小(D_min)和最大(D_max)扩散系数

Table 3. The minimum (D_min) and maximum (D_max) Li⁺ diffusion coefficient of Li-poor and Li-rich LLTO(001) surfaces at different temperatures.

T/K	Li-poor phase/(cm²·S^–1)		Li-rich phase/(cm²·S^–1)
T/K	D_min	D_max	D_min	D_max
550	1.06×10^–7	2.37×10^–7	7.02×10^–7	1.14×10^–6
600	2.02×10^–7	8.12×10^–7	9.96×10^–7	2.53×10^–6
650	3.84×10^–7	1.46×10^–6	2.26×10^–6	3.38×10^–6
700	1.77×10^–6	2.01×10^–6	3.34×10^–6	4.80×10^–6
750	2.22×10^–6	3.27×10^–6	4.69×10^–6	7.08×10^–6
800	4.03×10^–6	4.28×10^–6	6.33×10^–6	9.36×10^–6

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map

[1]	Famprikis T, Canepa P, Dawson J A, Islam M S, Masquelier C 2019 Nat. Mater. 18 1278 Google Scholar
[2]	Manthiram A, Yu X W, Wang S F 2017 Nat. Rev. Mater. 2 1 Google Scholar
[3]	Zhao Q, Stalin S, Zhao C-Z, Archer L A 2020 Nat. Rev. Mater. 5 229 Google Scholar
[4]	Wu M S, Xu B, Lei X L, Huang K, Ouyang C Y 2018 J. Mater. Chem. A 6 1150 Google Scholar
[5]	Yan S, Yim C H, Pankov V, Bauer M, Baranova E, Weck A, Merati A, Abu-Lebdeh Y 2021 Batteries 7 75 Google Scholar
[6]	Sun Y D, Guan P Y, Liu Y J, Xu H L, Li S, Chu D W 2018 Crit. Rev. Solid State 44 265 Google Scholar
[7]	Hua C, Fang X, Wang Z, Chen L 2013 Electrochem. Commun. 32 5 Google Scholar
[8]	Stramare S, Thangadurai V, Weppner W 2003 Chem. Mater. 15 3974 Google Scholar
[9]	Chen C H, Amine K 2001 Solid State Ion. 144 51 Google Scholar
[10]	Inaguma o, Liquan C, Itoh M, Nakamura T 1993 Solid State Commun. 86 689 Google Scholar
[11]	Han F D, Westover A S, Yue J, Fan X L, Wang F, Chi M F, Leonard D N, Dudney N, Wang H, Wang C S 2019 Nat. Energy 4 187 Google Scholar
[12]	Wu B B, Wang S Y, Lochala J S, Desrochers D, Liu B, Zhang W Q, Yang J H, Xiao J 2018 Energy Environ. Sci. 11 1803 Google Scholar
[13]	Cervantes J M, Pilo J, Rosas-Huerta J L, Antonio J E, Muñoz H, Oviedo-Roa R, Carvajal E 2021 J. Electrochem. Soc. 168 080516 Google Scholar
[14]	Zhao Q S, Xue H T, Tang F L, Wei C D 2021 Solid State Ion. 373 115797 Google Scholar
[15]	Cheng L, Chen W, Kunz M, Persson K, Tamura N, Chen G Y, Doeff M 2015 ACS Appl. Mater. Interface 7 2073 Google Scholar
[16]	Belousov V V 2007 Russ. J. Phys. Chem. A 81 441 Google Scholar
[17]	Wu M S, Xu B, Luo W W, Sun B Z, Shi J, Ouyang C Y 2020 Appl. Surf. Sci. 510 145394 Google Scholar
[18]	Jung S C, Han Y K 2011 Phys. Chem. Chem. Phys. 13 21282 Google Scholar
[19]	Nakayama M, Usui T, Uchimoto Y, Wakihara M, Yamamoto M 2005 J. Phys. Chem. B 109 4135 Google Scholar
[20]	Inaguma Y, Itoh M 1996 Solid State Ion. 86-88 257
[21]	Maruyama Y, Ogawa H, Kamimura M, Kobayashi M 2006 J. Phys. Soc. Jpn. 75 064602 Google Scholar
[22]	Ren Y Y, Shen Y, Lin Y H, Nan C W 2019 ACS Appl. Mater. Interface 11 5928 Google Scholar
[23]	Catti M 2008 J. Phys. Chem. C 112 11068 Google Scholar
[24]	Qian D N, Xu B, Cho H M, Hatsukade T, Carroll K J, Meng Y S 2012 Chem. Mater. 24 2744 Google Scholar
[25]	Kresse G, Furthmuller J 1996 Phys. Rev. B 54 11169 Google Scholar
[26]	Kresse G, Hafner J 1994 Phys. Rev. B 49 14251 Google Scholar
[27]	Perdew J P, Burke K, Ernzerhof M 1996 Phys. Rev. Lett. 77 3865 Google Scholar
[28]	Perdew J P, Ernzerhof M, Burke K 1996 J. Chem. Phys. 105 9982 Google Scholar
[29]	Blochl P E 1994 Phys. Rev. B 50 17953 Google Scholar
[30]	Kresse G, Joubert D 1999 Phys. Rev. B 59 1758 Google Scholar
[31]	Monkhorst H J, Pack J D 1976 Phys. Rev. B 13 5188 Google Scholar
[32]	Plimpton S 1995 J. Comput. Phys. 117 1 Google Scholar
[33]	Chen C H, Du J C, Chen L Q 2015 J. Am. Ceram. Soc. 98 534 Google Scholar
[34]	Symington A R, Molinari M, Dawson J A, Statham J M, Purton J, Canepa P, Parker S C 2021 J. Mater. Chem. A 9 6487 Google Scholar
[35]	Ono S, Seki Y, Kashida S, Kobayashi M 2006 Solid State Ion. 177 1145 Google Scholar
[36]	Kim D H, Kim D H, Jeong Y C, Seo H I, Kim Y C 2012 Ceram. Int. 38 S S467
[37]	Bohnke O 2008 Solid State Ion. 179 9 Google Scholar

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Effects of Li content on stability, electronic and Li-ion diffusion properties of Li_3xLa_(2/3)–x†_(1/3)–2xTiO₃ surface

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Corresponding author: Sun Bao-Zhen, bzsun@jxnu.edu.cn ; Xu Bo, bxu4@mail.ustc.edu.cn

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