氧化物玻璃中的类分子结构单元

万法琦; 马艳平; 董丹丹; 丁万昱; 姜宏; 董闯; 贺建雄

doi:10.7498/aps.69.20191892

摘要

本文引入团簇加连接原子模型来解析硅酸盐玻璃相关氧化物的结构, 并给出了这些氧化物的最小结构单元——类分子结构单元. 参与网络形成体的氧化物主要以三角形或者四面体的配位体形式存在, 构建玻璃的三维网络状骨架. 如基础的网络形成体SiO₂, 其类分子结构单元团簇式是为[Si-O₄]Si, 含有的价电子数为32, 形成四面体网络. 中间体以同时形成八面体和四面体为特征, 网络外体则以立方体和八面体为主. 经证实, 这些类分子结构单元无一例外, 均满足八电子规则(即每个结构单元所含的价电子总数为8的整数倍), 具有分子的属性. 玻璃中氧化物类分子结构单元概念的提出, 将为后续的玻璃成分设计工作打下基础.

关键词:

Abstract

Silica glasses are composed of multi-oxides, apart from the major component silica. Though it is a general practice in the industries to prepare glasses at specific oxide ratios, the composition rule is largely missing, complicated by the implication of multi-oxides. Necessarily, their interpretation is rooted in chemical units, on which the specific compositions depend. However, in silica glasses the inter-atomic bonding network is continuous and there is no weak bonds, like the inter-molecular ones in molecular compounds, to define molecular entities that carry the chemical information of the materials. As the first stage towards understanding the composition rule, the present paper introduces a new method, so-called the cluster-plus-glue-atom model, to unveil the molecule-like structural units of the glass-relevant oxides. It is pointed out that their respective contributions to the construction of glass networks originate from their characteristic cluster structures, and from which molecule-like structural units are proposed that represent the smallest structural units of these oxides. Oxides participating in the glass network formation mainly present triangular or tetrahedral clusters which are required for a three-dimensional glassy network. For example, the basic network former SiO₂ is formulated as [Si-O₄]Si and contains 32 valence electrons. The intermediate oxides are characterized by the simultaneous formation of both octahedra and tetrahedra. The network modifiers present mainly cubes and octahedra. It is confirmed that the molecule-like structural units of the glass-formation oxides all meet octet rule (that is, the total number of valence electrons contained in each structural unit is an integer multiple of 8), just like common molecules. The proposed concept of molecular structural units sheds a new light on understanding the composition rule of silicate glasses and can eventually solve the long-standing problem of composition design of silica glasses.

Keywords:

作者及机构信息

1.
海南大学海南省特种玻璃重点实验室&南海海洋资源利用国家重点实验室, 海口　570228

2.
大连大学物理科学与技术学院, 大连　116622

3.
大连交通大学材料科学与工程学院, 大连　116028

4.
大连理工大学三束材料改性教育部重点实验室, 大连　116024

5.
海南中航特玻科技有限公司&特种玻璃国家重点实验室, 海口　579124

通信作者: 马艳平, myp@hainanu.edu.cn ; 姜宏, jhong63908889@sina.com ;

基金项目: 省部级-海南省重大科技计划项目(No.ZDKJ2017011)

Authors and contacts

1.
Key Laboratory of Special Glass of Hainan Province and State Key Laboratory of South China Sea Resources Utilization, Hainan University, Haikou 570228, China

2.
College of Physical Science and Technology, Dalian University, Dalian 116622, China

3.
School of Materials Science and Engineering, Dalian Jiaotong University, Dalian 116028, China

4.
Key Laboratory for Materials Modification by Laser, Ion and Electron Beam, Dalian University of Technology, Dalian 116024, China

5.
Hainan Zhonghang Special Glass Technology Co., Ltd. & State Key Laboratory of Special Glass, Haikou 579124, China

Corresponding author: Ma Yan-Ping, myp@hainanu.edu.cn ; Jiang Hong, jhong63908889@sina.com ;

文章全文 : translate this paragraph

参考文献

[1]	王建成 2015 中国工业评论 0 4 Wang J C 2015 China Industry Review 0 4
[2]	马艳平 2019 博士学位论文 (大连: 大连理工大学) Ma Y P 2019 Ph. D. Dissertation (Dalian: Dalian University of Technology) (in Chinese)
[3]	Ma Y P, Dong D D, Wu A M, Dong C 2018 Inorg. Chem. 57 710 Google Scholar
[4]	Nuernberg F, Kuehn B, Rollmann K Metrology of Fused Silica Laser-Induced Damage in Optical Materials Boulder, Colorado, United States, September 25 2016, p10014
[5]	Salmon P S 2002 Nat. Mater. 1 7 Google Scholar
[6]	Elliot S R 1984 Physics of Amorphous Materials (London: Longman) pp20–27
[7]	Scholze H 1992 Appl. Opt. 31 31
[8]	Dong C, Wang Z J, Zhang S, Wang Y M 2020 Int. Mater. Rev. 65 286 Google Scholar
[9]	董闯, 董丹丹, 王清 2018 金属学报 54 293 Google Scholar Dong C, Dong D D, Wang Q 2018 Acta Mater 54 293 Google Scholar
[10]	Dong C, Wang Q, Qiang J B, Wang Y M, Jiang N, Han G, Li Y H, Wu J, Xia J H 2007 Phys. D: Appl. Phys. 40 273 Google Scholar
[11]	Han G, Qian J, Li F, Yuan L, Quan S G, Wang Q, Wang Y M, Dong C, Peter Häusslerl 2011 Acta. Mater. 59 5917 Google Scholar
[12]	Du J, We B, Melnik R, Yoshiyuki K 2014 Acta. Mater. 75 113 Google Scholar
[13]	Chen J X, Wang Q, Wang Y M, Qiang J B, Dong C 2010 Phil. Mag. Lett. 90 683 Google Scholar
[14]	Dong D D, Zhang S, Wang Z J, Dong C, Häusslerl P 2016 Mater. Des. 96 115 Google Scholar
[15]	董丹丹 2017 博士学位论文 (大连: 大连理工大学) Dong D D 2017 Ph. D. Dissertation (Dalian: Dalian University of Technology) (in Chinese)
[16]	张爽 2019 博士学位论文 (大连: 大连理工大学) Zhang S 2019 Ph. D. Dissertation (Dalian: Dalian University of technology) (in Chinese)
[17]	Lewis G N 1916 J. Am. Chem. Soc. 38 762 Google Scholar
[18]	Miracle D, Sanders W, Senkov O N 2003 Philos. Mag. 83 2409 Google Scholar
[19]	Villars P, Calvert L D 1985 Pearson’s Handbook of Crystallographic Data For Intermetallic Phases (Ohio, USA: American Society for Metals) pp2579−2580
[20]	周艳艳, 张希艳 2014 玻璃化学) (北京: 化学工业出版社) 第220−225页 Zhou Y Y, Zhang X Y 2014 Glass Chemistry (Beijing: Chemical Industry Press) pp220−225
[21]	田英良, 孙诗兵 2009 新编玻璃工艺学 (北京: 中国轻工业出版社) 第25—30页 TianY L, Sun S B 2009 New Glass Technology (Version 1) (Beijing: China Light Industry Press) pp25–30
[22]	Özgür Ü, Alivov Y I, Liu C, Teke A, Reshchikov M A, Doğan S, Avrutin V, Chong S J, Morkoç H 2005 Appl. Phys. 98 041301 Google Scholar
[23]	余小红 2015 博士学位论文 (武汉: 中国地质大学) Yu X H 2015 Ph. D. Dissertation (Wuhan: China University of Geosciences) (in Chinese)
[24]	戴培赞, 戚凭, 姜富城, 鲁萌萌 2006 青岛大学学报 19 22 Dai P Z, Qi P, Jiang F C, Lu M M 2006 Journal of Qingdao University 19 22
[25]	Hazen R M, Finger L W 1986 J. Appl. Phys. 59 372 8
[26]	Boettger J C, Wills J M 1996 Phys. Rev. B 54 8965 Google Scholar

施引文献

图 1 水分子的电子结构^[2]

Fig. 1. Electron structure of water molecule^[2].

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图 2 基于[Si-O₄]四面体的鳞石英β-SiO₂晶体结构^[3]

Fig. 2. Crystal structure of β-SiO₂ using tetrahedral cluster [Si-O₄]^[3].

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图 3 氧化硅玻璃的结构示意图, 显示了长程无序和近程有序(硅氧四面体)特征^[4]

Fig. 3. The amorphous structure of glassy silica (SiO₂) in two dimensions^[4]

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图 4 (a) 团簇加连接原子模型^[11]; (b) 团簇的间距为r₃

Fig. 4. (a) Cluster-plus-glue-atom model^[11]; (b) the inter-cluster distance is r₃.

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图 5 (a) β-SiO₂(SiO₂结构, 空间群194)的主团簇[Si-O₄]和[O-Si₂], 大原子为O, 小原子为Si; (b)类分子结构单元[Si-O₄]Si

Fig. 5. (a)Principal cluster [Si-O₄] and [O-Si₂] in β-SiO₂ structure (space group 194). Large and small spheres are O and Si atoms, respectively; (b) molecule-like structural unit[Si-O₄]Si.

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图 6 氧化物的单胞结构, 大原子为O:　(a) B₂O₃(P3₁); (b) B₂O₃(Cmc2₁); (c) GeO₂(P4₁2₁2); (d) P₂O₅(Pnma)

Fig. 6. The cell structure of oxides, and large atoms are O: (a) B₂O₃(P3₁); (b) B₂O₃(Cmc2₁); (c) GeO₂(P4₁2₁2); (d) P₂O₅(Pnma).

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图 7 反萤石结构Li₂O的团簇[Li-O₄]与[O-Li₈], 后者为主团簇. 大原子为O, 小原子为Li

Fig. 7. Clusters in anti-fluorite Li₂O, [Li-O₄] and [O-Li₈] (principal cluster). Large spheres represent O and small spheres represent Li.

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图 8 NaCl结构CaO的团簇[Ca-O₆]与[O-Ca₆], 前者为主团簇. 大原子为O, 小原子为Ca

Fig. 8. Clusters in NaCl structure of Li₂O, [Ca-O₆] (principal cluster)and [O-Ca₆]. Large spheres represent O and small spheres represent Li.

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图 9 α-Al₂O₃中的团簇: 四面体[O-Al₄]与八面体[Al-O₆](主团簇), 小原子为Al

Fig. 9. Clusters in α-Al₂O₃ unit cell, including [O-Al₄] and [Al-O₆] (principal cluster). Small spheres represent Al.

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图 10 γ-Al₂O₃(Al₂MgO₄尖晶石结构)中的团簇, 含有两种四面体[O-Al₄]和[Al-O₄](主团簇)与一种八面体[Al-O₆], 小原子为Al

Fig. 10. Clusters in γ-Al₂O₃ (Al₂MgO₄ structure), including [O-Al₄], [Al-O₄] (principal cluster), and [Al-O₆]. Small spheres represent Al.

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图 11 ZnO的单胞结构, 小原子为Zn　(a) ZnO ($ F{\bar 4}3 m$); (b) ZnO (P6₃mc)

Fig. 11. The cell structure of ZnO, and small spheres represent Ti: (a) ZnO ($ F{\bar 4}3 m$); (b) ZnO (P6₃mc).

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图 12 ZnO(NaCl结构)中的八面体团簇[Zn-O₆]与[O-Zn₆], 前者为主团簇. 小原子为Zn

Fig. 12. Octahedral clusters [Zn-O₆] (principal cluster) and [O-Zn₆] in ZnO (NaCl structure). Small spheres represent Zn.

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图 13 TiO₂的单胞结构, 小原子为Ti　(a) TiO₂(P4₂/mnm); (b) TiO₂(I4₁/amd); (c) TiO₂( Pbca); (d) TiO₂ (P2₁/m)

Fig. 13. The cell structure of TiO₂, and small spheres represent are Ti: (a) TiO₂(P4₂/mnm); (b) TiO₂(I4₁/amd); (c) TiO₂( Pbca); (d) TiO₂ (P2₁/m)

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表 1 鳞石英(Tridymite)β-SiO₂的晶体结构数据表^[19]

Table 1. Crystal structure data of Tridymite β-SiO₂^[19].

O₂Si		Structure type O₂Si	Pearson symbol hP12		Space group P6₃/mmc	No.194
a = 0.5052(9) nm			c = 0.827(2) nm			γ = 120°
O1	2c	$ {\bar 6}m2$	x = 1/3	y = 2/3	z = 1/4	occ. = 1
Si	4f	3m.	x = 1/3	y = 2/3	z = 0.0620	occ. = 1
O2	6g	.2/m	x = 1/2	y = 0	z = 0	occ. = 1

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表 2 硅酸盐玻璃相关氧化物的类分子结构单元, 分为中心为阳离子和阴离子O两种; 依托于主团簇的类分子结构单元用黑体标出

Table 2. Molecule-like structural units of glass-relevant oxides. Molecule-like structural unit, based on principal clusters, are bolded.

Classification	Oxide (space group)	Cationic structural unit (e/u)	Anion structural unit (e/u)
Network formation	β-SiO₂ (P6₃/mmc)	[Si-O₄]Si = 2{SiO₂} (32)	[O-Si₂]O₃= 2{SiO₂} (32)
	B₂O₃ (P3₁)	[B-O₃]B = {B₂O₃} (24)	[O-B₂]O₂ = {B₂O₃} (24)
	B₂O₃ (Cmc2₁)	[B-O₄]B₃O₂ = 2{B₂O₃} (48)	[O-B₂]O₂ = {B₂O₃} (24)
			[O-B₃]O₅B₁ = 2{B₂O₃} (48)
	GeO₂ (P4₁2₁2)	[Ge-O₄]Ge = 2{GeO₂} (32)	[O-Ge₂]O₃ = 2{GeO₂} (32)
	P₂O₅ (Pnma)	[P-O₄]P₁O₁ = {P₂O₅} (40)	[O-P₂]O₄ = {P₂O₅} (40)
			[O-P₁]P₁O₄ = {P₂O₅} (40)
Network outside body	(Li, Na_,K)₂O (anti-fluorite$ Fm{\bar 3}m$)	[(Li, Na_,K)-O₄](Li, Na_,K)₇ = 4{(Li, Na_,K)O₂} (32)	[O-(Li, Na_,K)₈]O₃ = 4{(Li, Na_,K)O₂} (32)
	(Mg, Ca, Ba)O (Halite, $ Fm{\bar 3}m$)	[(Mg, Ca, Ba)-O₆](Mg, Ca, Ba)₅ = 6{(Mg, Ca, Ba)O} (48)	[O-(Mg, Ca, Ba)₆]O₅ = 4{(Mg, Ca, Ba)O} (48)
	ZrO₂ (rutile, P4₂/mnm)	[Zr-O₆]Zr₂ = 3{ZrO₂} (48)	[O-Zr₃]O₅ = 3{ZrO₂} (48)
Network intermediate	(Be, Zn)O (sphalerite, P43m)	[(Be, Zn)-O₄](Be, Zn)₃ = 4{(Be, Zn)O} (32)	[O-(Be, Zn)₄]O₃ = 4{(Be, Zn)O} (32)
	(Be, Zn)O (Wurtzite, P6₃mc)	[Zn-O₄]Zn₃ = 4{ZnO} (32)	[O-Zn₄]O₃ = 4{ZnO} (32)
	(Be, Zn)O (Halite, $ Fm{\bar 3}m$)	[Zn-O₆]Zn₅ = 6{ZnO} (48)	[O-Zn₆]O₅ = 6{ZnO} (48)
	α-Al₂O₃ ($ R{\bar 3}c$)	[Al-O₆]Al₃ = 2{Al₂O₃} (48)	[O-Al₄]O₅ = 2{Al₂O₃} (48)
	γ-Al₂O₃ (Spinel, $ Fd{\bar 3}m$)	[Al-O₄]O₂Al₃ = 2{Al₂O₃} (48)	[O-Al₄]O₅ = 2{Al₂O₃} (48)
		[Al-O₆]Al₃ = 2{Al₂O₃} (48)
	Ga₂O₃ (α-Al₂O₃, $ R{\bar 3}c$)	[Ga-O₆]Ga₃ = 2{Ga₂O₃} (48)	[O-Ga₄]O₅ = 2{Ga₂O₃} (48)
	Ga₂O₃ (Spinel, $ Fd{\bar 3}m$)	[Ga-O₄]O₂Ga₃ = 2{Ga₂O₃} (48)	[O-Ga₄]O₅ = 2{Ga₂O₃} (48)
		[Ga-O₆]Ga₃ = 2{Ga₂O₃} (48)
	Fe₂O₃ (α-Al₂O₃, $ R{\bar 3}c$)	[Fe-O₆]Fe₃ = 2{Fe₂O₃} (48)	[O-Fe₄]O₅ = 2{Fe₂O₃} (48)
	Fe₃O₄ (Spinel, $ Fd{\bar 3}m$)	[Fe-O₄]Fe₂ = {Fe₃O₄} (32)	[O-Fe₄]O₇Fe₂ = 2{Fe₃O₄} (64)
		[Fe-O₆]Fe₅O₂ = 2{Fe₃O₄} (64)	[O-Fe₄]O₇Fe₂ = 2{Fe₃O₄} (64)
	TiO₂ (Rutile, P4₂/mnm)	[Ti-O₆]Ti₂ = 3{TiO₂} (48)	[O-Ti₃]O₅ = 3{TiO₂} (48)
	TiO₂ (Anatase, I4₁/amd)	[Ti-O₆]Ti₂ = 3{TiO₂} (48)	[O-Ti₃]O₅ = 3{TiO₂} (48)
	TiO₂ (Brookite, Pbca)	[Ti-O₆]Ti₂ = 3{TiO₂} (48)	[O-Ti₃]O₅ = 3{TiO₂} (48)
	TiO₂ (P2₁/m)	[Ti-O₄]Ti = 2{TiO₂} (32)	[O-Ti₂]O₃ = 2{TiO₂} (32)
		[Ti-O₃]TiO = 2{TiO₂} (32)	[O-Ti]O₃Ti = 2{TiO₂} (32)

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[1]	王建成 2015 中国工业评论 0 4 Wang J C 2015 China Industry Review 0 4
[2]	马艳平 2019 博士学位论文 (大连: 大连理工大学) Ma Y P 2019 Ph. D. Dissertation (Dalian: Dalian University of Technology) (in Chinese)
[3]	Ma Y P, Dong D D, Wu A M, Dong C 2018 Inorg. Chem. 57 710 Google Scholar
[4]	Nuernberg F, Kuehn B, Rollmann K Metrology of Fused Silica Laser-Induced Damage in Optical Materials Boulder, Colorado, United States, September 25 2016, p10014
[5]	Salmon P S 2002 Nat. Mater. 1 7 Google Scholar
[6]	Elliot S R 1984 Physics of Amorphous Materials (London: Longman) pp20–27
[7]	Scholze H 1992 Appl. Opt. 31 31
[8]	Dong C, Wang Z J, Zhang S, Wang Y M 2020 Int. Mater. Rev. 65 286 Google Scholar
[9]	董闯, 董丹丹, 王清 2018 金属学报 54 293 Google Scholar Dong C, Dong D D, Wang Q 2018 Acta Mater 54 293 Google Scholar
[10]	Dong C, Wang Q, Qiang J B, Wang Y M, Jiang N, Han G, Li Y H, Wu J, Xia J H 2007 Phys. D: Appl. Phys. 40 273 Google Scholar
[11]	Han G, Qian J, Li F, Yuan L, Quan S G, Wang Q, Wang Y M, Dong C, Peter Häusslerl 2011 Acta. Mater. 59 5917 Google Scholar
[12]	Du J, We B, Melnik R, Yoshiyuki K 2014 Acta. Mater. 75 113 Google Scholar
[13]	Chen J X, Wang Q, Wang Y M, Qiang J B, Dong C 2010 Phil. Mag. Lett. 90 683 Google Scholar
[14]	Dong D D, Zhang S, Wang Z J, Dong C, Häusslerl P 2016 Mater. Des. 96 115 Google Scholar
[15]	董丹丹 2017 博士学位论文 (大连: 大连理工大学) Dong D D 2017 Ph. D. Dissertation (Dalian: Dalian University of Technology) (in Chinese)
[16]	张爽 2019 博士学位论文 (大连: 大连理工大学) Zhang S 2019 Ph. D. Dissertation (Dalian: Dalian University of technology) (in Chinese)
[17]	Lewis G N 1916 J. Am. Chem. Soc. 38 762 Google Scholar
[18]	Miracle D, Sanders W, Senkov O N 2003 Philos. Mag. 83 2409 Google Scholar
[19]	Villars P, Calvert L D 1985 Pearson’s Handbook of Crystallographic Data For Intermetallic Phases (Ohio, USA: American Society for Metals) pp2579−2580
[20]	周艳艳, 张希艳 2014 玻璃化学) (北京: 化学工业出版社) 第220−225页 Zhou Y Y, Zhang X Y 2014 Glass Chemistry (Beijing: Chemical Industry Press) pp220−225
[21]	田英良, 孙诗兵 2009 新编玻璃工艺学 (北京: 中国轻工业出版社) 第25—30页 TianY L, Sun S B 2009 New Glass Technology (Version 1) (Beijing: China Light Industry Press) pp25–30
[22]	Özgür Ü, Alivov Y I, Liu C, Teke A, Reshchikov M A, Doğan S, Avrutin V, Chong S J, Morkoç H 2005 Appl. Phys. 98 041301 Google Scholar
[23]	余小红 2015 博士学位论文 (武汉: 中国地质大学) Yu X H 2015 Ph. D. Dissertation (Wuhan: China University of Geosciences) (in Chinese)
[24]	戴培赞, 戚凭, 姜富城, 鲁萌萌 2006 青岛大学学报 19 22 Dai P Z, Qi P, Jiang F C, Lu M M 2006 Journal of Qingdao University 19 22
[25]	Hazen R M, Finger L W 1986 J. Appl. Phys. 59 372 8
[26]	Boettger J C, Wills J M 1996 Phys. Rev. B 54 8965 Google Scholar

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