Influence of additives on the tetragonal phase purity and grain size of zirconia

doi:10.3969/j.issn.2095-4344.0679

Abstract

Abstract:

BACKGROUND: Numerous studies have been made on the experimental parameters that influence the grain size of zirconia crystal and purity of tetragonal phase of zirconia. Until now, however, there is no unified conclusion on the influence of additives (ethylenediaminetetraacetic acid or glycerol) on the grain size of zirconia

crystal and purity of tetragonal phase of zirconia.

OBJECTIVE: To investigate the influence of additives (ethylenediaminetetraacetic acid or glycerol) on the grain size of zirconia crystal and purity of tetragonal phase of zirconia.

METHODS: Nitrates were adopted as raw materials, ethylenediaminetetraacetic acid or glycerol was adopted as additives, and ammonium hydroxide was chosen to adjust the pH of the solution. Then six kinds of zirconia were synthesized using hydrothermal method. The mole ratio of Zr⁴⁺:ethylenediaminetetraacetic acid:glycerol were 1:0:0, 1:1:0, 1:0:1, 1:0.5:0.5, 1:0.25:0.75, 1:0.75:0.25, and the samples were numbered 1-6 and characterized by X-ray diffraction. Afterwards, the influence of additives (ethylenediaminetetraacetic acid or glycerol) on the grain size and purity of tetragonal phase of zirconia was analyzed.

RESULTS AND CONCLUSION: Sample No. 3 was pure tetragonal zirconia and had the largest grain size. The other five samples contained two kinds of crystalline phases: tetragonal and monoclinic phases. Meanwhile, the content of tetragonal phase was higher than that of monoclinic phase. The grain size of samples No. 3-6 was larger than that of samples No. 1 and 2. The content of tetragonal phase of samples No. 1 and 3 was higher than that of samples No. 2, 4, 5, and 6. Our experimental data indicate that ethylenediaminetetraacetic acid could decrease the grain size and proportion of tetragonal phase of zirconia, while glycerol could increase the proportion and grain size of tetragonal phase of zirconia.

中国组织工程研究杂志出版内容重点：生物材料；骨生物材料; 口腔生物材料; 纳米材料; 缓释材料; 材料相容性；组织工程

Key words: Dental Materials, Edetic Acid, Glycerol, Tissue Engineering

CLC Number:

R318

Zang Sitian, Yang Qian, He Ningxiang, Ji Yang, Yang Huazhe. Influence of additives on the tetragonal phase purity and grain size of zirconia[J]. Chinese Journal of Tissue Engineering Research, 2018, 22(34): 5445-5451.

Figures/Tables 6

6个样品中Zr4+∶EDTA∶丙三醇的值分别为1∶0∶0，1∶1∶0，1∶0∶1，1∶0.5∶0.5，1∶0.25∶0.75， 1∶0.75∶0.25，6个样品的X射线衍射图谱都出现了较为明显的4个衍射峰，说明样品均形成了晶体。从4个主要衍射峰的位置上来看，在20°-65°范围内，6个样品并无明显差别，但是从衍射峰强度来看却有较为明显的差别。与JCPDS库中标准卡片对比，确定了6个样品中均有四方相氧化锆，(101)峰位分别为30.180°、30.420°、30.340°、30.306°、30.380°、30.296°，(110)峰位分别为35.338°、35.518°、35.360°、35.302°、35.340°、35.381°，(112)峰位分别为50.300°、50.540°、50.680°、50.460°、50.480°、50.480°，(211)峰位分别为60.179°、60.398°、60.280°、60.099°、60.200°、60.281°，(202)峰位分别为62.940°、63.040°、63.120°、63.000°、63.240°、63.240°。其中，3#样品为纯四方相氧化锆，1#、2#、4#、5#、6#样品均出现了杂相峰，与标准卡片对比，确定了5个样品中均出现有单斜相氧化锆，(-111)峰位分别为28.197°、28.280°、28.241°、28.182°、28.320°，(-211)峰位分别为40.827°、40.911°、40.901°、40.834°、40.880°，(112)峰位分别为44.887°、45.017°、45.216°、45.221°、44.996°，(013)峰位分别为55.453°、55.540°、55.796°、55.561°、55.572°。所以，实验制得的样品均为氧化锆，X射线衍射图谱并未出现其他物质衍射峰，说明样品中不含有其他物质杂相。其中，3#样品为纯四方相氧化锆，1#、2#、4#、5#、6#样品为四方相氧化锆和单斜相氧化锆2种晶型结构。说明与其他样品相比，未添加EDTA、只添加丙三醇时可制得纯四方相氧化锆。取It为四方相氧化锆(T-ZrO2)最强衍射峰峰高，Im为样品中主要杂相单斜相氧化锆(M-ZrO2)最强衍射峰峰高，根据公式(1)得出，1#、2#、4#、5#、6#样品单斜相与四方相氧化锆最强峰的峰高比值分别为0.299(Zr4+∶EDTA∶丙三醇=1∶0∶0)，0.408(Zr4+∶EDTA∶丙三醇=1∶1∶0)，0(Zr4+∶EDTA∶丙三醇=1∶0.5∶0.5)，0.377(Zr4+∶EDTA∶丙三醇=1∶0.25∶0.75)，0.384(Zr4+∶EDTA∶丙三醇=1∶0.75∶0.25)，如表2和图3所示。Im/It值均< 1，说明样品中四方相氧化锆的含量大于单斜相氧化锆的含量，且两相比例与各添加剂的量无明显线性关系，说明此次实验条件更利于四方相氧化锆的形成。与无添加剂的1# (Im/It=0.299) 样品相比，2#只添加EDTA时四方相比例(Im/It=0.408)减小，3#只添加丙三醇时为纯四方相氧化锆。与1#、3#样品相比，其余4个样品，无论是单独添加EDTA还是同时添加EDTA和丙三醇，均会使四方相比例(Im/It分别为0.408、0.469、0.377、0.384)降低。"

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