B2O3-SiO2-Na2O缓释材料的合成工艺参数优化及其缓释机理

doi:10.15541/jim20180359

摘要/Abstract

摘要：

为优化工艺参数、减少原料损失和控制生产成本, 本研究采用单因素法研究不同升温速率、保温时间、熔制温度和起始温度对硼酸盐缓释材料(BCRM)在制备过程中B₂O₃挥发量和气泡生成情况的影响规律。运用X射线衍射分析、红外光谱和X射线光电子能谱仪表征缓释前后BCRM理化性质变化, 通过Korsmeyer-Peppas模型分析BCRM缓释机理。结果表明, 在起始温度1050 ℃、保温时间2 h和熔制温度1050 ℃的最优工艺参数下, B₂O₃挥发量可降低至1.08%, BCRM澄清透明, 无气泡生成, 缓释性能良好。此外, 温度会影响BCRM的缓释机理, 在30和35 ℃时, 释放机理为Super Case II转运; 在40 ℃时, 释放机制为non-Fickian扩散。但在不同温度下, 硼累积释放率均高于95%。

关键词: 硼酸盐, 工艺参数优化, B₂O₃挥发, 缓释机理

Abstract:

Aiming at optimization of synthetic process, reduction of raw materials loss and control of production cost, the single factor method was used to study the effects of different heating rate, holding time, melting temperature, and initial temperature on the B₂O₃ volatilization and bubble formation during the preparation of borate controlled- release material (BCRM). The physicochemical properties of BCRM before and after controlled-release were characterized by X-ray diffraction analysis, infrared spectroscopy and X-ray photoelectron spectroscopy, and the release mechanism of BCRM was analyzed by Korsmeyer-Peppas model. The results show that the amount of B₂O₃ volatilization can be reduced to 1.08%, no bubble forms in the transparent BCRM, and controlled-release performance is acceptable under optimum conditions of initial temperature 1050 ℃, holding time 2 h and melting temperature 1050 ℃. Controlled-release mechanism of BCRM, affected by temperature, is Super Case II transport at 30 and 35 ℃ while it is non-Fickian diffusion at 40 ℃. However, the cumulative release rate of boron is greater than 95% at different temperatures.

Key words: borate, process parameter optimization, volatilization volume, release mechanism

中图分类号:

TB321

黄长兴, 崔骏, 裴元生. B₂O₃-SiO₂-Na₂O缓释材料的合成工艺参数优化及其缓释机理[J]. 无机材料学报, 2019, 34(6): 653-659.

Chang-Xing HUANG, Jun CUI, Yuan-Sheng PEI. B₂O₃-SiO₂-Na₂O Controlled-release Material: Synthetic Parameters Optimization and Release Mechanisms Exploration[J]. Journal of Inorganic Materials, 2019, 34(6): 653-659.

图/表 8

参考文献 35

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Release exponent, n	Release mechanism
Cylinder	Release mechanism
n ≤ 0.45	Fickian diffusion
0.45 < n < 0.89	Non-Fickian diffusion
n = 0.89	Case II transport
n > 0.89	Super Case II transport

Release exponent, n	Release mechanism
Cylinder	Release mechanism
n ≤ 0.45	Fickian diffusion
0.45 < n < 0.89	Non-Fickian diffusion
n = 0.89	Case II transport
n > 0.89	Super Case II transport

Conditions	Parameters	Boron concentration /(mg·L^-1)	Recovery/%	Theoretical values of B₂O₃/wt%	Test values of B₂O₃/wt%	B₂O₃ volatilization/%
Heating rate/ (℃?min^-1)	4	91.728	95.02-102.32	60	59.08	1.53
	6	90.657			58.39	2.68
	8	89.278			57.50	4.17
	10	87.638			56.44	5.93
Holding time/h	0.5	92.372	95.41-104.29	60	59.49	0.85
	1	91.808			59.13	1.45
	1.5	90.491			58.28	2.87
	2	90.442			58.25	2.92
Melting temperature/℃	1025	90.612	100.27-105.42	60	58.36	2.73
	1050	90.144			58.06	3.23
	1075	88.986			57.31	4.48
Initial temperature/℃	300	90.404	100.63-106.42	60	58.22	2.97
	800	91.300			58.80	2.00
	1050	92.148			59.35	1.08

Conditions	Parameters	Boron concentration /(mg·L^-1)	Recovery/%	Theoretical values of B₂O₃/wt%	Test values of B₂O₃/wt%	B₂O₃ volatilization/%
Heating rate/ (℃?min^-1)	4	91.728	95.02-102.32	60	59.08	1.53
	6	90.657			58.39	2.68
	8	89.278			57.50	4.17
	10	87.638			56.44	5.93
Holding time/h	0.5	92.372	95.41-104.29	60	59.49	0.85
	1	91.808			59.13	1.45
	1.5	90.491			58.28	2.87
	2	90.442			58.25	2.92
Melting temperature/℃	1025	90.612	100.27-105.42	60	58.36	2.73
	1050	90.144			58.06	3.23
	1075	88.986			57.31	4.48
Initial temperature/℃	300	90.404	100.63-106.42	60	58.22	2.97
	800	91.300			58.80	2.00
	1050	92.148			59.35	1.08

Before controlled-release		After controlled-release
Wavenumber/cm^-1	Corresponding characteristic vibrations ascription	Wavenumber/cm^-1	Corresponding characteristic vibrations ascription
463.46	Si-O-Si bending vibrations	466.53	Si-O-Si bending vibrations
694.02	[BO₃] bending vibrations	798.51	O-Si-O stretching vibrations
1061.16	Si-O-Si asymmetric stretching vibrations	1083.89	Si-O-Si asymmetric stretching vibrations
1268.39	[BO₃] stretching vibrations	1637.42	H₂O
1392.97	[BO₃] antisymmetry stretching vibrations	3448.34	H-O stretching vibrations
3448.20	H-O stretching vibrations

B₂O₃-SiO₂-Na₂O缓释材料的合成工艺参数优化及其缓释机理

B₂O₃-SiO₂-Na₂O Controlled-release Material: Synthetic Parameters Optimization and Release Mechanisms Exploration

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Temperature/℃	Models	R²
30	${{M}_{t}}/{{M}_{\infty }}=10.06{{t}^{0.97}}$	0.9959
35	${{M}_{t}}/{{M}_{\infty }}=14.33{{t}^{0.95}}$	0.9935
40	${{M}_{t}}/{{M}_{\infty }}=23.75{{t}^{0.77}}$	0.9574
45	-	-

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