基于Box-Behnken响应面法优化无水磷石膏疏水改性工艺

硅酸盐通报 ›› 2022, Vol. 41 ›› Issue (10): 3599-3607.

基于Box-Behnken响应面法优化无水磷石膏疏水改性工艺

刘浩¹, 聂晨晨¹, 李宏萍¹, 周俊¹, 杨兰文¹, 谢贵明^1,2

1.贵州大学化学与化工学院,贵阳 550025;
2.贵州省绿色化工与清洁能源技术重点实验室,贵阳 550025

收稿日期:2022-06-01 修回日期:2022-07-20 出版日期:2022-10-15 发布日期:2022-10-26
通讯作者: 谢贵明,博士,副教授。E-mail:gmxie@gzu.edu.cn
作者简介:刘浩(1997—),男,硕士研究生。主要从事复合材料的研究。E-mail:2929827559@qq.com
基金资助:
贵州省普通高等学校青年科技人才成长项目(黔教合KY字[2021]091);贵州大学培育项目([2020]64)

Optimization of Hydrophobic Modification Process of Anhydrous Phosphogypsum Based on Box-Behnken Response Surface Methodology

LIU Hao¹, NIE Chenchen¹, LI Hongping¹, ZHOU Jun¹, YANG Lanwen¹, XIE Guiming^1,2

1. School of Chemistry and Chemical Engineering, Guizhou University, Guiyang 550025, China;
2. Key Laboratory of Guizhou Province for Green Chemical Industry and Clean Energy Technology, Guiyang 550025, China

Received:2022-06-01 Revised:2022-07-20 Online:2022-10-15 Published:2022-10-26

摘要/Abstract

摘要： 磷石膏(PG)是磷酸湿法工艺中产生的固体废渣,大量堆存造成环境污染。PG经球磨和煅烧处理得到的无水磷石膏(APG)再经表面疏水改性后可用作高分子材料的填料,在材料中起到增韧、增强作用,提高材料的综合力学性能,成为PG资源化利用的一种有效途径。以APG为主要原料,以活化指数为响应值,通过单因素试验和响应面法对APG疏水改性工艺条件进行优化。结果表明,响应曲面建立的数学模型拟合度较高,NaOH浓度、KH570添加量和反应时间3个因素对活化指数均有显著影响,其中KH570添加量是影响改性效果的主要因素。APG最优疏水改性条件为:NaOH浓度2.6 mol/L,KH570添加量3.10 g,反应时间149 min。最优条件下改性APG的活化指数为0.968 9,接触角为84.51°。

关键词: 响应面法, 无水磷石膏, 填料, 改性, 活化指数, 疏水, 工艺优化

Abstract: Phosphogypsum (PG) is an industrial solid waste produced in the wet process of phosphoric acid, which piles up in large quantities and pollutes the environment. However, anhydrous phosphogypsum (APG) obtained by PG after ball milling and calcination can be used as filler for polymer materials after hydrophobic modification on the surface, to improve the comprehensive mechanical properties of the materials by toughening and strengthening the materials, and it is an effective way for the resource utilization of PG. In this study, taking APG as the main raw material and the activation index as the response value, the process conditions of hydrophobic modification of APG were optimized by single factor test and the response surface methodology. The results show that the mathematical model established by the response surface has a high fitting degree. NaOH concentration, KH570 dosage and reaction time have significant effects on the activation index, and the dosage of KH570 is the main factor affecting the modification. The optimal hydrophobic modification conditions of APG are as follows: NaOH concentration is 2.6 mol/L, KH570 dosage is 3.10 g, and the reaction time is 149 min. Under the optimal conditions, the activation index and contact angle of the modified APG are 0.968 9 and 84.51°, respectively.

Key words: response surface methodology, anhydrous phosphogypsum, filler, modification, activation index, hydrophobic, process optimization

中图分类号:

X705

刘浩, 聂晨晨, 李宏萍, 周俊, 杨兰文, 谢贵明. 基于Box-Behnken响应面法优化无水磷石膏疏水改性工艺[J]. 硅酸盐通报, 2022, 41(10): 3599-3607.

LIU Hao, NIE Chenchen, LI Hongping, ZHOU Jun, YANG Lanwen, XIE Guiming. Optimization of Hydrophobic Modification Process of Anhydrous Phosphogypsum Based on Box-Behnken Response Surface Methodology[J]. BULLETIN OF THE CHINESE CERAMIC SOCIETY, 2022, 41(10): 3599-3607.

参考文献

[1] 石鑫,杨绍利,马兰.“三石膏”综合利用现状及其新工艺[J].现代化工,2020,40(9):8-13+19.
SHI X, YANG S L, MA L. Present situation of comprehensive utilization of “three-gypsum” and new technologies[J]. Modern Chemical Industry, 2020, 40(9): 8-13+19 (in Chinese).
[2] REN H M, LIU W B, ZHANG D W. Application of phosphogypsum to solidification of silty soil: mechanical properties and microstructure[J]. Mechanics of Advanced Materials and Structures, 2021: 1-13.
[3] TAYIBI H, CHOURA M, LÓPEZ F A, et al. Environmental impact and management of phosphogypsum[J]. Journal of Environmental Management, 2009, 90(8): 2377-2386.
[4] 刘露,练川,李星和,等.贵州省磷石膏综合利用现状[J].科技风,2019(1):171-171+179.
LIU L, LIAN C, LI X H, et al. Present situation of comprehensive utilization of phosphogypsum in Guizhou Province[J]. Technology Trend, 2019(1): 171-171+179. (in Chinese)
[5] 郑兴莉,刘心韵,付海,等.改性超细磷石膏对PE-HD力学性能的影响[J].工程塑料应用,2019,47(4):117-122.
ZHENG X L, LIU X Y, FU H, et al. Effect of modified ultrafine phosphogypsum on mechanical properties of PE-HD[J]. Engineering Plastics Application, 2019, 47(4): 117-122 (in Chinese).
[6] 岳文香.α-半水磷石膏晶须改性聚乙烯(PE)复合材料的研究[D].贵阳:贵州大学,2017.
YUE W X. Study on polyethylene(PE) composites modified by alpha-hemihydrate phosphogypsum whisker[D]. Guiyang: Guizhou University, 2017 (in Chinese).
[7] GONG S, LI X L, SONG F X, et al. Preparation and application in HDPE of nano-CaSO₄ from phosphogypsum[J]. ACS Sustainable Chemistry & Engineering, 2020, 8(11): 4511-4520.
[8] ALI Z M. A study of the effect of silica particles addition on some physical properties of PVC as a packaging material[J]. Iraqi Journal of Physics (IJP), 2019, 13(26): 76-91.
[9] ZHU D H, NAI X Y, LAN S J, et al. Surface modification of magnesium hydroxide sulfate hydrate whiskers using a silane coupling agent by dry process[J]. Applied Surface Science, 2016, 390: 25-30.
[10] PRAVEEN K M, THOMAS S, GROHENS Y, et al. Investigations of plasma induced effects on the surface properties of lignocellulosic natural coir fibres[J]. Applied Surface Science, 2016, 368: 146-156.
[11] LEE J H, ZAPATA P, CHOI S, et al. Effect of nanowhisker-modified zeolites on mechanical and thermal properties of poly(vinyl acetate) composites with pure-silica MFI[J]. Polymer, 2010, 51(24): 5744-5755.
[12] DANG L, NAI X Y, ZHU D H, et al. Study on the mechanism of surface modification of magnesium oxysulfate whisker[J]. Applied Surface Science, 2014, 317: 325-331.
[13] PRACHAYAWARAKORN J, KHUNSUMLED S, THONGPIN C, et al. Effects of silane and MAPE coupling agents on the properties and interfacial adhesion of wood-filled PVC/LDPE blend[J]. Journal of Applied Polymer Science, 2008, 108(6): 3523-3530.
[14] NAKAMURA Y, HARADA A, GOTOH T, et al. Effect of silane chain length on the mechanical properties of silane-treated glass beads-filled PVC[J]. Composite Interfaces, 2007, 14(2): 117-130.
[15] WANG Q H, LUO Y Y, FENG C F, et al. Reinforcement of natural rubber with core-shell structure silica-poly(methyl methacrylate) nanoparticles[J]. Journal of Nanomaterials, 2012, 2012: 782986.
[16] SUN M, SUN Q, ZHANG J, et al. Surface modification of phosphogypsum and application in polyolefin composites[J]. Environmental Science and Pollution Research, 2022, 29: 66177-66190.
[17] ZHAO F, HUANG Y D. Preparation and properties of polyhedral oligomeric silsesquioxane and carbon nanotube grafted carbon fiber hierarchical reinforcing structure[J]. Journal of Materials Chemistry, 2011, 21(9): 2867-2870.
[18] CHEN H Y, WANG J, MA P Y, et al. Influence of hydroxylation on fabrication of PVC/CaSO₄ composite[J]. Applied Surface Science, 2015, 357: 2320-2326.
[19] 刘娜,陈灵智,张彦,等.响应面优化超声提取汉麻大麻素及其抗氧化性研究[J].现代化工,2019,39(1):144-149.
LIU N, CHEN L Z, ZHANG Y, et al. Response surface optimization on ultrasound-assisted extraction of hemp cannabinoids and study on anti-oxidation property[J]. Modern Chemical Industry, 2019, 39(1): 144-149 (in Chinese).
[20] 雷文平,吴诗敏,李彩虹,等.响应面法优化凝固型发酵椰奶工艺[J].中国酿造,2019,38(2):212-216.
LEI W P, WU S M, LI C H, et al. Process optimization of set-style fermented coconut milk by response surface methodology[J]. China Brewing, 2019, 38(2): 212-216 (in Chinese).
[21] 李正月,李东泽,孙秀英,等.球磨辅助海藻酸钠降解工艺参数的优化及其产物的结构和性能[J].材料导报,2022,36(6):208-213.
LI Z Y, LI D Z, SUN X Y, et al. Process optimization for ball milling-assisted degradation of sodium alginate as well as its structure and property[J]. Materials Reports, 2022, 36(6): 208-213 (in Chinese).
[22] 李莉,张赛,何强,等.响应面法在试验设计与优化中的应用[J].实验室研究与探索,2015,34(8):41-45.
LI L, ZHANG S, HE Q, et al. Application of response surface methodology in experiment design and optimization[J]. Research and Exploration in Laboratory, 2015, 34(8): 41-45 (in Chinese).
[23] 陈曦,李国林,陈梦玉,等.响应面法优化发酵蓝莓果醋发酵工艺条件[J].中国酿造,2018,37(9):67-71.
CHEN X, LI G L, CHEN M Y, et al. Optimization of blueberry vinegar fermentation process by response surface methodology[J]. China Brewing, 2018, 37(9): 67-71 (in Chinese).
[24] 吴婧婧,梁贵秋,陆春霞,等.响应面法对桑果醋发酵工艺的优化[J].南方农业学报,2014,45(2):278-284.
WU J J, LIANG G Q, LU C X, et al. Optimization of fermentation process for mulberry vinegar by response surface methodology[J]. Journal of Southern Agriculture, 2014, 45(2): 278-284 (in Chinese).