响应曲面法优化粉煤灰、赤泥和污泥基陶粒制备及除水中低浓度铅机制

赵明佳; 杨毅; 赵睿; 董承璇; 舒麒麟

doi:10.13205/j.hjgc.202504024

响应曲面法优化粉煤灰、赤泥和污泥基陶粒制备及除水中低浓度铅机制

doi: 10.13205/j.hjgc.202504024

赵明佳¹,
杨毅^1,2,3,,
赵睿¹,
董承璇¹,
舒麒麟^1,2,3

1. 西安建筑科技大学环境与市政工程学院,西安 710055;
2. 西安建筑科技大学陕西省环境工程重点实验室,西安 710055;
3. 西安建筑科技大学西北水资源与环境生态教育部重点实验室,西安 710055

基金项目:

国家自然科学基金项目（52070154；21407119）；陕西省自然科学基础研究计划项目（2021JM-375）；西安建筑科技大学自然科学专项（ZR21019）

详细信息

作者简介:
赵明佳（1998-），女，硕士研究生，主要研究方向为固体废物资源化利用。1625267577@qq.com

通讯作者:
杨毅（1976-），女，博士，副教授，主要研究方向为固体废物资源化与环境中溶解性有机物的特性。yangyi@xauat.edu.cn
杨毅（1976-），女，博士，副教授，主要研究方向为固体废物资源化与环境中溶解性有机物的特性。yangyi@xauat.edu.cn

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出版历程
- 收稿日期: 2023-08-02
- 录用日期: 2024-01-22
- 修回日期: 2023-12-26
- 刊出日期: 2025-04-01

Optimization of preparation of ceramsite using fly ash， red mud and sludge by response surface methodology and its lead removal mechanism

ZHAO Mingjia¹,
YANG Yi^{1,2,3
,},
ZHAO Rui¹,
DONG Chengxuan¹,
SHU Qilin^1,2,3

1. School of Environmental and Municipal Engineering, Xi'an University of Architecture and Technology, Xi'an 710055, China;
2. Key Laboratory of Environmental Engineering, Shaanxi Province, Xi'an University of Architecture and Technology, Xi'an 710055, China;
3. Key Laboratory of Northwest Water Resource, Environment and Ecology, Ministry of Education, Xi'an University of Architecture and Technology, Xi'an 710055, China

摘要

摘要: 以粉煤灰、赤泥和污泥为原料采用烧结法制陶粒，在单因素实验基础上利用响应曲面法优化陶粒制备条件，根据陶粒表征分析及吸附动力学和吸附等温模型拟合探究其对水中低浓度Pb²⁺吸附特性。结果表明：响应曲面模型拟合预测效果较好，实测值与预测值的相对误差为1.75%；制备因素对陶粒吸附Pb²⁺效果影响顺序为烧结温度 > 烧结时间 > 预热温度。在原料（粉煤灰：赤泥：污泥）质量比为75∶20∶5、预热温度359 ℃、烧结温度1053 ℃、烧结时间9 min条件下制备陶粒，对Pb²⁺初始浓度为10 mg/L的去除率和吸附量分别为91.05%和9.11 mg/g。陶粒对Pb²⁺（初始浓度分别为5，10 mg/L）的吸附符合准二级动力学模型（R²分别为0.9992和0.9981）和Langmuir吸附等温模型（R²分别为0.9986和0.9967），吸附过程中O—H、C＝O、C＝C、Si—O和Al—O起重要作用，吸附Pb²⁺后陶粒矿物成分的结晶度减少。
- 响应曲面法 /
- 固体废物 /
- 陶粒 /
- Pb²⁺ /
- 吸附 /
- 机理
Abstract: Fly ash， red mud， and sludge were utilized as raw materials to prepare the ceramsite by the sintering method in this research， to investigate the adsorption effect of ceramsite and mechanism for Pb²⁺ removal. The optimal conditions for preparing ceramsite of fly ash， red mud， and sludge were determined by using the response surface method on the basis of the insights gained from preliminary single factor experiments. In order to investigate the adsorption characteristics of the ceramsite on low concentrations of Pb²⁺ in water， characterization analysis was conducted on the ceramsite， combined with the adsorption kinetics and adsorption isotherm model fitting. The results showed that the response surface model had a good prediction performance， and the relative error between the measured values and the predicted values was 1.75%. The influence of each preparation factor on the adsorption effect of Pb²⁺ on ceramsite followed a descending order of sintering temperature， sintering time and preheating temperature. The ceramsite prepared in the conditions of raw material ratio （fly ash：red mud：sludge） of 75∶20∶5， preheating temperature of 359℃， sintering temperature of 1053℃， and sintering time of 9 min had the best adsorption performance， and the removal rate and adsorption capacity of Pb²⁺ at an initial concentration of 10 mg/L by the ceramsite were found to be 91.05% and 9.11 mg/g， respectively. The adsorption process of Pb²⁺ with an initial concentration of 5， 10mg/L by ceramsite， was in accordance with the quasi secondary kinetic model （with the R² of 0.9992 and 0.9981， respectively） and Langmuir adsorption isothermal model （with the R² of 0.9986 and 0.9967， respectively）. The functional groups such as O—H， C＝O， C＝C， Si—O and Al—O played an important role in the adsorption process of Pb²⁺ by ceramsite. The crystallinity of ceramsite mineral components decreased after the adsorption of Pb²⁺.
- response surface methodology /
- solid waste /
- ceramsite /
- Pb²⁺ /
- adsorption /
- mechanism

HTML全文

1 原料配比对Pb²⁺吸附效果的影响

1. Effects of raw material ratio on the adsorption of Pb²⁺

下载: 全尺寸图片幻灯片

2 陶粒制备条件对Pb²⁺吸附效果的影响

2. Effects of preparation conditions of ceramsite on the adsorption of Pb²⁺

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3 预热温度、烧结温度和烧结时间对吸附效果的响应曲面

3. Response surface diagrams of preheating temperature， sintering temperature， and sintering time to adsorption efficiency

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4 陶粒吸附Pb²⁺前后的FTIR图谱

4. FTIR spectra of the ceramsite before and after Pb²⁺ adsorption

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5 陶粒吸附Pb²⁺前后的SEM图像

5. SEM images of ceramsite before and after Pb²⁺ adsorption

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6 陶粒的X射线衍射图谱

6. X-ray diffraction patterns of ceramsite

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1 原料的主要成分

1. Main components of raw materials

原料	SiO₂	Al₂O₃	Fe₂O₃	TiO₂	MgO	Na₂O
粉煤灰	56.74	24.58	6.55	1.86	1.45	1.34
赤泥	25.79	11.06	7.39	2.02	1.01	1.11
脱水污泥	31.25	7.67	18.61	3.02	0.85	1.06

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2 实验因素与水平

2. Experimental factors and levels

水平	A预热温度/℃	B烧结温度/℃	C烧结时间/min
-1	300	1025	5
0	350	1050	10
1	400	1075	15

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3 响应曲面实验设计及实验结果

3. Experimental design and results of response surface

编号	A（预热温度/℃）	B（烧结温度/℃）	C（烧结时间/min）	D（去除率/%）	编号	A（预热温度/℃）	B（烧结温度/℃）	C（烧结时间/min）	D（去除率/%）
1	350	1050	10	93.49	10	350	1025	15	70.96
2	300	1050	5	87.53	11	300	1050	15	80.91
3	400	1075	10	81.06	12	350	1025	5	75.78
4	400	1050	15	87.93	13	400	1050	5	87.54
5	350	1050	10	91.81	14	400	1025	10	74.26
6	300	1025	10	75.05	15	350	1075	15	75.06
7	350	1050	10	92.27	16	350	1050	10	90.23
8	300	1075	10	78.21	17	350	1075	5	80.82
9	350	1050	10	93.21	—	—	—	—	—

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4 回归方程方差分析

4. Analysis of variance for regression equations

项目	平方和	自由度	均方	F值	P值
Model	917.29	9	101.92	58.20	< 0.0001
A	10.33	1	10.33	5.90	0.0455
B	45.60	1	45.60	26.04	0.0014
C	35.32	1	35.32	20.17	0.0028
AB	3.31	1	3.31	1.89	0.2114
AC	12.29	1	12.29	7.01	0.0330
BC	0.22	1	0.22	0.13	0.7329
A²	23.60	1	23.60	13.47	0.0080
B²	678.02	1	678.02	387.15	< 0.0001
C²	62.65	1	62.65	35.77	0.0006
残差	12.26	7	1.75	‒	‒
失拟项	5.64	3	1.85	1.10	0.4468
纯误差	6.72	4	1.68	‒	‒
总离差	929.55	16	‒	‒	‒

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5 准一级动力学模型拟合参数

5. Fitting parameters of the quasi first order kinetic model

初始浓度	q/(mg/g)	q_e/(mg/g)	K₁/min^-1	R²
5 mg/L	4.66	1.63	0.0048	0.8765
10 mg/L	9.20	4.23	0.0059	0.9372

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6 准二级动力学模型拟合参数

6. Fitting parameters of the quasi second order kinetic model

初始浓度	q/(mg/g)	q_e/(mg/g)	K₂/[g/(mg∙min)]	R²
5 mg/L	4.66	4.79	0.0068	0.9992
10 mg/L	9.20	9.67	0.0025	0.9981

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7 颗粒内扩散学模型拟合参数

7. Fitting parameters of the intragranular diffusion model

初始浓度	K_p₁/[mg/(g·min^1/2)]	R₁²	C₁	K_p₂/[mg/(g·min^1/2)]	R₂²	C₂
5 mg/L	0.14151	0.9710	1.98996	0.0067	0.7596	4.38906
10 mg/L	0.3029	0.9852	3.40667	0.02136	0.9729	8.53676

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8 吸附等温模型拟合参数

8. Parameters of adsorption isothermal model fitting results

温度/℃	Langmuir吸附模型			Freundlich吸附模型			Temkin吸附模型
温度/℃	q_max/(mg/g)	K_L/(L/mg)	R²	K_F/{mg/[g·(1/mg)^1/ⁿ ]}	1/n	R²	B_T	K_T/(L/mg)	R²
25	15.63	1.42	0.9986	7.59	0.49	0.8961	3.13	17.12	0.9777
35	18.14	1.28	0.9967	8.64	0.52	0.9526	3.51	17.09	0.9817

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