电解锰渣-赤泥路面砖中锰的浸出行为研究及长期释放预测

刘博; 梁宇廷; 孟棒棒; 岳波; 王涛; 高红

doi:10.13198/j.issn.1001-6929.2023.09.01

电解锰渣-赤泥路面砖中锰的浸出行为研究及长期释放预测

doi: 10.13198/j.issn.1001-6929.2023.09.01

刘博^{1, 2,},
梁宇廷²,
孟棒棒²,
岳波^2, ,,
王涛^{1, 2},
高红^1, ,

1.
昆明理工大学建筑工程学院，云南昆明　650504
2.
中国环境科学研究院固体废物污染控制技术研究所，北京　100012

基金项目: 贵州省交通运输厅科技项目(No.2021-122-005)；贵州省科技计划项目(No.黔科合重大专项[2022]002)

详细信息

作者简介:
刘博（1997-），男，河南商丘人，1014501187@qq.com

通讯作者:
①岳波(1980-)，男，重庆人，研究员，博士，主要从事固体废物污染防治研究，yuebo@craes.org.cn

②高红(1967-)，男，云南昆明人，讲师，博士，主要从事固体废物污染防治研究，gaohong208@163.com

中图分类号: X705
计量
- 文章访问数: 63
- HTML全文浏览量: 9
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- 被引次数: 0
出版历程
- 收稿日期: 2023-07-14
- 修回日期: 2023-08-21
- 网络出版日期: 2023-09-05

Study on Leaching Behavior of Manganese in Electrolytic Manganese Residue and Red Mud Paving Bricks and Long-Term Release Prediction

LIU Bo^{1, 2
,},
LIANG Yuting²,
MENG Bangbang²,
YUE Bo^{2
, ,},
WANG Tao^{1, 2},
GAO Hong^{1
, ,}

1.
Faculty of Civil Engineering and Mechanics, Kunming University of Science and Technology, Kunming 650504, China
2.
Research Institute of Solid Waste Management, Chinese Research Academy of Environmental Sciences, Beijing 100012, China

Funds: Guizhou Provincial Department of Transportation Science and Technology Project, China (No.2021-122-005); Guizhou Provincial Science and Technology Plan Project, China (No.Qiankehe Major Special Project [2022]002)

摘要

摘要: 电解锰渣和赤泥是电解锰和氧化铝生产过程中的副产物，由于缺乏有效的管理手段，导致其存量持续积累，造成了严重的环境影响和资源浪费，因此有必要对其进行资源化利用，以减小环境影响并促进冶炼锰、铝行业的绿色可持续发展. 该研究使用无害化渣和水洗无害化渣，结合水泥、石料和河砂等原料，按一定配比制备得到透水混凝土路面砖(permeable concrete paving bricks，PCB)和水洗透水混凝土路面砖(washed permeable concrete paving bricks，WPCB)，为评估两种路面砖在柳州市长期使用过程中存在的潜在环境风险，采用欧盟标准化组织制定的NEN 7375方法研究特征污染物Mn²⁺的浸出行为，通过多种动力学方程拟合并预测Mn²⁺的浸出行为，并借助IWEM模型对路面砖的拟利用路面区域进行评估. 结果表明：①在相同的配比条件下，WPCB中Mn²⁺的累积释放量较PCB更低；在不同的配比条件下，Mn²⁺的累积释放量随渣掺量的增加呈现先降低后升高的趋势. ②除水洗无害化渣和水泥掺量分别为8%和25%的WPCB-2在全浸出阶段中Mn²⁺的浸出行为受扩散控制影响外，其余样品均受表面冲刷影响. ③对于选取的4种动力学方程，Elovich方程更适合描述Mn²⁺的浸出行为，且PCB和WPCB于10年和20年内Mn²⁺的预计释放量分别在1.51~13.78和1.71~16.54 μg/kg之间. ④IWEM模型的模拟结果显示，路面砖符合环境安全性要求. 研究显示，两种无害化渣所制得的路面砖在实际应用场景中均无潜在的环境风险，可进一步扩展其资源化利用场景.
- 电解锰渣 /
- 赤泥 /
- 路面砖 /
- 浸出行为 /
- 动力学方程
Abstract: Electrolytic manganese residue and red mud are byproducts during production of electrolytic manganese and aluminum oxide. Due to insufficient management, these substances accumulate, causing environmental problems and resource waste. Thus, resource utilization becomes necessary to mitigate the impacts and promote the sustainable development of related industries. This study utilized harmless slag and washed harmless slag, and combined with materials such as cement, stone, and river sand in specific proportions to fabricate permeable concrete paving bricks (PCB) and water-washed permeable concrete paving bricks (WPCB). In order to evaluate the environmental risks during the long-term use of PCB and WPCB in Liuzhou City, the study adopted the NEN 7375 method established by the European Union Standardization Organization. This method used a variety of kinetic equations to study the leaching behavior of the characteristic contaminant manganese. Furthermore, the manganese leaching behavior was delineated through the fitting and prediction of numerous kinetic equations, while the IWEM model was employed to assess the prospective utilization of these paving bricks in road areas. The research results show that: (1) Under identical proportioning conditions, the cumulative release of Mn²⁺ in WPCB is notably lower than that in PCB. Moreover, under different proportioning conditions, the cumulative release of Mn²⁺ shows a trend of initially diminishing and subsequently escalating with the increase in slag content. (2) In addition to washed harmless slag and WPCB-2 with cement content of 8% and 25% respectively, which is influenced by diffusion-controlled leaching throughout the complete leaching phase, the other samples were largely impacted by surface flushing. (3) Among the four selected kinetic equations, the Elovich equation is more suitable for describing Mn²⁺ leaching behavior. The releases were estimated from 1.51 μg/kg to 13.78 μg/kg over 10 years and from 1.71 μg/kg to 16.54 μg/kg over 20 years. (4) The simulation results of the IWEM model reveal that the pavement bricks meet the requisites of environmental safety. Both types of slag-derived bricks showed no latent environmental risks, thus paving the way for an expanded horizon in their resourceful utilization.
- electrolytic manganese residue /
- red mud /
- paving bricks /
- leaching behavior /
- kinetic equations

HTML全文

图 1 电解锰渣、赤泥和粉煤灰的XRD图

Figure 1. XRD patterns of the electrolytic manganese residue, red mud, and coal fly ash

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图 2 试验工艺流程

Figure 2. Flowchart of the experimental

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图 3 试验装置示意

注：1—PCB/WPCB；2—出水阀门；3—试块支架.

Figure 3. Illustration of the experimental setup

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图 4 路面砖暴露场景示意

Figure 4. Diagram of paving brick in an exposed setting

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图 5 PCB和WPCB浸出液的pH、密度和渗透系数

Figure 5. Graph of pH, density, and permeability coefficient of leaching solution for PCB and WPCB

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图 6 PCB和WPCB在各阶段中Mn²⁺的浸出行为

Figure 6. Leaching behavior of Mn²⁺during the leaching stages of PCB and WPCB

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图 7 污染物的主要释放机制和影响因素

Figure 7. Primary release mechanisms and influencing factors of pollutants

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图 8 双常数方程、Elovich方程、抛物线方程和二级动力学方程拟合曲线

Figure 8. Dual-constant equation, Elovich equation, parabolic equation, and second-order kinetic equation fitted curves

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图 9 IWEM模拟地下水流向、监测井方位与拟评估路段关系示意

Figure 9. Schematic diagram of the relationship between the simulated groundwater flow direction, monitoring well orientation, and the proposed evaluation section in the IWEM model

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表 1 供试材料基本性质及化学成分

Table 1. Fundamental characteristics and chemical composition of raw materials

供试材料	pH	含水率/%	化学成分占比/%
供试材料	pH	含水率/%	SiO₂	CaO	Fe₂O₃	MnO	Al₂O₃	TiO₂	MgO	Na₂O	K₂O	SO₃
电解锰渣	6.59	31.67	32.85	18.49	14.07	7.93	2.43	—	2.10	—	—	8.99
赤泥	11.90	33.84	5.68	10.00	47.28	—	12.24	4.61	—	3.76	—	—
粉煤灰	8.95	0.85	53.63	4.75	4.83	—	30.02	—	—		2.08	—

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表 2 不同路面砖中原材料配比

Table 2. Composition of raw materials in various paving bricks

样品编号	质量比/%
样品编号	无害化渣/水洗无害化渣	水泥	石料	河砂
PCB-1/WPCB-1	6	27	50	17
PCB-2/WPCB-2	8	25	50	17
PCB-3/WPCB-3	10	23	50	17
PCB-4/WPCB-4	12	21	50	17
PCB-5/WPCB-5	14	19	50	17
PCB-6/WPCB-6	16	17	50	17
PCB-7/WPCB-7	18	15	50	17
PCB-8/WPCB-8	20	13	50	17

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表 3 不同浸出阶段的释放机制

Table 3. Mechanisms of release in different leaching stages

浸出区间	rc≤0.35	0.35＜rc≤0.65	rc>0.65
rc_2-7	表面冲刷	扩散控制	溶解作用
rc_5-8	耗竭作用	扩散控制	溶解作用
rc_4-7	耗竭作用	扩散控制	溶解作用
rc_3-6	耗竭作用	扩散控制	溶解作用
rc_2-5	耗竭作用	扩散控制	溶解作用
rc_1-4	表面冲刷	扩散控制	延滞作用

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表 4 不同配比路面砖的浸出试验液固比

Table 4. Liquid-to-solid ratios in leaching experiments of different paving bricks

砖体编号	液固比/(L/kg)	砖体编号	液固比/(L/kg)
PCB-1	2.01	WPCB-1	2.04
PCB-2	2.05	WPCB-2	2.15
PCB-3	2.29	WPCB-3	2.04
PCB-4	1.97	WPCB-4	1.94
PCB-5	1.94	WPCB-5	1.83
PCB-6	2.07	WPCB-6	2.00
PCB-7	2.20	WPCB-7	2.15
PCB-8	2.32	WPCB-8	2.23

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表 5 Mn²⁺在不同浸出阶段下的释放机制

Table 5. Mechanisms of Mn²⁺ release at different stages

浸出阶段	PCB-1	PCB-2	PCB-3	PCB-4	PCB-5	PCB-6	PCB-7	PCB-8
阶段2-7	表面冲刷	表面冲刷	表面冲刷	表面冲刷	表面冲刷	表面冲刷	表面冲刷	表面冲刷
阶段5-8	耗竭作用	耗竭作用	耗竭作用	耗竭作用	耗竭作用	耗竭作用	耗竭作用	耗竭作用
阶段4-7	耗竭作用	耗竭作用	耗竭作用	耗竭作用	耗竭作用	耗竭作用	耗竭作用	耗竭作用
阶段3-6	耗竭作用	耗竭作用	耗竭作用	耗竭作用	耗竭作用	耗竭作用	耗竭作用	耗竭作用
阶段2-5	耗竭作用	耗竭作用	耗竭作用	耗竭作用	耗竭作用	耗竭作用	耗竭作用	耗竭作用
阶段1-4	表面冲刷	表面冲刷	表面冲刷	表面冲刷	扩散控制	表面冲刷	扩散控制	扩散控制

浸出阶段	WPCB-1	WPCB-2	WPCB-3	WPCB-4	WPCB-5	WPCB-6	WPCB-7	WPCB-8
阶段2-7	表面冲刷	扩散控制	表面冲刷	表面冲刷	表面冲刷	表面冲刷	表面冲刷	表面冲刷
阶段5-8	耗竭作用	扩散控制	耗竭作用	耗竭作用	耗竭作用	耗竭作用	耗竭作用	耗竭作用
阶段4-7	耗竭作用	扩散控制	耗竭作用	耗竭作用	耗竭作用	耗竭作用	耗竭作用	耗竭作用
阶段3-6	耗竭作用	扩散控制	耗竭作用	耗竭作用	耗竭作用	耗竭作用	耗竭作用	耗竭作用
阶段2-5	耗竭作用	扩散控制	耗竭作用	耗竭作用	耗竭作用	耗竭作用	耗竭作用	耗竭作用
阶段1-4	表面冲刷	扩散控制	表面冲刷	扩散控制	表面冲刷	表面冲刷	扩散控制	扩散控制

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表 6 Mn²⁺的预测模型及预测释放量

Table 6. Predictive model for Mn²⁺ and predicted release quantity

砖体编号	符合模型	模型表达式	R²	残差平方和	Mn²⁺的10年预测释放量/(μg/kg)	Mn²⁺的20年预测释放量/(μg/kg)
PCB-1	双常数方程	Q=exp(0.184 7ln t+1.256 4)	0.930 0	0.104 8	5.37	6.11
PCB-2	Elovich方程	Q=1.164 2ln t+4.389 1	0.939 4	0.201 9	8.33	9.03
PCB-3	Elovich方程	Q=0.529 7ln t+1.223 9	0.986 5	0.008 9	4.16	4.85
PCB-4	Elovich方程	Q=0.620 9ln t+1.289 6	0.991 9	0.006 7	2.72	3.15
PCB-5	二级动力学方程	Q=t/(0.213 0t+0.701 2)	0.975 8	0.045 9	3.53	4.03
PCB-6	Elovich方程	Q=1.178 4ln t+2.653 7	0.965 7	0.114 0	5.37	6.18
PCB-7	Elovich方程	Q=2.703 8ln t+4.771 8	0.983 7	0.253 2	11.00	12.87
PCB-8	Elovich方程	Q=3.981 2ln t+4.615 1	0.996 1	0.137 9	13.78	16.54
WPCB-1	Elovich方程	Q=1.081 7ln t+2.572 3	0.969 7	0.084 4	5.47	6.28
WPCB-2	双常数方程	Q=e^{(0.460 2ln t+0.213 3)}	0.995 3	0.025 7	3.57	4.91
WPCB-3	Elovich方程	Q=0.677 9ln t+1.684 4	0.995 5	0.004 5	3.25	3.72
WPCB-4	Elovich方程	Q=0.899 6ln t+0.684 2	0.995 8	0.007 5	2.76	3.38
WPCB-5	Elovich方程	Q=0.284 2ln t+0.776 6	0.985 1	0.002 8	1.51	1.71
WPCB-6	Elovich方程	Q=0.615 7ln t+1.206 5	0.995 3	0.003 9	2.62	3.05
WPCB-7	Elovich方程	Q=2.381 2ln t+3.600 6	0.985 0	0.181 1	9.08	10.73
WPCB-8	Elovich方程	Q=2.851 9ln t+4.026 0	0.989 9	0.177 3	10.59	12.57

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电解锰渣-赤泥路面砖中锰的浸出行为研究及长期释放预测

doi: 10.13198/j.issn.1001-6929.2023.09.01

作者简介:
刘博（1997-），男，河南商丘人，1014501187@qq.com

通讯作者:
①岳波(1980-)，男，重庆人，研究员，博士，主要从事固体废物污染防治研究，yuebo@craes.org.cn

②高红(1967-)，男，云南昆明人，讲师，博士，主要从事固体废物污染防治研究，gaohong208@163.com

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Study on Leaching Behavior of Manganese in Electrolytic Manganese Residue and Red Mud Paving Bricks and Long-Term Release Prediction

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电解锰渣-赤泥路面砖中锰的浸出行为研究及长期释放预测

doi: 10.13198/j.issn.1001-6929.2023.09.01

作者简介: 刘博（1997-），男，河南商丘人，1014501187@qq.com

通讯作者: ①岳波(1980-)，男，重庆人，研究员，博士，主要从事固体废物污染防治研究，yuebo@craes.org.cn ②高红(1967-)，男，云南昆明人，讲师，博士，主要从事固体废物污染防治研究，gaohong208@163.com

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Study on Leaching Behavior of Manganese in Electrolytic Manganese Residue and Red Mud Paving Bricks and Long-Term Release Prediction

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出版历程

目录

作者简介:
刘博（1997-），男，河南商丘人，1014501187@qq.com

通讯作者:
①岳波(1980-)，男，重庆人，研究员，博士，主要从事固体废物污染防治研究，yuebo@craes.org.cn

②高红(1967-)，男，云南昆明人，讲师，博士，主要从事固体废物污染防治研究，gaohong208@163.com