硅铝添加剂对机械化学法稳定飞灰中重金属的影响机制研究

doi:10.19964/j.issn.1006-4990.2022-0401

Abstract

Abstract:

Bentonite，kaolin，silica fume and red mud were used as silicon-aluminum additives to stabilize heavy metals in municipal solid waste incineration（MSWI） fly ash（FA） by mechanochemical method.The experiment results indicated that the composition of the immobilized products was related to the Si/Al ratio of the additives.There were okenite，calcite and calcium oxide in immobilized products derived by adding bentonite.The main phases of immobilized products were hydrocalumite and calcite，when kaolin or red mud was used as additive.For silica fume，calcite and a few of calsil were found in immobilized products.The agglomeration would happen after mechanochemical process，which leading to increasing of the pore diameter.The results showed that the leaching of Pb and Zn was inhibited after mechanochemical process.Furthermore，the oxidable form and residual form of Pb and Zn in FA was increased after mechanochemical reaction with silicon-aluminum additives.By comprehensive comparison，the order of immobilization effect was red mud>kaolin≈silica fume>bentonite.The encapsulation and agglomeration of particles，newly formed hydrocalumite and calsil，the elution of soluble salt were major cause of the solidification/stabilization of heavy metals in MSWI fly ash by mechanochemical method with external silicon-aluminum additives.

Key words: fly ash, mechanochemistry, heavy metals, red mud

CLC Number:

X705

LI Wen, WANG Wenxiang, FANG Hongsheng, WU Pingxiao. Study on effect mechanism of silicon-aluminum additives on stabilization of heavy metals in fly ash by mechanochemical stabilization method[J]. Inorganic Chemicals Industry, 2023, 55(4): 84-91.

Figures/Tables 10

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References 31

1	刘雪梅，罗思梦.固化稳定化技术对垃圾焚烧飞灰中重金属的研究[J].应用化工，2022，51（3）：816-820.
	LIU Xuemei， LUO Simeng.Study on heavy metals in MSWI fly ash by solidification stabilization technology[J].Applied Chemical Industry，2022，51（3）：816-820.
2	马懿，郑仁栋，周志昊，等.生活垃圾焚烧飞灰处置技术与应用瓶颈[J].环境工程，2022，40（5）：237-243.
	MA Yi， ZHENG Rendong， ZHOU Zhihao，et al.Bottleneck and disposal technology of fly ash from municipal solid waste incineration[J].Environmental Engineering，2022，40（5）：237-243.
3	杨延梅，慕宗宇，王菲，等.螯合剂固化生活垃圾焚烧飞灰中重金属的机理研究进展[J].环境科学研究，2022，35（10）：2388-2395.
	YANG Yanmei， MU Zongyu， WANG Fei，et al.Review on mechanisms of chelating agents to solidify heavy metals in municipal solid waste incineration fly ash[J].Research of Environmental Sciences，2022，35（10）：2388-2395.
4	王文祥，李宝花，周海彪，等.水洗-球磨法降解飞灰中二噁英的研究[J].环境科学学报，2017，37（6）：2232-2237.
	WANG Wenxiang， LI Baohua， ZHOU Haibiao，et al.Degradation of dioxin in fly ash by water-ball milling process[J].Acta Scientiae Circumstantiae，2017，37（6）：2232-2237.
5	CHEN Zhiliang， TANG Minghui， LU Shengyong，et al.Mechanochemical degradation of PCDD/Fs in fly ash within different milling systems[J].Chemosphere，2019，223：188-195.
6	HU Jun， HUANG Zhiyong， YU Jianming.Highly-effective mechanochemical destruction of hexachloroethane and hexachlorobenzene with Fe/Fe₃O₄ mixture as a novel additive[J].Science of the Total Environment，2019，659：578-586.
7	CHEN Zhiliang， LU Shengyong， TANG Minghui，et al.Mechanochemical stabilization of heavy metals in fly ash with additives[J].The Science of the Total Environment，2019，694.Doi：10.1016/j.scitotenv.2019.133813 .
8	YUAN Qixin， ZHANG Yongsheng， WANG Tao，et al.Mechanochemical stabilization of heavy metals in fly ash from coal-fired power plants via dry milling and wet milling[J].Waste Management，2021，135：428-436.
9	SHI Dezhi， HU Chunyan， ZHANG Jinlu，et al.Silicon-aluminum additives assisted hydrothermal process for stabilization of heavy metals in fly ash from MSW incineration[J].Fuel Processing Technology，2017，165：44-53.
10	LI Xinying， CHEN Quanyuan， ZHOU Yasu，et al.Stabilization of heavy metals in MSWI fly ash using silica fume[J].Waste Management，2014，34（12）：2494-2504.
11	金会心，王尚杰夫，肖媛丹，等.赤泥与粉煤灰资源特性及其协同利用现状研究[J].贵州大学学报：自然科学版，2022，39（2）：18-26.
	JIN Huixin， WANG Shangjiefu， XIAO Yuandan，et al.Study on the characteristics and collaborative utilization of red mud and fly ash resources[J].Journal of Guizhou University：Natural Sciences，2022，39（2）：18-26.
12	YU Shuyao， DU Bing， BAHEIDUOLA A，et al.HCB dechlorination combined with heavy metals immobilization in MSWI fly ash by using n-Al/CaO dispersion mixture[J].Journal of Hazardous Materials，2020，392.Doi：10.1016/j.jhazmat.2020.122510 .
13	ROJAS R.Copper，lead and cadmium removal by Ca Al layered double hydroxides[J].Applied Clay Science，2014，87：254-259.
14	LIU Qiang， LI Yajun， ZHANG Jia，et al.Effective removal of zinc from aqueous solution by hydrocalumite[J].Chemical Engineering Journal，2011，175：33-38.
15	向跟华，刘涛，张一敏，等.页岩提钒中和渣制备硫酸钙晶须填料的研究[J].无机盐工业，2018，50（10）：48-53.
	XIANG Genhua， LIU Tao， ZHANG Yimin，et al.Study on preparation of calcium sulfate whisker filler from shale vanadium neutralized slag[J].Inorganic Chemicals Industry，2018，50（10）：48-53.
16	朱莹，丁竑瑞，李艳，等.不同亚类硅酸盐矿物的中红外光谱学特征[J].矿物学报，2019，39（2）：173-182.
	ZHU Ying， DING Hongrui， LI Yan，et al.The middle-infrared spectroscopic characteristics of several common silicate minerals[J].Acta Mineralogica Sinica，2019，39（2）：173-182.
17	朱莹，丁竑瑞，李艳，等.含白云石天然碳酸盐岩在中红外波段的辐射特性研究[J].岩石矿物学杂志，2019，38（6）：743-752.
	ZHU Ying， DING Hongrui， LI Yan，et al.A study of the middle in-frared emission properties of dolomitic natural carbonate rock[J].Acta Petrologica et Mineralogica，2019，38（6）：743-752.
18	郭雪飞，宋华玲，龙泉树，等.不同亚类硅酸盐宝玉石矿物的近红外光谱研究[J].昆明理工大学学报：自然科学版，2019，44（3）：22-25.
	GUO Xuefei， SONG Hualing， LONG Quanshu，et al.A study on near-infrared spectroscopy of different subgroup silicate gemstone minerals[J].Journal of Kunming University of Science and Technology：Natural Science，2019，44（3）：22-25.
19	彭春元，赵辉.利用红外光谱技术分析水泥性能[J].水泥技术，2001（4）：63-65.
	PENG Chunyuan， ZHAO Hui.Analysis of cement properties by infrared spectroscopy[J].Cement Technology，2001（4）：63-65.
20	LI Mingguo， SUN C J， GAU S H，et al.Effects of wet ball milling on lead stabilization and particle size variation in municipal solid waste incinerator fly ash[J].Journal of Hazardous Materials，2010，174（1/2/3）：586-591.
21	陈志良.机械化学法降解垃圾焚烧飞灰中二噁英及协同稳定化重金属的机理研究[D].杭州：浙江大学，2019.
	CHEN Zhiliang.Mechanism study of mechanochemistry on PCDD/Fs degradation and on heavy metals stabilization in MSWI fly ash[D].Hangzhou：Zhejiang University，2019.
22	黎雯.类水滑石/碳纳米管复合材料的构建及其对双酚A的催化降解研究[D].广州：华南理工大学，2015.
	LI Wen.Frabrication of hydrotalcite/carbon nanotube composites and its application in catalytic degradation of BPA[D].Guangzhou：South China University of Technology，2015.
23	CHEN Qian， LONG Ling， LIU Xiaobo，et al.Low-toxic zeolite fabricated from municipal solid waste incineration fly ash via microwave-assisted hydrothermal process with fusion pretreatment[J].Journal of Material Cycles and Waste Management，2020，22（4）：1196-1207.
24	ELIANA GATTULLO C， D'ALESSANDRO C， ALLEGRETTA I，et al.Alkaline hydrothermal stabilization of Cr（Ⅵ） in soil using glass and aluminum from recycled municipal solid wastes[J].Journal of Hazardous Materials，2018，344：381-389.
25	ZHOU Xian， ZHOU Min， WU Xian，et al.Reductive solidification/stabilization of chromate in municipal solid waste incineration fly ash by ascorbic acid and blast furnace slag[J].Chemosphere，2017，182：76-84.
26	WANG Wenxia， GAO Xiangpeng， LI Tinghao，et al.Stabilization of heavy metals in fly ashes from municipal solid waste incineration via wet milling[J].Fuel，2018，216：153-159.
27	杨凤玲，李鹏飞，叶泽甫，等.城市生活垃圾焚烧飞灰组成特性及重金属熔融固化处理技术研究进展[J].洁净煤技术，2021，27（1）：169-180.
	YANG Fengling， LI Pengfei， YE Zefu，et al.Study progress on the composition characteristics of fly ash from municipal solid waste incineration and treatment technology of heavy metal melting and solidification[J].Clean Coal Technology，2021，27（1）：169-180.
28	SHI Huisheng， KAN Lili.Leaching behavior of heavy metals from municipal solid wastes incineration（MSWI） fly ash used in concrete[J].Journal of Hazardous Materials，2009，164（2/3）：750-754.
29	ZHANG Haiying， ZHAO Youcai.Study on physicochemical characteristics of municipal solid waste incineration（MSWI） fly ash[C]//IEEE.2009 International Conference on Environmental Science and Information Application Technology，2009：28-31.
30	ZHAO Xinyue， YANG Jinyan， NING Ning，et al.Chemical stabilization of heavy metals in municipal solid waste incineration fly ash：A review[J].Environmental Science and Pollution Research， 2022，29（27）：40384-40402.
31	杨南如.机械力化学过程及效应（Ⅱ）：机械力化学过程及应用[J].建筑材料学报，2000，3（2）：93-97.
	YANG Nanru.Processes and effects of mechanochemistry（Ⅱ）—Processes and application of mechanochemistry[J].Journal of Building Materials，2000，3（2）：93-97.

编号	添加剂	液体	编号	添加剂	液体
MC-1	无	纯水	MC-4	高岭土	NaOH溶液
MC-2	无	NaOH溶液	MC-5	硅灰	NaOH溶液
MC-3	膨润土	NaOH溶液	MC-6	赤泥	NaOH溶液

原料	主要元素质量分数¹/%								重金属质量分数²/%
原料	Na	Al	Si	Fe	Ca	Mg	K	Cl	Pb	Zn	Cr
FA	3.37	0.77	1.86	0.55	28.82	0.84	4.01	22.37	0.22	0.84	0.13
膨润土	1.56	14.56	58.45	4.46	5.23	2.56	4.14	0.02	—	—	—
煅烧高岭土	0.06	46.39	48.64	0.49	0.35	0.11	0.21	—	—	—	—
硅灰	—	0.13	43.95	0.19	—	—	—	0.03	—	—	—
赤泥	8.46	11.12	12.28	16.22	2.34	0.19	1.29	0.18	—	—	0.02

样品编号	S_BET/（m²·g^-1）	V_P/（cm³·g^-1）	D_P/nm
MC-3	44.80	0.16	14.23
MC-4	43.27	0.20	18.50
MC-5	64.13	0.27	17.09
MC-6	34.36	0.16	18.93

样品编号	浸出浓度/（mg·L^-1）			浸出系数/%
样品编号	Pb	Cr	Zn	Pb	Cr	Zn
FA	16.04±0.80	2.15±0.04	1.28±0.04	5.94	1.34	0.13
MC-1	2.24±0.16	1.91±0.07	0.34±0.05	0.83	1.19	0.03
MC-2	1.71±0.25	1.20±0.23	0.41±0.04	0.63	0.74	0.04
MC-3	0.11±0.01	0.73±0.13	<0.001	0.05	0.65	0.00
MC-4	0.05±0.01	2.34±0.47	<0.001	0.02	2.09	0.00
MC-5	0.04±0.01	3.40±0.26	<0.001	0.02	3.04	0.00
MC-6	0.02±0.01	0.17±0.08	<0.001	0.01	0.15	0.00
浓度限值（GB 5085.3—2007）	5	15	100	—	—	—

样品编号	ρ（Pb）/（mg·L^-1）	ρ（Cr）/（mg·L^-1）	ρ（Zn）/（mg·L^-1）
MC-1	0.44	3.25	0.05
MC-2	0.29	5.22	0.13
MC-3	0.05	1.58	0.08
MC-4	0.25	1.77	0.02
MC-5	0.05	2.75	0.40
MC-6	0.05	1.05	0.09

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Inorganic Acid-Base-Salt Committee of CIESC

Study on effect mechanism of silicon-aluminum additives on stabilization of heavy metals in fly ash by mechanochemical stabilization method

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