Synergistic effect of silicon-aluminum addition and seed-induced on stabilization of heavy metals in MSW incineration fly ash during hydrothermal process

doi:10.11949/j.issn.0438-1157.20180046

Abstract

Abstract:

Coal fly ash (CFA), bentonite, kaolin and diatomite were selected as silicon-aluminium additives and tobermorite crystal were synthesized as seed added. Synergistic effect of silicon-aluminium addition and seed-induced on stabilization of heavy metals including Pb, Zn, Cu, Cd, and Cr in municipal solid waste (MSW) incineration fly ash (FA) during hydrothermal process under 150℃ was studied. Zeolites could not be formed by hydrothermal treatment (HT) mainly due to the high content of Ca but low content of Si, Al in FA, which led to the leaching toxicity of Pb (5.45 mg·L^-1) beyond the limited value of non-hazardous waste. Hibschite or katoite were found in HT products with 10% mass of additives solely or combined added. Tobermorite could be successfully synthesized with higher 30% mass of additives solely or combined added, which was attributed to the proper element of Ca/(Al+Si) adjusted near 0.67-1.20. Leaching toxicity of Pb in HT products decreased to 0.30 mg·L^-1 with 30% mass of combined additives including CFA and diatomite(1:1), and it decreased to lowest level (0.28 mg·L^-1) with more 3% mass of seed added which owing to the effective synthesis of tobermorite from first 6 h. Furthermore, seed-induced hydrothermal treatment of FA with combined silicon-aluminium additives could cause the inhibition of heavy metals migration into liquid during hydrothermal process. The decrease of heavy metals in liquid phase, and the decrease of leaching toxicity of heavy metals in solid phase (HT products) were observed, which indicated that heavy metals were really stabled in solid phase.

Key words: silicon-aluminum additive, seed-induced, hydrothermal method, MSW incineration fly ash, heavy metals

摘要：

研究了选取的粉煤灰、膨润土、高岭土、硅藻土作为外源硅铝调理剂添加与雪硅钙石人工晶种诱导对150℃水热法稳定垃圾焚烧飞灰中重金属Pb、Zn、Cu、Cd、Cr的协同影响。飞灰由于富钙而低硅铝的元素特征，导致其在水热条件下无法直接合成沸石类，Pb的浸出浓度仍然超标；当单一或混合添加硅铝调理剂添加量为10%时，其水热产物中有水钙铝榴石或加藤石生成；提高添加量至30%时，均有目标雪硅钙石的生成，这与30%添加量下飞灰中Ca/（Al+Si）元素比接近雪硅钙石的理想元素比值0.67~1.20直接相关。混合添加30%的粉煤灰与硅藻土为最佳选择，水热产物Pb的浸出浓度降低至0.30 mg·L^-1，且在此基础上再添加3%的诱导晶种可加速从第6 h开始即合成雪硅钙石，并使Pb的浸出浓度下降到最低值0.28 mg·L^-1。硅铝调控（30%的复合硅铝调理剂，其中粉煤灰：硅藻土为1：1）与晶种诱导的协同影响下高效生成雪硅钙石，并显著抑制Pb、Zn等在水热过程中向液相的转移、降低其在水热液相中的浓度，使飞灰中的重金属在水热后确实稳定于水热固相产物中而非迁移至水热液相造成污染转移，真正实现了飞灰中重金属的固定化。

关键词: 硅铝调理剂, 晶种诱导, 水热法, 垃圾焚烧飞灰, 重金属

CLC Number:

X799.3

SHI Dezhi, WANG Pan, HU Chunyan, LI Pengfei, ZHANG Chao, WEI Yunmei, GU Li. Synergistic effect of silicon-aluminum addition and seed-induced on stabilization of heavy metals in MSW incineration fly ash during hydrothermal process[J]. CIESC Journal, 2018, 69(8): 3651-3661.

石德智, 王攀, 胡春艳, 李鹏飞, 张超, 魏云梅, 古励. 硅铝调控与晶种诱导对水热稳定飞灰中重金属的协同影响[J]. 化工学报, 2018, 69(8): 3651-3661.

References 37

[1]	MENARD Y, ASTHANA A, PATISSON F, et al. Thermodynamic study of heavy metals behaviour during municipal waste incineration[J]. Process Safety & Environmental Protection, 2006, 84(4):290-296.
[2]	SHI D Z, LI P F, ZAHNG C, et al. Level and patterns of polychlorinated biphenyls in residues from incineration of established source-classified MSW in China[J]. Toxicological & Environmental Chemistry, 2015, 97(10):1337-1349.
[3]	JIN Y Q, MA X J, JIANG X G, et al. Effects of hydrothermal treatment on the major heavy metals in fly ash from municipal solid waste incineration[J]. Energy & Fuels, 2013, 27(1):394-400.
[4]	SHAN C C, JING Z Z, PAN L L, et al. Hydrothermal solidification of municipal solid waste incineration fly ash[J]. Research on Chemical Intermediates, 2011, 37:551-565.
[5]	熊祖鸿, 范根育, 鲁敏, 等. 垃圾焚烧飞灰处置技术研究进展[J]. 化工进展, 2013, 32(7):1678-1683. XIONG Z H, FAN G Y, LU M, et al. Treatment technologies of municipal solid waste incinerator fly ash:a review[J]. Chemical Industry & Engineering Progress, 2013, 32(7):1678-1683.
[6]	BAYUSENO A P, SCHMAHL W W, MULLEJANS T. Hydrothermal processing of MSWI fly ash-towards new stable minerals and fixation of heavy metals[J]. Journal of Hazardous Materials, 2009, 167(1/2/3):250-259.
[7]	王磊. 水热法外加硅铝源稳定医疗废物焚烧飞灰中重金属的研究[D]. 杭州:浙江大学, 2012. WANG L. A study on hydrothermal process to stabilize heavy metals from MWI fly ash with silicon-aluminum[D]. Hangzhou:Zhejiang University, 2012.
[8]	ZHANG Z Z, QIN B, ZHANG X W, et al. The seeds effect on zeolite NU-87:synthesis parameters and structural properties[J]. Journal of Porous Materials, 2013, 20(3):515-521.
[9]	JI Y Y, WANG Y Q, XIE B, et al. Zeolite seeds:third type of structure directing agents in the synthesis of zeolites[J]. Comments on Inorganic Chemistry, 2016, 36(1):1-16.
[10]	SUZUKI K, HAYAKAWA T. The effects of seeding in the synthesis of zeolite ZSM-48 in the presence of tetramethylammoniumion[J]. Microporous & Mesoporous Materials, 2005, 77(2/3):131-137.
[11]	CAULLET P, HAZM J, GUTH J L, et al. Synthesis of zeolite beta from nonalkaline fluoride aqueous aluminosilicate gels[J]. Zeolites, 1992, 12(3):240-250.
[12]	HOUSTON J R, MAXWELL R S, CARROLL S A. Transformation of meta-stable calcium silicate hydrates to tobermorite:reaction kinetics and molecular structure from XRD and NMR spectroscopy[J]. Geochemical Transactions, 2009, 10(1):1-14.
[13]	中华人民共和国国家环境保护总局. 固体废弃物浸出毒性浸出方法硫酸硝酸法:HJ/T 299-2007[S]. 北京:中国环境科学出版社, 2007. State Environmental Protection Administration of the People's Republic of China. Solid waste-Extraction procedure for leaching toxicity-Sulphuric acid & nitric acid method:HJ/T 299-2007[S]. Beijing:China Environmental Science Press, 2007.
[14]	YAO Z D, TAMURA C, MATSUDA M, et al. Resource recovery of waste incineration fly ash:synthesis of tobermorite as ion exchanger[J]. Journal of Materials Research, 1999, 14(11):4437-4442.
[15]	BOGUSH A, STEGEMANN J A, WOOD I, et al. Element composition and mineralogical characterisation of air pollution control residue from UK energy-from-waste facilities[J]. Waste Management, 2015, 36:119-129.
[16]	JOSEWICZ W, GULLET B K. Reaction mechanisms of dry Ca-based sorbents with gaseous HCl[J]. Industrial Engineering Chemistry Research, 1995, 34(2):607-612.
[17]	PAN Y, WU Z, ZHOU J, et al. Chemical characteristics and risk assessment of typical municipal solid waste incineration(MSWI) fly ash in China[J]. Journal of Hazardous Materials, 2013, 261(20):269-276.
[18]	中华人民共和国国家环境保护总局, 国家质量监督检验检疫总局. 危险废物鉴别标准浸出毒性鉴别:GB 5085.3-2007[S]. 北京:中国环境科学出版社, 2007. State Environmental Protection Administration, General Administration of Quality Supervision of the People's Republic of China. Identification standards for hazardous wastes-Identification for extraction toxicity:GB 5085.3-2007[S]. Beijing:China Environmental Science Press, 2007.
[19]	ABANADES S, FLAMANT G, GAGNEPAIN B, et al. Fate of heavy metals during municipal solid waste incineration[J]. Waste Management & Research the Journal of the International Solid Wastes & Public Cleansing Association Iswa, 2002, 20(1):55-68.
[20]	JING Z Z, JIN F, HASHIDA T, et al. Hydrothermal solidification of blast furnace slag by formation of tobermorite[J]. Journal of Materials Science, 2007, 42(19):8236-8241.
[21]	GEELHOED J S, MEEUSSEN J C L, ROE M J, et al. Chromium remediation or release? Effect of iron(Ⅱ) sulfate addition on chromium(Ⅵ) leaching from columns of chromite ore processing residue[J]. Environmental Science & Technology, 2003, 37(14):3206-3213.
[22]	HILLIER S, LUMSDON D G, BRYDSON R, et al. Hydrogarnet:a host phase for Cr(Ⅵ) in chromite ore processing residue(COPR) and other high pH wastes[J]. Environmental Science & Technology, 2007, 41(6):1921-1927.
[23]	COLEMAN N J, BRASSINGTON D S. Synthesis of Al-substituted 11Å tobermorite from newsprint recycling residue:a feasibility study[J]. Materials Research Bulletin, 2003, 38(3):485-497.
[24]	KIKUMA J, TSUNASHIMA M, ISHIKAWA T, et al. Effects of quartz particle size and water-to-solid ratio on hydrothermal synthesis of tobermorite studied by in-situ time-resolved X-ray diffraction[J]. Journal of Solid State Chemistry, 2011, 184(8):2066-2074.
[25]	KLIMESCH D S, RAY A, GUERBOIS J P. Differential scanning calorimetry evaluation of autoclaved cement based building materials made with construction and demolition waste[J]. Thermochimica Acta, 2002, 389(1/2):195-198.
[26]	MELLER N, HALL C, PHIPPS J S. A new phase diagram for the CaO-Al2O3-SiO2-H2O hydroceramic system at 200℃[J]. Materials Research Bulletin, 2005, 40(5):715-723.
[27]	刘贺. 利用钾长石合成雪硅钙石粉体反应机理研究[D]. 北京:中国地质大学, 2006. LIU H. Synthesis of bermorite powder from potassium feldspar:reactive mechanism research[D]. Beijing:China University of Geosciences, 2006.
[28]	YASUE T, SHIOYA Y, ARAL Y. Synthesis and characteristics of Al-substituted tobermorite by alkoxide method[J]. Journal of the Ceramic Society of Japan, 1991, 99(1153):780-787.
[29]	LIU F M, CHEN D P, NI W, et al. Effect of Al3+ on tobermorite crystallinity[J]. Journal of University of Science and Technology Beijing, 2000, 7(2):79-81.
[30]	PEREZ-BARRADO E, PUJOL M C, AGUILO M, et al. Fast aging treatment for the synthesis of hydrocalumites using microwaves[J]. Applied Clay Science, 2013, 80/81(4):313-319.
[31]	LIU Q, LI Y J, ZHANG J, et al. Effective removal of zinc from aqueous solution by hydrocalumite[J]. Chemical Engineering Journal, 2011, 175(22):33-38.
[32]	HU Y Y, ZHANG P F, LI J P, et al. Stabilization and separation of heavy metals in incineration fly ash during the hydrothermal treatment process[J]. Journal of Hazardous Materials, 2015, 299(4):149-157.
[33]	JIN J, LI X D, CHI Y, et al. Co-disposal of heavy metals containing waste water and medical waste incinerator fly ash by hydrothermal process with addition of sodium carbonate:a case study on Cu(Ⅱ) removal[J]. Water Air & Soil Pollution, 2010, 209(1):391-400.
[34]	IZQUIERDO M, QUEROL X. Leaching behavior of elements from coal combustion fly ash:an overview[J]. International Journal of Coal Geology, 2012, 94(3):54-66.
[35]	ZHANG H, HE P J, SHAO L M, et al. Leaching behavior of Pb and Zn in air pollution control residues and their modeling prediction[J]. Journal of Environmental Sciences, 2006, 18(3):583-586.
[36]	JING Z Z, FAN X W, LEI Z, et al. Hydrothermal solidification behavior of municipal solid waste incineration bottom ash without any additives[J]. Waste Management, 2013, 33(5):1182-1189.
[37]	JIAO F C, ZHANG L. Study on the species of heavy metals in MSW incineration fly ash and their leaching behavior[J]. Fuel Processing Technology, 2016, 152:108-115.