Study on removal of heavy metal ions by mg (OH)2@fly ash composite
WANG Zhi-xue1, WANG Cai-li1,2, WANG Bin1, YAO Guo-xin1, QIU Ying1, YANG Run-quan1, WANG Hui-fa1
1. College of Mining Engineering, Taiyuan University of Technology, Taiyuan 030024, China; 2. State Environmental Protection Key Laboratory of Mineral Metallurgical Resources Utilization and Pollution Control, Wuhan University of Science and Technology, Wuhan 430081, China
Abstract:Nano-magnesium hydroxide@fly ash composite with core-shell structure was prepared with non-uniform nucleation method taking fly ash as the carrier, MgCl2 and NaOH as reaction coating agents according to the idea of "particle design" and its adsorption properties of Cu(II), Ni(II) and Pb(II) in wastewater were studied. The composite powders before and after coating were characterized by scanning electron microscopy (SEM), energy dispersive (EDS), specific surface area analyzer (BET), X-ray diffraction (XRD) and infrared spectroscopy (FTIR). The results show that the surface of the composite powder is uniformly coated with a large amount of nano-magnesium hydroxide and a small amount of hydrated magnesium carbonate, the specific surface area increased to more than 30 times of the original (fly ash 1.79 m2/g), the average pore size increased from 11 nm to 14.7 nm, and the average pore width increased from 12.8 nm to 15.4nm, respectively. Si-O-C-O-Mg and Si-O-Mg-OH are formed between Si-O-Si, Si-O-C and magnesium hydroxide on the surface of fly ash. The removal efficiency of heavy metals by the composite powder is significantly higher than that of fly ash, and the unit saturated adsorption capacity reaches 216.30, 160.96 and 116.50 mg/g. According to Zeta potential, FTIR and simulation equations, the adsorption mechanism of heavy metal ions by composite powder was analyzed. The results show that the composite adsorbs heavy metal ions through precipitation reaction, electrostatic attraction and ion exchange, etc. The adsorption process isotherm, the kinetics and the thermodynamics conform to the Langmuir isotherm model, intraparticle diffusion model and spontaneous endothermic reaction, reapectively. The desorption experiment indicates that the composite powder has a good regeneration performance in the adsorption process.
王志学, 王彩丽, 王斌, 姚国鑫, 秋颖, 杨润全, 王怀法. Mg (OH)2@粉煤灰复合材料对重金属离子的去除研究[J]. 中国环境科学, 2022, 42(12): 5713-5724.
WANG Zhi-xue, WANG Cai-li, WANG Bin, YAO Guo-xin, QIU Ying, YANG Run-quan, WANG Hui-fa. Study on removal of heavy metal ions by mg (OH)2@fly ash composite. CHINA ENVIRONMENTAL SCIENCECE, 2022, 42(12): 5713-5724.
Wu Y, Pang H, Liu Y, et al. Environmental remediation of heavy metal ions by novel-nanomaterials a review[J]. Environmental Pollution, 2019,246:608-620.
[2]
陈颢明,胡亦舒,李真.溶磷微生物改性生物炭吸附重金属的机理研究[J]. 中国环境科学, 2021,41(2):684-692. Chen H M, Hu Y S, Li Z. Adsorption mechanism of heavy metals by phosphate-solubilizing microorganism modified biochar[J]. China Environmental Science, 2021,41(2):684-692.
[3]
Baby R, Saifullah B, Hussein M. Palm Kernel Shell as an effective adsorbent for the treatment of heavy metal contaminated water[J]. Scientific Reports, 2019,9(1):1-11.
[4]
Baby S, Saifullah B, Rehman F. Greener method for the removal of toxic metal ions from the wastewater by application of agricultural waste as an adsorbent[J]. Water, 2018,10(10):1316-1330.
[5]
Bashir A, Malik A, Ahad S, et al. Removal of heavy metal ions from aqueous system by ion-exchange and biosorption methods[J]. Environmental Chemistry Letters, 2019,17(2):729-754.
[6]
Zhang W, Liang Z, Feng Q, et al. Reed hemicellulose-based hydrogel prepared by glow discharge electrolysis plasma and its adsorption properties for heavy metal ions[J]. Fresenius Environ Bull, 2016,25:1791-1798.
[7]
Montana M, Camacho A, Serrano I, et al. Removal of radionuclides in drinking water by membrane treatment using ultrafiltration, reverse osmosis and electrodialysis reversal[J]. Journal of Environmental Radioactivity, 2013,125:86-92.
[8]
Nędzarek A. The use of pressure membrane separation for heavy metal removal or recovery[M]. Practical Aspects of Chemical Engineering. Springer, Cham, 2018:339-347.
[9]
Song X, Yan D, Liu Z, et al. Performance of laboratory-scale constructed wetlands coupled with micro-electricfield for heavy metal-contaminating wastewater treatment[J]. Ecological Engin-eering, 2011,37(12):2061-2065.
[10]
Song S, Zhang S, Huang S, et al. A novel multi-shelled Fe3O4@MnOx hollow microspheres for immobilizing U(VI) and Eu (III)[J]. Chemical Engineering Journal, 2019,355:697-709.
[11]
王冰凝,刘守军,杨颂,等.红土镍矿基材料吸附及有氧降解水体污染物[J]. 中国环境科学, 2022,42(2):736-744. Wang B N, Li S J, Yang S, et al. Adsorption and aerobic degradation of water pollutants by laterite nickel ore-based materials[J]. China Environmental Science, 2022,42(2):736-744.
[12]
Wang C, Wang J, Wang S, et al. Preparation Mg(OH)2/calcined fly ash nanocomposite for removal of heavy metals from aqueous acidic solutions[J]. Materials, 2020,13(20):4621-4634.
[13]
Li Z, Wu C, Yu Q, et al. Phase transformat-ion of carbothermal reduction coal fly ash[J]. Journal of China Coal Society, 2016,41(3):769-775.
[14]
Purbasari A, Ariyanti D, Sumardiono S. Preparation and application of fly ash-based geopolymer for heavy metal removal[C]. AIP conference proceedings. AIP Publishing LLC, 2020,2197(1):050006.
[15]
Tauanov Z, Azat S, Baibatyrova A. A mini-review on coal fly ash properties, utilization and synthesis of zeolites[J]. International Journal of Coal Preparation and Utilization, 2022,42(7):1968-1990.
[16]
王春峰,李健生,王连军,等.粉煤灰合成NaA型沸石对重金属离子的吸附动力学[J]. 中国环境学, 2009,29(1):36-41. Wang C F, Li J S, Wang L J et al. Adsorption kinetics of heavy metal ions on NaA zeolite synthesized from fly ash[J]. China Environmental Science, 2009,29(1):36-41.
[17]
李鹏,肖启飞,李彩霞.粉煤灰在废水处理中的影响因素及应用综述[C]//2009中国选矿技术高峰论坛暨设备展示会论文, 2009:392-396. Li P, Xiao Q F, Li C X. Review on the influencing factors and application of fly ash in wastewater treatment[C]//2009. China Mineral Processing Technology Summit Forum and Equipment Exhibition Papers, 2009:392-396.
[18]
Blissett R S, Rowson N A. A review of the multi-component utilisation of coal fly ash[J]. Fuel, 2012,97:1-23.
[19]
赵鑫.合成条件对改性粉煤灰吸附镉能力的影响和机理[D]. 杨凌:西北农林科技大学, 2022. Zhao X. Effect and mechanisms of synthesis conditions on the cadmium adsorption capacity of modified fly ash[D]. Yangling:Northwest A & F University, 2022.
[20]
王彩丽,王静,杨润全,等.核壳结构粉煤灰基复合粉体制备及填充聚合物的性能[J]. 高分子材料科学与工程, 2020,36(8):87-92. Wang C L, Wang J, Yang R Q, et al. Preparation of core-shell fiy ash based composite and its application in filling polymer[J]. Polymer Materials Science & Engineering, 2020,36(8):87-92.
[21]
Chen Z, Xu C, Chen H, et al. The influence of process parameters on the preparation of CaF2@Al(OH)3 composite powder via heterogeneous nucleation[J]. International Journal of Materials Research, 2015,106(2):188-191.
[22]
Ali R M, Hamad H A, Hussein M M, et al. Potential of using green adsorbent of heavy metal removal from aqueous solutions:adsorption kinetics, isotherm, thermodynamic, mechanism and economic analysis[J]. Ecological Engineering, 2016,91:317-332.
[23]
王哲,徐毅,黄国和,等.对硝基苯酚和重金属在高炉水淬渣上的竞争吸附研究[J]. 中国环境科学, 2016,36(12):3686-3695. Wang Z, Xu Y, Huang G H, et al. Competitive adsorption of p-nitrophenol and heavy metals on water-quenched blast furnace slag[J]. China Environmental Science, 2016,36(12):3686-3695.
[24]
Tourania S, Behvandia A, Aghajaria A, et al. Adsorption of heavy metal ions from aqueous solutions using metal organic frame works:kinetic and thermodynamic study[J]. Desalination and Water Treatment, 2019,162:193-206.
[25]
Nagarajah R, Wong K T, Lee G, et al. Synthesis of a unique nanostructured magnesium oxide coated magnetite cluster composite and its application for the removal of selected heavy metals[J]. Separation and Purification Technology, 2017,174:290-300.
[26]
廖艳芬,曹亚文,吴淑梅,等.基于TG-FTIR的印染污泥与烟煤掺烧特性研究[J]. 华南理工大学学报, 2016,44(4):1-9. Liao Y F, Cao Y W, Wu S M, et al. Investigation into Co-combustion characteristics of dyeing sludge and bituminous coal based on TG-FTIR[J]. Journal of South China University of Technology, 2016, 44(4):1-9.
[27]
Das P S, Bakuli S, Samanta A, et al. Very high Cu(II) adsorption efficacy of designed nano-platelet Mg(OH)2 assembly[J]. Materials Research Express, 2017,4(2):025025-025039.
[28]
Wang C, Yang R, Wang H. Synthesis of ZIF-8/fly ash composite for adsorption of Cu2+, Zn2+ and Ni2+ from aqueous solutions[J]. Materials, 2020,13(1):214-228.
[29]
杨念,况守英,岳蕴辉.几种常见无水碳酸盐矿物的红外吸收光谱特征分析[J]. 矿物岩石, 2015,35(4):37-42. Yang N, Kuang S Y, Yue Y H. Infrared spectra analysis of several common anhydrous carbonate minerals[J]. Mineralogy and Petrology, 2015,35(4):37-42.
[30]
Wu Y, Pang H, Liu Y, et al. Environmental remediation of heavy metal ions by novel-nanomaterials:a review[J]. Environmental Pollution, 2019,246:608-620.
[31]
刘秀芸,王刚,雷雨昕,等.巯基改性玉米秸秆对水中Cu(Ⅱ)的吸附特性[J]. 中国环境科学, 2022,42(3):1220-1229. Liu X Y, Wang G, Lei Y X et al. Adsorption performance and mechanism of mercaptoacetyl corn straw for Cu(Ⅱ) in aqueous solution[J]. China Environmental Science, 2022,42(2):736-744.
[32]
Jangkorn S, Youngme S, Praipipat P. Comparative lead adsorptions in synthetic wastewater by synthesized zeolite A of recycled industrial wastes from sugar factory and power plant[J]. Heliyon, 2022,8(4):09323-09340.