Occurrence, leaching behavior, and detoxification of heavy metal Cr in coal gasification slag

doi:10.1016/j.cjche.2022.10.013

Chinese Journal of Chemical Engineering ›› 2023, Vol. 58 ›› Issue (6): 11-19.DOI: 10.1016/j.cjche.2022.10.013

Occurrence, leaching behavior, and detoxification of heavy metal Cr in coal gasification slag

Jiangshan Qu^1,2, Jianbo Zhang¹, Huiquan Li^1,2, Shaopeng Li¹, Da Shi^1,3, Ruiqi Chang^1,2, Wenfen Wu¹, Ganyu Zhu¹, Chennian Yang¹, Chenye Wang¹

1. CAS Key Laboratory of Green Process and Engineering, National Engineering Research Center of Green Recycling for Strategic Metal Resources, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100090, China;
2. School of Chemical Engineering, University of Chinese Academy of Sciences, Beijing 100049, China;
3. School of Resources and Civil Engineering, Northeastern University, Shenyang 110819, China

Received:2022-08-26 Revised:2022-10-24 Online:2023-08-31 Published:2023-06-28
Contact: Huiquan Li,E-mail:hqli@ipe.ac.cn
Supported by:
The work was finally supported by the National Natural Science Foundation of China (52174390, U1810205), Innovation Academy for Green Manufacture of the Chinese Academy of Sciences China (IAGM2022D04), and Strategic Priority Research Program of the Chinese Academy of Sciences China (XDA21040601).

Occurrence, leaching behavior, and detoxification of heavy metal Cr in coal gasification slag

Jiangshan Qu^1,2, Jianbo Zhang¹, Huiquan Li^1,2, Shaopeng Li¹, Da Shi^1,3, Ruiqi Chang^1,2, Wenfen Wu¹, Ganyu Zhu¹, Chennian Yang¹, Chenye Wang¹

1. CAS Key Laboratory of Green Process and Engineering, National Engineering Research Center of Green Recycling for Strategic Metal Resources, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100090, China;
2. School of Chemical Engineering, University of Chinese Academy of Sciences, Beijing 100049, China;
3. School of Resources and Civil Engineering, Northeastern University, Shenyang 110819, China

通讯作者: Huiquan Li,E-mail:hqli@ipe.ac.cn
基金资助:
The work was finally supported by the National Natural Science Foundation of China (52174390, U1810205), Innovation Academy for Green Manufacture of the Chinese Academy of Sciences China (IAGM2022D04), and Strategic Priority Research Program of the Chinese Academy of Sciences China (XDA21040601).

Abstract

Abstract: Coal gasification slag (CGS) is a type of solid waste produced during coal gasification, in which heavy metals severely restrict its resource utilization. In this work, the mineral occurrence and distribution of typical heavy metal Cr in CGS is investigated. The leaching behavior of Cr under different conditions is studied in detail. Acid leaching-selective oxidation-coprecipitation method is proposed based on the characteristics of Cr in CGS. The detoxification of Cr in CGS is realized, and the detoxification mechanism is clarified. Results show that Cr is highly enriched in CGS. The speciation of Cr is mainly residual fraction (74.47%-86.12%), which is combined with amorphous aluminosilicate. Cr³⁺ and Cr⁶⁺ account for 90.93%-94.82% and 5.18%-9.07% of total Cr, respectively. High acid concentration and high liquid-solid ratio are beneficial to destroy the lattice structure of amorphous aluminosilicate, thus improving the leaching efficiency of Cr, which can reach 97.93% under the optimal conditions. Acid leaching-selective oxidation-coprecipitation method can realize the detoxification of Cr in CGS. Under the optimal conditions, the removal rates of Fe³⁺ and Cr³⁺ in the leaching solution are 80.99%-84.79% and 70.58%-71.69%, respectively, while the loss rate of Al³⁺ is only 1.10%-3.35%. Detoxification slag exists in the form of Fe-Cr coprecipitation (Fe_1-xCr_xOOH), which can be used for smelting. The detoxification acid leaching solution can be used to prepare inorganic polymer composite coagulant poly-aluminum chloride (PAC). This study can provide theoretical and data guidance for detoxification of heavy metal Cr in CGS and achieve resource utilization of coal gasification solid waste.

Key words: Coal gasification slag, Heavy metal, Distributions, Leaching, Detoxification, Precipitation

摘要： Coal gasification slag (CGS) is a type of solid waste produced during coal gasification, in which heavy metals severely restrict its resource utilization. In this work, the mineral occurrence and distribution of typical heavy metal Cr in CGS is investigated. The leaching behavior of Cr under different conditions is studied in detail. Acid leaching-selective oxidation-coprecipitation method is proposed based on the characteristics of Cr in CGS. The detoxification of Cr in CGS is realized, and the detoxification mechanism is clarified. Results show that Cr is highly enriched in CGS. The speciation of Cr is mainly residual fraction (74.47%-86.12%), which is combined with amorphous aluminosilicate. Cr³⁺ and Cr⁶⁺ account for 90.93%-94.82% and 5.18%-9.07% of total Cr, respectively. High acid concentration and high liquid-solid ratio are beneficial to destroy the lattice structure of amorphous aluminosilicate, thus improving the leaching efficiency of Cr, which can reach 97.93% under the optimal conditions. Acid leaching-selective oxidation-coprecipitation method can realize the detoxification of Cr in CGS. Under the optimal conditions, the removal rates of Fe³⁺ and Cr³⁺ in the leaching solution are 80.99%-84.79% and 70.58%-71.69%, respectively, while the loss rate of Al³⁺ is only 1.10%-3.35%. Detoxification slag exists in the form of Fe-Cr coprecipitation (Fe_1-xCr_xOOH), which can be used for smelting. The detoxification acid leaching solution can be used to prepare inorganic polymer composite coagulant poly-aluminum chloride (PAC). This study can provide theoretical and data guidance for detoxification of heavy metal Cr in CGS and achieve resource utilization of coal gasification solid waste.

关键词: Coal gasification slag, Heavy metal, Distributions, Leaching, Detoxification, Precipitation

Jiangshan Qu, Jianbo Zhang, Huiquan Li, Shaopeng Li, Da Shi, Ruiqi Chang, Wenfen Wu, Ganyu Zhu, Chennian Yang, Chenye Wang. Occurrence, leaching behavior, and detoxification of heavy metal Cr in coal gasification slag[J]. Chinese Journal of Chemical Engineering, 2023, 58(6): 11-19.

References

[1] Y.F. Wang, Y.G. Tang, X. Guo, Q. Xie, R.B. Finkelman, P.Y. Li, P.X. Chen, Fate of potentially hazardous trace elements during the entrained-flow coal gasification processes in China, Sci. Total. Environ. 668 (2019) 854-866
[2] X.D. Liu, Z.W. Jin, Y.H. Jing, P.P. Fan, Z.L. Qi, W.R. Bao, J.C. Wang, X.H. Yan, P. Lv, L.P. Dong, Review of the characteristics and graded utilisation of coal gasification slag, Chin. J. Chem. Eng. 35 (2021) 92-106.
[3] J.S. Qu, J.B. Zhang, H.Q. Li, S.P. Li, A high value utilization process for coal gasification slag: preparation of high modulus sodium silicate by mechano-chemical synergistic activation, Sci. Total Environ. 801 (2021) 149761
[4] D. Shi, J.B. Zhang, X.J. Hou, S.P. Li, H.Q. Li, F.Y. He, Adsorption mechanism of a new combined collector (PS-1) on unburned carbon in gasification slag, Sci. Total Environ. 818 (2022) 151856
[5] Y.G. Tang, Y.F. Wang, B.B. Huan, X. Guo, R.B. Finkelman, Leachability of hazardous trace elements from entrained-flow coal gasification residues in ningdong, China, Energy Fuels 31 (9) (2017) 9703-9716
[6] P. Jiang, C.R. Xie, C.L. Luo, W. Meng, G. Yang, G.S. Yu, Y. Gong, M.X. Xu, T. Wu, Distribution and modes of occurrence of heavy metals in opposed multi-burner coal-water-slurry gasification plants, Fuel 303 (2021) 121163
[7] Y. Guo, Y.X. Zhang, X. Zhao, J. Xu, G.F. Qiu, W.K. Jia, J.J. Wu, F.H. Guo, Multifaceted evaluation of distribution, occurrence, and leaching features of typical heavy metals in different-sized coal gasification fine slag from Ningdong region, China: a case study, Sci. Total. Environ. 831 (2022) 154726
[8] M. Díaz-Somoano, M.R. Martínez-Tarazona, Trace element evaporation during coal gasification based on a thermodynamic equilibrium calculation approach, Fuel 82 (2) (2003) 137-145
[9] R. Yoshiie, Y. Taya, T. Ichiyanagi, Y. Ueki, I. Naruse, Emissions of particles and trace elements from coal gasification, Fuel 108 (2013) 67-72
[10] J.R. Bunt, F.B. Waanders, Volatile trace element behaviour in the Sasol^® fixed-bed dry-bottom (FBDB)^TM gasifier treating coals of different rank, Fuel Process. Technol. 92 (8) (2011) 1646-1655
[11] Y.G. Tang, X. Guo, Q. Xie, R.B. Finkelman, S.C. Han, B.B. Huan, X. Pan, Petrological characteristics and trace element partitioning of gasification residues from slagging entrained-flow gasifiers in ningdong, China, Energy Fuels 32 (3) (2018) 3052-3067
[12] W.P. Ma, S.Q. Liu, Z. Li, J.F. Lv, L.H. Yang, Release and transformation mechanisms of hazardous trace elements in the ash and slag during underground coal gasification, Fuel 281 (2020) 118774.
[13] Y. Guo, C.F. Ma, Y.X. Zhang, L. Zhou, Z.K. Guo, Z.K. Miao, X. Zhao, J.J. Wu, F.H. Guo, Comparative study on the structure characteristics, combustion reactivity, and potential environmental impacts of coal gasification fine slag with different particle size fractions, Fuel 311 (2022) 122493.
[14] L. Wang, J. Li, Y. Jin, M. Chen, J.H. Luo, X.H. Zhu, Y.Q. Zhang, Study on the removal of chromium(III) from leather waste by a two-step method, J. Ind. Eng. Chem. 79 (2019) 172-180.
[15] X.R. Zhang, G. Li, J. Wu, N. Xiong, X.J. Quan, Leaching of valuable elements from the waste chromite ore processing residue: a kinetic analysis, ACS Omega 5 (31) (2020) 19633-19638.
[16] X. Huang, R.L. Zhuang, F. Muhammad, L. Yu, Y. Shiau, D.W. Li, Solidification/stabilization of chromite ore processing residue using alkali-activated composite cementitious materials, Chemosphere 168 (2017) 300-308.
[17] A.A. Yahya, N. Ali, N.L. Mohd Kamal, S. Shahidan, S. Beddu, M.F. Nuruddin, N. Shafiq, Reducing heavy metal element from coal bottom ash by using citric acid leaching treatment, MATEC Web Conf. 103 (2017) 01004.
[18] C.R. Cheeseman, C.J. Sollars, S. McEntee, Properties, microstructure and leaching of sintered sewage sludge ash, Resour. Conserv. Recycl. 40 (1) (2003) 13-25.
[19] Y.C. Chen, F.Y. Chen, F. Zhou, M. Lu, H.B. Hou, J.P. Li, D.M. Liu, T. Wang, Early solidification/stabilization mechanism of heavy metals (Pb, Cr and Zn) in Shell coal gasification fly ash based geopolymer, Sci. Total. Environ. 802 (2022) 149905.
[20] J. Xin, L. Liu, L.H. Xu, J.Y. Wang, P. Yang, H.S. Qu, A preliminary study of aeolian sand-cement-modified gasification slag-paste backfill: Fluidity, microstructure, and leaching risks, Sci. Total Environ. 830 (2022) 154766.
[21] X.N. Xiong, X.M. Liu, I.K.M. Yu, L. Wang, J. Zhou, X. Sun, J. Rinklebe, S.M. Shaheen, Y.S. Ok, Z. Lin, D.C.W. Tsang, Potentially toxic elements in solid waste streams: fate and management approaches, Environ. Pollut. 253 (2019) 680-707.
[22] Z.K. Miao, Z.K. Guo, G.F. Qiu, Y.X. Zhang, J.J. Wu, Synthesis of activated carbon from high-ash coal gasification fine slag and their application to CO₂ capture, J. CO₂ Util. 50 (2021) 101585.
[23] Y. Tang, H.F. Yin, H.D. Yuan, H. Shuai, Y.L. Xin, Phase and morphological transformation stages during carbothermal reduction nitridation process: from coal gasification slag wastes to Ca-α-SiAlON powders, Adv. Powder Technol. 27 (5) (2016) 2232-2237.
[24] Y.Y. Gu, X.C. Qiao, A carbon silica composite prepared from water slurry coal gasification slag, Microporous Mesoporous Mater. 276 (2019) 303-307.
[25] M. Pueyo, J. Mateu, A. Rigol, M. Vidal, J.F. López-Sánchez, G. Rauret, Use of the modified BCR three-step sequential extraction procedure for the study of trace element dynamics in contaminated soils, Environ. Pollut. 152 (2) (2008) 330-341.
[26] L. Bartoňová, H. Raclavská, Behavior of Cr during coal combustion: an overview, Fuel 322 (2022) 124210.
[27] R.B. Finkelman, C.A. Palmer, P.P. Wang, Quantification of the modes of occurrence of 42 elements in coal, Int. J. Coal Geol. 185 (2018) 138-160.
[28] Y.S. Zhang, P.F. Shang, J.W. Wang, P. Norris, C.E. Romero, W.P. Pan, Trace element (Hg, As, Cr, Cd, Pb) distribution and speciation in coal-fired power plants, Fuel 208 (2017) 647-654.
[29] Y. Liu, G.J. Liu, C.C. Qi, S.W. Cheng, R.Y. Sun, Chemical speciation and combustion behavior of chromium (Cr) and vanadium (V) in coals, Fuel 184 (2016) 42-49.
[30] E. Sočo, J. Kalembkiewicz, Investigations on Cr mobility from coal fly ash, Fuel 88 (8) (2009) 1513-1519.
[31] L. Chang, Y.C. Zhao, Y. Zhang, X.H. Yu, Z.H. Li, B.G. Gong, H. Liu, S.Z. Wei, H. Wu, J.Y. Zhang, Mercury species and potential leaching in sludge from coal-fired power plants, J. Hazard. Mater. 403 (2021) 123927.
[32] D. Chew, K. Drost, J.H. Marsh, J.A. Petrus, LA-ICP-MS imaging in the geosciences and its applications to geochronology, Chem. Geol. 559 (2021) 119917.
[33] M. Zaeem, M. Nadeem, T. Huong Pham, W. Ashiq, W. Ali, S. Shah Mohioudin Gillani, E.R.D. Moise, H. Leier, V. Kavanagh, L. Galagedara, M. Cheema, R. Thomas, Development of a hyperspectral imaging technique using LA-ICP-MS to show the spatial distribution of elements in soil cores, Geoderma 385 (2021) 114831.
[34] F. Goodarzi, F.E. Huggins, Speciation of chromium in feed coals and ash byproducts from Canadian power plants burning subbituminous and bituminous coals, Energy Fuels 19 (6) (2005) 2500-2508.
[35] F. Goodarzi, F.E. Huggins, H. Sanei, Assessment of elements, speciation of As, Cr, Ni and emitted Hg for a Canadian power plant burning bituminous coal, Int. J. Coal Geol. 74 (1) (2008) 1-12.
[36] M.X. Guo,P.D.Sun, J.Q.Luo, Extraction of chromium from electroplating sludge by sodium oxidization method, Environ. Sci. Technol. 32 (2009) 50-53.
[37] A.K. Prabhakar, B. Cadiam Mohan, T.S. Tay, S.S.C. Lee, S.L.M. Teo, C.H. Wang, Incinerated Sewage Sludge Bottom Ash-Chemical processing, Leaching patterns and Toxicity testing, J. Hazard. Mater. 402 (2021) 123350.
[38] H.W. Luo, Y. Cheng, D.Q. He, E.H. Yang, Review of leaching behavior of municipal solid waste incineration (MSWI) ash, Sci. Total Environ. 668 (2019) 90-103.
[39] W. Liu, Y.X. Yu, Removal of recalcitrant trivalent chromium complexes from industrial wastewater under strict discharge standards, Environ. Technol. Innov. 23 (2021) 101644.
[40] Y.L. Tang, J.T. Zhao, J.F. Zhou, Y.H. Zeng, W.H. Zhang, B. Shi, Highly efficient removal of Cr(III)-poly(acrylic acid) complex by coprecipitation with polyvalent metal ions: Performance, mechanism, and validation, Water Res. 178 (2020) 115807.
[41] A. Ishfaq, S. Ilyas, A. Yaseen, M. Farhan, Hydrometallurgical valorization of chromium, iron, and zinc from an electroplating effluent, Sep. Purif. Technol. 209 (2019) 964-971.
[42] I. Bibi, B. Singh, E. Silvester, Akaganéite (β-FeOOH) precipitation in inland acid sulfate soils of south-western New South Wales (NSW), Australia, Geochimica Cosmochimica Acta 75 (21) (2011) 6429-6438.
[43] Z.L. Huang, C.G. Chen, J.Y. Xie, Z.X. Wang, The evolution of dehydration and thermal decomposition of nanocrystalline and amorphous chromium hydroxide, J. Anal. Appl. Pyrolysis 118 (2016) 225-230.
[44] S.K. Roy, D. Nayak, S.S. Rath, A review on the enrichment of iron values of low-grade Iron ore resources using reduction roasting-magnetic separation, Powder Technol. 367 (2020) 796-808.
[45] W. Lan, H.Q. Qiu, J. Zhang, Y.J. Yu, K.L. Yang, Z.Z. Liu, G.J. Ding, Characteristic of a novel composite inorganic polymer coagulant-PFAC prepared by hydrochloric pickle liquor, J. Hazard. Mater. 162 (1) (2009) 174-179.

Occurrence, leaching behavior, and detoxification of heavy metal Cr in coal gasification slag

Occurrence, leaching behavior, and detoxification of heavy metal Cr in coal gasification slag

PDF (PC)

Knowledge

Abstract

Cite this article

share this article

References

Related Articles 15

Recommended Articles

Metrics

Comments

[1]	Bo Yu, Guang Fu, Xinpei Li, Libo Zhang, Jing Li, Hongtao Qu, Dongbin Wang, Qingfeng Dong, Mengmeng Zhang. Arsenic removal from acidic industrial wastewater by ultrasonic activated phosphorus pentasulfide [J]. Chinese Journal of Chemical Engineering, 2023, 60(8): 46-52.
[2]	Alexander Nti Kani, Evans Dovi, Aaron Albert Aryee, Runping Han, Zhaohui Li, Lingbo Qu. Mechanisms and reusability potentials of zirconium-polyaziridine-engineered tiger nut residue towards anionic pollutants [J]. Chinese Journal of Chemical Engineering, 2023, 60(8): 275-292.
[3]	Guangyuan Chen, Tong Zhou, Meng Zhang, Zhongxiang Ding, Zhikun Zhou, Yuanhui Ji, Haiying Tang, Changsong Wang. Effects of heavy metal ions Cu²⁺/Pb²⁺/Zn²⁺ on kinetic rate constants of struvite crystallization [J]. Chinese Journal of Chemical Engineering, 2023, 57(5): 10-16.
[4]	Jingran Liu, Yue Wu, Jie Tang, Tao Wang, Feng Ni, Qiumin Wu, Xijiao Yang, Ayyaz Ahmad, Naveed Ramzan, Yisheng Xu. Polymeric assembled nanoparticles through kinetic stabilization by confined impingement jets dilution mixer for fluorescence switching imaging [J]. Chinese Journal of Chemical Engineering, 2023, 56(4): 89-96.
[5]	Yong Niu, Xiaowu Peng, Jinfeng Li, Yuze Zhang, Fugen Song, Dong Shi, Lijuan Li. Recovery of Li₂CO₃ and FePO₄ from spent LiFePO₄ by coupling technics of isomorphic substitution leaching and solvent extraction [J]. Chinese Journal of Chemical Engineering, 2023, 54(2): 306-315.
[6]	Qing Lin, Guoquan Zhang, Kun Wang, Dongmei Luo, Siyang Tang, Hairong Yue. Two-stage cyclic ammonium sulfate roasting and leaching of extracting vanadium and titanium from vanadium slag [J]. Chinese Journal of Chemical Engineering, 2022, 47(7): 39-47.
[7]	Qilong Ge, Qi Tian, Sufang Wang, Fang Zhu. Synergistic effects of phosphoric acid modified hydrochar and coal gangue-based zeolite on bioavailability and accumulation of cadmium and lead in contaminated soil [J]. Chinese Journal of Chemical Engineering, 2022, 46(6): 150-160.
[8]	Lanting Ke, Xiaobin Liu, Bingqing Du, Yuanpeng Wang, Yanmei Zheng, Qingbiao Li. Component analysis and risk assessment of biogas slurry from biogas plants [J]. Chinese Journal of Chemical Engineering, 2022, 44(4): 182-191.
[9]	Xiaobin Chen, Yuting Tang, Chuncheng Ke, Chaoyue Zhang, Sichun Ding, Xiaoqian Ma. CO₂ capture by double metal modified CaO-based sorbents from pyrolysis gases [J]. Chinese Journal of Chemical Engineering, 2022, 43(3): 40-49.
[10]	Hengyu Shen, Run Zou, Yangtao Zhou, Xing Guo, Yanan Guan, Duo Na, Jinsong Zhang, Xiaolei Fan, Yilai Jiao. Additive manufacturing of sodalite monolith for continuous heavy metal removal from water sources [J]. Chinese Journal of Chemical Engineering, 2022, 42(2): 82-90.
[11]	Zhaofeng Zhang, Juanjuan Ding, Min Wu, Bochao Liu, Huiwen Song, Shengping You, Wei Qi, Rongxin Su, Zhimin He. Development of an integrated process for the production of high-purity γ-aminobutyric acid from fermentation broth [J]. Chinese Journal of Chemical Engineering, 2022, 50(10): 361-368.
[12]	Fangqi Mao, Peipei Hao, Yuquan Zhu, Xianggui Kong, Xue Duan. Layered double hydroxides: Scale production and application in soil remediation as super-stable mineralizer [J]. Chinese Journal of Chemical Engineering, 2022, 41(1): 42-48.
[13]	Shichao Yu, Rui Liao, Baojun Yang, Chaojun Fang, Zhentang Wang, Yuling Liu, Baiqiang Wu, Jun Wang, Guanzhou Qiu. Chalcocite (bio)hydrometallurgy—current state, mechanism, and future directions: A review [J]. Chinese Journal of Chemical Engineering, 2022, 41(1): 109-120.
[14]	Yonghou Xiao, Shuang Qiu, Qidong Zhao, Yuhao Zhu, Chirag B. Godiya, Gaohong He. Numerical simulation of low-concentration CO₂ adsorption on fixed bed using finite element analysis [J]. Chinese Journal of Chemical Engineering, 2021, 36(8): 47-56.
[15]	Xiaodong Liu, Zhengwei Jin, Yunhuan Jing, Panpan Fan, Zhili Qi, Weiren Bao, Jiancheng Wang, Xiaohui Yan, Peng Lv, Lianping Dong. Review of the characteristics and graded utilisation of coal gasification slag [J]. Chinese Journal of Chemical Engineering, 2021, 35(7): 92-106.