Full Text:   <702>

Summary:  <912>

CLC number: X773

On-line Access: 2021-03-10

Received: 2020-06-10

Revision Accepted: 2020-07-17

Crosschecked: 2021-01-14

Cited: 0

Clicked: 1341

Citations:  Bibtex RefMan EndNote GB/T7714


Hao Zhou


Yu-jian Xing


-   Go to

Article info.
Open peer comments

Journal of Zhejiang University SCIENCE A 2021 Vol.22 No.3 P.207-221


In-situ investigation of melting characteristics of waste selective catalytic reduction catalysts during harmless melting treatment

Author(s):  Hao Zhou, Yu-jian Xing, Jia-nuo Xu, Ming-xi Zhou

Affiliation(s):  State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou 310027, China; more

Corresponding email(s):   zhouhao@zju.edu.cn

Key Words:  Waste selective catalytic reduction (SCR) catalyst, Thermal melting treatment, Melting characteristics, Additives, Heating stage microscope, Leaching toxicity

Hao Zhou, Yu-jian Xing, Jia-nuo Xu, Ming-xi Zhou. In-situ investigation of melting characteristics of waste selective catalytic reduction catalysts during harmless melting treatment[J]. Journal of Zhejiang University Science A, 2021, 22(3): 207-221.

@article{title="In-situ investigation of melting characteristics of waste selective catalytic reduction catalysts during harmless melting treatment",
author="Hao Zhou, Yu-jian Xing, Jia-nuo Xu, Ming-xi Zhou",
journal="Journal of Zhejiang University Science A",
publisher="Zhejiang University Press & Springer",

%0 Journal Article
%T In-situ investigation of melting characteristics of waste selective catalytic reduction catalysts during harmless melting treatment
%A Hao Zhou
%A Yu-jian Xing
%A Jia-nuo Xu
%A Ming-xi Zhou
%J Journal of Zhejiang University SCIENCE A
%V 22
%N 3
%P 207-221
%@ 1673-565X
%D 2021
%I Zhejiang University Press & Springer
%DOI 10.1631/jzus.A2000192

T1 - In-situ investigation of melting characteristics of waste selective catalytic reduction catalysts during harmless melting treatment
A1 - Hao Zhou
A1 - Yu-jian Xing
A1 - Jia-nuo Xu
A1 - Ming-xi Zhou
J0 - Journal of Zhejiang University Science A
VL - 22
IS - 3
SP - 207
EP - 221
%@ 1673-565X
Y1 - 2021
PB - Zhejiang University Press & Springer
ER -
DOI - 10.1631/jzus.A2000192

Selective catalytic reduction (SCR) catalyst waste is a hazardous solid waste that seriously threatens the environment and public health. In this study, a thermal melting technology is proposed for the treatment of waste SCR catalysts. The melting characteristics and mineral phase transformation of waste SCR catalysts blended with three different groups of additives were explored by heating stage microscopy, thermogravimetric analysis/differential scanning calorimetry (TG/DSC) analysis, thermodynamic simulation, and X-ray diffraction (XRD) analysis; heavy metal leaching toxicity was tested by inductively coupled plasma-atomic emission spectrometry (ICP-AES) analysis. The results indicated that the melting point of waste SCR catalysts can be effectively reduced with proper additives. The additive formula of 39.00% Fe2O3 (in weight), 6.50% CaO, 3.30% SiO2, and 1.20% Al2O3 achieves the optimal fluxing behavior, significantly decreasing the initial melting temperature from 1223 °C to 1169 °C. Furthermore, the whole heating process of waste SCR catalysts can be divided into three stages: the solid reaction stage, the sintering stage, and the primary melting stage. The leaching concentrations of V, As, Pb, and Se are significantly reduced, from 10.64, 1.054, 0.195, and 0.347 mg/L to 0.178, 0.025, 0.048, and 0.003 mg/L, respectively, much lower than the standard limits after melting treatment, showing the strong immobilization capacity of optimal additives for heavy metals in waste SCR catalysts. The results demonstrate the feasibility of harmless melting treatments for waste SCR catalysts with relatively low energy consumption, providing theoretical support for a novel method of disposing of hazardous waste SCR catalysts.


创新点:1. 对加入添加剂后废弃SCR催化剂的无害化熔融处理过程进行了原位研究;2. 确定了最佳的添加剂配比,进而显著降低了重金属浸出浓度.
结论:1. 添加剂可有效降低废弃SCR催化剂的熔点;39.00% Fe2O3、6.50% CaO、3.30% SiO2和1.20% Al2O3的添加剂配方具有最佳的助熔性能,可将初始熔化温度从1223 °C降至1169 °C.2. 废弃SCR催化剂的加热过程可分为三个阶段:固相反应阶段、烧结阶段和初始熔融阶段.3. 熔融处理可显著降低重金属V、As、Pb和Se的浸出浓度;以较低的能耗对废弃SCR催化剂进行无害化熔融处理是可行的.


Darkslateblue:Affiliate; Royal Blue:Author; Turquoise:Article


[1]Chen JN, Xu SS, Guo SK, 2016. National hazardous wastes catalogue. Shanghai Building Materials, 4:1-11 (in Chinese).

[2]Cheng LC, Wu SH, Huang KL, et al., 2013. Evaluation of effect of reducing additives during vitrification via simulation and experiment. Journal of the Air & Waste Management Association, 63(10):1182-1189.

[3]Cheng TW, Chu JP, Tzeng CC, et al., 2002. Treatment and recycling of incinerated ash using thermal plasma technology. Waste Management, 22(5):485-490.

[4]Choi IH, Kim HR, Moon G, et al., 2018. Spent V2O5-WO3/ TiO2 catalyst processing for valuable metals by soda roasting-water leaching. Hydrometallurgy, 175:292-299.

[5]Furimsky E, 1996. Spent refinery catalysts: environment, safety and utilization. Catalysis Today, 30(4):223-286.

[6]Gupta SK, Gupta RP, Bryant GW, et al., 1998. The effect of potassium on the fusibility of coal ashes with high silica and alumina levels. Fuel, 77(11):1195-1201.

[7]Jak E, 2002. Prediction of coal ash fusion temperatures with the F*A*C*T thermodynamic computer package. Fuel, 81(13):1655-1668.

[8]Kandiel TA, Robben L, Alkaim A, et al., 2013. Brookite versus anatase TiO2 photocatalysts: phase transformations and photocatalytic activities. Photochemical & Photobiological Sciences, 12(4):602-609.

[9]Kikuchi R, 2001. Recycling of municipal solid waste for cement production: pilot-scale test for transforming incineration ash of solid waste into cement clinker. Resources, Conservation and Recycling, 31(2):137-147.

[10]Kuo YM, Lin TC, Tsai PJ, 2003. Effect of SiO2 on immobilization of metals and encapsulation of a glass network in slag. Journal of the Air & Waste Management Association, 53(11):1412-1416.

[11]Lee JB, Eom YS, Kim JH, et al., 2013. Regeneration of waste SCR catalyst by air lift loop reactor. Journal of Central South University, 20(5):1314-1318.

[12]Li JZ, Wang XY, Wang B, et al., 2017. Effect of silica and alumina on petroleum coke ash fusibility. Energy & Fuels, 31(12):13494-13501.

[13]Li M, Liu B, Wang XR, et al., 2018. A promising approach to recover a spent SCR catalyst: deactivation by arsenic and alkaline metals and catalyst regeneration. Chemical Engineering Journal, 342:1-8.

[14]Li RD, Wang L, Yang TH, et al., 2007. Investigation of MSWI fly ash melting characteristic by DSC-DTA. Waste Management, 27(10):1383-1392.

[15]Li ZM, Li JF, Sun YQ, et al., 2016. Effect of Al2O3 addition on the precipitated phase transformation in Ti-bearing blast furnace slags. Metallurgical and Materials Transactions B, 47:1390-1399.

[16]Liang ZY, Yan GY, Zheng LP, et al., 2011. A primary study on preparation of mullite with solid waste. Advanced Materials Research, 233-235:1067-1072.

[17]Lin KL, Huang WJ, Chen KC, et al., 2009. Behaviour of heavy metals immobilized by co-melting treatment of sewage sludge ash and municipal solid waste incinerator fly ash. Waste Management & Research, 27(7):660-667.

[18]Lindberg D, Molin C, Hupa M, 2015. Thermal treatment of solid residues from WtE units: a review. Waste Management, 37:82-94.

[19]Liu B, He QH, Jiang ZH, et al., 2013. Relationship between coal ash composition and ash fusion temperatures. Fuel, 105:293-300.

[20]Liu GR, Zhan JY, Zheng MH, et al., 2015. Field pilot study on emissions, formations and distributions of PCDD/Fs from cement kiln co-processing fly ash from municipal solid waste incinerations. Journal of Hazardous Materials, 299: 471-478.

[21]Liu YY, Wang JJ, Lin X, et al., 2012. Microstructures and thermal properties of municipal solid waste incineration fly ash. Journal of Central South University, 19(3):855-862.

[22]Marafi M, Stanislaus A, 2003. Options and processes for spent catalyst handling and utilization. Journal of Hazardous Materials, 101(2):123-132.

[23]MEE (Ministry of Ecology and Environment of the People’s Republic of China), 2007a. Identification Standards for Hazardous Waste–Identification for Extraction Toxicity, GB 5085.3-2007. Standardization Administration of the People’s Republic of China (in Chinese).

[24]MEE (Ministry of Ecology and Environment of the People’s Republic of China), 2007b. Solid Waste–Extraction Procedure for Leaching Toxicity–Acetic Acid Buffer Solution Method, HJ/T 300-2007. MEE (in Chinese).

[25]Min Y, Qin CD, Shi PY, et al., 2017. Effect of municipal solid waste incineration fly ash addition on the iron ore sintering process, mineral phase and metallurgical properties of iron ore sinter. ISIJ International, 57(11):1955-1961.

[26]Min Y, Liu CJ, Shi PY, et al., 2018. Effects of the addition of municipal solid waste incineration fly ash on the behavior of polychlorinated dibenzo-p-dioxins and furans in the iron ore sintering process. Waste Management, 77:287-293.

[27]Mymrin V, Pedroso AM, Ponte HA, et al., 2017. Thermal engineering method application for hazardous spent petrochemical catalyst neutralization. Applied Thermal Engineering, 110:1428-1436.

[28]Pan JR, Huang C, Kuo JJ, et al., 2008. Recycling MSWI bottom and fly ash as raw materials for Portland cement. Waste Management, 28(7):1113-1118.

[29]Peng Y, Li JH, Si WZ, et al., 2015. Deactivation and regeneration of a commercial SCR catalyst: comparison with alkali metals and arsenic. Applied Catalysis B: Environmental, 168-169:195-202.

[30]Qiu JR, Li F, Zheng Y, et al., 1999. The influences of mineral behaviour on blended coal ash fusion characteristics. Fuel, 78(8):963-969.

[31]Ramezani A, Emami SM, Nemat S, 2017. Reuse of spent FCC catalyst, waste serpentine and kiln rollers waste for synthesis of cordierite and cordierite-mullite ceramics. Journal of Hazardous Materials, 338:177-185.

[32]Rani DA, Gome E, Boccaccini AR, et al., 2008. Plasma treatment of air pollution control residues. Waste Management, 28(7):1254-1262.

[33]Sakai SI, Hiraoka M, 2000. Municipal solid waste incinerator residue recycling by thermal processes. Waste Management, 20(2-3):249-258.

[34]Shang XS, Li JR, Yu XW, et al., 2012. Effective regeneration of thermally deactivated commercial V-W-Ti catalysts. Frontiers of Chemical Science and Engineering, 6(1):38-46.

[35]Shi J, He F, Ye CQ, et al., 2017. Preparation and characterization of CaO-Al2O3-SiO2 glass-ceramics from molybdenum tailings. Materials Chemistry and Physics, 197: 57-64.

[36]Song WJ, Tang LH, Zhu XD, et al., 2010. Effect of coal ash composition on ash fusion temperatures. Energy & Fuels, 24(1):182-189.

[37]Sun DD, 2003. Stabilization treatment for reutilization of spent refinery catalyst into value-added product. Energy Sources, 25(6):607-615.

[38]Sun DD, Tay JH, Cheong HK, et al., 2001. Recovery of heavy metals and stabilization of spent hydrotreating catalyst using a glass-ceramic matrix. Journal of Hazardous Materials, 87(1-3):213-223.

[39]Takaoka M, Takeda N, Miura S, 1997. The behaviour of heavy metals and phosphorus in an ash melting process. Water Science and Technology, 36(11):275-282.

[40]Verbinnen B, Billen P, van Caneghem J, et al., 2017. Recycling of MSWI bottom ash: a review of chemical barriers engineering application and treatment technologies. Waste and Biomass Valorization, 8(5):1453-1466.

[41]Wang L, Jamro IA, Chen Q, et al., 2016. Immobilization of trace elements in municipal solid waste incinerator (MSWI) fly ash by producing calcium sulphoaluminate cement after carbonation and washing. Waste Management & Research, 34(3):184-194.

[42]Wang XT, Jin BS, Xu B, et al., 2017. Melting characteristics during the vitrification of MSW incinerator fly ash by swirling melting treatment. Journal of Material Cycles and Waste Management, 19(1):483-495.

[43]Wu WC, Tsai TY, Shen YH, 2016. Tungsten recovery from spent SCR catalyst using alkaline leaching and ion exchange. Minerals, 6(4):107.

[44]Xiao HP, Ru Y, Peng Z, et al., 2018. Destruction and formation of polychlorinated dibenzo-p-dioxins and dibenzofurans during pretreatment and co-processing of municipal solid waste incineration fly ash in a cement kiln. Chemosphere, 210:779-788.

[45]Xu SX, Chen T, Li XD, et al., 2018. Behavior of PCDD/Fs, PCBs, CBzs and PAHs during thermal treatment of various fly ash from steel industry. Aerosol and Air Quality Research, 18:1008-1018.

[46]Yan TG, Kong LX, Bai J, et al., 2016. Thermomechanical analysis of coal ash fusion behavior. Chemical Engineering Science, 147:74-82.

[47]Yan TG, Bai J, Kong LX, et al., 2017. Effect of SiO2/Al2O3 on fusion behavior of coal ash at high temperature. Fuel, 193:275-283.

[48]Yang JK, Xiao B, Boccaccini AR, 2009. Preparation of low melting temperature glass-ceramics from municipal waste incineration fly ash. Fuel, 88(7):1275-1280.

[49]Yang MR, Lv XW, Wei RR, et al., 2018. Wetting behavior of TiO2 by calcium ferrite slag at 1523 K. Metallurgical and Materials Transactions B, 49(5):2667-2680.

[50]You KK, Ma XC, Liu JT, et al., 2012. Characteristic analysis of SCR flue gas denitrification catalyst in power plant. Advanced Materials Research, 518-523:2423-2426.

[51]Zhang YK, Ren QQ, Deng HX, et al., 2017. Ash fusion properties and mineral transformation behavior of gasified semichar at high temperature under oxidizing atmosphere. Energy & Fuels, 31(12):14228-14236.

[52]Zhang ZK, Li AM, Liang XY, 2014. Effects of basicity (CaO/SiO2) on the behavior of heavy metals from sludge incineration ash by vitrification treatment. Advanced Materials Research, 878:284-291.

[53]Zhao ZP, Guo M, Zhang M, 2015. Extraction of molybdenum and vanadium from the spent diesel exhaust catalyst by ammonia leaching method. Journal of Hazardous Materials, 286:402-409.

[54]Zheng YJ, Jensen AD, Johnsson JE, 2005. Deactivation of V2O5-WO3-TiO2 SCR catalyst at a biomass-fired combined heat and power plant. Applied Catalysis B: Environmental, 60(3-4):253-264.

[55]Zhou H, Guo XT, Zhou MX, 2017. Influence of different additives on harmless melting treatment of waste SCR catalysts. Journal of Chinese Society of Power Engineering, 37(12):999-1006 (in Chinese).

[56]Zhu KR, Zhang MS, Hong JM, et al., 2005. Size effect on phase transition sequence of TiO2 nanocrystal. Materials Science and Engineering: A, 403(1-2):87-93.

Open peer comments: Debate/Discuss/Question/Opinion


Please provide your name, email address and a comment

Journal of Zhejiang University-SCIENCE, 38 Zheda Road, Hangzhou 310027, China
Tel: +86-571-87952783; E-mail: cjzhang@zju.edu.cn
Copyright © 2000 - Journal of Zhejiang University-SCIENCE