A promising approach to recover a spent SCR catalyst: Deactivation by arsenic and alkaline metals and catalyst regeneration

被引:84
作者
Li, Meng [1 ,2 ,3 ]
Liu, Biao [2 ]
Wang, Xinran [2 ]
Yu, Xiaobin [5 ]
Zheng, Shili [2 ]
Du, Hao [2 ,4 ]
Dreisinger, David [3 ]
Zhang, Yi [2 ]
机构
[1] Northeastern Univ, Sch Met, Shenyang 110819, Liaoning, Peoples R China
[2] Chinese Acad Sci, Inst Proc Engn, Natl Engn Lab Hydromet Cleaner Prod Technol, Key Lab Green Proc & Engn, Beijing 100190, Peoples R China
[3] Univ British Columbia, Dept Mat Engn, Vancouver, BC V6T 1Z4, Canada
[4] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[5] Tianjin Univ, Sch Chem Engn, Tianjin 300072, Peoples R China
基金
中国国家自然科学基金;
关键词
Spent SCR catalyst; Hazardous waste; Arsenic; Oxidative ammonium leaching; Catalyst regeneration; RADICAL GENERATION; VANADIUM; EXTRACTION; MOLYBDENUM; POTASSIUM; IRON;
D O I
10.1016/j.cej.2017.12.132
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
A large amount of spent selective catalytic reduction (SCR) catalyst is generated annually. The spent SCR catalyst is poisoned by arsenic and alkaline metals. These spent catalysts also contain substantial amounts of heavy metals and are therefore considered as hazardous solid waste. In order to decontaminate the catalysts from As, K and Na poisoning, recover the valuable metals (V and W) and regenerate the catalysts, an efficient and green advanced oxidation process (AOPs) named oxidative ammonium bicarbonate leaching (OABL) at moderate temperature and ambient pressure was developed. The effect of the leaching parameters on the V, W, As, Na, K and Ti leaching efficiencies was investigated. The mechanisms of V5+ and W6+ species extraction process were investigated. Furthermore, the mechanism of extraction of the low valent As3+ was studied by ESR and a V4+ triggered Fenton-like reaction was proposed. The crystal structure of the catalyst substrate anatase (TiO2) was not affected by the leaching process. After impregnation with active components, the activity of the regenerated SCR catalyst was close to the level of the fresh catalyst with an NO conversion of 91% at 400 degrees C. Therefore, this work has introduced a new method for efficient regeneration of the spent catalyst.
引用
收藏
页码:1 / 8
页数:8
相关论文
共 44 条
[1]   Radical generation by the interaction of transition metals with common oxidants [J].
Anipsitakis, GP ;
Dionysiou, DD .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2004, 38 (13) :3705-3712
[2]   A review on Fenton and improvements to the Fenton process for wastewater treatment [J].
Babuponnusami, Arjunan ;
Muthukumar, Karuppan .
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING, 2014, 2 (01) :557-572
[3]   HOMOGENEOUS BASE-CATALYZED DECOMPOSITION OF HYDROGEN PEROXIDE [J].
DUKE, FR ;
HAAS, TW .
JOURNAL OF PHYSICAL CHEMISTRY, 1961, 65 (02) :304-&
[4]   Activation of persulfate with vanadium species for PCBs degradation: A mechanistic study [J].
Fang, Guodong ;
Wu, Wenhui ;
Liu, Cun ;
Dionysiou, Dionysios D. ;
Deng, Yamei ;
Zhou, Dongmei .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2017, 202 :1-11
[5]   Accelerated crystallization of zeolites via hydroxyl free radicals [J].
Feng, Guodong ;
Cheng, Peng ;
Yan, Wenfu ;
Boronat, Mercedes ;
Li, Xu ;
Su, Ji-Hu ;
Wang, Jianyu ;
Li, Yi ;
Corma, Avelino ;
Xu, Ruren ;
Yu, Jihong .
SCIENCE, 2016, 351 (6278) :1188-1191
[6]   Present status and perspectives in de-NOx SCR catalysis [J].
Forzatti, P .
APPLIED CATALYSIS A-GENERAL, 2001, 222 (1-2) :221-236
[7]   Thermodynamic and kinetic studies of palladium (II) extraction by extractant mixtures containing LIX 63 Part I. Thermodynamic study [J].
Foulon, C ;
Pareau, D ;
Durand, G .
HYDROMETALLURGY, 1999, 51 (02) :139-153
[8]   RECOVERY OF CO, NI, MO, AND V FROM UNROASTED SPENT HYDROREFINING CATALYSTS BY SELECTIVE CHLORINATION [J].
GABALLAH, I ;
DJONA, M .
METALLURGICAL AND MATERIALS TRANSACTIONS B-PROCESS METALLURGY AND MATERIALS PROCESSING SCIENCE, 1995, 26 (01) :41-50
[9]   Hydroxyl radical generation linked with iron dissolution and dissolved oxygen consumption in zero-valent iron wastewater treatment process [J].
Harada, Takuma ;
Yatagai, Tomonori ;
Kawase, Yoshinori .
CHEMICAL ENGINEERING JOURNAL, 2016, 303 :611-620
[10]  
He L.-P., 2016, ACS SUSTAINABLE CHEM