Low-temperature CO selective catalytic reduction denitrification and sulfuric acid regeneration mechanism of Cu-Ce/AC catalyst poisoned with zinc salt

被引:4
|
作者
Wen, Zhenjing [1 ,2 ]
Huang, Bangfu [1 ,2 ,3 ]
Shi, Zhe [1 ,2 ]
Li, Wanjun [1 ,2 ]
Luo, Liubin [1 ,2 ]
Zi, Gaoyong [1 ,2 ]
Yang, Linjing [1 ]
机构
[1] Kunming Univ Sci & Technol, Fac Met & Energy Engn, Kunming 650093, Peoples R China
[2] Univ Yunnan Prov, Clean Met Key Lab Complex Iron Resources, Kunming 650093, Peoples R China
[3] Kunming Univ Sci & Technol, Univ Yunnan Prov, Fac Met & Energy Engn, Clean Met Key Lab Complex Iron Resources, Kunming 650093, Yunnan, Peoples R China
基金
中国国家自然科学基金;
关键词
Sulfuric acid; Regeneration mechanism; Zinc salt; Poison mechanism; Cu -Ce/AC catalyst; ACTIVATED SEMI-COKE; METAL-OXIDES; NO; NH3-SCR; CARBON; SCR; MN; REMOVAL; DEACTIVATION; DENITRATION;
D O I
10.1016/j.fuel.2023.129621
中图分类号
TE [石油、天然气工业]; TK [能源与动力工程];
学科分类号
0807 ; 0820 ;
摘要
To explore Cu-Ce/activated carbon (AC) catalyst poisoned of with zinc salt and its mechanism of lowtemperature CO selective catalytic reduction (CO-SCR) denitrification following sulfuric acid regeneration, this paper uses ZnCl2 and ZnSO4 to poison Cu-Ce/AC catalyst and H2SO4 pickling to regenerate the poisoned catalyst. Not only the catalyst denitrification activity was investigated but also the surface morphology, pore structure, variation of active component phases and elemental valence, surface functional groups, reduction characteristics and adsorption mechanism of catalyst before and after regeneration were systematically characterized. The low-temperature CO-SCR denitrification mechanism of the poisoned Cu-Ce/AC catalyst was revealed. After being poisoned with zinc salt, the oxide on the catalyst surface aggregated, causing the blockage of the pore, thereby inhibiting the adsorption capacity of the reaction gas and the synergistic reaction between Cu-Ce. Moreover, zinc salt not only occupies the active site, but also destroys the -C=O and -OH oxygencontaining functional groups. This not only reduces the chemically adsorbed oxygen (O & beta;) and oxygen vacancy but also leads to the reduction of Cu+-CO species, the reduction of catalyst redox capacity, and the reduction of NO conversion rate. The regeneration mechanism of the sulfuric acid method was as follows. First, the solid particles deposited on the catalyst surface are removed, thereby restoring its specific surface area and pore structure, and increasing the adsorption area of reaction gas. Additionally, the content of Cu and Ce active components was increased, which promoted the synergistic reaction, and the content of Cu+-CO species, oxygen vacancy, and O & beta; was increased, resulting in enhanced redox capacity. Finally, sulfuric acid impregnation generated S2O82  groups, which sulfated the surface of the catalyst, and its S=O reacted with Zn to form S-O-S, which prevented zinc salt from destroying the oxygen-containing functional groups and improved the reducing capacity and CO adsorption capacity of the catalyst, thereby restoring the denitrification activity of the catalyst.
引用
收藏
页数:15
相关论文
共 32 条
  • [21] Superior performance of Cu/TiO2 catalyst prepared by ice melting method for low-temperature selective catalytic reduction of NOx by NH3
    Wang, Xueman
    Chen, Xiongbo
    Ye, Lyumeng
    Lu, Peng
    Liu, Ying
    You, Jiaqi
    Zeng, Wenhao
    Lu, Long
    Hu, Chunhua
    Chen, Dingsheng
    MOLECULAR CATALYSIS, 2020, 497 (497)
  • [22] The activity and mechanism study of Fe-Mn-Ce/γ-Al2O3 catalyst for low temperature selective catalytic reduction of NO with NH3
    Cao, Fan
    Su, Sheng
    Xiang, Jun
    Wang, Pengying
    Hu, Song
    Sun, Lushi
    Zhang, Anchao
    FUEL, 2015, 139 : 232 - 239
  • [23] Selective catalytic reduction of nitric oxide with a novel Mn-Ti-Ce oxide core-shell catalyst having improved low-temperature activity and water tolerance
    Li, Huirong
    Schill, Leonhard
    Fehrmann, Rasmus
    Riisager, Anders
    JOURNAL OF THE ENERGY INSTITUTE, 2023, 109
  • [24] A strategy for constructing highly efficient yolk-shell Ce@Mn@TiOx catalyst with dual active sites for low-temperature selective catalytic reduction of NO with NH3
    Huang, Xiaosheng
    Dong, Fang
    Zhang, Guodong
    Guo, Yan
    Tang, Zhicheng
    CHEMICAL ENGINEERING JOURNAL, 2021, 419
  • [25] A comparative study on the activity and adsorption of bimetallic MOF-derived Me-Cu/TiO2 (Me=Fe, Co, Ni) for low-temperature selective catalytic reduction of NO by CO
    Shi, Yong
    Ma, Xin Lan
    Gao, Jin Suo
    Yu, Feng Yun
    Li, Chun Yan
    Xiong, Wei
    Huang, Li Ping
    SURFACES AND INTERFACES, 2024, 53
  • [26] Catalytic ozonation for low-temperature NOx (x=1, 2) removal with •OH radicals over Cu doped Ce0.90Co0.10O2 - δ catalysts and mechanism analysis
    Guo, Lina
    Zhong, Qin
    Ding, Jie
    Deng, Zhiyong
    Zhao, Wenkai
    FUEL PROCESSING TECHNOLOGY, 2017, 167 : 545 - 554
  • [27] In Situ DRIFTs Investigation of the Low-Temperature Reaction Mechanism over Mn-Doped Co3O4 for the Selective Catalytic Reduction of NOx with NH3
    Hu, Hang
    Cai, Sixiang
    Li, Hongrui
    Huang, Lei
    Shi, Liyi
    Zhang, Dengsong
    JOURNAL OF PHYSICAL CHEMISTRY C, 2015, 119 (40) : 22924 - 22933
  • [28] Activity Test and Mechanism Study of 3DOM Ce0.8M0.1Zr0.1O2 (M=Cr, Sn, Fe, Co, Ni, Mn, Cu) Catalyst in the Selective Catalytic Reduction of NO by CO**
    Liu, Xia
    Liu, Hao
    Li, Danyang
    Ning, Gangjie
    Li, Xinxin
    Dong, Lihui
    Li, Bin
    CHEMCATCHEM, 2021, 13 (23) : 4998 - 5011
  • [29] Influence of SiO2 on MiTiO2 (M = Cu, Mn, and Ce) Formulations for Low-Temperature Selective Catalytic Reduction of NOx with NH3: Surface Properties and Key Components in Relation to the Activity of NOx Reduction
    Boningari, Thirupathi
    Pappas, Dimitrios K.
    Ettireddy, Padmanabha R.
    Kotrba, Adam
    Smirniotis, Panagiotis G.
    INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2015, 54 (08) : 2261 - 2273
  • [30] Synergistic effect and mechanism of FeOx and CeOx co-doping on the superior catalytic performance and SO2 tolerance of Mn-Fe-Ce/ACN catalyst in low-temperature NH3-SCR of NOx
    Jiang, Lijun
    Liang, Ya
    Liu, Weizao
    Wu, Hongli
    Aldahri, Tahani
    Carrero, Dennise Sosa
    Liu, Qingcai
    JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING, 2021, 9 (06):