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Laox Modi Ed Mnox Loaded Biomass Activated Carbon and Its Enhanced LaOx Modied MnOx Loaded Biomass Activated Carbon and its Enhanced Performance for Simultaneous Abatement of NO and Hg0 Lei Yi University of South China Jinke Xie University of South China Caiting Li Hunan University Jian Shan University of South China Yingyun Liu University of South China Junwen Lv University of South China Mi Li University of South China Lei Gao ( [email protected] ) University of South China Research Article Keywords: simultaneous removal, NO, elemental mercury(Hg0), SO2 tolerance, H2O resistance Posted Date: June 12th, 2021 DOI: https://doi.org/10.21203/rs.3.rs-554847/v1 License: This work is licensed under a Creative Commons Attribution 4.0 International License. Read Full License Version of Record: A version of this preprint was published at Environmental Science and Pollution Research on August 7th, 2021. See the published version at https://doi.org/10.1007/s11356-021-15752- y. 1 LaOx modified MnOx loaded biomass activated carbon and its enhanced performance for 2 simultaneous abatement of NO and Hg0 3 Lei Yi#,a, Jinke Xie#,a, Caiting Lib, Jian Shana, Yingyun Liua, Junwen Lva, Mi Lia, Lei Gao,a,b 4 aSchool of Resources Environment and Safety Engineering, University of South China, Hengyang 5 421001, PR China 6 bCollege of Environmental Science and Engineering, Hunan University, Changsha 410082, PR 7 China 8 # These authors contributed equally to this work and should be considered co-first authors 9 Corresponding author. Tel.: +15274800478 E-mail address: [email protected]; [email protected]. 10 Abstract 11 A battery of agricultural straw derived biomass activated carbons supported LaOx modified 12 MnOx (LaMn/BACs) was prepared by a facile impregnation method and then tested for the 13 efficiency of simultaneous abatement of NO and Hg0. 15%LaMn/BAC manifested excellent 14 removal efficiency of Hg0 (100%) and NO (86.7%) at 180 °C, which also exhibited splendid 0 15 resistance to SO2 and H2O. The interaction between Hg removal and NO removal was explored, 16 thereinto Hg0 removal had no influence on NO removal, while NO removal preponderated over 0 17 Hg removal. The inhibitory effect of NH3 was greater than the accelerative effect of NO and O2 18 on Hg0 removal. The physicochemical characterization of related samples were characterized by 19 SEM, XRD, BET, H2-TPR, NH3-TPD and XPS. After incorporating suitable LaOx into 20 15%Mn/BAC, the synergistic effect between LaOx and MnOx contributed to the improvement of 21 BET surface area and total pore volume, the promotion of redox ability, surface active oxygen 22 species and acid sites, inhibiting the crystallization of MnOx. 15%LaMn/BAC has the best 23 catalytic oxidation activity at low temperature. That might be answerable for superior performance 24 and preferable tolerance to SO2 and H2O. Finally, the principle of catalytic oxidation was also 25 discussesed in this article. 0 26 Keywords: simultaneous removal, NO, elemental mercury(Hg ), SO2 tolerance, H2O resistance 27 28 29 30 31 32 1. Introduction 33 With the implementation of the ultra-low emission and energy saving of coal-fired power 34 plant plan since 2015 in China, electrostatic precipitator (ESP) or fabric filter (FF) system, wet 35 flue gas desulfurization (WFGD) unit and selective catalytic reduction (SCR) devices have been 36 extensively adopted for corresponding pollutants abatement (Liu et al., 2018; Zhao et al., 2019a; 37 Gao et al., 2018a). Consequently, following SO2, NOx and dust, mercury emission has triggered 38 tremendous concerns due to its severe toxicity, high persistence, toilless mobility and strong 39 biological magnification in the food chain and ecosystem after it is converted into more venomous 40 methylmercury (Gao et al., 2018a; Xu et al., 2018a; Wang et al., 2017; Liu et al., 2019a). It is well 41 recognized that elemental mercury (Hg0), oxidized mercury (Hg2+) and particle-bound mercury 42 (Hgp) coexist in coal-fired flue gas (Wang et al., 2017; Yang et al., 2019a). Thereinto, Hg2+ and 43 Hgp can be readily captured by WFGD and ESP or FF, respectively (Xu et al., 2018a; Chi et al., 44 2017; Shan et al., 2019). However, Hg0 (the major mercury form) is untoward to remove by 45 currently environmental protection devices in consideration of its water insolubility and strong 46 volatility (Gao et al., 2018b; Xu et al., 2016; Shen et al., 2018a; Jiang et al., 2018). Thus, the 47 emphasis and difficulty of eliminating mercury pollution lie in controlling Hg0 emission. 48 In response to increasing environmental consciousness and rigorous mercury emission 49 regulations, plentiful technologies including catalytic oxidation and adsorption have been 50 tremendously researched for Hg0 removal in recent years (Gao et al., 2018a; Zhang et al., 2017a; 51 Yang et al., 2019a). To date, activated carbon injection (ACI) for Hg0 abatement is a commercial 52 technology (Shen et al., 2018b; Zhao et al., 2018; Shi et al., 2019). However, it suffers from some 53 intractable bottlenecks, such as potential secondary contamination, huge operating costs, tardy 54 regeneration rates and the value deterioration of fly ash (Zhang et al., 2017a; Zhao et al., 2018; 55 Zhang et al., 2018). Furthermore, controlling NO and Hg0 emissions by utilizing SCR and ACI 56 independently confronts several inevitable shortcomings such as large equipment investment, high 57 land requirement, huge maintaining and operating costs (Gao et al., 2018a; Gao et al., 2018b; 58 Chen et al., 2020). It is essential to use the ameliorative SCR catalyst to achieve efficient 0 59 reduction of NOx and oxidation of Hg without subjoining equipment for considering 60 comprehensive benefits, various types of SCR catalysts have been studied to that (Li et al., 2018; 61 Zhang et al., 2021). Fortunately, it is well accepted that vanadium-based SCR catalyst can make 62 part Hg0 oxidize to Hg2+, but the converting ability from Hg0 to Hg2+ is relatively limited in low 63 chlorine flue gas (Jiang et al., 2018; Zhang et al., 2018; Chen et al., 2018). In addition, such 64 catalyst has to operate at a temperature range of 300–400 °C and that urges SCR unit to be placed 65 upstream of desulfurization and dedusting devices where catalyst is readily impaired by SO2 and 66 dust (Jiang et al., 2018; Zhang et al., 2021). Moreover, V2O5 itself poses certain threat to the 67 environment and human health (Li et al., 2018; Zhang et al., 2021). Notably, to overcome 68 above-mentioned deficiencies, it is significantly needful to develop preferable cryogenic catalysts 69 with outstanding demercuration and denitration efficiencies, realizing simultaneous removal of 70 Hg0 and NO by the existing gas purification devices. 71 Thus, in order to achieve these objectives, numerous novel catalysts, such as Mn-Ce/TiO2, 72 CuO-MnOx/AC-H, La0.8Ce0.2MnO3, have been researched for simultaneous abatement of NO and 73 Hg0 (Shen et al., 2018b; Zhao et al., 2019; Zhang et al., 2017b). Thereinto, manganese oxides 74 (MnOx) catalysts with splendid cryogenic performance have been extensively investigated for NO 75 and Hg0 removal in view of preeminent properties of Mn species, such as the nature of labile 76 oxygen, outstanding redox properties, diversiform oxidation states and high oxygen 77 storage/release capacity as well as environmental friendliness, abundant reserves and cheap price 78 (Zhao et al., 2019b; Xu et al., 2018b; Fan et al., 2018). Nevertheless, some MnOx-based catalysts 79 especially unsupported ones often bore with several shortcomings, such as poor tolerance to SO2 80 and H2O, low thermal stability and little specific surface area, which impeded their actual 81 applications (Zhang et al., 2018; Fan et al., 2018). Furthermore, La2O3 can be used as an effective 82 promoter to improve the dispersion of active components to obtain a catalyst with high stability 83 and activity (Shen et al., 2018b). Studies have shown that the addition of La promotes the low 84 temperature activity to Hg0 and NO (Gao et al., 2018b; Yang et al., 2018a). Therefore, the 85 manganese-based catalyst modified by lanthanum species may exhibit excellent 86 performance. 87 As shown in literature, numerous carbon-based catalysts with AC/BAC carriers not only 88 exhibited good performances for Hg0 and NO simultaneous abatement at low temperature, but also 89 often demonstrated great resistance to SO2 and H2O (Gao et al., 2018a; Ren et al., 2017). That 90 preeminent manifestations were possibly attributed to the excellent physicochemical 91 characteristics of carbonaceous materials, and the good SO2 tolerance was related to the large 92 surface areas and abundant oxygen-containing functional groups (Ren et al., 2017; Guo et al., 93 2015), while the high H2O resistance might be associated with hydrophobic property of carbon 94 materials (Abdelouahab-Reddam et al., 2015; Joung et al., 2014). Therefore, manganese oxides 95 loaded on BAC derived from agricultural straw wastes may be a promising catalyst for Hg0 and 96 NO simultaneous removal at low temperature. To the best of our knowledge, few studies related to 0 97 LaOx modified MnOx/BAC for simultaneous abatement of Hg and NO have been reported in 98 publications, in which the synergistic effect between MnOx and LaOx might have a positive role 99 on aggrandizing performance and tolerance to SO2 and H2O. Consequently, a battery of systematic 100 tests are performed to elucidate its performance for NO and Hg0 simultaneous abatement over 101 LaMn/BAC catalysts in this work. 102 2. Materials and methods 103 2.1. Materials preparation 104 The manufacture method of BAC carrier was detailedly presented in our previous paper (Gao 105 et al., 2018a). Lanthanum nitrates or manganese acetates acted as the precursors of LaOx and 106 MnOx, respectively. The preparation steps of La/BAC, Mn/BAC and LaMn/BAC were shown 107 below.
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