Abstract：FeMnCoNi-O nanoparticles (NPs) with outstanding structural stability and catalytic performance were synthesized by coprecipitation and consequent calcination method. The FeMnCoNi-O NPs were carefully characterized by X-Ray diffraction (XRD), transmission electron microscope (TEM), Fourier transform infrared spectroscopy (FT-IR), thermal gravimetric analyzer (TG) and X-ray photoelectron spectroscopy (XPS) techniques. Furthermore, the obtained catalyst was applied to activate potassium persulfate (PMS) and degrade Rhodamine B (RhB). The effects of reaction conditions such as the concentration of the RhB, PMS and catalysts concentration, the kinds of pollutant and aqueous pH values, on the degradation process and the recycling performance were systematically investigated. Via the calcined treatment (200oC, 2h), the final product was the multi-metal oxide, which exhibited enhanced catalytic performance for the RhB degradation. FeMnCoNi-O NPs can achieve complete degradation of RhB (20mg/L) in 10minutes by activating trace amounts of PMS (0.2mmol/L). With the help of free radical quenching experiment and XPS analysis, it is found the main active substances in the degradation system were 1O2 and SO4·- generated via persulfate activation.
[1] Van Vliet M T H, Jones E R, flörke M, et al. Global water scarcity including surface water quality and expansions of clean water technologies [J]. Environmental Research Letters, 2021,16:024020. [2] Zhang R, Li Z, Wang X, et al. Adsorption equilibrium of activated carbon amid fluctuating benzene concentration in indoor environments [J]. Building and Environment, 2023,245:110964. [3] Janjhi F A, Ihsanullah I, Bilal M, et al. MXene-based materials for removal of antibiotics and heavy metals from wastewater- a review [J]. Water Resources and Industry, 2023,29:100202. [4] Ramesh B, Saravanan A, Senthil Kumar P, et al. A review on algae biosorption for the removal of hazardous pollutants from wastewater: Limiting factors, prospects and recommendations [J]. Environmental Pollution, 2023,327:121572. [5] Ganiyu S O, Sable S, Gamal El-Din M. Advanced oxidation processes for the degradation of dissolved organics in produced water: A review of process performance, degradation kinetics and pathway [J]. Chemical Engineering Journal, 2022,429:132492. [6] Oturan M A, Aaron JJ. Advanced oxidation processes in water/ wastewater treatment: principles and applications. A review [J]. Critical Reviews in Environmental Science and Technology, 2014,44:2577. [7] 寇梦瑶,郑芳菲,胥 雯,等.碱催化过氧化氢体系降解四环素的作用规律与机制解析 [J]. 化工学报, 2024,75:2362.Kou M Y, Zheng F F, Xu W, et al. Degradation of tetracycline by alkali-catalyzed hydrogen peroxide system [J]. Journal of Chemical Engineering, 2024,75:2362. [8] 范新露,任学昌,杨林海,等.Cu/Co共掺杂氮化碳复合材料光-芬顿降解罗丹明B(RhB) [J]. 环境工程学报, 2024,18:777.Fan X L, Ren X C, Yang L H, et al. Photo-Fenton degradation of rhodamine B (RhB) by Cu/Co co-doped carbon nitride composites [J]. Journal of Environmental Engineering, 2024,18:777. [9] Li J, Xu M, Yao G, et al. Enhancement of the degradation of atrazine through CoFe2O4 activated peroxymonosulfate (PMS) process: Kinetic, degradation intermediates, and toxicity evaluation [J]. Chemical Engineering Journal, 2018,348:1012. [10] Wang F X, Zhang Z C, Yi X H, et al. A micron-sized Co-MOF sheet to activate peroxymonosulfate for efficient organic pollutant degradation [J]. Cryst. Eng. Comm., 2022,24:5557. [11] Wang Z, Almatrafi E, Wang H, et al. Cobalt single atoms anchored on oxygen-doped tubular carbon nitride for efficient peroxymonosulfate activation: Simultaneous Coordination structure and morphology modulation [J]. Angewandte Chemie Internation Edition in English, 2022,61:e202202338. [12] Di J, Jamakanga R, Chen Q, et al. Degradation of Rhodamine B by activation of peroxymonosulfate using Co3O4-rice husk ash composites [J]. The Science of the Total Environment, 2021,784:147258. [13] Zhang X, Gu W, Liu D, et al. Fe(II) and Pyridinic N complex sites synergy to activate PMS for specific generation of 1O2 to degrade antibiotics with high efficiency [J]. The Science of the Total Environment, 2023,892:164067. [14] Liu C, Pan D, Tang X, et al. Degradation of Rhodamine B by the α-MnO2/peroxymonosulfate system [J]. Water, Air, & Soil Pollution, 2016,227:92. [15] Lin K Y A, Chen B J, Chen C K. Evaluating Prussian blue analogues MII3[MIII(CN)6] 2 (MII = Co, Cu, Fe, Mn, Ni; MIII = Co, Fe) as activators for peroxymonosulfate in water [J]. RSC Advances, 2016,6:92923. [16] Liu J, Zhao Z, Shao P, et al. Activation of peroxymonosulfate with magnetic Fe3O4-MnO2 core-shell nanocomposites for 4-chlorophenol degradation [J]. Chemical Engineering Journal, 2015,262:854. [17] Shi Q, Deng S, Zheng Y, et al. The application of transition metal-modified biochar in sulfate radical based advanced oxidation processes [J]. Environmental Research, 2022,212:113340. [18] Wang L, Luo D, Yang J, et al. Metal-organic frameworks-derived catalysts for contaminant degradation in persulfate-based advanced oxidation processes [J]. Journal of Cleaner Production, 2022,375:134118. [19] Cattermull J, Pasta M, Goodwin A L. Structural complexity in Prussian blue analogues [J]. Materials Horizons, 2021,8:3178. [20] Peng J, Zhang W, Liu Q, et al. Prussian Blue analogues for sodium-ion batteries: Past, present, and future [J]. Advanced Materials, 2022,34:e2108384. [21] Yi H, Qin R, Ding S, et al. Structure and properties of Prussian Blue analogues in energy storage and conversion applications [J]. Advanced Functional Materials, 2020,31:2006970. [22] Xiao X, Zhang G, Xu Y, et al. A new strategy for the controllable growth of MOF@PBA architectures [J]. Journal of Materials Chemistry A, 2019,7:17266. [23] Qi H, Shi X, Liu Z, et al. In situ etched graphite felt modified with CuFe2O4/Cu2O/Cu catalyst derived from CuFe PBA for the efficient removal of sulfamethoxazole through a heterogeneous electro-Fenton process [J]. Applied Catalysis B: Environmental, 2023,331:122722. [24] Wang S Q, Huo W Y, Feng H C, et al. Controlled self-assembly of hollow core-shell FeMn/CoNi prussian blue analogs with boosted electrocatalytic activity [J]. Small, 2022,18:2203713. [25] Wu F, Wang H, Shi J, et al. Surface modification of silicon nanoparticles by an "ink" layer for advanced lithium ion batteries [J]. ACS Applied Materials & Interfaces, 2018,10:19639. [26] Dong C, Fang W, Yi Q, et al. A comprehensive review on reactive oxygen species (ROS) in advanced oxidation processes (AOPs) [J]. Chemosphere, 2022,308:136205. [27] Gao R, Huang Z, Xu J, et al. Pollutant degradation by Fenton-like system with Prussian blue analogs (PBAs) on cotton and modified oyster shell: Via re-Fenton reaction [J]. Separation and Purification Technology, 2024,334:126339. [28] Yang L Y, Gao Y, Guo Y P, et al. Bimetal-Organic Framework-Derived CoMn@C Catalysts for Fischer-Tropsch Synthesis [J]. Catalysts, 2023,13:633. [29] Peng Y, Tang H, Yao B, et al. Activation of peroxymonosulfate (PMS) by spinel ferrite and their composites in degradation of organic pollutants: A review [J]. Chemical Engineering Journal, 2021,414:128800. [30] Wang Z, Du Y, Liu Y, et al. Degradation of organic pollutants by NiFe2O4/peroxymonosulfate: Efficiency, influential factors and catalytic mechanism [J]. RSC Advances, 2016,6:11040. [31] Wei J, Li F, Zhou L, et al. Strategies for enhancing peroxymonosulfate activation by heterogenous metal-based catalysis: A review [J]. Chinese Journal of Chemical Engineering, 2022,50:12. [32] Zhang M, Gu W. Advanced heterogeneous fenton treatment of coalbed methane-produced water containing fracturing fluid [J]. Processes, 2018,6:40. [33] 陈思良,孙 雯,洪耀良.氮掺杂生物炭负载CuS活化过硫酸盐去除橙黄G [J]. 中国环境科学, 2024,44:2483.Chen S l, Sun W, Hong Y l. Nitrogen-doped biochar supported CuS activated persulfate to remove orange G [J].China Environmental Science, 2024,44:2483. [34] Wang J, Wang S. Effect of inorganic anions on the performance of advanced oxidation processes for degradation of organic contaminants [J]. Chemical Engineering Journal, 2021,411:128392. [35] Zhao Y, An H, Dong G, et al. Oxygen vacancies induced heterogeneous catalysis of peroxymonosulfate by Ni-doped AgFeO2 materials: Evolution of reactive oxygen species and mechanism [J]. Chemical Engineering Journal, 2020,388:124371. [36] Wang L, Xiao K, Zhao H. The debatable role of singlet oxygen in persulfate-based advanced oxidation processes [J]. Water Research, 2023,235:119925. [37] Wang D, He Y, Chen Y, et al. Electron transfer enhancing the Mn(II)/Mn(III) cycle in MnO/CN towards catalytic ozonation of atrazine via a synergistic effect between MnO and CN [J]. Water Research, 2023,230:119574. [38] Zhang L S, Jiang X H, Zhong Z A, et al. Carbon nitride supported high-loading Fe single-atom catalyst for activation of peroxymonosulfate to generate 1O2 with 100% selectivity [J]. Angewandte Chemie Internation Edition in English, 2021,60:21751. [39] Fang L, Liu K, Li F, et al. New insights into stoichiometric efficiency and synergistic mechanism of persulfate activation by zero-valent bimetal (Iron/Copper) for organic pollutant degradation [J]. Journal of Hazardous Materials, 2021,403:123669. [40] Kang J, Zhang H, Duan X, et al. Magnetic Ni-Co alloy encapsulated N-doped carbon nanotubes for catalytic membrane degradation of emerging contaminants [J]. Chemical Engineering Journal, 2019,362:251. [41] Wang F, Liu X, Guo C, et al. A novel cobalt-iron bimetallic hydrochar for the degradation of triclosan in the aqueous solution: Performance, reusability, and synergistic degradation mechanism [J]. Environmental Pollution, 2024,358:124487. [42] Wu L, Zhang Z, Wang H, et al. Enhanced degradation of methyl orange with CoFe2O4@Zeolite catalyst as peroxymonosulfate activator: Performance and mechanism [J]. Journal of Inorganic Materials, 2023,38:469.
