Preparation of foam SiC-based titanium suboxide electrode and the performance of electrocatalytic oxidation acid orange G
YU Zhangjun1, WANG Xiang1, DENG Zejun1, MA Li2, WEI Qiuping1,2
1. School of Materials Science and Engineering, Central South University, Changsha 410083, China; 2. State Key Laboratory of Powder Metallurgy, Central South University, Changsha 410083, China
Abstract:Three dimensional foam SiC based titanium suboxide (SiC/TinO2n-1) electrode was prepared by sol-gel sintering method. The surface morphology, phase composition, and electrochemical property of titanium suboxide electrodes were characterized by scanning electron microscopy, X-ray diffraction, and electrochemical workstation. The degradation effect of organic pollutants was tested using a ultraviolet-visible spectrophotometer. The results show that the coating of foam SiC based titanium suboxide electrode prepared at 1 050 ℃/2 h sintering condition has good quality, continuous and uniform distribution, and the content of conductive phase Ti4O7 is the highest (mass fraction is 37.5%), the film charge transfer resistance is the lowest (16.75 Ω). It shows a faster degradation rate (reaction rate constant is 0.60 h-1) and lower energy consumption (11.63 (kW∙h)/m3) for simulated pollutant acid orange G. Both •OH and $ \mathrm{SO}_{4}^{.-}$ are involved in the degradation of acid orange G, and their contributions to the removal of acid orange G are almost the same. The presence of inorganic ions $ \mathrm{HCO}_{3}^{-}$, $ \mathrm{NO}_{3}^{-}$, $ \mathrm{H}_{2} \mathrm{PO}_{4}^{-}$ has an inhibitory effect on the degradation of acid orange G, while Cl- promotes the degradation. The electrode exhibits high stability in multiple degradations.
余章俊, 王项, 邓泽军, 马莉, 魏秋平. 泡沫SiC基亚氧化钛电极的制备及电催化氧化酸性橙G的性能[J]. 粉末冶金材料科学与工程, 2024, 29(3): 221-230.
YU Zhangjun, WANG Xiang, DENG Zejun, MA Li, WEI Qiuping. Preparation of foam SiC-based titanium suboxide electrode and the performance of electrocatalytic oxidation acid orange G. Materials Science and Engineering of Powder Metallurgy, 2024, 29(3): 221-230.
[1] MOREIRA F C, BOAVENTURA R A R, BRILLAS E, et al. Electrochemical advanced oxidation processes: a review on their application to synthetic and real wastewaters[J]. Applied Catalysis B-Environmental, 2017, 202(3): 217-261. [2] DARGAHI A, SHOKOOHI R, ASGARI G, et al.Moving-bed biofilm reactor combined with three-dimensional electrochemical pretreatment (MBBR-3DE) for 2,4-D herbicide treatment: application for real wastewater, improvement of biodegradability[J]. RSC Advances, 2021, 11(16): 9608-9620. [3] ZHANG Y Y, ZHANG C P, SHAO D, et al.Magnetically assembled electrodes based on Pt, RuO2-IrO2-TiO2 and Sb-SnO2 for electrochemical oxidation of wastewater featured by fluctuant Cl- concentration[J]. Journal of Hazardous Materials, 2022, 421(1): 126803. [4] CHAPLIN B P.Critical review of electrochemical advanced oxidation processes for water treatment applications[J]. Environmental Science-Processes & Impacts, 2014, 16(6): 1182-1203. [5] YU L H, XUE J Q, ZHANG L H, et al.Fabrication of a stable Ti/Pb-TiOxNWs/PbO2 anode and its application in benzoquinone degradation[J]. Electrochimica Acta, 2021, 368(4): 137532. [6] RODGERS J D, JEDRAL W, BUNCE N I.Electrochemical oxidation of chlorinated phenols[J]. Environmental Science & Technology, 1999, 33(9): 1453-1457. [7] KAUR R, KUSHWAHA J P, SINGH N.Electro-oxidation of amoxicillin trihydrate in continuous reactor by Ti/RuO2 anode[J]. Science of the Total Environment, 2019, 677(32): 84-97. [8] 黄小清, 甘卫平, 杨杰, 等. 掺钴氧化钌(RuO2/Co3O4)·nH2O复合薄膜电极的制备与表征[J]. 粉末冶金材料科学与工程, 2013, 18(1): 107-112. HUANG Xiaoqing, GAN Weiping, YANG Jie, et al.Preparation and characteristic of co-doped (RuO2/Co3O4)·nH2O composite film slsctrode[J]. Materials Science and Engineering of Powder Metallurgy, 2013, 18(1): 107-112. [9] YU H, ZHANG Z, ZHANG L, et al.Improved norfloxacin degradation by urea precipitation Ti/SnO2-Sb anode under photo-electro catalysis and kinetics investigation by BPneural-network-physical modeling[J]. Journal of Cleaner Production, 2021, 280(3): 124412. [10] YU S, HAO C T, LI Z L, et al.Promoting the electrocatalytic performance of PbO2 nanocrystals via incorporation of Y2O3 nanoparticles: degradation application and electrocatalytic mechanism[J]. Electrochimica Acta, 2021, 369(5): 137671. [11] LIN M H, BULMAN D M, REMUCAL C K, et al.Chlorinated byproduct formation during the electrochemical advanced oxidation process at magneli phase Ti4O7 electrodes[J]. Environmental Science & Technology, 2020, 54(19): 12673-12683. [12] 窦金杰, 刘典宏, 蒋鸾, 等. Ti基镶嵌金刚石颗粒掺硼金刚石电极及其性能[J]. 粉末冶金材料科学与工程, 2024, 29(1): 45-52. DOU Jinjie, LIU Dianhong, JIANG Luan, et al.Ti plate embedding diamond particles boron-doped diamond electrode and its properties[J]. Materials Science and Engineering of Powder Metallurgy, 2024, 29(1): 45-52. [13] GAYEN P, CHEN C, ABIADE J T, et al.Electrochemical oxidation of atrazine and clothianidin on Bi-doped SnO2-TinO2n-1 electrocatalytic reactive electrochemical membranes[J]. Environmental Science & Technology, 2018, 52(21): 12675-12684. [14] ZHI D, ZHANG J, WANG J B, et al.Electrochemical treatments of coking wastewater and coal gasification wastewater with Ti/Ti4O7 and Ti/RuO2-IrO2 anodes[J]. Journal of Environmental Management, 2020, 265(13): 110571. [15] GANIYU S O, OTURAN N, RAFFY S, et al.Sub-stoichiometric titanium oxide (Ti4O7) as a suitable ceramic anode for electrooxidation of organic pollutants: a case study of kinetics, mineralization and toxicity assessment of amoxicillin[J]. Water Research, 2016, 106(19): 171-182. [16] GUO L, JING Y, CHAPLIN B P.Development and characterization of ultrafiltration TiO2 magneli phase reactive electrochemical membranes[J]. Environmental Science & Technology, 2016, 50(3): 1428-1436. [17] SANTOS M C, ELABD Y A, JING Y, et al.Highly porous Ti4O7 reactive electrochemical water filtration membranes fabricated via electrospinning/electrospraying[J]. Aiche Journal, 2016, 62(2): 508-524. [18] CHAPLIN B P.The prospect of electrochemical technologies advancing worldwide water treatment[J]. Accounts of Chemical Research, 2019, 52(3): 596-604. [19] KOKALJ A J, NOVAK S, TALABER I, et al.The first comprehensive safety study of Magneli phase titanium suboxides reveals no acute environmental hazard[J]. Environmental Science-Nano, 2019, 6(4): 1131-1139. [20] LIANG S, PIERCE R D, LIN H, et al.Electrochemical oxidation of PFOA and PFOS in concentrated waste streams[J]. Remediation Journal, 2018, 28(2): 127-134. [21] 陈峰磊, 杨万林, 朱俊奎, 等. 低压快速氢化引入氧空位增强TiO2光催化降解性能[J]. 粉末冶金材料科学与工程, 2023, 28(6): 545-553. CHEN Fenglei, YANG Wanlin, ZHU Junkui, et al.Low pressure rapid hydrogenation induced oxygen vacancy to enhance the photocatalytic degradation performance of TiO2[J]. Materials Science and Engineering of Powder Metallurgy, 2023, 28(6): 545-553. [22] GARCIA-SEGURA S, NIENHAUSER A B, FAJARDO A S, et al.Disparities between experimental and environmental conditions: research steps toward making electrochemical water treatment a reality[J]. Current Opinion in Electrochemistry, 2020, 22(4): 9-16. [23] 周志超, 段学臣, 朱奕漪, 等. 溶胶凝胶法制备掺杂纳米TiO2粉末及其光催化性能[J]. 粉末冶金材料科学与工程, 2013, 18(3): 434-440. ZHOU Zhichao, DUAN Xuechen, ZHU Yiyi, et al.Doped nano titania powder prepared by sol-gel technique and its photocatalytic activity[J]. Materials Science and Engineering of Powder Metallurgy, 2013, 18(3): 434-440. [24] 陈儒, 方国赵, 谭小平, 等. 多孔V2O5微球的制备与电化学性能[J]. 粉末冶金材料科学与工程, 2019, 24(1): 80-88. CHEN Ru, FANG Guozhao, TAN Xiaoping, et al.Synthesis and electrochemical performance of porous V2O5 microspheres[J]. Materials Science and Engineering of Powder Metallurgy, 2019, 24(1): 80-88. [25] WEI K X, ARMUTLULU A, WANG Y X, et al.Visible-light-driven removal of atrazine by durable hollow core-shell TiO2@LaFeO3 heterojunction coupling with peroxymonosulfate via enhanced electron-transfer[J]. Applied Catalysis B-Environmental, 2022, 303(4): 120889. [26] XU B Q, SOHN H Y, MOHASSAB Y, et al.Structures, preparation and applications of titanium suboxides[J]. RSC Advances, 2016, 6: 79706-79722. [27] WANG H J, LI Z Y, ZHANG F Y, et al.Comparison of Ti/Ti4O7, Ti/Ti4O7-PbO2-Ce, and Ti/Ti4O7 nanotube array anodes for electro-oxidation of p-nitrophenol and real wastewater[J]. Separation and Purification Technology, 2021, 266(13): 118600. [28] COMNINELLIS C, PULGARIN C.Anodic oxidation of phenol for waste water treatment[J]. Journal of Applied Electrochemistry, 1991, 21(8): 703-708. [29] CHEN Z, ZHANG Y M, ZHOU L C, et al.Performance of nitrogen-doped graphene aerogel particle electrodes for electro-catalytic oxidation of simulated bisphenol a wastewaters[J]. Journal of Hazardous Materials, 2017, 332(12): 70-78. [30] CHEN G.Electrochemical technologies in wastewater treatment[J]. Separation and Purification Technology, 2004, 38(1): 11-41. [31] DING J F, SHEN L L, YAN R P, et al.Heterogeneously activation of H2O2 and persulfate with goethite for bisphenol a degradation: a mechanistic study[J]. Chemosphere, 2020, 261(24): 127715. [32] WANG L, LU J H, LI L, et al.Effects of chloride on electrochemical degradation of perfluorooctanesulfonate by Magneli phase Ti4O7 and boron doped diamond anodes[J]. Water Research, 2020, 170(3): 115254. [33] CHOI J, CUI M, LEE Y, et al.Hydrodynamic cavitation and activated persulfate oxidation for degradation of bisphenol A: kinetics and mechanism[J]. Chemical Engineering Journal, 2018, 338(8): 323-332. [34] ZHU F, ZHOU S Y, SUN M Y, et al.Heterogeneous activation of persulfate by Mg doped Ni(OH)2 for efficient degradation of phenol[J]. Chemosphere, 2022, 286(1): 131647. [35] CAI J J, ZHOU M H, DU X D, et al.Enhanced mechanism of 2,4-dichlorophenoxyacetic acid degradation by electrochemical activation of persulfate on blue-TiO2 nanotubes anode[J]. Separation and Purification Technology, 2021, 254(1): 117560. [36] FENG W, LIN H, ARMUTLULU A, et al.Anodic activation of persulfate by V-mediated Ti4O7: improved stability and ROS generation[J]. Separation and Purification Technology, 2022, 299(20): 121794.