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Abstract
N-doped activated carbon (AC) was employed in a three-dimensional electrode system (3DES) to enhance the removal of sulfur-containing volatile organic compounds (S-VOC). The technical parameters for preparing N-doped AC were optimized based on CS2 removal and COS accumulation, where the mass ratio of AC to urea was 1:1.0, and the activation temperature and heat-treatment time were 400 °C and 120 min, respectively. When the mixing S-VOC were purified under an operating voltage of 8 V and peroxydisulfate concentration of 0.15 mol/L, CS2 removal in the 3DES system with N-doped AC reached 100% within 75 min, and was above 83% as purification time extended to 200 min. Additionally, the COS content in the outlet gas was usually undetectable within 120 min, and was lower than that in the other electrochemical systems. Modification of raw AC through urea impregnation and subsequent heat treatment significantly improved its surface structure and pore size distribution. Moreover, polar functional groups, such as C=O and pyridinic-N, increased noticeably, enhancing the S-VOC adsorption capacity and dielectric properties. Consequently, highly reactive substances were more efficiently activated in 3DES system with N-doped AC, and oxidizing species HO• and 1O2 had important contributions to S-VOC purification compared to SO4–• radicals. A pathway was proposed to elucidate the transformation of sulfur-containing components, such as CH3SH and CS2. This study provides an efficient approach for S-VOC purification.
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Keywords
N-doped activated carbon
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Sulfur-containing VOC
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Three-dimensional electrode system
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Electrochemical oxidation
Highlight
| ● The urea-modified AC enhanced S-VOCs purification in 3DES system. |
| ● Particle electrode enhanced adsorption capacity and dielectric properties. |
| ● PDS was efficiently activated by carbon-based material and electrochemistry. |
| ● Radical and non-radical oxidation had significant contributions for S-VOC purification. |
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Rui Luo, Shugen Liu, Senlin Tian, Chen Li, Ping Ning.
N-doped activated carbon promoting sulfur-containing VOC removal in three-dimension electrode system.
Front. Environ. Sci. Eng., 2025, 19(5): 71 DOI:10.1007/s11783-025-1991-x
| [1] |
Chen J Y, Chen A G, Qiu P L, Huang L W, Zhou Q H. (2019). Removal of carbon disulfide from air stream by absorption combined with electrochemical oxidation. Journal of Environmental Chemical Engineering, 7(3): 103167
|
| [2] |
Chen W S, Jhou Y C, Huang C P. (2014). Mineralization of dinitrotoluenes in industrial wastewater by electro-activated persulfate oxidation. Chemical Engineering Journal, 252: 166–172
|
| [3] |
Cui Y H, Lv X D, Lei J X, Liu Z Q. (2017). Synergistic effect of cathode/peroxymonosulfate/Fe3+ on phenol degradation. Electrochimica Acta, 245: 201–210
|
| [4] |
Ding L, Liang H C, Li X Z. (2012). Oxidation of CH3SH by in situ generation of ferrate (VI) in aqueous alkaline solution for odour treatment. Separation and Purification Technology, 91: 117–124
|
| [5] |
Erlind M, Marco S, Saveria S, Salvatore P, Nicoletta D, Paola B, Mariangela L. (2023). Enhanced ORR activity of S- and N-modified non-noble metal-doped carbons with bamboo-like C nanotubes grafted onto their surface. Electrochimica Acta, 464: 142946
|
| [6] |
Feng Y, Lee P H, Wu D, Shih K. (2017). Surface-bound sulfate radical-dominated degradation of 1,4-dioxane by alumina-supported palladium (Pd/Al2O3) catalyzed peroxymonosulfate. Water Research, 120: 12–21
|
| [7] |
Ghosh S, Barg S, Jeong S M, Ostrikov K K. (2020). Heteroatom-doped and oxygen-functionalized nanocarbons for high-performance supercapacitors. Advanced Energy Materials, 10(32): 2001239
|
| [8] |
He D D, Hao H, Chen D K, Liu J P, Yu J, Lu J C, Liu F, Wan G, He S F, Luo Y M. (2017). Synthesis and application of rare-earth elements (Gd, Sm, and Nd) doped ceria-based solid solutions for methyl mercaptan catalytic decomposition. Catalysis Today, 281: 559–565
|
| [9] |
He E Y, Huang G, Fan H L, Yang C, Wang H, Tian Z, Wang L J, Zhao Y R. (2019). Macroporous alumina- and titania-based catalyst for carbonyl sulfide hydrolysis at ambient temperature. Fuel, 246: 277–284
|
| [10] |
Hong J, Jo C. (2024). Study on morphology and N-doping effects of carbon cathodes for zinc-ion hybrid supercapacitors. Journal of Power Sources, 594: 234006
|
| [11] |
HuangZ F, Bao H W, YaoY Y, LuW Y, ChenW X (2014). Novel green activation processes and mechanism of peroxymonosulfate based on supported cobalt phthalocyanine catalyst. Applied Catalysis B: Environmental, 154–154: 36–43
|
| [12] |
Jin H K, An Z Y, Li Q C, Duan Y Q, Zhou Z H, Sun Z K, Duan L. (2021). Catalysts of ordered mesoporous alumina with a large pore size for low-temperature hydrolysis of carbonyl sulfide. Energy & Fuels, 35(10): 8895–8908
|
| [13] |
Jing H L, Yang H T, Yu X H, Hu C Q, Li R X, Li H T. (2022). Treatment of organic matter and ammonia nitrogen in wastewater by electrocatalytic oxidation: a review of anode material preparation. Environmental Science. Water Research & Technology, 8(2): 226–248
|
| [14] |
Li J, Yan J F, Yao G, Zhang Y H, Li X, Lai B. (2019). Improving the degradation of atrazine in the three-dimensional (3D) electrochemical process using CuFe2O4 as both particle electrode and catalyst for persulfate activation. Chemical Engineering Journal, 361: 1317–1332
|
| [15] |
Li X Y, Wu Y, Zhu W, Xue F Q, Qian Y, Wang C W. (2016). Enhanced electrochemical oxidation of synthetic dyeing wastewater using SnO2-Sb-doped TiO2-coated granular activated carbon electrodes with high hydroxyl radical yields. Electrochimica Acta, 220: 276–284
|
| [16] |
Li X, Sun F, Qu Z, Zhu X, Gao J H, Zhao G B, Zhang L Q. (2023). Insight into synergistic effects of oxygen and nitrogen dual-dopants in carbon catalysts on selective catalytic reduction of NOx with NH3: a combined computational and experimental verification. Chemical Engineering Journal, 454: 140098
|
| [17] |
Liang C, Huang C, Mohanty N, Kurakalva R M. (2008). A rapid spectrophotometric determination of persulfate anion in ISCO. Chemosphere, 73(9): 1540–1543
|
| [18] |
Liu Z, Ding H J, Zhao C, Wang T, Wang P, Dionysiou D D. (2019). Electrochemical activation of peroxymonosulfate with ACF cathode: kinetics, influencing factors, mechanism, and application potential. Water Research, 159: 111–121
|
| [19] |
Luo R, Liu S G, Li C, Huang X F, Ning P, Tian S L. (2024). Synergistic removal of sulphur-containing malodourous gases via peroxydisulfate activation in three-dimensional electrode system. Journal of Environmental Chemical Engineering, 12(2): 112169
|
| [20] |
Lyu Y C, Liu X M, Liu W Q, Tian Y P, Qin Z. (2020). Adsorption/oxidation of ethyl mercaptan on Fe-N-modified active carbon catalyst. Chemical Engineering Journal, 393: 124680
|
| [21] |
Ma Y H, Wang D, Xu Y, Lin H, Zhang H. (2022). Nonradical electron transfer-based peroxydisulfate activation by a Mn-Fe bimetallic oxide derived from spent alkaline battery for the oxidation of bisphenol A. Journal of Hazardous Materials, 436: 129172
|
| [22] |
Qu J, Wang X Q, Wang L L, Xu B, Ning P, Ma Y X, Xie Y B, Cao R, Ma Q. (2022). The investigation of the role of nitrogen in the improvement of catalytic activity and stability of Zr/Ti-based material for carbon disulfide hydrolysis. Separation and Purification Technology, 296: 121357
|
| [23] |
Song H R, Yan L X, Ma J, Jiang J, Cai G Q, Zhang W J, Zhang Z X, Zhang J, Yang T. (2017). Nonradical oxidation from electrochemical activation of peroxydisulfate at Ti/Pt anode: efficiency mechanism and influencing factors. Water Research, 116: 182–193
|
| [24] |
Sun H W, He F, Choi W Y. (2020). Production of reactive oxygen species by the reaction of periodate and hydroxylamine for rapid removal of organic pollutants and waterborne bacteria. Environmental Science & Technology, 54(10): 6427–6437
|
| [25] |
Tian R, Lu J C, Xu Z Z, Zhang W J, Liu J P, Wang L L, Xie Y B, Zhao Y T, Cao X H, Luo Y M. (2023). Unraveling the synergistic reaction and the deactivation mechanism for the catalytic degradation of double components of sulfur-containing VOCs over ZSM-5-based materials. Environmental Science & Technology, 57(3): 1443–1455
|
| [26] |
Wang B S, Zhao P Y, Zhang X N, Zhang Y, Liu Y M. (2024). Three-dimensional electro-Fenton system with iron-carbon packing as a particle electrode for nitrobenzene wastewater treatment. Frontiers of Environmental Science & Engineering, 18(11): 138
|
| [27] |
Wang J, Duan X, Gao J, Shen Y, Feng X H, Yu Z J, Tan X Y, Liu S M, Wang S B. (2020). Roles of structure defect oxygen groups and heteroatom doping on carbon in nonradical oxidation of water contaminants. Water Research, 185: 116244
|
| [28] |
Wang Z Q, Huang J C, Wang B, Hu W, Xie D, Liu S, Qiao Y. (2022). Co-hydrothermal carbonization of sewage sludge and model compounds of food waste: influence of mutual interaction on nitrogen transformation. Science of the Total Environment, 807(3): 150997
|
| [29] |
Xiao Q L, Cai S Y, Liu J Z. (2021). Microbial and thermogenic hydrogen sulfide in the Qianjiang depression of Qianghan basin: insights from sulfur isotope and volatile organic sulfur compounds measurements. Applied Geochemistry, 126: 104865
|
| [30] |
Yang J L, Huang Y J, Chen Y W, Xia D H, Mou C Y, Hu L L, Zeng J W, He C, Wong P K, Zhu H Y. (2020). Active site-directed tandem catalysis on CuO/VO-MnO2 for efficient and stable catalytic ozonation of S-VOCs under mild condition. Nano Today, 35: 100944
|
| [31] |
Yang S Y, Li L, Xiao T, Zheng D, Zhang Y T. (2016). Role of surface chemistry in modified ACF (activated carbon fiber)-catalyzed peroxymonosulfate oxidation. Applied Surface Science, 383: 142–150
|
| [32] |
Yao X L, Wan K, Yu W X, Liu Z. (2024). Enhancing comprehension of water vapor on adsorption performance of VOC on porous carbon materials and its application challenge. Frontiers of Environmental Science & Engineering, 18(9): 110
|
| [33] |
Zhang C, Jiang Y H, Li Y, Hu Z, Zhou L, Zhou M. (2013). Three-dimensional electrochemical process for wastewater treatment: a general review. Chemical Engineering Journal, 228: 455–467
|
| [34] |
Zhao S Z, Yi H H, Tang X L, Kang D J, Gao F Y, Wang J G, Huang Y H, Yang Z. (2018). Removal of volatile odorous organic compounds over NiAl mixed oxides at low temperature. Journal of Hazardous Materials, 344: 797–810
|
| [35] |
Zheng W T, Liu Y B, Liu W, Ji H D, Li F, Shen C S, Fang X F, Li X, Duan X G. (2021). A novel electrocatalytic filtration system with carbon nanotube supported nanoscale zerovalent copper toward ultrafast oxidation of organic pollutants. Water Research, 194: 116961
|
| [36] |
Zhu S S, Huang X C, Ma F, Wang L, Duan X G, Wang S B. (2018). Catalytic removal of aqueous contaminants on N-doped graphitic biochars: inherent roles of adsorption and nonradical mechanisms. Environmental Science & Technology, 52(15): 8649–8658
|
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