Preparation of nitrogen-doped petroleum coke based activated carbon and its performance in catalytic oxidation of hydrogen sulfide at room temperature
ZHENG Hao-ming1, ZHU Wen-fu1, LUO Ying-hong1, WANG Zi-kun1, LIU Mei-yin1, HUANG Hao-min1,2, YE Dai-qi1,2, LI Hong-xiang3, WU Jun-liang1,2
1. School of Environment and Energy, South China University of Technology, Guangzhou 510006, China; 2. National Engineering Laboratory for VOCs Pollution Control Technology and Equipment, Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control, Guangzhou 510006, China; 3. Shanxi Xinhua Chemical CO., LTD., Taiyuan 030008, China
Abstract:A novel nitrogen-doped porous carbon was successfully prepared using petroleum coke as the carbon source and the solid waste from melamine production as the nitrogen source. The catalyst exhibited excellent H2S catalytic oxidation capacity in room temperature with a breakthrough sulfur capacity of 398.4mg/g. Three process parameters, namely, the amount of activator, nitrogen doping temperature and nitrogen source, changed the specific surface, N configuration and N content of the catalysts, respectively, during the preparation process. By optimizing the process conditions, the highest reactive center, pyridine N, could be achieved at 2.88at.%. Compared with the catalyst prepared using traditional raw material, it achieves waste utilization and green preparation. The results of this paper provide a new approach for the preparation of porous carbon materials with low cost and high breakthrough sulfur capacity.
郑皓鸣, 朱文富, 罗颖鸿, 王子琨, 刘美茵, 黄皓旻, 叶代启, 李洪祥, 吴军良. 掺氮石油焦基活性炭常温催化氧化硫化氢研究[J]. 中国环境科学, 2023, 43(9): 4550-4560.
ZHENG Hao-ming, ZHU Wen-fu, LUO Ying-hong, WANG Zi-kun, LIU Mei-yin, HUANG Hao-min, YE Dai-qi, LI Hong-xiang, WU Jun-liang. Preparation of nitrogen-doped petroleum coke based activated carbon and its performance in catalytic oxidation of hydrogen sulfide at room temperature. CHINA ENVIRONMENTAL SCIENCECE, 2023, 43(9): 4550-4560.
Yan R, Chin T, Ng Y L, et al. Influence of surface properties on the mechanism of H2S removal by alkaline activated carbons[J]. Environmental Science & Technology, 2004,38(1):316-323.
[2]
Yang C, Wang Y, Fan H, et al. Bifunctional ZnO-MgO/activated carbon adsorbents boost H2S room temperature adsorption and catalytic oxidation[J]. Applied Catalysis B:Environmental, 2020,266.
[3]
庄荣玉,王磊刚,李美燕,等.异养菌与新型填料成膜性及BTF处理屠宰H2S废气[J]. 中国环境科学, 2020,40(3):1106-1115. Zhuang Y Y, Wang L G, Li M Y, et al. Biofilm formation of a heterotrophic bacterium on the novel packing material and the removal of hydrogen sulfide produced in a slaughtering process by biotrickling filter[J]. China Environmental Science, 2020,40:1106-1115.
[4]
Beauchamp R O, Bus J S, Popp J A, et al. A critical review of the literature on hydrogen sulfide toxicity[J]. Critical Reviews In Toxicology, 1984,13(1):25-97.
[5]
王亘,翟增秀,耿静,等.40种典型恶臭物质嗅阈值测定[J]. 安全与环境学报, 2015,15(6):348-351. Wang G, Zhai Z H, Geng J, et al. Testing and determination of the olfactory thresholds of the 40kinds of typical malodorous substances[J]. Journal of Safety and Environment, 2015,15:348-351.
[6]
Masi A d, Ascenzi P. H2S:a "double face" molecule in health and disease[J]. Biofactors, 2013,39(2):186-196.
[7]
Garcia-Arriaga V, Alvarez-Ramirez J, Amaya M, et al. H2S and O2 influence on the corrosion of carbon steel immersed in a solution containing 3M diethanolamine[J]. Corrosion Science, 2010,52(7):2268-2279.
[8]
Xu Z Y, Zhao W B, Xie X H, et al. Liquid-liquid phase-change absorption of hydrogen sulfide by superbase 1,8-diazabicyclo[5.4.0] undec-7-ene and its chemical regeneration[J]. Separation and Purification Technology, 2020,250:117244.
[9]
Gu J, Shao P, Luo L, et al. Microporous triazine-based ionic hyper-crosslinked polymers for efficient and selective separation of H2S/CH4/N2[J]. Separation and Purification Technology, 2022,285:120377.
[10]
Hao J, Rice P A, Stem S A. Upgrading low-quality natural gas with H2S and CO2selective polymer membranes Part I. Process design and economics of membrane stages without recycle streams[J]. Journal of Membrane Science, 2002,209(1):177-206.
[11]
Dobslaw D, Ortlinghaus O. Biological waste air and waste gas treatment:Overview, challenges, operational efficiency, and current trends[J]. Sustainability, 2020,12(20):8577.
[12]
Yang C, Yang S, Fan H L, et al. A sustainable design of ZnO-based adsorbent for robust H2S uptake and secondary utilization as hydrogenation catalyst[J]. Chemical Engineering Journal, 2020,382.
[13]
Zheng X H, Li Y L, Zheng Y, et al. Highly efficient porous FexCe1-xO2-delta with three-dimensional hierarchical nanoflower morphology for H2S-selective oxidation[J]. ACS Catalysis, 2020, 10(7):3968-3983.
[14]
Khabazipour M, Anbia M. Removal of hydrogen sulfide from gas streams using porous materials:A review[J]. Industrial & Engineering Chemistry Research, 2019,58(49):22133-22164.
[15]
Adib F, Bagreev A, Bandosz T J. Effect of surface characteristics of wood-based activated carbons on adsorption of hydrogen sulfide[J]. Journal of Colloid and Interface Science, 1999,214(2):407-415.
[16]
Adib F, Bagreev A, Bandosz T J. Adsorption/oxidation of hydrogen sulfide on nitrogen-containing activated carbons[J]. Langmuir, 1999, 16(4):1980-1986.
[17]
Adib F, Bagreev A, Bandosz T J. Analysis of the relationship between H2S removal capacity and surface properties of unimpregnated activated carbons[J]. Environmental Science & Technology, 2000, 34(4):686-692.
[18]
Zhang Z X, Wang J T, Li W C, et al. Millimeter-sized mesoporous carbon spheres for highly efficient catalytic oxidation of hydrogen sulfide at room temperature[J]. Carbon, 2016,96:608-615.
[19]
Yang C, Yang S, Fan H, et al. Tuning the ZnO-activated carbon interaction through nitrogen modification for enhancing the H(2)S removal capacity[J]. Journal of Colloid and Interface Science, 2019, 555:548-557.
[20]
Yu Z F, Wang X Z, Song X D, et al. Molten salt synthesis of nitrogen-doped porous carbons for hydrogen sulfide adsorptive removal[J]. Carbon, 2015,95:852-860.
[21]
Sun F G, Liu J, Chen H C, et al. Nitrogen-rich mesoporous carbons:highly efficient, regenerable metal-free catalysts for low-temperature oxidation of H2S[J]. ACS Catalysis, 2013,3(5):862-870.
[22]
Wang X T, Ouyang T, Wang L, et al. Surface reorganization on electrochemically-induced Zn-Ni-Co spinel oxides for enhanced oxygen electrocatalysis[J]. Angewandte Chemie International Edition, 2020,59(16):6492-6499.
[23]
Ren J T, Wan C Y, Pei T Y, et al. Promotion of electrocatalytic nitrogen reduction reaction on N-doped porous carbon with secondary heteroatoms[J]. Applied Catalysis B:Environmental, 2020,266.
[24]
Dlamini M W, Phaahlamohlaka T N, Kumi D O, et al. Post doped nitrogen-decorated hollow carbon spheres as a support for Co Fischer-Tropsch catalysts[J]. Catalysis Today, 2020,342:99-110.
[25]
王莹,魏成耀,黄天寅,等.氮掺杂碳纳米管活化过一硫酸盐降解酸性橙AO7[J]. 中国环境科学, 2017,37(7):2583-2590. Wang Y, Wei C Y, Huang T Y, et al. Activation of peroxymonosulfate by nitrogen-doped carbon nanotubes to decolorize acid orange 7[J]. China Environmental Science, 2017,37:2583-2590.
[26]
陈爱侠,关娟娟,卫潇,等.同步活化氮掺杂海藻酸钠基多孔碳制备及对双酚A的高效吸附[J]. 中国环境科学, 2002,42(1):160-171. Chen A X, Guan J J, Wei X, et al. Efficient adsorption of BPA by alginate-based porous carbon with the preparation of synchronous activation and nitrogen doping[J]. China Environmental Science, 2002,42:160-171.
[27]
Wu J, Chen W, Chen L, et al. Super-high N-doping promoted formation of sulfur radicals for continuous catalytic oxidation of H2S over biomass derived activated carbon[J]. Journal of Hazardous Materials, 2022,424(Pt D):127648.
[28]
Chen W H, Zhang G C, Li D, et al. Preparation of nitrogen-doped porous carbon from waste polyurethane Foam by hydrothermal carbonization for H2S adsorption[J]. Industrial & Engineering Chemistry Research, 2020,59(16):7447-7456.
[29]
Xiao Y, Pudasainee D, Gupta R, et al. Bromination of petroleum coke for elemental mercury capture[J]. Journal of Hazardous Materials, 2017,336:232-239.
[30]
Wu J, Montes V, Virla L D, et al. Impacts of amount of chemical agent and addition of steam for activation of petroleum coke with KOH or NaOH[J]. Fuel Processing Technology, 2018,181:53-60.
[31]
钟悦之,宋晓晖,王彦超,等.中国平板玻璃行业大气污染物排放特征研究[J]. 中国环境科学, 2018,38(12):4451-4459. Zhong Y Z, Song X H, Wang Y C, et al. Emission characteristics from flat-glass industry in China[J]. China Environmental Science, 2018, 38(12):4451-4459.
[32]
Yang M L, Guo L P, Hu G S, et al. Adsorption of CO2 by petroleum coke nitrogen-doped porous carbons synthesized by combining ammoxidation with KOH activation[J]. Industrial & Engineering Chemistry Research, 2016,55(3):757-765.
[33]
Yang J, Yue L M, Lin B B, et al. CO2 adsorption of nitrogen-doped carbons prepared from nitric acid preoxidized petroleum Coke[J]. Energy & Fuels, 2017,31(10):11060-11068.
[34]
Zhu W, Wang Y, Yao F, et al. One-pot synthesis of N-doped petroleum coke-based microporous carbon for high-performance CO2 adsorption and supercapacitors[J]. Journal of Environmental Sciences, 2024, 139:93-104.
[35]
Chen L, Yuan J, Li T, et al. A regenerable N-rich hierarchical porous carbon synthesized from waste biomass for H2S removal at room temperature[J]. Science of the Total Environment, 2021,768:144452.
[36]
Kazmierczak-Razna J, Gralak-Podemska B, Nowicki P, et al. The use of microwave radiation for obtaining activated carbons from sawdust and their potential application in removal of NO2 and H2S[J]. Chemical Engineering Journal, 2015,269:352-358.
[37]
Chen L, Jiang X, Chen W, et al. H2O2-assisted self-template synthesis of N-doped biochar with interconnected mesopore for efficient H2S removal[J]. Separation and Purification Technology, 2022.
[38]
Surra E, Costa Nogueira M, Bernardo M, et al. New adsorbents from maize cob wastes and anaerobic digestate for H2S removal from biogas[J]. Waste Management, 2019,94:136-145.
[39]
Sun M, Wang X, Li Y, et al. Integration of desulfurization and lithium-sulfur batteries enabled by amino-functionalized porous carbon nanofibers[J]. Energy & Environmental Materials, 2023,6(2):e12349.
[40]
Klein J, Henning K-D. Catalytic oxidation of hydrogen sulphide on activated carbons[J]. Fuel, 1984,63(8):1064-1067.
[41]
Le Leuch L M, Subrenat A, Le Cloirec P. Hydrogen sulfide adsorption and oxidation onto activated carbon cloths:Applications to odorous gaseous emission treatments[J]. Langmuir, 2003,19(26):10869-10877.
[42]
Huang Y, Wang J, Ma S, et al. A confined MoN2@N-rich carbon catalyst derived from β-cyclodextrin encapsulating phosphomolybdic acid for oxidative removal of H2S[J]. Chemical Engineering Journal, 2023,457.
[43]
Bandosz T J. On the adsorption/oxidation of hydrogen sulfide on activated carbons at ambient temperatures[J]. Journal of Colloid and Interface Science, 2002,246(1):1-20.
[44]
Lillo-Rodenas M A, Cazorla-Amoros D, Linares-Solano A. Understanding chemical reactions between carbons and NaOH and KOH:An insight into the chemical activation mechanism[J]. Carbon, 2003,41(2):267-275.
[45]
Lin G, Ma R, Zhou Y, et al. KOH activation of biomass-derived nitrogen-doped carbons for supercapacitor and electrocatalytic oxygen reduction[J]. Electrochimica Acta, 2018,261:49-57.
[46]
Zhu X, Zhang L, Zhang M, et al. Effect of N-doping on NO2 adsorption and reduction over activated carbon:An experimental and computational study[J]. Fuel, 2019,258:116109.
[47]
Li S Y, Liu Y F, Gong H M, et al. N-doped 3D mesoporous carbon/carbon nanotubes monolithic catalyst for H2S selective oxidation[J]. ACS Applied Nano Materials, 2019,2(6):3780-3792.
[48]
Chen Q J, Wang Z, Long D H, et al. Role of pore structure of activated carbon fibers in the catalytic oxidation of H2S[J]. Industrial & Engineering Chemistry Research, 2010,49(7):3152-3159.
[49]
Wang S, Wang Y, Zhang S L, et al. Supporting ultrathin ZnIn2S4 nanosheets on Co/N-doped graphitic carbon Nanocages for efficient photocatalytic H2 generation[J]. Advanced Materials, 2019,31(41):e1903404.
[50]
Wu Y, Cao J P, Zhuang Q Q, et al. Biomass-derived three-dimensional hierarchical porous carbon network for symmetric supercapacitors with ultra-high energy density in ionic liquid electrolyte[J]. Electrochimica Acta, 2021,371.
[51]
Ning H, Guo D L, Wang X S, et al. Efficient CO2 electroreduction over N-doped hieratically porous carbon derived from petroleum pitch[J]. Journal of Energy Chemistry, 2021,56:113-120.
[52]
孙鹏,柳佳鹏,王维大,等.活性炭强化热活化过硫酸盐降解对硝基苯酚[J]. 中国环境科学, 2020,40(11):4779-4785. Sun P, Liu J P, Wang W D, et al. Active carbon enhanced thermal activation of persulfate for degradation of p-nitrophenol[J]. China Environmental Science, 2020,40:4779-4785.
[53]
Zhang W L, Sun H X, Zhu Z Q, et al. N-doped hard carbon nanotubes derived from conjugated microporous polymer for electrocatalytic oxygen reduction reaction[J]. Renewable Energy, 2020,146:2270-2280.
[54]
Li D, Chen W H, Wu J P, et al. The preparation of waste biomass-derived N-doped carbons and their application in acid gas removal:focus on N functional groups[J]. Journal of Materials Chemistry A, 2020,8(47):24977-24995.
[55]
Xiong W, Wang Z N, He S L, et al. Nitrogen-doped carbon nanotubes as a highly active metal-free catalyst for nitrobenzene hydrogenation[J]. Applied Catalysis B:Environmental, 2020,260.
[56]
Leng L, Xu S, Liu R, et al. Nitrogen containing functional groups of biochar:An overview[J]. Bioresource Technology, 2020,298:122286.
[57]
Yu W, Lian F, Cui G, et al. N-doping effectively enhances the adsorption capacity of biochar for heavy metal ions from aqueous solution[J]. Chemosphere, 2018,193:8-16.
[58]
Zhang J, Xia Z, Dai L. Carbon-based electrocatalysts for advanced energy conversion and storage[J]. Science Advances, 2015,1(7):e1500564.
[59]
Guo D, Shibuya R, Akiba C, et al. Active sites of nitrogen-doped carbon materials for oxygen reduction reaction clarified using model catalysts[J]. Science, 2016,351(6271):361-365.
[60]
Li J, Yin S, Dong F, et al. Tailoring active sites via synergy between graphitic and pyridinic N for enhanced catalytic efficiency of a Carbocatalyst[J]. ACS Applied Materials & Interfaces, 2017,9(23):19861-19869.
[61]
Adib F, Bagreev A, Bandosz T J. On the possibility of water regeneration of unimpregnated activated carbons used as hydrogen sulfide adsorbents[J]. Industrial & Engineering Chemistry Research, 2000,39(7):2439-2446.
[62]
Bagreev A, Bandosz T J. H2S adsorption/oxidation on unmodified activated carbons:importance of prehumidification[J]. Carbon, 2001,39(15):2303-2311.
[63]
Tuerhong T, Kuerban Z. Preparation and characterization of cattle manure-based activated carbon for hydrogen sulfide removal at room temperature[J]. Journal of Environmental Chemical Engineering, 2022,10(2):107177.