The effect of the NH3 activation temperature of graphene/carbon composite nanofibers on their NO catalytic oxidation performance at room temperature
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摘要: 以聚丙烯腈（PAN）为碳前驱体，氧化石墨烯（GO）为添加物，通过静电纺丝技术制备了石墨烯/炭纳米复合纤维原丝，分别在900、1 000、1 100和1 200℃下氨气中炭化10 min，并在NH3中活化处理20 min得到多孔、N掺杂的石墨烯/炭纳米复合纤维。分别将4种样品用于室温下低浓度NO（50 ppm）的吸附和催化氧化研究。结果表明，复合纳米纤维对NO的催化氧化性能随着处理温度的升高而增强，在样品PGCNF1200达到最大转化率（49.7%），而对NO和NO2的吸附能力则强烈的依赖于纤维比表面积的大小。此外，经NH3活化处理后可以在纤维表面引入含氮官能团，可以和作为催化活性位点的GO共同对室温下NO的催化氧化起到促进作用。Abstract: N-doped graphene/carbon composite porous nanofibers were prepared by electrospinning, followed by carbonization in nitrogen and activation in NH3 at 900, 1 000, 1 100 and 1 200℃ for 20 min, using polyacrylonitrile as a carbon precursor and graphene oxide as an additive. Their NO (50 ppm) adsorption and catalytic oxidation performances at room temperature were tested. Results showed that the catalytic oxidation activity increased with the activation temperature and a maximum conversion of 49.7% was achieved for the sample activated at 1 200℃. The adsorption capacity for NO and NO2 depended on their specific surface areas. The nitrogen-containing functional groups introduced by NH3 and the active sites formed in graphene sheets jointly increased NO conversion at room temperature.
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Key words:
- Graphene oxide /
- Electrospinning /
- NH3 treatment /
- Nitric oxide /
- Catalytic oxidation
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Tang Q, Zhang Z G, Zhu W P, et al. SO2 and NO selective adsorption properties of coal-based activated carbons[J]. Fuel, 2005, 84(4): 461-465. Guo Z C, Xie Y S, Hong I Y, et al. Catalytic oxidation of NO to NO2 on activated carbon[J]. Energy Conversion and Management, 2001, 42(15-17): 2005-2018. Wang M X, Huang Z H, Shimohara T, et al. NO removal by electrospun porous carbon nanofibers at room temperature[J]. Chemical Engineering Journal, 2011, 170(2-3): 505-511. Mochida I, Korai Y, Shirahama M, et al. Removal of SOx and NOx over activated carbon fibers[J]. Carbon, 2000, 38(2): 227-239. Brandenberger S, Kroecher O, Tissler A, et al. The state of the art in selective catalytic reduction of NOx by ammonia using metal-exchanged zeolite catalysts[J]. Catal Rev-Sci Eng, 2008, 50(4): 492-531. Tang X, Hao J, Xu W, et al. Low temperature selective catalytic reduction of NOx with NH3 over amorphous MnOx catalysts prepared by three methods[J]. Catalysis Communications, 2007, 8(3): 329-334. Wang M X, Guo Z, Huang Z H, et al. NH3-activated carbon nanofibers for low-concentration NO removal at room temperature[J]. Catalysis Communications, 2015, 62: 83-88. Ramakrishna S, Fujihara K, Teo W-E, et al. Electrospun nanofibers: solving global issues[J]. Materials Today, 2006, 9(3): 40-50. 张振兴, 杜鸿达, 李佳, 等. 静电纺丝制备定向排列聚酰亚胺基炭纳米纤维[J]. 新型炭材料, 2015, 30(4): 289-294. (ZHANG Zhen-xing, DU Hong-da, LI Jia, et al. Preparation of aligned polyimide-based carbon nanofibers by electrospinning. New Carbon Materials, 2015, 30(4): 289-294.) Hammel E, Tang X, Trampert M, et al. Carbon nanofibers for composite applications[J]. Carbon, 2004, 42(5-6): 1153-1158. Ji L W, Zhang X W. Electrospun carbon nanofibers containing silicon particles as an energy-storage medium[J]. Carbon, 2009, 47(14): 3219-3226. Merino C, Soto P, Vilaplana-Ortego E, et al. Carbon nanofibres and activated carbon nanofibres as electrodes in supercapacitors[J]. Carbon, 2005, 43(3): 551-557. Tan Z L, Xiao H N, Zhang R D, et al. Potential to use mesoporous carbon as catalyst support for hydrodesulfurization[J]. New Carbon Materials, 2009, 24(4): 333-342. Dadvar S, Tavanai H, Morshed M, et al. The removal of 2-chloroethyl ethyl sulfide using activated carbon nanofibers embedded with MgO and Al2O3 nanoparticles[J]. Journal of Chemical and Engineering Data, 2012, 57(5): 1456-1462. Aykut Y. Enhanced field electron emission from electrospun Co-loaded activated porous carbon nanofibers[J]. ACS applied materials & interfaces, 2012, 4(7): 3405-3415. Wan X K, Zou X Q, Shi H X, et al. Nitrogen doping of activated carbon loading Fe2O3 and activity in carbon-nitric oxide reaction[J]. Journal of Zhejiang University-Science A, 2007, 8(5): 707-711. Yang C M, Kaneko K. Adsorption properties of nitrogen-alloyed activated carbon fiber[J]. Carbon, 2001, 39(7): 1075-1082. Sousa J P S, Pereira M F R, Figueiredo J L. Catalytic oxidation of NO to NO2 on N-doped activated carbons[J]. Catalysis Today, 2011, 176(1): 383-387. Li D, Kaner R B. Materials science. Graphene-based materials[J]. Science, 2008, 320(5880): 1170-1171. Novoselov K S, Fal'ko V I, Colombo L, et al. A roadmap for graphene[J]. Nature, 2012, 490(7419): 192-200. Stankovich S, Dikin D A, Dommett G H, et al. Graphene-based composite materials[J]. Nature, 2006, 442(7100): 282-286. Marcano D C, Kosynkin D V, Berlin J M, et al. Improved synthesis of graphene oxide[J]. Acs Nano, 2010, 4(8): 4806-4814. Guo Z, Wang M, Huang Z-H, et al. Preparation of graphene/carbon hybrid nanofibers and their performance for NO oxidation[J]. Carbon, 2015, 87: 282-291. Wang Y, Serrano S, Santiago-Avilés JJ. Raman characterization of carbon nanofibers prepared using electrospinning[J]. Synthetic Metals, 2003, 138(3): 423-427. Wang M X, Huang Z H, Shen K, et al. Catalytically oxidation of NO into NO2 at room temperature by graphitized porous nanofibers[J]. Catalysis Today, 2013, 201: 109-114. -
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