介质阻挡放电技术再生Pd/AC催化剂的机理探讨

doi:10.3969/j.issn.0438-1157.2013.01.033

化工学报 ›› 2013, Vol. 64 ›› Issue (1): 297-302.DOI: 10.3969/j.issn.0438-1157.2013.01.033

• 催化、动力学与反应器 • 上一篇下一篇

介质阻挡放电技术再生Pd/AC催化剂的机理探讨

高文立¹, 王骁¹, 李中坚¹, 张兴旺¹, 余青霓^1,2, 雷乐成¹

1. 生物质化工教育部重点实验室(浙江大学),浙江杭州 310027;
2. 中国航天员科研训练中心,北京 100094

收稿日期:2012-04-17 修回日期:2012-05-28 出版日期:2013-01-05 发布日期:2013-01-05
通讯作者: 雷乐成
作者简介:高文立(1986—),男,硕士研究生。

Regeneration mechanism of Pd/AC catalyst in dielectric barrier discharge plasma

GAO Wenli¹, WANG Xiao¹, LI Zhongjian¹, ZHANG Xingwang¹, YU Qingni^1,2, LEI Lecheng¹

1. Key Laboratory of Biomass Chemical Engineering(Zhejiang University), Ministry of Education, Hangzhou 310027, Zhejiang, China;
2. China Astronaut Research and Training Center, Beijing 100094, China

Received:2012-04-17 Revised:2012-05-28 Online:2013-01-05 Published:2013-01-05

摘要/Abstract

摘要： 利用介质阻挡放电对失活钯炭催化剂(Pd/AC)进行再生,并通过催化臭氧氧化硝基苯反应评价再生后催化剂的活性。运用扫描电镜(SEM)、比表面积测定(BET)、热重分析(TG)等测定手段对Pd/AC进行表征;并对放电过程进行臭氧产量测定和等离子体发射光谱诊断,分析了Pd/AC催化剂再生的机理。结果表明,催化剂经放电处理30 min后再生率为95%;利用在最优条件下再生的Pd/AC进行催化臭氧氧化反应,硝基苯的降解率为87%;再生过程中臭氧贡献率仅为25.6%,表明放电过程中产生的强氧化性自由基是促使催化剂再生的主要因素。

关键词: Pd/AC催化剂, 介质阻挡放电, 催化剂再生, 自由基

Abstract: Regeneration of deactivated Pd/AC catalyst was carried out in a dielectric barrier discharge (DBD) plasma reactor and activities of regenerated catalysts were assessed by catalytic ozonation reactions.The surface morphology,surface area and organic compounds were characterized by SEM,BET and TG respectively.In order to investigate regeneration mechanism of Pd/AC catalyst,concentration of O₃ and plasma emission spectra during DBD process were detected.The results showed that regeneration efficiency could be by 95% after 30 min treatment.Nitrobenzene degradation efficiency was 87% using ozonation reaction catalyzed by Pd/AC catalyst regenerated under the optimized condition.The regeneration efficiency with ozone solely was only 25.6%,indicating that radicals with strong oxidation ability produced in DBD process was main factor for Pd/AC catalyst regeneration.

Key words: Pd/AC catalyst, dielectric barrier discharge, catalyst regeneration, free radicals

中图分类号:

TQ426.81

高文立, 王骁, 李中坚, 张兴旺, 余青霓, 雷乐成. 介质阻挡放电技术再生Pd/AC催化剂的机理探讨[J]. 化工学报, 2013, 64(1): 297-302.

GAO Wenli, WANG Xiao, LI Zhongjian, ZHANG Xingwang, YU Qingni, LEI Lecheng. Regeneration mechanism of Pd/AC catalyst in dielectric barrier discharge plasma[J]. CIESC Journal, 2013, 64(1): 297-302.

参考文献 17

[1]	Ormerod R Mark,Baddeley Christopher J,Hardacre Christopher,Lambert Richard M.Chemisorption and reactivity of furan on Pd{111}[J].Surface Science,1996,360(1/2/3):1-9
[2]	Hoeben W F L M,van Veldhuizen E M,Rutgers W R,Kroesen G M W.Gas phase corona discharges for oxidation of phenol in an aqueous solution[J].Phys.D:Appl. Phys.,1999,32(24):133-137
[3]	Sunka P,Babicky V,Clupek M,Lukes P,Simek M,Schmidt J,Cernak M.Generation of chemically active species by electrical discharges in water[J].Plasma Sources Sci.Technol.,1999,8(2):258-268
[4]	Wang C H,Li G F,Wu Y,Wang Y,Li J,Li D,Wang N H.Role of bipolar pulsed DBD on the growth of microcystis aeruginosa in three-phase discharge plasma reactor[J].Plasma Chemistry and Plasma Processing,2007,27(1):65-83
[5]	Sun Q,Zhu A M,Yang X F,Niu J H,Xu Y,Song Z M,Liu J.Selective catalytic reduction of NOx in dielectric barrier discharge plasmas[J].European Physical Journal-Applied Physics,2005, 30(2):129-133
[6]	Lu B,Zhang X,Yu X,Feng T,Yao S.Catalytic oxidation of benzene using DBD corona discharges[J].Journal of Hazardous Materials,2006,137(1):633-637
[7]	Park J Y,Tomicic I,Round G F,Chang J S.Simultaneous removal of NOx and SO2 from NO-SO2-CO2-N2-O2 gas mixtures by corona radical shower systems[J].J. Phys. D:Appl.Phys.,1999,32(9):1006-1011
[8]	Huang Liwei,Nakajyo Katsuhiko,Hari Takaaki,Ozawa Shoji,Matsuda Hitoki.Decomposition of carbon tetrachloride by a pulsed corona reactor incorporated with in situ absorption[J].Ind.Eng.Chem.Res.,2001,40(23):5481-5486
[9]	Goossens O,Dekempeneer E,Vangeneugden D,Leest R Van de,Leys C.Application of atmospheric pressure dielectric barrier discharges in deposition,cleaning and activation[J].Surface and Coatings Technology,2001,142-144:474-481
[10]	Baravian G,Chaleix D,Choquet P,Nauche P L,Puech V,Rozoy M.Oil removal from iron surfaces by atmospheric-pressure barrier discharges[J].Surface and Coatings Technology,1999,115(1):66-69
[11]	Thiebaut J M,Belmonte T,Chaleix D,Choquet P,Baravian G,Puech V,Michel H.Comparison of surface cleaning by two atmospheric pressure discharges[J].Surface and Coatings Technology,2003,169-170:186-189
[12]	Lei Lecheng,Gu Li,Zhang Xingwang,Su Yaling. Catalytic oxidation of highly concentrated real industrial wastewater by integrated ozone and activated carbon[J].Applied Catalysis A:General,2007,327(2):287-294
[13]	Figueiredo J L,Pereira M F R,Freitas M M A,Orfao J J M.Modification of the surface chemistry of activated carbons[J].Carbon,1999,37(9):1379-1389
[14]	Rodriguez-reinoso Francisco.The role of carbon materials in heterogeneous catalysis[J].Carbon,1998,36(3):159-175
[15]	Samaranayake W J M,Miyahara Y,Namihira T,Katsuki S,Sakugawa T,Hackam R,Akiyama H.Pulsed streamer discharge characteristics of ozone production in dry air[J].IEEE Trans.Dilectr.Electr.Insul.,2000,7(2):254-260
[16]	Malik Muhammad Arif,Ghaffar Abdul,Malik Salman Akbar.Water purification by electrical discharges[J].Plasma Sources Sci.Techonl.,2001,10(1):82-91
[17]	Sugiarto Anto Tri,Ito Shunsuke,Ohshima Takayuki,Sato Massayuki,Skalny Jan D.Oxidative decoloration of dyes by pulsed pulsed plasma in water[J].Journal of Electrostatics,2003,58(1/2):135-145

介质阻挡放电技术再生Pd/AC催化剂的机理探讨

Regeneration mechanism of Pd/AC catalyst in dielectric barrier discharge plasma

PDF (PC)

可视化

被引次数

摘要/Abstract

引用本文

使用本文

参考文献 17

相关文章 15

编辑推荐

Metrics

本文评价

[1]	李锦潼, 邱顺, 孙文寿. 煤浆法烟气脱硫中草酸和紫外线强化煤砷浸出过程[J]. 化工学报, 2023, 74(8): 3522-3532.
[2]	何晓崐, 刘锐, 薛园, 左然. MOCVD生长AlN单晶薄膜的气相和表面化学反应综述[J]. 化工学报, 2023, 74(7): 2800-2813.
[3]	张兰河, 赖青燚, 王铁铮, 关潇卓, 张明爽, 程欣, 徐小惠, 贾艳萍. H₂O₂对SBR脱氮效率和污泥性能的影响[J]. 化工学报, 2023, 74(5): 2186-2196.
[4]	李瑞康, 何盈盈, 卢维鹏, 王园园, 丁皓东, 骆勇名. 电化学强化钴基阴极活化过一硫酸盐的研究[J]. 化工学报, 2023, 74(5): 2207-2216.
[5]	杨庆云, 李青松, 陈泽铭, 邓靖, 李玉瑛, 杨帆, 陈国元, 李国新. UV/PMS、UV/PDS、UV/SPC工艺降解尼泊金甲酯[J]. 化工学报, 2023, 74(3): 1322-1331.
[6]	李雨萧, 王青月, Ho Lim Khak, 李晓辉, Erlita Mastan, 彭博, 王文俊. 自由基聚合反应动力学常数测定技术[J]. 化工学报, 2023, 74(2): 559-570.
[7]	章承浩, 罗京, 张吉松. 微反应器内基于氮氧自由基催化剂连续氧气/空气氧化反应的研究进展[J]. 化工学报, 2023, 74(2): 511-524.
[8]	邓靖, 杨庆云, 陈民杰, 李青松, 杨帆, 陈国元, 李国新. UV-LED/NaClO工艺降解尼泊金甲酯：不同活性物种的作用[J]. 化工学报, 2022, 73(9): 4113-4121.
[9]	靳文章, 张玉玲, 贾晓宇. 电化学高级氧化对HEDP的降解效能研究[J]. 化工学报, 2022, 73(9): 4062-4069.
[10]	刘坤, 尹远, 耿文强, 夏昊天. 不同操作参数下介质阻挡放电的固氮性能研究及机理分析[J]. 化工学报, 2022, 73(9): 4045-4053.
[11]	郑默, 李晓霞. ReaxFF MD模拟揭示的煤热解挥发分自由基反应的竞争与协调[J]. 化工学报, 2022, 73(6): 2732-2741.
[12]	肖习羽, 李青松, 吴俊文, 李国新, 陈国元. VUV/UV/NaClO工艺降解百里香酚协同效应及活性物质贡献[J]. 化工学报, 2022, 73(5): 2233-2241.
[13]	张红锐, 张田, 隆曦孜, 李先宁. 光催化与微生物燃料电池耦合对Cu-EDTA的降解特性[J]. 化工学报, 2022, 73(5): 2149-2157.
[14]	余彬彬, 蒋新生, 禹进, 蔡运雄, 李玉玺, 何东海, 于佳佳. 全氟己酮抑制航空煤油燃烧实验及化学动力学研究[J]. 化工学报, 2022, 73(4): 1834-1844.
[15]	闫帅, 杨家宝, 龚岩, 郭庆华, 于广锁. CO₂稀释对甲烷反扩散火焰结构的影响研究[J]. 化工学报, 2022, 73(3): 1335-1342.