惰性气体对氢氧等离子体直接合成过氧化氢的影响

doi:10.3969/j.issn.0438-1157.2012.11.019

化工学报 ›› 2012, Vol. 63 ›› Issue (11): 3513-3518.DOI: 10.3969/j.issn.0438-1157.2012.11.019

• 催化、动力学与反应器 • 上一篇下一篇

惰性气体对氢氧等离子体直接合成过氧化氢的影响

高天龙¹, 易颜辉¹, 张家良², 赵越¹, 王丽¹, 郭洪臣¹

1. 大连理工大学化工学院催化化学与工程系及精细化工国家重点实验室, 辽宁大连 116023;
2. 大连理工大学物理与光电工程学院, 辽宁大连 116023

收稿日期:2012-03-10 修回日期:2012-05-02 出版日期:2012-11-05 发布日期:2012-11-05
通讯作者: 郭洪臣
作者简介:高天龙(1986-),男,硕士研究生。

Influence of inert gases on direct synthesis of hydrogen peroxide via hydrogen-oxygen plasma

GAO Tianlong¹, YI Yanhui¹, ZHANG Jialiang², ZHAO Yue¹, WANG Li¹, GUO Hongchen¹

1. Department of Catalytic Chemistry and Engineering & National Key Laboratory of Fine Chemicals, Dalian University of Technology, Dalian 116023, Liaoning, China;
2. Department of Physics and Optoelectronic Engineering, Dalian University of Technology, Dalian 116023, Liaoning, China

Received:2012-03-10 Revised:2012-05-02 Online:2012-11-05 Published:2012-11-05

摘要/Abstract

摘要： 在H₂/O₂体系中添加惰性气体(Ar、He、N₂)进行常压介质阻挡放电,合成了H₂O₂水溶液。系统研究了不同惰性气体对体系击穿电压及H₂O₂合成能效的影响。结果表明,添加气体对击穿电压、O₂转化率、H₂O₂选择性、H₂O₂收率及能量效率能产生较大影响。其中Ar的引入不仅降低了击穿电压,还提高了合成H₂O₂的能量效率;当Ar添加量为56.6 ml·min^-1时,击穿电压由11.8 kV降为10.2 kV;合成H₂O₂的能量效率提高51%,由3.45 g·(kW·h)^-1提高至5.20 g·(kW·h)^-1(以100%H₂O₂计)。发射光谱表征发现,在H₂-O₂-Ar放电体系中存在以亚稳态为末态的辐射Ar(696.5、794.8、811.5 nm),表明亚稳态Ar物种的潘宁电离作用可能是降低击穿电压的主要因素。由示波器测量的放电电流波形图可知,Ar的加入增大了体系电子密度,使得相同功率下O₂转化速率大幅提高,从而使合成H₂O₂能量效率显著提高。

关键词: 惰性气体, 过氧化氢, 等离子体, 氢气, 氧气

Abstract: In double dielectric barrier discharge aqueous electrodes reactor(DDBD),hydrogen peroxide was prepared in a mixture of hydrogen and oxygen by using DBD discharge with inert gas(Ar,He and N₂)as additive gas.The influence of different inert gases on the breakdown voltage and energy efficiency of H₂O₂ synthesis was studied.The results showed that breakdown voltage,conversion of O₂,selectivity of H₂O₂,yield of H₂O₂ and energy efficiency were obviously affected by different inert gases.The breakdown voltage could be reduced with He and Ar as additive gas,however,it became higher when N₂ was the additive gas.On the other hand,energy efficiency of H₂O₂ synthesis was reduced dramatically with N₂ as the additive gas,and little changed with He as the additive gas.However,energy efficiency of H₂O₂ synthesis increased markedly with Ar as the additive gas.When Ar flow rate was 56.6 ml穖in^-1,breakdown voltage could be reduced from 11.8 kV to 10.2 kV;energy efficiency of H₂O₂ synthesis increased by about 51%,from 3.45 g?(kW穐)^-1 to 5.20 g?(kW穐)^-1(100% H₂O₂).Therefore,the addition of Ar could not only reduce breakdown voltage,but also increase energy efficiency of H₂O₂ synthesis.The optical emission spectra revealed that Penning ionization effects of metastable state Ar species(696.5,794.8,811.5 nm)existing in H₂-O₂-Ar discharge system might be responsible for the decrease of breakdown voltage.From the waveform of discharge current,the addition of Ar increased electron density,which obviously facilitated the increase of O₂ conversion and energy efficiency of H₂O₂ synthesis at the same power.

Key words: inert gas, hydrogen peroxide, plasma, hydrogen, oxygen

中图分类号:

TQ123.6

高天龙, 易颜辉, 张家良, 赵越, 王丽, 郭洪臣. 惰性气体对氢氧等离子体直接合成过氧化氢的影响[J]. 化工学报, 2012, 63(11): 3513-3518.

GAO Tianlong, YI Yanhui, ZHANG Jialiang, ZHAO Yue, WANG Li, GUO Hongchen. Influence of inert gases on direct synthesis of hydrogen peroxide via hydrogen-oxygen plasma[J]. CIESC Journal, 2012, 63(11): 3513-3518.

参考文献 22

[1]	Sato K,Aoki M,Noyori R.A "green" route to adipic acid:direct oxidation of cyclohexenes with 30 percent hydrogen peroxide[J].Science,1998,281:1646
[2]	Campos-Martin J M,Blanco-Brieva G,Fierro J L. Hydrogen peroxide synthesis:an outlook beyond the anthraquinone process[J].Angew. Chem. Int. Ed.,2006,45:2-25
[3]	Vasant R Choudhary,Prabhas Jana.Direct oxidation of H2 to H2O2 over PdO/Al2O3 catalysts in aqueous acidic medium:influence on H2O2 formation of Pd loading,calcination temperature and reduction of catalyst and presence of halide anions[J].Catal. Comm.,2008,9:2371-2375
[4]	Liu Qingsheng,Gath Kerrie K,Bauer J Chris,Schaak Raymond E,Lunsford Jack H.The active phase in the direct synthesis of H2O2 from H2 and O2 over Pd/SiO2 catalyst in a H2SO4/ethanol system[J].Catal. Lett.,2009, 132:342-348
[5]	Ma Shuqi,Li Gang,Wang Xiangsheng.Direct synthesis of hydrogen peroxide from H2/O2 and oxidation of thiophene over supported gold catalysts[J].Chem. Eng. J.,2010,156:532-539
[6]	Piccinini Marco,Ntainjua N Edwin,Edwards Jennifer K,Carley Albert F,Moulijn Jacob A,Hutchings Graham J.Effect of the reaction conditions on the performance of Au-Pd/TiO2 catalyst for the direct synthesis of hydrogen peroxide[J].Phys. Chem. Chem. Phys.,2010,12:2488-2492
[7]	Li Ping,He Chongheng,Campestrini Sandro,Corain Benedetto,Yuana Weikang,Han Yifan.Synthesis of hydrogen peroxide from H2 and O2 in water and ethanol catalyzed by nanoclustered Pd0 on silica:strong selectivity enhancement exerted by the addition of ionic liquids[J].Phys. Chem. Chem. Phys.,2010,12:2170-2176
[8]	Pritchard James C,He Qian,Ntainjua Edwin N,Piccinini Marco,Edwards Jennifer K,Herzing Andrew A,Carley Albert F,Moulijn Jacob A,Kiely Christopher J,Hutchings Graham J.The effect of catalyst preparation method on the performance of supported Au-Pd catalysts for the direct synthesis of hydrogen peroxide[J].Green Chem.,2010,12:915-921
[9]	Kogelschatz Ulrich.Dielectric-barrier discharges:their history,discharge physics,and industrial applications[J].Plasma Chem. Plasma P.,2003,23(1):1-46
[10]	Yan Binhang(颜彬航),Wang Qi(王琦),Jin Yong(金涌),Cheng Yi(程易).Carbon dioxide and methane reforming using DC arc plasma reactor[J].CIESC Journal(化工学报),2010,61(11):2919-2923
[11]	Chen Kui(陈亏),Gao Jing(高晶),Yu Jianyong(俞建勇),Huan Weihai(还伟海),Ma Yizi(马一梓).Surface modification of low temperature plasma-pretreated ePTFE film by AAc graft copolymerization[J].CIESC Journal(化工学报),2011,62(4):1170-1176
[12]	Zhou Juncheng(周军成),Gou Jianxia(苟建霞),Chen Lixing(陈黎行),Guo Hongchen(郭洪臣),Wang Xiangsheng(王祥生).Direct synthesis of hydrogen peroxide via hydrogen oxygen plasma[J].Journal of Chemical Industry and Engineering(China)(化工学报),2006,57(4):821-823
[13]	Zhou Juncheng,Guo Hongchen,Wang Xiangsheng,Guo Mingxing,Zhao Jiangli,Chen Lixing,Gong Weimin. Direct and continuous synthesis of concentrated hydrogen peroxide by the gaseous reaction of H2/O2 non-equilibrium plasma[J].Chem. Comm.,2005,12:1631-1633
[14]	Wang Xinxin(王新新),Li Chengrong(李成榕).Review of homogenous dielectric barrier discharge in nitrogen at atmospheric pressure[J].High Voltage Engineering(高电压技术),2011,37(6):1405-1415
[15]	Kolokolov N B,Kudrjavtsev A A.Interaction processes with creation of fast electrons in the low temperature plasma[J].Phys. Scr.,1994,50(4):371-402
[16]	Jones M T,Dreiling T D,Setser D W,Mcdonald R N.Branching fractions for Penning ionization in quenching of He(23S),Ar(3P2,0),and Ne(3P2,0)atoms[J].J. Phys. Chem.,1985,89(21):4501-4517
[17]	Yang L,Wang X L,Hao Y P.Investigations of Penning ionization of dielectric barrier discharges in helium at atmospheric pressure by optical emission spectrometry//2008 International Conference on High Voltage Engineering and Application[C].Chongqing,China,2008:725-727
[18]	Dony M F,Ricard A,Dauchot J P,Hecq M,Wautelet M.Optical diagnostics of d.c.and r.f.argon magnetron discharges[J].Surf. Coat. Technol.,1995,74/75:479-484
[19]	Gicquel A,Chenevier M,Hassouni K,Tserepi A,Dubus M. Validation of actinometry for estimating relative hydrogen atom densities and electron energy evolution in plasma assisted diamond deposition reactor[J].J. Appl. Phys.,1998,83(12):7504-7521
[20]	Ahn J W,Craig D,Fiksel G,Den Hartog D J,Anderson J K,O’Mullance M G.Emission intensities and line ratios from a fast neutral helium beam[J].Phys. Plasmas.,2007,14:083301
[21]	Dong Lifang(董丽芳),Mao Zhiguo(毛志国),Zhang Lianshui(张连水),Ran Junxia(冉俊霞).Spectrum of dielectric barrier discharge at atmospheric pressure intensified by mixing a little argon[J].Spectroscopy and Spectral Analysis(光谱学与光谱分析),2005,25(10):1542-1544
[22]	Pinhao N R,Janeco A,Branco J B.Influence of helium on the conversion of methane and carbon dioxide in a dielectric barrier discharge[J].Plasma Chem. Plasma Process.,2011,31:427-439

惰性气体对氢氧等离子体直接合成过氧化氢的影响

Influence of inert gases on direct synthesis of hydrogen peroxide via hydrogen-oxygen 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 22

相关文章 15

编辑推荐

Metrics

本文评价

[1]	李木金, 胡松, 施德磐, 赵鹏, 高瑞, 李进龙. 环氧丁烷尾气溶剂吸收及精制工艺[J]. 化工学报, 2023, 74(4): 1607-1618.
[2]	高靖博, 孙强, 李青, 王逸伟, 郭绪强. 考虑水合物结构转变的含氢气体水合物相平衡模型[J]. 化工学报, 2023, 74(2): 666-673.
[3]	杜峰, 尹思琦, 罗辉, 邓文安, 李传, 黄振薇, 王文静. H₂在Mo _x S _y 团簇上吸附解离的尺寸效应研究[J]. 化工学报, 2022, 73(9): 3895-3903.
[4]	陈晨, 杨倩, 陈云, 张睿, 刘冬. 不同氧浓度下煤挥发分燃烧的化学动力学研究[J]. 化工学报, 2022, 73(9): 4133-4146.
[5]	许贤伦, 钱旸, 张兴旺, 雷乐成. 高压脉冲介质阻挡放电降解土壤中芘的研究[J]. 化工学报, 2022, 73(9): 4025-4033.
[6]	张淑君, 王诗慧, 张欣, 吉旭, 戴一阳, 党亚固, 周利. 集成轻烃回收单元代理模型的氢气网络多目标优化[J]. 化工学报, 2022, 73(4): 1658-1672.
[7]	张欣, 周利, 王诗慧, 吉旭, 毕可鑫. 考虑原油性质波动的炼厂氢气网络集成优化[J]. 化工学报, 2022, 73(4): 1631-1646.
[8]	王小西, 李笑艳, 王保伟. 介质阻挡放电微等离子体分解二氧化碳研究[J]. 化工学报, 2022, 73(3): 1343-1350.
[9]	霍猛, 彭晓婉, 赵金, 马秋伟, 邓春, 刘蓓, 陈光进. 基于COSMO-RS的离子液体吸收CO的溶剂筛选及H₂/CO分离实验[J]. 化工学报, 2022, 73(12): 5305-5313.
[10]	杨霄, 丁锐, 李墨含, 宋正昶. 氧浓度对微通道内甲烷均相/非均相耦合反应特性的影响[J]. 化工学报, 2022, 73(12): 5427-5437.
[11]	刘立, 蒋鹏, 王伟, 张同桓, 穆立文, 陆小华, 朱家华. 基于过程模拟和随机森林模型的生物质制氢过程因素分析与预测[J]. 化工学报, 2022, 73(11): 5230-5239.
[12]	吴一, 温小萍, 张素梅, 郭志东, 邓浩鑫, 纪文涛. 垂直圆管内掺氢甲烷燃烧不稳定性研究[J]. 化工学报, 2022, 73(10): 4780-4790.
[13]	雷明川, 喻健良, 闫兴清, 吕先舒, 侯玉洁, 詹潇兵. 惰性气体对氢气/空气爆轰传播的抑制作用[J]. 化工学报, 2022, 73(10): 4754-4761.
[14]	石秀娟, 梁文俊, 尹国彬, 王金柱. 低温等离子体协同Mn基催化剂降解氯苯研究[J]. 化工学报, 2022, 73(10): 4472-4483.
[15]	韦双明, 余明高, 裴蓓, 李世梁, 康亚祥, 徐梦娇, 郭佳琪. 三元混合气体燃料爆炸特性实验研究[J]. 化工学报, 2022, 73(1): 451-460.