非平衡等离子体放电模式及反应器结构对氨气分解制氢的影响

引用本文: 赵越, 王丽, 张家良, 郭洪臣. 非平衡等离子体放电模式及反应器结构对氨气分解制氢的影响[J]. 物理化学学报, 2014, 30(4): 738-744. doi: 10.3866/PKU.WHXB201402141 shu

Citation: ZHAO Yue, WANG Li, ZHANG Jia-Liang, GUO Hong-Chen. Influence of Non-Thermal Plasma Discharge Mode and Reactor Structure on Ammonia Decomposition to Hydrogen[J]. Acta Physico-Chimica Sinica, 2014, 30(4): 738-744. doi: 10.3866/PKU.WHXB201402141 shu

非平衡等离子体放电模式及反应器结构对氨气分解制氢的影响

赵越 ^1, ,
王丽 ^1, ,
张家良 ^2, ,
郭洪臣 ^1,

基金项目:
国家自然科学基金（20473016，20673018）资助项目

摘要:

在常压下研究了不同等离子体放电模式及反应器结构对氨分解制氢反应的影响. 实验中调节反应器结构分别产生了介质阻挡放电和交流弧放电两种放电模式. 通过对两种放电模式的放电图像、电压-电流波形和氨分解过程中等离子体区活性物种的发射光谱（OES）研究发现，与介质阻挡放电相比，交流弧放电为局部强放电，具有更高的电源效率和电子密度. 因此，在介质阻挡放电中氨气分子大部分通过生成电子激发态物种NH₃^*，再与载能电子碰撞断裂N―H键进行氨分解反应；而在交流弧放电中载能电子具有更高的平均电子能量，可直接断裂氨气分子的N―H键生成NH₂和NH等高活性物种，促进氨分解反应的进行. 结果表明，交流弧放电的氨分解效果要明显优于介质阻挡放电. 在交流弧放电模式下不同类型反应器对氨气分解转化率由高到低的顺序为：管-管> 管-板> 针-板> 板-板. 在输入功率为30 W，气隙间距为6 mm时，管-管交流弧放电的氨气转化率达到60%左右，而板-板介质阻挡放电的氨气转化率仅为4%.

关键词:

English

Influence of Non-Thermal Plasma Discharge Mode and Reactor Structure on Ammonia Decomposition to Hydrogen

1.
1 State Key Laboratory of Fine Chemicals, Department of Catalytic Chemistry and Engineering, Schol of Chemical Engineering, Dalian University of Technology, Dalian 116024, Liaoning Province, P. R. China;
2 School of Physics and Optoelectronic Engineering, Dalian University of Technology, Dalian 116024, Liaoning Province, P. R. China
Received Date: 04 December 2013
Available Online: 31 March 2014
Fund Project:
国家自然科学基金（20473016，20673018）资助项目

Abstract:

At ambient pressure, the effect of plasma discharge mode and reactor structure on ammonia decomposition to hydrogen was investigated. Dielectric barrier discharge (DBD) and alternating current (AC) arc discharge were produced upon adjusting the structure of the plasma reactor. By studying the discharge images, the voltage-current waveforms and the optical emission spectra in two discharge modes, we found that the AC arc discharge was a spatially partially stronger discharge compared with DBD. The AC arc discharge had a higher power efficiency and higher electron density than the dielectric barrier discharge. The ammonia molecules were mainly transformed into NH₃^* in an electronic excited state, and the N―H bond ruptured upon collision with a high-energy electron in DBD. However, electrons with a high average electron energy upon AC arc discharge can rupture the N―H bond directly to form highly active NH₂ and NH species, which can enhance the ammonia decomposition reaction. Results show that AC arc discharge had better performance toward ammonia decomposition than dielectric barrier discharge. The ability of different reactor structures to decompose ammonia under AC arc discharge increased in the following order: tube-tube>tube-flat>point-flat>flat-flat. The ammonia conversion can be as high as 60% under the tube-tube AC arc discharge with an input power of 30 W and a gap distance of 6 mm, while it was only 4% under the flat-flat dielectric barrier discharge.

Key words:

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沈阳化工大学材料科学与工程学院沈阳 110142

非平衡等离子体放电模式及反应器结构对氨气分解制氢的影响

English

Influence of Non-Thermal Plasma Discharge Mode and Reactor Structure on Ammonia Decomposition to Hydrogen

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

非平衡等离子体放电模式及反应器结构对氨气分解制氢的影响

English

Influence of Non-Thermal Plasma Discharge Mode and Reactor Structure on Ammonia Decomposition to Hydrogen

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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