基于多孔镍电极的液相放电等离子体分解甲醇制氢实验研究

doi:10.11949/0438-1157.20250483

摘要/Abstract

摘要：

液相放电等离子体技术可突破传统热化学路径的限制，在常温常压下实现液态燃料的快速在线分解制氢。本研究设计了一种基于多孔镍材料的新型高压电极，搭建了可视化放电实验平台，系统开展了甲醇液相放电分解制氢过程的特性研究，重点分析了放电、气泡行为、能质传递特性及其对制氢性能的影响。实验结果表明，多孔电极显著增大了滑动弧放电等离子体气泡体积，并改善了放电通道的时空分布，从而有效提升了甲醇与等离子体间的反应界面与传质效率。与传统针电极相比，采用多孔电极后产氢速率提升至791.6 ml/min，增长38%；单位产氢能耗降低至1.45 kWh/m³ H₂，降幅达33.78%。在长周期运行过程中，多孔电极体系的甲醇分解性能衰减率较传统系统降低超过72%，展现出优异的运行稳定性与寿命特性。研究结果为液相等离子体制氢反应器的高效化、稳定化设计提供了理论依据与关键技术支撑。

关键词: 制氢, 甲醇, 多孔电极, 液相放电等离子体, 气泡行为

Abstract:

Liquid-phase discharge plasma technology can break through the limitations of the traditional thermochemical pathway and realize rapid on-line decomposition of liquid fuels for hydrogen production at ambient temperature and pressure. In this study, a new high-voltage electrode based on porous nickel material was designed, and a visual discharge experimental platform was constructed to systematically carry out the characterization of methanol liquid-phase discharge plasma decomposition for hydrogen production, focusing on the analysis of the discharge mode, the bubble behavior, the energy-mass transfer characteristics and their effects on the hydrogen production performance. The experimental results show that in the sliding arc discharge mode, the use of porous electrodes significantly increases the plasma bubble volume and improves the spatial and temporal distribution of the discharge channel, which effectively enhances the reaction interface between methanol and plasma and the mass transfer efficiency. Compared with the traditional needle electrode, the use of porous electrodes increased the hydrogen production rate to 791.6 ml/min, a 38% increase. The unit energy consumption for hydrogen production was reduced to 1.45 kWh/m³ H₂, a 33.78% decrease. During the long cycle operation, the methanol decomposition performance decay rate of the porous electrode system was reduced by more than 72% compared with the traditional system, showing excellent operational stability and lifetime characteristics. The results provide a theoretical basis and key technical support for the design of liquid-phase plasma hydrogen generation reactor with high efficiency and stability.

Key words: hydrogen production, methanol, porous electrodes, liquid-discharge plasma, bubble behavior

中图分类号:

TK 91

双舒炎, 张伟, 王家乐, 王军锋. 基于多孔镍电极的液相放电等离子体分解甲醇制氢实验研究[J]. 化工学报, 2025, 76(11): 5753-5763.

Shuyan SHUANG, Wei ZHANG, Jiale WANG, Junfeng WANG. Experimental study on hydrogen production from methanol decomposition by liquid-phase discharge using porous nickel electrodes[J]. CIESC Journal, 2025, 76(11): 5753-5763.

图/表 12

图1 基于多孔电极的液相放电等离子体制氢实验系统

Fig.1 Liquid-phase discharge plasma hydrogen generation experimental system based on porous electrode

图2 等离子体气泡图像处理

Fig.2 Image processing of plasma bubble

图3 滑动弧放电电压-电流波形：(a) 针电极 (61.28 W)；(b)110 ppi多孔电极 (62.99 W)

Fig.3 Voltage-current wave of GAD: (a) needle electrode (61.28 W); (b) 110 ppi porous electrode (62.99 W)

图4 不同电极分解甲醇过程中等离子体发射光谱：（a）镍针电极；（b）多孔镍电极

Fig.4 Optical emission spectra of plasma during methanol decomposition with different electrodes: (a) nickel needle electrode; (b) porous nickel electrode

图5 不同孔隙密度多孔电极与针电极分解甲醇产气速率对比

Fig. 5 Comparison of syngas production yield from methanol decomposition by needle electrode and porous electrodes with different pore densities

图6 不同孔隙密度多孔电极与针电极分解甲醇气相产物组分对比

Fig. 6 Comparison of gas-phase product fractions of methanol decomposition by porous electrode and needle electrode with different pore densities

图7 不同孔隙密度多孔电极与针电极分解甲醇制氢能耗对比

Fig. 7 Comparison of energy consumption for hydrogen production from methanol decomposition by needle electrodes and porous electrodes with different pore densities

图8 不同高压电极对等离子体气泡形貌时空演变规律的影响：(a) 针电极；(b) 多孔镍电极

Fig. 8 Effects of different high-voltage electrodes on the spatial and temporal evolution of plasma bubble morphology: (a) needle electrode; (b) porous nickel electrode

图9 不同电极滑动弧放电产生的等离子体气泡尺寸变化趋势

Fig. 9 Trends in plasma bubble size from gliding arc discharge by different electrodes

图10 高压电极放电1 h表面SEM图：(a) 针电极（无多孔镍保护）；(b) 针电极（多孔镍保护）；(c) 多孔镍

Fig. 10 SEM images of the surface of the high-voltage electrode discharged for 1 hour: (a) needle electrode (no porous nickel protection); (b) needle electrode (porous nickel protection); (c) porous nickel

图11 EDS电极表面元素组成分析

Fig. 11 Analysis of the elemental composition of the electrode surface by EDS

图12 持续放电过程中甲醇分解性能变化：(a) 不同电极分解甲醇稳定性对比；(b) 多孔电极产气流量变化

Fig. 12 Variation of methanol decomposition properties during continuous discharges: (a) comparison of methanol decomposition stability of different electrodes; (b) variation of syngas flow rate by porous electrodes

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