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固体氧化物电池因其高效能量转换及低污染排放的特点，成为能源领域的研究热点。然而燃料极支撑固体氧化物电解池(SOEC)在电解CO2时面临传质极化大和电解性能有待提高等问题。本研究提出微观结构优化与材料双改性策略，显著提升了SOEC在CO2电解模式下的性能，通过对电极支撑体共流延过程中对功能层引入4%淀粉作为造孔剂，有效降低了传质阻力，使电解电流密度在750℃、1.6 V条件下提升至0.64 A·cm–2；同时采用溶胶–凝胶法合成Ce0.8Gd0.15Ni0.05O2并浸渍至燃料极，经还原处理后形成均匀分布的金属镍颗粒。电化学测试表明，改性电池在1.1 V和1.6 V下的电解电流密度分别进一步提高了58%和64%。X射线光电子能谱分析显示，第二活性相的修饰显著提高了电极材料氧空位浓度的增加，进一步促进了电解过程中氧离子传导。改性后电池在100 h长期测试中表现出良好的电压稳定性，为提升SOEC性能提供了有效的设计思路。
Abstract：Introduction Solid oxide electrolysis cells(SOECs) are promising devices that use high-temperature electrolysis to convert H_2O and CO2 into valuable fuels like H2 and CO.Compared with conventional electrolysis,SOECs operate at elevated temperatures,which improves efficiency via utilizing industrial waste heat and renewable energy sources.However,CO2 electrolysis faces challenges due to the chemical stability of CO2,requiring a high energy input to break its bonds.NiO-YSZ based fuel electrode-supported SOECs are widely used due to their good electrochemical performance and mechanical strength at a high temperature.Nonetheless,some issues such as reduced electrode conductivity,chemical stability,and interface reaction activity during long-term operation hinder their performance and lifespan.It is thus important for the enhancement of gas transport and catalytic activity to optimize the micro structure and composition of the fuel electrode.Methods In this work,a dual modification strategy for micro structure optimization and impregnation modification was proposed to improve SOEC fuel electrode performance for CO2 electrolysis.The electrode micro structure was optimized via introducing starch as a pore former during slurry preparation to adjust the porosity and improve gas diffusion.Half-cells consisting of NiO-YSZ support,NiO-YSZ functional layer,and YSZ electrolyte were fabricated by tape casting and sintered at 1350 ℃.In addition,Ce0.8Gd0.15Ni0.05O2(CGN) was synthesized by a sol-gel method and impregnated into the porous fuel electrode.After impregnation,samples were reduced in hydrogen to produce Ni nanoparticles dispersed on the Ce-based matrix.The micro structure was characterized by scanning electron microscopy(SEM) and X-ray diffraction(XRD),while the oxygen vacancies and active sites were determined by X-ray photoelectron spectroscopy(XPS),electron paramagnetic resoance(EPR),and carbon dioxide temperature programmed desorption(CO2-TPD).The electrochemical performance was evaluated by impedance spectroscopy and current-voltage measurements.Results and Discussion The introduction of starch effectively increases the electrode porosity,thus reducing mass transfer polarization resistance and enhancing gas transport.The results of electrochemical tests demonstrate that the optimized electrode has a current density of 0.64 A·cm-2 at 750℃ and 1.6 V under CO2 electrolysis atmosphere.The impregnation of CGN precursor leads to the uniform dispersion of Ni nanoparticles and increases oxygen vacancy concentration.These modifications significantly improves catalytic activity toward CO2 reduction,and the electrolysis current density is increased by 58% and 64% at 1.1 V and1.6 V,respectively.The impedance data indicate a marked decrease in polarization resistance.The long-term stability tests over 100 hours show a stable electrochemical performance,indicating that the combined structural and compositional modifications effectively enhance electrode durability and activity.Conclusions The dual modification approach integrating micro structural optimization and CGN impregnation significantly enhanced SOEC fuel electrode performance in CO2 electrolysis.Increased porosity improved gas transport,while Ni catalyst modification boosted catalytic activity and oxygen ion transport.This strategy could provide a practical and cost-effective method to improve SOEC durability and efficiency without using expensive noble metals.The findings could offer a valuable guidance for the development of next-generation high-performance SOEC systems for carbon-neutral energy applications.
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基本信息:
DOI：10.14062/j.issn.0454-5648.20250217
中图分类号:TM911.4
引用信息:
[1]项永康,丁镇发,张肖鑫,等.固体氧化物电解池燃料极表界面的传质/活化双改性策略[J].硅酸盐学报,2025,53(10):2952-2962.DOI:10.14062/j.issn.0454-5648.20250217.
基金信息:
国家自然科学基金(22472134,22272136)
2025-03-26
2025
2025-03-27
2025
1
2025-10-15
2025-10-15