中温质子导体电解池型氨合成反应器研究  

Research on intermediate-temperature protonic ceramic electrolysis cells as ammonia synthesis reactors

作　　者：朱行志 陈楚 苗笑云 叶晓峰[1,2] 温兆银 ZHU Xingzhi;CHEN Chu;MIAO Xiaoyun;YE Xiaofeng;WEN Zhaoyin(Shanghai Institute of Ceramics,Chinese Academy of Sciences,Shanghai 200050,China;University of Chinese Academy of Sciences,Beijing 100049,China)

机构地区：[1]中国科学院上海硅酸盐研究所,上海200050 [2]中国科学院大学,北京1000049

出　　处：《燃料化学学报(中英文)》2025年第2期262-271,共10页Journal of Fuel Chemistry and Technology

基　　金：国家自然科学基金(52372246)资助。

摘　　要：当前传统的氨气规模化生产造成了大量的能源消耗和碳排放,需要寻找一种低碳的技术途径,因此,绿氨合成成为“双碳”背景下的重要研究课题之一。质子导体型陶瓷电解池(Protonic Ceramic Electrolysis Cells,PCECs)可采用可再生电力电解水蒸气原位制氢,有望用作绿氨合成反应器。本研究采用Ni-BaCe_(0.7)Zr_(0.1)Y_(0.2)O_(3)−δ(BCZY)多孔复合陶瓷,研究了质子导体燃料电极的材料特性和合成氨反应条件,650℃时获得了1.04×10^(−10) mol/(s·cm^(2))合成氨速率。基于以上结果,以等静压-浸渍-共烧的工艺方法制备了活性面积达到10 cm^(2)的管式质子导体型电解池。其在650℃,1.4 V电压下获得3 A电解电流,并在合成氨工况条件下稳定运行;管式电池原位产氢能够用于Ni-BCZY燃料电极上的合成氨过程并显著促进了氨产率的提升,合成氨速率达到7.02×10^(−10) mol/(s·cm^(2))。200 h的测试结果表明,电解池的电化学性能与合成氨速率均表现出良好的稳定性,显示了作为绿氨合成反应器的潜力。Ammonia is a carbon-free fuel with high energy density,offering advantages over hydrogen due to its easier liquefaction,which facilitates storage and transportation.This makes it a promising candidate for future applications in energy storage and transportation.Currently,traditional ammonia production relies primarily on the Haber-Bosch process,which requires high temperatures and pressures,leading to significant fossil fuel consumption and carbon emissions.Thus,it is necessary to develop low-carbon technological pathway for ammonia synthesis,making green ammonia synthesis a critical research area under the“dual carbon”goals.Protonic ceramic electrolysis cells(PCECs)can utilize renewable electricity to electrolyze steam at the oxygen electrode,generating protons that are then used at the fuel electrode to synthesize ammonia.This process offers higher energy efficiency,positioning PCECs as potential reactors for green ammonia synthesis.In this study,a porous Ni-BaCe_(0.7)Zr_(0.1)Y_(0.2)O_(3)−δ(BCZY)composite ceramic was employed to investigate the material properties of the composite fuel electrode and the working conditions for ammonia synthesis.At 650℃,with a nitrogen-to-hydrogen partial pressure ratio of 1∶3,an ammonia synthesis rate of 1.04×10^(−10) mol/(s·cm^(2))was achieved.Building on these results,a tubular protonic ceramic electrolysis cell with an active area of 10 cm^(2) was fabricated using isostatic pressing-impregnation-cosintering method.Each part of cell was firmly bonded without delamination.The tubular cell demonstrated excellent hydrogen production performance,achieving an electrolysis current of 3 A at 650℃under a 1.4 V applied voltage,and operated stably under ammonia synthesis conditions.The significant voltage-dependent response in ammonia synthesis rate confirmed that the in-situ hydrogen production within the tubular cell effectively facilitated the ammonia synthesis process on the Ni-BCZY fuel electrode,with an enhanced ammonia synthesis rate reaching 7.02×10^(−10) mol

关 键 词：质子导体 合成氨 产率 稳定性 

分 类 号：TM911.4[电气工程—电力电子与电力传动]