基于负载型SBA-15催化剂的等离子体协同催化合成氨研究  

Research on Plasma-Synergized Catalytic Ammonia Synthesis Based on Supported SBA-15 Catalysts

作　　者：陈金飞 杜学森[1,2] 苏小军 李超凡 沈小强 胡陈龙 CHEN Jinfei;DU Xuesen;SU Xiaojun;LI Chaofan;SHEN Xiaoqiang;HU Chenlong(School of Energy and Power Engineering,Chongqing University,Chongqing 400044,China;Key Laboratory of Low-Grade Energy Utilization Technologies and Systems,Ministry of Education of PRC,Chongqing University,Chongqing 400044,China)

机构地区：[1]重庆大学能源与动力工程学院,重庆400044 [2]重庆大学低品位能源利用技术及系统教育部重点实验室,重庆400044

出　　处：《能源环境保护》2025年第2期151-160,共10页Energy Environmental Protection

基　　金：国家重点研发计划政府间国际科技创新合作专项(2021YFE0110800);国家自然科学基金资助项目(52176100)。

摘　　要：等离子体协同催化制氨展现出巨大的发展潜力,构建高效催化剂以提升等离子体与催化剂的协同作用是当前颇具挑战性的研究重点。通过对一系列负载型SBA-15催化剂(M/SBA-15,M=5Fe、5Co、5Ni、10Ni、15Ni)进行实验,探究等离子体强化氨合成反应的过程。研究结果表明,相较于Fe和Co,Ni表现出更出色的氨合成能力;等离子体催化合成氨的浓度随Ni负载量的增加呈现先增加而减小的火山形曲线关系,当Ni负载量从5%提升至10%时,氨合成性能提升8.0%,进一步提升Ni负载量至15%时,性能则下降了3.3%。经活性筛选出的性能最优催化剂(10Ni/SBA-15)的放电表征发现,该填充配置下的放电更均匀且更稳定,电流簇的平均电流值更高,这促进产生了数量更为庞大的高能电子和激发态活性粒子参与氨合成,从而实现了更高的氨合成性能。运行稳定性测试显示,催化剂的活性在前180 min内快速下降,随后基本维持不变,揭示了孔道结构对于等离子体催化合成氨反应的重要性。值得强调的是,在10Ni/SBA-15催化剂上实现了高达9927 mg/m^(3)的氨浓度和0.88 g/(kW·h)的能量产率,与相关前沿研究相比拥有较强的竞争力,为等离子体催化合成氨领域的高效催化剂设计提供了新的见解。Plasma-catalytic ammonia synthesis has garnered significant attention due to its potential for reducing energy consumption and mitigating environmental impact,emerging as a promising alternative to traditional thermal catalytic ammonia synthesis processes.Developing efficient catalysts to enhance the synergy between plasma and catalytic materials remains a key challenge.This study experimentally investigated a series of supported SBA-15 catalysts(M/SBA-15,M=5Fe,5Co,5Ni,10Ni,and 15Ni)to examine the process of plasma-enhanced ammonia synthesis.The initial characterization results indicated that the active metal species in all catalysts were present as metallic elements and oxides,both on the catalyst surface and within the pores,exhibiting uniform dispersion.Activity tests revealed that catalytic performance was not correlated with the specific surface area of the catalysts;rather,the inherent ammonia synthesis properties of the active metal species had a more significant impact.Notably,Ni-based catalysts exhibited superior catalytic activity compared to those based on Fe and Co.Further investigation into the ammonia synthesis activity of catalysts with varying Ni loadings revealed a volcano-shaped curve in plasma-assisted ammonia concentration,which initially increased and then decreased with increased Ni loading.Specifically,increasing the Ni loading from 5%to 10%improved ammonia synthesis performance by 8.0%,while further increasing the Ni loading to 15%led to a 3.3%decrease in performance.This relationship implied that a critical Ni loading threshold existed,above which excessive Ni loading could damage the catalyst's pore structure or cause surface poisoning.Subsequently,the discharge characteristics of the 10Ni/SBA-15 catalyst,which exhibited the highest ammonia synthesis performance,were analyzed.The results revealed a transition in discharge mode from filamentary discharge to a combination of filamentary and surface discharge,in contrast to an empty tube.This transition led to a more uniform and stable disc

关 键 词：介质阻挡放电等离子体 催化剂 氨合成 SBA-15 协同作用 

分 类 号：X511[环境科学与工程—环境工程]