等离子体辅助铈基催化剂催化氨制氢的性能研究  

Catalytic Performance of Plasma-Assisted Ceria-Based Catalysts for Hydrogen Generation From Ammonia

作　　者：高一博 胡二江[1] 殷阁媛 黄佐华[1] GAO Yibo;HU Erjiang;YIN Geyuan;HUANG Zuohua(State Key Laboratory of Multiphase Flow in Power Engineering,Xi′an Jiaotong University,Xi′an 710049,China)

机构地区：[1]西安交通大学动力工程多相流国家重点实验室,陕西西安710049

出　　处：《石油学报（石油加工）》2023年第5期1173-1183,共11页Acta Petrolei Sinica(Petroleum Processing Section)

基　　金：国家自然科学基金项目(51888103,52176131);西安交通大学基础科研业务费(xzy022022043)资助。

摘　　要：以铈基纳米球(CeO_(2)-S)为载体,掺杂3d过渡金属(Fe、Co和Ni),研究金属掺杂CeO_(2)基催化剂在氨分解制氢反应中的催化性能。采用X射线衍射仪(XRD)、高角度环形暗场扫描透射电镜(HAADF-STEM)、能量色散X射线能谱(EDX-mapping)、拉曼(Raman)等表征方法对催化剂的理化性质进行分析。结果表明,与单金属掺杂相比,双金属共掺杂的CeO_(2)基催化剂增加了催化剂的氧空位,促进了电子从CeO_(2)载体向活性金属的转移,进而促进氨分解。在非热平衡等离子体(输入电压8000 V)辅助催化氨分解反应中,FeCo/CeO_(2)-S催化剂的H2生成速率最高,达到29.3 mmol/(g_(cat)·min),并在550℃下实现NH_(3)的完全转化。等离子体与催化剂协同可进一步提高氨分解制氢的性能,为能源载体制氢提供一种新思路。The performance of ceria catalyst for hydrogen production from ammonia decomposition was studied by doping 3d transition metals(Fe,Co and Ni)with ceria nanospheres(CeO_(2)-S)as carrier.The physicochemical properties of the catalyst were characterized by X-ray diffraction(XRD),high angle annular dark field-scanning transmission electron microscopy(HAADF-STEM),energy dispersive X-ray-mapping(EDX-mapping),Raman spectroscopy(Raman),and etc.The results show that compared with the mono-metal doped catalysts,the bimetal co-doped ceria-based catalyst has enriched oxygen vacancy of the catalyst and facilitated the transfer of electrons from the CeO_(2)carrier to metals,thus promoting ammonia decomposition.In the non-thermal plasma(input voltage 8000 V)assisted-catalysis in ammonia decomposition,the FeCo/CeO_(2)-S catalyst achieved the highest hydrogen production rate of 29.3 mmol/(g_(cat)·min),and the complete conversion of NH_(3)at 550℃.The combination of plasma and catalyst can further improve the performance of ammonia decomposition for hydrogen production,thus providing a new idea for energy carrier hydrogen generation.

关 键 词：氨制氢 氧化铈载体 形貌效应 3d过渡金属掺杂 等离子体 

分 类 号：TQ426.94[化学工程]