负载型过渡金属氮化物氨合成反应性能研讨.pdfVIP

G022 负载型过渡金属氮化物氨合成反应性能研究 卢春山，马磊，刘武灿，韩文锋，李小年* （浙江工业大学资源与环境催化研究所，绿色化学合成技术 国家重点实验室培育基地，杭州310032 ） 摘 要 本文采用氨程序升温氮化还原法制备了CoxMoyN/ γ-Al2O3、NixMoyN/ γ-Al2O3 和FexMoyN/ γ -Al2O3 三种双过渡金属氮化物催化剂，并对其进行了XRD 、TPR-MS 和常压氨合成反应催化性能表征。结 果表明，在实验范围内，利用非原位XRD 无法检测到清晰的金属氮化物的特征峰；但在TPR-MS 谱图中， 出现了两种明显的 N2 脱附峰，其来源于催化剂表面氮化物物种中的渗入氮，可分别归结为氮化物晶型转 变和氮化物物种的进一步分解；负载型双金属氮化物催化剂的氨合成催化活性远远高于单金属氮化钼催化 剂，也远高于文献报道的非负载型双金属氮化物催化剂。 关键词 氮化物 氨合成 催化剂 STUDY OF CATALYTIC ACTIVITY OF SUPPORTED BIMETALLIC NITRIDES FOR AMMONIA SYNTHESIS LU Chunshan, MA Lei, LIU Wucan, HAN Wenfeng, LI Xiaonian* （Resources Environment Catalysis Institute of Zhejiang University of Technology, State Key Laboratory Breeding Base of Green Chemistry Synthesis Technology, Hangzhou 310032 ） Abstract A series of bimetallic nitrides supported on γ-Al2O3 were prepared by temperature-programmed reaction with NH3 and their corresponding oxide precursors. Catalytic activity test, TPR-MS, and XRD were employed to investigate the catalytic activity for ammonia synthesis, also to obtain better insight into the structure of the bimetallic nitride. No marked characteristic diffraction peaks of bimetallic nitrides have been observed in the XRD spectra due to that the bimetallic nitrides highly disperse or may be generated in amorphous state on the surface of γ-Al2O3. Two nitrogen desorption peaks at temperatures of 400-700 oC and 727-1000 oC could be ascribed to the structural change and the farther decomposition of formed nitrides respectively. The experimental results of ammonia synthesis activity show that supported bimetallic nitrides are more active than monometallic nitrides or unsupported bimetallic nitrides reported in the literature[11]