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氨合成铁催化剂上化学吸附物种的in-situ FTIR谱; In-situ FTIR Spectra of Chemisorbed Species on Iron Catalysts for Ammonia Synthesis
廖代伟 ; 林种玉 ; 蔡启瑞
1996-09
关键词原位傅里哀变换红外光谱 合成氨催化反应机理 化学吸附物种 同位素验证 In-situ FTIR Catalytic reaction mechanism of ammonia synthesis Chemisorbed species Isotopic verification
英文摘要[中文文摘]应用原位傅里哀变换红外光谱方法,分别在400~450℃、常压、高空速(12000~14400h.s.v.g.)的H2、N2/3H2或N2气氛的动态条件下,检测了双促进氨合成铁催化剂上的化学吸附物种,并分别在D2、N2/3D2或15NH3/H2气氛中,进行了常规同位素验证实验.结果表明,催化剂表面的主要含氮化学吸附物种是分子态的N2.ad,其u(N-N)=2036cm-1(s),2012cm-1(w)和1935cm-1(w),而不是原子态的Nad,其u(Fe-N)=1087cm-1(vw),和NHad其u(Fe-N)=886cm-1(vw),表面有相当量的化学吸附氢存在,其v(Fe-H)=2056cm-1(s),1950cm-1(ms),1931cm-1(m),1902cm-1(w),915cm-1(s,桥式)等.作为与报道过的激光拉曼光谱的互补研究,本结果支持了以缔合式途径为主、解离式途径为次的平行竞争缔合式合成氨催化反应机理.[英文文摘]Chemisorbed species on doubiy promoted ammonia synthesis iron catalysts are investigated by in-situ Fourier transform infrared spectroscopy under dynamic conditions of H2, N2/3H2, and N2, respectively, with high space velocity (12 000~14 400 h-1) at 1 atm and400 ~450℃. Also, the general isotopic verifications are carred out with D2, N2/3D2, and NH3/H2, respectively. The results indicated that, under above reaction condition, the most aboundant chemisorbed N-containing species are molecular N2,ad with u(N-N)=2036 cm-1(s),2012 cm-1(w) and 1935 cm-1(w),rather than atomic Nad with u(Fe-N)=1087 cm-1(vw) and NHad with u(Fe-N)=886 cm-1 (vw).There are a lot of chemisorbed hydrogen with u(Fe-H)=2056 cm-1(s),1950 cm-1(ms),1931 cm-1(m),1902 cm-1(w) and 915 cm-1(s,dridge).As a complementary study for the laser Raman spectra previously reported,this paper supported the associative catalytic reaction mechanism of ammonia synthesis with both parallel competitive major associative pathway and minor dissociative pathway.
语种中文
出版者《厦门大学学报(自然科学版)》编辑部
内容类型期刊论文
源URL[http://dspace.xmu.edu.cn/handle/2288/12352]  
专题化学化工-已发表论文
推荐引用方式
GB/T 7714
廖代伟,林种玉,蔡启瑞. 氨合成铁催化剂上化学吸附物种的in-situ FTIR谱, In-situ FTIR Spectra of Chemisorbed Species on Iron Catalysts for Ammonia Synthesis[J],1996.
APA 廖代伟,林种玉,&蔡启瑞.(1996).氨合成铁催化剂上化学吸附物种的in-situ FTIR谱..
MLA 廖代伟,et al."氨合成铁催化剂上化学吸附物种的in-situ FTIR谱".(1996).
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