An IR Study on Selective Hydrogenation of 1,3-Butadiene on Transition Metal Nitrides: 1,3-Butadiene and 1-Butene Adsorption on Mo2N/γ-Al2O3 Catalyst

An IR Study on Selective Hydrogenation of 1,3-Butadiene on Transition Metal Nitrides: 1,3-Butadiene and 1-Butene Adsorption on Mo2N/γ-Al2O3 Catalyst
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DOI:
10.1021/jp002488w
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发表时间:
2000-11
影响因子:
3.3
通讯作者:
Zili Wu;Zhixian Hao;Pinliang Ying;Can Li;Q. Xin
Zili Wu;Zhixian Hao;Pinliang Ying;Can Li;Q. Xin
中科院分区:
化学3区
文献类型:
--
作者:
Zili Wu;Zhixian Hao;Pinliang Ying;Can Li;Q. Xin

文献摘要

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利用原位红外光谱(FT-IR)对Mo2N/γ-Al2O3催化剂上吸附1,3-丁二烯和1-丁烯形成的表面物质进行了表征,试图深入了解1,3-丁二烯在过渡金属氮化物催化剂上的选择性加氢作用。1,3-丁二烯在Mo2N/γ-Al2O3催化剂上吸附形成几种化学吸附表面物质:π吸附丁二烯(πs和πd);σ键物种;种物种。氮化催化剂表面存在π键丁烯和σ键丁烯,对1-丁烯进行吸附和反应。π吸附丁二烯的存在显著地阻止了1-丁烯在氮化催化剂上的吸附、进一步加氢和异构化,从而使得1,3-丁二烯加氢成1-丁烯具有很高的选择性。表面氮原子削弱了1,3-丁二烯与催化剂表面的相互作用,使得1,3-丁二烯加氢成1-丁烯具有较高的选择性。
The surface species formed from the adsorption of 1,3-butadiene and 1-butene on Mo2N/γ-Al2O3 catalyst have been characterized by in situ FT-IR spectroscopy with an attempt to get insight into the selective hydrogenation of 1,3-butadiene on transition metal nitride catalysts. 1,3-Butadiene adsorption on the Mo2N/γ-Al2O3 catalyst forms several kinds of chemisorbed surface species: π-adsorbed butadiene (πs and πd); σ-bonded species; dehydrogenated species. πs- and σ-bonded butene species are present on the surface for 1-butene adsorption and reaction on the nitride catalyst. The presence of the πd-adsorbed butadiene significantly prevents 1-butene from its adsorption, further hydrogenation, and isomerization on the nitrided catalyst, accordingly resulting in high selectivity in the hydrogenation of 1,3-butadiene to 1-butene. The surface nitrogen atoms weaken the interaction between 1,3-butadiene and the catalyst surface, and result in the high selectivity in the hydrogenation of 1,3-butadiene to 1-butene.