Microcalorimetric adsorption and infrared spectroscopic studies of supported nickel catalysts for the hydrogenation of diisopropylimine to diisopropylamine
Microcalorimetric adsorption and infrared spectroscopic studies of supported nickel catalysts for the hydrogenation of diisopropylimine to diisopropylamine
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DOI：
10.1016/j.jcat.2018.03.022
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发表时间：
2018-06
影响因子：
7.3
通讯作者：
L. Deng;Jianxin Zhu;Hui Chen;Hui Wang;Jianyi Shen
中科院分区：
文献类型：
--
作者：
L. Deng;Jianxin Zhu;Hui Chen;Hui Wang;Jianyi Shen
以二异丙亚胺（DIPI）为探针分子，研究了 Ni/Al2O3、Ni/LaAlO 和 Ni/LaOx 催化剂上 C 双键 N 的加氢反应。应用微量热吸附和红外光谱测定反应物和产物的表面键强度和结构。研究发现，酸性载体有利于DIPI和H2在Ni上的吸附和活化，导致DIPI加氢活性（TOF）增加，而碱性载体则促进胺产物在Ni上的脱氢，不利于DIPI加氢。特别是，当使用异丙醇（IPA）作为溶剂时，由于IPA和DIPI之间的氢转移反应（HTR），DIPI的转化率显着增加，共吸附的IPA和DIPI的红外光谱进一步证明了这一点。
Diisopropylimine (DIPI) was used as a probe molecule to investigate the hydrogenation of Cdouble bondN on the Ni/Al2O3, Ni/LaAlO and Ni/LaOx catalysts. Microcalorimetric adsorption and infrared spectroscopy were applied to determine the surface bond strengths and structures of the reactant and product. It was found that the acidic support favored the adsorption and activation of DIPI and H2on Ni, leading to the increased activity (TOF) for the hydrogenation of DIPI, while the basic support promoted the dehydrogenation of the amine product on Ni, being unfavorable for the hydrogenation of DIPI. In particular, the conversion of DIPI was significantly increased when isopropanol (IPA) was used as a solvent, due to the hydrogen transfer reaction (HTR) between IPA and DIPI, which was further evidenced by the infrared spectrum of co-adsorbed IPA and DIPI.