水对Ni/MgAlO催化丙酮加氢的影响

doi:10.1016/S1872-2067(14)60240-0

催化学报 ›› 2015, Vol. 36 ›› Issue (3): 380-387.DOI: 10.1016/S1872-2067(14)60240-0

水对Ni/MgAlO催化丙酮加氢的影响

陈慧, 赵杰, 李少中, 徐军, 沈俭一

南京大学化学化工学院, 介观化学教育部重点实验室, 江苏南京210093

收稿日期:2014-08-15 修回日期:2014-09-29 出版日期:2015-02-14 发布日期:2015-02-14
通讯作者: 沈俭一
基金资助:
国家自然科学基金(21273105); 江苏省自然科学基金青年基金(BK20140596); 国家高技术研究发展计划(863计划, 2013AA031703).

Effects of water on the hydrogenation of acetone over Ni/MgAlO catalysts

Hui Chen, Jie Zhao, Shaozhong Li, Jun Xu, Jianyi Shen

Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210093, Jiangsu, China

Received:2014-08-15 Revised:2014-09-29 Online:2015-02-14 Published:2015-02-14
Supported by:
This work was supported by the National Natural Science Foundation of China (21273105), the Natural Science Foundation of Jiangsu Province, China (BK20140596), and the National High Technology Development Program of China (863 Program, 2013AA031703).

摘要/Abstract

摘要：

研究了H₂O对Ni/MgAlO催化剂上丙酮加氢为异丙醇的催化反应的影响.结果发现, 在丙酮中添加少量H₂O可提高丙酮转化率, 但超过5%的H₂O量则会显著降低催化剂活性.吸附量热结果表明, 催化剂表面吸附少量H₂O会明显降低异丙醇的吸附热, 但对丙酮吸附热的影响较小, 这也许是反应体系中少量的H₂O能促进丙酮加氢活性的原因之一.当催化剂表面吸附较多H₂O后, 丙酮、异丙醇和H₂的吸附热都降低了, 因此反而抑制了丙酮的加氢反应.此外, 红外光谱结果表明, 预吸附水抑制了催化剂表面异丙醇脱氢生成丙酮, 并抑制吸附的丙酮在表面生成烯醇盐或异丙叉丙酮等物种, 这也许是少量水能促进丙酮加氢生成异丙醇的另一个重要原因.

关键词: 镍, 负载型催化剂, 丙酮加氢, 水的影响, 吸附量热, 红外光谱

Abstract:

The effect of water on the hydrogenation of acetone to isopropanol (IPA) on the Ni/MgAlO catalyst was studied. It was found that small amount of water added in the acetone promoted the conversion of acetone to IPA, while more H₂O added (>5%) significantly decreased the conversion of acetone. Microcalorimetric adsorption results showed that the presence of small amount of pre-adsorbed water (4% coverage) enhanced the adsorption of acetone while inhibited the adsorption of IPA on Ni, which might be the important reasons for the promotion effect of some water on the hydrogenation of acetone to IPA. On the other hand, the heats for the adsorption of H₂, acetone and IPA on the Ni/MgAlO were significantly decreased when more water was pre-adsorbed, which might explain the inhibition effect of more water on the hydrogenation of acetone. The results of infrared spectroscopy revealed that the presence of water suppressed the dehydrogenation of adsorbed IPA to acetone and the formation of enolate and mesityl oxide species from adsorbed acetone, which might be the other reasons for the positive effect of water on the hydrogenation of acetone to IPA.

Key words: Nickel, Supported catalyst, Hydrogenation of acetone, Effect of water, Microcalorimetric adsorption, Fourier transform infrared spectroscopy

陈慧, 赵杰, 李少中, 徐军, 沈俭一 . 水对Ni/MgAlO催化丙酮加氢的影响[J]. 催化学报, 2015, 36(3): 380-387.

Hui Chen, Jie Zhao, Shaozhong Li, Jun Xu, Jianyi Shen . Effects of water on the hydrogenation of acetone over Ni/MgAlO catalysts[J]. Chinese Journal of Catalysis, 2015, 36(3): 380-387.

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水对Ni/MgAlO催化丙酮加氢的影响

Effects of water on the hydrogenation of acetone over Ni/MgAlO catalysts

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