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作者

Kun Liu Yongbin Sun Jie Feng Yang Liu Jian Zhu Chengjun Han Changzhi Chen Tianyi Bao Xiaoqun Cao Xiaomin Zhao Yong Yang Guofeng Zhao

作者单位

²Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai 200062, China ⁵Zhejiang Xinhua CHEMICAL CO., LTD., Jiande 311607, China ³School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, China ⁴Department of Chemistry, Zhejiang University, Hangzhou 310058, China ¹Institute of Optical Functional Materials for Biomedical Imaging, School of Chemistry and Pharmaceutical Engineering, Shandong First Medical University & Shandong Academy of Medical Sciences, Taian 271016, China

刊名

Chemical Engineering Journal

年份

2022

页码

140059

ISSN

1385-8947

关键词

Acetone hydrogenation Isopropanol Metal-oxide interface Interface catalysis Oxygen vacancy Acetone adsorption

摘要

The gas-phase acetone hydrogenation to isopropanol is an environmentally benign process relevant to chemical, energy and medical fields, but the catalysts qualified at low temperature and pressure remain challenging. Herein, we show the intensified gas-phase hydrogenation of acetone to isopropanol at metal-oxide interface. The Pt/CeO catalyst with highly active and stable Pt-CeO interface delivers 92% acetone conversion with 99% isopropanol selectivity at 80 C, weight hourly space velocity of 10...更多

The gas-phase acetone hydrogenation to isopropanol is an environmentally benign process relevant to chemical, energy and medical fields, but the catalysts qualified at low temperature and pressure remain challenging. Herein, we show the intensified gas-phase hydrogenation of acetone to isopropanol at metal-oxide interface. The Pt/CeO catalyst with highly active and stable Pt-CeO interface delivers 92% acetone conversion with 99% isopropanol selectivity at 80 C, weight hourly space velocity of 10 h, H/acetone molar ratio of 2, and 0.1 MPa, and its catalytic performance is preserved during a single-running test of 200 h. A series of electron microscopic, thermal, and spectroscopic analyses testify that acetone could be efficiently adsorbed on oxygen vacancy at Pt-CeO interface. The H atoms dissociated by Pt spill over to the interface to hydrogenate the chemically-adsorbed acetone thereon to form isopropanol. Inspired by such observation, the Pt-CeO interface was extended to other metal-oxide interfaces , all exhibiting excellent catalytic performance. For example, the Ni/CeO could offer 91% acetone conversion and 99% isopropanol selectivity, identical to that of Pt/CeO under the same conditions. This work particularly investigated the acetone adsorption at the metal-oxide interface, establishing the foundation for rational design of high cost performance catalysts for aldehydes/ketones hydrogenation and other reactions.收起

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