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Role of Manganese Oxide in Syngas Conversion to Light Olefins

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† State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Zhongshan Road 457, Dalian 116023, People’s Republic of China
‡ University of Chinese Academy of Sciences, Beijing 100049, People’s Republic of China
§ State Key Laboratory of Functional Materials for Informatics, Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences, Shanghai 200050, People’s Republic of China
∥ School of Physical Science and Technology, ShanghaiTech University, Shanghai 200031, People’s Republic of China
*E-mail for X.P.: [email protected]
*E-mail for X.B.: [email protected]
Cite this: ACS Catal. 2017, 7, 4, 2800–2804
Publication Date (Web):March 23, 2017
https://doi.org/10.1021/acscatal.7b00221
Copyright © 2017 American Chemical Society
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Abstract

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The key of syngas (a mixture of CO and H2) chemistry lies in controlled dissociative activation of CO and C–C coupling. We demonstrate here that a bifunctional catalyst of partially reducible manganese oxide in combination with SAPO-34 catalyzes the selective formation of light olefins, which validates the generality of the OX-ZEO (oxide-zeolite) concept for syngas conversion. Results from in situ ambient-pressure X-ray photoelectron spectroscopy, infrared spectroscopy, and temperature-programmed surface reactions reveal the critical role of oxygen vacancies on the oxide surface, where CO dissociates and is converted into surface carbonate and carbon species. They are converted to CO2 and CHx in the presence of H2. The limited C–C coupling and hydrogenation activities of MnO enable the reaction selectivity to be controlled by the confined pores of SAPO-34. Thus, a selectivity of light olefins up to 80% is achieved, far beyond the limitation of Anderson–Shultz–Flory distribution. These findings open up possibilities to explore other active metal oxides for more efficient syngas conversion.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acscatal.7b00221.

  • Details of the experiments and Tables S1 and S2 and Figures S1–S8 as described in the text (PDF)

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