Role of Manganese Oxide in Syngas Conversion to Light Olefins

被引：239

作者：

Zhu, Yifeng ^{[1
]}

Pan, Xiulian ^{[1
]}

Jiao, Feng ^{[1
,2
]}

Li, Jian ^{[1
,2
]}

Yang, Junhao ^{[1
,2
]}

Ding, Minzheng ^{[1
]}

Han, Yong ^{[3
,4
]}

Liu, Zhi ^{[3
,4
]}

Bao, Xinhe ^{[1
]}

机构：

[1] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Zhongshan Rd 457, Dalian 116023, Peoples R China

[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China

[3] Chinese Acad Sci, Shanghai Inst Microsyst & Informat Technol, State Key Lab Funct Mat Informat, Shanghai 200050, Peoples R China

[4] ShanghaiTech Univ, Sch Phys Sci & Technol, Shanghai 200031, Peoples R China

来源：

ACS CATALYSIS | 2017年 / 7卷 / 04期

基金：

中国博士后科学基金; 美国国家科学基金会;

关键词：

syngas chemistry; light olefins; manganese oxides; CO dissociation; bifunctional catalysts; heterogeneous catalysis; oxide-zeolite; WATER-GAS SHIFT; FISCHER-TROPSCH SYNTHESIS; SELECTIVE CONVERSION; ELECTRONIC-STRUCTURE; DEPTH-PROFILE; CATALYSTS; RANGE; OXIDATION; CERIA; XPS;

D O I：

10.1021/acscatal.7b00221

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

The key of syngas (a mixture of CO and H-2) 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 H-2. 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.

引用

页码：2800 / 2804

页数：5

共 26 条

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