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Direct Conversion of Syngas into Light Olefins over Zirconium‐Doped Indium(III) Oxide and SAPO‐34 Bifunctional Catalysts: Design of Oxide Component and Construction of Reaction Network
ChemCatChem ( IF 3.8 ) Pub Date : 2018-02-27 , DOI: 10.1002/cctc.201702054
Junjie Su 1 , Dong Wang 1 , Yangdong Wang 1 , Haibo Zhou 1 , Chang Liu 1 , Su Liu 1 , Chuanming Wang 1 , Weimin Yang 1 , Zaiku Xie 2 , Mingyuan He 3
Affiliation  

The direct synthesis of light olefins from syngas over a bifunctional catalyst containing an oxide and zeolite has been proven to be a promising strategy. Nevertheless, an unclear reaction network hinders any further enhancement in catalytic performance, such as increasing the conversion of CO. We herein report a novel bifunctional catalyst composed of a InZr binary oxide and SAPO‐34 zeolite displaying superior CO conversion (27.7 %) with selectivity to light olefins (73.6 %) at 400 °C, 2.0 MPa. We demonstrate that the Zr‐doped body‐centered cubic In2O3 phase, exhibiting higher stability than pure In2O3 under a reducing atmosphere, is the active oxide component for the initial activation of CO. A complete reaction network is proposed by DFT calculations and model reactions, revealing that CO activation over Zr‐In2O3 follows a quasi‐CO2 hydrogenation pathway and methanol is the key intermediate to be transformed into light olefins in zeolites. Moreover, inhibiting excessive hydrogenation is an effective strategy to achieve higher performance.

中文翻译:

锆掺杂的氧化铟(III)和SAPO-34双功能催化剂将合成气直接转化为轻烯烃:氧化物组分的设计和反应网络的构建

由合成气在含氧化物和沸石的双官能催化剂上直接合成轻烯烃已被证明是一种有前途的策略。然而,不清楚的反应网络阻碍了催化性能的任何进一步提高,例如增加了CO的转化率。我们在此报告了一种由InZr二元氧化物和SAPO-34沸石组成的新型双功能催化剂,具有优异的CO转化率(27.7%),具有选择性在400°C,2.0 MPa下制得轻质烯烃(73.6%)。我们证明了Zr掺杂的体心立方In 2 O 3相比纯In 2 O 3具有更高的稳定性。DFT计算和模型反应提出了一个完整的反应网络,表明在Zr‐In 2 O 3上的CO活化遵循准CO 2加氢途径,并且在还原性气氛下,CO的初始活化是活性氧化物组分。甲醇是在沸石中转化为轻质烯烃的关键中间体。此外,抑制过度氢化是实现更高性能的有效策略。
更新日期:2018-02-27
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