Conversion of syngas into light olefins over bifunctional ZnCeZrO/SAPO-34 catalysts: regulation of the surface oxygen vacancy concentration and its relation to the catalytic performance,Catalysis Science & Technology

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Conversion of syngas into light olefins over bifunctional ZnCeZrO/SAPO-34 catalysts: regulation of the surface oxygen vacancy concentration and its relation to the catalytic performance
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2020-11-02 , DOI: 10.1039/d0cy01759k
Yaoya Luo _{1,

2,

3,

4,

5} , Sen Wang _{1,

2,

3,

4,

5} , Shujia Guo _{1,

2,

3,

4,

5} , Kai Yuan _{1,

2,

3,

4,

5} , Hao Wang _{1,

2,

3,

4,

5} , Mei Dong _{1,

2,

3,

4,

5} , Zhangfeng Qin _{1,

2,

3,

4,

5} , Weibin Fan _{1,

2,

3,

4,

5} , Jianguo Wang _{5,

6,

7}

Affiliation

The surface oxygen vacancy concentration on ZnCeZrO composite oxides was finely tuned through modulating the preparation method and altering the precursor calcination temperature; the effect of the surface oxygen vacancy concentration on the performance of bifunctional ZnCeZrO/SAPO-34 catalysts in the direct conversion of syngas into light olefins (STO) was then investigated. The results indicate that the surface oxygen vacancy concentration of Zn_0.5CeZrO_x composite oxides can be markedly elevated by preparation through a sol–gel method with glucose as the complexing agent and calcination at 500 °C; a higher surface oxygen vacancy concentration leads to a higher space–time yield of methanol for syngas conversion over the Zn_0.5CeZrO_x oxide. When combined with SAPO-34 molecular sieves, the bifunctional Zn_0.5CeZrO_x/SAPO-34 catalyst with high surface oxygen vacancy concentration also exhibits a high space–time yield of light olefins (ethene to butenes) in the synthesis of olefins directly from syngas. With the help of in situ DRIFTS, it can be concluded that the surface oxygen vacancies on the ZnCeZrO oxide play an important role in the catalytic conversion of syngas. The abundant surface oxygen vacancies on Zn_0.5CeZrO_x can improve the formation of methanol-related intermediates from the syngas over the Zn_0.5CeZrO_x moiety, promote the evolution of these intermediates into the olefin products over the SAPO-34 moiety, and then enhance the overall capacity of the bifunctional Zn_0.5CeZrO_x/SAPO-34 composite catalyst in STO.

中文翻译：

在双功能ZnCeZrO / SAPO-34催化剂上将合成气转化为轻质烯烃：表面氧空位浓度的调节及其与催化性能的关系

通过调节制备方法和改变前驱体的煅烧温度，对ZnCeZrO复合氧化物表面的氧空位浓度进行了微调。然后研究了在合成气直接转化为轻质烯烃（STO）中表面氧空位浓度对双功能ZnCeZrO / SAPO-34催化剂性能的影响。结果表明，采用葡萄糖-络合剂溶胶-凝胶法制备并在500°C下煅烧，可以显着提高Zn _0.5 CeZrO _x复合氧化物的表面氧空位浓度。较高的表面氧空位浓度导致在Zn _0.5 CeZrO _x上用于合成气转化的甲醇的时空产率更高氧化物。当与SAPO-34分子筛结合使用时，具有高表面氧空位浓度的双功能Zn _0.5 CeZrO _x / SAPO-34催化剂在直接从合成气合成烯烃中也显示出高时空产率的轻质烯烃（乙烯到丁烯）。借助于原位DRIFTS，可以得出结论，ZnCeZrO氧化物的表面氧空位在合成气的催化转化中起重要作用。Zn _0.5 CeZrO _x上大量的表面氧空位可以改善合成气在Zn _0.5 CeZrO _x上与甲醇相关的中间体的形成部分，促进这些中间体在SAPO-34部分上演变为烯烃产物，然后提高STO中双功能Zn _0.5 CeZrO _x / SAPO-34复合催化剂的总容量。

更新日期：2020-11-16

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