Near 100% CO selectivity in nanoscaled iron-based oxygen carriers for chemical looping methane partial oxidation

被引：120

作者：

Liu, Yan ^{[1
]}

Qin, Lang ^{[1
]}

Cheng, Zhuo ^{[1
]}

Goetze, Josh W. ^{[1
]}

Kong, Fanhe ^{[1
]}

Fan, Jonathan A. ^{[2
]}

Fan, Liang-Shih ^{[1
]}

机构：

[1] Ohio State Univ, Dept Chem & Biomol Engn, 151W Woodruff Ave, Columbus, OH 43210 USA

[2] Stanford Univ, Dept Elect Engn, Ginzton Lab, Spilker Engn & Appl Sci, 348 Via Pueblo Mall, Stanford, CA 94305 USA

来源：

NATURE COMMUNICATIONS | 2019年 / 10卷 / 1期

关键词：

TOTAL-ENERGY CALCULATIONS; MESOPOROUS SILICA; METALS;

D O I：

10.1038/s41467-019-13560-0

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

Chemical looping methane partial oxidation provides an energy and cost effective route for methane utilization. However, there is considerable CO2 co-production in current chemical looping systems, rendering a decreased productivity in value-added fuels or chemicals. In this work, we demonstrate that the co-production of CO2 can be dramatically suppressed in methane partial oxidation reactions using iron oxide nanoparticles embedded in mesoporous silica matrix. We experimentally obtain near 100% CO selectivity in a cyclic redox system at 750-935 degrees C, which is a significantly lower temperature range than in conventional oxygen carrier systems. Density functional theory calculations elucidate the origins for such selectivity and show that low-coordinated lattice oxygen atoms on the surface of nanoparticles significantly promote Fe-O bond cleavage and CO formation. We envision that embedded nanostructured oxygen carriers have the potential to serve as a general materials platform for redox reactions with nanomaterials at high temperatures.

引用

页数：6