Fabricating Ga doped and MgO embedded nanomaterials for sorption-enhanced steam reforming of methanol

Zhao Sun, Junpeng Liu, Rongjun Zhang, Yu Wu, Hongwei Li, Sam Toan, Zhiqiang Sun

Research output: Contribution to journalArticlepeer-review

14 Scopus citations

Abstract

Sorption-enhanced steam reforming of methanol (SE-SRM) is a promising approach to creating a high-purity hydrogen supply. However, catalysts suffer from activity deactivation and low CO2 uptake capacity. In this study, we investigate the role of Ga doping of Cu-MgO in SE-SRM by synthesizing a series of MgO embedded xGaCuMg catalytic sorbents via a sol-gel method. The TEM-EDX mapping results indicate that MgO nanoparticles can be successfully embedded in the bulk-phase of the catalytic sorbent with a stabilized microstructure. The results from in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) reveal that the Ga-doped catalytic sorbent is conducive to promoting the conversion of C-containing intermediates in SE-SRM, and absorbing CO2 in the form of bidentate carbonate rather than monodentate carbonate. Experimental studies verify that the best uptake capacity of 18GaCuMg catalytic sorbent (36.25 mg CO2/g MgO) achieves almost complete conversion of methanol (99.70%) with 100% H2 selectivity at 200 °C. Specifically, no CO is formed during the kinetic-control stage of SE-SRM. Density functional theory (DFT) calculations based on the Cu(111)Ga2O3(202)MgO(200) model revealed that the Ga doping can enhance the adsorption energies of methanol and carbon dioxide, promoting methanol activation and increasing CO2 uptake capacity. These findings provide valid strategies for functionalized nanomaterial design, which will substantially promote the SE-SRMR performance with desired catalytic sorbent recyclability.

Original languageEnglish (US)
Pages (from-to)7300-7313
Number of pages14
JournalJournal of Materials Chemistry A
Volume10
Issue number13
DOIs
StatePublished - Feb 16 2022

Bibliographical note

Funding Information:
This work was supported by the National Natural Science Foundation of China (52106193 and 51876224), the Natural Science Foundation of Hunan Province (2021JJ40756), the State Key Laboratory of Catalytic Materials and Reaction Engineering (RIPP and SINOPEC), the Science and Technology Innovation Program of Hunan Province (2020GK2070 and 2021RC4006), and the Innovation-Driven Project of Central South University (2020CX008, 2021zzts0655 and CX20210228).

Publisher Copyright:
© 2022 The Royal Society of Chemistry

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