Surface Structure Dependent Activation of Hydrogen over Metal Oxides During Syngas Conversion

Overview

Journal J Am Chem Soc

Publisher American Chemical Society

Specialty Chemistry

Date 2024 Dec 2

PMID 39620729

Authors

Bing Bai

Yihan Ye

Feng Jiao

Jianping Xiao

Yang Pan

Zehua Cai

Mingshu Chen

Xiulian Pan

Xinhe Bao

Affiliations

Soon will be listed here.

Abstract

Despite the extensive studies on the adsorption and activation of hydrogen over metal oxides, it remains a challenge to investigate the structure-dependent activation of hydrogen and its selectivity mechanism in hydrogenation reactions. Herein we take spinel and solid solution MnGaO with a similar bulk chemical composition and study the hydrogen activation mechanism and reactivity in syngas conversion. The results show that MnGaO-Solid Solution (MnGaO-SS) is a typical Mn-doped hexagonal close-packed (HCP) GaO with a Ga-rich surface. Upon exposure to hydrogen, Ga-H and O-H species are simultaneously generated. Ga-H species are highly active but unselective in CO activation, forming CHO, and ethylene hydrogenation, forming ethane. In contrast, MnGaO-Spinel is a face-centered-cubic (FCC) spinel phase featuring a Mn-rich surface, thus effectively suppressing the formation of Ga-H species. Interestingly, only part of the O-H species are active for CO activation while the O-H species are inert for olefin hydrogenation over MnGaO-Spinel. Therefore, MnGaO-Spinel exhibits a higher activity and higher light-olefin selectivity than MnGaO-SS in combination with SAPO-18 during syngas conversion. These fundamental understandings are essential to guide the design and further optimization of metal oxide catalysts for selectivity control in hydrogenations.

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