Origin of the superior activity of surface doped SmMn2O5 mullites for NO oxidation: A first-principles based microkinetic study

Yang, Jixing; Zhang, Jie; Liu, Xiao; Duan, Xianbao; Wen, Yanwei; Chen, Rong; Shan, Bin

doi:10.1016/j.jcat.2018.01.002

Cited by 47 publications

(32 citation statements)

References 34 publications

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“…Clearly, such narrowly distributed surface O p-band centers are not capable of describing the trend in the chemisorption energies, as shown in Figure 2(c) and 2(f). catalytic activity in redox catalysis 42 , is correlated to the chemisorption energies. The…”

Section: Dft Calculationmentioning

confidence: 99%

Surface phase diagrams of La-based perovskites towards the O-rich limit from first principles

Yang

Zhu

et al. 2019

Phys. Chem. Chem. Phys.

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Section: Dft Calculationmentioning

confidence: 99%

Surface phase diagrams of La-based perovskites towards the O-rich limit from first principles

Yang

Zhu

et al. 2019

Phys. Chem. Chem. Phys.

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“…[ 74 ] On the mullite oxide surface, different mechanisms have been proposed. [ 38,71,75 ] The initial understanding was that NO oxidation reaction occurs via the Eley–Rideal (ER, Figure 5b) mechanism, under which oxygen molecules are dissociatively adsorbed on neighboring Mn 4+ –Mn 4+ dimers. Based on first‐principles calculations, Wang et al proposed that the adjacent Mn 4+ –Mn 4+ sites in octahedral units energetically prefer to adsorb O 2 compared with NO.…”

Section: Origin Of Catalytic Activity and Reaction Mechanismsmentioning

confidence: 99%

“…The release of the NO 2 gas molecule creates an oxygen vacancy site, which is replenished by the gas‐phase O 2 , regenerating the surface for the next cycle. [ 75 ]…”

Section: Origin Of Catalytic Activity and Reaction Mechanismsmentioning

confidence: 99%

“…Yang et al, using microkinetic analysis under realistic conditions, showed that surface doping of La, Ba, or Sr in SmMn 2 O 5 can promote mullite oxides’ activity: La doping lowers the MnO α bond strength in SmMn 2 O 5 , which is beneficial in creating oxygen vacancies, activating O 2 , and thus facilitating easy dissociation of reaction intermediates. [ 75 ] Furthermore, Feng et al demonstrated that La doping in the Sm site results in higher catalytic performance in La 0.3 Sm 0.7 Mn 2 O δ over pristine SmMn 2 O 5 . The light‐off temperature of La 0.3 Sm 0.7 Mn 2 O δ catalyst is lowered by 30 °C (220 °C vs 250 °C for pristine SmMn 2 O 5 ) and attained a maximum conversion efficiency of 85% at 290 °C with an activation energy of 36 kJ mol −1 .…”

Section: Strategies To Optimize the Catalytic Performance Of Mullite mentioning

confidence: 99%

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Earth‐Abundant Transition Metal‐Based Mullite‐Type Oxide Catalysts for Heterogeneous Oxidation Reactions

Thampy

Ashburn

Cho

et al. 2021

Adv Energy and Sustain Res

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Driving innovations in the field of catalysis and electrocatalysis for a sustainable future necessitates the development of highly active, thermally stable, and low‐cost heterogeneous catalysts. Earth‐abundant transition metal‐based oxide catalysts are highly sought after to replace expensive platinum group metals. Identifying new catalyst formulations and design principles to tune materials’ bulk electronic structures and surface energetics for enhanced catalytic activity accelerates the search. Herein, the inherent attributes of mullite‐type oxides in catalyzing various oxidation reactions—crystal structure, electronic structure, stability, and catalytic activity—are reviewed. A comprehensive understanding of the nature of active sites, oxidation mechanisms, strategies to enhance the catalytic performance and regeneration of active sites, emerging opportunities in electrocatalysis and sensors, and challenges in computational methodologies is discussed. Finally, a perspective on expanding mullite‐type oxides’ viability for commercial applications in environmental and sustainable energy production through the integration of advanced synthetic approaches, operando spectroscopic techniques, and high‐throughput computational tools is outlined.

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“…This is in good agreement with surface studies for each material. [15][16][17] Although the NO adsorption-desorption process for CeO2 was only observed on the (100) surface, both the (111) and (110) surfaces were also considered since they are known stable surfaces. However, these surfaces proved to have a weak affinity for NO binding.…”

Section: Temperature Programmed Desorptionmentioning

confidence: 99%

Integrated Experimental–Theoretical Approach To Determine Reliable Molecular Reaction Mechanisms on Transition-Metal Oxide Surfaces

Ashburn

Zheng

Thampy

et al. 2019

ACS Appl. Mater. Interfaces

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By combining experimental and theoretical approaches, we investigate the quantitative relationship between molecular desorption temperature and binding energy on d and f metal oxide surfaces. We demonstrate how temperature programmed desorption (TPD) can be used to quantitatively correlate the theoretical surface chemistry of metal oxides (via on-site Hubbard U correction) to gas surface interactions for catalytic reactions. For this purpose, both CO and NO oxidation mechanisms are studied in a step by step reaction process for perovskite and mullite-type oxides, respectively. Additionally, we show solutions for over-binding issues found in COx, NOx, SOx, and other covalently bonded molecules which must be considered during surface reaction modeling. This work shows the high reliability of using TPD and density functional theory (DFT) in conjunction to create accurate surface chemistry information for a variety of correlated metal oxide materials.

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Origin of the superior activity of surface doped SmMn2O5 mullites for NO oxidation: A first-principles based microkinetic study

Cited by 47 publications

References 34 publications

Surface phase diagrams of La-based perovskites towards the O-rich limit from first principles

Surface phase diagrams of La-based perovskites towards the O-rich limit from first principles

Earth‐Abundant Transition Metal‐Based Mullite‐Type Oxide Catalysts for Heterogeneous Oxidation Reactions

Integrated Experimental–Theoretical Approach To Determine Reliable Molecular Reaction Mechanisms on Transition-Metal Oxide Surfaces

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