Cation-exchanged zeolites for the selective oxidation of methane to methanol

Ambarish R. Kulkarni*, Zhi Jian Zhao, Samira Siahrostami, Jens K. Nørskov, Felix Studt

*Corresponding author for this work

Research output: Contribution to journalReviewResearchpeer-review

Abstract

Motivated by the increasing availability of cheap natural gas resources, considerable experimental and computational research efforts have focused on identifying selective catalysts for the direct conversion of methane to methanol. One promising class of catalysts are cation-exchanged zeolites, which have steadily increased in popularity over the past decade. In this article, we first present a broad overview of this field from a conceptual perspective, and highlight the role of theory in developing a molecular-level understanding of the reaction. Next, by performing and analyzing a large database of density functional theory (DFT) calculations for a wide range of transition metal cations, zeolite topologies and active site motifs, we present a unifying picture of the methane activation process in terms of active site stability, C-H bond activation and methanol extraction. Based on the trade-offs of active site stability and reactivity, we propose a framework for identifying new, promising active site motifs in these systems. Further, we show that the high methanol selectivity arises due to the strong binding nature of the C-H activation products. Finally, using the atomistic and mechanistic insight obtained from these analyses, we summarize the key challenges and future strategies for improving the performance of cation-exchanged zeolites for this industrially relevant conversion.

Original languageEnglish
JournalCatalysis Science and Technology
Volume8
Issue number1
Pages (from-to)114-123
ISSN2044-4753
DOIs
Publication statusPublished - 2018
Externally publishedYes

Cite this

Kulkarni, Ambarish R. ; Zhao, Zhi Jian ; Siahrostami, Samira ; Nørskov, Jens K. ; Studt, Felix. / Cation-exchanged zeolites for the selective oxidation of methane to methanol. In: Catalysis Science and Technology. 2018 ; Vol. 8, No. 1. pp. 114-123.
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abstract = "Motivated by the increasing availability of cheap natural gas resources, considerable experimental and computational research efforts have focused on identifying selective catalysts for the direct conversion of methane to methanol. One promising class of catalysts are cation-exchanged zeolites, which have steadily increased in popularity over the past decade. In this article, we first present a broad overview of this field from a conceptual perspective, and highlight the role of theory in developing a molecular-level understanding of the reaction. Next, by performing and analyzing a large database of density functional theory (DFT) calculations for a wide range of transition metal cations, zeolite topologies and active site motifs, we present a unifying picture of the methane activation process in terms of active site stability, C-H bond activation and methanol extraction. Based on the trade-offs of active site stability and reactivity, we propose a framework for identifying new, promising active site motifs in these systems. Further, we show that the high methanol selectivity arises due to the strong binding nature of the C-H activation products. Finally, using the atomistic and mechanistic insight obtained from these analyses, we summarize the key challenges and future strategies for improving the performance of cation-exchanged zeolites for this industrially relevant conversion.",
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Cation-exchanged zeolites for the selective oxidation of methane to methanol. / Kulkarni, Ambarish R.; Zhao, Zhi Jian; Siahrostami, Samira; Nørskov, Jens K.; Studt, Felix.

In: Catalysis Science and Technology, Vol. 8, No. 1, 2018, p. 114-123.

Research output: Contribution to journalReviewResearchpeer-review

TY - JOUR

T1 - Cation-exchanged zeolites for the selective oxidation of methane to methanol

AU - Kulkarni, Ambarish R.

AU - Zhao, Zhi Jian

AU - Siahrostami, Samira

AU - Nørskov, Jens K.

AU - Studt, Felix

PY - 2018

Y1 - 2018

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AB - Motivated by the increasing availability of cheap natural gas resources, considerable experimental and computational research efforts have focused on identifying selective catalysts for the direct conversion of methane to methanol. One promising class of catalysts are cation-exchanged zeolites, which have steadily increased in popularity over the past decade. In this article, we first present a broad overview of this field from a conceptual perspective, and highlight the role of theory in developing a molecular-level understanding of the reaction. Next, by performing and analyzing a large database of density functional theory (DFT) calculations for a wide range of transition metal cations, zeolite topologies and active site motifs, we present a unifying picture of the methane activation process in terms of active site stability, C-H bond activation and methanol extraction. Based on the trade-offs of active site stability and reactivity, we propose a framework for identifying new, promising active site motifs in these systems. Further, we show that the high methanol selectivity arises due to the strong binding nature of the C-H activation products. Finally, using the atomistic and mechanistic insight obtained from these analyses, we summarize the key challenges and future strategies for improving the performance of cation-exchanged zeolites for this industrially relevant conversion.

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JO - Catalysis Science & Technology

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SN - 2044-4753

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