Simplifying computational workflows with the Multiscale Atomic Zeolite Simulation Environment (MAZE)

Antonio, Dexter; Guo, Jiawei; Holton, Sam; Kulkarni, Ambarish

doi:10.1016/j.softx.2021.100797

Cited by 6 publications

(5 citation statements)

References 15 publications

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“…These motifs are labeled according to the valence state and site geometry: Cr 2+ for divalent chromium, Cr 3+ for trivalent chromium, Cr 6+ O for hexavalent chromium with one CrO double bond, and Cr 6+ OO for tetrahedral hexavalent chromium with two CrO double bonds. Taking all 12 unique T-sites in the MFI framework and the possible variations of the same chromium site motif on a single T-site into account, a comprehensive library of chromium structures was generated using the MAZE package . Note that this approach inherently assumes that all of the chromium atoms occupy identical sites in the framework; accounting for the contributions from possible site heterogeneities is beyond the scope of this analysis.…”

Section: Resultsmentioning

confidence: 99%

Reduction of Cofed Carbon Dioxide Modifies the Local Coordination Environment of Zeolite-Supported, Atomically Dispersed Chromium to Promote Ethane Dehydrogenation

Zhou,

Felvey,

Guo

et al. 2024

J. Am. Chem. Soc.

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The reduction of CO 2 is known to promote increased alkene yields from alkane dehydrogenations when the reactions are cocatalyzed. The mechanism of this promotion is not understood in the context of catalyst active-site environments because CO 2 is amphoteric, and even general aspects of the chemistry, including the significance of competing side reactions, differ significantly across catalysts. Atomically dispersed chromium cations stabilized in highly siliceous MFI zeolite are shown here to enable the study of the role of parallel CO 2 reduction during ethylene-selective ethane dehydrogenation. Based on infrared spectroscopy and X-ray absorption spectroscopy data interpreted through calculations using density functional theory (DFT), the synthesized catalyst contains atomically dispersed Cr cations stabilized by silanol nests in micropores. Reactor studies show that cofeeding CO 2 increases stable ethylene-selective ethane dehydrogenation rates over a wide range of partial pressures. Operando X-ray absorption near-edge structure (XANES) and extended X-ray absorption fine-structure (EXAFS) spectra indicate that during reaction at 650 °C the Cr cations maintain a nominal 2+ charge and a total Cr−O coordination number of approximately 2. However, CO 2 reduction induces a change, correlated with the CO 2 partial pressure, in the population of two distinct Cr−O scattering paths. This indicates that the promotional effect of parallel CO 2 reduction can be attributed to a subtle change in Cr−O bond lengths in the local coordination environment of the active site. These insights are made possible by simultaneously fitting multiple EXAFS spectra recorded in different reaction conditions; this novel procedure is expected to be generally applicable for interpreting operando catalysis EXAFS data.

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Section: Resultsmentioning

confidence: 99%

Reduction of Cofed Carbon Dioxide Modifies the Local Coordination Environment of Zeolite-Supported, Atomically Dispersed Chromium to Promote Ethane Dehydrogenation

Zhou,

Felvey,

Guo

et al. 2024

J. Am. Chem. Soc.

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“…This method begins by creating an exhaustive database of DFT-optimized structures that can be used to model the experimental EXAFS. , While uniform atomically dispersed catalysts are more amenable to analysis by QuantEXAFS, this approach has been extended to more complex systems such as Pt/ZSM-5 . The latter study is particularly interesting due to the complexity of the zeolite support; the authors use a zeolite-specific simulation codebase to enumerate all possible bonding sites of Pt 2+ and [Pt–OH] 1+ species in the MFI topology. Although questions about the uniformity of the proposed Pt 2+ site remain open, a key advantage of QuantEXAFS is the ability to compare the modeled EXAFS spectra of different types of sites (e.g., all possible Pt 2+ vs all possible [PtOH] 1+ ) rather than only considering a few plausible configurations.…”

Section: How Is Exafs Being Currently Used By the Catalysis Science C...mentioning

confidence: 99%

Bridging the Gap between the X-ray Absorption Spectroscopy and the Computational Catalysis Communities in Heterogeneous Catalysis: A Perspective on the Current and Future Research Directions

et al. 2022

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X-ray absorption spectroscopy (XAS) [extended X-ray absorption fine structure (EXAFS) and X-ray absorption near-edge structure (XANES)] is a key technique within the heterogeneous catalysis community to probe the structure and properties of the active site(s) for a diverse range of catalytic materials. However, the interpretation of the raw experimental data to derive an atomistic picture of the catalyst requires modeling and analysis; the EXAFS data are compared to a model, and a goodness of fit parameter is used to judge the best fit. This EXAFS modeling can often be nontrivial and time-consuming; overcoming or improving these limitations remains a central challenge for the community. Considering these limitations, this Perspective highlights how recent developments in analysis software, increased availability of reliable computational models, and application of data science tools can be used to improve the speed, accuracy, and reliability of EXAFS interpretation. In particular, we emphasize the advantages of combining theory and EXAFS as a unified technique that should be treated as a standard (when applicable) to identify catalytic sites and not two separate complementary methods. Building on the recent trends in the computational catalysis community, we also present a community-driven approach to adopt FAIR Guiding Principles for the collection, analysis, dissemination, and storage of XAS data. Written with both the experimental and theory audience in mind, we provide a unified roadmap to foster collaborations between the two communities.

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“…98,99 While uniform atomically dispersed catalysts are more amenable by QuantEXAFS, this approach has been extended to more complex systems such as Pt/ZSM-5. 101 The latter study is particularly interesting due to the complexity of the zeolite support; the authors use a zeolite-specific simulation codebase 102 to enumerate all possible bonding sites of Pt 2+ and [Pt-OH] 1+ species in the MFI topology. Although questions about the uniformity of the proposed Pt 2+ site remain open, a key advantage of QuantEXAFS is the ability to compare the modeled EXAFS spectra of different types of sites (e.g., all possible Pt 2+ vs. all possible…”

Section: Categorymentioning

confidence: 99%

Bridging the Gap between the X-ray Absorption Spectroscopy and the Computational Catalysis Communities in Heterogeneous Catalysis: A Perspective on the Current and Future Research Directions

Rana

Vila

Kulkarni

et al. 2022

Preprint

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X-ray absorption spectroscopy (XAS), (Extended X-ray Absorption Fine Structure (EXAFS) and X-ray Absorption Near-Edge Structure (XANES)), is a key technique within the heterogeneous catalysis community to probe the structure and properties of active site(s) for a diverse range of catalytic materials. However, the interpretation of the raw experimental data to derive an atomistic picture of the catalyst requires modeling and analysis; the EXAFS data are compared to a model and a goodness of fit parameter is used to judge the best fit. This EXAFS modeling can often be non-trivial and time-consuming; overcoming or improving these limitations remains a central challenge for the community. Considering these limitations, this Perspective highlights how recent developments in analysis software, increased availability of reliable computational models and application of data science tools can be used to improve the speed, accuracy, and reliability of EXAFS interpretation. In particular, we emphasize the advantages of combining theory and EXAFS as a unified technique that should be treated as a standard (when applicable) to identify catalytic sites and not two separate complementary methods. Building on the recent trends in the computational catalysis community, we also present a community-driven approach to adopt FAIR Guiding Principles for the collection, analysis, dissemination, and storage of XAS data. Written with both the experimental and theory audience in mind, we provide unified roadmap to foster collaborations between the two communities.

show abstract

Simplifying computational workflows with the Multiscale Atomic Zeolite Simulation Environment (MAZE)

Cited by 6 publications

References 15 publications

Reduction of Cofed Carbon Dioxide Modifies the Local Coordination Environment of Zeolite-Supported, Atomically Dispersed Chromium to Promote Ethane Dehydrogenation

Reduction of Cofed Carbon Dioxide Modifies the Local Coordination Environment of Zeolite-Supported, Atomically Dispersed Chromium to Promote Ethane Dehydrogenation

Bridging the Gap between the X-ray Absorption Spectroscopy and the Computational Catalysis Communities in Heterogeneous Catalysis: A Perspective on the Current and Future Research Directions

Bridging the Gap between the X-ray Absorption Spectroscopy and the Computational Catalysis Communities in Heterogeneous Catalysis: A Perspective on the Current and Future Research Directions

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