Neutron Scattering Studies of Heterogeneous Catalysis

Yu, Xinbin; Cheng, Yongqiang; Li, Yuanyuan; Polo-Garzon, Felipe; Liu, Jue; Mamontov, Eugene; Li, Meijun; Lennon, David; Parker, Stewart F.; Ramirez-Cuesta, Anibal J.; Wu, Zili

doi:10.1021/acs.chemrev.3c00101

Cited by 15 publications

(8 citation statements)

References 470 publications

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“…The molecular diffusion within the zeolite pores is an important influence on the efficacy of catalytic reactions and neutron scattering techniques, with their sensitivity to hydrogen, can be important probes of the dynamics of the diffusing species. In the study of Matam et al [ 10 ] Quasi Elastic Neutron Scattering (QENS) [ 11 , 12 ] is used to determine the diffusion of methanol in a series of zeolites at different temperatures is outlined. The zeolite catalyst studied, ZSM-5, is important in methanol to hydrocarbon (MTH) reactions and understanding the diffusion of methanol in these materials is accordingly both environmentally and commercially important since alternative methods of producing gasoline, olefins, and aromatics without relying on fossil fuels are key in achieving net zero carbon emission targets.…”

Section: Prefacementioning

confidence: 99%

“…QENS data have been acquired at the ISIS neutron source for different ZSM-5 zeolites which have different Si/Al ratios, and the results are compared with those from molecular dynamics simulations which probe similar timescales. The different Si/Al ratios determine the number of Brønsted acid sites which strongly influence methanol diffusion [ 11 , 12 ]. As the Si/Al ratio is increased, the fraction of mobile methanol increases and the nature of the methanol dynamics also changes from rotational to translational diffusion.…”

Section: Prefacementioning

confidence: 99%

See 1 more Smart Citation

Exploring the length scales, timescales and chemistry of challenging materials (Part 2)

Wilding,

Sella,

Howard

et al. 2023

Phil. Trans. R. Soc. A.

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This themed issue explores the different length and timescales that determine the physics and chemistry of a variety of key of materials, explored from the perspective of a wide range of disciplines, including physics, chemistry materials science, Earth science and biochemistry. The topics discussed include catalysis, chemistry under extreme conditions, energy materials, amorphous and liquid structure, hybrid organic materials and biological materials. The issue is in two parts, with this second set of contributions exploring hybrid organic materials, catalysis low-dimensional and graphitic materials, biological materials and naturally occurring, super-hard material as well as dynamic high pressure and new developments in imaging techniques pressure. This article is part of the theme issue 'Exploring the length scales, timescales and chemistry of challenging materials (Part 2)'.

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Section: Prefacementioning

confidence: 99%

Section: Prefacementioning

confidence: 99%

Exploring the length scales, timescales and chemistry of challenging materials (Part 2)

Wilding,

Sella,

Howard

et al. 2023

Phil. Trans. R. Soc. A.

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“…Accordingly, in this work we performed in-situ small-angle neutron scattering (SANS), adopting the set-up from Randle et al 41 and Draper. 42 Neutron beams interact differently to matter compared to X-ray beams, 43 which leads to intrinsic differences in values of scattering length density (SLD) for neutrons compared to X-rays. 44 With appropriate contrast-matching, some features that might be concealed in X-ray scattering could be revealed under SANS.…”

Section: Introductionmentioning

confidence: 99%

Development of Robust Redox-Active Lyotropic Liquid Crystal Structures for Bioelectrodes

Liu,

Hann,

White

et al. 2024

Preprint

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The fabrication of stable and highly performing enzyme-based electrodes is key for the effective generation of biodevices and bioelectronics, such as electrochemical biosensors. In this context, redox-active lyotropic liquid crystals based on 3D nanomaterials, known as lipid cubic phases (LCP), hold great potential due to the large specific surface area and the possibility to be functionalized. In this study, we functionalized a monoolein (MO) LCP matrix by incorporating an amphiphilic redox shuttle within its matrix with the aim to enhance the electrochemical performance of a glucose oxidase (GOx) based electrode and we investigated the stability of the overall system. The use of dodecyl(ferrocenylmethyl)dimethylammonium bromide (Fc12-Br) resulted in an electroactivity loss with time of the resulting Fc12-Br/MO electrode, probably due to the formation of a passivating layer between the bromide counterions and the electrode surface. Hence, bromine (Br-) was replaced with hexafluorophosate (PF6-), leading to Fc12-PF6/MO. Both structures were used for GOx entrapment and the resulting electro-activity towards glucose was assessed. Though the sensitivity obtained with the Fc12-Br/MO/GOx and Fc12-PF6/MO/GOx systems was comparable, the latter showed superior stability over time, with more than 80% activity retained for > 20 days. Moreover, when the concentration of the Fc12 redox shuttle within the cubic phase was increased by 10, a 4 times greater current density was generated. Consequently, the Fc12-PF6/MO electrode shows superior stability and performance than previously reported redox lyotropic LCP systems, thus paving the way for promising applications in enzyme-based biodevices.

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“…The relevance of INS spectroscopy in catalysis is highlighted by several papers and reviews on the topic that have been published in the last years, such as the very broad review recently written by Yu et al covering the main applications of neutron techniques in catalysis, [23] and the one written by Polo-Garzon et al summarized the findings related to the species formed upon interaction with H 2 of supported metal nanoparticles and oxides. [24] Indeed, the INS spectra of a catalyst collected under different environmental conditions can very often provide a very broad range of details related to different aspects of its physico-chemical nature and of its interaction with reactants.…”

Section: Introductionmentioning

confidence: 99%

Supported Metal Nanoparticles‐Based Catalysts and their Interactions with H₂: Insights from Inelastic Neutron Scattering Spectroscopy

Vottero,

Groppo,

Piovano

2023

ChemCatChem

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The investigation of supported metal nanoparticle in the presence of H2 is fundamental to better understand their behavior as hydrogenation catalysts. In this respect, this review will focus on the main recent results obtained by Inelastic Neutron Scattering (INS) spectroscopy, which is of particular interest thanks to its ability to provide very detailed vibrational spectra of the H‐containing species in the sample. The review will cover the main results concerning the characterization of the H‐species already present in the pristine catalyst, with a particular focus on carbon‐based materials and their modification upon the interaction with metal nanoparticles. Successively, the forms in which H2 interacts with the catalysts will be examined, starting from H2 physisorption, to then pass to the metal hydride species formed through the splitting of dihydrogen upon the active metallic phase, and finally to the migration of atomic hydrogen from the metal nanoparticles onto the support as a result of hydrogen spillover. The aim of the review is to present an overview of all the hydrogenous species identifiable by INS spectroscopy in hydrogenation catalysts, focusing on the specific case of supported metal nanoparticles systems.

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Neutron Scattering Studies of Heterogeneous Catalysis

Abstract: Published as part of the Chemical Reviews virtual special issue "Operando and In Situ Studies in Catalysis and Electrocatalysis".

Cited by 15 publications

References 470 publications

Exploring the length scales, timescales and chemistry of challenging materials (Part 2)

Exploring the length scales, timescales and chemistry of challenging materials (Part 2)

Development of Robust Redox-Active Lyotropic Liquid Crystal Structures for Bioelectrodes

Supported Metal Nanoparticles‐Based Catalysts and their Interactions with H₂: Insights from Inelastic Neutron Scattering Spectroscopy

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Neutron Scattering Studies of Heterogeneous Catalysis

Abstract: Published as part of the Chemical Reviews virtual special issue "Operando and In Situ Studies in Catalysis and Electrocatalysis".

Cited by 15 publications

References 470 publications

Exploring the length scales, timescales and chemistry of challenging materials (Part 2)

Exploring the length scales, timescales and chemistry of challenging materials (Part 2)

Development of Robust Redox-Active Lyotropic Liquid Crystal Structures for Bioelectrodes

Supported Metal Nanoparticles‐Based Catalysts and their Interactions with H2: Insights from Inelastic Neutron Scattering Spectroscopy

Contact Info

Product

Resources

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Supported Metal Nanoparticles‐Based Catalysts and their Interactions with H₂: Insights from Inelastic Neutron Scattering Spectroscopy