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Article: Spectroscopy Identification of the Bimetallic Surface of Metal–Organic Framework-Confined Pt–Sn Nanoclusters with Enhanced Chemoselectivity in Furfural Hydrogenation

Goh, Tian Wei / Huang, Wenyu / Tsung, Chia-Kuang

ACS applied materials & interfaces. 2019 June 07, v. 11, no. 26

2019

Abstract: Research and development in bimetallic nanoparticles have gained great interest over their monometallic counterparts because of their distinct and unique properties in a wide range of applications such as catalysis, energy storage, and bio/plasmonic ... ...

Abstract	Research and development in bimetallic nanoparticles have gained great interest over their monometallic counterparts because of their distinct and unique properties in a wide range of applications such as catalysis, energy storage, and bio/plasmonic imaging. Identification and characterization of these bimetallic surfaces for application in heterogeneous catalysis remain a challenge and heavily rely on advanced characterization techniques such as aberration-corrected electron microscopy and synchrotron X-ray absorption studies. In this article, we have reported a strategy to prepare sub-2 nm bimetallic Pt–Sn nanoclusters confined in the pores of a Zr-based metal–organic framework (MOF). The Pt–Sn nanoclusters encapsulated in the Zr-MOF pores show enhanced chemoselectivity from 51 to 93% in an industrially relevant reaction, furfural hydrogenation to furfuryl alcohol. The presence of bimetallic Pt–Sn surfaces was investigated by a surface-sensitive characterization technique utilizing diffuse reflectance infrared Fourier transform spectroscopy of adsorbed CO to probe the bimetallic surface of the encapsulated ultrafine Pt–Sn nanocluster. Complementary techniques such as aberration-corrected high-angle annular dark-field scanning transmission electron microscopy with energy-dispersive X-ray spectroscopy and X-ray photoelectron spectroscopy were also used to characterize the Pt–Sn nanoclusters.
Keywords	catalytic activity ; chemoselectivity ; coordination polymers ; encapsulation ; energy ; energy-dispersive X-ray analysis ; Fourier transform infrared spectroscopy ; furfural ; furfuryl alcohol ; hydrogenation ; image analysis ; nanoparticles ; research and development ; transmission electron microscopy ; X-ray absorption spectroscopy ; X-ray photoelectron spectroscopy
Language	English
Dates of publication	2019-0607
Size	p. 23254-23260.
Publishing place	American Chemical Society
Document type	Article
ISSN	1944-8252
DOI	10.1021/acsami.9b06229
Database	NAL-Catalogue (AGRICOLA)

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Article ; Online: Spectroscopy Identification of the Bimetallic Surface of Metal-Organic Framework-Confined Pt-Sn Nanoclusters with Enhanced Chemoselectivity in Furfural Hydrogenation.

Goh, Tian Wei / Tsung, Chia-Kuang / Huang, Wenyu

ACS applied materials & interfaces

2019 Volume 11, Issue 26, Page(s) 23254–23260

Abstract	Research and development in bimetallic nanoparticles have gained great interest over their monometallic counterparts because of their distinct and unique properties in a wide range of applications such as catalysis, energy storage, and bio/plasmonic imaging. Identification and characterization of these bimetallic surfaces for application in heterogeneous catalysis remain a challenge and heavily rely on advanced characterization techniques such as aberration-corrected electron microscopy and synchrotron X-ray absorption studies. In this article, we have reported a strategy to prepare sub-2 nm bimetallic Pt-Sn nanoclusters confined in the pores of a Zr-based metal-organic framework (MOF). The Pt-Sn nanoclusters encapsulated in the Zr-MOF pores show enhanced chemoselectivity from 51 to 93% in an industrially relevant reaction, furfural hydrogenation to furfuryl alcohol. The presence of bimetallic Pt-Sn surfaces was investigated by a surface-sensitive characterization technique utilizing diffuse reflectance infrared Fourier transform spectroscopy of adsorbed CO to probe the bimetallic surface of the encapsulated ultrafine Pt-Sn nanocluster. Complementary techniques such as aberration-corrected high-angle annular dark-field scanning transmission electron microscopy with energy-dispersive X-ray spectroscopy and X-ray photoelectron spectroscopy were also used to characterize the Pt-Sn nanoclusters.
Language	English
Publishing date	2019-06-19
Publishing country	United States
Document type	Journal Article
ISSN	1944-8252
ISSN (online)	1944-8252
DOI	10.1021/acsami.9b06229
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: The impact of synthetic method on the catalytic application of intermetallic nanoparticles.

Williams, Benjamin P / Qi, Zhiyuan / Huang, Wenyu / Tsung, Chia-Kuang

Nanoscale

2020 Volume 12, Issue 36, Page(s) 18545–18562

Abstract: Intermetallic alloy nanocrystals have emerged as a promising next generation of nanocatalyst, largely due to their promise of surface tunability. Atomic control of the geometric and electronic structure of the nanoparticle surface offers a precise ... ...

Abstract	Intermetallic alloy nanocrystals have emerged as a promising next generation of nanocatalyst, largely due to their promise of surface tunability. Atomic control of the geometric and electronic structure of the nanoparticle surface offers a precise command of the catalytic surface, with the potential for creating homogeneous active sites that extend over the entire nanoparticle. Realizing this promise, however, has been limited by synthetic difficulties, imparted by differences in parent metal crystal structure, reduction potential, and atomic size. Further, little attention has been paid to the impact of synthetic method on catalytic application. In this review, we seek to connect the two, organizing the current synthesis methods and catalytic scope of intermetallic nanoparticles and suggesting areas where more work is needed. Such analysis should help to guide future intermetallic nanoparticle development, with the ultimate goal of generating precisely controlled nanocatalysts tailored to catalysis.
Language	English
Publishing date	2020-09-03
Publishing country	England
Document type	Journal Article
ZDB-ID	2515664-0
ISSN	2040-3372 ; 2040-3364
ISSN (online)	2040-3372
ISSN	2040-3364
DOI	10.1039/d0nr04699j
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Engineering Second Sphere Interactions in a Host-Guest Multicomponent Catalyst System for the Hydrogenation of Carbon Dioxide to Methanol.

Rayder, Thomas M / Bensalah, Adam T / Li, Banruo / Byers, Jeffery A / Tsung, Chia-Kuang

Journal of the American Chemical Society

2021 Volume 143, Issue 3, Page(s) 1630–1640

Abstract: Many enzymes utilize interactions extending beyond the primary coordination sphere to enhance catalyst activity and/or selectivity. Such interactions could improve the efficacy of synthetic catalyst systems, but the supramolecular assemblies employed by ... ...

Abstract	Many enzymes utilize interactions extending beyond the primary coordination sphere to enhance catalyst activity and/or selectivity. Such interactions could improve the efficacy of synthetic catalyst systems, but the supramolecular assemblies employed by biology to incorporate second sphere interactions are challenging to replicate in synthetic catalysts. Herein, a strategy is reported for efficiently manipulating outer-sphere influence on catalyst reactivity by modulating host-guest interactions between a noncovalently encapsulated transition-metal-based catalyst guest and a metal-organic framework (MOF) host. This composite consists of a ruthenium PNP pincer complex encapsulated in the MOF UiO-66 that is used in tandem with the zirconium oxide nodes of UiO-66 and a ruthenium PNN pincer complex to hydrogenate carbon dioxide to methanol. Due to the method used to incorporate the complexes in UiO-66, structure-activity relationships could be efficiently determined using a variety of functionalized UiO-66-X hosts. These investigations uncovered the beneficial effects of the ammonium functional group (i.e., UiO-66-NH
Language	English
Publishing date	2021-01-19
Publishing country	United States
Document type	Journal Article ; Research Support, U.S. Gov't, Non-P.H.S.
ZDB-ID	3155-0
ISSN	1520-5126 ; 0002-7863
ISSN (online)	1520-5126
ISSN	0002-7863
DOI	10.1021/jacs.0c08957
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article: Molecular-Level Insights into Selective Transport of Mg²⁺ in Metal–Organic Frameworks

Wang, Yang / Luo, Tongtong / Li, Yang / Wang, Ailun / Wang, Dunwei / Bao, Junwei Lucas / Mohanty, Udayan / Tsung, Chia-Kuang

ACS applied materials & interfaces. 2021 July 30, v. 13, no. 44

2021

Abstract: Metal–organic frameworks (MOF) are promising media for achieving solid-state Mg²⁺ conduction and developing a magnesium-based battery. To this end, the chemical behavior and transport properties of an Mg(TFSI)₂/DME electrolyte system inside Mg-MOF-74 ... ...

Abstract	Metal–organic frameworks (MOF) are promising media for achieving solid-state Mg²⁺ conduction and developing a magnesium-based battery. To this end, the chemical behavior and transport properties of an Mg(TFSI)₂/DME electrolyte system inside Mg-MOF-74 were studied by density functional theory (DFT). We found that inside the MOF chemical environment, solvent and anion molecules occupy the coordinatively unsaturated open metal sites of Mg-MOF-74, while Mg²⁺ ions adsorb directly onto the carboxylate group of the MOF organic linker. These predicted binding geometries were further corroborated by IR spectroscopy. We computed the free energies of desolvation of Mg²⁺ ions inside MOF to investigate the capacity of Mg-MOF-74 thin film to act as a separator for selective Mg²⁺ transport. We showed that Mg-MOF-74 could facilitate partial, but not full, desolvation of Mg²⁺. We found that the dominant minimum-energy pathway (MEP) for Mg²⁺ conduction inside Mg-MOF-74 corresponds to a “solvent hopping” mechanism, with an energy barrier of 4.4 kcal/mol. The molar conductivity of Mg²⁺ associated with the idealized solvent hopping mechanism along the MOF one-dimensional channel was predicted to be 2.4 × 10–³ S cm–¹ M–¹, which is one to two orders of magnitude greater than the experimentally measured value of 1.2 × 10–⁴ S cm–¹ M–¹ (with an estimated Mg²⁺ concentration). We have discussed several possible factors contributing to this apparent discrepancy. The current work demonstrates the validity of the computational strategies applied and the structural models constructed for the understanding of fast and selective Mg²⁺ transport in Mg-MOF-74, which serves as a cornerstone for studying transport of multivalent ions in MOFs. Furthermore, it provides detailed molecular-level insights that are not yet accessible experimentally.
Keywords	batteries ; density functional theory ; energy ; films (materials) ; infrared spectroscopy ; physicochemical properties ; solvents
Language	English
Dates of publication	2021-0730
Size	p. 51974-51987.
Publishing place	American Chemical Society
Document type	Article
ISSN	1944-8252
DOI	10.1021/acsami.1c08392
Database	NAL-Catalogue (AGRICOLA)

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Article ; Online: Hierarchically encapsulating enzymes with multi-shelled metal-organic frameworks for tandem biocatalytic reactions.

Man, Tiantian / Xu, Caixia / Liu, Xiao-Yuan / Li, Dan / Tsung, Chia-Kuang / Pei, Hao / Wan, Ying / Li, Li

Nature communications

2022 Volume 13, Issue 1, Page(s) 305

Abstract: Biocatalytic transformations in living organisms, such as multi-enzyme catalytic cascades, proceed in different cellular membrane-compartmentalized organelles with high efficiency. Nevertheless, it remains challenging to mimicking biocatalytic cascade ... ...

Abstract	Biocatalytic transformations in living organisms, such as multi-enzyme catalytic cascades, proceed in different cellular membrane-compartmentalized organelles with high efficiency. Nevertheless, it remains challenging to mimicking biocatalytic cascade processes in natural systems. Herein, we demonstrate that multi-shelled metal-organic frameworks (MOFs) can be used as a hierarchical scaffold to spatially organize enzymes on nanoscale to enhance cascade catalytic efficiency. Encapsulating multi-enzymes with multi-shelled MOFs by epitaxial shell-by-shell overgrowth leads to 5.8~13.5-fold enhancements in catalytic efficiencies compared with free enzymes in solution. Importantly, multi-shelled MOFs can act as a multi-spatial-compartmental nanoreactor that allows physically compartmentalize multiple enzymes in a single MOF nanoparticle for operating incompatible tandem biocatalytic reaction in one pot. Additionally, we use nanoscale Fourier transform infrared (nano-FTIR) spectroscopy to resolve nanoscale heterogeneity of vibrational activity associated to enzymes encapsulated in multi-shelled MOFs. Furthermore, multi-shelled MOFs enable facile control of multi-enzyme positions according to specific tandem reaction routes, in which close positioning of enzyme-1-loaded and enzyme-2-loaded shells along the inner-to-outer shells could effectively facilitate mass transportation to promote efficient tandem biocatalytic reaction. This work is anticipated to shed new light on designing efficient multi-enzyme catalytic cascades to encourage applications in many chemical and pharmaceutical industrial processes.
MeSH term(s)	Alcohol Dehydrogenase/metabolism ; Biocatalysis ; Enzymes, Immobilized/metabolism ; Metal-Organic Frameworks/chemistry ; NAD/metabolism
Chemical Substances	Enzymes, Immobilized ; Metal-Organic Frameworks ; NAD (0U46U6E8UK) ; Alcohol Dehydrogenase (EC 1.1.1.1)
Language	English
Publishing date	2022-01-13
Publishing country	England
Document type	Journal Article ; Research Support, Non-U.S. Gov't
ZDB-ID	2553671-0
ISSN	2041-1723 ; 2041-1723
ISSN (online)	2041-1723
ISSN	2041-1723
DOI	10.1038/s41467-022-27983-9
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article: Vibrational Properties of Pd Nanocubes.

Flor, Alberto / Feliu, Juan M / Tsung, Chia-Kuang / Scardi, Paolo

Nanomaterials (Basel, Switzerland)

2019 Volume 9, Issue 4

Abstract: The atomic disorder and the vibrational properties of Pd nanocubes have been studied through a combined use of X-ray diffraction and molecular dynamics simulations. The latter show that the trend of the mean square relative displacement as a function of ... ...

Abstract	The atomic disorder and the vibrational properties of Pd nanocubes have been studied through a combined use of X-ray diffraction and molecular dynamics simulations. The latter show that the trend of the mean square relative displacement as a function of the radius of the coordination shells is characteristic of the nanoparticle shape and can be described by a combined model: A correlated Debye model for the thermal displacement and a parametric expression for the static disorder. This combined model, supplemented by results of line profile analysis of the diffraction patterns collected at different temperatures (100, 200, and 300 K) can explain the observed increase in the Debye-Waller coefficient, and shed light on the effect of the finite domain size and of the atomic disorder on the vibrational properties of metal nanocrystals.
Language	English
Publishing date	2019-04-12
Publishing country	Switzerland
Document type	Journal Article
ZDB-ID	2662255-5
ISSN	2079-4991
ISSN	2079-4991
DOI	10.3390/nano9040609
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Encapsulation of yellow phosphors into nanocrystalline metal-organic frameworks for blue-excitable white light emission.

Liu, Xiao-Yuan / Li, Yang / Tsung, Chia-Kuang / Li, Jing

Chemical communications (Cambridge, England)

2019 Volume 55, Issue 72, Page(s) 10669–10672

Abstract: Host-guest based highly emissive and solution processable nanocomposites are achieved by in situ encapsulation of yellow-emitting molecular dyes into ZIF-8 and UiO-66 during their nanocrystal formation, which can be effectively excited by blue light to ... ...

Abstract	Host-guest based highly emissive and solution processable nanocomposites are achieved by in situ encapsulation of yellow-emitting molecular dyes into ZIF-8 and UiO-66 during their nanocrystal formation, which can be effectively excited by blue light to generate white light.
Language	English
Publishing date	2019-08-14
Publishing country	England
Document type	Journal Article
ZDB-ID	1472881-3
ISSN	1364-548X ; 1359-7345 ; 0009-241X
ISSN (online)	1364-548X
ISSN	1359-7345 ; 0009-241X
DOI	10.1039/c9cc05533a
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Integration of Biomolecules with Metal-Organic Frameworks.

Zhuang, Jia / Young, Allison P / Tsung, Chia-Kuang

Small (Weinheim an der Bergstrasse, Germany)

2017 Volume 13, Issue 32

Abstract: Owing to the progressive development of metal-organic-frameworks (MOFs) synthetic processes and considerable potential applications in last decade, integrating biomolecules into MOFs has recently gain considerable attention. Biomolecules, including ... ...

Abstract	Owing to the progressive development of metal-organic-frameworks (MOFs) synthetic processes and considerable potential applications in last decade, integrating biomolecules into MOFs has recently gain considerable attention. Biomolecules, including lipids, oligopeptides, nucleic acids, and proteins have been readily incorporated into MOF systems via versatile formulation methods. The formed biomolecule-MOF hybrid structures have shown promising prospects in various fields, such as antitumor treatment, gene delivery, biomolecular sensing, and nanomotor device. By optimizing biomolecule integration methods while overcoming existing challenges, biomolecule-integrated MOF platforms are very promising to generate more practical applications.
MeSH term(s)	Biosensing Techniques ; Drug Delivery Systems ; Metal-Organic Frameworks
Chemical Substances	Metal-Organic Frameworks
Language	English
Publishing date	2017-06-22
Publishing country	Germany
Document type	Journal Article ; Research Support, Non-U.S. Gov't ; Research Support, U.S. Gov't, Non-P.H.S. ; Review
ISSN	1613-6829
ISSN (online)	1613-6829
DOI	10.1002/smll.201700880
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article: Encapsulation of yellow phosphors into nanocrystalline metal–organic frameworks for blue-excitable white light emission

Liu, Xiao-Yuan / Li, Jing / Li, Yang / Tsung, Chia-Kuang

Chemical communications. 2019 Sept. 5, v. 55, no. 72

2019

Abstract: Host–guest based highly emissive and solution processable nanocomposites are achieved by in situ encapsulation of yellow-emitting molecular dyes into ZIF-8 and UiO-66 during their nanocrystal formation, which can be effectively excited by blue light to ... ...

Abstract	Host–guest based highly emissive and solution processable nanocomposites are achieved by in situ encapsulation of yellow-emitting molecular dyes into ZIF-8 and UiO-66 during their nanocrystal formation, which can be effectively excited by blue light to generate white light.
Keywords	blue light ; chemical reactions ; coordination polymers ; dyes ; encapsulation ; nanocomposites ; nanocrystals ; white light
Language	English
Dates of publication	2019-0905
Size	p. 10669-10672.
Publishing place	The Royal Society of Chemistry
Document type	Article
ZDB-ID	1472881-3
ISSN	1364-548X ; 1359-7345 ; 0009-241X
ISSN (online)	1364-548X
ISSN	1359-7345 ; 0009-241X
DOI	10.1039/c9cc05533a
Database	NAL-Catalogue (AGRICOLA)

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