Electrochemical oxidation of 5-hydroxymethylfurfural on ternary metal-organic frameworks nanoarrays: enhancement from electronic structure modulation

2021 ◽  
Author(s):  
Xiaojue Bai ◽  
Wenxiu He ◽  
Xingyu Lu ◽  
Yu Fu ◽  
Wei Qi
Keyword(s):  
Electronic Structure ◽  
Carboxylic Acid ◽  
Electrochemical Oxidation ◽  
Rational Design ◽  
Metal Organic Frameworks ◽  
Highly Active ◽  
Ternary Metal ◽  
Metal Organic ◽  
Structure Modulation

The rational design and exploitation of highly active and stable catalysts for the electrochemical oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) to valuable chemical 2,5-furandi-carboxylic acid (FDCA), is of great significance. Herein,...

Rational design of phosphonocarboxylate metal–organic frameworks for light hydrocarbon separations

2018 ◽  
Vol 2 (8) ◽  
pp. 1436-1440 ◽  
Author(s):  
Lan Li ◽  
Qi Yin ◽  
Hong-Fang Li ◽  
Tian-Fu Liu ◽  
Rong Cao
Keyword(s):  
Carboxylic Acid ◽  
Rational Design ◽  
Metal Organic Frameworks ◽  
Light Hydrocarbon ◽  
Phosphate Group ◽  
Metal Organic

By introducing a coordinative phosphate group into a carboxylic acid linker, a ligand was successfully synthesized and used to construct phonocarboxylate framework with narrow approachable channels.

scholarly journals Tuning Atomically Dispersed Fe Sites in Metal–Organic Frameworks Boosts Peroxidase-Like Activity for Sensitive Biosensing

2020 ◽  
Vol 12 (1) ◽  
Author(s):  
Weiqing Xu ◽  
Yikun Kang ◽  
Lei Jiao ◽  
Yu Wu ◽  
Hongye Yan ◽  
...  
Keyword(s):  
Active Sites ◽  
Rational Design ◽  
Limit Of Detection ◽  
Theoretical Calculations ◽  
Organophosphorus Pesticides ◽  
Metal Organic Frameworks ◽  
Atomic Scale ◽  
Electronic Effects ◽  
Highly Active ◽  
Metal Organic

AbstractAlthough nanozymes have been widely developed, accurate design of highly active sites at the atomic level to mimic the electronic and geometrical structure of enzymes and the exploration of underlying mechanisms still face significant challenges. Herein, two functional groups with opposite electron modulation abilities (nitro and amino) were introduced into the metal–organic frameworks (MIL-101(Fe)) to tune the atomically dispersed metal sites and thus regulate the enzyme-like activity. Notably, the functionalization of nitro can enhance the peroxidase (POD)-like activity of MIL-101(Fe), while the amino is poles apart. Theoretical calculations demonstrate that the introduction of nitro can not only regulate the geometry of adsorbed intermediates but also improve the electronic structure of metal active sites. Benefiting from both geometric and electronic effects, the nitro-functionalized MIL-101(Fe) with a low reaction energy barrier for the HO* formation exhibits a superior POD-like activity. As a concept of the application, a nitro-functionalized MIL-101(Fe)-based biosensor was elaborately applied for the sensitive detection of acetylcholinesterase activity in the range of 0.2–50 mU mL−1 with a limit of detection of 0.14 mU mL−1. Moreover, the detection of organophosphorus pesticides was also achieved. This work not only opens up new prospects for the rational design of highly active nanozymes at the atomic scale but also enhances the performance of nanozyme-based biosensors.

scholarly journals Electronic Structure Modulation of Metal–Organic Frameworks for Hybrid Devices

2014 ◽  
Vol 6 (24) ◽  
pp. 22044-22050 ◽  
Author(s):  
Keith T. Butler ◽  
Christopher H. Hendon ◽  
Aron Walsh
Keyword(s):  
Electronic Structure ◽  
Metal Organic Frameworks ◽  
Metal Organic ◽  
Structure Modulation ◽  
Hybrid Devices

Connecting Wires: Photoinduced Electronic Structure Modulation in Metal–Organic Frameworks

2019 ◽  
Vol 141 (13) ◽  
pp. 5350-5358 ◽  
Author(s):  
Ekaterina A. Dolgopolova ◽  
Vladimir A. Galitskiy ◽  
Corey R. Martin ◽  
Haley N. Gregory ◽  
Brandon J. Yarbrough ◽  
...  
Keyword(s):  
Electronic Structure ◽  
Metal Organic Frameworks ◽  
Metal Organic ◽  
Structure Modulation

Message Passing Neural Networks for Partial Charge Assignment to Metal-Organic Frameworks

2020 ◽  
Author(s):  
Ali Raza ◽  
Arni Sturluson ◽  
Cory Simon ◽  
Xiaoli Fern
Keyword(s):  
Electronic Structure ◽  
Message Passing ◽  
Gas Adsorption ◽  
Metal Organic Frameworks ◽  
Computational Cost ◽  
Electronic Structure Calculations ◽  
High Fidelity ◽  
Partial Charges ◽  
Metal Organic ◽  
Structure Calculations

Virtual screenings can accelerate and reduce the cost of discovering metal-organic frameworks (MOFs) for their applications in gas storage, separation, and sensing. In molecular simulations of gas adsorption/diffusion in MOFs, the adsorbate-MOF electrostatic interaction is typically modeled by placing partial point charges on the atoms of the MOF. For the virtual screening of large libraries of MOFs, it is critical to develop computationally inexpensive methods to assign atomic partial charges to MOFs that accurately reproduce the electrostatic potential in their pores. Herein, we design and train a message passing neural network (MPNN) to predict the atomic partial charges on MOFs under a charge neutral constraint. A set of ca. 2,250 MOFs labeled with high-fidelity partial charges, derived from periodic electronic structure calculations, serves as training examples. In an end-to-end manner, from charge-labeled crystal graphs representing MOFs, our MPNN machine-learns features of the local bonding environments of the atoms and learns to predict partial atomic charges from these features. Our trained MPNN assigns high-fidelity partial point charges to MOFs with orders of magnitude lower computational cost than electronic structure calculations. To enhance the accuracy of virtual screenings of large libraries of MOFs for their adsorption-based applications, we make our trained MPNN model and MPNN-charge-assigned computation-ready, experimental MOF structures publicly available.<br>

Synergistic effect of phosphomolybdic acid on rhodium-based metal-organic frameworks for the efficient selective photocatalytic reduction of CO2 to CO

2021 ◽  
Author(s):  
Yurong Shan ◽  
Dexiang Liu ◽  
Chunyan Xu ◽  
Peng Zhan ◽  
Hui Wang ◽  
...  
Keyword(s):  
Carbon Dioxide ◽  
Electronic Structure ◽  
Synergistic Effect ◽  
Metal Organic Frameworks ◽  
Phosphomolybdic Acid ◽  
Photocatalytic Reduction ◽  
Structure And Morphology ◽  
Spherical Structure ◽  
Metal Organic ◽  
Reduction Of Co2

In this work, PMA@NH2-MIL-68(Rh) with a mangosteen spherical structure was successfully synthesized by a hydrothermal method for the photocatalytic reduction of carbon dioxide. The electronic structure and morphology of the...

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