☆ 4.7 Article

The effects of electronic polarization on water adsorption in metal-organic frameworks: H2O in MIL-53(Cr)

JOURNAL OF CHEMICAL PHYSICS (2012)

获取全文
添加到收藏夹

期刊

JOURNAL OF CHEMICAL PHYSICS
卷 137, 期 5, 页码 -

出版社

AMER INST PHYSICS
DOI: 10.1063/1.4739254

关键词

-

类别

Chemistry, Physical Physics, Atomic, Molecular & Chemical

资金

  1. University of California, San Diego

向作者/读者索取更多资源

Protocol

社区支持

Reagent

社区支持

The effects of electronic polarization on the adsorption of water in the MIL-53(Cr) metal-organic framework are investigated using molecular dynamics simulations. For this purpose a fully polarizable force field for MIL-53(Cr) was developed which is compatible with the ab initio-based TTM3-F water model. The analysis of the spatial distributions of the water molecules within the MIL-53(Cr) nanopores calculated as a function of loading indicates that polarization effects play an important role in the formation of hydrogen bonds between the water molecules and the hydroxyl groups of the framework. As a result, large qualitative differences are found between the radial distribution functions calculated with non-polarizable and polarizable force fields. The present analysis suggests that polarization effects can significantly impact molecular adsorption in metal-organic frameworks under hydrated conditions. (C) 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.4739254]

作者

我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。

评论

主要评分

4.7
评分不足

次要评分

新颖性
-
重要性
-
科学严谨性
-
评价这篇论文

推荐

Article Chemistry, Physical

Density functional theory of water with the machine-learned DM21 functional

Etienne Palos, Eleftherios Lambros, Saswata Dasgupta, Francesco Paesani

Summary: Recent research has shown that the deep-learned DM21 functional can overcome the delocalization error of traditional DFAs, but its ability to accurately predict the energetics of water clusters varies significantly with cluster size. Additionally, the size-dependent functional-driven errors identified in the analysis of small clusters calculated with the DM21 functional result in the MB-DM21 potential systematically overestimating the hydrogen-bond strength when used in simulations of liquid water.

JOURNAL OF CHEMICAL PHYSICS (2022)

添加到收藏夹
Article Chemistry, Inorganic & Nuclear

Elucidating the exchange interactions in a {GdIIICuII4} propellor

Maria Jose Heras Ojea, Claire Wilson, Jordi Cirera, Hiroki Oshio, Eliseo Ruiz, Mark Murrie

Summary: A new family of 3d-4f complexes with an unusual four-blade propeller topology containing four Cu centers is designed using the multinucleating ligand H6L. The coordination of four {Cu(H4L)} units around the central Ln ion is achieved by using Cl- and ClO4- as co-ligands. Magneto-structural analysis reveals that the geometric arrangement of the Cu(ii) centers defined by the H4L2- ligands controls the magnetic communication between the different metal centers.

DALTON TRANSACTIONS (2023)

添加到收藏夹
Article Chemistry, Physical

A short blanket dilemma for a state-of-the-art neural network potential for water: Reproducing experimental properties or the physics of the underlying many-body interactions?

Yaoguang Zhai, Alessandro Caruso, Sigbjorn Loland Bore, Zhishang Luo, Francesco Paesani

Summary: Deep neural network (DNN) potentials have gained popularity in computer simulations of molecular systems. This study combines the computational efficiency of the DeePMD framework and the accuracy of the MB-pol potential to train a DNN potential for large-scale simulations of water. The DNN potential can reproduce MB-pol results for liquid water but lacks accuracy for vapor-liquid equilibrium properties. Attempts to include many-body effects result in a new DNN potential that accurately reproduces vapor-liquid equilibrium properties but loses accuracy in liquid properties.

JOURNAL OF CHEMICAL PHYSICS (2023)

添加到收藏夹
Article Chemistry, Multidisciplinary

Connecting the dots for fundamental understanding of structure-photophysics-property relationships of COFs, MOFs, and perovskites using a Multiparticle Holstein Formalism

Raja Ghosh, Francesco Paesani

Summary: Photoactive organic and hybrid organic-inorganic materials exhibit interesting photophysical properties upon interaction with light. A theoretical model that accurately describes the structure-photophysics-property relationships is crucial for understanding these materials. This perspective introduces a unified theoretical framework and discusses excitonic and polaronic photophysical signatures in different materials using the Multiparticle Holstein Formalism. The integration of advanced computational methods with the Multiparticle Holstein Formalism is expected to identify new design strategies for next-generation energy materials.

CHEMICAL SCIENCE (2023)

添加到收藏夹
Article Biochemistry & Molecular Biology

The Wild-Type tRNA Adenosine Deaminase Enzyme TadA Is Capable of Sequence-Specific DNA Base Editing

Brodie L. Ranzau, Kartik L. Rallapalli, Mallory Evanoff, Francesco Paesani, Alexis C. Komor

Summary: Base editors are genome editing tools that modify nucleobases in DNA to enable precise base conversions. Adenine base editors convert A.T base pairs to G.C base pairs by using an adenosine deaminase enzyme. Previous experiments showed that the wild-type TadA enzyme had no activity on DNA, but we demonstrated that it can perform base editing in both bacterial and mammalian cells.

CHEMBIOCHEM (2023)

添加到收藏夹
Article Chemistry, Physical

MB-pol(2023): Sub-chemical Accuracy for Water Simulations from the Gas to the Liquid Phase

Xuanyu Zhu, Marc Riera, Ethan F. Bull-Vulpe, Francesco Paesani

Summary: Using the MB-pol theoretical/computational framework, we have introduced a new family of data-driven many-body potential energy functions (PEFs) for water, named MB-pol(2023). By employing larger training sets and adopting sophisticated machine-learned representations, the MB-pol(2023) PEFs achieve sub-chemical accuracy in modeling hexamer isomers and outperform existing PEFs in describing water clusters in the gas phase. Moreover, the MB-pol(2023) PEFs show remarkable agreement with experimental results for various properties of liquid water, improving upon the original MB-pol PEF and closing the gap with experimental measurements.

JOURNAL OF CHEMICAL THEORY AND COMPUTATION (2023)

添加到收藏夹
Article Chemistry, Multidisciplinary

Unveiling Unexpected Modulator-CO2 Dynamics within a Zirconium Metal-Organic Framework

Thomas M. Rayder, Filip Formalik, Simon M. Vornholt, Hilliary Frank, Seryeong Lee, Maytham Alzayer, Zhihengyu Chen, Debabrata Sengupta, Timur Islamoglu, Francesco Paesani, Karena W. Chapman, Randall Q. Snurr, Omar K. Farha

Summary: Carbon capture, storage, and utilization (CCSU) is an opportunity to reduce carbon emissions and combat global climate change. Metal-organic frameworks (MOFs) have shown great potential as effective CO2 sorbents in CCSU through gas adsorption. Understanding the properties of MOF pores and their dynamic behavior during sorption can lead to the development of more efficient CCSU materials.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2023)

添加到收藏夹
Article Multidisciplinary Sciences

Realistic phase diagram of water from first principles data-driven quantum simulations

Sigbjrn Lland Bore, Francesco Paesani

Summary: Since the early 1900s, scientists have been trying to understand the stability of ice polymorphs in water's phase diagram. This study combines the MB-pol data-driven many-body potential for water with advanced enhanced-sampling algorithms to simulate water's phase diagram with a high level of realism. The study provides insights into the role of enthalpic, entropic, and nuclear quantum effects in shaping the free-energy landscape of water and bridges the gap between experiments and simulations.

NATURE COMMUNICATIONS (2023)

添加到收藏夹
Article Chemistry, Multidisciplinary

Structure and thermodynamics of water adsorption in NU-1500-Cr

Ching-Hwa Ho, Mason L. L. Valentine, Zhijie Chen, Haomiao Xie, Omar Farha, Wei Xiong, Francesco Paesani

Summary: This study investigates the water adsorption mechanism in the hydrophilic metal-organic framework NU-1500-Cr using molecular dynamics simulations and infrared spectroscopy. It is found that water initially adsorbs at the open Cr3+ sites and then forms water chains that gradually fill the framework. The insights gained from this study can contribute to the design of efficient water harvesting materials.

COMMUNICATIONS CHEMISTRY (2023)

添加到收藏夹
Article Chemistry, Physical

Engineering Flat and Dispersive Bands in 2D Layered COFs via Interlayer Stacking and Donor-Acceptor Strategy

Yuanhui Pan, Ching-Hwa Ho, Francesco Paesani, Raja Ghosh

Summary: Covalent organic frameworks (COFs) are 2D organic materials with unique electronic and transport properties. In this study, the impact of interlayer stacking arrangements on the electronic structure and coherence of polarons in donor-acceptor COFs was investigated through density functional theory and multiparticle Holstein formalism simulations. It was found that the stacking arrangement significantly influences the transport properties, with varying behavior from metallic to highly localized states. The extent of charge delocalization is sensitive to the type and precise arrangement of interlayer stacking and donor-acceptor fragments in the COF structure. The results suggest that interlayer interactions can aid in enhancing charge delocalization and guide the design of new COF structures for potential applications in organic electronics.

CHEMISTRY OF MATERIALS (2023)

添加到收藏夹
Article Chemistry, Physical

MBX: A many-body energy and force calculator for data-driven many-body simulations

Marc Riera, Christopher Knight, Ethan F. Bull-Vulpe, Xuanyu Zhu, Henry Agnew, Daniel G. A. C. Smith, Andrew Simmonett, Francesco Paesani

Summary: MBX is a C++ library that implements many-body potential energy functions (PEFs) within the many-body energy (MB-nrg) formalism. MB-nrg PEFs integrate an underlying polarizable model with explicit machine-learned representations of many-body interactions to achieve chemical accuracy from the gas to the condensed phases. MBX can be used as a standalone package or integrated with other molecular simulation software as an energy/force engine. It allows for classical and quantum molecular simulations with MB-nrg PEFs, as well as hybrid simulations combining conventional force fields and MB-nrg PEFs for diverse systems.

JOURNAL OF CHEMICAL PHYSICS (2023)

添加到收藏夹
Article Chemistry, Physical

Toward Data-Driven Many-Body Simulations of Biomolecules in Solution: N-Methyl Acetamide as a Proxy for the Protein Backbone

Ruihan Zhou, Marc Riera, Francesco Paesani

Summary: We introduce a data-driven many-body energy potential energy function (MB-nrg PEF) to accurately describe the energetics and structural properties of N-methylacetamide (NMA), as well as the NMA-water interactions. The results show that the MB-nrg PEF is able to accurately represent many-body effects in both gas and liquid phases, making it a promising molecular model for predictive simulations of biomolecular systems.

JOURNAL OF CHEMICAL THEORY AND COMPUTATION (2023)

添加到收藏夹
Article Materials Science, Multidisciplinary

Humidity-Responsive Polymorphism in CALF-20: A Resilient MOF Physisorbent for CO2 Capture

Zhihengyu Chen, Ching-Hwa Ho, Xiaoliang Wang, Simon M. Vornholt, Thomas M. Rayder, Timur Islamoglu, Omar K. Farha, Francesco Paesani, Karena W. Chapman

Summary: CALF-20, a metal-organic framework, shows selective CO2 physisorption. This study reveals that CALF-20 undergoes a structure transformation when exposed to humid environments, resulting in a new polymorph. The transformation is reversible, and the original structure can be regenerated. Computational evaluation indicates that the new polymorph has a higher CO2 heat of adsorption, potentially leading to improved CO2 sorption selectivity at low partial pressures.

ACS MATERIALS LETTERS (2023)

添加到收藏夹
Article Materials Science, Multidisciplinary

Computational insights into the interaction of water with the UiO-66 metal-organic framework and its functionalized derivatives

Jierui Zhang, Francesco Paesani, Martina Lessio

Summary: Studies have shown that incorporating hydrophilic functional groups into the UiO-66 metal-organic framework (MOF) can improve its water uptake ability at low relative humidity (RH). This computational study provides insights into the adsorption mechanism of water in UiO-66 and its functionalized derivatives, revealing the preferential interaction sites and the formation of localized water clusters inside the octahedral pores. The presence of functional groups allows water to cluster in the pores at lower RH, making the MOF a more efficient water harvester.

JOURNAL OF MATERIALS CHEMISTRY C (2023)

添加到收藏夹
Article Chemistry, Physical

Fine-tuning of the spin-crossover properties of Fe(iii) complexes via ligand design

Daniel Vidal, Jordi Cirera, Jordi Ribas-Arino

Summary: Exploring the chemical space of a ligand and modulating its ligand field strength is an effective strategy for fine-tuning the physical properties of spin-crossover complexes. This computational study investigates how ligand substituent effects can modulate the transition temperature (T-1/2) in Fe(iii) SCO systems and identifies suitable descriptors for predicting these changes. The study provides insights into the design of new SCO systems with specific T-1/2 values based on ligand design.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2023)

添加到收藏夹
暂无数据
研讨会 海报 问题 讨论圈 基金 期刊 论文 科研社交 资讯集成 审稿人 关于我们 常见问题 移动App 隐私条款 使用条款
© Peeref 2019-2024. All rights reserved.