A cellulose-derived supramolecule for fast ion transport

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Abstract

Supramolecular frameworks have been widely synthesized for ion transport applications. However, conventional approaches of constructing ion transport pathways in supramolecular frameworks typically require complex processes and display poor scalability, high cost, and limited sustainability. Here, we report the scalable and cost-effective synthesis of an ion-conducting (e.g., Na ⁺) cellulose-derived supramolecule (Na-CS) that features a three-dimensional, hierarchical, and crystalline structure composed of massively aligned, one-dimensional, and ångström-scale open channels. Using wood-based Na-CS as a model material, we achieve high ionic conductivities (e.g., 0.23 S/cm in 20 wt% NaOH at 25 °C) even with a highly dense microstructure, in stark contrast to conventional membranes that typically rely on large pores (e.g., submicrometers to a few micrometers) to obtain comparable ionic conductivities. This synthesis approach can be universally applied to a variety of cellulose materials beyond wood, including cotton textiles, fibers, paper, and ink, which suggests excellent potential for a number of applications such as ion-conductive membranes, ionic cables, and ionotronic devices.

Abstract

A cellulose-derived supramolecule with aligned, one-dimensional and ångström-scale channels for fast ion transport is developed.

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Most cited references 82

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A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu.

Stefan Grimme, Jens Antony, Stephan Ehrlich … (2010)

The method of dispersion correction as an add-on to standard Kohn-Sham density functional theory (DFT-D) has been refined regarding higher accuracy, broader range of applicability, and less empiricism. The main new ingredients are atom-pairwise specific dispersion coefficients and cutoff radii that are both computed from first principles. The coefficients for new eighth-order dispersion terms are computed using established recursion relations. System (geometry) dependent information is used for the first time in a DFT-D type approach by employing the new concept of fractional coordination numbers (CN). They are used to interpolate between dispersion coefficients of atoms in different chemical environments. The method only requires adjustment of two global parameters for each density functional, is asymptotically exact for a gas of weakly interacting neutral atoms, and easily allows the computation of atomic forces. Three-body nonadditivity terms are considered. The method has been assessed on standard benchmark sets for inter- and intramolecular noncovalent interactions with a particular emphasis on a consistent description of light and heavy element systems. The mean absolute deviations for the S22 benchmark set of noncovalent interactions for 11 standard density functionals decrease by 15%-40% compared to the previous (already accurate) DFT-D version. Spectacular improvements are found for a tripeptide-folding model and all tested metallic systems. The rectification of the long-range behavior and the use of more accurate C(6) coefficients also lead to a much better description of large (infinite) systems as shown for graphene sheets and the adsorption of benzene on an Ag(111) surface. For graphene it is found that the inclusion of three-body terms substantially (by about 10%) weakens the interlayer binding. We propose the revised DFT-D method as a general tool for the computation of the dispersion energy in molecules and solids of any kind with DFT and related (low-cost) electronic structure methods for large systems.

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Effect of the damping function in dispersion corrected density functional theory.

Stefan Grimme, Stephan Ehrlich, Lars Goerigk (2011)

It is shown by an extensive benchmark on molecular energy data that the mathematical form of the damping function in DFT-D methods has only a minor impact on the quality of the results. For 12 different functionals, a standard "zero-damping" formula and rational damping to finite values for small interatomic distances according to Becke and Johnson (BJ-damping) has been tested. The same (DFT-D3) scheme for the computation of the dispersion coefficients is used. The BJ-damping requires one fit parameter more for each functional (three instead of two) but has the advantage of avoiding repulsive interatomic forces at shorter distances. With BJ-damping better results for nonbonded distances and more clear effects of intramolecular dispersion in four representative molecular structures are found. For the noncovalently-bonded structures in the S22 set, both schemes lead to very similar intermolecular distances. For noncovalent interaction energies BJ-damping performs slightly better but both variants can be recommended in general. The exception to this is Hartree-Fock that can be recommended only in the BJ-variant and which is then close to the accuracy of corrected GGAs for non-covalent interactions. According to the thermodynamic benchmarks BJ-damping is more accurate especially for medium-range electron correlation problems and only small and practically insignificant double-counting effects are observed. It seems to provide a physically correct short-range behavior of correlation/dispersion even with unmodified standard functionals. In any case, the differences between the two methods are much smaller than the overall dispersion effect and often also smaller than the influence of the underlying density functional. Copyright © 2011 Wiley Periodicals, Inc.

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Canonical sampling through velocity rescaling

Giovanni Bussi, Davide Donadio, Michele Parrinello (2007)

The authors present a new molecular dynamics algorithm for sampling the canonical distribution. In this approach the velocities of all the particles are rescaled by a properly chosen random factor. The algorithm is formally justified and it is shown that, in spite of its stochastic nature, a quantity can still be defined that remains constant during the evolution. In numerical applications this quantity can be used to measure the accuracy of the sampling. The authors illustrate the properties of this new method on Lennard-Jones and TIP4P water models in the solid and liquid phases. Its performance is excellent and largely independent of the thermostat parameter also with regard to the dynamic properties.

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All references

Author and article information

Contributors

Qi Dong:

ORCID: https://orcid.org/0000-0002-7553-4213

Role: ConceptualizationRole: Formal analysisRole: InvestigationRole: MethodologyRole: Project administrationRole: SupervisionRole: ValidationRole: VisualizationRole: Writing - original draftRole: Writing - review & editing

Xin Zhang:

ORCID: https://orcid.org/0000-0001-8127-3809

Role: ConceptualizationRole: Formal analysisRole: InvestigationRole: ResourcesRole: SoftwareRole: ValidationRole: VisualizationRole: Writing - original draftRole: Writing - review & editing

Ji Qian:

ORCID: https://orcid.org/0000-0001-5788-1302

Role: InvestigationRole: ValidationRole: Writing - original draft

Shuaiming He:

ORCID: https://orcid.org/0000-0002-6130-0352

Role: InvestigationRole: ValidationRole: Writing - review & editing

Yimin Mao:

ORCID: https://orcid.org/0000-0002-6240-3791

Role: ConceptualizationRole: Data curationRole: Formal analysisRole: InvestigationRole: MethodologyRole: ResourcesRole: SoftwareRole: ValidationRole: Writing - review & editing

Alexandra H. Brozena:

ORCID: https://orcid.org/0000-0002-5045-2123

Role: VisualizationRole: Writing - review & editing

Ye Zhang:

ORCID: https://orcid.org/0000-0001-7897-7485

Role: Investigation

Travis P. Pollard:

ORCID: https://orcid.org/0000-0001-6240-5423

Role: Formal analysisRole: InvestigationRole: VisualizationRole: Writing - original draftRole: Writing - review & editing

Oleg A. Borodin:

ORCID: https://orcid.org/0000-0002-9428-5291

Role: Data curationRole: Formal analysisRole: InvestigationRole: MethodologyRole: Project administrationRole: ResourcesRole: VisualizationRole: Writing - original draftRole: Writing - review & editing

Yanbin Wang: Role: Data curationRole: Formal analysisRole: MethodologyRole: Software

Bhargav Sai Chava: Role: Formal analysisRole: InvestigationRole: MethodologyRole: ResourcesRole: Visualization

Siddhartha Das:

ORCID: https://orcid.org/0000-0002-1705-721X

Role: Formal analysisRole: InvestigationRole: MethodologyRole: SoftwareRole: Writing - original draftRole: Writing - review & editing

Peter Zavalij:

ORCID: https://orcid.org/0000-0001-5762-3469

Role: MethodologyRole: Validation

Carlo U. Segre:

ORCID: https://orcid.org/0000-0001-7664-1574

Role: Formal analysisRole: InvestigationRole: MethodologyRole: Writing - review & editing

Dongyang Zhu:

ORCID: https://orcid.org/0000-0002-3413-5419

Role: Investigation

Lin Xu: Role: Writing - review & editing

Yanliang Liang:

ORCID: https://orcid.org/0000-0001-6771-5172

Role: Formal analysisRole: Validation

Yan Yao:

ORCID: https://orcid.org/0000-0002-8785-5030

Role: Investigation

Robert M. Briber:

ORCID: https://orcid.org/0000-0002-8358-5942

Role: ConceptualizationRole: Funding acquisitionRole: MethodologyRole: Project administrationRole: ResourcesRole: SupervisionRole: VisualizationRole: Writing - original draftRole: Writing - review & editing

Tian Li:

ORCID: https://orcid.org/0000-0002-1087-0662

Role: ConceptualizationRole: InvestigationRole: MethodologyRole: Project administrationRole: ResourcesRole: ValidationRole: Writing - original draftRole: Writing - review & editing

Liangbing Hu:

ORCID: https://orcid.org/0000-0002-9456-9315

Role: ConceptualizationRole: Data curationRole: Funding acquisitionRole: MethodologyRole: Project administrationRole: SupervisionRole: VisualizationRole: Writing - original draftRole: Writing - review & editing

Journal

Journal ID (nlm-ta): Sci Adv

Journal ID (iso-abbrev): Sci Adv

Journal ID (publisher-id): sciadv

Journal ID (hwp): advances

Title: Science Advances

Publisher: American Association for the Advancement of Science

ISSN (Electronic): 2375-2548

Publication date Collection: December 2022

Publication date (Electronic, pub): 09 December 2022

Volume: 8

Issue: 49

Electronic Location Identifier: eadd2031

Affiliations

[ ¹ ]Department of Materials Science and Engineering, University of Maryland College Park, College Park, MD 20742, USA.

[ ² ]National Institute of Standards and Technology, Gaithersburg, MD 20783, USA.

[ ³ ]Department of Electrical and Computer Engineering, University of Houston, Houston, TX 77204, USA.

[ ⁴ ]Texas Center for Superconductivity at the University of Houston (TcSUH), Houston, TX 77204, USA.

[ ⁵ ]Battery Science Branch, Energy Science Division, Sensor and Electron Devices Directorate, DEVCOM Army Research Laboratory, Adelphi, MD 20783, USA.

[ ⁶ ]School of Mechanical Engineering, Purdue University, West Lafayette, IN 47907, USA.

[ ⁷ ]Department of Mechanical Engineering, University of Maryland College Park, College Park, MD 20742, USA.

[ ⁸ ]Department of Chemistry and Biochemistry, University of Maryland College Park, College Park, MD 20742, USA.

[ ⁹ ]Center for Synchrotron Radiation Research and Instrumentation (CSRRI), Illinois Institute of Technology, Physics Department, Chicago, IL 60616, USA.

[ ¹⁰ ]Center for Materials Innovation, University of Maryland College Park, College Park, MD 20742, USA.

Author notes

[†]

These authors contributed equally to this work.

[* ]Corresponding author. Email: binghu@ 123456umd.edu (L.H.); tianli@ 123456purdue.edu (T.L.)

Author information

Qi Dong https://orcid.org/0000-0002-7553-4213

Xin Zhang https://orcid.org/0000-0001-8127-3809

Ji Qian https://orcid.org/0000-0001-5788-1302

Shuaiming He https://orcid.org/0000-0002-6130-0352

Yimin Mao https://orcid.org/0000-0002-6240-3791

Alexandra H. Brozena https://orcid.org/0000-0002-5045-2123

Ye Zhang https://orcid.org/0000-0001-7897-7485

Travis P. Pollard https://orcid.org/0000-0001-6240-5423

Oleg A. Borodin https://orcid.org/0000-0002-9428-5291

Siddhartha Das https://orcid.org/0000-0002-1705-721X

Peter Zavalij https://orcid.org/0000-0001-5762-3469

Carlo U. Segre https://orcid.org/0000-0001-7664-1574

Dongyang Zhu https://orcid.org/0000-0002-3413-5419

Yanliang Liang https://orcid.org/0000-0001-6771-5172

Yan Yao https://orcid.org/0000-0002-8785-5030

Robert M. Briber https://orcid.org/0000-0002-8358-5942

Tian Li https://orcid.org/0000-0002-1087-0662

Liangbing Hu https://orcid.org/0000-0002-9456-9315

Article

Publisher ID: add2031

DOI: 10.1126/sciadv.add2031

PMC ID: 9733924

PubMed ID: 36490337

SO-VID: 93c74457-a4f1-4645-869a-8551f75b661f

Copyright © Copyright © 2022 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution License 4.0 (CC BY).

License:

This is an open-access article distributed under the terms of the Creative Commons Attribution license, which permits which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.

History

Date received : 27 May 2022

Date accepted : 28 October 2022

Funding

Funded by: FundRef http://dx.doi.org/10.13039/100000015, U.S. Department of Energy;

Award ID: DE-AC02-06CH11357

Funded by: FundRef http://dx.doi.org/10.13039/100008639, A. James Clark School of Engineering;

Funded by: FundRef http://dx.doi.org/10.13039/100017300, Texas Center for Superconductivity, University of Houston;

A cellulose-derived supramolecule for fast ion transport

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Most cited references 82

A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu.

Effect of the damping function in dispersion corrected density functional theory.

Canonical sampling through velocity rescaling

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