skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.

Explore Research Products in the PAR
It may take a few hours for recently added research products to appear in PAR search results.


  • NSF Public Access
  • Search Results
  • Pushing the Limits of Heat Conduction in Covalent Organic Frameworks Through High‐Throughput Screening of Their Thermal Conductivity
Title: Pushing the Limits of Heat Conduction in Covalent Organic Frameworks Through High‐Throughput Screening of Their Thermal Conductivity
Abstract Tailor‐made materials featuring large tunability in their thermal transport properties are highly sought‐after for diverse applications. However, achieving `user‐defined’ thermal transport in a single class of material system with tunability across a wide range of thermal conductivity values requires a thorough understanding of the structure‐property relationships, which has proven to be challenging. Herein, large‐scale computational screening of covalent organic frameworks (COFs) for thermal conductivity is performed, providing a comprehensive understanding of their structure‐property relationships by leveraging systematic atomistic simulations of 10,750 COFs with 651 distinct organic linkers. Through the data‐driven approach, it is shown that by strategic modulation of their chemical and structural features, the thermal conductivity can be tuned from ultralow (≈0.02 W m−1K−1) to exceptionally high (≈50 W m−1K−1) values. It is revealed that achieving high thermal conductivity in COFs requires their assembly through carbon–carbon linkages with densities greater than 500 kg m−3, nominal void fractions (in the range of ≈0.6–0.9) and highly aligned polymeric chains along the heat flow direction. Following these criteria, it is shown that these flexible polymeric materials can possess exceptionally high thermal conductivities, on par with several fully dense inorganic materials. As such, the work reveals that COFs mark a new regime of materials design that combines high thermal conductivities with low densities.  more » « less
Award ID(s):
2119365
PAR ID:
10521003
Author(s) / Creator(s):
;
Publisher / Repository:
Wiley
Date Published:
Journal Name:
Small
ISSN:
1613-6810
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. ; ; ; ; ; ; ; (, npj Computational Materials)
    Abstract Thermal energy management in metal-organic frameworks (MOFs) is an important, yet often neglected, challenge for many adsorption-based applications such as gas storage and separations. Despite its importance, there is insufficient understanding of the structure-property relationships governing thermal transport in MOFs. To provide a data-driven perspective into these relationships, here we perform large-scale computational screening of thermal conductivitykin MOFs, leveraging classical molecular dynamics simulations and 10,194 hypothetical MOFs created using the ToBaCCo 3.0 code. We found that high thermal conductivity in MOFs is favored by high densities (> 1.0 g cm−3), small pores (< 10 Å), and four-connected metal nodes. We also found that 36 MOFs exhibit ultra-low thermal conductivity (< 0.02 W m−1 K−1), which is primarily due to having extremely large pores (~65 Å). Furthermore, we discovered six hypothetical MOFs with very high thermal conductivity (> 10 W m−1 K−1), the structures of which we describe in additional detail. 
    more » « less
  2. ; ; ; ; ; ; ; ; ; ; et al (, Science Advances)
    To push upper boundaries of thermal conductivity in polymer composites, understanding of thermal transport mechanisms is crucial. Despite extensive simulations, systematic experimental investigation on thermal transport in polymer composites is limited. To better understand thermal transport processes, we design polymer composites with perfect fillers (graphite) and defective fillers (graphite oxide), using polyvinyl alcohol (PVA) as a matrix model. Measured thermal conductivities of ~1.38 ± 0.22 W m−1K−1in PVA/defective filler composites is higher than those of ~0.86 ± 0.21 W m−1K−1in PVA/perfect filler composites, while measured thermal conductivities in defective fillers are lower than those of perfect fillers. We identify how thermal transport occurs across heterogeneous interfaces. Thermal transport measurements, neutron scattering, quantum mechanical modeling, and molecular dynamics simulations reveal that vibrational coupling between PVA and defective fillers at PVA/filler interfaces enhances thermal conductivity, suggesting that defects in polymer composites improve thermal transport by promoting this vibrational coupling. 
    more » « less
  3. ; ; ; ; ; ; ; (, Advanced Functional Materials)
    Abstract Hafnium pentatelluride (HfTe5) has attracted extensive interest due to its exotic electronic, optical, and thermal properties. As a highly anisotropic crystal (layered structure with in‐plane chains), it has highly anisotropic electrical‐transport properties, but the anisotropy of its thermal‐transport properties has not been established. Here, accurate experimental measurements and theoretical calculations are combined to resolve this issue. Time‐domain thermoreflectance measurements find a highly anisotropic thermal conductivity, 28:1:8, with values of 11.3 ± 2.2, 0.41 ± 0.04, and 3.2 ± 2.0 W m-1K-1along the in‐planea‐axis, through‐planeb‐axis, and in‐planec‐axis, respectively. This anisotropy is even larger than what was recently established for ZrTe5(12:1:6), but the individual values are somewhat higher, even though Zr has a smaller atomic mass than Hf. Density‐functional‐theory calculations predict thermal conductivities in good agreement with the experimental data, provide comprehensive insights into the results, and reveal the origin of the apparent anomaly of the relative thermal conductivities of the two pentatellurides. These results establish that HfTe5and ZrTe5, and by implication their alloys, have highly anisotropic and ultralow through‐plane thermal conductivities, which can provide guidance for the design of materials for new directional‐heat‐management applications and potentially other thermal functionalities. 
    more » « less
  4. ; ; ; (, physica status solidi (a))
    The performances of porous graphitic foams in flexible electronic, electrochemical, and thermal management devices can be enhanced by increasing the interfacial charge or heat transport between the 3D graphitic network and the functional materials filled into the pore space. Herein, an investigation of the effects of chemical vapor deposition (CVD) conditions on the structure and thermal conductivities of both graphitic foams grown from reticular Ni foams and dendritic graphitic foams (DGFs) synthesized from electrodeposited dendritic Ni foams is reported. A room‐temperature solid thermal conductivity () up to 800 W m−1 K−1is obtained from the graphitic foams (GF) with less than 1% volume fraction. In comparison, the DGFs, which provide a large increase of the specific surface area for enhanced interfacial heat transfer, achieve an effective thermal conductivity of 2.5 ± 0.2 W m−1 K−1because of an enhanced volume fraction to about 5% despite a compromised around 200 W m−1 K−1due to the increased defect density. Through systematical variations of the catalyst template morphology and CVD conditions, this work reveals the distinct roles of catalyst surface curvature and graphitic strut thickness in controlling the properties of GFs and DGFs for thermal management. 
    more » « less
  5. ; ; (, Physical Chemistry Chemical Physics)
    Efficient heat dissipation in batteries is important for thermal management against thermal runaway and chemical instability at elevated temperatures. Nevertheless, thermal transport processes in battery materials have not been well understood especially considering their complicated microstructures. In this study, lattice thermal transport in lithium cobalt oxide (LiCoO 2 ), a popular cathode material for lithium ion batteries, is investigated via molecular dynamics-based approaches and thermal resistance models. A LiCoO 2 single-crystal is shown to have thermal conductivities in the order of 100 W m −1 K −1 with strong anisotropy, temperature dependence, and size effects. By comparison, polycrystalline LiCoO 2 is more isotropic with much lower thermal conductivities. This difference is caused by random grain orientations, the thermal resistance of grain boundaries, and size-dependent intra-grain thermal conductivities that are unique to polycrystals. The grain boundary thermal conductance is calculated to be in the range of 7.16–25.21 GW m −2 K −1 . The size effects of the intra-grain thermal conductivities are described by two empirical equations. Considering all of these effects, two thermal resistance models are developed to predict the thermal conductivity of polycrystalline LiCoO 2 . The two models predict a consistent thermal conductivity–grain size relationship that agrees well with molecular dynamics simulation results. The insights revealed by this study may facilitate future efforts on battery materials design for improved thermal management. 
    more » « less
  • Citation Formats
  • MLA
  • APA
  • Chicago
  • BibTeX
  • Save / Share this Record
  • Send to Email