Nature Communications (Nov 2024)

Pressure-regulated rotational guests in nano-confined spaces suppress heat transport in methane hydrates

  • Chengyang Yuan,
  • Hongxiang Zong,
  • Hongsheng Dong,
  • Lei Yang,
  • Yufei Gao,
  • Zhen Fan,
  • Lunxiang Zhang,
  • Jiafei Zhao,
  • Yongchen Song,
  • John S. Tse

DOI
https://doi.org/10.1038/s41467-024-53698-0
Journal volume & issue
Vol. 15, no. 1
pp. 1 – 9

Abstract

Read online

Abstract Materials with low lattice thermal conductivity are essential for various heat-related applications like thermoelectrics, and usual approaches for achieving this rely on specific crystalline structures. Here, we report a strategy for thermal conductivity reduction and regulation via guest rotational dynamics and their couplings with lattice vibrations. By applying pressure to manipulate rotational states, we find the intensified rotor-lattice couplings of compressed methane hydrate MH-III can trigger strong phonon scatterings and phonon localizations, enabling an almost three-fold suppression of thermal conductivity. Besides, the disorder in methane rotational dynamics results in anharmonic interactions and nonlinear pressure-dependent heat transport. The overall guest rotational dynamics and heat conduction changes can be flexibly regulated by the rotor-lattice coupling strength. We further underscore that this reduction mechanism can be extended to a wide range of systems with different structures. The results demonstrate a potentially universal method for reducing or controlling heat transport by developing a hybrid system with tailored molecular rotors.