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In situ alloying between gallium and many metallic fillers like copper and silver, however, leads to a deteriorated composite stability. This paper presents an interfacial engineering approach using 3\u2010chloropropyltriethoxysilane (CPTES) to serve as effective thermal linkers and diffusion barriers at the copper\u2010gallium oxide interfaces in the LM matrix, achieving an enhancement in both thermal conductivity and stability of the composite. By mixing LM with copper particles modified by CPTES, a thermal conductivity (\u03ba) as high as 65.9 W m<jats:sup>\u22121<\/jats:sup> K<jats:sup>\u22121<\/jats:sup> is achieved. In addition, \u03ba\u00a0can be tuned by altering the terminal groups of silane molecules, demonstrating the flexibility of this approach. The potential use of such composite as a TIM is also shown in the heat dissipation of a computer central processing unit. While most studies on LM\u2010based composites enhance the material performance via direct mixing of various fillers, this work provides a different approach to fabricate high\u2010performance LM\u2010based composites and may further advance their applications in various areas including thermal management systems, flexible electronics, consumer electronics, and biomedical systems.<\/jats:p>","DOI":"10.1002\/adma.202103104","type":"journal-article","created":{"date-parts":[[2021,9,12]],"date-time":"2021-09-12T13:13:11Z","timestamp":1631452391000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":209,"title":["Liquid Metal Composites with Enhanced Thermal Conductivity and Stability Using Molecular Thermal Linker"],"prefix":"10.1002","volume":"33","author":[{"given":"Han","family":"Wang","sequence":"first","affiliation":[{"name":"Center of Hydrogen Science, School of Materials Science and Engineering Shanghai Jiao Tong University  800 Dong Chuan Road Shanghai 200240 P. 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