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Passive radiative cooling technology provides a sustainable way of cooling by the combination of emitting heat to the cold universe and reflecting solar light without any energy input. However, the massive consumption of non‐degradable radiative cooling materials causes resource waste and environmental pollution. Meanwhile, the cooling efficiency can be easily affected by dirt contamination in outdoor environments. Here, by the combination of biomimetic hierarchical structure design and stereo‐complex crystals, a degradable and superhydrophobic (152°) stereo‐complex poly (lactic acid) aerogel with low thermal conductivity (37 mW m–1 K–1), high compression strength (0.1 MPa) and self‐cleaning ability via a simple water‐assisted thermally induced phase separation method is developed. The optimal aerogel has a high sunlight reflection (89%) and strong infrared emissivity (93%) that gets a temperature drop of 3.5 °C during the daytime and 5.8 °C during the nighttime. This aerogel opens an environmentally sustainable pathway to radiative cooling applications. [ABSTRACT FROM AUTHOR]

• Layer-by-layer scraping can produce a powerful shearing effect for UHPE/GNPs gel. • Strong shearing induced dense stacking and ordered alignment of GNPs and PE chains. • The dense and ordered structure drastically enhanced in-plane TC up to 28.88 W/mK. • The solar-thermal conversion ability was also improved by the ordered structure. The simultaneous achievement of ordered alignment for fillers and polymer matrix is highly desired in polymer-based thermally conductive composites, but it is still extremely challenging. Herein, we put forward a layer-by-layer scraping (LbLS) method to simultaneously arrange ultra-high molecular weight polyethylene (UHPE) chains and graphene nanoplates (GNP) into a highly oriented structure. When UHPE/GNP gel suffering the strong shearing effect during LbLS process, the inner UHPE chains and GNP were dragged and orderly arranged along shearing direction, and these oriented structures were retained after rapidly drying by distillation. After layer-by-layer stacking, nacre-like UHPE/GNP films with tightly layered structure were obtained. By adjusting the scraping gap from 200 to 50 μm, the oriented structure can be effectively reinforced with the Herman orientation factors f increasing from 0.83 to 0.88 for GNP and 0.75 to 0.82 for UHPE chains. The highly ordered structure can form a tight and oriented thermal conduction network with low interfacial thermal resistance in plane. The LbLS composite film thus significantly enhanced the in-plane thermal conductivity up to 28.88 W/mK, compared with traditional solution casting film (9.63 W/mK). Moreover, the highly oriented structure can significantly increase the solar-thermal conversion performance (58.1 °C@100 mW/cm2) by improving its light absorption ability comparing to that of solution casting film. Besides, the mechanical strength and toughness that depend on the filler and chain alignment were effectively increased by the oriented structure. [ABSTRACT FROM AUTHOR]

[Display omitted] • ANF-carbonized welding is used to reduce the ITR of 3D graphene architecture. • PCM containing graphene architecture shows a TC of 4.85 W/mK at 4.26 vol% content. • Thermal conductive architecture achieves the rapid heat transfer/storage in PCM. • Graphene architecture enables PCM solar/electric-to-thermal conversion capacity. Graphene-based porous architectures are promising in addressing the poor thermal conductivity, leakage, shape stability problems of organic phase change materials (PCMs), meanwhile endowing them with excellent solar/electric-to-heat conversion ability, but they are still limited by the high interfacial thermal/electrical resistance in architectures caused by organic "binders". In this work, in view of the excellent gel ability of aramid nanofibers (ANF) and its highly ordered conjugate molecular structure, a promising graphene porous architecture assisted by ANF was constructed by unidirectional freeze casting coupled with carbonization welding technique. Due to the similar graphite lattice structure of ANF-derived carbonization and graphene, the interfacial thermal/electrical resistance in highly vertically oriented graphene architecture was greatly reduced. As a result, the PCMs composite encapsulated by the graphene architecture carbonizing at 1500 °C exhibited an outstanding thermal conductivity of as high as 4.85 W/mK at only 4.26 vol%, which enables a rapid heat transfer and storage in PCM composite. The honeycomb porous graphene architecture with high porosity can accommodate sufficient PCMs for energy storage, showing a high latent heat enthalpy of 149.7 J/g with excellent shape stability during phase change process. More importantly, the graphene architecture endows PCM composites with excellent solar/electric-to-thermal conversion capacities, which not only expands the types of energy stored by PCMs, but is also promising in the thermal management application requiring a continuous and stable temperature environment. [ABSTRACT FROM AUTHOR]

[Display omitted] • Ammonium polyphosphate functionalized BNNS (BNNS@APP) was prepared by one-step wet ball milling method. • The macromolecular APP play the role of organic "binders" to construct 3D BNNS skeleton. • The 3D BNNS@APP skeleton with a highly oriented structure was obtained by unidirectional freezing. • The EP/BNNS@APP composite presented excellent thermal conductivity and flame retardancy. Three-dimensional (3D) boron nitride skeleton has a promising prospect in improving the thermal conductivity and flame retardancy of polymer composites, yet the problems of interface thermal resistance and combustion collapse in the skeleton caused by organic adhesives still need to be solved. In this work, macromolecular flame retardancy, ammonium polyphosphate (APP) with high polymerization degree, was firstly used to modify and assemble boron nitride nanosheets (BNNS) into 3D thermally conductive skeleton, in which APP with rich amino groups can result in the strong grafting modification to reduce the interfacial thermal resistance in BNNS skeleton, meanwhile, the catalytic carbonization of APP can reinforce the 3D skeleton barrier without collapse during combustion. Typically, one-step wet ball-milling with assisted APP was used to exfoliate and modify BNNS, followed by unidirectional freezing to achieve 3D BNNS@APP skeleton with highly oriented structure. As expected, the constructing 3D skeleton with low interfacial thermal resistance can effectively form a heat transfer path in polymer matrix. The obtained epoxy-based composite showed a high thermal conductivity of 3.28 W/mK at 9.28 vol% BNNS@APP. Meanwhile, the producing 3D skeleton barrier during combustion induced the significant improvement in flame retardancy, with heat release rate (HRR) and total heat release (THR) decreasing by 68.3% and 52.7%, respectively. This work provides a new adhesive choice in constructing 3D thermal conductive and flame retardant skeleton, which exhibits high potential in thermal management application. [ABSTRACT FROM AUTHOR]

With the rapid development of new-generation wireless communication technologies and portable intelligent electronic devices, the development of composites with excellent thermal conductivity and electromagnetic shielding properties has become an urgent challenge. In this work, a unique fibers-induced segregated-like structure strategy for fabricating thermoplastic polyurethane/polydopamine/silver (TPU/PDA/Ag) composites film with high thermal conductivity (TC) and excellent electromagnetic interference (EMI) shielding performance is demonstrated via electrospinning-electroless depositing-pressing technology. The TPU/PDA/Ag composites film exhibit excellent in-plane TC of 20.9 W/(m⋅K) at 75 wt% Ag loading, which shows excellent thermal management capability as heat spreaders of high-power light-emitting diode (LED) modules in practice. Meanwhile, the composites film presents outstanding EMI shielding efficiency of 109 dB (8.2–12.4 GHz) with a thickness of 45 μm and prominent EMI shielding reliability after 1000 cycles of bending. In addition, the composites film shows good tensile strength (12.1 MPa), elongation at break (108.0%), and toughness (11.59 MJ/m3). The obtained TPU/PDA/Ag composites film achieves the desired balance among thermal conductivity, EMI shielding, and mechanical properties, indicating broad application prospects in new-generation wireless communication technologies and portable intelligent electronic devices. [ABSTRACT FROM AUTHOR]

[Display omitted] • Ionic liquid functionalized BNNS (BNNS@IL) was performed by one-step ball milling. • High-orientation layered EP/BNNS@IL film was fabricated via CLbL blade-casting. • Well-dispersed BNNS@IL is highly stacked in EP matrix along the in-plane direction. • The film showed excellent anisotropic thermal conductivity and flame retardancy. Increasing power density and excess heat production in integrated electronic devices create the strong demand for polymeric thermal management materials with excellent thermal stability, flame retardancy and thermal conductivity. To this end, high-performance ionic liquid-wrapped boron nitride nanosheets (BNNS@IL) were firstly simultaneously exfoliated and flame-retardant functionalized via one-step ball milling process based on the strong mechanochemical action. Epoxy (EP)-based layered films with highly in-plane oriented BNNS@IL were then fabricated by a novel, effective and solvent-free cyclic layer-by-layer (CLbL) blade-casting method. Arising from the highly flat oriented structure and rich flame-retardant functional groups of BNNS@IL, as well as the high compatibility between filler and matrix, the as-fabricated EP/BNNS@IL films exhibited high anisotropic thermal conductivity (K ∥ of 8.3 and K ⊥ of 0.8 W m−1 K−1), outstanding thermal stability and flame retardancy with a dramatic decrease in PHRR (104.2 W/g) and THR (8.1 kJ/g) corresponding to reductions of 72.9% and 75.7% compared with neat EP, respectively. Additionally, the flat oriented structure and strong interfacial interaction also endow EP/BNNS@IL films with high flexibility and excellent mechanical properties. Therefore, the high-effective CLbL casting method and the obtained high-performance EP-based film exhibit a significant potential application in high power flexible electrical devices and thermal management products. [ABSTRACT FROM AUTHOR]

[Display omitted] • Carbon welding is used to reduce filler-to-filler ITR in 3D graphene skeleton. • Introducing the graphene skeleton into PCM improves its thermal conductivity. • The graphene skeleton can avoid the leakage of PCM during solid–liquid phase change. • The graphene skeleton endows PCM with solar-to-heat conversion capacity. Advanced phase change materials (PCMs) with three-dimensional (3D) thermal conductive skeletons reveal the promising prospect in the thermal management of lithium battery. However, the high filler-to-filler interfacial thermal resistance (ITR) arising from the weak interfacial contact connection in 3D skeleton is still challenging. Herein, we demonstrate a "carbon welding" strategy for reducing the filler-to-filler ITR in 3D graphene skeleton by achieving the lattice connection between contact graphene. Typically, the ordered 3D graphene skeleton was constructed by unidirectionally ice template assembling graphene nanoplates (GNP) with the assistance of poly (amic acid) (PAA). Imidization and carbonization treatments were employed to weld the adjacent GNP in 3D skeleton. The similar lattice structure of carbonized polyimide (PI) and graphene can result in the significant reduction of phonon scattering and ITR at these contact areas. After impregnation with polyvinyl alcohol (PEG), the high-performance PCMs with high-efficient phonon transmission expressway were obtained. As expected, the prepared composites reveal the high thermal conductivities with a maximum value of 7.032 W m−1 K−1 at ~11.6 vol% GNP, which is more than two-fold than that of the composite with uncarbonized skeleton. Finite element simulation and nonlinear model analyses confirm that the reduced filler-to-filler ITR in skeleton is the main reason for the improving thermal conductivity. In addition, the presence of 3D graphene skeleton can effectively avoid the leakage during solid–liquid phase change, and significantly improve the shape stability of the PCMs. At the same time, the graphene skeleton can endow the PCM with an excellent solar-to-heat conversion performance, which ensure a wide range of application in actual environment. [ABSTRACT FROM AUTHOR]

Boron nitride/multiwalled carbon nanotubes/carbon (BN/MWCNTs/C) networks were prepared via a rape pollen (RP) biological template assisted strategy. The highly thermally conductive epoxy resin (EP) composites were prepared by impregnating EP into the 3D BN/MWCNTs/C networks. Fourier transform infrared spectra and X-ray photoelectron spectroscopy analyses indicated that the successful modification of BN (m-BN) and the interaction between RP, carboxyl functionalized MWCNTs (c-MWCNTs) and m-BN. Scanning electron microscopy images clearly present the network morphology constructed by MWCNTs connected to m-BN. Thermogravimetric analyzer curves determine the mass concentration of m-BN in EP-based composites. The thermal conductivity (K) reached 1.84 W/(m·K) in the composites at a BN content of 21.3 wt%, displaying a significant enhancement of 868% compared with pure EP. The enhanced K is attributed to the effective connection of BN by the MWCNTs covered on the surface of RP. Meanwhile, the composites exhibit a tensile strength of 39.2 MPa, electrically insulating with a volume electrical resistivity about 9.17 × 1010 Ω cm and good flame retardancy. [Display omitted] • 3D BN/MWCNTs/C thermal conductive networks were prepared via a biological template assisted strategy. • Epoxy-based composites were prepared by a vacuum-assisted impregnation method. • Thermal conductivity was significantly enhanced in this system. • Electrical insulation and flame retardancy performances were observed as well. [ABSTRACT FROM AUTHOR]

The rapid development of electronic devices has led to widespread demand and research on electronic packaging materials with electromagnetic shielding and thermal conductivity (TC) properties due to the inevitable issues of the electromagnetic radiation and thermal accumulation. However, there exists a huge challenge to simultaneously achieve high electromagnetic shielding and TC as well as the electrical insulation requirement as electromagnetic shielding predominantly relies on electrical conductivity of materials. Multilayer structure can endow composite materials with a variety of properties. Therefore, in this work, we fabricated sandwiched cellulose nanofiber/boron nitride nanosheet/Ti 3 C 2 T x MXene films by using a simple and effective alternating vacuum filtration method, and as a result, the special sandwich structure endows the film with excellent electromagnetic shielding, insulation and TC performance. The composite film has an extremely high electromagnetic shielding effectiveness up to 60.7 dB at 8.2 GHz as well as still maintains good electrical insulation properties due to the presence of the CNF/BNNS layer on the surface. Moreover, when the content of BNNS in the CNF/BNNS layer reaches 70 wt%, the sandwiched film has excellent in-plane TC of 19.97 W m−1 K−1. The sandwiched film with excellent electromagnetic shielding and high TC yet insulation performance has great application value in highly integrated electronic devices. [Display omitted] [ABSTRACT FROM AUTHOR]