LI Yang, LI Bin, LI Zhongming, et al. Preparation and EMI shielding properties of three-dimensional hollow MXene-rGO-CNT composites[J]. Acta Materiae Compositae Sinica, 2025, 42(2): 937-948. DOI: 10.13801/j.cnki.fhclxb.20240518.002
Citation: LI Yang, LI Bin, LI Zhongming, et al. Preparation and EMI shielding properties of three-dimensional hollow MXene-rGO-CNT composites[J]. Acta Materiae Compositae Sinica, 2025, 42(2): 937-948. DOI: 10.13801/j.cnki.fhclxb.20240518.002

Preparation and EMI shielding properties of three-dimensional hollow MXene-rGO-CNT composites

More Information
  • Received Date: March 13, 2024
  • Revised Date: April 27, 2024
  • Accepted Date: May 05, 2024
  • Available Online: June 12, 2024
  • Published Date: May 19, 2024
  • With the continuous development of science and technology, "strong absorption, broadband, lightweight" electromagnetic interference shielding materials need to be developed. In this paper, three-dimensional hollow MXene-reduced graphene oxide-carbon nanotube (MXene-rGO-CNT) composites were prepared by a sacrificial template method using polymethyl methacrylate (PMMA) microspheres and ice templates, and material morphology, structure and electromagnetic interference shielding properties of the composites were characterized. The results show that the construction of rich microporous structure reduces the agglomeration of MXene flakes and the density of the composites (below 0.26 g/cm3). Meanwhile, the interconnected porous structure can cause multiple reflections and scattering of electromagnetic waves, enhancing the electromagnetic interference shielding performance of the composite material. The MXene-rGO-CNT composites exhibit good electromagnetic interference shielding performance over a wide frequency range measured from 1-18 GHz, with a high electromagnetic interference shielding effectiveness of 54 dB at peak value. This work provides a convenient method for preparing nanocomposites for efficient electromagnetic interference shielding applications.

  • Objectives 

    With the continuous development of science and technology, electromagnetic interference (EMI) has become a new type of pollution, adversely affecting human health and the use of electronic devices. Therefore, EMI shielding materials with "strong absorption, broadband, and lightweight" are urgently needed to be developed. MXene and carbon nanomaterials represented by reduced graphene oxide (GO) and carbon nanotubes (CNT) have wide applications in the field of EMI shielding due to their good electrical conductivity and processability. This study aimed to construct a conductive network by collaboratively using TiCT MXene, GO and CNT, and introduce polymethyl methacrylate (PMMA) microspheres to prepare a 3D porous hollow MXene-rGO-CNT composite material

    Methods 

    Three conductive materials, TiCT MXene, graphene oxide (GO) and CNT, are combined by solution blending to construct a conductive network, and PMMA microsphere structure is introduced to form PMMA@MXene-GO-CNT core-shell structured composites, and the ice template and PMMA microsphere templates are removed by freeze-drying and heat-treatment, and the 3D hollow structure MXene -rGO-CNT composites. The micro-morphology, chemical structure, and electromagnetic shielding performance of the composite material were investigated in detail.

    Results 

    1. SEM and XRD results demonstrated that the Al element of the TiAlC MAX phase precursor was successfully etched by in-situ HF etching, and the few-layer/monolayer TiCT MXene nanosheets were obtained by subsequent ultrasonication. 2. SEM, TEM, and EDS results observed that the TiCT MXene was uniformly distributed in the composite material and coated on the surface of PMMA microspheres along with GO nanosheets, and formed bridges between the microspheres, CNT materials were interconnected in a web-like structure, assisting in the construction of the conductive network. After heat treatment, TiCT MXene and GO nanosheets were able to form self-supporting hollow spherical films. 3. XRD, XPS, Raman spectroscopy and thermogravimetric analysis characterized the chemical structures at different stages of the composite preparation process. The results showed that solution mixing successfully composited PMMA, GO, and CNT with TiCT MXene, and during the heat treatment process, PMMA microspheres underwent in situ pyrolysis, and GO was reduced to rGO. 4. Ice templates and PMMA microsphere templates were used to construct the 3D hollow-structure MXene-rGO-CNT composites, which effectively enhanced the lightweight characteristics of the composites, and reduced the composites' The density was reduced to 0.26 g/cm. 5. The synergistic effect formed by MXene, rGO, and CNT materials enhances the EMI shielding performance of TiCT MXene, so that the EMI shielding effectiveness (SE) of MXene-rGO-CNT composites reaches more than 25 dB over a wide electromagnetic wave frequency range of 1~18 GHz. 6. The removal of PMMA microsphere templates constructs the porous hollow structure of the composites, which improved the conductivity issue caused by the easy stacking of MXene nanosheets. Meanwhile, it can form a larger interface area and more multiple reflective surfaces, which further enhances the EMI shielding performance of the MXene-rGO-CNT composites, and the SE value of the MXene-rGO-CNT composites in the frequency range of electromagnetic waves frequency range of 1~18 GHz is 31.49~54.01 dB. In addition, more multiple reflective surfaces enable the electromagnetic wave to form an electromagnetic interference shielding mechanism dominated by absorption loss inside the MXene-rGO-CNT composites.Conclusions:1. The use of TiCT MXene, GO and CNT as conductive materials to construct a conductive network, along with the introduction of PMMA microspheres and ice templates, resulted in a three-dimensional porous hollow MXene-rGO-CNT composite material with a macro-porous and micro-hollow spherical structure, achieving a low density of 0.26 g/cm). 2. The synergistic effect of rGO and CNT materials with MXene nanosheets enhanced the EMI shielding performance of the composite material. The prepared MXene-rGO-CNT composites have good electromagnetic interference shielding performance with EMI SE of more than 25 dB under a wide range of electromagnetic wave frequencies from 1 to 18 GHz. The conductive network within the hollow structure of the material effectively reflected and attenuated electromagnetic waves, achieving a peak electromagnetic shielding effectiveness of 54 dB and providing an absorption-dominated electromagnetic shielding mechanism. The prepared MXene-rGO-CNT composites have potential applications in electromagnetic interference shielding.

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