Acta Phys. -Chim. Sin. ›› 2022, Vol. 38 ›› Issue (1): 2012091.doi: 10.3866/PKU.WHXB202012091

Special Issue: Graphene: Functions and Applications

• ARTICLE • Previous Articles     Next Articles

Fabrication of Three-Dimensional Copper@Graphene Phase Change Composite with High Structural Stability and Low Leakage Rate

Xiaoming Li1, Yidan Gao1, Qingqiang Kong1, Lijing Xie1, Zhuo liu1, Xiaoqian Guo1, Yanzhen Liu1, Xianxian Wei3, Xiao Yang1, Xinghua Zhang1, Chengmeng Chen1,2,*()   

  1. 1 Key Laboratory of Carbon Materials, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China
    2 College of Materials Sciences and Opto-Electronic Technology, University of Chinese Academy of Sciences, Beijing 100049, China
    3 College of Environment and Safety, Taiyuan University of Science and Technology, Taiyuan 030024, China
  • Received:2020-12-31 Accepted:2021-02-18 Published:2021-02-25
  • Contact: Chengmeng Chen
  • About author:Chengmeng Chen. Email:; Tel.: +86-351-404-9061
  • Supported by:
    the National Natural Science Foundation of China(21922815);the National Natural Science Foundation of China(51802325);the Natural Science Foundation of Shanxi Province(201901D211585);the Scientific and Technological Key Project of Shanxi Province(20191102003);the Patent Promotion and Implementation Project of Shanxi Province(20200716);the Key Research and Development (R&D) Projects of Shanxi Province(201903D121007)


Owing to the continuous increase in energy consumption and the growing depletion of traditional fossil fuels, the development of renewable energy is becoming increasingly urgent. Renewable energy has come to the fore, represented by geothermal energy and solar energy. However, the application of these energy sources is highly susceptible to weather, season, location, and time. Thus, these alternative energies are unstable, random, fluctuating, intermittent, and inefficient. The development of energy storage technologies can efficiently solve these problems, storing and releasing energy when needed. Among the key materials used in various energy-storage technologies, phase-change materials (PCMs) are strong candidates for smart thermal energy management and portable thermal energy sectors. As most innate PCMs face issues of low thermal conductivity, environmental pollution, and leakage over their melting point, encapsulating PCMs into supporting materials is necessary. However, these supporting materials face significant challenges in their application. First, skeleton materials should be resistant to the PCM volume changes during melting and solidification processes to achieve suitable structural stability. Second, skeleton materials should also have high thermal conductivity and a low leakage rate. Graphene aerogel (GA) has proven to be an effective supporting skeleton to improve the shape-stability of PCMs; however, the leakage caused by the phase transition and the brittleness of the network structure is a primary problem restricting its application. Skeleton materials play a crucial role in the performance of PCMs. Herein, we propose a double-pulse plating reinforcement strategy for fabricating copper@graphene aerogel (Cu@GA) as a skeleton material for phase change energy. In this design, individual nanosheets of the GA were uniformly covered and interlinked by copper particles. The Cu@GA interlinked networks ensure suitable thermal conductivity and a robust framework, beneficial for phase change heat transfer and leak-suppression performance. In addition, we prepared a PCM composite with high structural stability and low leakage rate by encapsulating octadecylamine (ODA) in Cu@GA through vacuum impregnation to ensure homogeneous ODA dispersion in the Cu@GA porous structure. The influence of different skeletons on the PCM composite leakage rate was investigated by comparing the weight change of the PCM composite. Benefiting from these structural features, the optimized composite phase change material (CPCM) Cu@GA/ODA showed a reduced leakage rate of 19.82% (w, mass fraction) compared to 80.31% (w) of GA/ODA and 72.99% (w) of GOA/ODA after 20 heat storage and release cycles. The cycled skeleton morphology was investigated using scanning electron microscopy to determine the origin of this influence. The skeleton integrity of Cu@GA/ODA was well maintained, while the three-dimensional network structures of GOA/ODA and GA/ODA showed shrinkage or collapse. Thus, the copper coating increased the skeleton's microstructural stability, conducive to high structural stability and reducing the leakage rate of the PCM composite. This study paves the way for the construction of ideal metal-coating GA composites with an excellent comprehensive performance for future phase change energy storage, porous microwave absorption, and energy storage applications.

Key words: Electroplating, Copper@graphene aerogel, 3D graphene skeleton, Phase change material, Friability