Multi-hierarchy heterostructure assembling on MnO2 nanowires for optimized electromagnetic response
Graphical abstract
Introduction
The rapid development of wireless communication, especially the arrival of 5G area, has greatly promoted the development of artificial intelligence and wearable electronic devices [[1], [2], [3]]. However, the accompanying EM interference can also be harmful to people's health [[4], [5], [6]]. The development of high-performance microwave absorbers is an efficient way to solve this problem [7].
In general, the design of microwave absorbing materials focuses on two aspects: rational component design as well as unique structures [8,9]. Typically, the large heterojunction surface and high conductivity of 2D nanosheet materials contribute to enhanced dielectric loss. Furthermore, establishing layered structure in 2D material absorbers allows to combine the advantages of components and structures [10]. On the other hand, the enhanced polarization caused by multiple reflections between layers makes it easier for EM waves to penetrate the system, thereby optimizing the impedance matching [[11], [12], [13]]. In particular, recent reports show that the combination of 1D, 2D and 3D EM-related materials can achieve strong attenuation capability [[14], [15], [16], [17]].
Layered double hydroxides (LDHs), a novel category of layered materials containing divalent and trivalent metal ions, have attracted much attention in EM wave absorption (EMA) due to their flexible and tunable composition, high specific surface area and unique 2D layered structure [[18], [19], [20]]. Nevertheless, LDHs nanosheets are prone to aggregation, and bulk LDHs exhibit feeble EMA performance due to their poor impedance matching [21,22]. Among them, the introduction of structurally diverse and dimensionally tunable metal-organic frameworks (MOFs) as templates to construct LDHs materials with hollow or core-shell architectures is an efficient approach to address this issue [[23], [24], [25]]. Using distinctively shaped MOFs as templates is an efficient way to address the aggregation of pure LDHs nanosheets [26]. For example, Wang et al. observed that ZIF-8 nanoparticles were converted into LDHs nanosheets during the transition [27]; Wang et al. prepared hollow NiCo compound@MXene networks by etching ZIF-67 templates and subsequently anchoring Ti3C2Tx nanosheets by electrostatic self-assembly [28]; Wen et al. prepared layered bilayer hydroxide@carbon composites by a simple three-step method using MOFs as precursors [29].
Nevertheless, the nano-sized MOFs possess high surface energy and are prone to aggregation [30]. Here, we choose 1D nanowires as the substrate for the reaction. 1D EMA -related materials tend to form of axial carrier transport paths under the action of EM fields due to their anisotropy and large aspect ratio [31]. In addition, the surface of MnO2 nanowires is enriched with oxygen-containing functional groups, which can be fully utilized to promote the nucleation and growth of MOFs [[32], [33], [34], [35]]. Furthermore, two metal ions Co and Ni were introduced with the assistance of precipitating agents, and the intermediate MnO2@ZIF-8 was etched into a new 1D and 2D integrated graded porous 3D MnO2@LDHs material [36,37]. In this regard, the constructed network facilitates the enhancement of EMA in multiple ways. (i) The porous structures produced by layered network enhance their contact with air, which optimizes the impedance matching characteristics of the largest entrance of EM waves and prolong the propagation path of EM waves. (ii) The multi-scattering of the incident waves also facilitates the enhancement of the interaction between absorbers. (iii) LDHs have a large surface area that facilitates strong conduction loss as well as dipole and defect polarization for efficient attenuation. Based on the superiority of the unique structure and the synergistic effect of multiple components, MnO2@LDHs absorbers demonstrate exceptional EMA performance. Compared with binary and monovalent LDHs, MnO2@ZnCoNi-LDHs presents extraordinary EMA capability with an optimum RLmin of −56.3 dB at 2.4 mm and fE up to 4.6 GHz at 2.1 mm.
Section snippets
Raw materials
Potassium permanganate (KMnO4), Manganese sulfate monohydrate (MnSO4·H2O), Dimethylimidazole (C4H6N2), Cobalt nitrate hexahydrate (Co (NO3)2·6H2O), Nickel nitrate hexahydrate (Ni (NO3)2·6H2O), Zinc nitrate hexahydrate (Zn (NO3)2·6H2O), Hexamethylenetetramine (C6H12N4), Methanol (CH₃OH), Ethanol (C2H5OH) were bought from Aladdin. All chemicals were of analytical grade (AR) and used without further purification. The water was ultrapure water (18.25 MΩ cm).
Preparation of MnO2 nanowires
MnO2 nanowires were prepared by facile
Preparation and morphology analysis
The synthesis procedure of ZnCoNi-LDHs@MnO2 heterogeneous materials is illustrated in Fig. 1. Firstly, divalent Zn2+ is anchored on the nanowires due to the abundant oxygen-containing groups on the surface of MnO2, and the manganese oxide provides a platform for the nucleation and growth of ZIF-8. Subsequently, with the addition of nitrate, the protons generated by the hydrolysis of divalent nickel and divalent cobalt ions corrode the surface of ZIF-8, then the Zn2+ originally present in ZIF-8
Conclusions
In summary, a heterogeneous structure assembly strategy has been developed to account for the strongly reflected EM waves of 1D MnO2 nanowires. With the 2D layer LDHs, the as-synthesized MnO2@ZnCoNi-LDHs illustrated optimal impedance matching and EM attenuation characteristic. The optimal reflection loss of the layered MnO2@ZnCoNi-LDHs composite is as high as −56.3 dB at 2.4 mm and 4.6 GHz frequency response at 2.1 mm. The reinforced EMA capacity primarily stems from its strong EM loss ability
Credit author statement
Yue Liu and Zirui Jia: related literature, designed experiment and writing- Original draft preparation. Jixi Zhou: Visualization, Investigation. Guanglei Wu: some great enlightenment and helpful advices during the writing process.
Declaration of competing interest
The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Acknowledgements
This work is financially supported by the Natural Science Foundation of Shandong Province (No. ZR2019YQ24), Taishan Scholars and Young Experts Program of Shandong Province (No. tsqn202103057), the Qingchuang Talents Induction Program of Shandong Higher Education Institution (Research and Innovation Team of Structural-Functional Polymer Composites) and Special Financial of Shandong Province (Structural Design of High-efficiency Electromagnetic Wave-absorbing Composite Materials and Construction
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Contributed equally to this work.