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Intercalation and Hybridization of Low-dimensional Nanostructures for Chemical and Physical Study

Rashid khan  
【摘要】:Two-dimensional(2D)layered transition metal dichalcogenides(TMDCs)and transition metal oxides have unique chemical and physical properties for useful spintronic and electrochemical potential applications.It is highly desirable to modulate TMDC's structures and compositions for realizing the tunable physical and chemical properties for many specific applications.In this dissertation,multifunctional and high-quality TMDCs and transition metal oxides related nanomaterials are synthesized,functionalized and intercalated.Subsequently,the chemical and physical properties of the obtained low-dimensional nanomaterials are investigated in detail,along with their potential exploration in the field of the supercapacitors.We are hopeful that these results will be useful for the production of low-cost materials for supercapacitor and spintronic devices.(1)Transition metal oxides are widely studied in recent years in the field of electrochemical energy storage due to their high specific capacitance,abundant resource and low cost.Here,we synthesized the CuFe_2O_4-Fe_2O_3 hybrid nanomaterial for highly efficient supercapacitor electrode by using eco-friendly low-temperature co-precipitation method.The composite CuFe_2O_4-Fe_2O_3 demonstrated the excellent specific capacitance of 638.24 F/g and long cyclic stability up to 2000 charge/discharge cycles.Particularly,the calculated specific capacitance value is 16 times higher than that of pure CuFe_2O_4.All characterizations and analysis revealed the superior performance of CuFe_2O_4-Fe_2O_3 composite as supercapacitor electrode with excellent capacitance retention in comparison to CuFe_2O_4.The enhanced electrochemical performance of CuFe_2O_4-Fe_2O_3 composite can be attributed to the synergistic effect which is responsible for redox coupling between Cu2+ and Fe3+ that has never been achieved by single component before.(2)Hafnium diselenide(HfSe_2)is a 2D layered crystal with various unique physical properties.In this study,we synthesized high-quality HfSe_2 and Cu-intercalated HfSe_2 single crystals via chemical vapor transport(CVT)technique.Various characterizations were performed to confirm the structures of the growth samples.The synthesized materials were also contrastively evaluated as supercapacitor electrode for the possible application of energy storage devices.The calculated specific capacitance values are 27.24 and 141.83 F/g at the scan rate of 10 mV/s for HfSe_2 and Cu-intercalated HfSe_2,respectively.Moreover,due to the unique microstructure of 2D materials,the electrodes also showed a high value of specific capacitance,excellent cycling stability and energy density.(3)Tantalum diselenide(TaSe_2)is a unique layered TMDCs with interesting phenomena such as charge-density wave and superconductivity.Herein,we synthesized high-quality TaSe_2 layered single crystals by an improved CVT technique,and also intercalated it with copper(Cu)to alter its magnetic properties.The ferromagnetism was clearly observed in TaSe_2 and Cu-intercalated TaSe_2 layered single crystals,which was also supported by first principle DFT calculations.With the intercalation of Cu in TaSe_2,the saturation magnetization(Ms)values were found to increase from 0.0035 emu/g to 0.0056 emu/g at 300 K and from 0.0169 emu/g to 0.1554 emu/g at 10 K,illustrating approximately nine times increase in contrast to the pristine TaSe_2.Moreover,our DFT calculations further validated the existence of the room-temperature ferromagnetism in TaSe_2,which became more stable after Cu-intercalation due to the increased spin-orbit interaction of Cu atoms compared to Ta atoms.These results affirm the enhancement of ferromagnetism after Cu intercalation in TaSe_2 crystals,which may provide a facile route to tune intrinsic magnetism in 2D materials.

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