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Controllable Preparation Of Semiconductor Nanostructures Under Ambient Conditions And Their Performance Research

Posted on:2024-09-06Degree:DoctorType:Dissertation
Country:ChinaCandidate:D D ZhangFull Text:PDF
GTID:1521307334478444Subject:Materials Science and Engineering
Abstract/Summary:PDF Full Text Request
As the size of semiconductor nanomaterials decreases,their energy gradually changes from a continuous distribution to a discrete level distribution,and the proportion of surface atoms increases sharply.Therefore,they exhibit significant size effects,surface effects,and quantum tunneling effects,which are key foundations for developing novel and efficient advanced optoelectronic devices.The core challenge is the controllable and large-scale preparation of semiconductor nanomaterials.Currently,the synthesis of nanomaterials generally requires high temperature,high pressure,and the assistance of organic/toxic reagents,which are complex and time-consuming processes that make it difficult to achieve precise control and large-scale preparation of nanomaterial growth.Therefore,achieving large-scale controllable preparation of semiconductor nanostructures under ambient conditions is crucial for advancing its practical applications and has significant scientific significance and application value.This article uses the principle of sonochemistry to achieve controllable growth and large-scale preparation of a series of semiconductor nanomaterials under ambient conditions based on the physical effects of mechanical,thermal,optical,and activation effects caused by acoustic cavitation.The growth mechanism of semiconductor nanostructures is explored through first-principles calculations and finite element simulations,and their applications in sensing,energy conversion,and energy storage are advanced.This article conducts systematic research on advanced preparation technology,growth mechanism explanation,and novel and efficient material property research of semiconductor nanomaterials,achieving the following main innovations:(1)A kilogram-scale production ofγ-Ga2O3 nanomaterials at room temperature and atmospheric pressure was achieved using sonochemical strategy to address the challenge of mass synthesis of crystalline Ga2O3 nanostructures.Combining first-principles calculations and finite element simulations,ethylenediamine(EDA)and ultrasound were identified as critical factors for the formation of Ga2O3 nanomaterials.The prepared Ga2O3 nanostructures exhibited excellent electromagnetic wave absorption properties,and the constructed gas sensor demonstrated outstanding sensing performance for NH3,including ultra-high sensitivity(S=730 vs 100 ppm),fast response(30 s),dynamic recovery(4 s),ultra-low detection limit(0.2 ppm),and excellent selectivity.(2)To address the issues of capacity,cycle life,and room-temperature atmospheric-pressure controllable synthesis of Ga2O3-based lithium-ion batteries,a sonochemical strategy was employed to achieve kilogram-scale production ofγ-Ga2O3@rGO core-shell nanostructures at room temperature and atmospheric pressure.The constructed lithium-ion battery exhibited excellent comprehensive electrochemical properties,including high specific capacity(600 m Ah g-1 after 1000 cycles at a current density of500 m A g-1)and long-term cycle stability(80%of the specific capacity retained after1000 cycles).(3)A sonochemical strategy was employed to address the challenge of controllable growth of crystalline ZnO nanostructures at room temperature and atmospheric pressure.By adjusting the solution p H and changing the charges on crystal polar surfaces,the controlled synthesis of single-crystal ZnO nanostructures was achieved.The prepared ZnO nanosheets exhibited efficient NH3 gas sensing performance at room temperature,including high responsiveness(S=610 vs 100 ppm),good gas selectivity,and fast response/recovery times(70 s/4 s),low detection limit(S=2 vs 0.5 ppm),and excellent cycling reversibility.(4)A sonochemical strategy was employed to address the challenge of large-area room-temperature atmospheric-pressure synthesis of vertically aligned two-dimensional(2D)semiconductor nanostructures.A square centimeter-scale controllable preparation of ZnO nanosheet arrays(Zn@SC-ZnO)on metal Znwas achieved at room temperature and atmospheric pressure,and the growth of large-area ZnO nanowire arrays on glass,silicon,and polyethylene terephthalate(PET)substrates confirmed the universality of this technique.The constructed symmetrical battery exhibited an extremely low polarization overpotential(as low as~20 m V).Moreover,the water-based zinc-ion battery(ZIB)assembled with Mn O2 as the positive electrode demonstrated high specific capacity of 300 m Ah g-1 and high voltage efficiency of 88.2%at a current density of500 m A g-1(at 50%discharge depth),with a cycle life of up to 700 cycles,showing promising practical application prospects in advanced energy storage systems.(5)To further address the controllable growth of crystalline sulfur group semiconductor nanostructures at room temperature and atmospheric pressure,a kilogram-scale preparation of Cd S nanosheets(Cd S NSs)/ZnS nanoparticles(ZnS NPs)1D/2D heterostructure(Cd S-NSs/ZnS-NPs)was reported based on sonochemical strategy.The Cd S-NSs/ZnS-NPs-0.6 photocatalyst exhibited significantly enhanced hydrogen evolution efficiency(reaching 14.02 mmol h-1 g-1),which is about 10 and 85times higher than that of Cd S NSs and Cd S NPs,respectively,under visible light(λ>400nm)irradiation at room temperature and atmospheric pressure,and it showed excellent stability with high durability of 58 hours and good resistance to photogenerated hydrogen corrosion.Finally,with the aid of first-principles calculations,the mechanism of enhancing photocatalytic activity by II-Z mixed 1D/2D heterojunction in Cd S-NSs/ZnS-NPs was proposed.This work provides a certain reference for the large-scale preparation of nanostructures at room temperature and atmospheric pressure and the development of advanced photocatalysts.
Keywords/Search Tags:sonochemical, ambient conditions, semiconductor nanostructures, crystal growth, performance research
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