Browsing by Author "Fang, Mei-Jing"

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Au-Cd1-xZnxS core-alloyed shell nanocrystals: boosting the interfacial charge dynamics by adjusting the shell composition
(2018-09-28)
Pu, Ying-Chih
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Chen, Wei-Ta
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Fang, Mei-Jing
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Chen, Yu-Lin
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Tsai, Kai-An
Au-Cd1-xZnxS core-shell nanocrystals (NCs) with controllable shell compositions (from x = 0 to x = 0.37) were synthesized by using the hot-injection method. By increasing the mole fraction of ZnS in the Cd1-xZnxS shell, the conduction band of Cd1-xZnxS can be cathodically shifted to cause an increase of energy difference between the conduction band level of the Cd1-xZnxS shell and the Fermi level of the Au core, thereby enlarging the driving force of interfacial electron transfer to enhance the photoelectrochemical (PEC) efficiency. The interfacial charge dynamics of the samples were examined by time-resolved photoluminescence (TRPL) spectroscopy. The results showed that the interfacial electron transfer rate constant (k(et)) from the Cd1-xZnxS shell to the Au core was increased by 2 orders of magnitude, from 2.41 x 10(7) to 4.91 x 10(9) s(-1) as the mole fraction of ZnS increased from 0 to 0.37. Furthermore, PEC characterization, including Mott-Schottky analysis and photovoltage decay measurements, illustrated that gradually introducing ZnS into the shell composition of Au-Cd1-xZnxS NCs can modify the band structure and enhance the effectiveness of interfacial ET for advancing the PEC properties. The practical use of Au-Cd1-xZnxS NCs in PEC methanol oxidation was also demonstrated, revealing their promising potential as viable photoelectrodes for various PEC applications. The present study delivers an alternative approach of modulating the interfacial ET dynamics of core-shell MSNs by means of shell composition adjustment. The illustrations provide an empirical guideline to the intelligent design of core-shell metal-semiconductor nanoheterostructures (MSNs) for the desired PEC applications.
Au@Cu2O core@shell nanocrystals as dual-functional catalysts for sustainable environmental applications
(2019-03-01)
Kuo, Ming-Yu
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Hsiao, Chih-Feng
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Chiu, Yi-Hsuan
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Lai, Ting-Hsuan
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Fang, Mei-Jing
This work reports the synthesis of Au@Cu2O core@shell nanocrystals with controllable shell thicknesses and demonstrates their use as the dual-functional catalyst that can continuously operate under illumination and darkness conditions for efficient E. con inactivation. On account of the peroxidase mimics of the Au core and Fenton reactivity of the Cu2O shell, the Au@Cu2O nanocrystals exhibit intrinsic peroxidase-like property with the reaction kinetics in accordance with the typical Michaelis-Menten mechanism. On the other hand, time resolved photoluminescence spectra suggest the prevalence of pronounced charge separation for Au@Cu2O nanocrystals, an important advantage that is favourable for photocatalysis. By combining the photocatalytic capability with the peroxidase mimics features, Au@Cu2O nanocrystals can perform practical photocatalytic decomposition of E. coil under visible light illumination but still show vital activity towards E. coil inactivation after light illumination was turned off. The current study delivers a new catalyst configuration by exploiting the multiple functionalities of nanosized Au and Cu2O for advanced environmental and energy conversion applications.
Enhanced photoelectrochemical hydrogen generation in neutral electrolyte using non-vacuum processed CIGS photocathodes with an earth-abundant cobalt sulfide catalyst
(2019-02-28)
Wang, Mingqing
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Chang, Yung-Shan
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Tsao, Chun-Wen
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Fang, Mei-Jing
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Hsu, Yung-Jung
This work reports the novelty of using eco-friendly and cost-effective non-vacuum Electrostatic Spray-Assisted Vapour Deposited Cu(In, Ga) SSe (CIGS) thin films as photocathodes, combined with the earth abundant cobalt sulfide (Co-S) as a catalyst to accelerate the kinetics of photogenerated electron transfer and hydrogen generation for photoelectrochemical water splitting. CdS and ZnO layers were subsequently deposited on top of the selenised CIGS films to increase the charge separation and lower the charge recombination for the photocathodes. In order to improve the lifetime and scalability of the CIGS photocathode and the other cell components, a photoelectrochemical test was conducted in a neutral electrolyte of 0.5 M Na2SO4 under simulated sunlight (AM 1.5G). Both the photocurrent densities and the onset potentials of the photocathodes were significantly improved by the electro-deposition of the low cost and earth-abundant Co-S catalyst, with a photocurrent density as high as 19.1 mA cm(-2) at -0.34 V vs. reversible hydrogen electrode (RHE), comparable with and even higher than that of the control photocathode using rare and precious Pt as a catalyst.
Semiconductor nanoheterostructures for photoconversion applications
(2020-04-01)
Fang, Mei-Jing
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Tsao, Chun-Wen
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Hsu, Yung-Jung
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交大名義發表
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材料科學與工程學系
The ever-growing energy crisis and environmental degradation have instigated scientists to explore sophisticated, versatile energy conversion systems. Photoconversion, which conveys solar power to chemical energy, has emerged as an eminent energy conversion approach to accomplish the demands. Recent years have seen the rocketing rise of semiconductor heterostructures as an ideal material paradigm for the realization of miscellaneous photoconversion applications ranging from water splitting, CO2 reduction and environmental purification to photosynthesis. With tailored functionalities from synergetic effects, semiconductor heterostructures come into prominence as the forefront of photocatalyst development. This topical review summarizes the photoconversion applications developed so far by employing semiconductor heterostructures, with a focus on the heterostructure design principle, interfacial charge dynamics and key factors dictating the overall performance. Future research outlooks and perspectives on the progress of photoconversion technology are also presented.
TiO2 Nanowire-Supported Sulfide Hybrid Photocatalysts for Durable Solar Hydrogen Production
(2019-01-23)
Hsieh, Ping-Yen
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Chiu, Yi-Hsuan
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Lai, Ting-Hsuan
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Fang, Mei-Jing
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Wang, Yu-Ting
As the feet of clay, photocorrosion induced by hole accumulation has placed serious limitations on the widespread deployment of sulfide nanostructures for photoelectrochemical (PEC) water splitting. Developing sufficiently stable electrodes to construct durable PEC systems is therefore the key to the realization of solar hydrogen production. Here, an innovative charge-transfer manipulation concept based on the aligned hole transport across the interface has been realized to enhance the photostability of In2S3 electrodes toward PEC solar hydrogen production. The concept was realized by conducting compact deposition of In2S3 nanocrystals on the TiO2 nanowire array. Under PEC operation, the supporting TiO2 nanowires functioned as an anisotropic charge-transfer backbone to arouse aligned charge transport across the TiO2-In2S3 interface. Because of the aligned hole transport, the TiO2 nanowire-supported In2S3 hybrid nanostructures (TiO2 In2S3) exhibited improved hole-transfer dynamics at the TiO2-In2S3 interface and enhanced hole injection kinetics at the electrode surface, substantially increasing the long-term photostability toward solar hydrogen production. The PEC durability tests showed that TiO2-In2S3 electrodes can achieve nearly 90.9% retention of initial photocurrent upon continuous irradiation for 6 h, whereas the pure In2S3 merely retained 20.8% of initial photocurrent. This double-gain charge-transfer manipulation concept is expected to convey a viable approach to the intelligent design of highly efficient and sufficiently stable sulfide photocatalysts for sustainable solar fuel generation.
TiO2-Au-Cu2O Photocathodes: Au-Mediated Z-Scheme Charge Transfer for Efficient Solar-Driven Photoelectrochemical Reduction
(2018-12-01)
Li, Jing-Mei
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Tsao, Chun-Wen
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Fang, Mei-Jing
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Chen, Chun-Chi
;
Liu, Chen-Wei
An Au-mediated Cu2O-based Z-scheme heterostructure system is demonstrated for use as efficient photocathodes in photoelectrochemical (PEC) reduction. The samples are prepared by electrodepositing a Cu2O layer on the surface of Au particle-coated TiO2 nanorods. For TiO2-Au-Cu2O, the embedded Au particles function as a charge transfer mediator to enhance the electron transportation from the conduction band of TiO2 to the valence band of Cu2O. Such a vectorial charge transfer leads to the concentration of electrons at the conduction band of Cu2O and the collection of holes at the valence band of TiO2, providing TiO2-Au-Cu2O with substantially high redox abilities for reduction applications. Time-resolved photoluminescence spectra and electrochemical impedance spectroscopy analysis suggest that interfacial charge transfer is significantly improved because of the Au-mediated Z-scheme charge transfer mechanism. By virtue of the high redox ability and improved interfacial charge transfer, TiO2-Au-Cu2O performs much better as a photocathode in H2 production and CO2 reduction than pure Cu2O and binary TiO2-supported Cu2O do. Remarkably, the photocurrent density of TiO2-Au-Cu2O toward PEC CO2 reduction can reach as high as -1.82 mA/cm(2) at +0.11 V vs RHE. The incident photon-to-current conversion efficiency data manifest that TiO2-Au-Cu2O surpasses both pure Cu2O and binary TiO2-supported Cu2O in PEC reduction across the whole photoactive region. The current study paves a valuable approach of devising Z-scheme photocathode for the construction of sophisticated artificial photosynthesis systems capable of solar-to-fuel conversion.