Browsing by Author "Chiang, Chao-Lung"

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KSCN-activation of hydrogenated NiO/TiO2 for enhanced photocatalytic hydrogen evolution
(2020-05-01)
Wang, Tsai-Te
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Chiang, Chao-Lung
;
Lin, Yu-Chang
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Srinivasadesikan, Venkatesan
;
Lin, Ming-Chang
It was investigated the efficiency of hydrogen production from NiO-loaded TiO2 treated by methanol hydrogenation and functionalized by SCN ligand (SCN-M:(NiO/TiO2)). The effects of a p-n junction created between NiO and TiO2 were demonstrated to enhance significantly the overall photocatalytic performance. The optical and microstructural properties of SCN-M:(NiO/TiO2) were studied with ultraviolet-visible spectra (UV-Vis), photoluminescence (PL), Raman spectra, X-ray diffraction (XRD) and X-ray photoelectron spectra (XPS). The atomic and electronic configurations of SCN-M:(NiO/TiO2) were investigated with analysis of the X-ray absorption near-edge structure (XAS) in situ under irradiation with Xe lamp incorporating a filter (AM 1.5G). An effective quantum yield of 1.34% for hydrogen production was attained with SCN-M:(NiO/TiO2). Quantum-chemical calculations revealed a synergistic decrease of the band gap upon loading Ni, Ni-linked O-2 and anionic SCN-ligand binding. The optimal energy bandgap was decreased to 2.70 eV for (SCN/O-2)-3Ni@TiO2, which reasonably supported the enhancement of H-2 evolution.
N,P co-coordinated Fe species embedded in carbon hollow spheres for oxygen electrocatalysis
(2019-06-28)
Zhu, Xiaofeng
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Tan, Xin
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Wu, Kuang-Hsu
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Chiang, Chao-Lung
;
Lin, Yu-Chang
The increasing interest in fuel cell technology and metal-air batteries has led to the need for stable and effective catalyst materials to replace noble metal (such as Pt) based benchmarks for the oxygen reduction reaction (ORR). In this study, carbon hollow spheres with highly dispersed nitrogen and phosphorus co-coordinated iron atoms (FeNPC) on their surface have been successfully fabricated, exhibiting exceptional ORR activity in both alkaline and acidic solutions. Specifically, the obtained FeNPC catalyst is capable of catalyzing the ORR with an onset potential of 1.03 V and a half-wave potential of 0.88 V (both vs. the reversible hydrogen electrode) in alkaline solution, outperforming the commercial Pt/C catalyst under identical conditions. Experimental results and theoretical simulations reveal that the quasi-octahedral O-2-FeNxPy species are the active sites of the FeNPC composite. These species modify the electronic configuration of Fe centers and weaken the adsorption of the OH* intermediate, thereby promoting the ORR process. Additionally, the FeNPC catalyst also displays a catalytic activity towards the anodic oxygen evolution reaction (OER), making it an active air electrode catalyst in rechargeable Zn-air batteries with a high peak power density of 233.2 mW cm(-2) and an excellent cycling stability at 3 mA cm(-2) for over 15 h.
Sandwich-Nanostructured n-Cu2O/AuAg/p-Cu2O Photocathode with Highly Positive Onset Potential for Improved Water Reduction
(2019-10-23)
Lin, Yu-Chang
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Hsu, Liang-Ching
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Lin, Chia-Yu
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Chiang, Chao-Lung
;
Chou, Che-Min
An n-Cu2O layer formed a high-quality buried junction with p-Cu2O to increase the photovoltage and thus to shift the turn-on voltage positively. Mott-Schottky measurements confirmed that the improvement benefited from a positive shift in flat-band potential. The obtained extremely positive onset potential, 0.8 V-RHE in n-Cu2O/AuAg/p-Cu2O, is comparable with measurements from water reduction catalysts. The AuAg alloy sandwiched between the homo-junction of n-Cu2O and p-Cu2O improved the photocatalytic performance. This alloy both served as an electron relay and promoted electron-hole pair generation in nearby semiconductors; the charge transfer between n-Cu2O and p-Cu2O in the sandwich structure was measured with X-ray absorption spectra. The proposed sandwich structure can be considered as a new direction for the design of efficient solar-related devices.
Structural and Electronic Optimization of MoS2 Edges for Hydrogen Evolution
(2019-11-20)
Wang, Hao
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Xiao, Xu
;
Liu, Shuyuan
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Chiang, Chao-Lung
;
Kuai, Xiaoxiao
The activity and accessibility of MoS2 edge sites are critical to deliver high hydrogen evolution reaction (HER) efficiency. Here, a porous carbon network confining ultrasmall N-doped MoS2 nanocrystals (N-MoS2/CN) is fabricated by a self-templating strategy, which realizes synergistically structural and electronic modulations of MoS2 edges. Experiments and density functional theory calculations demonstrate that the N dopants could activate MoS2 edges for HER, while the porous carbon network could deliver high accessibility of the active sites from N-MoS2 nanocrystals. Consequently, N-MoS2/CN possesses superior HER activity with an overpotential of 114 mV at 10 mA cm(-2) and excellent stability over 10 h, delivering one of best MoS2-based HER electrocatalysts. Moreover, this study opens a new venue for optimizing materials with enhanced accessible catalytic sites for energy-related applications.