For the use of green hydrogen energy,it is crucial to have efficient photocatalytic activity for hydrogen generation by water reforming of methanol under mild conditions.Much attention has been paid to gC_(3)N_(4)as a...For the use of green hydrogen energy,it is crucial to have efficient photocatalytic activity for hydrogen generation by water reforming of methanol under mild conditions.Much attention has been paid to gC_(3)N_(4)as a promising photocatalyst for the generation of hydrogen.To improve the separation of photogenerated charge,porous nanosheet g-C_(3)N_(4)was modified with Pt nanoclusters(Pt/g-C_(3)N_(4))through impregnation and following photo-induced reduction.This catalyst showed excellent photocatalytic activity of water reforming of methanol fo r hydrogen production with a 17.12 mmol·g^(-1)·h^(-1)rate at room temperature,which was 311 times higher than that of the unmodified g-C_(3)N_(4).The strong interactions of Pt-N in Pt/g-C_(3)N_(4)constructed effective electron transfer channels to promote the separation of photogenerated electrons and holes effectively.In addition,in-situ infrared spectroscopy was used to investigate the intermediates of the hydrogen production reaction,which proved that methanol and water eventually turn into H_(2)and CO_(2)via formaldehyde and formate.This study provides insights for understanding the photocatalytic hydrogen production in the water reforming of methanol.展开更多
For the past few years,germanium-based semiconductor spintronics has attracted considerable interest due to its potential for integration into mainstream semiconductor technology.The main challenges in the development...For the past few years,germanium-based semiconductor spintronics has attracted considerable interest due to its potential for integration into mainstream semiconductor technology.The main challenges in the development of modern semiconductor spintronics are the generation,detection,and manipulation of spin currents.Here,the transport characteristics of a spin current generated by spin pumping through a GeBi semiconductor barrier in Y_(3)Fe_(5)O_(12)/GeBi/Pt heterostructures were investigated systematically.The effective spin-mixing conductance and inverse spin Hall voltage to quantitatively describe the spin transport characteristics were extracted.The spin-injection efficiency in the Y_(3)Fe_(5)O_(12)/GeBi/Pt heterostructures is comparable to that of the Y_(3)Fe_(5)O_(12)/Pt bilayer,and the inverse spin Hall voltage exponential decays with the increase in the barrier thickness.Furthermore,the band gap of the GeBi layer was tuned by changing the Bi content.The spin-injection efficiency at the YIG/semiconductor interface and the spin transportation within the semiconductor barrier are related to the band gap of the GeBi layer.Our results may be used as guidelines for the fabrication of efficient spin transmission structures and may lead to further studies on the impacts of different kinds of barrier materials.展开更多
Catalytic oxidation of CH_(4) has been proved to be an attractive option for landfill gas(LFG) upgrading.However, coking of catalysts in catalytic LFG deoxygen has been clearly observed in industrial applications. In ...Catalytic oxidation of CH_(4) has been proved to be an attractive option for landfill gas(LFG) upgrading.However, coking of catalysts in catalytic LFG deoxygen has been clearly observed in industrial applications. In this regard, it is necessary to investigate whether coke deposition originates from CH_(4) or volatile organic compounds present in LFG, and the influence of coke deposition on catalytic performance. Herein,we evaluate the LFG deoxygen on Pt/γ-Al_(2)O_(3) catalyst in simulated LFG(CH_(4), CO_(2), O_(2), N_(2)) and its co-feed with representative volatile organic compounds, ethylbenzene, toluene, benzene and cyclohexane. The results show that the coking of the catalyst is originated from volatile organic compounds rather than CH_(4). The Pt/γ-Al_(2)O_(3) catalyst does not deactivate during LFG deoxygen process, even significant amount of coke deposited, up to 18.15%(mass). Characterization analyses reveal that although coke deposition overall covers the catalyst surface, resulting in mesopores blockage and a reduced number of accessible Pt sites, however, the coke formed, H-rich carbonaceous components, behaves as counterpart for O_(2) elimination. Besides, the coke deposited is mainly filamentous. Thus, coke formation has little negative effect on the overall catalytic performance of Pt/γ-Al_(2)O_(3) catalyst ultimately. The results obtained in this work are helpful for the rational design of robust Pt based catalysts for LFG deoxygen without undue attention to their coking properties, and also favor the innovation of more attractive purification scheme configurations.展开更多
基金supported by the National Natural Science Foundation of China(51672081)the Program of Tri-three Talents Project of Hebei Province(China,A202110002)+1 种基金the Young Top Talents Fund Program of Higher Education Institutions of Heibei Province(BJ2020009)the Project of Science and Technology Innovation Team,Tangshan(20130203D)。
文摘For the use of green hydrogen energy,it is crucial to have efficient photocatalytic activity for hydrogen generation by water reforming of methanol under mild conditions.Much attention has been paid to gC_(3)N_(4)as a promising photocatalyst for the generation of hydrogen.To improve the separation of photogenerated charge,porous nanosheet g-C_(3)N_(4)was modified with Pt nanoclusters(Pt/g-C_(3)N_(4))through impregnation and following photo-induced reduction.This catalyst showed excellent photocatalytic activity of water reforming of methanol fo r hydrogen production with a 17.12 mmol·g^(-1)·h^(-1)rate at room temperature,which was 311 times higher than that of the unmodified g-C_(3)N_(4).The strong interactions of Pt-N in Pt/g-C_(3)N_(4)constructed effective electron transfer channels to promote the separation of photogenerated electrons and holes effectively.In addition,in-situ infrared spectroscopy was used to investigate the intermediates of the hydrogen production reaction,which proved that methanol and water eventually turn into H_(2)and CO_(2)via formaldehyde and formate.This study provides insights for understanding the photocatalytic hydrogen production in the water reforming of methanol.
基金Project supported by the National Key Research and Development Program of China(Grant No.2021YFA0718701)the China Postdoctoral Science Foundation(Grant No.2022M722888)the National Natural Science Foundation of China(Grant Nos.12174347 and 12004340).
文摘For the past few years,germanium-based semiconductor spintronics has attracted considerable interest due to its potential for integration into mainstream semiconductor technology.The main challenges in the development of modern semiconductor spintronics are the generation,detection,and manipulation of spin currents.Here,the transport characteristics of a spin current generated by spin pumping through a GeBi semiconductor barrier in Y_(3)Fe_(5)O_(12)/GeBi/Pt heterostructures were investigated systematically.The effective spin-mixing conductance and inverse spin Hall voltage to quantitatively describe the spin transport characteristics were extracted.The spin-injection efficiency in the Y_(3)Fe_(5)O_(12)/GeBi/Pt heterostructures is comparable to that of the Y_(3)Fe_(5)O_(12)/Pt bilayer,and the inverse spin Hall voltage exponential decays with the increase in the barrier thickness.Furthermore,the band gap of the GeBi layer was tuned by changing the Bi content.The spin-injection efficiency at the YIG/semiconductor interface and the spin transportation within the semiconductor barrier are related to the band gap of the GeBi layer.Our results may be used as guidelines for the fabrication of efficient spin transmission structures and may lead to further studies on the impacts of different kinds of barrier materials.
基金the financial supports from the National Natural Science Foundation of China (22076077, 21577060)Jiangsu Science and Technology Department (BK20191256)Analysis & Test Fund of Nanjing University。
文摘Catalytic oxidation of CH_(4) has been proved to be an attractive option for landfill gas(LFG) upgrading.However, coking of catalysts in catalytic LFG deoxygen has been clearly observed in industrial applications. In this regard, it is necessary to investigate whether coke deposition originates from CH_(4) or volatile organic compounds present in LFG, and the influence of coke deposition on catalytic performance. Herein,we evaluate the LFG deoxygen on Pt/γ-Al_(2)O_(3) catalyst in simulated LFG(CH_(4), CO_(2), O_(2), N_(2)) and its co-feed with representative volatile organic compounds, ethylbenzene, toluene, benzene and cyclohexane. The results show that the coking of the catalyst is originated from volatile organic compounds rather than CH_(4). The Pt/γ-Al_(2)O_(3) catalyst does not deactivate during LFG deoxygen process, even significant amount of coke deposited, up to 18.15%(mass). Characterization analyses reveal that although coke deposition overall covers the catalyst surface, resulting in mesopores blockage and a reduced number of accessible Pt sites, however, the coke formed, H-rich carbonaceous components, behaves as counterpart for O_(2) elimination. Besides, the coke deposited is mainly filamentous. Thus, coke formation has little negative effect on the overall catalytic performance of Pt/γ-Al_(2)O_(3) catalyst ultimately. The results obtained in this work are helpful for the rational design of robust Pt based catalysts for LFG deoxygen without undue attention to their coking properties, and also favor the innovation of more attractive purification scheme configurations.
