Nowadays,photoca-talytic water splitting for hydrogen production is widely recognized as a promising solution to solve both energy shortages and environmental pollution.Nevertheless,photocatalytic hydrogen evolution i...Nowadays,photoca-talytic water splitting for hydrogen production is widely recognized as a promising solution to solve both energy shortages and environmental pollution.Nevertheless,photocatalytic hydrogen evolution is currently hindered by challenges,such as inefficient photogenerated carrier separation and migration and inadequate light absorption by photocatalysts.To overcome such challenges,we herein engineered hollow Cu_(2-x)Se@ZnIn_(2)S_(4) core-shell heterostructures(HCSHs)via synergistic utilization of energy level engineering,interfacial engineering,and local surface plasmon resonance(LSPR)effect.The optimal sample exhibits an outstanding hydrogen evolution rate(46.78 mmol·g^(-1)·h^(-1))under visible-near-infrared(VIS-NIR)irradiation,which is 1.78 times that under VIS irradiation alone and 7.8 times that of ZnIn_(2)S_(4) reference under the same illumination condition.Comprehensive studies demonstrate that the built-in electric field within the p-n heterojunctions,along with the unique core-shell structure,significantly enhances the separation and directional migration of photogenerated carriers.Meanwhile,the NIR LSPR effect from the Cu_(2-x)Se component lowers the apparent activation energy and accelerates the reaction kinetics mainly via plasmonic hot electron-assisted cleavage of the adsorbed water,with photothermal heating providing a secondary contribution.This work is of great importance in developing highly efficient photocatalysts and in boosting LSPR-enhanced photocatalytic applications.展开更多
The effect of Au nanorods （NRs） on optical-to-electric conversion efficiency is investigated in inverted polymer solar cells, in which Au NRs are sandwiched between two layers of ZnO. Accompanied by the optimization...The effect of Au nanorods （NRs） on optical-to-electric conversion efficiency is investigated in inverted polymer solar cells, in which Au NRs are sandwiched between two layers of ZnO. Accompanied by the optimization of thickness of ZnO covered on Au NRs, a high-power conversion efficiency of 3.60% and an enhanced short-circuit current density （Jsc） of 10.87 mA/cm2 are achieved in the poly（3-hexylthiophene）： [6,6]-phenyl-C61-butyric acid methyl ester （P3HT：PC60BM）- based inverted cell and the power conversion efficiency （PCE） is enhanced by 19.6% compared with the control device. The detailed analyses of the light absorption characteristics, the simulated scattering induced by Au NRs, and the electromag- netic field around Au NRs show that the absorption improvement in the photoactive layer due to the light scattering from the longitudinal axis and the near-field increase around Au NRs induced by localized surface plasmon resonance plays a key role in enhancing the performances.展开更多
The methanation of CO_(2) using green hydrogen not only consumes CO_(2) as a carbon resource but also stores H_(2) with high density.However,the activation of CO_(2) molecules under mild conditions is challenging due ...The methanation of CO_(2) using green hydrogen not only consumes CO_(2) as a carbon resource but also stores H_(2) with high density.However,the activation of CO_(2) molecules under mild conditions is challenging due to their inert nature.Herein,we report an efficient photothermal catalytic system using light irradiation which realizes the complete conversion of CO_(2) to methane without external heating.Over optimum bimetallic Ni Fe nanoparticles(NPs)with a Ni/Fe atomic ratio of 7,the CO_(2) conversion can reach up to 98%with a CH_(4) selectivity of 99%,and no catalyst deactivation was observed for more than 100 h,outperforming the reported catalysts.The catalytic performance is strongly dependent on the structure promoters,light absorption efficiency,Ni Fe particle sizes,and Ni/Fe ratio.The Ni Fe alloy NPs with an average size of~21 nm dispersed on alumina nanosheets are evidenced to enhance the localized surface plasmon resonance(LSPR)effect,thus efficiently triggering the CO_(2) methanation.This work emphasizes and clarifies the important role of LSPR in CO_(2) hydrogenation,which may benefit the rational utilization of CO_(2) using solar power.展开更多
Utilizing plasmonic effects to assist electrochemical reactions exhibits a huge potential in tuning the reaction activities and product selectivity,which is most appealing especially in chemical reactions with multipl...Utilizing plasmonic effects to assist electrochemical reactions exhibits a huge potential in tuning the reaction activities and product selectivity,which is most appealing especially in chemical reactions with multiple products,such as CO_(2)reduction reaction(CO_(2)RR).However,a comprehensive review of the development and the underlying mechanisms in plasmon-assisted electrocatalytic CO_(2)RR remains few and far between.Herein,the fundamentals of localized surface plasmonic resonance(LSPR)excitation and the properties of typical plasmonic metals(including Au,Ag,and Cu)are retrospected.Subsequently,the potential mechanisms of plasmonic effects(such as hot carrier effects and photothermal effects)on the reaction performance in the field of plasmon-assisted electrocatalytic CO_(2)RR are summarized,which provides directions for the future development of this field.It is concluded that plasmonic catalysts exhibit potential capabilities in enhancing CO_(2)RR while more in situ techniques are essential to further clarify the inner mechanisms.展开更多
The rapid development of artificial intelligence and the Internet of Things has generated an urgent demand for brain-inspired computing systems characterized by high parallel processing capabilities.However,the power ...The rapid development of artificial intelligence and the Internet of Things has generated an urgent demand for brain-inspired computing systems characterized by high parallel processing capabilities.However,the power consumption of most reported artificial synaptic devices remains substantially higher than that of their biological counterparts,which operate at the femtojoule(fJ)level per synaptic event.To this end,this research aims to develop ultralow-power silicon carbide(SiC)plasmonic nanowire network(NWN)-based artificial synaptic devices for using in musical classification neural network system.By leveraging the neural network-like physical architecture of the NWN and the alteration of conductance states at NW-NW junctions,the SiC/SiO_(2)@Ag NWN devices successfully emulate both ultraviolet(UV)visual and electrical synaptic functions under both externally biased electric field modulation mode and zero-bias photoexcitation mode conditions.Furthermore,due to the confinement effects of one-dimensional nanomaterials and the localized surface plasmon resonance(LSPR)induced by Ag nanoparticles,these devices exhibit substantial synaptic responses at ultra-low currents with minimal power consumption.With its low power consumption,the SiC/SiO_(2)@Ag NWN synapses exhibit superior performance in simulating music classification recognition,achieving an accuracy exceeding 95%within 20 epochs.Notably,the innovative SiC NWN structure ensures robust synaptic performance and high precision in neural network computations.This advancement has the potential to drive the development of novel computing architectures,such as spiking neural networks(SNNs),which more closely mimic the operational principles of biological neural networks,thereby facilitating enhanced music information processing.展开更多
基金financially supported by the National Natural Science Foundation of China(NSFC,Nos.22272008 and 21872011).
文摘Nowadays,photoca-talytic water splitting for hydrogen production is widely recognized as a promising solution to solve both energy shortages and environmental pollution.Nevertheless,photocatalytic hydrogen evolution is currently hindered by challenges,such as inefficient photogenerated carrier separation and migration and inadequate light absorption by photocatalysts.To overcome such challenges,we herein engineered hollow Cu_(2-x)Se@ZnIn_(2)S_(4) core-shell heterostructures(HCSHs)via synergistic utilization of energy level engineering,interfacial engineering,and local surface plasmon resonance(LSPR)effect.The optimal sample exhibits an outstanding hydrogen evolution rate(46.78 mmol·g^(-1)·h^(-1))under visible-near-infrared(VIS-NIR)irradiation,which is 1.78 times that under VIS irradiation alone and 7.8 times that of ZnIn_(2)S_(4) reference under the same illumination condition.Comprehensive studies demonstrate that the built-in electric field within the p-n heterojunctions,along with the unique core-shell structure,significantly enhances the separation and directional migration of photogenerated carriers.Meanwhile,the NIR LSPR effect from the Cu_(2-x)Se component lowers the apparent activation energy and accelerates the reaction kinetics mainly via plasmonic hot electron-assisted cleavage of the adsorbed water,with photothermal heating providing a secondary contribution.This work is of great importance in developing highly efficient photocatalysts and in boosting LSPR-enhanced photocatalytic applications.
基金supported by the Ministry of Science and Technology,China(Grant No.2012CB933301)the National Natural Science Foundation of China(Grant Nos.61274065,51173081,61136003,BZ2010043,51372119,and 51172110)the Priority Academic Program Development of Jiangsu Provincial Higher Education Institutions and Synergetic Innovation Center for Organic Electronics and Information Displays,China
文摘The effect of Au nanorods （NRs） on optical-to-electric conversion efficiency is investigated in inverted polymer solar cells, in which Au NRs are sandwiched between two layers of ZnO. Accompanied by the optimization of thickness of ZnO covered on Au NRs, a high-power conversion efficiency of 3.60% and an enhanced short-circuit current density （Jsc） of 10.87 mA/cm2 are achieved in the poly（3-hexylthiophene）： [6,6]-phenyl-C61-butyric acid methyl ester （P3HT：PC60BM）- based inverted cell and the power conversion efficiency （PCE） is enhanced by 19.6% compared with the control device. The detailed analyses of the light absorption characteristics, the simulated scattering induced by Au NRs, and the electromag- netic field around Au NRs show that the absorption improvement in the photoactive layer due to the light scattering from the longitudinal axis and the near-field increase around Au NRs induced by localized surface plasmon resonance plays a key role in enhancing the performances.
基金supported by the National Natural Science Foundation of China (92145301,22121001,22222206,and U22A20392)the Fundamental Research Funds for the Central Universities (20720220008 and 20720220021)。
文摘The methanation of CO_(2) using green hydrogen not only consumes CO_(2) as a carbon resource but also stores H_(2) with high density.However,the activation of CO_(2) molecules under mild conditions is challenging due to their inert nature.Herein,we report an efficient photothermal catalytic system using light irradiation which realizes the complete conversion of CO_(2) to methane without external heating.Over optimum bimetallic Ni Fe nanoparticles(NPs)with a Ni/Fe atomic ratio of 7,the CO_(2) conversion can reach up to 98%with a CH_(4) selectivity of 99%,and no catalyst deactivation was observed for more than 100 h,outperforming the reported catalysts.The catalytic performance is strongly dependent on the structure promoters,light absorption efficiency,Ni Fe particle sizes,and Ni/Fe ratio.The Ni Fe alloy NPs with an average size of~21 nm dispersed on alumina nanosheets are evidenced to enhance the localized surface plasmon resonance(LSPR)effect,thus efficiently triggering the CO_(2) methanation.This work emphasizes and clarifies the important role of LSPR in CO_(2) hydrogenation,which may benefit the rational utilization of CO_(2) using solar power.
基金supported by the National Key R&D Program of China(Grant No.2022YFA1505000)the National Natural Science Foundation of China(Grant No.22072158)the Strategic Priority Research Program of Chinese Academy of Sciences(Grant No.XDB36000000).
文摘Utilizing plasmonic effects to assist electrochemical reactions exhibits a huge potential in tuning the reaction activities and product selectivity,which is most appealing especially in chemical reactions with multiple products,such as CO_(2)reduction reaction(CO_(2)RR).However,a comprehensive review of the development and the underlying mechanisms in plasmon-assisted electrocatalytic CO_(2)RR remains few and far between.Herein,the fundamentals of localized surface plasmonic resonance(LSPR)excitation and the properties of typical plasmonic metals(including Au,Ag,and Cu)are retrospected.Subsequently,the potential mechanisms of plasmonic effects(such as hot carrier effects and photothermal effects)on the reaction performance in the field of plasmon-assisted electrocatalytic CO_(2)RR are summarized,which provides directions for the future development of this field.It is concluded that plasmonic catalysts exhibit potential capabilities in enhancing CO_(2)RR while more in situ techniques are essential to further clarify the inner mechanisms.
基金supported by the National Natural Science Foundation of China (11875032)Natural Science Foundation of Shaanxi Province (2023-JC-QN-0268)+3 种基金Shaanxi Fundamental Science Research Project for Mathematics and Physics (23JSQ004)Shaanxi Provincial Department of Education (23JK0341)Foundations of Shaanxi Province (2023-JC-YB-022)Shaanxi Fundamental Science Research Project for Mathematics and Physics (22JSQ006)。
文摘The rapid development of artificial intelligence and the Internet of Things has generated an urgent demand for brain-inspired computing systems characterized by high parallel processing capabilities.However,the power consumption of most reported artificial synaptic devices remains substantially higher than that of their biological counterparts,which operate at the femtojoule(fJ)level per synaptic event.To this end,this research aims to develop ultralow-power silicon carbide(SiC)plasmonic nanowire network(NWN)-based artificial synaptic devices for using in musical classification neural network system.By leveraging the neural network-like physical architecture of the NWN and the alteration of conductance states at NW-NW junctions,the SiC/SiO_(2)@Ag NWN devices successfully emulate both ultraviolet(UV)visual and electrical synaptic functions under both externally biased electric field modulation mode and zero-bias photoexcitation mode conditions.Furthermore,due to the confinement effects of one-dimensional nanomaterials and the localized surface plasmon resonance(LSPR)induced by Ag nanoparticles,these devices exhibit substantial synaptic responses at ultra-low currents with minimal power consumption.With its low power consumption,the SiC/SiO_(2)@Ag NWN synapses exhibit superior performance in simulating music classification recognition,achieving an accuracy exceeding 95%within 20 epochs.Notably,the innovative SiC NWN structure ensures robust synaptic performance and high precision in neural network computations.This advancement has the potential to drive the development of novel computing architectures,such as spiking neural networks(SNNs),which more closely mimic the operational principles of biological neural networks,thereby facilitating enhanced music information processing.
