The increasing emission of carbon dioxide （CO2） caused by the unrestrained consumption of fossil fuels in recent hundreds of years, has caused global environmental and social problems. Meanwhile, CO2 is a cheap, abu...The increasing emission of carbon dioxide （CO2） caused by the unrestrained consumption of fossil fuels in recent hundreds of years, has caused global environmental and social problems. Meanwhile, CO2 is a cheap, abundant and renewable Cl-feedstock, which can be converted into alco- hols, ethers, acids and other value-added chemicals. Compared with the thermal reactions, electrochemical reduction of CO2 is more attractive because of its advantages by using the seasonal, geographical and intermittent energy （tide, wind and solar） under mild conditions. In recent years, taking ionic liquids （ILs） as electrolytes in the CO2 electrochemical reduction reaction has been paid much more attention due to the advantages of lowering the overpotential of CO2 electroreduction and improving the Faradaic efficiency. In this paper, we summarized the recent progresses of electrochemical re- duction of CO2 in ILs electrolytes, and analyzed the reaction mechanism of CO2 reaction in the electrode-electrolyte interface region by experimental and simulation methods. Finally, the research which needs to be highlighted in this area was proposed.展开更多
To satisfy the requirements of substantial green development,it is urgent to explore an innovative eco‐friendly semiconductor photocatalyst to efficiently achieve visible‐light‐driven photocatalytic H 2 evolution(P...To satisfy the requirements of substantial green development,it is urgent to explore an innovative eco‐friendly semiconductor photocatalyst to efficiently achieve visible‐light‐driven photocatalytic H 2 evolution(PHE).The strategy of promoting the spatial separation efficiency of photoinduced carriers can essentially enhance the PHE performance of a photocatalyst.Herein,a graphitic carbon nitride(g‐C 3 N 4)‐based donor–acceptor(D‐A)copolymer(CNDM x)is constructed by simple one‐pot thermal polycondensation,using urea and 5,8‐DibroMoquinoxaline(as an electron donor)as precursors.The electron D-A modulation consequently creates an internal electric field to facilitate the intramolecular charge transfer within the copolymer.A series of experimental characterizations and density functional theory calculations are applied to elucidate the variation and correlation of the structure and PHE performance of the as-prepared catalysts.It is found that the best average PHE rate of 3012.5μmolg^(−1) h^(−1) can be achieved over the optimal D-A copolymer under visible‐light(400<λ<800nm)irradiation,which is~3.3 times that of pure urea-derived g-C_(3)N_(4).The corresponding apparent quantum efficiency is 1.3% at 420nm.This study provides a protocol for designing effective visible-light photocatalysts via D-A modulation of polymeric semiconductors.展开更多
Constructing a built-in electric field has emerged as a key strategy for enhancing charge separation and transfer,thereby improving photoelectrochemical performance.Recently,considerable efforts have been devoted to t...Constructing a built-in electric field has emerged as a key strategy for enhancing charge separation and transfer,thereby improving photoelectrochemical performance.Recently,considerable efforts have been devoted to this endeavor.This review systematically summarizes the impact of built-in electric fields on enhancing charge separation and transfer mechanisms,focusing on the modulation of built-in electric fields in terms of depth and orderliness.First,mechanisms and tuning strategies for built-in electric fields are explored.Then,the state-of-the-art works regarding built-in electric fields for modulating charge separation and transfer are summarized and categorized according to surface and interface depth.Finally,current strategies for constructing bulk built-in electric fields in photoelectrodes are explored,and insights into future developments for enhancing charge separation and transfer in high-performance photoelectrochemical applications are provided.展开更多
Li[Li0.2Ni0.13Coo.13Mn0.54]O2 cathode materials were synthesized by carbonate-based co-precipitation method, and then, its surface was coated by thin layers of FePO4. The prepared samples were characterized by X-ray d...Li[Li0.2Ni0.13Coo.13Mn0.54]O2 cathode materials were synthesized by carbonate-based co-precipitation method, and then, its surface was coated by thin layers of FePO4. The prepared samples were characterized by X-ray diffraction （XRD）, field emission scanning electron micro- scope （FESEM）, energy-dispersive spectroscopy （EDS）, and transmission electron microscopy （TEM）. The XRD and TEM results suggest that both the pristine and the coated materials have a hexagonal layered structure, and the FePO4 coating layer does not make any major change in the crystal structure. The FePO4-coated sample exhibits both improved initial discharge capacity and columbic efficiency compared to the pristine one. More significantly, the FePO4 coating layer has a much positive influence on the cycling perfor- mance. The FePO4-coated sample exhibits capacity reten- tion of 82 % after 100 cycles at 0.5℃ between 2.0 and 4.8 V, while only 28 % for the pristine one at the same charge-discharge condition. The electrochemical impe- dance spectroscopy （EIS） results indicate that this improved cycling performance could be ascribed to the presence of FePO4 on the surface of Li[Li0.2Ni0.13Co0.13Mno.54102 par- ticle, which helps to protect the cathode from chemical attacks by HF and thus suppresses the large increase in charge transfer resistance.展开更多
Because of its importance in enhancing charge separation and transfer,built-in electric field engineering has been acknowledged as an effective technique for improving photocatalytic performance.Herein,a stable p–n h...Because of its importance in enhancing charge separation and transfer,built-in electric field engineering has been acknowledged as an effective technique for improving photocatalytic performance.Herein,a stable p–n heterojunction of 2D/2D(2D:twodimensional)Co_(3)O_(4)/ZnIn_(2)S_(4)with a strong built-in electric field is precisely constructed.The Co_(3)O_(4)/ZnIn_(2)S_(4)heterojunction exhibits a higher visible-light photocatalytic hydrogen(H2)evolution rate than the individual components,which is primarily attributed to the synergy effect of improved light absorption,abundant active sites,short charge transport distance,high separation efficiency of photogenerated carriers.Furthermore,the photoelectrochemical studies and density functional theory(DFT)calculation results demonstrate that the enhanced interfacial charge separation and migration induced by the generated built-in electric field are the critical reasons for the boosted photocatalytic performance.This research might pave the way for the rational design and manufacturing of 2D/2D heterojunction photocatalysts with extremely efficient photocatalytic performance for solar energy conversion.展开更多
Shock wave is a detriment in the development of supersonic aircrafts;it increases flow drag as well as surface heating from additional friction;it also initiates sonic boom on the ground which precludes supersonic jet...Shock wave is a detriment in the development of supersonic aircrafts;it increases flow drag as well as surface heating from additional friction;it also initiates sonic boom on the ground which precludes supersonic jetliner to fly overland. A shock wave mitigation technique is demonstrated by experiments conducted in a Mach 2.5 wind tunnel. Non-thermal air plasma generated symmetrically in front of a wind tunnel model and upstream of the shock, by on-board 60 Hz periodic electric arc discharge, works as a plasma deflector, it deflects incoming flow to transform the shock from a well-defined attached shock into a highly curved shock structure. In a sequence with increasing discharge intensity, the transformed curve shock increases shock angle and moves upstream to become detached with increasing standoff distance from the model. It becomes diffusive and disappears near the peak of the discharge. The flow deflection increases the equivalent cone angle of the model, which in essence, reduces the equivalent Mach number of the incoming flow, manifesting the reduction of the shock wave drag on the cone. When this equivalent cone angle exceeds a critical angle, the shock becomes detached and fades away. This shock wave mitigation technique helps drag reduction as well as eliminates sonic boom.展开更多
We have measured the electric dipole moment of several Scn-C60 molecules (n = 1 - 6) in gaseous phase, by coupling a matrix-assisted laser desorption source to an electric beam deflection setup which is an electric eq...We have measured the electric dipole moment of several Scn-C60 molecules (n = 1 - 6) in gaseous phase, by coupling a matrix-assisted laser desorption source to an electric beam deflection setup which is an electric equivalent of the famous Stern Gerlach [1] one. Experimental results are compared to a qualitative charge transfer that occurs between Sc and fullerene.展开更多
When the spacecraft flies much faster than the sound speed (~1200 km/h), the airflow disturbances deflected forward from the spacecraft cannot get away from the spacecraft and form a shock wave in front of it. Shock w...When the spacecraft flies much faster than the sound speed (~1200 km/h), the airflow disturbances deflected forward from the spacecraft cannot get away from the spacecraft and form a shock wave in front of it. Shock waves have been a detriment for the development of supersonic aircrafts, which have to overcome high wave drag and surface heating from additional friction. Shock wave also produces sonic booms. The noise issue raises environmental concerns, which have precluded routine supersonic flight over land. Therefore, mitigation of shock wave is essential to advance the development of supersonic aircrafts. A plasma mitigation technique is studied. A theory is presented to show that shock wave structure can be modified via flow deflection. Symmetrical deflection evades the need of exchanging the transverse momentum between the flow and the deflector. The analysis shows that the plasma generated in front of the model can effectively deflect the incoming flow. A non-thermal air plasma, generated by on-board 60 Hz periodic electric arc discharge in front of a wind tunnel model, was applied as a plasma deflector for shock wave mitigation technique. The experiment was conducted in a Mach 2.5 wind tunnel. The results show that the air plasma was generated symmetrically in front of the wind tunnel model. With increasing discharge intensity, the plasma deflector transforms the shock from a welldefined attached shock into a highly curved shock structure with increasing standoff distance from the model;this curved shock has increased shock angle and also appears in increasingly diffused form. In the decay of the discharge intensity, the shock front is first transformed back to a well-defined curve shock, which moves downstream to become a perturbed oblique shock;the baseline shock front then reappears as the discharge is reduced to low level again. The experimental observations confirm the theory. The steady of the incoming flow during the discharge cycle is manifested by the repeat of the baseline shock front.展开更多
This work reveals essential details of plasma-surface interaction in atmospheric air that are important for a wide range of applications, beginning from airflow control and up to the high-voltage insulation. The paper...This work reveals essential details of plasma-surface interaction in atmospheric air that are important for a wide range of applications, beginning from airflow control and up to the high-voltage insulation. The paper discusses experimental data characterizing dynamics of development and kinetics of energy coupling in surface dielectric barrier discharge (SDBD), atmospheric air plasmas sustained over dielectric surfaces, over a wide range of time scales. The experiments have been conducted using microsecond pulse voltage waveform of single and alternating polarities. Time-resolved discharge development and mechanisms of coupling with quiescent air are analyzed using nanosecond gate camera imaging, electrical measurements, and original surface charge sensors. The results demonstrate several new, critically important processes overlooked in previous studies. Specifically, it is shown that SDBD plasmas energy release may be significantly increased by using an optimized waveform.展开更多
Localized surface plasmon resonance(LSPR)of nanostructures and the interfacial charge transfer(CT)of semiconductor materials play essential roles in the study of optical and photoelectronic properties.In this paper,a ...Localized surface plasmon resonance(LSPR)of nanostructures and the interfacial charge transfer(CT)of semiconductor materials play essential roles in the study of optical and photoelectronic properties.In this paper,a composite substrate of Ag2S quantum dots(QDs)coated plasmonic Au bowtie nanoantenna(BNA)arrays with a metalinsulator-metal(MIM)configuration was built to study the synergistic effect of LSPR and interfacial CT using surface-enhanced Raman scattering(SERS)in the near-infrared(NIR)region.The Au BNA array structure with a large enhancement of the localized electric field(E-field)strongly enhanced the Raman signal of adsorbed p-aminothiophenol(PATP)probe molecules.Meanwhile,the broad enhanced spectral region was achieved owing to the coupling of LSPR The as-prepared Au BNA array structure facilitated enhancements of the excitation as well as the emission of Raman signal simultaneously,which was established by finite-difference time-domain simulation.Moreover,Ag2S semiconductor QDs were introduced into the BNA/PATP system to further enhance Raman signals,which benefited from the interfacial CT resonance in the BNA/Ag2S-QDs/PATP system.As a result,the Raman signals of PATP in the BNA/Ag2S-QDs/PATP system were strongly enhanced under 785 nm laser excitation due to the synergistic effect of E-field enhancement and interfacial CT.Furthermore,the SERS polarization dependence effeas of the BNA/Ag2S-QDs/PATP system were also investigated.The SERS spectra indicated that the polarization dependence of the substrate increased with decreasing polarization angles(θpola)of excitation from p-polarized(θpola=90°)excitation to s-polarized(θpola=0°)excitation.This study provides a strategy using the synergistic effect of interfacial CT and E-field enhancement for SERS applications and provides a guidance for the development of SERS study on semiconductor QD-based plasmonic substrates,and can be farther extended to other material-nanostructure systems for various optoelectronic and sensing applications.展开更多
基金This work was supported by Fundamental Research and the National Key Projects for Development of China （2018YFB0605802）, the National Natural Science Foundation of China （21425625 ＆ 21506219）, Beijing Natural Science Founda- tion （2182072）, the Research Council of Norway {267615）, and Beijing Hundreds of Leading Talents Training Project of Science and Technology （Z171100001117154）.
文摘The increasing emission of carbon dioxide （CO2） caused by the unrestrained consumption of fossil fuels in recent hundreds of years, has caused global environmental and social problems. Meanwhile, CO2 is a cheap, abundant and renewable Cl-feedstock, which can be converted into alco- hols, ethers, acids and other value-added chemicals. Compared with the thermal reactions, electrochemical reduction of CO2 is more attractive because of its advantages by using the seasonal, geographical and intermittent energy （tide, wind and solar） under mild conditions. In recent years, taking ionic liquids （ILs） as electrolytes in the CO2 electrochemical reduction reaction has been paid much more attention due to the advantages of lowering the overpotential of CO2 electroreduction and improving the Faradaic efficiency. In this paper, we summarized the recent progresses of electrochemical re- duction of CO2 in ILs electrolytes, and analyzed the reaction mechanism of CO2 reaction in the electrode-electrolyte interface region by experimental and simulation methods. Finally, the research which needs to be highlighted in this area was proposed.
基金This study was financially supported by the National Key Research and Development Program of China(2018YFB1502001)the National Natural Science Foundation of China(51922081,51961135303,51932007,and U1705251).
文摘To satisfy the requirements of substantial green development,it is urgent to explore an innovative eco‐friendly semiconductor photocatalyst to efficiently achieve visible‐light‐driven photocatalytic H 2 evolution(PHE).The strategy of promoting the spatial separation efficiency of photoinduced carriers can essentially enhance the PHE performance of a photocatalyst.Herein,a graphitic carbon nitride(g‐C 3 N 4)‐based donor–acceptor(D‐A)copolymer(CNDM x)is constructed by simple one‐pot thermal polycondensation,using urea and 5,8‐DibroMoquinoxaline(as an electron donor)as precursors.The electron D-A modulation consequently creates an internal electric field to facilitate the intramolecular charge transfer within the copolymer.A series of experimental characterizations and density functional theory calculations are applied to elucidate the variation and correlation of the structure and PHE performance of the as-prepared catalysts.It is found that the best average PHE rate of 3012.5μmolg^(−1) h^(−1) can be achieved over the optimal D-A copolymer under visible‐light(400<λ<800nm)irradiation,which is~3.3 times that of pure urea-derived g-C_(3)N_(4).The corresponding apparent quantum efficiency is 1.3% at 420nm.This study provides a protocol for designing effective visible-light photocatalysts via D-A modulation of polymeric semiconductors.
基金financially supported by the Industrial Technology Innovation Program of IMAST(No.2023JSYD 01003)the National Natural Science Foundation of China(Nos.52104292 and U2341209)。
文摘Constructing a built-in electric field has emerged as a key strategy for enhancing charge separation and transfer,thereby improving photoelectrochemical performance.Recently,considerable efforts have been devoted to this endeavor.This review systematically summarizes the impact of built-in electric fields on enhancing charge separation and transfer mechanisms,focusing on the modulation of built-in electric fields in terms of depth and orderliness.First,mechanisms and tuning strategies for built-in electric fields are explored.Then,the state-of-the-art works regarding built-in electric fields for modulating charge separation and transfer are summarized and categorized according to surface and interface depth.Finally,current strategies for constructing bulk built-in electric fields in photoelectrodes are explored,and insights into future developments for enhancing charge separation and transfer in high-performance photoelectrochemical applications are provided.
基金financially supported by the National Nature Science Foundation of China (No.51302017)the National High Technology Research and Development Program of China (No.2012AA110102)the fund from the Science and Technology Commission of Beijing (No.2121100006712002)
文摘Li[Li0.2Ni0.13Coo.13Mn0.54]O2 cathode materials were synthesized by carbonate-based co-precipitation method, and then, its surface was coated by thin layers of FePO4. The prepared samples were characterized by X-ray diffraction （XRD）, field emission scanning electron micro- scope （FESEM）, energy-dispersive spectroscopy （EDS）, and transmission electron microscopy （TEM）. The XRD and TEM results suggest that both the pristine and the coated materials have a hexagonal layered structure, and the FePO4 coating layer does not make any major change in the crystal structure. The FePO4-coated sample exhibits both improved initial discharge capacity and columbic efficiency compared to the pristine one. More significantly, the FePO4 coating layer has a much positive influence on the cycling perfor- mance. The FePO4-coated sample exhibits capacity reten- tion of 82 % after 100 cycles at 0.5℃ between 2.0 and 4.8 V, while only 28 % for the pristine one at the same charge-discharge condition. The electrochemical impe- dance spectroscopy （EIS） results indicate that this improved cycling performance could be ascribed to the presence of FePO4 on the surface of Li[Li0.2Ni0.13Co0.13Mno.54102 par- ticle, which helps to protect the cathode from chemical attacks by HF and thus suppresses the large increase in charge transfer resistance.
基金the National Key R&D Program of China(No.2020YFC1808401)the National Natural Science Foundation of China(Nos.22078213,21938006,51973148,and 21776190)+2 种基金cutting-edge technology basic research project of Jiangsu(No.BK20202012)the project supported by the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD).G.P.Z.is also grateful for support from the Project funded by China Postdoctoral Science Foundation(No.2021M702389)Jiangsu Funding Program for Excellent Postdoctoral Talent(No.2022ZB536).
文摘Because of its importance in enhancing charge separation and transfer,built-in electric field engineering has been acknowledged as an effective technique for improving photocatalytic performance.Herein,a stable p–n heterojunction of 2D/2D(2D:twodimensional)Co_(3)O_(4)/ZnIn_(2)S_(4)with a strong built-in electric field is precisely constructed.The Co_(3)O_(4)/ZnIn_(2)S_(4)heterojunction exhibits a higher visible-light photocatalytic hydrogen(H2)evolution rate than the individual components,which is primarily attributed to the synergy effect of improved light absorption,abundant active sites,short charge transport distance,high separation efficiency of photogenerated carriers.Furthermore,the photoelectrochemical studies and density functional theory(DFT)calculation results demonstrate that the enhanced interfacial charge separation and migration induced by the generated built-in electric field are the critical reasons for the boosted photocatalytic performance.This research might pave the way for the rational design and manufacturing of 2D/2D heterojunction photocatalysts with extremely efficient photocatalytic performance for solar energy conversion.
文摘Shock wave is a detriment in the development of supersonic aircrafts;it increases flow drag as well as surface heating from additional friction;it also initiates sonic boom on the ground which precludes supersonic jetliner to fly overland. A shock wave mitigation technique is demonstrated by experiments conducted in a Mach 2.5 wind tunnel. Non-thermal air plasma generated symmetrically in front of a wind tunnel model and upstream of the shock, by on-board 60 Hz periodic electric arc discharge, works as a plasma deflector, it deflects incoming flow to transform the shock from a well-defined attached shock into a highly curved shock structure. In a sequence with increasing discharge intensity, the transformed curve shock increases shock angle and moves upstream to become detached with increasing standoff distance from the model. It becomes diffusive and disappears near the peak of the discharge. The flow deflection increases the equivalent cone angle of the model, which in essence, reduces the equivalent Mach number of the incoming flow, manifesting the reduction of the shock wave drag on the cone. When this equivalent cone angle exceeds a critical angle, the shock becomes detached and fades away. This shock wave mitigation technique helps drag reduction as well as eliminates sonic boom.
文摘We have measured the electric dipole moment of several Scn-C60 molecules (n = 1 - 6) in gaseous phase, by coupling a matrix-assisted laser desorption source to an electric beam deflection setup which is an electric equivalent of the famous Stern Gerlach [1] one. Experimental results are compared to a qualitative charge transfer that occurs between Sc and fullerene.
文摘When the spacecraft flies much faster than the sound speed (~1200 km/h), the airflow disturbances deflected forward from the spacecraft cannot get away from the spacecraft and form a shock wave in front of it. Shock waves have been a detriment for the development of supersonic aircrafts, which have to overcome high wave drag and surface heating from additional friction. Shock wave also produces sonic booms. The noise issue raises environmental concerns, which have precluded routine supersonic flight over land. Therefore, mitigation of shock wave is essential to advance the development of supersonic aircrafts. A plasma mitigation technique is studied. A theory is presented to show that shock wave structure can be modified via flow deflection. Symmetrical deflection evades the need of exchanging the transverse momentum between the flow and the deflector. The analysis shows that the plasma generated in front of the model can effectively deflect the incoming flow. A non-thermal air plasma, generated by on-board 60 Hz periodic electric arc discharge in front of a wind tunnel model, was applied as a plasma deflector for shock wave mitigation technique. The experiment was conducted in a Mach 2.5 wind tunnel. The results show that the air plasma was generated symmetrically in front of the wind tunnel model. With increasing discharge intensity, the plasma deflector transforms the shock from a welldefined attached shock into a highly curved shock structure with increasing standoff distance from the model;this curved shock has increased shock angle and also appears in increasingly diffused form. In the decay of the discharge intensity, the shock front is first transformed back to a well-defined curve shock, which moves downstream to become a perturbed oblique shock;the baseline shock front then reappears as the discharge is reduced to low level again. The experimental observations confirm the theory. The steady of the incoming flow during the discharge cycle is manifested by the repeat of the baseline shock front.
文摘This work reveals essential details of plasma-surface interaction in atmospheric air that are important for a wide range of applications, beginning from airflow control and up to the high-voltage insulation. The paper discusses experimental data characterizing dynamics of development and kinetics of energy coupling in surface dielectric barrier discharge (SDBD), atmospheric air plasmas sustained over dielectric surfaces, over a wide range of time scales. The experiments have been conducted using microsecond pulse voltage waveform of single and alternating polarities. Time-resolved discharge development and mechanisms of coupling with quiescent air are analyzed using nanosecond gate camera imaging, electrical measurements, and original surface charge sensors. The results demonstrate several new, critically important processes overlooked in previous studies. Specifically, it is shown that SDBD plasmas energy release may be significantly increased by using an optimized waveform.
基金Chinese Academy of Sciences(QYZDB-SSWSYS038)National Natural Science Foundation of China(11674178,11774340,91750205,61705227)+1 种基金K.C.Wong Education Foundation(GJTD-2018-08)Jilin Provincial Science&Technology Development Project(20180414019GH)。
文摘Localized surface plasmon resonance(LSPR)of nanostructures and the interfacial charge transfer(CT)of semiconductor materials play essential roles in the study of optical and photoelectronic properties.In this paper,a composite substrate of Ag2S quantum dots(QDs)coated plasmonic Au bowtie nanoantenna(BNA)arrays with a metalinsulator-metal(MIM)configuration was built to study the synergistic effect of LSPR and interfacial CT using surface-enhanced Raman scattering(SERS)in the near-infrared(NIR)region.The Au BNA array structure with a large enhancement of the localized electric field(E-field)strongly enhanced the Raman signal of adsorbed p-aminothiophenol(PATP)probe molecules.Meanwhile,the broad enhanced spectral region was achieved owing to the coupling of LSPR The as-prepared Au BNA array structure facilitated enhancements of the excitation as well as the emission of Raman signal simultaneously,which was established by finite-difference time-domain simulation.Moreover,Ag2S semiconductor QDs were introduced into the BNA/PATP system to further enhance Raman signals,which benefited from the interfacial CT resonance in the BNA/Ag2S-QDs/PATP system.As a result,the Raman signals of PATP in the BNA/Ag2S-QDs/PATP system were strongly enhanced under 785 nm laser excitation due to the synergistic effect of E-field enhancement and interfacial CT.Furthermore,the SERS polarization dependence effeas of the BNA/Ag2S-QDs/PATP system were also investigated.The SERS spectra indicated that the polarization dependence of the substrate increased with decreasing polarization angles(θpola)of excitation from p-polarized(θpola=90°)excitation to s-polarized(θpola=0°)excitation.This study provides a strategy using the synergistic effect of interfacial CT and E-field enhancement for SERS applications and provides a guidance for the development of SERS study on semiconductor QD-based plasmonic substrates,and can be farther extended to other material-nanostructure systems for various optoelectronic and sensing applications.
