The photocatalytic degradation of norfloxacin by bismuth tungstate(Bi2WO6)with different hierarchical architectures wasinvestigated under visible light irradiation.Bi2WO6was prepared by hydrothermal method with the re...The photocatalytic degradation of norfloxacin by bismuth tungstate(Bi2WO6)with different hierarchical architectures wasinvestigated under visible light irradiation.Bi2WO6was prepared by hydrothermal method with the reaction solution pH rangingfrom4to11.The relatively ultrathin Bi2WO6nanoflakes prepared at pH4showed excellent adsorption and photodegradationefficiency towards norfloxacin.The characterization results showed that Bi2WO6prepared at pH4had a larger specific area andfaster photo-generated carrier separation rate.The decay rate reached the maximum in weak alkaline reaction solution,which couldbe attributed to the presence of moderate OH-anions.The present study demonstrated that the smaller size of Bi2WO6could be anefficient photocatalyst on the degradation of norfloxacin in the aquatic environment.展开更多
Using renewable energy to drive carbon dioxide reduction reaction(CO_(2)RR)electrochemically into chemicals with high energy density is an efficient way to achieve carbon neutrality,where the effective utilization of ...Using renewable energy to drive carbon dioxide reduction reaction(CO_(2)RR)electrochemically into chemicals with high energy density is an efficient way to achieve carbon neutrality,where the effective utilization of CO_(2) and the storage of renewable energy are realized.The reactivity and selectivity of CO_(2)RR depend on the structure and composition of the catalyst,applied potential,electrolyte,and pH of the solution.Besides,multiple electron and proton transfer steps are involved in CO_(2)RR,making the reaction pathways even more complicated.In pursuit of molecular-level insights into the CO_(2)RR processes,in situ vibrational methods including infrared,Raman and sum frequency generation spectroscopies have been deployed to monitor the dynamic evolution of catalyst structure,to identify reactive intermediates as well as to investigate the effect of local reaction environment on CO_(2)RR performance.This review summarizes key findings from recent electrochemical vibrational spectrosopic studies of CO_(2)RR in addressing the following issues:the CO_(2)RR mechanisms of different pathways,the role of surface-bound CO species,the compositional and structural effects of catalysts and electrolytes on CO_(2)RR activity and selectivity.Our perspectives on developing high sensitivity wide-frequency infrared spectroscopy,coupling different spectroelectrochemical methods and implementing operando vibrational spectroscopies to tackle the CO_(2)RR process in pilot reactors are offered at the end.展开更多
Molecular frame photoemission is a very sensitive probe of the photoionization (PI) dynamics of molecules. This paper reports a comparative study of non-resonant and resonant photoionization of D2 induced by VUV cir...Molecular frame photoemission is a very sensitive probe of the photoionization (PI) dynamics of molecules. This paper reports a comparative study of non-resonant and resonant photoionization of D2 induced by VUV circularly polarized synchrotron radiation at SOLEIL at the level of the molecular frame photoelectron angular distributions (MFPADs). We use the vector correlation method which combines imaging and time-of-flight resolved electron-ion coincidence techniques, and a generalized formalism for the expression of the Ⅰ(χ, θe, Фe) MFPADs, where χ is the orientation of the molecular axis with respect to the light quantization axis and (θe, Фe) the electron emission direction in the molecular frame. Selected MFPADs for a molecule aligned parallel or perpendicular to linearly polarized light, or perpendicular to the propagation axis of circularly polarized light, are presented for dissociative photoionization (DPI) of D2 at two photon excitation energies, hv=19 eV, where direct PI is the only channel opened, and hv=32.5 eV, i.e. in the region involving resonant excitation of Q1 and Q2 doubly excited state series. We discuss in particular the properties of the circular dichroism characterizing photoemission in the molecular frame for direct and resonant PI. In the latter case, a remarkable behavior is observed which may be attributed to the interference occurring between undistinguishable autoionization decay channels.展开更多
Laser lipolysis can effectively treat obesity and its associated diseases, such as hypertension, fatty liver, and hyperlipidemia. However, currently available invasive laser lipolysis, which transmits laser to a fiber...Laser lipolysis can effectively treat obesity and its associated diseases, such as hypertension, fatty liver, and hyperlipidemia. However, currently available invasive laser lipolysis, which transmits laser to a fiber-optic catheter inserted into the subcutaneous tissue for irradiation through an incision, may cause hematomas, infections, and empyrosis. The current study presents a novel, noninvasive approach for laser lipolysis, which directly irradiates the intact skin surface without an incision and preferentially targets adipose tissue at the near-infrared band. High laser energy is necessary to damage adipocytes; however, this may carbonate and burn the dermis. Therefore, the introduction of skin cooling is essential to avoid unwanted hyperthermal injury and improve the threshold of radiant exposure. In the current study, we investigated a novel noninvasive approach assisted with skin cooling by establishing a homogeneous multi-layer skin model. In this method, light propagation in the skin was simulated by using the Monte Carlo method. Skin cooling was employed before laser irradiation to protect the epidermis from thermal damage, which was treated as a boundary condition based on Newton's law. The numerical results showed that the photons were deposited in the adipose layer more than in the other layers. Laser can effectively destroy adipose tissue at an energy density of >200 J/cm^2 at 1210 nm wavelength, whereas at least 300 J/cm^2 is required at 1064 nm to achieve the same effect. In this experiment, at >5 s pulse width, the selectivity of adipose was not obvious. Moreover, the results indicated that 60 ms R134a or R404a spray can effectively reduce the temperature of the epidermis. R404a exhibited a stronger cooling effect than R134a. Cold air cooling at -10 °C for 10 s could effectively decrease the skin temperature, and deeper cooling could be achieved by cold air cooling compared with cryogen spray cooling.展开更多
基金Projects(51579096,51222805,51521006,51508175) supported by the National Natural Science Foundation of ChinaProject supported by the National Program for Support of Top-Notch Young Professionals of China+1 种基金Project(NCET–11–0129) supported by the Program for New Century Excellent Talents in University from the Ministry of Education of ChinaProject(CX2015B095) supported by the Hunan Province Innovation Foundation for Postgraduate,China
文摘The photocatalytic degradation of norfloxacin by bismuth tungstate(Bi2WO6)with different hierarchical architectures wasinvestigated under visible light irradiation.Bi2WO6was prepared by hydrothermal method with the reaction solution pH rangingfrom4to11.The relatively ultrathin Bi2WO6nanoflakes prepared at pH4showed excellent adsorption and photodegradationefficiency towards norfloxacin.The characterization results showed that Bi2WO6prepared at pH4had a larger specific area andfaster photo-generated carrier separation rate.The decay rate reached the maximum in weak alkaline reaction solution,which couldbe attributed to the presence of moderate OH-anions.The present study demonstrated that the smaller size of Bi2WO6could be anefficient photocatalyst on the degradation of norfloxacin in the aquatic environment.
文摘Using renewable energy to drive carbon dioxide reduction reaction(CO_(2)RR)electrochemically into chemicals with high energy density is an efficient way to achieve carbon neutrality,where the effective utilization of CO_(2) and the storage of renewable energy are realized.The reactivity and selectivity of CO_(2)RR depend on the structure and composition of the catalyst,applied potential,electrolyte,and pH of the solution.Besides,multiple electron and proton transfer steps are involved in CO_(2)RR,making the reaction pathways even more complicated.In pursuit of molecular-level insights into the CO_(2)RR processes,in situ vibrational methods including infrared,Raman and sum frequency generation spectroscopies have been deployed to monitor the dynamic evolution of catalyst structure,to identify reactive intermediates as well as to investigate the effect of local reaction environment on CO_(2)RR performance.This review summarizes key findings from recent electrochemical vibrational spectrosopic studies of CO_(2)RR in addressing the following issues:the CO_(2)RR mechanisms of different pathways,the role of surface-bound CO species,the compositional and structural effects of catalysts and electrolytes on CO_(2)RR activity and selectivity.Our perspectives on developing high sensitivity wide-frequency infrared spectroscopy,coupling different spectroelectrochemical methods and implementing operando vibrational spectroscopies to tackle the CO_(2)RR process in pilot reactors are offered at the end.
文摘Molecular frame photoemission is a very sensitive probe of the photoionization (PI) dynamics of molecules. This paper reports a comparative study of non-resonant and resonant photoionization of D2 induced by VUV circularly polarized synchrotron radiation at SOLEIL at the level of the molecular frame photoelectron angular distributions (MFPADs). We use the vector correlation method which combines imaging and time-of-flight resolved electron-ion coincidence techniques, and a generalized formalism for the expression of the Ⅰ(χ, θe, Фe) MFPADs, where χ is the orientation of the molecular axis with respect to the light quantization axis and (θe, Фe) the electron emission direction in the molecular frame. Selected MFPADs for a molecule aligned parallel or perpendicular to linearly polarized light, or perpendicular to the propagation axis of circularly polarized light, are presented for dissociative photoionization (DPI) of D2 at two photon excitation energies, hv=19 eV, where direct PI is the only channel opened, and hv=32.5 eV, i.e. in the region involving resonant excitation of Q1 and Q2 doubly excited state series. We discuss in particular the properties of the circular dichroism characterizing photoemission in the molecular frame for direct and resonant PI. In the latter case, a remarkable behavior is observed which may be attributed to the interference occurring between undistinguishable autoionization decay channels.
基金financially supported by the National Natural Science Foundation of China (Grant No.51336006 and 51727811)
文摘Laser lipolysis can effectively treat obesity and its associated diseases, such as hypertension, fatty liver, and hyperlipidemia. However, currently available invasive laser lipolysis, which transmits laser to a fiber-optic catheter inserted into the subcutaneous tissue for irradiation through an incision, may cause hematomas, infections, and empyrosis. The current study presents a novel, noninvasive approach for laser lipolysis, which directly irradiates the intact skin surface without an incision and preferentially targets adipose tissue at the near-infrared band. High laser energy is necessary to damage adipocytes; however, this may carbonate and burn the dermis. Therefore, the introduction of skin cooling is essential to avoid unwanted hyperthermal injury and improve the threshold of radiant exposure. In the current study, we investigated a novel noninvasive approach assisted with skin cooling by establishing a homogeneous multi-layer skin model. In this method, light propagation in the skin was simulated by using the Monte Carlo method. Skin cooling was employed before laser irradiation to protect the epidermis from thermal damage, which was treated as a boundary condition based on Newton's law. The numerical results showed that the photons were deposited in the adipose layer more than in the other layers. Laser can effectively destroy adipose tissue at an energy density of >200 J/cm^2 at 1210 nm wavelength, whereas at least 300 J/cm^2 is required at 1064 nm to achieve the same effect. In this experiment, at >5 s pulse width, the selectivity of adipose was not obvious. Moreover, the results indicated that 60 ms R134a or R404a spray can effectively reduce the temperature of the epidermis. R404a exhibited a stronger cooling effect than R134a. Cold air cooling at -10 °C for 10 s could effectively decrease the skin temperature, and deeper cooling could be achieved by cold air cooling compared with cryogen spray cooling.