递归蒙特卡洛(Sequential Monte Carlo,SMC)算法是一种有效降低算法复杂度的次优化算法,该算法嵌入到迭代Turbo接收机中可形成低复杂度、高解调性能的SMC+Turbo MIMO解调接收机.该文针对该解调接收机中的混合型SMC MIMO解调算法,运用动...递归蒙特卡洛(Sequential Monte Carlo,SMC)算法是一种有效降低算法复杂度的次优化算法,该算法嵌入到迭代Turbo接收机中可形成低复杂度、高解调性能的SMC+Turbo MIMO解调接收机.该文针对该解调接收机中的混合型SMC MIMO解调算法,运用动态化参数进行改进.仿真结果表明,动态混合型SMC+Turbo MIMO解调算法可以在不增加算法复杂度的基础上有效地提高一般混合型方案的性能.展开更多
The kinetics and dynamics of photocatalyzed dissociation of ethanol on TiO2(110) sur- face have been studied using the time-dependent and time-resolved femtosecond two-photon photoemission spectroscopy respectively,...The kinetics and dynamics of photocatalyzed dissociation of ethanol on TiO2(110) sur- face have been studied using the time-dependent and time-resolved femtosecond two-photon photoemission spectroscopy respectively, in order to unravel the photochemical properties of ethanol on this prototypical metal oxide surface. By monitoring the time evolution of the photoinduced excited state which is associated with the photocatalyzed dissociation of ethanol on Ti5c sites of Ti02(ll0), the fractal-like kinetics of this surface photocatalytic reaction has been obtgined. The measured photocatalytic dissociation rate on reduced TiO2(l10) is faster than that on the oxidized surface. This is attributed to the larger defect density on the reduced surface which lowers the reaction barrier of the photocatalytic reaction at least methodologically. Possible reasons associated with the defect electrons for the acceleration have been discussed. By performing the interferometric two-pulse corre- lation on ethanol/TiO2(l10) interface, the ultrafast electron dynamics of the excited state has been measured. The analyzed lifetime (24 fs) of the excited state is similar to that on methanol/TiO2(110). The appearance of the excited state provides a channel to mediate the electron transfer between the TiO2 substrate and its environment. Therefore studying its ultrafast electron dynamics may lead to the understanding of the microscopic mechanism of photocatalysis and photoelectrochemical energy conversion on TiO2.展开更多
A surface femtosecond two-photon photoemission (2PPE) spectrometer devoted to the study of ultrafast excited electron dynamics and photochemical kinetics on metal and metal oxide surfaces has been constructed. Low e...A surface femtosecond two-photon photoemission (2PPE) spectrometer devoted to the study of ultrafast excited electron dynamics and photochemical kinetics on metal and metal oxide surfaces has been constructed. Low energy photoelectrons are measured using a hemispherical electron energy analyzer with an imaging detector that allows us to detect the energy and the angular distributions of the photoelectrons simultaneously. A Mach-Zehnder interferom- eter was built for the time-resolved 2PPE (TR-2PPE) measurement to study ultrafast surface excited electron dynamics, which was demonstrated on the Cu(111) surface. A scheme for measuring time-dependent 2PPE (TD-2PPE) spectra has also been developed for studies of surface photochemistry. This technique has been applied to a preliminary study on the photochemical kinetics on ethanol/TiO2(110). We have also shown that the ultrafast dynamics of photoinduced surface excited resonances can be investigated in a reliable way by combining the TR-2PPE and TD-2PPE techniques.展开更多
We constructed two types of copper-doped metal-organic framework(MOF),i.e.,Cu@UiO-66-NH2 and Cu-UiO-66-NH2.In the former,Cu2+ions are impregnated in the pore space of the amine-functionalized,Zr-based UiO-66-NH2;while...We constructed two types of copper-doped metal-organic framework(MOF),i.e.,Cu@UiO-66-NH2 and Cu-UiO-66-NH2.In the former,Cu2+ions are impregnated in the pore space of the amine-functionalized,Zr-based UiO-66-NH2;while in the latter,Cu^2+ions are incorporated to form a bimetal-center MOF,with Zr^4+being partially replaced by Cu2+in the Zr-O oxo-clusters.Ultrafast spectroscopy revealed that the photoinduced relaxation kinetics associated with the ligand-to-cluster charge-transfer state is promoted for both Cudoped MOFs relative to undoped one,but in a sequence of Cu-UiO-66-NH2>Cu@UiO-66-NH2>UiO-66-NH2.Such a sequence turned to be in line with the trend observed in the visible-light photocatalytic hydrogen evolution activity tests on the three MOFs.These findings highlighted the subtle effect of copper-doping location in this Zr-based MOF system,further suggesting that rational engineering of the specific metal-doping location in alike MOF systems to promote the photoinduced charge separation and hence suppress the detrimental charge recombination therein is beneficial for achieving improved performances in MOF-based photocatalysis.展开更多
Solid concentration and particle velocity distributions in the transition section of a Ф 200 mm turbulent fluidized bed (TFB) and a q5200 mrn annulus turbulent fluidized bed (A-TFB) with a Ф 50 mm central standp...Solid concentration and particle velocity distributions in the transition section of a Ф 200 mm turbulent fluidized bed (TFB) and a q5200 mrn annulus turbulent fluidized bed (A-TFB) with a Ф 50 mm central standpipe were measured using a PVBD optical probe. It is concluded that in turbulent regime, the axial distribution of solid concentration in A-TFB was similar to that in TFB, but the former had a shorter transition section. The axial solid concentration distribution, probability density, and power spectral distributions revealed that the standpipe hin- dered the turbulence of gas-solid two-phase flow at a low superficial gas velocity. Consequently, the bottom flow of A-TFB approached the bubbling fluidization pattern. By contrast, the standpipe facilitated the turbulence at a high superficial gas velocity, thus making the bottom flow of A-TFB approach the fast fluidization pattern. Both the particle velocity and solid concentration distribution presented a unimodal distribution in A-TFB and TFB. However, the standpipe at a high gas velocity and in the transition or dilute phase section significantly affected the radial distribution of flow parameters, presenting a bimodal distribution with particle concentration higher near the internal and external walls and in downward flow. Conversely, particle concentration in the middle an- nulus area was lower, and particles flowed upward. This result indicated that the standpipe destroyed the coreannular structure of TFB in the transition and dilute phase sections at a high gas velocity and also improved the particle distribution of TFB. In conclusion, the standpipe improved the fluidization quality and flow homogeneity at high gas velocity and in the transition or dilute phase section, but caused opposite phenomena at low gas velocity and in the dense-phase section.展开更多
文摘The kinetics and dynamics of photocatalyzed dissociation of ethanol on TiO2(110) sur- face have been studied using the time-dependent and time-resolved femtosecond two-photon photoemission spectroscopy respectively, in order to unravel the photochemical properties of ethanol on this prototypical metal oxide surface. By monitoring the time evolution of the photoinduced excited state which is associated with the photocatalyzed dissociation of ethanol on Ti5c sites of Ti02(ll0), the fractal-like kinetics of this surface photocatalytic reaction has been obtgined. The measured photocatalytic dissociation rate on reduced TiO2(l10) is faster than that on the oxidized surface. This is attributed to the larger defect density on the reduced surface which lowers the reaction barrier of the photocatalytic reaction at least methodologically. Possible reasons associated with the defect electrons for the acceleration have been discussed. By performing the interferometric two-pulse corre- lation on ethanol/TiO2(l10) interface, the ultrafast electron dynamics of the excited state has been measured. The analyzed lifetime (24 fs) of the excited state is similar to that on methanol/TiO2(110). The appearance of the excited state provides a channel to mediate the electron transfer between the TiO2 substrate and its environment. Therefore studying its ultrafast electron dynamics may lead to the understanding of the microscopic mechanism of photocatalysis and photoelectrochemical energy conversion on TiO2.
文摘A surface femtosecond two-photon photoemission (2PPE) spectrometer devoted to the study of ultrafast excited electron dynamics and photochemical kinetics on metal and metal oxide surfaces has been constructed. Low energy photoelectrons are measured using a hemispherical electron energy analyzer with an imaging detector that allows us to detect the energy and the angular distributions of the photoelectrons simultaneously. A Mach-Zehnder interferom- eter was built for the time-resolved 2PPE (TR-2PPE) measurement to study ultrafast surface excited electron dynamics, which was demonstrated on the Cu(111) surface. A scheme for measuring time-dependent 2PPE (TD-2PPE) spectra has also been developed for studies of surface photochemistry. This technique has been applied to a preliminary study on the photochemical kinetics on ethanol/TiO2(110). We have also shown that the ultrafast dynamics of photoinduced surface excited resonances can be investigated in a reliable way by combining the TR-2PPE and TD-2PPE techniques.
基金the National Key Research and Development Program on Nano Science and Technology of the Ministry of Science and Technology of China(No.2016YFA0200602 and No.2018YFA0208702)the National Natural Science Foundation of China(No.21573211 and No.21633007)the Anhui Initiative in Quantum Information Technologies(No.AHY090200)。
文摘We constructed two types of copper-doped metal-organic framework(MOF),i.e.,Cu@UiO-66-NH2 and Cu-UiO-66-NH2.In the former,Cu2+ions are impregnated in the pore space of the amine-functionalized,Zr-based UiO-66-NH2;while in the latter,Cu^2+ions are incorporated to form a bimetal-center MOF,with Zr^4+being partially replaced by Cu2+in the Zr-O oxo-clusters.Ultrafast spectroscopy revealed that the photoinduced relaxation kinetics associated with the ligand-to-cluster charge-transfer state is promoted for both Cudoped MOFs relative to undoped one,but in a sequence of Cu-UiO-66-NH2>Cu@UiO-66-NH2>UiO-66-NH2.Such a sequence turned to be in line with the trend observed in the visible-light photocatalytic hydrogen evolution activity tests on the three MOFs.These findings highlighted the subtle effect of copper-doping location in this Zr-based MOF system,further suggesting that rational engineering of the specific metal-doping location in alike MOF systems to promote the photoinduced charge separation and hence suppress the detrimental charge recombination therein is beneficial for achieving improved performances in MOF-based photocatalysis.
基金Supported by the National Natural Science Foundation of China(U1361112,U1162125)
文摘Solid concentration and particle velocity distributions in the transition section of a Ф 200 mm turbulent fluidized bed (TFB) and a q5200 mrn annulus turbulent fluidized bed (A-TFB) with a Ф 50 mm central standpipe were measured using a PVBD optical probe. It is concluded that in turbulent regime, the axial distribution of solid concentration in A-TFB was similar to that in TFB, but the former had a shorter transition section. The axial solid concentration distribution, probability density, and power spectral distributions revealed that the standpipe hin- dered the turbulence of gas-solid two-phase flow at a low superficial gas velocity. Consequently, the bottom flow of A-TFB approached the bubbling fluidization pattern. By contrast, the standpipe facilitated the turbulence at a high superficial gas velocity, thus making the bottom flow of A-TFB approach the fast fluidization pattern. Both the particle velocity and solid concentration distribution presented a unimodal distribution in A-TFB and TFB. However, the standpipe at a high gas velocity and in the transition or dilute phase section significantly affected the radial distribution of flow parameters, presenting a bimodal distribution with particle concentration higher near the internal and external walls and in downward flow. Conversely, particle concentration in the middle an- nulus area was lower, and particles flowed upward. This result indicated that the standpipe destroyed the coreannular structure of TFB in the transition and dilute phase sections at a high gas velocity and also improved the particle distribution of TFB. In conclusion, the standpipe improved the fluidization quality and flow homogeneity at high gas velocity and in the transition or dilute phase section, but caused opposite phenomena at low gas velocity and in the dense-phase section.