This short review paper aims at assembling the present state of the art of the multiuses of metal oxides in heterogeneous catalysis, concerning liquid and gaseous phases of the reactant mixtures on solid catalysts. It...This short review paper aims at assembling the present state of the art of the multiuses of metal oxides in heterogeneous catalysis, concerning liquid and gaseous phases of the reactant mixtures on solid catalysts. It includes the description of the main types of metal oxide catalysts, of their various preparation procedures and of the main reactions catalysed by them (acid-base type, selective and total oxidations, bi-functional catalysis, photocatalysis, biomass treatments, environmental catalysis and some of the numerous industrial applications). Challenges and prospectives are also discussed.展开更多
When a proton reduction cocatalyst is loaded on an n-type semiconductor for photocatalytic overall water splitting(POWS),the location of water oxidation sites is generally considered at the surface of the semiconducto...When a proton reduction cocatalyst is loaded on an n-type semiconductor for photocatalytic overall water splitting(POWS),the location of water oxidation sites is generally considered at the surface of the semiconductor due to upward band-bending of n-type semiconductor which may ease the transfer of the photogenerated holes to the surface.However,this is not the case for Pt/SrTiO_(3),a model semiconductor based photocatalyst for POWS.It was found that the photogenerated holes are more readily accumulated at the interface between Pt cocatalyst and SrTiO_(3) photocatalyst as probed by photo-oxidative deposition of PbO_(2),indicating that the water oxidation sites are located at the interface between Pt and SrTiO_(3).Electron paramagnetic resonance and scanning transmission electron microscope studies suggest that the interfacial oxygen atoms between Pt and SrTiO_(3) in Pt/SrTiO_(3) after POWS are more readily lost to form oxygen vacancies upon vacuum heat treatment,regardless of Pt loading by photodeposition or impregnation methods,which may serve as additional support for the location of the active sites for water oxidation at the interface.Density functional theory calculations also suggest that the oxygen evolution reaction more readily occurs at the interfacial sites with the lowest overpotential.These experimental and theoretical studies reveal that the more active sites for water oxidation are located at the interface between Pt and SrTiO_(3),rather than on the surface of SrTiO_(3).Hence,the tailor design and control of the interfacial properties are extremely important for the achievement or improvement of the POWS on cocatalyst loaded semiconductor photocatalyst.展开更多
Two-dimensional(2D)carbon nitride(CN)photocatalysts are attracting extensive attention owing to their excellent photocatalytic properties.In this study,we successfully prepared CN materials with heterogeneous structur...Two-dimensional(2D)carbon nitride(CN)photocatalysts are attracting extensive attention owing to their excellent photocatalytic properties.In this study,we successfully prepared CN materials with heterogeneous structures via hydrothermal treatment,high-temperature roasting,ball milling,sintering,and other processes.Benefitting from interface interactions in hybrid architectures,the CN photocatalysts exhibited high photocatalytic activity.The rate of hydrogen production using these CN photocatalysts reached 17028.82μmol h^(−1)g^(−1),and the apparent quantum efficiency was 11.2%at 420 nm.The ns-level time-resolved photoluminescence(PL)spectra provided information about the time-averaged lifetime of fluorescence charge carriers;the lifetime of the charge carriers causing the fluorescence of CN reached 9.99 ns.Significantly,the CN photocatalysts displayed satisfactory results in overall water splitting without the addition of sacrificial agents.The average hydrogen and oxygen production rates were 270.95μmol h^(−1)g^(−1)and 115.21μmol h^(−1)g^(−1)in 7 h,respectively,which were promising results for the applications of the catalysts in overall water splitting processes.We investigated the high efficiency of the prepared CN photocatalysts via a series of tests(UV-vis diffuse reflectance spectroscopy,photocurrent response measurements,PL emission spectroscopy,time-resolved PL spectroscopy,and Brunauer-Emmett-Teller analysis).Furthermore,the Mott-Schottky plot and current-voltage curve were acquired via electrochemical tests.The fabricated CN photocatalyst had a small p-n junction in its heterogeneous structure,which further enhanced its photocatalytic efficiency.Therefore,this work can promote the development of CN photocatalysts.展开更多
Herein, novel plasmonic Bi metal in situ deposited in reduced Ti O2 microspheres(Bi@R-Ti O2) are fabricated via a bimetallic MOF-derived synthesized strategy by adjusting the synthesizing temperature. Different charac...Herein, novel plasmonic Bi metal in situ deposited in reduced Ti O2 microspheres(Bi@R-Ti O2) are fabricated via a bimetallic MOF-derived synthesized strategy by adjusting the synthesizing temperature. Different characterization techniques, including XRD, SEM, TEM, XPS, DRS, PL, EIS, and photocurrent generation, are performed to investigate the structural and optical properties of the as-prepared samples. The results indicate that the Bi particles are generated inside and outside of reduced Ti O2 microspheres via the reduction of Ti4+ and Bi3+ by ethylene glycol. When the annealing temperature is controlled at 300 o C, the corresponding Bi@R-Ti O2-300 sample with an appropriate amount of Bi nanoparticles exhibits the highest full solar spectrum photocatalytic oxygen evolution activity(4728.709 μmol h–1 g–1), which is 5.9 and 9.5 times higher than that of pure Ti O2 and Bi-Ti bimetal organic frameworks(Bi-Ti-MOFs). Several reasons are suggested for the above results:(1) Bi metal behaves as an "electron acceptor" to accelerate the charge carrier transfer from Ti O2 to Bi;(2) The surface plasmon resonance effect of loaded metallic Bi particles can enhance the visible and NIR light absorption capacity;(3) The generation of Ti3+ further narrows the band gap of TiO2.展开更多
Full-spectrum photofixation of N_(2) with remarkable NH_(3) production rate of 228μmol/(g·h)was achieved by W atoms doped Ti_(3)C_(2)T_(x)MXene(W/Ti_(3)C_(2)T_(x)-U)catalyst without sacrificial agents at room te...Full-spectrum photofixation of N_(2) with remarkable NH_(3) production rate of 228μmol/(g·h)was achieved by W atoms doped Ti_(3)C_(2)T_(x)MXene(W/Ti_(3)C_(2)T_(x)-U)catalyst without sacrificial agents at room temperature.The effects of W doping and ultrasonic intercalation of Ti_(3)C_(2)T_(x)MXene were studied.Scanning transmission electron microscope,electron spin resonance spectra,X-ray photoemission spectroscopy,UV-Vis spectrophotometer,temperature programmed adsorption analyzer and density functional theory calculation were used to characterize the obtained catalysts.Results showed that Ti_(3)C_(2)T_(x)MXene harvested ultraviolet-visible and near-infrared light to generate hot electrons.In addition,the doped W atoms played an effective role in adsorbing and activating N_(2) molecules by donating electrons to the anti-bonding orbital of N_(2) molecules to elongate the bond length of N≡N.展开更多
Simultaneous generation of H_(2) fuel and value-added chemicals has attracted increasing attention since the photogenerated electrons and holes can be both employed to convert solar light into chemical energy.Herein,f...Simultaneous generation of H_(2) fuel and value-added chemicals has attracted increasing attention since the photogenerated electrons and holes can be both employed to convert solar light into chemical energy.Herein,for realizing UV-visible-NIR light driven dehydrogenation of benzyl alcohol(BA)into benzaldehydes(BAD)and H_(2),a novel localized surface plasmon resonance(LSPR)enhanced S-scheme heterojunction was designed by combining noble-metal-free plasmon MoO_(3-x) as oxidation semiconductor and Zn_(0.1)Cd_(0.9)S as reduction semiconductor.The photoredox system of Zn_(0.1)Cd_(0.9)S/MoO_(3-x) displayed an unconventional reaction model,in which the BA served as both electron donor and acceptor.The S-scheme charge transfer mechanism induced by the formed internal electric field enhanced the redox ability of charge carriers thermodynamically and boosted charge separation kinetically.Moreover,due to the LSPR effect of MoO_(3-x) nanosheets,Zn_(0.1)Cd_(0.9)S/MoO_(3-x) photocatalysts exhibited strong absorption in the region of full solar spectrum.Therefore,the Zn_(0.1)Cd_(0.9)S/MoO_(3-x) composite generated H_(2) and BAD simultaneously via selective oxidation of BA with high production(34.38 and 33.83 mmol×g^(–1) for H_(2) and BAD,respectively)upon full solar illumination.Even under NIR light irradiation,the H_(2) production rate could up to 94.5 mmol×g^(–1)×h^(–1).In addition,the Zn_(0.1)Cd_(0.9)S/MoO_(3-x) composite displayed effective photocatalytic H_(2) evolution rate up to 149.2 mmol×g^(–1)×h^(–1) from water,which was approximate 6 times that of pure Zn_(0.1)Cd_(0.9)S.This work provides a reference for rational design of plasmonic S-scheme heterojunction photocatalysts for coproduction of high-value chemicals and solar fuel production.展开更多
Exploring low-cost and highly active photocatalysts is very urgent to accomplish complete removal of phenolic contaminants and overcome the limitations of the existing photocatalysts.In this study,we designed and synt...Exploring low-cost and highly active photocatalysts is very urgent to accomplish complete removal of phenolic contaminants and overcome the limitations of the existing photocatalysts.In this study,we designed and synthesized noble metal-free TiO2 photocatalysts by introducing bismuth nanoparticles as modifiers of a TiO2 single crystal(Bi-SCTiO2).The Bi-SCTiO2 can make full use of the synergistic effect of a small band overlap and low charge carrier density(Bi)with a high conductivity(single crystal),significantly boosting the separation and migration of the photogenerated charge pairs.Therefore,the Bi-SCTiO2 photocatalyst exhibits a significantly enhanced degradation rate(12 times faster)of 4-nitrophenol than a TiO2 single crystal under simulated sunlight irradiation.Notably,the complete removal of phenolic contaminants is achieved in various water matrices,which not only successfully overcomes the incomplete degradation in many reported photocatalytic systems,but also manifests a significant practical potential for sewage disposal.Therefore,this work presents a new insight in designing and constructing noble metal-free decorated semiconductor single-crystal photocatalysts with excellent activity and cyclability.展开更多
Visible light induced titanium dioxide (TiO2) pillared montmorillonite clay (MMT) photocatalyst coupling-doped with S and N elements was prepared by the two-step ad- sorption method.The photocatalyst was characterized...Visible light induced titanium dioxide (TiO2) pillared montmorillonite clay (MMT) photocatalyst coupling-doped with S and N elements was prepared by the two-step ad- sorption method.The photocatalyst was characterized by X-ray photoelectron spectros- copy (XPS) and ultraviolet-visible (UV-vis) absorption spectroscopy.The photocatalysic ef- ficacy of the prepared photocatalyst for degrading gaseous formaldehyde was evaluated under visible light irradiation.The degrading rate of gaseous formaldehyde is nearly 85% in 300 min visible light irradiation.The results demonstrate that the much higher visible light photocatalytic activity of the photocatalyst is due to the synergistic effects of coupling- doping of S and N elements to TiO2,extensive specific surface area of MMT and quantum sized efficacy between layers of MMT.展开更多
Water vapor in the earth′s upper atmosphere plays a crucial role in the radiative balance, hydrological process, and climate change. Based on the latest moderate-resolution imaging spectroradiometer(MODIS) data, this...Water vapor in the earth′s upper atmosphere plays a crucial role in the radiative balance, hydrological process, and climate change. Based on the latest moderate-resolution imaging spectroradiometer(MODIS) data, this study probes the spatio-temporal variations of global water vapor content in the past decade. It is found that overall the global water vapor content declined from 2003 to 2012(slope b = –0.0149, R = 0.893, P = 0.0005). The decreasing trend over the ocean surface(b = –0.0170, R = 0.908, P = 0.0003) is more explicit than that over terrestrial surface(b = –0.0100, R = 0.782, P = 0.0070), more significant over the Northern Hemisphere(b = –0.0175, R = 0.923, P = 0.0001) than that over the Southern Hemisphere(b = –0.0123, R = 0.826, P = 0.0030). In addition, the analytical results indicate that water vapor content are decreasing obviously between latitude of 36°N and 36°S(b = 0.0224, R = 0.892, P = 0.0005), especially between latitude of 0°N and 36°N(b = 0.0263, R = 0.931, P = 0.0001), while the water vapor concentrations are increasing slightly in the Arctic regions(b = 0.0028, R = 0.612, P = 0.0590). The decreasing and spatial variation of water vapor content regulates the effects of carbon dioxide which is the main reason of the trend in global surface temperatures becoming nearly flat since the late 1990 s. The spatio-temporal variations of water vapor content also affect the growth and spatial distribution of global vegetation which also regulates the global surface temperature change, and the climate change is mainly caused by the earth's orbit position in the solar and galaxy system. A big data model based on gravitational-magmatic change with the solar or the galactic system is proposed to be built for analyzing how the earth's orbit position in the solar and galaxy system affects spatio-temporal variations of global water vapor content, vegetation and temperature at large spatio-temporal scale. This comprehensive examination of water vapor changes promises a holistic understanding of the global climate change and potential underlying mechanisms.展开更多
A Z-scheme is a promising approach to achieve broad-spectrum photocatalysis. Integration of TiO2 with another semiconductor with a band gap of -1.0 eV would be ideal to harvest both ultraviolet and visible-near infrar...A Z-scheme is a promising approach to achieve broad-spectrum photocatalysis. Integration of TiO2 with another semiconductor with a band gap of -1.0 eV would be ideal to harvest both ultraviolet and visible-near infrared light for photocatalysis; however, most narrow-bandgap semiconductors have straddling band structure alignments with TiO2, constituting an obstacle to forming the Z-scheme for photocatalytic hydrogen production. In this communication, we demonstrate Ag2S as a model system where the energy band upshift of the narrow-bandgap semiconductor that shares an interface with a metal can overcome this limitation. To fabricate the design, we developed a unique approach to synthesize Ag2S-Ag-TiO2 hybrid structures. The obtained ternary hybrid structures exhibited dramatically enhanced performance in photocatalytic hydrogen pro- duction under full-spectrum light illumination. The activities were significantly higher than the sum of those of Ag2S-Ag-TiO2 structures under λ〈 400 nm and λ 〉 400 nm irradiation as well as those of their counterparts under any light illumination conditions.展开更多
The energy crisis and global warming become severe issues. Solar-driven CO2 reduction provides a promising route to confront the predicaments, which has received much attention. The photoelectrochemical(PEC) process...The energy crisis and global warming become severe issues. Solar-driven CO2 reduction provides a promising route to confront the predicaments, which has received much attention. The photoelectrochemical(PEC) process,which can integrate the merits of both photocatalysis and electrocatalysis, boosts splendid talent for CO2 reduction with high efficiency and excellent selectivity. Recent several decades have witnessed the overwhelming development of PEC CO2 reduction. In this review, we attempt to systematically summarize the recent advanced design for PEC CO2 reduction. On account of basic principles and evaluation parameters, we firstly highlight the subtle construction for photocathodes to enhance the efficiency and selectivity of CO2 reduction, which includes the strategies for improving light utilization, supplying catalytic active sites and steering reaction pathway.Furthermore, diversiform novel PEC setups are also outlined.These exploited setups endow a bright window to surmount the intrinsic disadvantages of photocathode, showing promising potentials for future applications. Finally, we underline the challenges and key factors for the further development of PEC CO2 reduction that would enable more efficient designs for setups and deepen systematic understanding for mechanisms.展开更多
The field entropy of the system with two moving atoms interacting with the coherent state is investigated by means of the full quantum theory. Under the different initial states with two atoms, the influences of the l...The field entropy of the system with two moving atoms interacting with the coherent state is investigated by means of the full quantum theory. Under the different initial states with two atoms, the influences of the light field intensity and the atomic motion on the field entropy are discussed. The results indicate that the motion of the atoms leads to strict periodicity in the field entropy evolution. When the two atoms are in the Bell state |β11〉 initially, the system is in a completely disentangled state. For the atoms initially at other Bell states, the field periodically entangles with the atoms.展开更多
文摘This short review paper aims at assembling the present state of the art of the multiuses of metal oxides in heterogeneous catalysis, concerning liquid and gaseous phases of the reactant mixtures on solid catalysts. It includes the description of the main types of metal oxide catalysts, of their various preparation procedures and of the main reactions catalysed by them (acid-base type, selective and total oxidations, bi-functional catalysis, photocatalysis, biomass treatments, environmental catalysis and some of the numerous industrial applications). Challenges and prospectives are also discussed.
文摘When a proton reduction cocatalyst is loaded on an n-type semiconductor for photocatalytic overall water splitting(POWS),the location of water oxidation sites is generally considered at the surface of the semiconductor due to upward band-bending of n-type semiconductor which may ease the transfer of the photogenerated holes to the surface.However,this is not the case for Pt/SrTiO_(3),a model semiconductor based photocatalyst for POWS.It was found that the photogenerated holes are more readily accumulated at the interface between Pt cocatalyst and SrTiO_(3) photocatalyst as probed by photo-oxidative deposition of PbO_(2),indicating that the water oxidation sites are located at the interface between Pt and SrTiO_(3).Electron paramagnetic resonance and scanning transmission electron microscope studies suggest that the interfacial oxygen atoms between Pt and SrTiO_(3) in Pt/SrTiO_(3) after POWS are more readily lost to form oxygen vacancies upon vacuum heat treatment,regardless of Pt loading by photodeposition or impregnation methods,which may serve as additional support for the location of the active sites for water oxidation at the interface.Density functional theory calculations also suggest that the oxygen evolution reaction more readily occurs at the interfacial sites with the lowest overpotential.These experimental and theoretical studies reveal that the more active sites for water oxidation are located at the interface between Pt and SrTiO_(3),rather than on the surface of SrTiO_(3).Hence,the tailor design and control of the interfacial properties are extremely important for the achievement or improvement of the POWS on cocatalyst loaded semiconductor photocatalyst.
文摘Two-dimensional(2D)carbon nitride(CN)photocatalysts are attracting extensive attention owing to their excellent photocatalytic properties.In this study,we successfully prepared CN materials with heterogeneous structures via hydrothermal treatment,high-temperature roasting,ball milling,sintering,and other processes.Benefitting from interface interactions in hybrid architectures,the CN photocatalysts exhibited high photocatalytic activity.The rate of hydrogen production using these CN photocatalysts reached 17028.82μmol h^(−1)g^(−1),and the apparent quantum efficiency was 11.2%at 420 nm.The ns-level time-resolved photoluminescence(PL)spectra provided information about the time-averaged lifetime of fluorescence charge carriers;the lifetime of the charge carriers causing the fluorescence of CN reached 9.99 ns.Significantly,the CN photocatalysts displayed satisfactory results in overall water splitting without the addition of sacrificial agents.The average hydrogen and oxygen production rates were 270.95μmol h^(−1)g^(−1)and 115.21μmol h^(−1)g^(−1)in 7 h,respectively,which were promising results for the applications of the catalysts in overall water splitting processes.We investigated the high efficiency of the prepared CN photocatalysts via a series of tests(UV-vis diffuse reflectance spectroscopy,photocurrent response measurements,PL emission spectroscopy,time-resolved PL spectroscopy,and Brunauer-Emmett-Teller analysis).Furthermore,the Mott-Schottky plot and current-voltage curve were acquired via electrochemical tests.The fabricated CN photocatalyst had a small p-n junction in its heterogeneous structure,which further enhanced its photocatalytic efficiency.Therefore,this work can promote the development of CN photocatalysts.
基金the National Natural Science Foundation of China(51872173 and 51772176)Taishan Scholarship of Young Scholars(tsqn201812068)+2 种基金Natural Science Foundation of Shandong Province(ZR2017JL020)Taishan Scholarship of Climbing Plan(tspd20161006)Key Research and Development Program of Shandong Province(2018GGX102028)~~
文摘Herein, novel plasmonic Bi metal in situ deposited in reduced Ti O2 microspheres(Bi@R-Ti O2) are fabricated via a bimetallic MOF-derived synthesized strategy by adjusting the synthesizing temperature. Different characterization techniques, including XRD, SEM, TEM, XPS, DRS, PL, EIS, and photocurrent generation, are performed to investigate the structural and optical properties of the as-prepared samples. The results indicate that the Bi particles are generated inside and outside of reduced Ti O2 microspheres via the reduction of Ti4+ and Bi3+ by ethylene glycol. When the annealing temperature is controlled at 300 o C, the corresponding Bi@R-Ti O2-300 sample with an appropriate amount of Bi nanoparticles exhibits the highest full solar spectrum photocatalytic oxygen evolution activity(4728.709 μmol h–1 g–1), which is 5.9 and 9.5 times higher than that of pure Ti O2 and Bi-Ti bimetal organic frameworks(Bi-Ti-MOFs). Several reasons are suggested for the above results:(1) Bi metal behaves as an "electron acceptor" to accelerate the charge carrier transfer from Ti O2 to Bi;(2) The surface plasmon resonance effect of loaded metallic Bi particles can enhance the visible and NIR light absorption capacity;(3) The generation of Ti3+ further narrows the band gap of TiO2.
基金supported by the National Natural Science Foundation of China(Nos.51801235,11875258,11505187,51374255,51802356,51572299,41701359)the Natural Science Foundation of Hunan Province,China(No.2020JJ5690)。
文摘Full-spectrum photofixation of N_(2) with remarkable NH_(3) production rate of 228μmol/(g·h)was achieved by W atoms doped Ti_(3)C_(2)T_(x)MXene(W/Ti_(3)C_(2)T_(x)-U)catalyst without sacrificial agents at room temperature.The effects of W doping and ultrasonic intercalation of Ti_(3)C_(2)T_(x)MXene were studied.Scanning transmission electron microscope,electron spin resonance spectra,X-ray photoemission spectroscopy,UV-Vis spectrophotometer,temperature programmed adsorption analyzer and density functional theory calculation were used to characterize the obtained catalysts.Results showed that Ti_(3)C_(2)T_(x)MXene harvested ultraviolet-visible and near-infrared light to generate hot electrons.In addition,the doped W atoms played an effective role in adsorbing and activating N_(2) molecules by donating electrons to the anti-bonding orbital of N_(2) molecules to elongate the bond length of N≡N.
文摘Simultaneous generation of H_(2) fuel and value-added chemicals has attracted increasing attention since the photogenerated electrons and holes can be both employed to convert solar light into chemical energy.Herein,for realizing UV-visible-NIR light driven dehydrogenation of benzyl alcohol(BA)into benzaldehydes(BAD)and H_(2),a novel localized surface plasmon resonance(LSPR)enhanced S-scheme heterojunction was designed by combining noble-metal-free plasmon MoO_(3-x) as oxidation semiconductor and Zn_(0.1)Cd_(0.9)S as reduction semiconductor.The photoredox system of Zn_(0.1)Cd_(0.9)S/MoO_(3-x) displayed an unconventional reaction model,in which the BA served as both electron donor and acceptor.The S-scheme charge transfer mechanism induced by the formed internal electric field enhanced the redox ability of charge carriers thermodynamically and boosted charge separation kinetically.Moreover,due to the LSPR effect of MoO_(3-x) nanosheets,Zn_(0.1)Cd_(0.9)S/MoO_(3-x) photocatalysts exhibited strong absorption in the region of full solar spectrum.Therefore,the Zn_(0.1)Cd_(0.9)S/MoO_(3-x) composite generated H_(2) and BAD simultaneously via selective oxidation of BA with high production(34.38 and 33.83 mmol×g^(–1) for H_(2) and BAD,respectively)upon full solar illumination.Even under NIR light irradiation,the H_(2) production rate could up to 94.5 mmol×g^(–1)×h^(–1).In addition,the Zn_(0.1)Cd_(0.9)S/MoO_(3-x) composite displayed effective photocatalytic H_(2) evolution rate up to 149.2 mmol×g^(–1)×h^(–1) from water,which was approximate 6 times that of pure Zn_(0.1)Cd_(0.9)S.This work provides a reference for rational design of plasmonic S-scheme heterojunction photocatalysts for coproduction of high-value chemicals and solar fuel production.
文摘Exploring low-cost and highly active photocatalysts is very urgent to accomplish complete removal of phenolic contaminants and overcome the limitations of the existing photocatalysts.In this study,we designed and synthesized noble metal-free TiO2 photocatalysts by introducing bismuth nanoparticles as modifiers of a TiO2 single crystal(Bi-SCTiO2).The Bi-SCTiO2 can make full use of the synergistic effect of a small band overlap and low charge carrier density(Bi)with a high conductivity(single crystal),significantly boosting the separation and migration of the photogenerated charge pairs.Therefore,the Bi-SCTiO2 photocatalyst exhibits a significantly enhanced degradation rate(12 times faster)of 4-nitrophenol than a TiO2 single crystal under simulated sunlight irradiation.Notably,the complete removal of phenolic contaminants is achieved in various water matrices,which not only successfully overcomes the incomplete degradation in many reported photocatalytic systems,but also manifests a significant practical potential for sewage disposal.Therefore,this work presents a new insight in designing and constructing noble metal-free decorated semiconductor single-crystal photocatalysts with excellent activity and cyclability.
基金the Scientific Research Foundation for the Returned Overseas Chinese Scholars,State Education Ministry,China(LX-2006-3311)
文摘Visible light induced titanium dioxide (TiO2) pillared montmorillonite clay (MMT) photocatalyst coupling-doped with S and N elements was prepared by the two-step ad- sorption method.The photocatalyst was characterized by X-ray photoelectron spectros- copy (XPS) and ultraviolet-visible (UV-vis) absorption spectroscopy.The photocatalysic ef- ficacy of the prepared photocatalyst for degrading gaseous formaldehyde was evaluated under visible light irradiation.The degrading rate of gaseous formaldehyde is nearly 85% in 300 min visible light irradiation.The results demonstrate that the much higher visible light photocatalytic activity of the photocatalyst is due to the synergistic effects of coupling- doping of S and N elements to TiO2,extensive specific surface area of MMT and quantum sized efficacy between layers of MMT.
基金Under the auspices of National Key Research and Development Program(No.2016YFC0500203)National Natural Science Foundation of China(No.41571427)
文摘Water vapor in the earth′s upper atmosphere plays a crucial role in the radiative balance, hydrological process, and climate change. Based on the latest moderate-resolution imaging spectroradiometer(MODIS) data, this study probes the spatio-temporal variations of global water vapor content in the past decade. It is found that overall the global water vapor content declined from 2003 to 2012(slope b = –0.0149, R = 0.893, P = 0.0005). The decreasing trend over the ocean surface(b = –0.0170, R = 0.908, P = 0.0003) is more explicit than that over terrestrial surface(b = –0.0100, R = 0.782, P = 0.0070), more significant over the Northern Hemisphere(b = –0.0175, R = 0.923, P = 0.0001) than that over the Southern Hemisphere(b = –0.0123, R = 0.826, P = 0.0030). In addition, the analytical results indicate that water vapor content are decreasing obviously between latitude of 36°N and 36°S(b = 0.0224, R = 0.892, P = 0.0005), especially between latitude of 0°N and 36°N(b = 0.0263, R = 0.931, P = 0.0001), while the water vapor concentrations are increasing slightly in the Arctic regions(b = 0.0028, R = 0.612, P = 0.0590). The decreasing and spatial variation of water vapor content regulates the effects of carbon dioxide which is the main reason of the trend in global surface temperatures becoming nearly flat since the late 1990 s. The spatio-temporal variations of water vapor content also affect the growth and spatial distribution of global vegetation which also regulates the global surface temperature change, and the climate change is mainly caused by the earth's orbit position in the solar and galaxy system. A big data model based on gravitational-magmatic change with the solar or the galactic system is proposed to be built for analyzing how the earth's orbit position in the solar and galaxy system affects spatio-temporal variations of global water vapor content, vegetation and temperature at large spatio-temporal scale. This comprehensive examination of water vapor changes promises a holistic understanding of the global climate change and potential underlying mechanisms.
基金Acknowledgements This work was financially supported by the National Basic Research Program of China (973 Program) (No. 2014CB848900), National Natural Science Foundation of China (NSFC) (Nos. 21471141 and 21473166), Recruitment Program of Global Experts, Hundred Talent Program of CAS, and the Fundamental Research Funds for the Central Universities (Nos. WK2060190025, WK2310000035, and WK2090050027). Photoemission spectroscopy experiments were performed at the Catalysis and Surface Physics Endstation at the BL11U beamline in the National Synchrotron Radiation Laboratory (NSRL) in Hefei, China.
文摘A Z-scheme is a promising approach to achieve broad-spectrum photocatalysis. Integration of TiO2 with another semiconductor with a band gap of -1.0 eV would be ideal to harvest both ultraviolet and visible-near infrared light for photocatalysis; however, most narrow-bandgap semiconductors have straddling band structure alignments with TiO2, constituting an obstacle to forming the Z-scheme for photocatalytic hydrogen production. In this communication, we demonstrate Ag2S as a model system where the energy band upshift of the narrow-bandgap semiconductor that shares an interface with a metal can overcome this limitation. To fabricate the design, we developed a unique approach to synthesize Ag2S-Ag-TiO2 hybrid structures. The obtained ternary hybrid structures exhibited dramatically enhanced performance in photocatalytic hydrogen pro- duction under full-spectrum light illumination. The activities were significantly higher than the sum of those of Ag2S-Ag-TiO2 structures under λ〈 400 nm and λ 〉 400 nm irradiation as well as those of their counterparts under any light illumination conditions.
基金financially supported in part by the National Key R&D Program of China (2017YFA0207301)the National Basic Research Program of China (973 Program, 2014CB848900)+5 种基金the National Natural Science Foundation of China (21471141 and U1532135)the CAS Key Research Program of Frontier Sciences (QYZDB-SSW-SLH018)the CAS Interdisciplinary Innovation Team, the Innovative Program of Development Foundation of Hefei Center for Physical Science and Technology (2016FXCX003)the Recruitment Program of Global Experts, the CAS Hundred Talent Program, Anhui Provincial Natural Science Foundation (1708085QB26)China Postdoctoral Science Foundation (BH2060000034)the Fundamental Research Funds for the Central Universities (WK2060190064)
文摘The energy crisis and global warming become severe issues. Solar-driven CO2 reduction provides a promising route to confront the predicaments, which has received much attention. The photoelectrochemical(PEC) process,which can integrate the merits of both photocatalysis and electrocatalysis, boosts splendid talent for CO2 reduction with high efficiency and excellent selectivity. Recent several decades have witnessed the overwhelming development of PEC CO2 reduction. In this review, we attempt to systematically summarize the recent advanced design for PEC CO2 reduction. On account of basic principles and evaluation parameters, we firstly highlight the subtle construction for photocathodes to enhance the efficiency and selectivity of CO2 reduction, which includes the strategies for improving light utilization, supplying catalytic active sites and steering reaction pathway.Furthermore, diversiform novel PEC setups are also outlined.These exploited setups endow a bright window to surmount the intrinsic disadvantages of photocathode, showing promising potentials for future applications. Finally, we underline the challenges and key factors for the further development of PEC CO2 reduction that would enable more efficient designs for setups and deepen systematic understanding for mechanisms.
基金supported by the National Natural Science Foundation of Chinathe Nataral Science Foundation of Inner Mongolia of Chinathe Science Fund of Universiey in Inner Mongolia of China
文摘The field entropy of the system with two moving atoms interacting with the coherent state is investigated by means of the full quantum theory. Under the different initial states with two atoms, the influences of the light field intensity and the atomic motion on the field entropy are discussed. The results indicate that the motion of the atoms leads to strict periodicity in the field entropy evolution. When the two atoms are in the Bell state |β11〉 initially, the system is in a completely disentangled state. For the atoms initially at other Bell states, the field periodically entangles with the atoms.