Photocatalytic reduction of CO2 with H2 O to syngas is an effective way for producing high value-added chemical feedstocks such as methanol and light olefins in industry.Nevertheless,the precise control of CO/H2 ratio...Photocatalytic reduction of CO2 with H2 O to syngas is an effective way for producing high value-added chemical feedstocks such as methanol and light olefins in industry.Nevertheless,the precise control of CO/H2 ratio from photocatalytic CO2 reduction reaction still poses a great challenge for the further application.Herein,we prepared a series of highly efficient heterostructure based on highly dispersed palladium supported on ultrathin Co Al-layered double hydroxide(LDH).In conjunction with a Ru-complex sensitizer,the molar ratios of CO/H2 can be tuned from 1:0.74 to 1:3 under visible-light irradiation(λ>400 nm).More interestingly,the syngas can be obtained under light irradiation atλ>600 nm.Structure characterization and density functional theory calculations revealed that the remarkable catalytic activity can be due to the supported palladium,which improved the charge transfer efficiency.Meanwhile,more H atoms were used to generate H2 on the supported palladium for further tunable CO/H2 ratio.This work demonstrates a new strategy for harnessing abundant solar-energy to produce syngas from a CO2 feedstock.展开更多
The luminance in the road tunnel threshold zone attracts broad attention due to its enormous energy consumption and direct influence on tunnel transportation security.Current lighting design methods in threshold zones...The luminance in the road tunnel threshold zone attracts broad attention due to its enormous energy consumption and direct influence on tunnel transportation security.Current lighting design methods in threshold zones mostly adopt the reduction coefficient method.However,the determination of reduction coefficient k simply considers tunnel design speed and flow rate,while excluding outside tunnel luminance and threshold zone color temperature and luminance,which have a major impact on driver visual adaptation.Existing problems in the determination of k value are analyzed;a visual performance experiment is utilized;and the reaction time of drivers in changeable outside tunnel luminance and threshold zone color temperature and luminance conditions is obtained;thus,the equations concerning reduction coefficient variation law are derived.In the end,a comparative analysis is made of the k values of the reduction coefficient stipulated by various norms under different color temperature conditions.展开更多
Graphene （GR）-CdS nanocomposites with different weight addition ratios of GR have been assembled by a facile solvothermal treatment. The GR-CdS nanocomposite photocatalyst with an appropriate ratio of GR exhibits en...Graphene （GR）-CdS nanocomposites with different weight addition ratios of GR have been assembled by a facile solvothermal treatment. The GR-CdS nanocomposite photocatalyst with an appropriate ratio of GR exhibits enhanced photoactivity for selective reduction of aromatic nitro compounds to the corresponding aromatic amines in water under visible light irradiation as compared with blank-CdS. The characterization of GR-CdS nanocomposite photocatalysts by a collection of techniques discloses that： i） GR can tune the microscopic morphology of CdS nanoparticles and improve light absorption intensity in the visible light region; ii） GR scaffolds act as an electron reservoir to trap and shuttle the electrons photogenerated from CdS semiconductor under the visible light illumination; iii） the introduction of GR enhances the adsorption capacity of GR-CdS nanocomposites toward the substrates, aromatic nitro compounds. The synergistic effect of these factors should account for the photoactivity advancement of GR-CdS nanocomposites toward the probe reactions. Furthermore, because the photogenerated holes in the system are trapped by the quenching agent ammonium oxalate, the as-obtained GR-CdS photocataiyst is stable during the photocatalytic reduction reactions. A reasonable model has also been proposed to illustrate the reaction mechanism.展开更多
In this manuscript,Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6) nanocomposites was fabricated via an ultrasonic-assisted process.The activity of the as-obtained Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6) nanocomposites for photocatalytic CO_(2) ...In this manuscript,Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6) nanocomposites was fabricated via an ultrasonic-assisted process.The activity of the as-obtained Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6) nanocomposites for photocatalytic CO_(2) reduction was studied under visible light.The as-obtained Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6) nanocomposites show a superior activity for photocatalytic CO_(2) reduction to produce CH4 and CO,with an optimum activity achieved over 0.5 Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6).The obvious superior activity observed over Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6) nanocomposites as compared with bare Cs_(2)AgBiBr_(6) and bare Bi_(2)WO_(6) as well as a mechanical mixture of Cs_(2)AgBiBr_(6) and Bi_(2)WO_(6) can be owe to the fabrication of an efficient S-scheme heterojunction,which accelerates the separation of the photogenerated charge carriers in Cs_(2)AgBiBr_(6) and Bi_(2)WO_(6) without sacrificing the high redox capability of Cs_(2)AgBiBr_(6) and Bi_(2)WO_(6).This work demonstrates that the coupling of two photocatalytic materials with staggered band alignment to form an S-scheme heterojunction is an effective strategy to develop efficient photocatalytic systems and also highlights the promising role of using lead free perovskites in photocatalysis.展开更多
hree kinds of devices of drag reduction are presented swept wingtip,stage by stage swept wingtip and downbend wingtip. The effects of changing geometryparameters of the swept wingtip on the drag reducing are also pres...hree kinds of devices of drag reduction are presented swept wingtip,stage by stage swept wingtip and downbend wingtip. The effects of changing geometryparameters of the swept wingtip on the drag reducing are also presented. Wind-tunnelexperiment results indicate that a properly designed swept wingtip results in an incre-ment in induced efficiency of 4%～ 7% and that swept wingtip can increase longitudinalstatic-stability. Water-tunnel experiment results indicate that the reason for drag re-ducing of swept wingtip is that when the angle of attack is not zero, the strong end vor-tex of the wing is weakened by the combined effect of the leading edge and trailing edgevortices of the swept wingtip.展开更多
Traffic intersections are incredibly dangerous for drivers and pedestrians. Statistics from both Canada and the U.S. show a high number of fatalities and serious injuries related to crashes at intersections. In Canada...Traffic intersections are incredibly dangerous for drivers and pedestrians. Statistics from both Canada and the U.S. show a high number of fatalities and serious injuries related to crashes at intersections. In Canada, during 2019, the National Collision Database shows that 28% of traffic fatalities and 42% of serious injuries occurred at intersections. Likewise, the U.S. National Highway Traffic Administration (NHTSA) found that about 40% of the estimated 5,811,000 accidents in the U.S. during the year studied were intersection-related crashes. In fact, a major survey by the car insurance industry found that nearly 85% of drivers could not identify the correct action to take when approaching a yellow traffic light at an intersection. One major reason for these accidents is the “yellow light dilemma,” the ambiguous situation where a driver should stop or proceed forward when unexpectedly faced with a yellow light. This situation is even further exacerbated by the tendency of aggressive drivers to inappropriately speed up on the yellow just to get through the traffic light. A survey of Canadian drivers conducted by the Traffic Injury Research Foundation found that 9% of drivers admitted to speeding up to get through a traffic light. Another reason for these accidents is the increased danger of making a left-hand turn on yellow. According to the National Highway Traffic Safety Association (NHTSA), left turns occur in approximately 22.2% of collisions—as opposed to just 1.2% for right turns. Moreover, a study by CNN found left turns are three times as likely to kill pedestrians than right turns. The reason left turns are so much more likely to cause an accident is because they take a driver against traffic and in the path of oncoming cars. Additionally, most of these left turns occur at the driver’s discretion—as opposed to the distressingly brief left-hand arrow at busy intersections. Drive Safe Now proposes a workable solution for reducing the number of accidents occurring during a yellow light at intersections. We believe this fairly simple solution will save lives, prevent injuries, reduce damage to public and private property, and decrease insurance costs.展开更多
Semiconductor photocatalytic technology is widely recognized as one of the most promising technologies to solve current energy and environmental crisis, due to its ability to make effective use of solar energy. In rec...Semiconductor photocatalytic technology is widely recognized as one of the most promising technologies to solve current energy and environmental crisis, due to its ability to make effective use of solar energy. In recent years, graphite carbon nitride(g-C3N4), a new type of non-metallic polymer semiconductor photocatalyst, has rapidly become the focus of intense research in the field of photocatalysis because of its suitable bandgap energy, unique structure, and excellent chemical stability. In order to improve its intrinsic shortages of small specific surface area, narrow visible light response range, high electron-hole pair recombination rate, and low photon quantum efficiency, a simple method was utilized to synthesize Br-doped g-C3N4(CN–Br X, X = 5, 10, 20, 30), where X is a percentage mole ratio of NH4 Br to melamine. Experimental results showed that Br atoms were doped into the g-C3N4 lattice by replacing the bonded N atoms in the form of C–N=C, while the derived material retained the original framework of g-C3N4. The interaction of Br element with the g-C3N4 skeleton not only broadened the visible-light response of g-C3N4 to 800 nm with an adjustable band gap, but also greatly promoted the separation efficiency of the photogenerated charge carrier and the surface area. The photocurrent intensity of bare CN and CN–Br X(X = 5, 10, 20, 30) catalysts is calculated to be 1.5, 2.0, 3.1, 6.5, and 1.9 μA, respectively. And their specific surface area is measured to be 9.086, 9.326, 15.137, 13.397, and 6.932 m2/g. As a result, this Br-doped g-C3N4 gives significantly enhanced photocatalytic reduction of Cr(VI), achieving a twice enhancement over g-C3N4, with high stability during prolonged photocatalytic operation compared to bare g-C3N4 under visible light irradiation. Furthermore, an underlying photocatalytic reduction mechanism was proposed based on control experiments using radical scavengers.展开更多
Photo-thermal CO_(2) reduction with methane(CRM)is beneficial for solar energy harvesting and energy storage.The search for efficient photo-thermal catalysts is of great significance.Here,we reveal that group Ⅷ metal...Photo-thermal CO_(2) reduction with methane(CRM)is beneficial for solar energy harvesting and energy storage.The search for efficient photo-thermal catalysts is of great significance.Here,we reveal that group Ⅷ metal catalysts supported by optical material WO_(3) are more effective for photo-thermal CRM,giving catalytic activities with visible light assistance that are 1.4-2.4 times higher than that achieved under thermal conditions.The activity enhancement(1.4-2.4 times)was comparable to that achieved with plasmonic-Au-promoted catalysts(1.7 times).Characterization results indicated that WO_(3) was partially reduced to WO_(3-x) in situ under the reductive CRM reaction atmosphere,and that WO_(3-x) rather than WO_(3) enhanced the activities with visible light assistance.Our method provides a promising approach for improving the activity of catalysts under light irradiation.展开更多
Metal-organic frameworks(MOFs)have shown significant potential as photocatalysts.It has been widely assumed that all catalytic active sites within MOFs are functional in photocatalytic reactions but for a three-dimens...Metal-organic frameworks(MOFs)have shown significant potential as photocatalysts.It has been widely assumed that all catalytic active sites within MOFs are functional in photocatalytic reactions but for a three-dimensional MOF,whether the internal catalytic active sites can effectively absorb light and actively contribute to photocatalytic reactions remains to be explored.In this context,we synthesized a two-dimensional nanosheet MOF(2D-MOF)and a three-dimensional bulk MOF(3D-MOF)composed of Zr^(6) clusters and tetracarboxylic porphyrin(TCPP)by the approach described in the literature.Re(bpy)(CO)^(3)Cl(bpy=2,2’-bipyridine),which has remarkable CO_(2) photoreduction ability,was introduced to the two MOFs to create two new photocatalysts 2D-MOF-Re and 3D-MOF-Re,respectively.Photocatalytic CO_(2) reduction experiments show that based on the equal number of catalytic active sites,the CO turnover number(TON)of 2D-MOF-Re reaches 27.8 in 6 h,which is 50 times that of 3D-MOF-Re.The result shows that certain catalytic active sites inside the bulk MOF are inactive due to the inability to absorb light.This study illuminates the potential of the dimensional reduction approach in the design of photocatalysts to exploit the capabilities fully.展开更多
While photoreduction of CO_(2) to CH 4 is an effective means of producing value-added fuels,common pho-tocatalysts have poor activity and low selectivity in photocatalytic CO_(2)-reduction processes.Even though creati...While photoreduction of CO_(2) to CH 4 is an effective means of producing value-added fuels,common pho-tocatalysts have poor activity and low selectivity in photocatalytic CO_(2)-reduction processes.Even though creating defects is an effective photocatalyst fabrication route to improve photocatalytic activity,there are some challenges with the facile photocatalyst synthesis method.In this work,an O element is in-troduced into a graphitic carbon nitride(CN)skeleton through a precursory ultraviolet light irradiation pretreatment to increase the visible light absorption and enhance the carrier density of this modified non-metal CN photocatalyst;the charge transfer dynamics thereof are also studied through electrochem-ical tests,photoluminescence spectroscopy,and nanosecond transient absorption.We verify that the op-timized sample exhibits lower charge recombination and a suppressed 84 ns electron-trapping lifetime,compared to the 103 ns electron-trapping lifetime of the CN counterpart,and thereby contributes to ro-bust detrapping and a fast transfer of active electrons.Through density functional theory calculations,we find that the improved light absorption and increased electron density are ascribed to O-element doping,which enhances the CO_(2) adsorption energy and improves the CO_(2)-to-CH 4 photoreduction activity;it be-comes 17 times higher than that of the bare CN,and the selectivity is 3.8 times higher than that of CN.Moreover,the optimized sample demonstrates excellent cyclic stability in a 24-hour cycle test.展开更多
High qualityβ-Ga_(2)O_(3)single crystal nanobelts with length of 2−3 mm and width from tens of microns to 132μm were synthesized by carbothermal reduction method.Based on the grown nanobelt with the length of 600μm...High qualityβ-Ga_(2)O_(3)single crystal nanobelts with length of 2−3 mm and width from tens of microns to 132μm were synthesized by carbothermal reduction method.Based on the grown nanobelt with the length of 600μm,the dual-Schottky-junctions coupling device(DSCD)was fabricated.Due to the electrically floating Ga_(2)O_(3)nanobelt region coupling with the double Schottky-junctions,the current I_(S2)increases firstly and rapidly reaches into saturation as increase the voltage V_(S2).The saturation current is about 10 pA,which is two orders of magnitude lower than that of a single Schottky-junction.In the case of solar-blind ultraviolet(UV)light irradiation,the photogenerated electrons further aggravate the coupling physical mechanism in device.I_(S2)increases as the intensity of UV light increases.Under the UV light of 1820μW/cm^(2),I_(S2)quickly enters the saturation state.At V_(S2)=10 V,photo-to-dark current ratio(PDCR)of the device reaches more than 104,the external quantum efficiency(EQE)is 1.6×10^(3)%,and the detectivity(D*)is 7.5×10^(12)Jones.In addition,the device has a very short rise and decay times of 25−54 ms under different positive and negative bias.DSCD shows unique electrical and optical control characteristics,which will open a new way for the application of nanobelt-based devices.展开更多
基金supported by the Fundamental Research Funds for the Central Universities(XK1802-6,XK1902,XK1803-05,12060093063,2312018RC07)the National Natural Science Foundation of China(U1707603,21878008,21625101,20190816)。
文摘Photocatalytic reduction of CO2 with H2 O to syngas is an effective way for producing high value-added chemical feedstocks such as methanol and light olefins in industry.Nevertheless,the precise control of CO/H2 ratio from photocatalytic CO2 reduction reaction still poses a great challenge for the further application.Herein,we prepared a series of highly efficient heterostructure based on highly dispersed palladium supported on ultrathin Co Al-layered double hydroxide(LDH).In conjunction with a Ru-complex sensitizer,the molar ratios of CO/H2 can be tuned from 1:0.74 to 1:3 under visible-light irradiation(λ>400 nm).More interestingly,the syngas can be obtained under light irradiation atλ>600 nm.Structure characterization and density functional theory calculations revealed that the remarkable catalytic activity can be due to the supported palladium,which improved the charge transfer efficiency.Meanwhile,more H atoms were used to generate H2 on the supported palladium for further tunable CO/H2 ratio.This work demonstrates a new strategy for harnessing abundant solar-energy to produce syngas from a CO2 feedstock.
基金Project(51278507)supported by the National Natural Science Foundation of ChinaProject(cstc2017jcyjAX0346)supported by Chongqing Association for Science and Technology,China
文摘The luminance in the road tunnel threshold zone attracts broad attention due to its enormous energy consumption and direct influence on tunnel transportation security.Current lighting design methods in threshold zones mostly adopt the reduction coefficient method.However,the determination of reduction coefficient k simply considers tunnel design speed and flow rate,while excluding outside tunnel luminance and threshold zone color temperature and luminance,which have a major impact on driver visual adaptation.Existing problems in the determination of k value are analyzed;a visual performance experiment is utilized;and the reaction time of drivers in changeable outside tunnel luminance and threshold zone color temperature and luminance conditions is obtained;thus,the equations concerning reduction coefficient variation law are derived.In the end,a comparative analysis is made of the k values of the reduction coefficient stipulated by various norms under different color temperature conditions.
基金supported by the National Natural Science Foundation of China(NSFC)(21173045,20903023)the Award Program for Minjiang Scholar Professorship+3 种基金the Natural Science Foundation(NSF)of Fujian Province for Distinguished Young Investigator(Grant No.2012J06003)the Program for Changjiang Scholars and Innovative Research Team in Universities(PCSIRT0818)the Program for Returned High-Level Overseas Chinese Scholars of Fujian provincethe Project Sponsored by the Scientific Research Foundation for the Returned Overseas Chinese Scholars,State Education Ministry
文摘Graphene （GR）-CdS nanocomposites with different weight addition ratios of GR have been assembled by a facile solvothermal treatment. The GR-CdS nanocomposite photocatalyst with an appropriate ratio of GR exhibits enhanced photoactivity for selective reduction of aromatic nitro compounds to the corresponding aromatic amines in water under visible light irradiation as compared with blank-CdS. The characterization of GR-CdS nanocomposite photocatalysts by a collection of techniques discloses that： i） GR can tune the microscopic morphology of CdS nanoparticles and improve light absorption intensity in the visible light region; ii） GR scaffolds act as an electron reservoir to trap and shuttle the electrons photogenerated from CdS semiconductor under the visible light illumination; iii） the introduction of GR enhances the adsorption capacity of GR-CdS nanocomposites toward the substrates, aromatic nitro compounds. The synergistic effect of these factors should account for the photoactivity advancement of GR-CdS nanocomposites toward the probe reactions. Furthermore, because the photogenerated holes in the system are trapped by the quenching agent ammonium oxalate, the as-obtained GR-CdS photocataiyst is stable during the photocatalytic reduction reactions. A reasonable model has also been proposed to illustrate the reaction mechanism.
文摘In this manuscript,Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6) nanocomposites was fabricated via an ultrasonic-assisted process.The activity of the as-obtained Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6) nanocomposites for photocatalytic CO_(2) reduction was studied under visible light.The as-obtained Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6) nanocomposites show a superior activity for photocatalytic CO_(2) reduction to produce CH4 and CO,with an optimum activity achieved over 0.5 Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6).The obvious superior activity observed over Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6) nanocomposites as compared with bare Cs_(2)AgBiBr_(6) and bare Bi_(2)WO_(6) as well as a mechanical mixture of Cs_(2)AgBiBr_(6) and Bi_(2)WO_(6) can be owe to the fabrication of an efficient S-scheme heterojunction,which accelerates the separation of the photogenerated charge carriers in Cs_(2)AgBiBr_(6) and Bi_(2)WO_(6) without sacrificing the high redox capability of Cs_(2)AgBiBr_(6) and Bi_(2)WO_(6).This work demonstrates that the coupling of two photocatalytic materials with staggered band alignment to form an S-scheme heterojunction is an effective strategy to develop efficient photocatalytic systems and also highlights the promising role of using lead free perovskites in photocatalysis.
文摘hree kinds of devices of drag reduction are presented swept wingtip,stage by stage swept wingtip and downbend wingtip. The effects of changing geometryparameters of the swept wingtip on the drag reducing are also presented. Wind-tunnelexperiment results indicate that a properly designed swept wingtip results in an incre-ment in induced efficiency of 4%～ 7% and that swept wingtip can increase longitudinalstatic-stability. Water-tunnel experiment results indicate that the reason for drag re-ducing of swept wingtip is that when the angle of attack is not zero, the strong end vor-tex of the wing is weakened by the combined effect of the leading edge and trailing edgevortices of the swept wingtip.
文摘Traffic intersections are incredibly dangerous for drivers and pedestrians. Statistics from both Canada and the U.S. show a high number of fatalities and serious injuries related to crashes at intersections. In Canada, during 2019, the National Collision Database shows that 28% of traffic fatalities and 42% of serious injuries occurred at intersections. Likewise, the U.S. National Highway Traffic Administration (NHTSA) found that about 40% of the estimated 5,811,000 accidents in the U.S. during the year studied were intersection-related crashes. In fact, a major survey by the car insurance industry found that nearly 85% of drivers could not identify the correct action to take when approaching a yellow traffic light at an intersection. One major reason for these accidents is the “yellow light dilemma,” the ambiguous situation where a driver should stop or proceed forward when unexpectedly faced with a yellow light. This situation is even further exacerbated by the tendency of aggressive drivers to inappropriately speed up on the yellow just to get through the traffic light. A survey of Canadian drivers conducted by the Traffic Injury Research Foundation found that 9% of drivers admitted to speeding up to get through a traffic light. Another reason for these accidents is the increased danger of making a left-hand turn on yellow. According to the National Highway Traffic Safety Association (NHTSA), left turns occur in approximately 22.2% of collisions—as opposed to just 1.2% for right turns. Moreover, a study by CNN found left turns are three times as likely to kill pedestrians than right turns. The reason left turns are so much more likely to cause an accident is because they take a driver against traffic and in the path of oncoming cars. Additionally, most of these left turns occur at the driver’s discretion—as opposed to the distressingly brief left-hand arrow at busy intersections. Drive Safe Now proposes a workable solution for reducing the number of accidents occurring during a yellow light at intersections. We believe this fairly simple solution will save lives, prevent injuries, reduce damage to public and private property, and decrease insurance costs.
文摘Semiconductor photocatalytic technology is widely recognized as one of the most promising technologies to solve current energy and environmental crisis, due to its ability to make effective use of solar energy. In recent years, graphite carbon nitride(g-C3N4), a new type of non-metallic polymer semiconductor photocatalyst, has rapidly become the focus of intense research in the field of photocatalysis because of its suitable bandgap energy, unique structure, and excellent chemical stability. In order to improve its intrinsic shortages of small specific surface area, narrow visible light response range, high electron-hole pair recombination rate, and low photon quantum efficiency, a simple method was utilized to synthesize Br-doped g-C3N4(CN–Br X, X = 5, 10, 20, 30), where X is a percentage mole ratio of NH4 Br to melamine. Experimental results showed that Br atoms were doped into the g-C3N4 lattice by replacing the bonded N atoms in the form of C–N=C, while the derived material retained the original framework of g-C3N4. The interaction of Br element with the g-C3N4 skeleton not only broadened the visible-light response of g-C3N4 to 800 nm with an adjustable band gap, but also greatly promoted the separation efficiency of the photogenerated charge carrier and the surface area. The photocurrent intensity of bare CN and CN–Br X(X = 5, 10, 20, 30) catalysts is calculated to be 1.5, 2.0, 3.1, 6.5, and 1.9 μA, respectively. And their specific surface area is measured to be 9.086, 9.326, 15.137, 13.397, and 6.932 m2/g. As a result, this Br-doped g-C3N4 gives significantly enhanced photocatalytic reduction of Cr(VI), achieving a twice enhancement over g-C3N4, with high stability during prolonged photocatalytic operation compared to bare g-C3N4 under visible light irradiation. Furthermore, an underlying photocatalytic reduction mechanism was proposed based on control experiments using radical scavengers.
文摘Photo-thermal CO_(2) reduction with methane(CRM)is beneficial for solar energy harvesting and energy storage.The search for efficient photo-thermal catalysts is of great significance.Here,we reveal that group Ⅷ metal catalysts supported by optical material WO_(3) are more effective for photo-thermal CRM,giving catalytic activities with visible light assistance that are 1.4-2.4 times higher than that achieved under thermal conditions.The activity enhancement(1.4-2.4 times)was comparable to that achieved with plasmonic-Au-promoted catalysts(1.7 times).Characterization results indicated that WO_(3) was partially reduced to WO_(3-x) in situ under the reductive CRM reaction atmosphere,and that WO_(3-x) rather than WO_(3) enhanced the activities with visible light assistance.Our method provides a promising approach for improving the activity of catalysts under light irradiation.
文摘Metal-organic frameworks(MOFs)have shown significant potential as photocatalysts.It has been widely assumed that all catalytic active sites within MOFs are functional in photocatalytic reactions but for a three-dimensional MOF,whether the internal catalytic active sites can effectively absorb light and actively contribute to photocatalytic reactions remains to be explored.In this context,we synthesized a two-dimensional nanosheet MOF(2D-MOF)and a three-dimensional bulk MOF(3D-MOF)composed of Zr^(6) clusters and tetracarboxylic porphyrin(TCPP)by the approach described in the literature.Re(bpy)(CO)^(3)Cl(bpy=2,2’-bipyridine),which has remarkable CO_(2) photoreduction ability,was introduced to the two MOFs to create two new photocatalysts 2D-MOF-Re and 3D-MOF-Re,respectively.Photocatalytic CO_(2) reduction experiments show that based on the equal number of catalytic active sites,the CO turnover number(TON)of 2D-MOF-Re reaches 27.8 in 6 h,which is 50 times that of 3D-MOF-Re.The result shows that certain catalytic active sites inside the bulk MOF are inactive due to the inability to absorb light.This study illuminates the potential of the dimensional reduction approach in the design of photocatalysts to exploit the capabilities fully.
文摘While photoreduction of CO_(2) to CH 4 is an effective means of producing value-added fuels,common pho-tocatalysts have poor activity and low selectivity in photocatalytic CO_(2)-reduction processes.Even though creating defects is an effective photocatalyst fabrication route to improve photocatalytic activity,there are some challenges with the facile photocatalyst synthesis method.In this work,an O element is in-troduced into a graphitic carbon nitride(CN)skeleton through a precursory ultraviolet light irradiation pretreatment to increase the visible light absorption and enhance the carrier density of this modified non-metal CN photocatalyst;the charge transfer dynamics thereof are also studied through electrochem-ical tests,photoluminescence spectroscopy,and nanosecond transient absorption.We verify that the op-timized sample exhibits lower charge recombination and a suppressed 84 ns electron-trapping lifetime,compared to the 103 ns electron-trapping lifetime of the CN counterpart,and thereby contributes to ro-bust detrapping and a fast transfer of active electrons.Through density functional theory calculations,we find that the improved light absorption and increased electron density are ascribed to O-element doping,which enhances the CO_(2) adsorption energy and improves the CO_(2)-to-CH 4 photoreduction activity;it be-comes 17 times higher than that of the bare CN,and the selectivity is 3.8 times higher than that of CN.Moreover,the optimized sample demonstrates excellent cyclic stability in a 24-hour cycle test.
基金supported by Natural Science Basic Research Program in Shaanxi Province of China(No.2023-JCYB-574)National Natural Science Foundation of China(No.62204203).
文摘High qualityβ-Ga_(2)O_(3)single crystal nanobelts with length of 2−3 mm and width from tens of microns to 132μm were synthesized by carbothermal reduction method.Based on the grown nanobelt with the length of 600μm,the dual-Schottky-junctions coupling device(DSCD)was fabricated.Due to the electrically floating Ga_(2)O_(3)nanobelt region coupling with the double Schottky-junctions,the current I_(S2)increases firstly and rapidly reaches into saturation as increase the voltage V_(S2).The saturation current is about 10 pA,which is two orders of magnitude lower than that of a single Schottky-junction.In the case of solar-blind ultraviolet(UV)light irradiation,the photogenerated electrons further aggravate the coupling physical mechanism in device.I_(S2)increases as the intensity of UV light increases.Under the UV light of 1820μW/cm^(2),I_(S2)quickly enters the saturation state.At V_(S2)=10 V,photo-to-dark current ratio(PDCR)of the device reaches more than 104,the external quantum efficiency(EQE)is 1.6×10^(3)%,and the detectivity(D*)is 7.5×10^(12)Jones.In addition,the device has a very short rise and decay times of 25−54 ms under different positive and negative bias.DSCD shows unique electrical and optical control characteristics,which will open a new way for the application of nanobelt-based devices.
