Finely modulated light-induced charge separation and transfer is a central challenge to achieve efficient photocatalysis.Although progress has been made in this field,most of the previous research works focused on the...Finely modulated light-induced charge separation and transfer is a central challenge to achieve efficient photocatalysis.Although progress has been made in this field,most of the previous research works focused on the separation or migration of photogenerated carriers but did not build a bridge between the two.How to realize the strong driving and precise migration of carriers has become the focus of our work.We report an ingeniously designed ternary heterojunction.Taking NiFe-MOF as the“parent material”,the FeP_(4)/Ni_(x)P_(y)heterojunction is derived in situ while maintaining the frame structure through gas-solid reaction,and finally the Z-type electron transfer is realized.With Cu_(3)P anchoring spindle matrix,an electron transport tunnel is opened up in Cu_(3)P/FeP_(4)/Ni_(x)P_(y)ternary heterojunction under the action of p-n heterojunction built-in electric field driving and accurate energy band matching.The strong driving force of the built-in electric field provides an inexhaustible power for the transmission of electrons,and the fine series of electron transmission channels realizes the precise transmission of electrons.The above fine design makes the perfect fit between the built-in electric field and the electron transfer channel,which not only effectively improves the embarrassing situation of insufficient electron driving force of hydrogen evolution reaction in the previous research,but also makes up for the weakening of semi-conductor reduction ability caused by the construction of traditional p-n heterostructures.This research work provides a new idea for the construction of multiple heterostructures and the design of fine interface engineering in the future.展开更多
Integrated data and energy transfer(IDET)is capable of simultaneously delivering on-demand data and energy to low-power Internet of Everything(Io E)devices.We propose a multi-carrier IDET transceiver relying on superp...Integrated data and energy transfer(IDET)is capable of simultaneously delivering on-demand data and energy to low-power Internet of Everything(Io E)devices.We propose a multi-carrier IDET transceiver relying on superposition waveforms consisting of multi-sinusoidal signals for wireless energy transfer(WET)and orthogonal-frequency-divisionmultiplexing(OFDM)signals for wireless data transfer(WDT).The outdated channel state information(CSI)in aging channels is employed by the transmitter to shape IDET waveforms.With the constraints of transmission power and WDT requirement,the amplitudes and phases of the IDET waveform at the transmitter and the power splitter at the receiver are jointly optimised for maximising the average directcurrent(DC)among a limited number of transmission frames with the existence of carrier-frequencyoffset(CFO).For the amplitude optimisation,the original non-convex problem can be transformed into a reversed geometric programming problem,then it can be effectively solved with existing tools.As for the phase optimisation,the artificial bee colony(ABC)algorithm is invoked in order to deal with the nonconvexity.Iteration between the amplitude optimisation and phase optimisation yields our joint design.Numerical results demonstrate the advantage of our joint design for the IDET waveform shaping with the existence of the CFO and the outdated CSI.展开更多
Sluggish reaction kinetics of oxygen evolution reaction(OER), resulting from multistep proton-coupled electron transfer and spin constriction, limits overall efficiency for most reported catalysts. Herein, using model...Sluggish reaction kinetics of oxygen evolution reaction(OER), resulting from multistep proton-coupled electron transfer and spin constriction, limits overall efficiency for most reported catalysts. Herein, using modeled ZnFe_(2-x)Ni_xO_(4)(0 ≤ x ≤ 0.4) spinel oxides, we aim to develop better OER electrocatalyst through combining the construction of ferromagnetic(FM) ordering channels and generation of highly active reconstructed species. The number of symmetry-breaking Fe–O–Ni structure links to the formation of FM ordering electron transfer channels. Meanwhile, as the number of Ni^(3+)increases, more ligand holes are formed, beneficial for redirecting surface reconstruction. The electro-activated ZnFe_(1.6)Ni_(0.4)O_(4) shows the highest specific activity, which is 13 and 2.5 times higher than that of ZnFe_(2)O_(4) and unactivated ZnFe_(1.6)Ni_(0.4)O_(4), and even superior to the benchmark IrO_(2) under the overpotential of 350 mV. Applying external magnetic field can make electron spin more aligned, and the activity can be further improved to 39 times of ZnFe_(2)O_(4). We propose that intriguing FM exchange-field interaction at FM/paramagnetic interfaces can penetrate FM ordering channels into reconstructed oxyhydroxide layers, thereby activating oxyhydroxide layers as spin-filter to accelerate spin-selective electron transfer. This work provides a new guideline to develop highly efficient spintronic catalysts for water oxidation and other spin-forbidden reactions.展开更多
Gap junctions form intercellular channels for direct exchange of metabolites and second messengers between adjacent cells. The existence of a multi-gene family encoding gap junction proteins, i. e. the connexins (Cx),...Gap junctions form intercellular channels for direct exchange of metabolites and second messengers between adjacent cells. The existence of a multi-gene family encoding gap junction proteins, i. e. the connexins (Cx), has been recently demonstrated. Despite the overall sequence homologies and a similar predicted structural motif, their functional properties differ in various tissues. Because of coexpression of two or more connexin proteins in one tissue, determination of properties specific for each connexin is complicated. The regulation of expression of gap junctions and their roles in cellular activities remain mostly unelucidative. Controlled manipulation of connexin molecules in Xenopus oocyte expression system has been use-展开更多
In this study, the local characteristics of pressure drop and heat transfer were investigated experimentally for carbon dioxide condensation in a multi-port extruded aluminum test section, which had 10 circular channe...In this study, the local characteristics of pressure drop and heat transfer were investigated experimentally for carbon dioxide condensation in a multi-port extruded aluminum test section, which had 10 circular channels each with 1.31 mm inner diameter. The CO2 was cooled with cooling water flow inside the copper blocks that were attached at both sides of the test section. The temperatures at the outer surface of the test section were measured with 24 K-type thermocouples embedded in the upper and lower surfaces along the length. Local heat fluxes were measured with 12 heat flux sensors to estimate the local enthalpies, temperatures and heat transfer coefficients. Bulk mean temperatures of CO2 at the inlet and outlet of the test section were measured with 2 K-type thermocouples. The measurements were performed for the pressure ranged from 6.48 to 7.3 MPa, inlet temperature of CO2 from 21.63 to 31.33℃, heat flux from 1.10 to 8.12 kW/m2, mass velocity from 123.2 to 315.2 kg/m2s, and vapor quality from 0 to 1. The results indicate that pressure drop is very small along the test section, heat transfer coefficient in the two-phase region is higher than that in the single-phase, and mass velocity has important effect on condensation heat transfer characteristics. In addition, experimental data were compared with previous correlations and large discrepancies were observed.展开更多
In this study,femtosecond laser assisted-chemical vapor infiltration(LA-CVI)was employed to produce C/SiC composites with 1,3,and 5 rows of mass transfer channels.The effect of laser machining power on the quality of ...In this study,femtosecond laser assisted-chemical vapor infiltration(LA-CVI)was employed to produce C/SiC composites with 1,3,and 5 rows of mass transfer channels.The effect of laser machining power on the quality of produced holes was investigated.The results showed that the increase in power yielded complete hole structures.The as-obtained C/SiC composites with different mass transfer channels displayed higher densification degrees with flexural strengths reaching 546±15 MPa for row mass transfer channel of 3.The strengthening mechanism of the composites was linked to the increase in densification and formation of"dense band"during LA-CVI process.Multiphysics finite element simulations of the dense band and density gradient of LA-CVI C/SiC composites revealed C/SiC composites with improved densification and lower porosity due to the formation of"dense band"during LA-CVI process.In sum,LA-CVI method is promising for future preparation of ceramic matrix composites with high densities.展开更多
Exploring efficient co-catalysts to accurately steer the charge separation of semiconductor photocatalysts is highly desired yet remains challenging.Here,we tackle the significant challenge by in situ growing the Bi_(...Exploring efficient co-catalysts to accurately steer the charge separation of semiconductor photocatalysts is highly desired yet remains challenging.Here,we tackle the significant challenge by in situ growing the Bi_(12)O_(17)C_(l2)photocatalyst onto two-dimensional(2D)Cl-terminated Ti_(3)C_(2)MXene to construct 2D/2D heterojunction of Bi_(12)O_(17)C_(l2)and Ti_(3)C_(2).Firstly,2D few-layered Ti_(3)C_(2)MXene with chlorine groups has been successfully syn-thesized by Lewis acidic etching strategy with subsequent ultrasonic exfoliation.The grafting of chlorine terminations on the surface of MXene serves as nucleating centers and growth platform,resulting in the formation of strong interfacial bonds(Bi-Cl-Ti)between Bi_(12)O_(17)C_(l2)and Ti_(3)C_(2).These strong bonds can facilitate the separation and transfer of photo-generated charge carriers between Bi_(12)O_(17)C_(l2)photocatalyst and Ti_(3)C_(2)cocatalyst.As expec-ted,the photocatalytic degradation rate of Bi_(12)O_(17)C_(l2)/Ti_(3)C_(2)hybrids is 9.7 times higher than that of bare Bi_(12)O_(17)C_(l2)nanosheets.This work not only exhibits a new design concept to effectively steer the charge separation for photocatalysis,but also gives a reference for constructing efficient MXene-based photocatalytic systems.展开更多
Multiple pollutants including pathogenic microorganism contaminations and emerging organic contaminations(EOCs)have shown a growing threat to the environment,especially the natural waters.However,the control and remov...Multiple pollutants including pathogenic microorganism contaminations and emerging organic contaminations(EOCs)have shown a growing threat to the environment,especially the natural waters.However,the control and removal of pathogenic microorganism contaminations and EOCs have been greatly limited since limited knowledge of their environmental behaviors.Thus,a novel and efficient photocatalyst Ag_(2)O/BiOBr heterojunction was synthesized and used for removal of multiple pollutants including Escherichia coli(E.coli),Staphylococcus aureus(S.aureus),tetracycline and acetaminophen under visible light.The results showed that there were valid electron transfer pathways between BiOBr and Ag_(2)O,the main electron transfer direction was the BiOBr to Ag_(2)O.Photo-generated electrons were stored in Ag_(2)O and thus separation efficiency between holes and photo-generated electrons was obviously enhanced.Active oxygen species were highly produced and eventually end up with the high efficiency of removal of multiple pollutants.For Ag_(2)O/BiOBr with Ag_(2)O content at 3%(the best performance)under visible light,log decrease of E.coli was 7.16(removal efficiency was 100%)in 120 min,log decrease of S.aureus was 7.23(removal efficiency was 100%)in 160 min,C/C0 of tetracycline was 0.06 in 180 min,C/C0 of acetaminophen was 0.17 in 180 min.This work could provide a promising candidate in the actual contaminated natural waters for cleaning multiple pollutants.展开更多
The purpose of this study is to conduct the dryout point and heat transfer correlation for subcooled boiling flow in narrow annuli. First, the dryout point of subcooled flow boiling of water was measured in narrow ann...The purpose of this study is to conduct the dryout point and heat transfer correlation for subcooled boiling flow in narrow annuli. First, the dryout point of subcooled flow boiling of water was measured in narrow annular channels under the working condition of pressure ranging from 0.1 to 0.3 MPa and low mass flow rate from 6 to 60 kgm^-2 s^-1. Experimental test channels were annular and heated bilaterally with the channel gap of lmm and 1.5mm, and heated length of 1500mm.The location of the dryout was observed and measured by experiment with investigating the various system parameter effects on dryout point, and the results show that the location of dryout point is basically stable and repeating and the heat transfer coefficient increased with heat flux, mass flux and pressure, however, decreases with the gap size. Next, new correlations of CHF and critical vapor quality for narrow annular channels was proposed and calculation results shown a good agreement with the experimental data.展开更多
基金supported by the National Natural Science Foundation of China (Nos.22005117 and 52072146)。
文摘Finely modulated light-induced charge separation and transfer is a central challenge to achieve efficient photocatalysis.Although progress has been made in this field,most of the previous research works focused on the separation or migration of photogenerated carriers but did not build a bridge between the two.How to realize the strong driving and precise migration of carriers has become the focus of our work.We report an ingeniously designed ternary heterojunction.Taking NiFe-MOF as the“parent material”,the FeP_(4)/Ni_(x)P_(y)heterojunction is derived in situ while maintaining the frame structure through gas-solid reaction,and finally the Z-type electron transfer is realized.With Cu_(3)P anchoring spindle matrix,an electron transport tunnel is opened up in Cu_(3)P/FeP_(4)/Ni_(x)P_(y)ternary heterojunction under the action of p-n heterojunction built-in electric field driving and accurate energy band matching.The strong driving force of the built-in electric field provides an inexhaustible power for the transmission of electrons,and the fine series of electron transmission channels realizes the precise transmission of electrons.The above fine design makes the perfect fit between the built-in electric field and the electron transfer channel,which not only effectively improves the embarrassing situation of insufficient electron driving force of hydrogen evolution reaction in the previous research,but also makes up for the weakening of semi-conductor reduction ability caused by the construction of traditional p-n heterostructures.This research work provides a new idea for the construction of multiple heterostructures and the design of fine interface engineering in the future.
基金financial support of Natural Science Foundation of China(No.61971102,62132004)MOST Major Research and Development Project(No.2021YFB2900204)+1 种基金Sichuan Science and Technology Program(No.2022YFH0022)Key Research and Development Program of Zhejiang Province(No.2022C01093)。
文摘Integrated data and energy transfer(IDET)is capable of simultaneously delivering on-demand data and energy to low-power Internet of Everything(Io E)devices.We propose a multi-carrier IDET transceiver relying on superposition waveforms consisting of multi-sinusoidal signals for wireless energy transfer(WET)and orthogonal-frequency-divisionmultiplexing(OFDM)signals for wireless data transfer(WDT).The outdated channel state information(CSI)in aging channels is employed by the transmitter to shape IDET waveforms.With the constraints of transmission power and WDT requirement,the amplitudes and phases of the IDET waveform at the transmitter and the power splitter at the receiver are jointly optimised for maximising the average directcurrent(DC)among a limited number of transmission frames with the existence of carrier-frequencyoffset(CFO).For the amplitude optimisation,the original non-convex problem can be transformed into a reversed geometric programming problem,then it can be effectively solved with existing tools.As for the phase optimisation,the artificial bee colony(ABC)algorithm is invoked in order to deal with the nonconvexity.Iteration between the amplitude optimisation and phase optimisation yields our joint design.Numerical results demonstrate the advantage of our joint design for the IDET waveform shaping with the existence of the CFO and the outdated CSI.
基金supported by the National Key R&D Program of China (2020YFA0710000)the National Natural Science Foundation of China (22278307, 22008170, 21978200, 22161142002, and 22121004)+2 种基金the Applied Basic Research Program of Qinghai Province (2023-ZJ-701)the Haihe Laboratory of Sustainable Chemical Transformationsthe Tianjin Research Innovation Project for Postgraduate Students (2022BKYZ035)。
文摘Sluggish reaction kinetics of oxygen evolution reaction(OER), resulting from multistep proton-coupled electron transfer and spin constriction, limits overall efficiency for most reported catalysts. Herein, using modeled ZnFe_(2-x)Ni_xO_(4)(0 ≤ x ≤ 0.4) spinel oxides, we aim to develop better OER electrocatalyst through combining the construction of ferromagnetic(FM) ordering channels and generation of highly active reconstructed species. The number of symmetry-breaking Fe–O–Ni structure links to the formation of FM ordering electron transfer channels. Meanwhile, as the number of Ni^(3+)increases, more ligand holes are formed, beneficial for redirecting surface reconstruction. The electro-activated ZnFe_(1.6)Ni_(0.4)O_(4) shows the highest specific activity, which is 13 and 2.5 times higher than that of ZnFe_(2)O_(4) and unactivated ZnFe_(1.6)Ni_(0.4)O_(4), and even superior to the benchmark IrO_(2) under the overpotential of 350 mV. Applying external magnetic field can make electron spin more aligned, and the activity can be further improved to 39 times of ZnFe_(2)O_(4). We propose that intriguing FM exchange-field interaction at FM/paramagnetic interfaces can penetrate FM ordering channels into reconstructed oxyhydroxide layers, thereby activating oxyhydroxide layers as spin-filter to accelerate spin-selective electron transfer. This work provides a new guideline to develop highly efficient spintronic catalysts for water oxidation and other spin-forbidden reactions.
文摘Gap junctions form intercellular channels for direct exchange of metabolites and second messengers between adjacent cells. The existence of a multi-gene family encoding gap junction proteins, i. e. the connexins (Cx), has been recently demonstrated. Despite the overall sequence homologies and a similar predicted structural motif, their functional properties differ in various tissues. Because of coexpression of two or more connexin proteins in one tissue, determination of properties specific for each connexin is complicated. The regulation of expression of gap junctions and their roles in cellular activities remain mostly unelucidative. Controlled manipulation of connexin molecules in Xenopus oocyte expression system has been use-
文摘In this study, the local characteristics of pressure drop and heat transfer were investigated experimentally for carbon dioxide condensation in a multi-port extruded aluminum test section, which had 10 circular channels each with 1.31 mm inner diameter. The CO2 was cooled with cooling water flow inside the copper blocks that were attached at both sides of the test section. The temperatures at the outer surface of the test section were measured with 24 K-type thermocouples embedded in the upper and lower surfaces along the length. Local heat fluxes were measured with 12 heat flux sensors to estimate the local enthalpies, temperatures and heat transfer coefficients. Bulk mean temperatures of CO2 at the inlet and outlet of the test section were measured with 2 K-type thermocouples. The measurements were performed for the pressure ranged from 6.48 to 7.3 MPa, inlet temperature of CO2 from 21.63 to 31.33℃, heat flux from 1.10 to 8.12 kW/m2, mass velocity from 123.2 to 315.2 kg/m2s, and vapor quality from 0 to 1. The results indicate that pressure drop is very small along the test section, heat transfer coefficient in the two-phase region is higher than that in the single-phase, and mass velocity has important effect on condensation heat transfer characteristics. In addition, experimental data were compared with previous correlations and large discrepancies were observed.
基金support from the National Natural Science Foundation of China(Nos.51972269 and 51672217)the Fundamental Research Funds for the Central Universities(No.3102019ghxm014)the Creative Research Foundation of the Science and Technology on Thermostructural Composite Materials Laboratory(No.JCKYS2020607001)。
文摘In this study,femtosecond laser assisted-chemical vapor infiltration(LA-CVI)was employed to produce C/SiC composites with 1,3,and 5 rows of mass transfer channels.The effect of laser machining power on the quality of produced holes was investigated.The results showed that the increase in power yielded complete hole structures.The as-obtained C/SiC composites with different mass transfer channels displayed higher densification degrees with flexural strengths reaching 546±15 MPa for row mass transfer channel of 3.The strengthening mechanism of the composites was linked to the increase in densification and formation of"dense band"during LA-CVI process.Multiphysics finite element simulations of the dense band and density gradient of LA-CVI C/SiC composites revealed C/SiC composites with improved densification and lower porosity due to the formation of"dense band"during LA-CVI process.In sum,LA-CVI method is promising for future preparation of ceramic matrix composites with high densities.
基金financially supported by the Natural Science Foundation of Jiangsu Province (No. BK20211280)the National Natural Science Foundation of China (No. 21975129)
文摘Exploring efficient co-catalysts to accurately steer the charge separation of semiconductor photocatalysts is highly desired yet remains challenging.Here,we tackle the significant challenge by in situ growing the Bi_(12)O_(17)C_(l2)photocatalyst onto two-dimensional(2D)Cl-terminated Ti_(3)C_(2)MXene to construct 2D/2D heterojunction of Bi_(12)O_(17)C_(l2)and Ti_(3)C_(2).Firstly,2D few-layered Ti_(3)C_(2)MXene with chlorine groups has been successfully syn-thesized by Lewis acidic etching strategy with subsequent ultrasonic exfoliation.The grafting of chlorine terminations on the surface of MXene serves as nucleating centers and growth platform,resulting in the formation of strong interfacial bonds(Bi-Cl-Ti)between Bi_(12)O_(17)C_(l2)and Ti_(3)C_(2).These strong bonds can facilitate the separation and transfer of photo-generated charge carriers between Bi_(12)O_(17)C_(l2)photocatalyst and Ti_(3)C_(2)cocatalyst.As expec-ted,the photocatalytic degradation rate of Bi_(12)O_(17)C_(l2)/Ti_(3)C_(2)hybrids is 9.7 times higher than that of bare Bi_(12)O_(17)C_(l2)nanosheets.This work not only exhibits a new design concept to effectively steer the charge separation for photocatalysis,but also gives a reference for constructing efficient MXene-based photocatalytic systems.
基金the financial support by the National Natural Science Foundation of China as general projects(Nos.21722702 and 21677080)the Tianjin Commission of Science and Technology as Key Technologies R&D Projects(Nos.118YFZCSF00730,18YFZCSF00770 and 18ZXSZSF00230)。
文摘Multiple pollutants including pathogenic microorganism contaminations and emerging organic contaminations(EOCs)have shown a growing threat to the environment,especially the natural waters.However,the control and removal of pathogenic microorganism contaminations and EOCs have been greatly limited since limited knowledge of their environmental behaviors.Thus,a novel and efficient photocatalyst Ag_(2)O/BiOBr heterojunction was synthesized and used for removal of multiple pollutants including Escherichia coli(E.coli),Staphylococcus aureus(S.aureus),tetracycline and acetaminophen under visible light.The results showed that there were valid electron transfer pathways between BiOBr and Ag_(2)O,the main electron transfer direction was the BiOBr to Ag_(2)O.Photo-generated electrons were stored in Ag_(2)O and thus separation efficiency between holes and photo-generated electrons was obviously enhanced.Active oxygen species were highly produced and eventually end up with the high efficiency of removal of multiple pollutants.For Ag_(2)O/BiOBr with Ag_(2)O content at 3%(the best performance)under visible light,log decrease of E.coli was 7.16(removal efficiency was 100%)in 120 min,log decrease of S.aureus was 7.23(removal efficiency was 100%)in 160 min,C/C0 of tetracycline was 0.06 in 180 min,C/C0 of acetaminophen was 0.17 in 180 min.This work could provide a promising candidate in the actual contaminated natural waters for cleaning multiple pollutants.
基金This work is supported by the Project of National Natural Science Foundation of China （No. 50076014） and the Project of Major State Basic Research Program （No. G2000026303）.
文摘The purpose of this study is to conduct the dryout point and heat transfer correlation for subcooled boiling flow in narrow annuli. First, the dryout point of subcooled flow boiling of water was measured in narrow annular channels under the working condition of pressure ranging from 0.1 to 0.3 MPa and low mass flow rate from 6 to 60 kgm^-2 s^-1. Experimental test channels were annular and heated bilaterally with the channel gap of lmm and 1.5mm, and heated length of 1500mm.The location of the dryout was observed and measured by experiment with investigating the various system parameter effects on dryout point, and the results show that the location of dryout point is basically stable and repeating and the heat transfer coefficient increased with heat flux, mass flux and pressure, however, decreases with the gap size. Next, new correlations of CHF and critical vapor quality for narrow annular channels was proposed and calculation results shown a good agreement with the experimental data.
