With the significant discharge of antibiotic wastewater into the aquatic and terrestrial ecosystems, antibiotic pollution has become a serious problem and presents a hazardous risk to the environment. To address such ...With the significant discharge of antibiotic wastewater into the aquatic and terrestrial ecosystems, antibiotic pollution has become a serious problem and presents a hazardous risk to the environment. To address such issues, various investigations on the removal of antibiotics have been undertaken. Photocatalysis has received tremendous attention owing to its great potential in removing antibiotics from aqueous solutions via a green, economic, and effective process. However, such a technology employing traditional photocatalysts suffers from major drawbacks such as light absorption being restricted to the UV spectrum only and fast charge recombination. To overcome these issues, considerable effort has been directed towards the development of advanced visible light-driven photocatalysts. This mini review summarises recent research progress in the state-of-the-art design and fabrication of photocatalysts with visible-light response for photocatalytic degradation of antibiotic wastewater. Such design strategies involve the doping of metal and non-metal into ultraviolet light-driven photocatalysts, development of new semiconductor photocatalysts, construction of heterojunction photocatalysts, and fabrication of surface plasmon resonance-enhanced photocatalytic systems. Additionally, some perspectives on the challenges and future developments in the area of photocatalytic degradation of antibiotics are provided.展开更多
Annealing study of the Al/GaSb system was performed by using a slow positron beam and the measurement of X-ray diffraction. The S parameter against positron energy data were fitted by a three layer model (Al/interfac...Annealing study of the Al/GaSb system was performed by using a slow positron beam and the measurement of X-ray diffraction. The S parameter against positron energy data were fitted by a three layer model (Al/interface/GaSb). It was found there was a ~5 nm interfacial at the region between the Al layer and bulk in the sample of as-deposited. After the 400 ℃ annealing, this interfacial region extends to over 40 nm and S parameter dramatically drops. This is possibly due to a new phase formation induced by the atoms'inter-diffusion at the interface. The annealing out of the open volume defects in the Al layer was revealed by the decrease of the S parameter and the increase of the effective diffusion length of the Al layer. Annealing behaviors of Sb and Lb of the GaSb bulk showed the annealing out of positron traps at 250 ℃. However,further annealing at 400 ℃ induces formation of positron traps, which are possibly another kind of VGarelated defect and the positron shallow trap GaSb anti-site. The results of the X-ray diffraction experiment verified the conclusion of obtained by using positron technology.展开更多
Nitrogen-doped anatase TiO 2 microsheets with 65%(001) and 35%(101) exposed faces were fabricated by the hydrothermal method using TiN as precursor in the presence of HF and HCl. The samples were characterized by ...Nitrogen-doped anatase TiO 2 microsheets with 65%(001) and 35%(101) exposed faces were fabricated by the hydrothermal method using TiN as precursor in the presence of HF and HCl. The samples were characterized by scanning electron microscopy,X-ray diffraction,N2 adsorption,X-ray photoelectron spectroscopy,UV-visible spectroscopy,and electrochemical impedance spectroscopy. Their photocatalytic activity was evaluated using the photocatalytic reduction of CO2. The N-doped TiO 2 sample exhibited a much higher visible light photocatalytic activity for CO2 reduction than its precursor TiN and commercial TiO 2(P25). This was due to the synergistic effect of the formation of surface heterojunctions on the TiO 2 microsheet surface,enhanced visible light absorption by nitrogen-doping,and surface fluorination.展开更多
Narrow-band BiOI photocatalysts usually suffer from low photocatalysis efficiency under visible light exposure because of rapid charge recombination. In this work, to overcome this deficiency of photosensitive BiOI, o...Narrow-band BiOI photocatalysts usually suffer from low photocatalysis efficiency under visible light exposure because of rapid charge recombination. In this work, to overcome this deficiency of photosensitive BiOI, oxygen vacancies, Bi particles, and Bi2O2CO3 were co-induced in BiOI via a facile in situ assembly method at room temperature using NaBH4 as the reducing agent. In the synthesized ternary Bi/BiOI/(BiO)2CO3, the oxygen vacancies, dual heterojunctions (i.e., Bi/BiOI and Bi- OI/(BiO)2CO3), and surface plasmon resonance effect of the Bi particles contributed to efficient electron-hole separation and an increase in charge carrier concentration, thus boosting the overall visible light photocatalysis efficiency. The as-prepared catalysts were applied for the removal of NO in concentrations of parts per billion from air in continuous air flow under visible light illumination. Bi/BiOI/(BiO)2CO3 exhibited a highly enhanced NO removal ratio of 50.7%, much higher than that of the pristine BiOI (1.2%). Density functional theory calculations and experimental results revealed that the Bi/BiOI/(BiO)2CO3 composites promoted the production of reactive oxygen species for photocatalytic NO oxidation. Thus, this work provides a new strategy to modify narrow-band semiconductors and explore other bismuth-containing heterostructured visible-light-driven photocatalysts.展开更多
Photocatalytic CO_(2)reduction to sustainably product of fuels is a potential route to achieve clean energy conversion.Unfortunately,the sluggish charge transport dynamics and poor CO_(2)activation performance result ...Photocatalytic CO_(2)reduction to sustainably product of fuels is a potential route to achieve clean energy conversion.Unfortunately,the sluggish charge transport dynamics and poor CO_(2)activation performance result in a low CO_(2)conversion efficiency.Herein,we develop a multidimensional In_(2)O_(3)/In_(2)S_(3)(IO/IS)heterojunction with abundant lattice distortion structure and high concentration of oxygen defects.The close contact interfaces between the junction of the two phases ensure undisturbed transmission of electrons with high‐speed.The increased free electron concentration promotes the adsorption and activation of CO2 on the catalyst surface,leaving the key intermediate*COOH at a lower energy barrier.The perfect combination of the band matching oxide and sulfide effectively reduces the internal energy barrier of the CO2 reduction reaction.Furthermore,the lattice distortion structure not only provides additional active sites,but also optimizes the kinetics of the reaction through microstructural regulation.Remarkably,the optimal IO/IS heterojunction exhibits superior CO_(2)reduction performance with CO evolution rate of 12.22μmol g^(−1)h^(−1),achieving about 4 times compared to that of In_(2)O_(3)and In2S3,respectively.This work emphasizes the importance of tight interfaces of heterojunction in improving the performance of CO_(2)photoreduction,and provides an effective strategy for construction of heterojunction photocatalysts.展开更多
Solar-powered photocatalytic hydrogen production from water using semiconductors provides an eco-friendly and promising approach for converting solar energy into hydrogen fuel.Bulk semiconductors generally suffer from...Solar-powered photocatalytic hydrogen production from water using semiconductors provides an eco-friendly and promising approach for converting solar energy into hydrogen fuel.Bulk semiconductors generally suffer from certain limitations,such as poor visible-light utilization,rapid recombination of charge carriers,and low catalytic capability.The key challenge is to develop visible-light-driven heterojunction photocatalysts that are stable and highly active during the water splitting process.Here,we demonstrate the integration of one-dimensional(1D)Cd S nanorods with two-dimensional(2D)1 T-phase dominated WS_(2) nanosheets for constructing mixed-dimensional heterojunctions for the photocatalytic hydrogen evolution reaction(HER).The resulting 1D CdS/2D WS_(2) nanoheterojunction exhibited an ultrahigh hydrogen-evolution activity of~70 mmol·g^(-1)·h^(-1) that was visible to the naked eye,as well as long-term stability under visible light illumination.The results reveal that the synergy of hybrid nanoarchitectures and intimate interfacial contact between the 1D Cd S nanorods and 1T-phase dominated 2D WS_(2) nanosheets facilitates charge carrier transport,which is beneficial for achieving superior hydrogen evolution.展开更多
Heterogeneous-structured Cu samples composed of coarse-grained(CG) and ultrafine-grained(UFG) domains with a transitional interface were fabricated by friction stir processing, in order to investigate the effect of in...Heterogeneous-structured Cu samples composed of coarse-grained(CG) and ultrafine-grained(UFG) domains with a transitional interface were fabricated by friction stir processing, in order to investigate the effect of interface constraint on the yielding and fracture behaviors. Tensile test revealed that the synergetic strengthening induced by elastic/plastic interaction between incompatible domains increases with increasing the area of constraint interface. The strain distribution near interface and the fracture morphology were characterized using digital image correlation technique and scanning electron microscopy, respectively. Fracture dimples preferentially formed at the interface, possibly due to extremely high triaxial stress and strain accumulation near the interface. Surprisingly, the CG domain was fractured by pure shear instead of the expected voids growth caused by tensile stress.展开更多
The heterogeneous multilayer interface of VN/Ag coatings and transition multilayer interface of VN/Ag coatings were prepared on Inconel 781 and Si(100),and the microstructures,mechanical and tribological properties we...The heterogeneous multilayer interface of VN/Ag coatings and transition multilayer interface of VN/Ag coatings were prepared on Inconel 781 and Si(100),and the microstructures,mechanical and tribological properties were investigated from 25 to 700℃.The results showed that the surface roughness and average grain size of VN/Ag coatings with transition multilayer interface are obviously larger than those of VN/Ag coatings with heterogeneous multilayer interface.The coatings with transition multilayer interface have higher adhesion force and hardness than the coatings with heterogeneous multilayer interface,and both coatings can effectively restrict the initiation and propagation of microcracks.Both coatings have excellent self-adaptive lubricating properties with a decrease of friction coefficient as the temperature increases,but their wear rates reveal a drastic increase.The phase composition of the worn area of both coatings was investigated,which indicates that a smooth Ag,Magnéli phase(V2O5)and bimetallic oxides(Ag3VO4 and AgVO3)can be responsible to the excellent lubricity of both coatings.To sum up,the coatings with transition multilayer interface have excellent adaptive lubricating properties and can properly control the diffusion rate and release rate of the lubricating phase,indicating that they have great potential in solving the problem of friction and wear of mechanical parts.展开更多
Nitrogen-containing carbons were prepared by modification of activated carbons.The modified carbons were used as electrode materials with improved electrochemical performance.Precursor anthracite was activated by KOH(...Nitrogen-containing carbons were prepared by modification of activated carbons.The modified carbons were used as electrode materials with improved electrochemical performance.Precursor anthracite was activated by KOH(KOH:anthracite= 1:1), modified by melamine or urea and then treated at 1173 K to obtain the modified carbons.The porous structure, the chemical composition and the electrochemical characteristics of the carbons were investigated by nitrogen sorption, XPS and electrochemical methods respectively.Electrochemical experiments were performed in an organic electrolytic solution of 1 M(C2H5)4NBF4/PC.The samples modified by the different methods showed differences in chemical composition that introduced varying degrees of electrochemical performance enhancement.The presence of nitrogen enhanced the electron donor properties and the surface wettability of the activated carbons:this ensured a sufficient utilization of the exposed surface for charge storage.展开更多
Z-scheme photocatalytic system has been regarded as a popular field of research in photoelectrochemical(PEC)water splitting.Among the many obstacles facing a Z-scheme photocatalytic system,the analysis methods of inte...Z-scheme photocatalytic system has been regarded as a popular field of research in photoelectrochemical(PEC)water splitting.Among the many obstacles facing a Z-scheme photocatalytic system,the analysis methods of interfacial Z-scheme charge transfer still remain a significant challenge.Hence,in this study,CdS/Ti-Fe_(2)O_(3)heterojunction photoanodes are elaborately designed to explore the charge-transfer behavior in PEC water splitting.In this study,photophysical measurements,including the Kelvin probe measurement,surface photovoltage spectroscopy(SPV),and transient photovoltage spectroscopy(TPV),are used to monitor the migration behavior of photogenerated charges at the interface electric field of CdS/Ti-Fe_(2)O_(3)Z-scheme heterojunction photoanodes.The Kelvin probe and SPV measurements demonstrate that CdS/Ti-Fe_(2)O_(3)interfacial driving force favors the rapid transfer of photoexcited electrons to CdS.The double-beam strategy based on TPV indicates that more electrons of Ti-Fe_(2)O_(3)are combined with the holes of CdS owing to the intensive interface electric field.The results of these measurements successfully prove the Z-scheme migration mechanism of CdS/Ti-Fe_(2)O_(3)photoanodes.Benefiting from the desirable charge transfer at the interface electric field,CdS/Ti-Fe_(2)O_(3)photoanodes exhibit superior photocatalytic oxygen evolution reaction performance compared with that of pure Ti-Fe_(2)O_(3).The photocurrent density of the 25CdS/Ti-Fe_(2)O_(3)photoanode reaches 1.94 mA/cm^(2) at 1.23 V versus reversible hydrogen electrode without excess cocatalyst,and it is two times higher than that of pure Ti-Fe_(2)O_(3)photoanode.Therefore,an outstanding strategy is provided in this study to prove the Z-scheme charge-transfer mechanism of photocatalytic systems in PEC water splitting.展开更多
Isothermal solidification process of a dissimilar transient liquid phase (TLP) bonding of FSX-414/MBF80/IN738 system was simulated by finite difference method. The TLP joint model was divided into two parts and a mo...Isothermal solidification process of a dissimilar transient liquid phase (TLP) bonding of FSX-414/MBF80/IN738 system was simulated by finite difference method. The TLP joint model was divided into two parts and a moving liquid /solid interface model was used for the parts. Diffusion equations were solved for each half of the joints simultaneously up to the end of isothermal solidification. The completion time of isothermal solidification, concentration profiles and position of the solid/liquid interface for each half were calculated. The intersection of the solid/liquid interfaces of two halves was considered the end of isothermal solidification. To obtain some required diffusion data, TLP bonding of FSX-414/MBF80/IN738 was performed at different temperature and time under vacuum atmosphere. The calculated results show good agreement with the experimental results.展开更多
The surface and interface of heterojunction (HJ) formed with organic semiconductor (3,4,9,10-perylenetetracarboxylic dianhydride (PTCDA)) and inorganic semiconductor p-Si were measured and analyzed by X-ray photoelect...The surface and interface of heterojunction (HJ) formed with organic semiconductor (3,4,9,10-perylenetetracarboxylic dianhydride (PTCDA)) and inorganic semiconductor p-Si were measured and analyzed by X-ray photoelectron spectroscopy (XPS).The results indicate that, in PTCDA molecule,the binding energy ( E b) of C is 284.6 eV and 288.3 eV, corresponding to C of the perylene and C of the anhydride, respectively, and the binding energy of O is 531.3 eV and 531.1 eV, corresponding to C of C=O in the anhydrides and C of C-O-C, respectively. Moreover, PTCDA lost its anhydrides and only its perylenes were left in the HJ interface.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
Although photocatalytic water splitting has excellent potential for converting solar energy into chemical energy,the challenging charge separation process and sluggish surface catalytic reactions significantly limit p...Although photocatalytic water splitting has excellent potential for converting solar energy into chemical energy,the challenging charge separation process and sluggish surface catalytic reactions significantly limit progress in solar energy conversion using semiconductor photocatalysts.Herein,we demonstrate a feasible strategy involving the surface assembly of cobalt oxide species(CoO_(x))on a visible-light-responsive Cd_(0.9)Zn_(0.1)S(CZS)photocatalyst to fabricate a hierarchical CZS@CoO_(x) heterostructure.The unique hierarchical structure effectively accelerates the directional transfer of photogenerated charges,reducing charge recombination through the smooth interfacial heterojunction between CZS and CoO_(x),as evidenced by photoluminescence(PL)spectroscopy and various electrochemical characterizations.The surface cobalt species on the CZS material also act as efficient cocatalysts for photocatalytic hydrogen production,with activity even higher than that of noble metals.The well-defined CZS@CoO_(x) heterostructure not only enhances the interfacial separation of photoinduced charges,but also improves surface catalytic reactions.This leads to superior photocatalytic performances,with an apparent quantum efficiency of 20%at 420 nm for visible-light-driven hydrogen generation,which is one of the highest quantum efficiencies measured among noble-metal-free photocatalysts.Our work presents a potential pathway for controlling complex charge separation and catalytic reaction processes in photocatalysis,guiding the practical development of artificial photocatalysts for successful transformation of solar to chemical energy.展开更多
基金supported by the National Natural Science Foundation of China(21421001,21276116,21477050,21301076,21303074)Natural Science Foundation of Jiangsu Province(BK20140530,BK20150482)+5 种基金China Postdoctoral Science Foundation(2015M570409)Chinese-German Cooperation Research Project(GZ1091)Program for High-Level Innovative and Entrepreneurial Talents in Jiangsu ProvinceProgram for New Century Excellent Talents in University(NCET-13-0835)Henry Fok Education Foundation(141068)Six Talents Peak Project in Jiangsu Province(XCL-025)~~
文摘With the significant discharge of antibiotic wastewater into the aquatic and terrestrial ecosystems, antibiotic pollution has become a serious problem and presents a hazardous risk to the environment. To address such issues, various investigations on the removal of antibiotics have been undertaken. Photocatalysis has received tremendous attention owing to its great potential in removing antibiotics from aqueous solutions via a green, economic, and effective process. However, such a technology employing traditional photocatalysts suffers from major drawbacks such as light absorption being restricted to the UV spectrum only and fast charge recombination. To overcome these issues, considerable effort has been directed towards the development of advanced visible light-driven photocatalysts. This mini review summarises recent research progress in the state-of-the-art design and fabrication of photocatalysts with visible-light response for photocatalytic degradation of antibiotic wastewater. Such design strategies involve the doping of metal and non-metal into ultraviolet light-driven photocatalysts, development of new semiconductor photocatalysts, construction of heterojunction photocatalysts, and fabrication of surface plasmon resonance-enhanced photocatalytic systems. Additionally, some perspectives on the challenges and future developments in the area of photocatalytic degradation of antibiotics are provided.
基金This work was supported by the CERG, RGC, HKSAR (projects 7134/99P and 7107/02P)the National Science Foundation of China (No.10425072).
文摘Annealing study of the Al/GaSb system was performed by using a slow positron beam and the measurement of X-ray diffraction. The S parameter against positron energy data were fitted by a three layer model (Al/interface/GaSb). It was found there was a ~5 nm interfacial at the region between the Al layer and bulk in the sample of as-deposited. After the 400 ℃ annealing, this interfacial region extends to over 40 nm and S parameter dramatically drops. This is possibly due to a new phase formation induced by the atoms'inter-diffusion at the interface. The annealing out of the open volume defects in the Al layer was revealed by the decrease of the S parameter and the increase of the effective diffusion length of the Al layer. Annealing behaviors of Sb and Lb of the GaSb bulk showed the annealing out of positron traps at 250 ℃. However,further annealing at 400 ℃ induces formation of positron traps, which are possibly another kind of VGarelated defect and the positron shallow trap GaSb anti-site. The results of the X-ray diffraction experiment verified the conclusion of obtained by using positron technology.
基金supported by the National Basic Research Program of China(973 Program2013CB632402)+7 种基金the National Natural Science Foundation of China(513201050015137219051402025and 21433007)the Natural Science Foundation of Hubei Province(2015CFA001)the Fundamental Research Funds for the Central Universities(WUT:2014-VII-010)the Self-Determined and Innovative Research Funds of State Key Laboratory of Advanced Technology for Material Synthesis and ProcessingWuhan University of Technology(2013-ZD-1)~~
文摘Nitrogen-doped anatase TiO 2 microsheets with 65%(001) and 35%(101) exposed faces were fabricated by the hydrothermal method using TiN as precursor in the presence of HF and HCl. The samples were characterized by scanning electron microscopy,X-ray diffraction,N2 adsorption,X-ray photoelectron spectroscopy,UV-visible spectroscopy,and electrochemical impedance spectroscopy. Their photocatalytic activity was evaluated using the photocatalytic reduction of CO2. The N-doped TiO 2 sample exhibited a much higher visible light photocatalytic activity for CO2 reduction than its precursor TiN and commercial TiO 2(P25). This was due to the synergistic effect of the formation of surface heterojunctions on the TiO 2 microsheet surface,enhanced visible light absorption by nitrogen-doping,and surface fluorination.
基金supported by the National Natural Science Foundation of China(21501016,21777011,51871037,51501024)the Innovative Research Team of Chongqing(CXTDG201602014)+1 种基金the Key Natural Science Foundation of Chongqing(cstc2017jcyjBX0052)the Plan for "National Youth Talents" of the Organization Department of the Central Committee~~
文摘Narrow-band BiOI photocatalysts usually suffer from low photocatalysis efficiency under visible light exposure because of rapid charge recombination. In this work, to overcome this deficiency of photosensitive BiOI, oxygen vacancies, Bi particles, and Bi2O2CO3 were co-induced in BiOI via a facile in situ assembly method at room temperature using NaBH4 as the reducing agent. In the synthesized ternary Bi/BiOI/(BiO)2CO3, the oxygen vacancies, dual heterojunctions (i.e., Bi/BiOI and Bi- OI/(BiO)2CO3), and surface plasmon resonance effect of the Bi particles contributed to efficient electron-hole separation and an increase in charge carrier concentration, thus boosting the overall visible light photocatalysis efficiency. The as-prepared catalysts were applied for the removal of NO in concentrations of parts per billion from air in continuous air flow under visible light illumination. Bi/BiOI/(BiO)2CO3 exhibited a highly enhanced NO removal ratio of 50.7%, much higher than that of the pristine BiOI (1.2%). Density functional theory calculations and experimental results revealed that the Bi/BiOI/(BiO)2CO3 composites promoted the production of reactive oxygen species for photocatalytic NO oxidation. Thus, this work provides a new strategy to modify narrow-band semiconductors and explore other bismuth-containing heterostructured visible-light-driven photocatalysts.
文摘Photocatalytic CO_(2)reduction to sustainably product of fuels is a potential route to achieve clean energy conversion.Unfortunately,the sluggish charge transport dynamics and poor CO_(2)activation performance result in a low CO_(2)conversion efficiency.Herein,we develop a multidimensional In_(2)O_(3)/In_(2)S_(3)(IO/IS)heterojunction with abundant lattice distortion structure and high concentration of oxygen defects.The close contact interfaces between the junction of the two phases ensure undisturbed transmission of electrons with high‐speed.The increased free electron concentration promotes the adsorption and activation of CO2 on the catalyst surface,leaving the key intermediate*COOH at a lower energy barrier.The perfect combination of the band matching oxide and sulfide effectively reduces the internal energy barrier of the CO2 reduction reaction.Furthermore,the lattice distortion structure not only provides additional active sites,but also optimizes the kinetics of the reaction through microstructural regulation.Remarkably,the optimal IO/IS heterojunction exhibits superior CO_(2)reduction performance with CO evolution rate of 12.22μmol g^(−1)h^(−1),achieving about 4 times compared to that of In_(2)O_(3)and In2S3,respectively.This work emphasizes the importance of tight interfaces of heterojunction in improving the performance of CO_(2)photoreduction,and provides an effective strategy for construction of heterojunction photocatalysts.
文摘Solar-powered photocatalytic hydrogen production from water using semiconductors provides an eco-friendly and promising approach for converting solar energy into hydrogen fuel.Bulk semiconductors generally suffer from certain limitations,such as poor visible-light utilization,rapid recombination of charge carriers,and low catalytic capability.The key challenge is to develop visible-light-driven heterojunction photocatalysts that are stable and highly active during the water splitting process.Here,we demonstrate the integration of one-dimensional(1D)Cd S nanorods with two-dimensional(2D)1 T-phase dominated WS_(2) nanosheets for constructing mixed-dimensional heterojunctions for the photocatalytic hydrogen evolution reaction(HER).The resulting 1D CdS/2D WS_(2) nanoheterojunction exhibited an ultrahigh hydrogen-evolution activity of~70 mmol·g^(-1)·h^(-1) that was visible to the naked eye,as well as long-term stability under visible light illumination.The results reveal that the synergy of hybrid nanoarchitectures and intimate interfacial contact between the 1D Cd S nanorods and 1T-phase dominated 2D WS_(2) nanosheets facilitates charge carrier transport,which is beneficial for achieving superior hydrogen evolution.
基金Projects(11672195,51301092) supported by the National Natural Science Foundation of ChinaProject(2016JQ0047) supported by Sichuan Youth Science and Technology Foundation,China
文摘Heterogeneous-structured Cu samples composed of coarse-grained(CG) and ultrafine-grained(UFG) domains with a transitional interface were fabricated by friction stir processing, in order to investigate the effect of interface constraint on the yielding and fracture behaviors. Tensile test revealed that the synergetic strengthening induced by elastic/plastic interaction between incompatible domains increases with increasing the area of constraint interface. The strain distribution near interface and the fracture morphology were characterized using digital image correlation technique and scanning electron microscopy, respectively. Fracture dimples preferentially formed at the interface, possibly due to extremely high triaxial stress and strain accumulation near the interface. Surprisingly, the CG domain was fractured by pure shear instead of the expected voids growth caused by tensile stress.
基金Project(51505100)supported by the National Natural Science Foundation of China
文摘The heterogeneous multilayer interface of VN/Ag coatings and transition multilayer interface of VN/Ag coatings were prepared on Inconel 781 and Si(100),and the microstructures,mechanical and tribological properties were investigated from 25 to 700℃.The results showed that the surface roughness and average grain size of VN/Ag coatings with transition multilayer interface are obviously larger than those of VN/Ag coatings with heterogeneous multilayer interface.The coatings with transition multilayer interface have higher adhesion force and hardness than the coatings with heterogeneous multilayer interface,and both coatings can effectively restrict the initiation and propagation of microcracks.Both coatings have excellent self-adaptive lubricating properties with a decrease of friction coefficient as the temperature increases,but their wear rates reveal a drastic increase.The phase composition of the worn area of both coatings was investigated,which indicates that a smooth Ag,Magnéli phase(V2O5)and bimetallic oxides(Ag3VO4 and AgVO3)can be responsible to the excellent lubricity of both coatings.To sum up,the coatings with transition multilayer interface have excellent adaptive lubricating properties and can properly control the diffusion rate and release rate of the lubricating phase,indicating that they have great potential in solving the problem of friction and wear of mechanical parts.
基金Projects 50672025 and 50730003 supported by the National Natural Science Foundation of China
文摘Nitrogen-containing carbons were prepared by modification of activated carbons.The modified carbons were used as electrode materials with improved electrochemical performance.Precursor anthracite was activated by KOH(KOH:anthracite= 1:1), modified by melamine or urea and then treated at 1173 K to obtain the modified carbons.The porous structure, the chemical composition and the electrochemical characteristics of the carbons were investigated by nitrogen sorption, XPS and electrochemical methods respectively.Electrochemical experiments were performed in an organic electrolytic solution of 1 M(C2H5)4NBF4/PC.The samples modified by the different methods showed differences in chemical composition that introduced varying degrees of electrochemical performance enhancement.The presence of nitrogen enhanced the electron donor properties and the surface wettability of the activated carbons:this ensured a sufficient utilization of the exposed surface for charge storage.
文摘Z-scheme photocatalytic system has been regarded as a popular field of research in photoelectrochemical(PEC)water splitting.Among the many obstacles facing a Z-scheme photocatalytic system,the analysis methods of interfacial Z-scheme charge transfer still remain a significant challenge.Hence,in this study,CdS/Ti-Fe_(2)O_(3)heterojunction photoanodes are elaborately designed to explore the charge-transfer behavior in PEC water splitting.In this study,photophysical measurements,including the Kelvin probe measurement,surface photovoltage spectroscopy(SPV),and transient photovoltage spectroscopy(TPV),are used to monitor the migration behavior of photogenerated charges at the interface electric field of CdS/Ti-Fe_(2)O_(3)Z-scheme heterojunction photoanodes.The Kelvin probe and SPV measurements demonstrate that CdS/Ti-Fe_(2)O_(3)interfacial driving force favors the rapid transfer of photoexcited electrons to CdS.The double-beam strategy based on TPV indicates that more electrons of Ti-Fe_(2)O_(3)are combined with the holes of CdS owing to the intensive interface electric field.The results of these measurements successfully prove the Z-scheme migration mechanism of CdS/Ti-Fe_(2)O_(3)photoanodes.Benefiting from the desirable charge transfer at the interface electric field,CdS/Ti-Fe_(2)O_(3)photoanodes exhibit superior photocatalytic oxygen evolution reaction performance compared with that of pure Ti-Fe_(2)O_(3).The photocurrent density of the 25CdS/Ti-Fe_(2)O_(3)photoanode reaches 1.94 mA/cm^(2) at 1.23 V versus reversible hydrogen electrode without excess cocatalyst,and it is two times higher than that of pure Ti-Fe_(2)O_(3)photoanode.Therefore,an outstanding strategy is provided in this study to prove the Z-scheme charge-transfer mechanism of photocatalytic systems in PEC water splitting.
文摘Isothermal solidification process of a dissimilar transient liquid phase (TLP) bonding of FSX-414/MBF80/IN738 system was simulated by finite difference method. The TLP joint model was divided into two parts and a moving liquid /solid interface model was used for the parts. Diffusion equations were solved for each half of the joints simultaneously up to the end of isothermal solidification. The completion time of isothermal solidification, concentration profiles and position of the solid/liquid interface for each half were calculated. The intersection of the solid/liquid interfaces of two halves was considered the end of isothermal solidification. To obtain some required diffusion data, TLP bonding of FSX-414/MBF80/IN738 was performed at different temperature and time under vacuum atmosphere. The calculated results show good agreement with the experimental results.
文摘The surface and interface of heterojunction (HJ) formed with organic semiconductor (3,4,9,10-perylenetetracarboxylic dianhydride (PTCDA)) and inorganic semiconductor p-Si were measured and analyzed by X-ray photoelectron spectroscopy (XPS).The results indicate that, in PTCDA molecule,the binding energy ( E b) of C is 284.6 eV and 288.3 eV, corresponding to C of the perylene and C of the anhydride, respectively, and the binding energy of O is 531.3 eV and 531.1 eV, corresponding to C of C=O in the anhydrides and C of C-O-C, respectively. Moreover, PTCDA lost its anhydrides and only its perylenes were left in the HJ interface.
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Although photocatalytic water splitting has excellent potential for converting solar energy into chemical energy,the challenging charge separation process and sluggish surface catalytic reactions significantly limit progress in solar energy conversion using semiconductor photocatalysts.Herein,we demonstrate a feasible strategy involving the surface assembly of cobalt oxide species(CoO_(x))on a visible-light-responsive Cd_(0.9)Zn_(0.1)S(CZS)photocatalyst to fabricate a hierarchical CZS@CoO_(x) heterostructure.The unique hierarchical structure effectively accelerates the directional transfer of photogenerated charges,reducing charge recombination through the smooth interfacial heterojunction between CZS and CoO_(x),as evidenced by photoluminescence(PL)spectroscopy and various electrochemical characterizations.The surface cobalt species on the CZS material also act as efficient cocatalysts for photocatalytic hydrogen production,with activity even higher than that of noble metals.The well-defined CZS@CoO_(x) heterostructure not only enhances the interfacial separation of photoinduced charges,but also improves surface catalytic reactions.This leads to superior photocatalytic performances,with an apparent quantum efficiency of 20%at 420 nm for visible-light-driven hydrogen generation,which is one of the highest quantum efficiencies measured among noble-metal-free photocatalysts.Our work presents a potential pathway for controlling complex charge separation and catalytic reaction processes in photocatalysis,guiding the practical development of artificial photocatalysts for successful transformation of solar to chemical energy.