Two-dimensional mesoporous ultrathin Cd0.5Zn0.5S nanosheets with a thickness of~1.5 nm were fabricated using a multistep chemical transformation strategy involving inorganic–organic hybrid ZnS-ethylenediamine(denoted...Two-dimensional mesoporous ultrathin Cd0.5Zn0.5S nanosheets with a thickness of~1.5 nm were fabricated using a multistep chemical transformation strategy involving inorganic–organic hybrid ZnS-ethylenediamine(denoted as ZnS(en)0.5)as a hard template.Inorganic–organic hybrid ZnS(en)0.5,Cd0.5Zn0.5S(en)x,and Cd0.5Zn0.5S nanosheets were sequentially fabricated,and their transformation processes were analyzed in detail.The fabricated Cd0.5Zn0.5S nanosheets exhibited high photocatalytic hydrogen evolution reaction activity in the presence of a sacrificial agent.The Cd0.5Zn0.5S nanosheets exhibited remarkably high H2 production activity of~1395μmol∙h^−1∙g^−1 in pure water with no co-catalyst,which is the highest value reported thus far for bare photocatalysts,to the best of our knowledge.The high activity of these nanosheets is attributed to their distinct nanostructure(e.g.,short transfer distance of photoinduced charge carriers,large number of unsaturated surface atoms,and large surface area).Moreover,ternary NiCo2S4 nanoparticles were employed to facilitate the charge separation and enhance the surface kinetics of H2 evolution.The H2 production rate reached~62.2 and~2436μmol∙h^−1∙g^−1 in triethanolamine and pure water,respectively,over the NiCo2S4/Cd0.5Zn0.5S heterojunctions.The result indicated that the Schottky junction was critical to the enhanced activity.The proposed method can be used for fabricating other highly efficient CdZnS-based photocatalysts for solar-energy conversion or other applications.展开更多
The development of low-cost semiconductor photocatalysts for highly efficient and durable photocatalytic H2 evolution under visible light is very challenging.In this study,we combine low-cost metallic Ni3C cocatalysts...The development of low-cost semiconductor photocatalysts for highly efficient and durable photocatalytic H2 evolution under visible light is very challenging.In this study,we combine low-cost metallic Ni3C cocatalysts with twin nanocrystal Zn0.5Cd0.5S(ZCS)solid solution homojunctions for an efficient visible-light-driven H2 production by a simple approach.As-synthesized Zn0.5Cd0.5S-1%Ni3C(ZCS-1)heterojunction/homojunction nanohybrid exhibited the highest photocatalytic H2-evolution rate of 783μmol h‒1 under visible light,which is 2.88 times higher than that of pristine twin nanocrystal ZCS solid solution.The apparent quantum efficiencies of ZCS and ZCS-1 are measured to be 6.13%and 19.25%at 420 nm,respectively.Specifically,the homojunctions between the zinc blende and wurtzite segments in twin nanocrystal ZCS solid solution can significantly improve the light absorption and separation of photogenerated electron-hole pairs.Furthermore,the heterojunction between ZCS and metallic Ni3C NP cocatalysts can efficiently trap excited electrons from ZCS solid solution and enhance the H2-evolution kinetics at the surface for improving catalytic activity.This study demonstrates a unique one-step strategy for constructing heterojunction/homojunction hybrid nanostructures for a more efficient photocatalytic H2 evolution compared to other noble metal photocatalytic systems.展开更多
The design and construction of low‐cost and high‐performance hybrid materials for the photocatalytic hydrogen production reaction(HER)are extremely important for the large‐scale application of hydrogen energy.Metal...The design and construction of low‐cost and high‐performance hybrid materials for the photocatalytic hydrogen production reaction(HER)are extremely important for the large‐scale application of hydrogen energy.Metal‐organic frameworks(MOFs)are considered to be potential photocatalytic materials.Herein,monodisperse,small size,non‐precious metal transition metal phosphide Ni2P is encapsulated into a typical MOF(UiO‐66‐NH2)as a hybrid core‐shell cocatalyst to modify Zn_(0.5)Cd_(0.5)S for photocatalytic hydrogen production.Ni2P is wrapped in UiO‐66‐NH_(2)via an in situ solvothermal method,and Zn_(0.5)Cd_(0.5)S sulfide is decorated with a core‐shell Ni_(2)P@UiO‐66‐NH_(2)cocatalyst to obtain ternary Ni_(2)P@UiO‐66‐NH_(2)/Zn_(0.5)Cd_(0.5)S composite materials.Photoelectric and chemical characterization confirms that the ternary composites have good kinetic hydrogen production performance.The hydrogen production rate of 10%10 mg Ni_(2)P@UiO‐66‐NH_(2)/Zn_(0.5)Cd_(0.5)S reaches 40.91 mmol·g^(–1)·h^(–1)with an apparent quantum efficiency at 420 nm of 13.57%.The addition of 10 mg Ni_(2)P@UiO‐66‐NH_(2)increases the surface area of the ternary material,providing abundant reaction sites and forming an efficient charge transfer channel,which is conducive to efficient hydrogen production by the ternary photocatalysts.It is shown that the formation of a ternary composite system is beneficial to the occurrence of an efficient catalytic reaction.This study provides a new perspective for the construction of high‐performance photocatalytic materials.展开更多
The microstructure evolution and mechanical properties of Mg–6Zn–0.5Ce–xMn(x=0 and 1 wt.%)wrought magnesium alloys were researched,and the morphologies and role of Mn element in the experimental alloys were analyze...The microstructure evolution and mechanical properties of Mg–6Zn–0.5Ce–xMn(x=0 and 1 wt.%)wrought magnesium alloys were researched,and the morphologies and role of Mn element in the experimental alloys were analyzed.The research shows that all of Mn elements form theα-Mn pure phases,which do not participate in the formation of other phases,such as theτ-phases.The mechanical properties of Mn-containing alloys in as-extruded and aged states are superior to Mn-free alloys.During the hot extrusion process,the dispersed fineα-Mn particle phase hinders the migration of grain boundaries and inhibits dynamic recrystallization,which mainly takes effect of grain refining and dispersion hardening.During the aging treatments,the dispersed fineα-Mn particle phase not only hinders the growth of the solution-treated grains,but also becomes the nucleation cores ofβ1 rod-like precipitate phase,which is conducive to increasing the nucleation rate of the precipitate phase.For the aged alloy,the Mn addition mainly takes effect of grain refining and promoting aging strengthening.展开更多
The microstructure revolution and mechanical properties of as-extruded and peak-aged Mg−6Zn−1Mn−4Sn−0.5Ca(ZMT614−0.5Ca)alloy were studied by OM,SEM,TEM,hardness testing and tensile testing.The results showed that the ...The microstructure revolution and mechanical properties of as-extruded and peak-aged Mg−6Zn−1Mn−4Sn−0.5Ca(ZMT614−0.5Ca)alloy were studied by OM,SEM,TEM,hardness testing and tensile testing.The results showed that the as-cast ZMT614−0.5Ca alloy mainly consisted of α-Mg,Mg−Zn and CaMgSn phase.The hot extrusion process effectively refined the microstructure and led to a completely dynamic recrystallized microstructure.The average grain size of as-extruded alloy was^4.85μm.After solution treatment,remained CaMgSn with high melting point played a significant role in pinning effect and impeding the migration of grain boundary.After aging treatment,peak-aged ZMT614−0.5Ca alloy exhibited a good combination of strength and ductility,with yield strength,ultimate tensile strength and elongation being 338 MPa,383 MPa and 7.5%,respectively.The yield strength of the alloy increased significantly by around 36%compared with that in as-extruded condition,which should be attributed to the precipitation strengthening of β'phase.展开更多
Silver (I) was removed from aqueous environment by aloe vera shell ash supported Ni0.5Zn0.5Fe2O4 magnetic nanoparticles.The adsorbent was characterized by several methods including X-ray diffraction (XRD), scanning el...Silver (I) was removed from aqueous environment by aloe vera shell ash supported Ni0.5Zn0.5Fe2O4 magnetic nanoparticles.The adsorbent was characterized by several methods including X-ray diffraction (XRD), scanning electron microscopy (SEM), BETisotherm, vibrating sample magnetometer (VSM) and Fourier transform infrared spectroscopy (FT-IR). To determine the absorptionof silver (I) by this adsorbent, different pH values (2?7), adsorbent dose (0.01?0.5 g), concentrations of Ag+ (50, 100, 200, 300, 500,700 and 1000 mg/L) and exposure time (5?100 min) were experimented. The highest removal efficiency of Ag+ was achieved underoptimum condition (30 min and pH=5). The optimum adsorbent dose was 0.20 g (in 50 mL of 100 mg/L Ag+ solution), whichachieved a removal efficiency of 98.3%. The maximum monolayer adsorption capacity based on the Langmuir isotherm is243.90 mg/g. Characterization results revealed that specific surface area and porous volume were 814.23 m2/g and 0.726 cm3/g,respectively. The experimental data were fitted well with the Langmuir and Freundlich isotherm models. Synthesized adsorbent has desired surface area and adsorptive capacity for silver (I) adsorption in aquatic environment.展开更多
Photocatalytic water splitting for hydrogen(H_(2))production is a green sustainable technology,in which highly-efficient steady photocatalysts are fundamentally required.In this work,unique CdS/Cd_(0.5)Zn_(0.5)S-M0_(1...Photocatalytic water splitting for hydrogen(H_(2))production is a green sustainable technology,in which highly-efficient steady photocatalysts are fundamentally required.In this work,unique CdS/Cd_(0.5)Zn_(0.5)S-M0_(1-x)W_(x)S_(2) photocatalyst constructed by CdS hollow nano-spheres with successively surface-modified Cd_(0.5)Zn_(0.5)S shell and defect-rich MO_(1-x)W_(x)S_(2) ultrathin nanosheets was reported for the first time.Interestingly,the Cd_(0.5)Zn_(0.5)S shell could greatly enhance the photo-stability and reduce the carrier recombination of CdS.Meanwhile,enriching active sites and accelerating charge transfer could be achieved via anchoring defect-rich Mo_(1-x)W_(x)S_(2) onto CdS/Cd_(0.5)Zn_(0.5)S hollow heterostructures.Specifically,the optimized CdS/Cd_(0.5)Zn_(0.5)S-Mo_(1-x)W_(x)Sa(6 h Cd_(0.5)Zn_(0.5)S-coating,7 wt.%Mo_(1-x)W_(x)S_(2),x=0.5)hybrid delivered an exceptional H_(2) generation rate of 215.99 mmol·g^(-1)·h^(-1),which is approximately 502,134,and 23 times that of pure CdS,CdS/Cd_(0.5)Zn_(0.5)S,and 3 wt.%Pt-loaded CdS/Cd_(0.5)Zn_(0.5)S,respectively.Remarkably,a high H_(2) evolution reaction(HER)apparent quantum yield(AQY)of 64.81%was obtained under 420-nm irradiation.In addition,the CdS/Cd_(0.5)Zn_(0.5)S-Mo_(1-x)W_(x)S_(2) was also durable for H2 production under long-term irradiation.This work provides valuable inspirations to rational design and synthesis of efficient and stable hybrid photocatalysts for solar energy conversion.展开更多
Spin-polarized first-principle was performed to study the structural stability and the electronic states of Cr doped ZnS with the Cr component of 50% in zincblende （ZB）, wurtzite （W） and rocksalt （RS） structures...Spin-polarized first-principle was performed to study the structural stability and the electronic states of Cr doped ZnS with the Cr component of 50% in zincblende （ZB）, wurtzite （W） and rocksalt （RS） structures under pressure. The results show that the zincblende and wurtzite structures become unstable under low pressures of about 4.68 and 9.61 GPa, respectively, but the rocksalt structure can be maintained up to an extremely high pressure of about 32.92 GPa. Both zincblende and wurtzite Zno.sCro.5S display half metallic features under pressure, while rocksalt Zno.sCro.sS exhibits metallic feature. The half metallic features can be ascribed to the stronger interactions between S-3p and Cr-3d states and the metallic feature is due to the higher crystal symmetry of rocksalt Zn0.5Cr0.5S. These results can provide helpful guidance for Cr doped ZnS to be used in spintronic devices.展开更多
文摘Two-dimensional mesoporous ultrathin Cd0.5Zn0.5S nanosheets with a thickness of~1.5 nm were fabricated using a multistep chemical transformation strategy involving inorganic–organic hybrid ZnS-ethylenediamine(denoted as ZnS(en)0.5)as a hard template.Inorganic–organic hybrid ZnS(en)0.5,Cd0.5Zn0.5S(en)x,and Cd0.5Zn0.5S nanosheets were sequentially fabricated,and their transformation processes were analyzed in detail.The fabricated Cd0.5Zn0.5S nanosheets exhibited high photocatalytic hydrogen evolution reaction activity in the presence of a sacrificial agent.The Cd0.5Zn0.5S nanosheets exhibited remarkably high H2 production activity of~1395μmol∙h^−1∙g^−1 in pure water with no co-catalyst,which is the highest value reported thus far for bare photocatalysts,to the best of our knowledge.The high activity of these nanosheets is attributed to their distinct nanostructure(e.g.,short transfer distance of photoinduced charge carriers,large number of unsaturated surface atoms,and large surface area).Moreover,ternary NiCo2S4 nanoparticles were employed to facilitate the charge separation and enhance the surface kinetics of H2 evolution.The H2 production rate reached~62.2 and~2436μmol∙h^−1∙g^−1 in triethanolamine and pure water,respectively,over the NiCo2S4/Cd0.5Zn0.5S heterojunctions.The result indicated that the Schottky junction was critical to the enhanced activity.The proposed method can be used for fabricating other highly efficient CdZnS-based photocatalysts for solar-energy conversion or other applications.
文摘The development of low-cost semiconductor photocatalysts for highly efficient and durable photocatalytic H2 evolution under visible light is very challenging.In this study,we combine low-cost metallic Ni3C cocatalysts with twin nanocrystal Zn0.5Cd0.5S(ZCS)solid solution homojunctions for an efficient visible-light-driven H2 production by a simple approach.As-synthesized Zn0.5Cd0.5S-1%Ni3C(ZCS-1)heterojunction/homojunction nanohybrid exhibited the highest photocatalytic H2-evolution rate of 783μmol h‒1 under visible light,which is 2.88 times higher than that of pristine twin nanocrystal ZCS solid solution.The apparent quantum efficiencies of ZCS and ZCS-1 are measured to be 6.13%and 19.25%at 420 nm,respectively.Specifically,the homojunctions between the zinc blende and wurtzite segments in twin nanocrystal ZCS solid solution can significantly improve the light absorption and separation of photogenerated electron-hole pairs.Furthermore,the heterojunction between ZCS and metallic Ni3C NP cocatalysts can efficiently trap excited electrons from ZCS solid solution and enhance the H2-evolution kinetics at the surface for improving catalytic activity.This study demonstrates a unique one-step strategy for constructing heterojunction/homojunction hybrid nanostructures for a more efficient photocatalytic H2 evolution compared to other noble metal photocatalytic systems.
文摘The design and construction of low‐cost and high‐performance hybrid materials for the photocatalytic hydrogen production reaction(HER)are extremely important for the large‐scale application of hydrogen energy.Metal‐organic frameworks(MOFs)are considered to be potential photocatalytic materials.Herein,monodisperse,small size,non‐precious metal transition metal phosphide Ni2P is encapsulated into a typical MOF(UiO‐66‐NH2)as a hybrid core‐shell cocatalyst to modify Zn_(0.5)Cd_(0.5)S for photocatalytic hydrogen production.Ni2P is wrapped in UiO‐66‐NH_(2)via an in situ solvothermal method,and Zn_(0.5)Cd_(0.5)S sulfide is decorated with a core‐shell Ni_(2)P@UiO‐66‐NH_(2)cocatalyst to obtain ternary Ni_(2)P@UiO‐66‐NH_(2)/Zn_(0.5)Cd_(0.5)S composite materials.Photoelectric and chemical characterization confirms that the ternary composites have good kinetic hydrogen production performance.The hydrogen production rate of 10%10 mg Ni_(2)P@UiO‐66‐NH_(2)/Zn_(0.5)Cd_(0.5)S reaches 40.91 mmol·g^(–1)·h^(–1)with an apparent quantum efficiency at 420 nm of 13.57%.The addition of 10 mg Ni_(2)P@UiO‐66‐NH_(2)increases the surface area of the ternary material,providing abundant reaction sites and forming an efficient charge transfer channel,which is conducive to efficient hydrogen production by the ternary photocatalysts.It is shown that the formation of a ternary composite system is beneficial to the occurrence of an efficient catalytic reaction.This study provides a new perspective for the construction of high‐performance photocatalytic materials.
基金funded by National Natural Science Foundation of China(Project No.51701172)Foundation of China Railway Eryuan Engineering Group Co.Ltd.(Project No.KYY2020035(21-21))+1 种基金Natural Science Foundation of Hunan Province(Project No.2018JJ3504)China Postdoctoral Science Foundation(Project No.2018M632977).
文摘The microstructure evolution and mechanical properties of Mg–6Zn–0.5Ce–xMn(x=0 and 1 wt.%)wrought magnesium alloys were researched,and the morphologies and role of Mn element in the experimental alloys were analyzed.The research shows that all of Mn elements form theα-Mn pure phases,which do not participate in the formation of other phases,such as theτ-phases.The mechanical properties of Mn-containing alloys in as-extruded and aged states are superior to Mn-free alloys.During the hot extrusion process,the dispersed fineα-Mn particle phase hinders the migration of grain boundaries and inhibits dynamic recrystallization,which mainly takes effect of grain refining and dispersion hardening.During the aging treatments,the dispersed fineα-Mn particle phase not only hinders the growth of the solution-treated grains,but also becomes the nucleation cores ofβ1 rod-like precipitate phase,which is conducive to increasing the nucleation rate of the precipitate phase.For the aged alloy,the Mn addition mainly takes effect of grain refining and promoting aging strengthening.
基金Project(2016YFB0301101)supported by the National Key Research and Development Program of ChinaProjects(51571040,U1764253,51531002)supported by the National Natural Science Foundation of China。
文摘The microstructure revolution and mechanical properties of as-extruded and peak-aged Mg−6Zn−1Mn−4Sn−0.5Ca(ZMT614−0.5Ca)alloy were studied by OM,SEM,TEM,hardness testing and tensile testing.The results showed that the as-cast ZMT614−0.5Ca alloy mainly consisted of α-Mg,Mg−Zn and CaMgSn phase.The hot extrusion process effectively refined the microstructure and led to a completely dynamic recrystallized microstructure.The average grain size of as-extruded alloy was^4.85μm.After solution treatment,remained CaMgSn with high melting point played a significant role in pinning effect and impeding the migration of grain boundary.After aging treatment,peak-aged ZMT614−0.5Ca alloy exhibited a good combination of strength and ductility,with yield strength,ultimate tensile strength and elongation being 338 MPa,383 MPa and 7.5%,respectively.The yield strength of the alloy increased significantly by around 36%compared with that in as-extruded condition,which should be attributed to the precipitation strengthening of β'phase.
基金the Islamic Azad University-Bandar Abbas Branch for financial support
文摘Silver (I) was removed from aqueous environment by aloe vera shell ash supported Ni0.5Zn0.5Fe2O4 magnetic nanoparticles.The adsorbent was characterized by several methods including X-ray diffraction (XRD), scanning electron microscopy (SEM), BETisotherm, vibrating sample magnetometer (VSM) and Fourier transform infrared spectroscopy (FT-IR). To determine the absorptionof silver (I) by this adsorbent, different pH values (2?7), adsorbent dose (0.01?0.5 g), concentrations of Ag+ (50, 100, 200, 300, 500,700 and 1000 mg/L) and exposure time (5?100 min) were experimented. The highest removal efficiency of Ag+ was achieved underoptimum condition (30 min and pH=5). The optimum adsorbent dose was 0.20 g (in 50 mL of 100 mg/L Ag+ solution), whichachieved a removal efficiency of 98.3%. The maximum monolayer adsorption capacity based on the Langmuir isotherm is243.90 mg/g. Characterization results revealed that specific surface area and porous volume were 814.23 m2/g and 0.726 cm3/g,respectively. The experimental data were fitted well with the Langmuir and Freundlich isotherm models. Synthesized adsorbent has desired surface area and adsorptive capacity for silver (I) adsorption in aquatic environment.
基金support from the National Natural Science Foundation of China(Nos.51802170,51772162,and 21801150)the Natural Science Foundation of Shandong Province(Nos.ZR2019MB001,ZR2018BEM014,and ZR2019JQ14)+3 种基金the Youth Innovation and Technology Foundation of Shandong Higher Education Institutions,China(No.2019KJC004)the Taishan Scholar Project of Shandong Province(No.ts201712047)the Special Fund Project to Guide Development of Local Science and Technology by Central Government,the Open Research Fund of State Key Laboratory of Inorganic Synthesis and Preparative Chemistry of Jilin University(No.2019-22)the Taishan Scholar Program of Advantage and Characteristic Discipline Team of Eco-Chemical Process and Technology.
文摘Photocatalytic water splitting for hydrogen(H_(2))production is a green sustainable technology,in which highly-efficient steady photocatalysts are fundamentally required.In this work,unique CdS/Cd_(0.5)Zn_(0.5)S-M0_(1-x)W_(x)S_(2) photocatalyst constructed by CdS hollow nano-spheres with successively surface-modified Cd_(0.5)Zn_(0.5)S shell and defect-rich MO_(1-x)W_(x)S_(2) ultrathin nanosheets was reported for the first time.Interestingly,the Cd_(0.5)Zn_(0.5)S shell could greatly enhance the photo-stability and reduce the carrier recombination of CdS.Meanwhile,enriching active sites and accelerating charge transfer could be achieved via anchoring defect-rich Mo_(1-x)W_(x)S_(2) onto CdS/Cd_(0.5)Zn_(0.5)S hollow heterostructures.Specifically,the optimized CdS/Cd_(0.5)Zn_(0.5)S-Mo_(1-x)W_(x)Sa(6 h Cd_(0.5)Zn_(0.5)S-coating,7 wt.%Mo_(1-x)W_(x)S_(2),x=0.5)hybrid delivered an exceptional H_(2) generation rate of 215.99 mmol·g^(-1)·h^(-1),which is approximately 502,134,and 23 times that of pure CdS,CdS/Cd_(0.5)Zn_(0.5)S,and 3 wt.%Pt-loaded CdS/Cd_(0.5)Zn_(0.5)S,respectively.Remarkably,a high H_(2) evolution reaction(HER)apparent quantum yield(AQY)of 64.81%was obtained under 420-nm irradiation.In addition,the CdS/Cd_(0.5)Zn_(0.5)S-Mo_(1-x)W_(x)S_(2) was also durable for H2 production under long-term irradiation.This work provides valuable inspirations to rational design and synthesis of efficient and stable hybrid photocatalysts for solar energy conversion.
基金the financial support of the project from the National Natural Science Foundation of China (No. 11104175)the National Basic Research Program of China (No. 2011CB610406)+1 种基金the "111 Project" of China (No. B08040)the Research Fund of the State Key Laboratory of Solidification Processing, China
文摘Spin-polarized first-principle was performed to study the structural stability and the electronic states of Cr doped ZnS with the Cr component of 50% in zincblende （ZB）, wurtzite （W） and rocksalt （RS） structures under pressure. The results show that the zincblende and wurtzite structures become unstable under low pressures of about 4.68 and 9.61 GPa, respectively, but the rocksalt structure can be maintained up to an extremely high pressure of about 32.92 GPa. Both zincblende and wurtzite Zno.sCro.5S display half metallic features under pressure, while rocksalt Zno.sCro.sS exhibits metallic feature. The half metallic features can be ascribed to the stronger interactions between S-3p and Cr-3d states and the metallic feature is due to the higher crystal symmetry of rocksalt Zn0.5Cr0.5S. These results can provide helpful guidance for Cr doped ZnS to be used in spintronic devices.
