Photoelectrocatalytic seawater splitting is a promising low-cost method to produce green hydrogen in a large scale.The effects of Cl^(-)ions in seawater on the performance of a photoanode have been reported in previou...Photoelectrocatalytic seawater splitting is a promising low-cost method to produce green hydrogen in a large scale.The effects of Cl^(-)ions in seawater on the performance of a photoanode have been reported in previous studies.However,few researches have been done on the roles of Cl^(-)ions in a photocathode.Herein,for the first time,we find that Cl^(-)ions in the electrolyte improve the photocurrent of a Si/In_(2)S_(3) photocathode by 50% at-0.6 V_(RHE).An in-situ X-ray photoelectron spectroscopy(XPS)characterization combined with the time-of-flight secondary-ion mass spectrometry by simulating photoelectrochemical conditions was used to investigate the interface charge transfer mechanism.The results suggest that there is an In_(2)^(+3)S_(3-x)(OH)_(2x)layer on the surface of In_(2)S_(3) in the phosphate buffer solution(PBS)electrolyte,which plays a role as an interface charge transfer mediator in the Si/In_(2)S_(3) photocathode.The In_(2)^(+3)S_(3-x)(OH)_(2x)surface layer becomes In_(2)^(+3)S_(3-x)(Cl)_(2x)in the PBS electrolyte with NaCl and accelerates the charge transfer rate at the In_(2)S_(3)/electrolyte interface.These results offer a new concept of regulating interface charge transfer mediator to enhance the performance of photoelectrocatalytic seawater splitting for hydrogen production.展开更多
Molybdenum trioxide(MoO_(3))can be employed as an excellent host for intercalation due to its 2D lay-ered structure that connected by van der Waals interactions.Herein,a series of polyoxometalate-based MoO_(3) composi...Molybdenum trioxide(MoO_(3))can be employed as an excellent host for intercalation due to its 2D lay-ered structure that connected by van der Waals interactions.Herein,a series of polyoxometalate-based MoO_(3) composites(Al_(13)@MoO_(3))were successfully prepared by interpolating the Keggin-type polycationic AlO_(4)Al_(12)(OH)_(24)H_(2)O_(12)^(7+)(Al_(13))into MoO_(3)gallery.These composites can be applied to rapidly adsorb the anionic dye methyl orange(MO)through strong electrostatic interactions lead to compact and sta-ble gathering in the surrounding of the numerous charged Al_(13).Adsorption behaviors of composites with the different amount of Al_(13) were determined,these results revealed that Al_(13)-3.34%@MoO_(3)exhibited the most remarkable adsorption capacity.More importantly,the composite maintains superior adsorption capacity for five consecutive adsorption/desorption cycles,suggesting that Al_(13)@MoO_(3)can be an efficient and durable adsorbent.展开更多
A [ReO（Amino）2OH] complex was successfully synthesized by the ligand exchange method using oxorhenuim gluconate and an aminothiazole ligand. The complex was characterized elemental analysis and IR, UV-Vis, NMR and m...A [ReO（Amino）2OH] complex was successfully synthesized by the ligand exchange method using oxorhenuim gluconate and an aminothiazole ligand. The complex was characterized elemental analysis and IR, UV-Vis, NMR and mass spectroscopes. The technetium tracer 99mTcO-complex has also been synthesized by two methods using Ligand exchange method and direct reduction method. The radiochemical purity of the complex was over 95% as measured by thin layer chromatography. In vitro studies showed that the complex possessed good stability under physiological conditions. The partition coefficient indicated that the complex hydrophilic and the electrophoresis results showed that the complex neutral. Normal biodistributions of the 99mTC complex exhibit high lung, liver and spleen uptake of 27%, I 1%, and 12%, respectively. Blood and lungs clearance was quite, while liver activity remained high for a longer period with 12% injection dose present at 1 h post-inj ection. The radioactivity from the novel technetium complex was excreted mainly through the hepatobiliary system, which passed 35% of the complex at 1 h post-injection, and partially through the kidneys.展开更多
Zinc ion hybrid supercapacitors(ZHS)have received much attention due to the enhanced potential window range and high specific capacity.However,the appropriate positive materials with high electrochemical performance a...Zinc ion hybrid supercapacitors(ZHS)have received much attention due to the enhanced potential window range and high specific capacity.However,the appropriate positive materials with high electrochemical performance are still a challenge.Herein,NH_(4)^(+)and glycerate anions pre-inserted Mo glycerate(N-MoG)spheres are synthesized and serve as the template to form NH_(4)^(+)intercalated Ni_(3)S_(2)/Ni_(3)O_(2)(OH)_(4)@MoS_(2)core–shell nanoflower(N-NiMo-OS)in-situ grown on nickel foam(NF)(N-NiMo-OS/NF)by sulfurization treatment.Compared with the product using traditional MoG as a template,N-NiMo-OS/NF inheriting a larger core structure from N-MoG delivers enhanced space for ions transport and volume expansion during the energy storage process,together with the synergistic effects of multi-components and the heterostructure,the as-prepared N-NiMo-OS/NF nanoflower exhibits excellent performance for the battery-type hybrid supercapacitors(BHS)and ZHS devices.Notably,the ZHS device delivers superior electrochemical performance to the BHS device,such as a higher specific capacity of 327.5 mAh·g^(−1)at 1 A·g^(−1),a preeminent energy density of 610.6 Wh·kg^(−1)at 1710 W·kg^(−1),long cycle life.The in-situ Raman,ex-situ X-ray photoelectron spectroscopy(XPS),theoretical calculation demonstrate the extra Zn^(2+)insertion/extraction storage mechanism provides enhanced electrochemical performance for ZHS device.Therefore,the dual-ion pre-inserted strategy can be extended for other advanced electrode materials in energy storage fields.展开更多
基金supported by the National Natural Science Foundation of China(22279052)the China Postdoctoral Science Foundation(2023M741613)。
文摘Photoelectrocatalytic seawater splitting is a promising low-cost method to produce green hydrogen in a large scale.The effects of Cl^(-)ions in seawater on the performance of a photoanode have been reported in previous studies.However,few researches have been done on the roles of Cl^(-)ions in a photocathode.Herein,for the first time,we find that Cl^(-)ions in the electrolyte improve the photocurrent of a Si/In_(2)S_(3) photocathode by 50% at-0.6 V_(RHE).An in-situ X-ray photoelectron spectroscopy(XPS)characterization combined with the time-of-flight secondary-ion mass spectrometry by simulating photoelectrochemical conditions was used to investigate the interface charge transfer mechanism.The results suggest that there is an In_(2)^(+3)S_(3-x)(OH)_(2x)layer on the surface of In_(2)S_(3) in the phosphate buffer solution(PBS)electrolyte,which plays a role as an interface charge transfer mediator in the Si/In_(2)S_(3) photocathode.The In_(2)^(+3)S_(3-x)(OH)_(2x)surface layer becomes In_(2)^(+3)S_(3-x)(Cl)_(2x)in the PBS electrolyte with NaCl and accelerates the charge transfer rate at the In_(2)S_(3)/electrolyte interface.These results offer a new concept of regulating interface charge transfer mediator to enhance the performance of photoelectrocatalytic seawater splitting for hydrogen production.
基金the National Natural Science Foundation of China(Nos.21872021,21671033,22172022 and 22071019).
文摘Molybdenum trioxide(MoO_(3))can be employed as an excellent host for intercalation due to its 2D lay-ered structure that connected by van der Waals interactions.Herein,a series of polyoxometalate-based MoO_(3) composites(Al_(13)@MoO_(3))were successfully prepared by interpolating the Keggin-type polycationic AlO_(4)Al_(12)(OH)_(24)H_(2)O_(12)^(7+)(Al_(13))into MoO_(3)gallery.These composites can be applied to rapidly adsorb the anionic dye methyl orange(MO)through strong electrostatic interactions lead to compact and sta-ble gathering in the surrounding of the numerous charged Al_(13).Adsorption behaviors of composites with the different amount of Al_(13) were determined,these results revealed that Al_(13)-3.34%@MoO_(3)exhibited the most remarkable adsorption capacity.More importantly,the composite maintains superior adsorption capacity for five consecutive adsorption/desorption cycles,suggesting that Al_(13)@MoO_(3)can be an efficient and durable adsorbent.
文摘A [ReO（Amino）2OH] complex was successfully synthesized by the ligand exchange method using oxorhenuim gluconate and an aminothiazole ligand. The complex was characterized elemental analysis and IR, UV-Vis, NMR and mass spectroscopes. The technetium tracer 99mTcO-complex has also been synthesized by two methods using Ligand exchange method and direct reduction method. The radiochemical purity of the complex was over 95% as measured by thin layer chromatography. In vitro studies showed that the complex possessed good stability under physiological conditions. The partition coefficient indicated that the complex hydrophilic and the electrophoresis results showed that the complex neutral. Normal biodistributions of the 99mTC complex exhibit high lung, liver and spleen uptake of 27%, I 1%, and 12%, respectively. Blood and lungs clearance was quite, while liver activity remained high for a longer period with 12% injection dose present at 1 h post-inj ection. The radioactivity from the novel technetium complex was excreted mainly through the hepatobiliary system, which passed 35% of the complex at 1 h post-injection, and partially through the kidneys.
基金the National Natural Science Foundation of China(Nos.21702116,51772162,and 52072197)the 111 Project of China(No.D20017)+5 种基金Shandong Provincial Key Research and Development Program,China(No.2019GSF107087)Qingdao Postdoctoral Sustentation Fund,Youth Innovation and Technology Foundation of Shandong Higher Education Institutions,China(No.2019KJC004)Outstanding Youth Foundation of Shandong Province,China(No.ZR2019JQ14)Taishan Scholar Young Talent Program(No.tsqn201909114)Major Scientific and Technological Innovation Project(No.2019JZZY020405)Major Basic Research Program of Natural Science Foundation of Shandong Province(No.ZR2020ZD09).
文摘Zinc ion hybrid supercapacitors(ZHS)have received much attention due to the enhanced potential window range and high specific capacity.However,the appropriate positive materials with high electrochemical performance are still a challenge.Herein,NH_(4)^(+)and glycerate anions pre-inserted Mo glycerate(N-MoG)spheres are synthesized and serve as the template to form NH_(4)^(+)intercalated Ni_(3)S_(2)/Ni_(3)O_(2)(OH)_(4)@MoS_(2)core–shell nanoflower(N-NiMo-OS)in-situ grown on nickel foam(NF)(N-NiMo-OS/NF)by sulfurization treatment.Compared with the product using traditional MoG as a template,N-NiMo-OS/NF inheriting a larger core structure from N-MoG delivers enhanced space for ions transport and volume expansion during the energy storage process,together with the synergistic effects of multi-components and the heterostructure,the as-prepared N-NiMo-OS/NF nanoflower exhibits excellent performance for the battery-type hybrid supercapacitors(BHS)and ZHS devices.Notably,the ZHS device delivers superior electrochemical performance to the BHS device,such as a higher specific capacity of 327.5 mAh·g^(−1)at 1 A·g^(−1),a preeminent energy density of 610.6 Wh·kg^(−1)at 1710 W·kg^(−1),long cycle life.The in-situ Raman,ex-situ X-ray photoelectron spectroscopy(XPS),theoretical calculation demonstrate the extra Zn^(2+)insertion/extraction storage mechanism provides enhanced electrochemical performance for ZHS device.Therefore,the dual-ion pre-inserted strategy can be extended for other advanced electrode materials in energy storage fields.
