Cu metal and its oxides have attracted much attention for photocatalytic CO_(2)reduction reaction(CO_(2)RR),but the stability and effects of Cu oxidation states on CO_(2)RR are not fully understood.Cu^(x+)/Cu^(0)-load...Cu metal and its oxides have attracted much attention for photocatalytic CO_(2)reduction reaction(CO_(2)RR),but the stability and effects of Cu oxidation states on CO_(2)RR are not fully understood.Cu^(x+)/Cu^(0)-loaded graphitic carbon nitride(g-C_(3)N_(4))heterojunctions(Cu-CuO_(x)/g-C_(3)N_(4))are fabricated via a stepwise calcination method for efficient photocatalytic CO_(2)RR.Cu_(2)O is the main component of Cu-CuO_(x)and the mixed valence Cu includes Cu^(0),Cu^(+),and Cu^(2+),which play the role of charge trapping sites and redox catalytic centers during the photocatalytic CO_(2)RR process.The main products were CO and CH_(4)for the CO_(2)RR with production rates of 14.45 and 0.66μmol g^(-1)h^(-1)for CO and CH_(4),which were higher than those for g-C_(3)N_(4)and Cu-CuO_(x),respectively.This photocatalytic CO_(2)RR performance is attributed to the ultrafast switching of“Cu^(x+)−Cu^(0)”and e_(CB^(−))/h_(VB^(+))trapping transformation in Cu-CuO_(x)benefited from the built-in IEF between Cu-CuO_(x)and g-C_(3)N_(4),increasing the efficient photogenerated e_(CB^(−)),and enabling the stability of Cu-CuO_(x)/g-C_(3)N_(4).Cu^(x+)adsorbed by H_(2)O works as the electron trapping site to change to Cu^(0)and switch to the hole trapping site;Cu^(0)works as the hole trapping site to change to Cu^(x+)and switch to the electron trapping site,causing the CO_(2)RR of the adsorbed CO_(2).Moreover,the coordinated Cu^(0)and Cu^(+)species facilitate the activation of the adsorbed CO_(2)and^(∗)CO generation,these adsorbed^(∗)CO on Cu^(0)and Cu^(+)detected by in-situ DRIFTS quickly transformed to^(∗)CHO with a lower energy barrier benefited from the mixed Cu^(0)/Cu^(+)active sites during CORR to produce CH_(4).This finding provides a new insight into the influence of mixed valence Cu during photocatalytic CO_(2)RR.展开更多
以分析纯Zn O、Cu O、Al2O3、Ti O2以及Sr CO3为原料,采用传统固相法制备了（1-x）Zn0.99Cu0.01Al2O4-x Sr Ti O3（ZCAST,x=0~0.045）微波介质陶瓷,利用X射线衍射仪、扫描电镜和网络分析仪对其结构、形貌和微波介电性能进行表征。研究...以分析纯Zn O、Cu O、Al2O3、Ti O2以及Sr CO3为原料,采用传统固相法制备了（1-x）Zn0.99Cu0.01Al2O4-x Sr Ti O3（ZCAST,x=0~0.045）微波介质陶瓷,利用X射线衍射仪、扫描电镜和网络分析仪对其结构、形貌和微波介电性能进行表征。研究了不同x值对ZCAST陶瓷相组成、显微结构以及微波介电性能的影响。结果表明,ZCAST陶瓷的体积密度、介电常数εr随着Sr Ti O3含量的增多而增大。当x=0.04具有最佳微波介电性能：介电常数εr=14.12,品质因数Q×f=28700 GHz,频率温度系数τf=-1.8×10-6/℃。展开更多
2LiFe1-xCoxPO4-Li3V2（P04）3/C was synthesized using Fel-2xCo2xVO4 as precursor which was prepared by a simple co-precipitation method. 2LiFej-xCoxPO4-Li3V2（PO4）3/C samples were characterized by X-ray diffraction （...2LiFe1-xCoxPO4-Li3V2（P04）3/C was synthesized using Fel-2xCo2xVO4 as precursor which was prepared by a simple co-precipitation method. 2LiFej-xCoxPO4-Li3V2（PO4）3/C samples were characterized by X-ray diffraction （XRD）, scanning electron microscopy （SEM） and electrochemical measurements. All 2LiFel-xCoxPOa-Li3V2（PO4）3/C composites are of the similar crystal structure. The XRD analysis and SEM images show that 2LiFe0.96Co0.04PO4-Li3V2（PO4）3/C sample has the best-ordered structure and the smallest particle size. The charge-discharge tests demonstrate that these powders have the best electrochemical properties with an initial discharge capacity of 144.1 mA.h/g and capacity retention of 95.6% after 100 cycles when cycled at a current density of 0.1C between 2.5 and 4.5 V.展开更多
Storing solar energy in battery systems is crucial to achieving a green and sustainable society.However,the efficient development of photo-enhanced zinc-air batteries(ZABs)is limited by the rapid recombination of phot...Storing solar energy in battery systems is crucial to achieving a green and sustainable society.However,the efficient development of photo-enhanced zinc-air batteries(ZABs)is limited by the rapid recombination of photogenerated carriers on the photocathode.In this work,the visible-light-driven CoS_(2)/CuS@CNT-C_(3)N_(4)photocatalyst with unique petal-like layer structure was designed and developed,which can be used as air electrode for visible-light-driven ZABs.The superior performance of ZABs assembled by CoS_(2)/CuS@CNT-C_(3)N_(4)was mainly attributed to the successful construction of Schottky heterojunction between g-C_(3)N_(4)and carbon nanotubes(CNTs),which accelerates the transfer of electrons from g-C_(3)N_(4)to CoS_(2)/CuS cocatalysts,improves the carrier separation ability,and extends the carrier lifetime.Thereinto,the visible-driven ZABs assembled by CoS_(2)/CuS@CNT-C_(3)N_(4)photocatalyst has a power density of 588.90 mW cm^(-2) and a charge-discharge cycle of 643 h under visible light irradiation,which is the highest performance ever reported for photo-enhanced ZABs.More importantly,the charge-discharge voltage drop of ZABs was only 0.54 V under visible light irradiation,which is significantly lower than the voltage drop(0.94 V)in the dark.This study provides a new idea for designing efficient and stable visible-light-driven ZABs cathode catalysts.展开更多
Nano TiO2/Fe3O4 composite particles with different molar ratios of TiO2 to Fe3O4 were prepared via sol-gel method. X-ray diffraction, transmission electron microscopy, and vibration sample magnetometry were used to ch...Nano TiO2/Fe3O4 composite particles with different molar ratios of TiO2 to Fe3O4 were prepared via sol-gel method. X-ray diffraction, transmission electron microscopy, and vibration sample magnetometry were used to characterize the TiO2/Fe3O4 particles. The photocatalytic activity of the particles was tested by degrading methyl blue solution under UV illumination （254 nm）. The results indicate that with the content of TiO2 increasing, the photocatalytic activity of the composite particles enhances, while the magnetism of the particles decreases. When the molar ratio of TiO2 to Fe3O4 is about 8, both the photocatalytic activity and magnetism of the TiO2/Fe3O4 particles are relatively high, and their photocatalytic activity remains well after repeated use.展开更多
Ag3PO4 is widely used in the field of photocatalysis because of its unique activity. However, photocorrosion limits its practical application. Therefore, it is very urgent to find a solution to improve the light corro...Ag3PO4 is widely used in the field of photocatalysis because of its unique activity. However, photocorrosion limits its practical application. Therefore, it is very urgent to find a solution to improve the light corrosion resistance of Ag3PO4. Herein, the Z-scheme WO3(H2O)0.333/Ag3PO4 composites are successfully prepared through microwave hydrothermal and simple stirring. The WO3(H2O)0.333/Ag3PO4 composites are characterized by X-ray diffraction, scanning electron microscopy, X-ray photoelectron spectroscopy and UV-Vis spectroscopy. In the degradation of organic pollutants, WO3(H2O)0.333/Ag3PO4 composites exhibit excellent performance under visible light. This is mainly attributed to the synergy of WO3(H2O)0.333 and Ag3PO4. Especially, the photocatalytic activity of 15%WO3(H2O)0.333/Ag3PO4 is the highest, and the methylene blue can be completely degraded in 4 min. In addition, the stability of the composites is also greatly enhanced. After five cycles of testing, the photocatalytic activity of 15%WO3(H2O)0.333/Ag3PO4 is not obviously decreased. However, the degradation efficiency of Ag3PO4 was only 20.2%. This indicates that adding WO3(H2O)0.333 can significantly improve the photoetching resistance of Ag3PO4. Finally, Z-scheme photocatalytic mechanism is investigated.展开更多
基金support of the National Natu-ral Science Foundation of China(No.62004143,22476058,and 22076052)the Key R&D Program of Hubei Province(No.2022BAA084).
文摘Cu metal and its oxides have attracted much attention for photocatalytic CO_(2)reduction reaction(CO_(2)RR),but the stability and effects of Cu oxidation states on CO_(2)RR are not fully understood.Cu^(x+)/Cu^(0)-loaded graphitic carbon nitride(g-C_(3)N_(4))heterojunctions(Cu-CuO_(x)/g-C_(3)N_(4))are fabricated via a stepwise calcination method for efficient photocatalytic CO_(2)RR.Cu_(2)O is the main component of Cu-CuO_(x)and the mixed valence Cu includes Cu^(0),Cu^(+),and Cu^(2+),which play the role of charge trapping sites and redox catalytic centers during the photocatalytic CO_(2)RR process.The main products were CO and CH_(4)for the CO_(2)RR with production rates of 14.45 and 0.66μmol g^(-1)h^(-1)for CO and CH_(4),which were higher than those for g-C_(3)N_(4)and Cu-CuO_(x),respectively.This photocatalytic CO_(2)RR performance is attributed to the ultrafast switching of“Cu^(x+)−Cu^(0)”and e_(CB^(−))/h_(VB^(+))trapping transformation in Cu-CuO_(x)benefited from the built-in IEF between Cu-CuO_(x)and g-C_(3)N_(4),increasing the efficient photogenerated e_(CB^(−)),and enabling the stability of Cu-CuO_(x)/g-C_(3)N_(4).Cu^(x+)adsorbed by H_(2)O works as the electron trapping site to change to Cu^(0)and switch to the hole trapping site;Cu^(0)works as the hole trapping site to change to Cu^(x+)and switch to the electron trapping site,causing the CO_(2)RR of the adsorbed CO_(2).Moreover,the coordinated Cu^(0)and Cu^(+)species facilitate the activation of the adsorbed CO_(2)and^(∗)CO generation,these adsorbed^(∗)CO on Cu^(0)and Cu^(+)detected by in-situ DRIFTS quickly transformed to^(∗)CHO with a lower energy barrier benefited from the mixed Cu^(0)/Cu^(+)active sites during CORR to produce CH_(4).This finding provides a new insight into the influence of mixed valence Cu during photocatalytic CO_(2)RR.
文摘以分析纯Zn O、Cu O、Al2O3、Ti O2以及Sr CO3为原料,采用传统固相法制备了（1-x）Zn0.99Cu0.01Al2O4-x Sr Ti O3（ZCAST,x=0~0.045）微波介质陶瓷,利用X射线衍射仪、扫描电镜和网络分析仪对其结构、形貌和微波介电性能进行表征。研究了不同x值对ZCAST陶瓷相组成、显微结构以及微波介电性能的影响。结果表明,ZCAST陶瓷的体积密度、介电常数εr随着Sr Ti O3含量的增多而增大。当x=0.04具有最佳微波介电性能：介电常数εr=14.12,品质因数Q×f=28700 GHz,频率温度系数τf=-1.8×10-6/℃。
基金Project(51072233) supported by National Natural Science Foundation of China
文摘2LiFe1-xCoxPO4-Li3V2（P04）3/C was synthesized using Fel-2xCo2xVO4 as precursor which was prepared by a simple co-precipitation method. 2LiFej-xCoxPO4-Li3V2（PO4）3/C samples were characterized by X-ray diffraction （XRD）, scanning electron microscopy （SEM） and electrochemical measurements. All 2LiFel-xCoxPOa-Li3V2（PO4）3/C composites are of the similar crystal structure. The XRD analysis and SEM images show that 2LiFe0.96Co0.04PO4-Li3V2（PO4）3/C sample has the best-ordered structure and the smallest particle size. The charge-discharge tests demonstrate that these powders have the best electrochemical properties with an initial discharge capacity of 144.1 mA.h/g and capacity retention of 95.6% after 100 cycles when cycled at a current density of 0.1C between 2.5 and 4.5 V.
文摘Storing solar energy in battery systems is crucial to achieving a green and sustainable society.However,the efficient development of photo-enhanced zinc-air batteries(ZABs)is limited by the rapid recombination of photogenerated carriers on the photocathode.In this work,the visible-light-driven CoS_(2)/CuS@CNT-C_(3)N_(4)photocatalyst with unique petal-like layer structure was designed and developed,which can be used as air electrode for visible-light-driven ZABs.The superior performance of ZABs assembled by CoS_(2)/CuS@CNT-C_(3)N_(4)was mainly attributed to the successful construction of Schottky heterojunction between g-C_(3)N_(4)and carbon nanotubes(CNTs),which accelerates the transfer of electrons from g-C_(3)N_(4)to CoS_(2)/CuS cocatalysts,improves the carrier separation ability,and extends the carrier lifetime.Thereinto,the visible-driven ZABs assembled by CoS_(2)/CuS@CNT-C_(3)N_(4)photocatalyst has a power density of 588.90 mW cm^(-2) and a charge-discharge cycle of 643 h under visible light irradiation,which is the highest performance ever reported for photo-enhanced ZABs.More importantly,the charge-discharge voltage drop of ZABs was only 0.54 V under visible light irradiation,which is significantly lower than the voltage drop(0.94 V)in the dark.This study provides a new idea for designing efficient and stable visible-light-driven ZABs cathode catalysts.
基金supported by the National Natural Science Foundation of China (Nos. 50872011, 50402022, and 50672006)the National Basic Research Program of China (No. 2007CB613608)
文摘Nano TiO2/Fe3O4 composite particles with different molar ratios of TiO2 to Fe3O4 were prepared via sol-gel method. X-ray diffraction, transmission electron microscopy, and vibration sample magnetometry were used to characterize the TiO2/Fe3O4 particles. The photocatalytic activity of the particles was tested by degrading methyl blue solution under UV illumination （254 nm）. The results indicate that with the content of TiO2 increasing, the photocatalytic activity of the composite particles enhances, while the magnetism of the particles decreases. When the molar ratio of TiO2 to Fe3O4 is about 8, both the photocatalytic activity and magnetism of the TiO2/Fe3O4 particles are relatively high, and their photocatalytic activity remains well after repeated use.
基金supported by the National Natural Science Foundation of China(51572103 and 51502106)the Distinguished Young Scholar of Anhui Province(1808085J14)+2 种基金the Foundation for Young Talents in College of Anhui Province(gxyqZD2017051)the Key Foundation of Educational Commission of Anhui Province(KJ2016SD53)the Innovation Team of Design and Application of Advanced Energetic Materials(KJ2015TD003)~~
文摘Ag3PO4 is widely used in the field of photocatalysis because of its unique activity. However, photocorrosion limits its practical application. Therefore, it is very urgent to find a solution to improve the light corrosion resistance of Ag3PO4. Herein, the Z-scheme WO3(H2O)0.333/Ag3PO4 composites are successfully prepared through microwave hydrothermal and simple stirring. The WO3(H2O)0.333/Ag3PO4 composites are characterized by X-ray diffraction, scanning electron microscopy, X-ray photoelectron spectroscopy and UV-Vis spectroscopy. In the degradation of organic pollutants, WO3(H2O)0.333/Ag3PO4 composites exhibit excellent performance under visible light. This is mainly attributed to the synergy of WO3(H2O)0.333 and Ag3PO4. Especially, the photocatalytic activity of 15%WO3(H2O)0.333/Ag3PO4 is the highest, and the methylene blue can be completely degraded in 4 min. In addition, the stability of the composites is also greatly enhanced. After five cycles of testing, the photocatalytic activity of 15%WO3(H2O)0.333/Ag3PO4 is not obviously decreased. However, the degradation efficiency of Ag3PO4 was only 20.2%. This indicates that adding WO3(H2O)0.333 can significantly improve the photoetching resistance of Ag3PO4. Finally, Z-scheme photocatalytic mechanism is investigated.
