Bismuth containing nanomaterials recently received increasing attention with respect to environmental applications because of their low cost, high stability and nontoxicity. In this work, Bi–Bi_2O_2CO_3 heterojunctio...Bismuth containing nanomaterials recently received increasing attention with respect to environmental applications because of their low cost, high stability and nontoxicity. In this work, Bi–Bi_2O_2CO_3 heterojunctions were fabricated by in-situ decoration of Bi nanoparticles on Bi_2O_2CO_3 nanosheets via a simple hydrothermal synthesis approach. X-ray diffraction(XRD), scanning electron microscopy(SEM), transmission electron microscopy(TEM) and high-resolution TEM(HRTEM) were used to confirm the morphology of the nanosheet-like heterostructure of the Bi–Bi_2O_2CO_3 composite. Detailed ultrafast electronic spectroscopy reveals that the in-situ decoration of Bi nanoparticles on Bi_2O_2CO_3 nanosheets exhibit a dramatically enhanced electron-hole pair separation rate, which results in an extraordinarily high photocatalytic activity for the degradation of a model organic dye, methylene blue(MB) under visible light illumination. Cycling experiments revealed a good photochemical stability of the Bi–Bi_2O_2CO_3 heterojunction under repeated irradiation. Photocurrent measurements further indicated that the heterojunction incredibly enhanced the charge generation and suppressed the charge recombination of photogenerated electron-hole pairs.展开更多
Driven by safety issues,environmental concerns,and high costs,rechargeable aqueous zinc-ion batteries(ZIBs)have received increasing attention in recent years owing to their unique advantages.However,the sluggish kinet...Driven by safety issues,environmental concerns,and high costs,rechargeable aqueous zinc-ion batteries(ZIBs)have received increasing attention in recent years owing to their unique advantages.However,the sluggish kinetics of divalent charge Zn^(2+)in the cathode materials caused by the strong electrostatic interaction and their unsatisfactory cycle life hinder the development of ZIBs.Herein,organic cations and Zn^(2+)ions co-pre-inserted vanadium oxide([N(CH_(3))_(4)]_(0.77),Zn_(0.23))V_(8)O_(20)·3.8H_(2)O are reported as the cathode for ultra-stable aqueous ZIBs,in which the weaker electrostatic interactions between Zn^(2+)and organic ion-pinned vanadium oxide can induce the high reversibility of Zn^(2+)insertion and extraction,thereby improving the cycle life.It is demonstrated that([N(CH_(3))_(4)]_(0.77),Zn_(0.23))V_(8)O_(20)·3.8H_(2)O cathodes deliver a discharge capacity of 181 mA h g^(-1)at8 A g^(-1)and ultra-long life span(99.5%capacity retention after 2000 cycles).A reversible Zn^(2+)/H^(+)ions(de)intercalation storage process and pseudocapacitive charge storage are characterized.The weaker interactions between organic ion and Zn^(2+)open a novel avenue for the design of highly reversible cathode materials with long-term cycling stability.展开更多
Low-dimensional Bi2Fe4O9 nanosheets and microrods have been selectively prepared by a solvothermal method, from which the growth of the Bi2Fe4O9 crystals can be controlled by the variation of reaction conditions. Stru...Low-dimensional Bi2Fe4O9 nanosheets and microrods have been selectively prepared by a solvothermal method, from which the growth of the Bi2Fe4O9 crystals can be controlled by the variation of reaction conditions. Structure determination showed that the nanosheets are mainly exposed by {001} facets while the microrods are exposed by {110} facets. Ab- sorption spectra revealed that there are two bandgaps observed for both nanosheets （at 1.9 and 1.55 eV） and microrods （1.7 and 1.45 eV）, and they both would be available for the sunlight photocatalysis e ciently due to the intensive absorption ability in a wide region. Photocatalytic investigation demonstrated that the overall photocatalytic performance of the microrods is prior to that of the nanosheets due to the variation of bandgaps and exposed facets. The present report provides a useful alternative strategy for the controlling growth of nanostructures and/or microcrystals besides the present demonstration of the Bi2Fe4O9 crystals with diflerent bandgaps and facets that would be able to tune the corresponding photocatalytic ability selectively.展开更多
Gaseous nitrogen is abundant in the atmosphere,and its efficient conversion to ammonia is vital to the future of a greener and more sustainable world.Since the N≡N covalent triple bond is difficult to break,the adsor...Gaseous nitrogen is abundant in the atmosphere,and its efficient conversion to ammonia is vital to the future of a greener and more sustainable world.Since the N≡N covalent triple bond is difficult to break,the adsorption and activation of N_(2)molecules on the photocatalyst surface are critical to improve the efficiency of photocatalytic nitrogen fixation.In this work,Nb_(2)O_(5)·nH_(2)O nanosheets were synthesized by a hydrothermal reduction process with a weak reducing agent of glyoxal,which created more oxygen vacancies on their surfaces.Furthermore,their surface acidity was modulated by subsequent heat treatment in an Ar atmosphere.Thus,the effects of the oxygen vacancy and surface acidity on the photocatalytic nitrogen fixation performance of these Nb_(2)O_(5)·nH_(2)O nanosheets could be investigated.It was found that both factors contributed to the adsorption/activation of N_(2)and the charge carrier separation/transfer in these Nb_(2)O_(5)·nH_(2)O nanosheets.Owing to their synergistic effect,a high ammonia yield of 173.7μmol/(g·h)was achieved by these Nb_(2)O_(5)·nH_(2)O nanosheets through photocatalysis in pure water under simulated solar illumination without assistance from either sacrificial agents or cocatalysts.展开更多
High-efficiency photocatalysts are of great importance to satisfy the requirements of green chemistry nowadays.Here we reported a novel solar-driven photocatalyst fabricated by a facile surface modification method,wit...High-efficiency photocatalysts are of great importance to satisfy the requirements of green chemistry nowadays.Here we reported a novel solar-driven photocatalyst fabricated by a facile surface modification method,with the two-dimensional carboxylated zinc phthalocyanine-carboxylated C60-titanium dioxide(Zn Pc-C3-Ti O2)nanosheets,in which the surface modifications of Zn Pc and C60derivative were designed to extend the absorption range and promote charge separation,respectively.Benefiting from the unique structure and positive synergetic effect,the Zn Pc-C3-Ti O2 nanocomposite shows promising applications in selective reduction of nitroarenes for high-value-added aromatic amines under solar light.Especially,for the photocatalytic reduction of nitrobenzene to aniline,the Zn Pc-C3-Ti O2 nanocomposite possesses both high efficiency and selectivity(up to 99%).展开更多
The development of transition metal oxidebased electrode materials with proper controlled structures is highly desirable for high-performance supercapacitors.However,it remains a major challenge.Here,we present the fi...The development of transition metal oxidebased electrode materials with proper controlled structures is highly desirable for high-performance supercapacitors.However,it remains a major challenge.Here,we present the first synthesis of bowl-like Ni Co2O4nanosheet clusters through a simple soft template guided hydrothermal strategy.The resulting bowl-like clusters consist of numerous Ni Co2O4nanosheets with an average thickness of 19 nm and possess a mean diameter of 1μm along with a specific surface area of40 m2g^-1.Remarkably,serving as an electrode material in a three-electrode system,the bowl-like Ni Co2O4nanosheet clusters exhibit a high specific capacity of 1068 F g^-1at a current density of 1 A g^-1and excellent cycling stability with90%capacitance retention after 5000 charge-discharge cycles.Meanwhile,an asymmetric supercapacitor(ASC)assembled with the Ni Co2O4clusters and activated carbon(AC)as the two electrodes exhibits a high specific capacitance of 129 F g^-1at 1 A g^-1,along with a high energy density of 33 W h kg^-1at a power density of 0.66 k W kg^-1.Such performance is superior to those of many commercial supercapacitors.This study opens a new avenue for the construction of ordered complex particles with controlled architectures for energy storage and conversion applications.展开更多
NiCo2O4 nanosheets with sheaf-like nanostructure morphologies have been synthesized by a facile one-step hydrothermal reaction followed by annealing treatment. Impressively, the NiCo2O4 nanosheets exhibit rapid detect...NiCo2O4 nanosheets with sheaf-like nanostructure morphologies have been synthesized by a facile one-step hydrothermal reaction followed by annealing treatment. Impressively, the NiCo2O4 nanosheets exhibit rapid detection of eugenol. The linear range of detection is from 1-500μM, and the limit of detection is 5.4 μM. The NiCo2O4 modified electrode demonstrated high sensitivity, good repeatability and reproducibility, and long-term stability （7% decrease in response over 30 days）. Based on this work, an electrochemical reaction mechanism for eugenol oxidation was proposed, and in addition, the NiCo2O4 modified electrode was successfully employed for the analysis of eugenol in medicative balm samples. Recovery values for eugenol in medicative balm samples were in the range 98.7%-105.5%.展开更多
Single crystalline Bi2O3 nanosheets have been synthesized by the surfactant assisted solvothermal method, using oleic acid and sodium dodecyl benzene sulfonate （SDBS） as compound surfactants. The thickness of Bi2O3 ...Single crystalline Bi2O3 nanosheets have been synthesized by the surfactant assisted solvothermal method, using oleic acid and sodium dodecyl benzene sulfonate （SDBS） as compound surfactants. The thickness of Bi2O3 nanosheets is 40--70 nm with a monoclinic crystal structure. High-resolution transmission electron microscopy observation reveals that （ 345 ） lattice plane of the single crystal is parallel to the surface of the nanosheets. The cooperative effect of oleic acid encapsulated SDBS is the key to form single crystalline a-Bi2O3 nanosheets with a preferred growth orientation. An obvious blue shift of the single crystalline Bi2O3 nanosheets with a preferred surface （ 34-5 ） is observed due to quantum confinement effects in thickness and optical anisotropy.展开更多
Efforts in a large number of transition metal-carbon systems are devoted to the development of efficient catalysts for oxygen reduction reaction(ORR).However,unsatisfied O_(2)adsorption and slow reduction of OH*at the...Efforts in a large number of transition metal-carbon systems are devoted to the development of efficient catalysts for oxygen reduction reaction(ORR).However,unsatisfied O_(2)adsorption and slow reduction of OH*at the active centers hinder the further development of these catalysts.We here report a gasifiable reductant strategy,of which a new Cu-based metal organic framework(MOF:termed NTU-83)nanosheet was co-pyrolyzed with melamine to produce the N-coordinated atomic Cu and multi-oxidated Cu_(2+1)O active centers on the carbon foam with ultrathin skeleton.The engineered electrons and configuration of the active centers boost the catalyst(Cu/NC-1000)to show superior ORR activity(E_(1/2)=0.85 V),excellent stability,and methanol resistance.Further modeling calculation and controlled experiments reveal that the Cu_(2+1)O species play a crucial role in kinetically accelerated adsorption and activation of O_(2),while the N_(4)coordinated atomic Cu facilitates fast reduction of OH*.Such characteristics endow the Zn-air battery that containing Cu/NC-1000 as air cathode to show a high peak power density(138 mW·cm^(−2)),a high specific capacity of 763 mAh·gZn^(−1),and outstanding long-term cycle stability.The plausible mechanism and excellent performance show that gasifiable reductant strategy opens up a new route for regulation of the electronic of active sites but also provides a candidate for the practical application in energy conversion/storage devices.展开更多
基金DST,India for financial grant(SB/S1/PC-011/2013)DAE(India)for financial grant 2013/37P/73/BRNS,NTH-School‘‘Contacts in Nanosystems:Interactions,Control and Quantum Dynamics’’+1 种基金the Braunschweig International Graduate School of Metrology(IGSM)DFG-RTG 1952/1,Metrology for Complex Nanosystems
文摘Bismuth containing nanomaterials recently received increasing attention with respect to environmental applications because of their low cost, high stability and nontoxicity. In this work, Bi–Bi_2O_2CO_3 heterojunctions were fabricated by in-situ decoration of Bi nanoparticles on Bi_2O_2CO_3 nanosheets via a simple hydrothermal synthesis approach. X-ray diffraction(XRD), scanning electron microscopy(SEM), transmission electron microscopy(TEM) and high-resolution TEM(HRTEM) were used to confirm the morphology of the nanosheet-like heterostructure of the Bi–Bi_2O_2CO_3 composite. Detailed ultrafast electronic spectroscopy reveals that the in-situ decoration of Bi nanoparticles on Bi_2O_2CO_3 nanosheets exhibit a dramatically enhanced electron-hole pair separation rate, which results in an extraordinarily high photocatalytic activity for the degradation of a model organic dye, methylene blue(MB) under visible light illumination. Cycling experiments revealed a good photochemical stability of the Bi–Bi_2O_2CO_3 heterojunction under repeated irradiation. Photocurrent measurements further indicated that the heterojunction incredibly enhanced the charge generation and suppressed the charge recombination of photogenerated electron-hole pairs.
基金supported by the funding from the National Natural Science Foundation of China(grant nos.51902187,52072224,and 51732007)the Natural Science Foundation of Shandong Province(ZR2018BEM010)+3 种基金the Science Fund for Distinguished Young Scholars of Shandong Province(ZR2019JQ16)the Fundamental Research Funds of Shandong UniversityYoung Elite Scientist Sponsorship Program by CAST(YESS)the support from Collaborative Innovation Center of Technology and Equipment for Biological Diagnosis and Therapy in Universities of Shandong
文摘Driven by safety issues,environmental concerns,and high costs,rechargeable aqueous zinc-ion batteries(ZIBs)have received increasing attention in recent years owing to their unique advantages.However,the sluggish kinetics of divalent charge Zn^(2+)in the cathode materials caused by the strong electrostatic interaction and their unsatisfactory cycle life hinder the development of ZIBs.Herein,organic cations and Zn^(2+)ions co-pre-inserted vanadium oxide([N(CH_(3))_(4)]_(0.77),Zn_(0.23))V_(8)O_(20)·3.8H_(2)O are reported as the cathode for ultra-stable aqueous ZIBs,in which the weaker electrostatic interactions between Zn^(2+)and organic ion-pinned vanadium oxide can induce the high reversibility of Zn^(2+)insertion and extraction,thereby improving the cycle life.It is demonstrated that([N(CH_(3))_(4)]_(0.77),Zn_(0.23))V_(8)O_(20)·3.8H_(2)O cathodes deliver a discharge capacity of 181 mA h g^(-1)at8 A g^(-1)and ultra-long life span(99.5%capacity retention after 2000 cycles).A reversible Zn^(2+)/H^(+)ions(de)intercalation storage process and pseudocapacitive charge storage are characterized.The weaker interactions between organic ion and Zn^(2+)open a novel avenue for the design of highly reversible cathode materials with long-term cycling stability.
基金This work was supported by the National Natu-ral Science Foundation of China （No.21571166 and No.51271173） and the National Basic Research Pro- gram of China （No.2012CB922001）.
文摘Low-dimensional Bi2Fe4O9 nanosheets and microrods have been selectively prepared by a solvothermal method, from which the growth of the Bi2Fe4O9 crystals can be controlled by the variation of reaction conditions. Structure determination showed that the nanosheets are mainly exposed by {001} facets while the microrods are exposed by {110} facets. Ab- sorption spectra revealed that there are two bandgaps observed for both nanosheets （at 1.9 and 1.55 eV） and microrods （1.7 and 1.45 eV）, and they both would be available for the sunlight photocatalysis e ciently due to the intensive absorption ability in a wide region. Photocatalytic investigation demonstrated that the overall photocatalytic performance of the microrods is prior to that of the nanosheets due to the variation of bandgaps and exposed facets. The present report provides a useful alternative strategy for the controlling growth of nanostructures and/or microcrystals besides the present demonstration of the Bi2Fe4O9 crystals with diflerent bandgaps and facets that would be able to tune the corresponding photocatalytic ability selectively.
基金supported by the National Natural Science Foundation of China(No.52272125)the Fundamental Research Funds for the Central Universities(No.YX1199912371401-009)+2 种基金the Youth Science and Technology Innovation Research Team Project of Sichuan Province(No.2024NSFTD0016)the Science and Technology Program of Guizhou Province(No.[2023]414)the Research Project of China Three Gorges Co.(No.NBZZ202400321).
文摘Gaseous nitrogen is abundant in the atmosphere,and its efficient conversion to ammonia is vital to the future of a greener and more sustainable world.Since the N≡N covalent triple bond is difficult to break,the adsorption and activation of N_(2)molecules on the photocatalyst surface are critical to improve the efficiency of photocatalytic nitrogen fixation.In this work,Nb_(2)O_(5)·nH_(2)O nanosheets were synthesized by a hydrothermal reduction process with a weak reducing agent of glyoxal,which created more oxygen vacancies on their surfaces.Furthermore,their surface acidity was modulated by subsequent heat treatment in an Ar atmosphere.Thus,the effects of the oxygen vacancy and surface acidity on the photocatalytic nitrogen fixation performance of these Nb_(2)O_(5)·nH_(2)O nanosheets could be investigated.It was found that both factors contributed to the adsorption/activation of N_(2)and the charge carrier separation/transfer in these Nb_(2)O_(5)·nH_(2)O nanosheets.Owing to their synergistic effect,a high ammonia yield of 173.7μmol/(g·h)was achieved by these Nb_(2)O_(5)·nH_(2)O nanosheets through photocatalysis in pure water under simulated solar illumination without assistance from either sacrificial agents or cocatalysts.
基金supported by Beijing Natural Science Foundation(2182094)the National Natural Science Foundation of China(51772300 and 51832008)the Youth Innovation Promotion Association of CAS(2018039)。
文摘High-efficiency photocatalysts are of great importance to satisfy the requirements of green chemistry nowadays.Here we reported a novel solar-driven photocatalyst fabricated by a facile surface modification method,with the two-dimensional carboxylated zinc phthalocyanine-carboxylated C60-titanium dioxide(Zn Pc-C3-Ti O2)nanosheets,in which the surface modifications of Zn Pc and C60derivative were designed to extend the absorption range and promote charge separation,respectively.Benefiting from the unique structure and positive synergetic effect,the Zn Pc-C3-Ti O2 nanocomposite shows promising applications in selective reduction of nitroarenes for high-value-added aromatic amines under solar light.Especially,for the photocatalytic reduction of nitrobenzene to aniline,the Zn Pc-C3-Ti O2 nanocomposite possesses both high efficiency and selectivity(up to 99%).
基金supported by the National Natural Science Foundation of China(21774076,61774102 and 51573091)the National Key Research and Development Program of China(2017YFE0195800)+2 种基金the Program of the Shanghai Committee of Science and Technology(17JC1403200)the Program of Shanghai Academic Research Leader(19XD1421700)the Program of Distinguished Professor of Special Appointment at Shanghai Institutions of Higher Learning。
文摘The development of transition metal oxidebased electrode materials with proper controlled structures is highly desirable for high-performance supercapacitors.However,it remains a major challenge.Here,we present the first synthesis of bowl-like Ni Co2O4nanosheet clusters through a simple soft template guided hydrothermal strategy.The resulting bowl-like clusters consist of numerous Ni Co2O4nanosheets with an average thickness of 19 nm and possess a mean diameter of 1μm along with a specific surface area of40 m2g^-1.Remarkably,serving as an electrode material in a three-electrode system,the bowl-like Ni Co2O4nanosheet clusters exhibit a high specific capacity of 1068 F g^-1at a current density of 1 A g^-1and excellent cycling stability with90%capacitance retention after 5000 charge-discharge cycles.Meanwhile,an asymmetric supercapacitor(ASC)assembled with the Ni Co2O4clusters and activated carbon(AC)as the two electrodes exhibits a high specific capacitance of 129 F g^-1at 1 A g^-1,along with a high energy density of 33 W h kg^-1at a power density of 0.66 k W kg^-1.Such performance is superior to those of many commercial supercapacitors.This study opens a new avenue for the construction of ordered complex particles with controlled architectures for energy storage and conversion applications.
文摘NiCo2O4 nanosheets with sheaf-like nanostructure morphologies have been synthesized by a facile one-step hydrothermal reaction followed by annealing treatment. Impressively, the NiCo2O4 nanosheets exhibit rapid detection of eugenol. The linear range of detection is from 1-500μM, and the limit of detection is 5.4 μM. The NiCo2O4 modified electrode demonstrated high sensitivity, good repeatability and reproducibility, and long-term stability （7% decrease in response over 30 days）. Based on this work, an electrochemical reaction mechanism for eugenol oxidation was proposed, and in addition, the NiCo2O4 modified electrode was successfully employed for the analysis of eugenol in medicative balm samples. Recovery values for eugenol in medicative balm samples were in the range 98.7%-105.5%.
基金supported by the National Natural Science Foundation of China (Grant Nos.50431030 and 50871054)the Outstanding Scholar Supporting Program of NUST
文摘Single crystalline Bi2O3 nanosheets have been synthesized by the surfactant assisted solvothermal method, using oleic acid and sodium dodecyl benzene sulfonate （SDBS） as compound surfactants. The thickness of Bi2O3 nanosheets is 40--70 nm with a monoclinic crystal structure. High-resolution transmission electron microscopy observation reveals that （ 345 ） lattice plane of the single crystal is parallel to the surface of the nanosheets. The cooperative effect of oleic acid encapsulated SDBS is the key to form single crystalline a-Bi2O3 nanosheets with a preferred growth orientation. An obvious blue shift of the single crystalline Bi2O3 nanosheets with a preferred surface （ 34-5 ） is observed due to quantum confinement effects in thickness and optical anisotropy.
基金support from the National Natural Science Foundation of China(No.22171135)the Young and Middle-aged Academic Leader of Jiangsu Provincial Blue Project,the State Key Laboratory of Materials-Oriented Chemical Engineering(No.ZK201803)the Top-notch Academic Programs Project of Jiangsu Higher Education Institutions(TAPP).
文摘Efforts in a large number of transition metal-carbon systems are devoted to the development of efficient catalysts for oxygen reduction reaction(ORR).However,unsatisfied O_(2)adsorption and slow reduction of OH*at the active centers hinder the further development of these catalysts.We here report a gasifiable reductant strategy,of which a new Cu-based metal organic framework(MOF:termed NTU-83)nanosheet was co-pyrolyzed with melamine to produce the N-coordinated atomic Cu and multi-oxidated Cu_(2+1)O active centers on the carbon foam with ultrathin skeleton.The engineered electrons and configuration of the active centers boost the catalyst(Cu/NC-1000)to show superior ORR activity(E_(1/2)=0.85 V),excellent stability,and methanol resistance.Further modeling calculation and controlled experiments reveal that the Cu_(2+1)O species play a crucial role in kinetically accelerated adsorption and activation of O_(2),while the N_(4)coordinated atomic Cu facilitates fast reduction of OH*.Such characteristics endow the Zn-air battery that containing Cu/NC-1000 as air cathode to show a high peak power density(138 mW·cm^(−2)),a high specific capacity of 763 mAh·gZn^(−1),and outstanding long-term cycle stability.The plausible mechanism and excellent performance show that gasifiable reductant strategy opens up a new route for regulation of the electronic of active sites but also provides a candidate for the practical application in energy conversion/storage devices.
