Redox flow batteries have received wide attention for electrochemical energy conversion and storage devices due to their specific advantage of uncoupled power and energy devices,and therefore potentially to reduce the...Redox flow batteries have received wide attention for electrochemical energy conversion and storage devices due to their specific advantage of uncoupled power and energy devices,and therefore potentially to reduce the capital costs of energy storage.Terrific structural features of polyoxometalates exhibit unique advantages in redox flow batteries,such as,stable chemical properties,multi-electron reaction,good redox reversibility,low permeability,etc,which furnishes a novel perspective for settling various problems of redox flow batteries.This was a comprehensive and critical review of this type of batteries,focusing mainly on the chemistry of polyoxometalate electrolyte materials and introducing a systematic classification.Finally,challenges and perspectives of polyoxometalate electrolyte materials and polyoxometalate redox flow batteries are discussed.展开更多
Enhancing the stability of Pt-based electrocatalysts for the sluggish cathodic oxygen reduction reaction(ORR)is critical for proton exchange membrane fuel cells(PEMFCs).Herein,high-entropy intermetallic(HEI)L1_(2)-Pt(...Enhancing the stability of Pt-based electrocatalysts for the sluggish cathodic oxygen reduction reaction(ORR)is critical for proton exchange membrane fuel cells(PEMFCs).Herein,high-entropy intermetallic(HEI)L1_(2)-Pt(FeCoNiCuZn)3is designed for durable ORR catalysis.Benefiting from the unique HEI structure and the enhanced intermetallic phase stability,Pt(FeCoNiCuZn)3/C nanoparticles demonstrate significantly improved stability over Pt/C and PtCu_(3)/C catalysts.The Pt(FeCoNiCuZn)3/C exhibits a negligible decay of the half-wave potential during 30,000 potential cycles from 0.6 to 1.0 V,whereas Pt/C and PtCu_(3)/C are negatively shifted by 46 and 36 m V,respectively.Even after 10,000 cycles at potential up to 1.5 V,the mass activity of Pt(FeCoNiCuZn)3/C still shows~70%retention.As evidenced by the structural characterizations,the HEI structure of Pt(FeCoNiCuZn)3/C is well maintained,while PtCu_(3)/C nanoparticles undergo severe Cu leaching and particle growth.In addition,when assembled Pt(FeCoNiCuZn)3/C as the cathode in high-temperature PEMFC of 160℃,the H_(2)-O_(2)fuel cell delivers almost no degradation even after operating for 150 h,demonstrating the potential for fuel cell applications.This work provides a facile design strategy for the development of high-performance ultrastable electrocatalysts.展开更多
Potassium-ion batteries(KIBs)are a potential candidate to lithium-ion batteries(LIBs)but possess unsatisfactory capacity and rate properties.Herein,the metallic cobalt selenide quantum dots(Co0.85Se-QDs)encapsulated i...Potassium-ion batteries(KIBs)are a potential candidate to lithium-ion batteries(LIBs)but possess unsatisfactory capacity and rate properties.Herein,the metallic cobalt selenide quantum dots(Co0.85Se-QDs)encapsulated in mesoporous carbon matrix were designed via a direct hydrothermal method.Specifically,the cobalt selenide/carbon composite(Co0.85Se-QDs/C)possesses tertiary hierarchical structure,which is the primary quantum dots,the secondary petals flake,and the tertiary hollow micropolyhedron framework.Co0.85Se-QDs are homogenously embedded into the carbon petals flake,which constitute the hollow polyhedral framework.This unique structure can take the advantages of both nanoscale and microscale features:Co0.85Se-QDs can expand in a multidimensional and ductile carbon matrix and reduce the K-intercalation stress in particle dimensions;the micropetals can restrain the agglomeration of active materials and promote the transportation of potassium ion and electron.In addition,the hollow carbon framework buffers volume expansion,maintains the structural integrity,and increases the electronic conductivity.Benefiting from this tertiary hierarchical structure,outstanding K-storage performance(402 mAh g?1 after 100 cycles at 50 mA g?1)is obtained when Co0.85Se-QDs/C is used as KIBs anode.More importantly,the selenization process in this work is newly reported and can be generally extended to prepare other quantum dots encapsulated in edge-limited frameworks for excellent energy storage.展开更多
Light-weight and high-strength materials have attracted considerable attention owing to their outstanding properties, such as weight-reducing, acoustic absorption, thermal insulation, shock and vibration damping. Diam...Light-weight and high-strength materials have attracted considerable attention owing to their outstanding properties, such as weight-reducing, acoustic absorption, thermal insulation, shock and vibration damping. Diamond possesses specific stiffness and strength arising from its special crystal structure. In this work, inspired by the diamond crystal structure, hollow-tube nickel materials with the diamond structure were fabricated using a diamond structured polymer template based on the Stereo Lithography Appearance technology. The diamond structured template was coated with Ni-P by electroless plating. Finally, the template was removed by high temperature calcinations. The density of the hollow tube nickel materials is about 20 mg/cm3. The morphology and composition of the resultant materials were characterized by scanning electron microscope, energy-dispersive spectrometry, and X-ray diffraction. The results showed that the surface of the Ni film was uniform with the thickness of 4 μm.The mechanical property was also measured by stress and strain tester. The maximum compression stress can be reached to40.6 KPa.展开更多
As a novel class of metallic materials, bulk metallic glasses(BMGs) have attracted a great deal of attention owing to their technological promise for practical engineering applications. In nature, biological materials...As a novel class of metallic materials, bulk metallic glasses(BMGs) have attracted a great deal of attention owing to their technological promise for practical engineering applications. In nature, biological materials exhibit inherent multifunctional integration, which provides some inspiration for scientists and engineers to construct multifunctional artificial materials. In this contribution, inspired by superhydrophobic self-cleaning lotus leaves, multifunctional bulk metallic glasses(BMG) materials have been fabricated through the thermoplastic forming-based process followed by the SiO_2/soot deposition. To mimic the microscale papillae of the lotus leaf, the BMG micropillar with a hemispherical top was first fabricated using micro-patterned silicon templates based on thermoplastic forming. The deposited randomly distributed SiO_2/soot nanostructures covered on BMG micropillars are similar to the branch-like nanostructures on papillae of the lotus leaf. Micro-nanoscale hierarchical structures endow BMG replica with superhydrophobicity, a low adhesion towards water, and self-cleaning, similar to the natural lotus leaf. Furthermore, on the basis of the observation of the morphology of BMG replica in the Si mould, the formation mechanism of BMG replica was proposed in this work. The BMG materials with multifunction integration would extend their practical engineering applications and we expect this method could be widely adopted for the fabrication of other multifunctional BMG surfaces.展开更多
Direct liquid fuel cells(DLFCs)are proposed to address the problems of high cost and complex storage and transportation of hydrogen in traditional hydrogen-oxygen proton exchange membrane fuel cells.However,present fu...Direct liquid fuel cells(DLFCs)are proposed to address the problems of high cost and complex storage and transportation of hydrogen in traditional hydrogen-oxygen proton exchange membrane fuel cells.However,present fuels of organic small molecules used in DLFCs are restricted to problems of sluggish electrochemical kinetics and easily poisoning of precious metal catalysts.Herein,we demonstrate reduced phosphotungstic acid as a liquid fuel for DLFCs based on its advantages of high chemical and electrochemical stability,high electrochemical activity on common carbon material electrodes,and low permeability through proton exchange membranes.The application of phosphotungstic acid fuel effectively solves the problems of high cost of anode catalysts and serious fuel permeation loss in traditional DLFCs.A phosphotungstic acid fuel cell achieves a peak power density of466 mW cm^(-2)at a cell voltage of 0.42 V and good stability at current densities in the range from 20 to 200 mA cm^(-2).展开更多
Demand for efficient and continuous application for high-grid energy storage systems involves the study towards novel battery technologies. Hence, considering the vast naturally available resources of potassium all ov...Demand for efficient and continuous application for high-grid energy storage systems involves the study towards novel battery technologies. Hence, considering the vast naturally available resources of potassium all over the world and its encouraging intercalation chemistries, it has recently enticed attention in electrochemical energy storage industry in the form of potassium ion batteries (PIBs). The major factor in this K+ based battery, is to develop efficient approaches to manufacture electrode substance to intercalate its big size potassium ions with considerable voltage, kinetics, charge/discharge capacity, capacity retention, cost, etc. This study contributes in the recent developments of anode and cathode materials for PIBs, including several electrode materials in regards to synthesis, structure, electrochemical performance, and K-storage mechanisms. Finally, the review contributes to provide helpful sources for the increasing number of scientists working in this industry regarding its critical issues and challenges and also to indicate the future direction of electrode materials in PIBs.展开更多
Remediation of wastewater containing dye molecules is necessary to alleviate the significant threat that poses to human health and the environment.Current treatment technologies are seriously limited by their low effi...Remediation of wastewater containing dye molecules is necessary to alleviate the significant threat that poses to human health and the environment.Current treatment technologies are seriously limited by their low efficiency for removing small dye molecules or/and inferior regenerability.Herein,we report a bio-inspired,solar-driven,regenerable separation device capable of separating small dye molecules from the wastewater with high efficiency.The device is composed of porous super-hydrophilic ceramic and carbon nanotubes(CNTs).In comparison with previously reported systems,the resultant device not only achieved a highly promising separation efficiency of>99%for dye-containing wastewater,even for small dye molecules(<1.25 nm),but also demonstrated excellent separation stability and strong resistance to acid/alkali.Moreover,the device demonstrated impressive regenerability on simple calcination and re-coating of the CNT layer after it was blocked.This novel separation device shows potential for application in many fields,such as dye separation,wastewater purification and desalination.展开更多
High-temperature proton-exchange membrane fuel cells(HT-PEMFCs)have shown a broad prospect of applications due to the enhanced reaction kinetics and simplified supporting system.However,the proton conductor,phosphoric...High-temperature proton-exchange membrane fuel cells(HT-PEMFCs)have shown a broad prospect of applications due to the enhanced reaction kinetics and simplified supporting system.However,the proton conductor,phosphoric acid,tends to poison the active sites of Pt,resulting in high Pt consumption.Herein,Pt nanoparticles anchored on SiO_(2)-modified carbon nanotubes(CNT@SiO_(2)-Pt)are prepared as high-performance cathode catalysts for HT-PEMFCs.The SiO_(2)in CNT@SiO_(2)-Pt can induce the adsorption of phosphoric acid transferring from Pt active sites in the catalytic layer,avoiding the poisoning of the Pt,and the phosphate fixed by SiO_(2)provide a high-speed proton conduction highway for oxygen reduction reactions.Accordingly,The CNT@SiO_(2)-Pt cathode achieve superior power density of 765 mW cm^(−2)(160℃)and 1,061 mW cm^(−2)(220℃)due to the rapid proton-coupled electron process and outstanding stability in HT-PEMFCs.This result provides a new road to resolve the phosphate poisoning for the commercialization of HT-PEMFCs.展开更多
基金supported by the National Natural Science Foundation of China(No.22178012,21722601)China Postdoctoral Science Foundation(No.2019M660389).
文摘Redox flow batteries have received wide attention for electrochemical energy conversion and storage devices due to their specific advantage of uncoupled power and energy devices,and therefore potentially to reduce the capital costs of energy storage.Terrific structural features of polyoxometalates exhibit unique advantages in redox flow batteries,such as,stable chemical properties,multi-electron reaction,good redox reversibility,low permeability,etc,which furnishes a novel perspective for settling various problems of redox flow batteries.This was a comprehensive and critical review of this type of batteries,focusing mainly on the chemistry of polyoxometalate electrolyte materials and introducing a systematic classification.Finally,challenges and perspectives of polyoxometalate electrolyte materials and polyoxometalate redox flow batteries are discussed.
基金supported by the National Natural Science Foundation(22279036)the Innovation and Talent Recruitment Base of New Energy Chemistry and Device(B21003)。
文摘Enhancing the stability of Pt-based electrocatalysts for the sluggish cathodic oxygen reduction reaction(ORR)is critical for proton exchange membrane fuel cells(PEMFCs).Herein,high-entropy intermetallic(HEI)L1_(2)-Pt(FeCoNiCuZn)3is designed for durable ORR catalysis.Benefiting from the unique HEI structure and the enhanced intermetallic phase stability,Pt(FeCoNiCuZn)3/C nanoparticles demonstrate significantly improved stability over Pt/C and PtCu_(3)/C catalysts.The Pt(FeCoNiCuZn)3/C exhibits a negligible decay of the half-wave potential during 30,000 potential cycles from 0.6 to 1.0 V,whereas Pt/C and PtCu_(3)/C are negatively shifted by 46 and 36 m V,respectively.Even after 10,000 cycles at potential up to 1.5 V,the mass activity of Pt(FeCoNiCuZn)3/C still shows~70%retention.As evidenced by the structural characterizations,the HEI structure of Pt(FeCoNiCuZn)3/C is well maintained,while PtCu_(3)/C nanoparticles undergo severe Cu leaching and particle growth.In addition,when assembled Pt(FeCoNiCuZn)3/C as the cathode in high-temperature PEMFC of 160℃,the H_(2)-O_(2)fuel cell delivers almost no degradation even after operating for 150 h,demonstrating the potential for fuel cell applications.This work provides a facile design strategy for the development of high-performance ultrastable electrocatalysts.
基金financially supported by Beijing Natural Science Foundation(No.2192034)China Postdoctoral Science Foundation(No.2018M631335)National Key R&D Program of China(No.2018YFB0905600).
文摘Potassium-ion batteries(KIBs)are a potential candidate to lithium-ion batteries(LIBs)but possess unsatisfactory capacity and rate properties.Herein,the metallic cobalt selenide quantum dots(Co0.85Se-QDs)encapsulated in mesoporous carbon matrix were designed via a direct hydrothermal method.Specifically,the cobalt selenide/carbon composite(Co0.85Se-QDs/C)possesses tertiary hierarchical structure,which is the primary quantum dots,the secondary petals flake,and the tertiary hollow micropolyhedron framework.Co0.85Se-QDs are homogenously embedded into the carbon petals flake,which constitute the hollow polyhedral framework.This unique structure can take the advantages of both nanoscale and microscale features:Co0.85Se-QDs can expand in a multidimensional and ductile carbon matrix and reduce the K-intercalation stress in particle dimensions;the micropetals can restrain the agglomeration of active materials and promote the transportation of potassium ion and electron.In addition,the hollow carbon framework buffers volume expansion,maintains the structural integrity,and increases the electronic conductivity.Benefiting from this tertiary hierarchical structure,outstanding K-storage performance(402 mAh g?1 after 100 cycles at 50 mA g?1)is obtained when Co0.85Se-QDs/C is used as KIBs anode.More importantly,the selenization process in this work is newly reported and can be generally extended to prepare other quantum dots encapsulated in edge-limited frameworks for excellent energy storage.
基金support of the National Basic Research Program of China(2010CB934700)the National Natural Science Foundation of China(51372010)
文摘Light-weight and high-strength materials have attracted considerable attention owing to their outstanding properties, such as weight-reducing, acoustic absorption, thermal insulation, shock and vibration damping. Diamond possesses specific stiffness and strength arising from its special crystal structure. In this work, inspired by the diamond crystal structure, hollow-tube nickel materials with the diamond structure were fabricated using a diamond structured polymer template based on the Stereo Lithography Appearance technology. The diamond structured template was coated with Ni-P by electroless plating. Finally, the template was removed by high temperature calcinations. The density of the hollow tube nickel materials is about 20 mg/cm3. The morphology and composition of the resultant materials were characterized by scanning electron microscope, energy-dispersive spectrometry, and X-ray diffraction. The results showed that the surface of the Ni film was uniform with the thickness of 4 μm.The mechanical property was also measured by stress and strain tester. The maximum compression stress can be reached to40.6 KPa.
基金the National Natural Science Foundation of China (21273016, 51271195)the National Basic Research Program of China (2013CB933003, 2015CB856800)+1 种基金the Program for New Century Excellent Talents in University, Beijing Higher Education Young Elite Teacher Project, the Fundamental Research Funds for the Central Universities, 111 project (B14009)the Key Research Program of the Chinese Academy of Sciences (KJZDEW-M01, M03)
文摘As a novel class of metallic materials, bulk metallic glasses(BMGs) have attracted a great deal of attention owing to their technological promise for practical engineering applications. In nature, biological materials exhibit inherent multifunctional integration, which provides some inspiration for scientists and engineers to construct multifunctional artificial materials. In this contribution, inspired by superhydrophobic self-cleaning lotus leaves, multifunctional bulk metallic glasses(BMG) materials have been fabricated through the thermoplastic forming-based process followed by the SiO_2/soot deposition. To mimic the microscale papillae of the lotus leaf, the BMG micropillar with a hemispherical top was first fabricated using micro-patterned silicon templates based on thermoplastic forming. The deposited randomly distributed SiO_2/soot nanostructures covered on BMG micropillars are similar to the branch-like nanostructures on papillae of the lotus leaf. Micro-nanoscale hierarchical structures endow BMG replica with superhydrophobicity, a low adhesion towards water, and self-cleaning, similar to the natural lotus leaf. Furthermore, on the basis of the observation of the morphology of BMG replica in the Si mould, the formation mechanism of BMG replica was proposed in this work. The BMG materials with multifunction integration would extend their practical engineering applications and we expect this method could be widely adopted for the fabrication of other multifunctional BMG surfaces.
基金financialy supported by the National Key R&D Program of China(No.2018YFB1502303)the National Natural Science Foundation of China(No.21722601,U19A2017)China Postdoctoral Science Foundation(No.2019M660389)。
文摘Direct liquid fuel cells(DLFCs)are proposed to address the problems of high cost and complex storage and transportation of hydrogen in traditional hydrogen-oxygen proton exchange membrane fuel cells.However,present fuels of organic small molecules used in DLFCs are restricted to problems of sluggish electrochemical kinetics and easily poisoning of precious metal catalysts.Herein,we demonstrate reduced phosphotungstic acid as a liquid fuel for DLFCs based on its advantages of high chemical and electrochemical stability,high electrochemical activity on common carbon material electrodes,and low permeability through proton exchange membranes.The application of phosphotungstic acid fuel effectively solves the problems of high cost of anode catalysts and serious fuel permeation loss in traditional DLFCs.A phosphotungstic acid fuel cell achieves a peak power density of466 mW cm^(-2)at a cell voltage of 0.42 V and good stability at current densities in the range from 20 to 200 mA cm^(-2).
基金The authors express their thanks to the research starting foundation from Shaanxi University of Science and Technology(Grant No.2018GBJ-04).
文摘Demand for efficient and continuous application for high-grid energy storage systems involves the study towards novel battery technologies. Hence, considering the vast naturally available resources of potassium all over the world and its encouraging intercalation chemistries, it has recently enticed attention in electrochemical energy storage industry in the form of potassium ion batteries (PIBs). The major factor in this K+ based battery, is to develop efficient approaches to manufacture electrode substance to intercalate its big size potassium ions with considerable voltage, kinetics, charge/discharge capacity, capacity retention, cost, etc. This study contributes in the recent developments of anode and cathode materials for PIBs, including several electrode materials in regards to synthesis, structure, electrochemical performance, and K-storage mechanisms. Finally, the review contributes to provide helpful sources for the increasing number of scientists working in this industry regarding its critical issues and challenges and also to indicate the future direction of electrode materials in PIBs.
基金supported by the National Natural Science Foundation of China(21103006)the Beijing Natural Science Foundation(2132030)+2 种基金the National High Technology Research and Development Program of China(2012AA030305)the Fundamental Research Funds for the Central Universities(YWF-10-01-B16,YWF-11-03-Q-214,YWF-13-DX-XYJL-004)the 111 Project(B14009)
基金Supported by the National Natural Science Foundation of China(Nos.91333120, 21271016) and the National Basic Research Program of China(No.2012CB720904).
基金supported by the National Natural Science Foundation of China(Grant Nos.21875011,51922018,51673010)the National Key Research and Development Program of China(Grant No.2017YFA0206904).
文摘Remediation of wastewater containing dye molecules is necessary to alleviate the significant threat that poses to human health and the environment.Current treatment technologies are seriously limited by their low efficiency for removing small dye molecules or/and inferior regenerability.Herein,we report a bio-inspired,solar-driven,regenerable separation device capable of separating small dye molecules from the wastewater with high efficiency.The device is composed of porous super-hydrophilic ceramic and carbon nanotubes(CNTs).In comparison with previously reported systems,the resultant device not only achieved a highly promising separation efficiency of>99%for dye-containing wastewater,even for small dye molecules(<1.25 nm),but also demonstrated excellent separation stability and strong resistance to acid/alkali.Moreover,the device demonstrated impressive regenerability on simple calcination and re-coating of the CNT layer after it was blocked.This novel separation device shows potential for application in many fields,such as dye separation,wastewater purification and desalination.
基金supported by National Key R&D Program of China(2020YFA0710000)the National Natural Science Foundation of China(21902047,21825201,U19A2017)+1 种基金the Provincial Natural Science Foundation of Hunan(2016TP1009 and 2020JJ5045)Hunan Graduate Education Innovation Project and Professional Ability Improvement Project(CX20200445)。
文摘High-temperature proton-exchange membrane fuel cells(HT-PEMFCs)have shown a broad prospect of applications due to the enhanced reaction kinetics and simplified supporting system.However,the proton conductor,phosphoric acid,tends to poison the active sites of Pt,resulting in high Pt consumption.Herein,Pt nanoparticles anchored on SiO_(2)-modified carbon nanotubes(CNT@SiO_(2)-Pt)are prepared as high-performance cathode catalysts for HT-PEMFCs.The SiO_(2)in CNT@SiO_(2)-Pt can induce the adsorption of phosphoric acid transferring from Pt active sites in the catalytic layer,avoiding the poisoning of the Pt,and the phosphate fixed by SiO_(2)provide a high-speed proton conduction highway for oxygen reduction reactions.Accordingly,The CNT@SiO_(2)-Pt cathode achieve superior power density of 765 mW cm^(−2)(160℃)and 1,061 mW cm^(−2)(220℃)due to the rapid proton-coupled electron process and outstanding stability in HT-PEMFCs.This result provides a new road to resolve the phosphate poisoning for the commercialization of HT-PEMFCs.
基金This work was supported by National Natural Science Foundation of China (Nos. 21571011, 21641006), National Basic Research Program of China (No. 2014CB931803), Fundamental Research Funds for the Central Universities (N0s. YWF-15-HHXY-019, YWF-16- JCTD-B-03) and China Postdoctoral Science Foundation Grant (No. 2015M580035).