Lithium(Li)metal is a potential anode for high-energy-density batteries because of its low potential and ultrahigh capacity.Nevertheless,the Li dendrites formation,the ununiform Li deposition,and the growth of Li dend...Lithium(Li)metal is a potential anode for high-energy-density batteries because of its low potential and ultrahigh capacity.Nevertheless,the Li dendrites formation,the ununiform Li deposition,and the growth of Li dendrites hamper its application,especially under high deposition capacity/high rate.Here,a spatially controlled Li deposition mode with array-oriented morphology is achieved based on the novel mixed ion/electron-conducting Li_(x)Cu_(y)P_(z) arrays constructed on Cu foil,which can be facile fabricated via an in-situ transformation of metal phosphide.Theoretic calculations indicate the excellent lithiophilicity and low Li diffusion barrier of the arrays,especially for the Li_(2)CuP phase,which are conducive to ho-mogenizing the Li nucleation/deposition of Li.Moreover,such mixed conducting arrays promote fast Li+diffusion via the continuous Li+pathways as well as modulate the Li+flux/electric field.Furthermore,the arrays with enlarged specific surface area and open spaces reduce the local current density and alle-viate the volume fluctuation of Li.Consequently,a dendrite-free Li anode is obtained under a high rate(20 mA cm^(–2))or a high deposition capacity(10 mAh cm^(–2)).In addition,even if the negative/positive ratio reduces to only 1.1,the full cells still perform outstanding stability for over 200 cycles.This work empha-sizes the importance of the design of the framework in terms of the intrinsic properties and structure and reveals a pathway for developing Li metal batteries.展开更多
Catalytic carbon dioxide(CO_(2))desorption has emerged as a promising approach to enhance the efficiency of CO_(2)capture while minimizing energy demands,crucial for advancing chemical absorption methods.This study in...Catalytic carbon dioxide(CO_(2))desorption has emerged as a promising approach to enhance the efficiency of CO_(2)capture while minimizing energy demands,crucial for advancing chemical absorption methods.This study investigates the catalytic potential of three metal phosphates(aluminium phosphate(AlPO4),cobaltous phosphate(Co_(3)(PO_(4))_(2)),and zinc phosphate(Zn_(3)(PO_(4))_(2)))in improving the MEA(monoethanolamine)-based CO_(2)absorption-desorption performance.Among the catalysts tested,AlPO_(4)demonstrated superior performance,enhancing CO_(2)absorption capacity by 4.2%to 9.3%and desorption capacity by 12.3%to 22.7%across five cycles.Notably,AlPO_(4)increased the CO_(2)desorption rate by over 104.4%at a desorption temperature of 81.3℃,simultaneously reducing the required sensible heat by 12.3%to 22.7%,compared to processes without catalysts.The improved efficiency is attributed to AlPO_(4)'s ability to effectively transfer hydrogen protons from protonated MEA to carbamate,thereby facilitating the decomposition of carbamate and regenerating CO_(2).This research introduces a viable,cost-effective,and eco-friendly solid acid catalyst strategy for CO_(2)desorption,contributing to the development of more energy-efficient CO_(2)capture technologies.展开更多
Considering a series of electromagnetic pollution problems brought by the development of electronic communication technology,more attention has been paid to the research of electromagnetic wave(EMW)absorbing materials...Considering a series of electromagnetic pollution problems brought by the development of electronic communication technology,more attention has been paid to the research of electromagnetic wave(EMW)absorbing materials with unique composition and structure.Herein,under the inspiration of mixeddimensional hierarchical structure,2D Ni_(2)P nanosheets anchored on 1D silk-derived carbon fiber is successfully fabricated as a gratifying resistor-dielectric type absorber.By a controllable pyrolyzation strategy and disproportionated reaction,high-density 2D Ni_(2)P nanosheets were grown vertically and cross-linked on the surface of 1D silk-derived carbon fiber.The sample exhibited superior EMW absorption performance with maximum reflection loss value of–56.9 d B at the thickness of 2.32 mm and the effective absorption bandwidth can reach to 7.2 GHz at the thickness of 1.93 mm.In addition,the pure Ni_(2)P shows remarkable dielectric characteristic and EMW absorption ability as well.The integration of dualconductive loss,enhanced polarization relaxation loss and the multiple scattering in the composites was proved to contribute to the good EMW absorption performance.Therefore,this work confirms the great potentials of Ni_(2)P as a high-efficient EMW absorbing materials and light a new way in construction of multidimensional absorber.展开更多
Exploring materials with high electrochemical activity is of keen interest for electrochemistry-controlled optical and energy storage devices.However,it remains a great challenge for transition metal oxides to meet th...Exploring materials with high electrochemical activity is of keen interest for electrochemistry-controlled optical and energy storage devices.However,it remains a great challenge for transition metal oxides to meet this feature due to their low electron conductivity and insufficient reaction sites.Here,we propose a type of transition metal phosphate(NiHPO_(4)·3H_(2)O,NHP)by a facile and scalable electrodeposition method,which can achieve the capability of efficient ion accommodation and injection/extraction for electrochromic energy storage applications.Specifically,the NHP film with an ultra-high transmittance(approach to 100%)achieves a large optical modulation(90.8%at 500 nm),high coloration efficiency(75.4 cm^(2)C^(-1)at 500 nm),and a high specific capacity of 47.8 mAh g^(-1)at 0.4 A g^(-1).Furthermore,the transformation mechanism of NHP upon electrochemical reaction is systematically elucidated using in situ and ex situ techniques.Ultimately,a large-area electrochromic smart window with 100 cm^(2)is constructed based on the NHP electrode,displaying superior electrochromic energy storage performance in regulating natural light and storing electrical charges.Our findings may open up new strategies for developing advanced electrochromic energy storage materials and smart windows.展开更多
The construction of metal phosphate coating layers has been widely recognized as an effective strategy for protecting high-energy cathode materials in lithium-ion batteries(LIBs).However,due to the low solubility of m...The construction of metal phosphate coating layers has been widely recognized as an effective strategy for protecting high-energy cathode materials in lithium-ion batteries(LIBs).However,due to the low solubility of metal phosphates,their precipitation in aqueous solution becomes too fast to control,making it a significant challenge to ensure a heterogeneous growth process towards surface coatings.Herein,we report a solution-based synthetic process to achieve conformal metal phosphate coating through coordination-assisted precipitation,which involved the reaction between phytic acid(PA),urea,and metal ions,particularly Nb^(5+),in ethanol solution to achieve a well-tamed coating effect.The use of PA,a plant-derived compound known as inositol hexaphosphoric acid,was facile to form soluble phytate-metal complex,which precipitated with urea to form metal-phosphate-containing coatings with thickness controlled at high precision.This proposed synthetic protocol was applied for the surface coating of high-voltage cathode materials in the form of LiNi_(0.5)Mn_(1.5)O_(4)(LNMO),leading to significantly enhanced structural and electrochemical stability for its working at 5 V.Notably,after 300 cycles,the modified LNMO was able to achieve capacity retention of 85.1%for its working at 45℃ at a current density of 1 C as compared to only 29.9%of the pristine sample.Our findings highlight the potential of solution-based processes in building conformal coatings for the stabilization of high-energy cathode materials in their LIBs application.展开更多
The exploration of cost-effective non-noble-metal electrocatalysts is highly imperative to replace the state-of-the-art platinum-based catalysts for oxygen reduction reaction(ORR). Here, we prepared cobalt phosphonate...The exploration of cost-effective non-noble-metal electrocatalysts is highly imperative to replace the state-of-the-art platinum-based catalysts for oxygen reduction reaction(ORR). Here, we prepared cobalt phosphonate-derived N-doped cobalt phosphate/carbon nanotube hybrids(Co Pi C-N/CNTs) by hydrothermal treatment of N-containing cobalt phosphonate and oxidized carbon nanotubes(o-CNT) followed by high-temperature calcination under nitrogen atmosphere. The resultant Co Pi C-N/CNT exhibits a superior electrocatalytic performance for the ORR in alkaline media, which is equal to the commercial Pt/C catalyst in the aspect of half-wave potential, onset potential and diffuse limiting current density. Furthermore, the excellent tolerance to methanol and strong durability outperform those of commercial Pt/C. It is found that cobalt phosphonate-derived N-doped cobalt phosphate and the in-situ formed graphitic carbons play key roles on the activity enhancement. Besides, introducing a suitable amount of CNTs enhances the electronic conductivity and further contributes to the improved ORR performance.展开更多
The design and development of new advanced superwetting porous membranes with antioil-fouling performance are still rare and highly desirable because of their potential widespread applications.A metallic phosphate nan...The design and development of new advanced superwetting porous membranes with antioil-fouling performance are still rare and highly desirable because of their potential widespread applications.A metallic phosphate nanoflower-covered mesh membrane with superhydrophilic and unprecedented antioil-fouling properties is prepared by an exceptionally simple and effective in-situ solution corrosion method.As demonstrated,the outstanding antioil-fouling property of the resulting mesh membrane is connected with the special phosphate group and the three-dimensional(3 D) nanoflower structure.Owing to the antioil-fouling property,upon to water,the oil-fouled mesh membrane can keep the surface free of various kinds of oils,including viscous crude oil to light n-hexane.Thanks to its unprecedented self-cleaning property,the superhydrophilic mesh membrane can effectively separate different oil/water mixtures without prior wetted by water,exhibiting great potential for practical spilled oil remediation.展开更多
基金This work was supported by the National Science Foundation of Tianjin(No.20JCQNJC00500)。
文摘Lithium(Li)metal is a potential anode for high-energy-density batteries because of its low potential and ultrahigh capacity.Nevertheless,the Li dendrites formation,the ununiform Li deposition,and the growth of Li dendrites hamper its application,especially under high deposition capacity/high rate.Here,a spatially controlled Li deposition mode with array-oriented morphology is achieved based on the novel mixed ion/electron-conducting Li_(x)Cu_(y)P_(z) arrays constructed on Cu foil,which can be facile fabricated via an in-situ transformation of metal phosphide.Theoretic calculations indicate the excellent lithiophilicity and low Li diffusion barrier of the arrays,especially for the Li_(2)CuP phase,which are conducive to ho-mogenizing the Li nucleation/deposition of Li.Moreover,such mixed conducting arrays promote fast Li+diffusion via the continuous Li+pathways as well as modulate the Li+flux/electric field.Furthermore,the arrays with enlarged specific surface area and open spaces reduce the local current density and alle-viate the volume fluctuation of Li.Consequently,a dendrite-free Li anode is obtained under a high rate(20 mA cm^(–2))or a high deposition capacity(10 mAh cm^(–2)).In addition,even if the negative/positive ratio reduces to only 1.1,the full cells still perform outstanding stability for over 200 cycles.This work empha-sizes the importance of the design of the framework in terms of the intrinsic properties and structure and reveals a pathway for developing Li metal batteries.
基金supports from the China Postdoctoral Science Foundation(2023M743768)National Natural Science Foundation of China(52006112)Xuzhou Bureau of Science and Technology(KC23293).
文摘Catalytic carbon dioxide(CO_(2))desorption has emerged as a promising approach to enhance the efficiency of CO_(2)capture while minimizing energy demands,crucial for advancing chemical absorption methods.This study investigates the catalytic potential of three metal phosphates(aluminium phosphate(AlPO4),cobaltous phosphate(Co_(3)(PO_(4))_(2)),and zinc phosphate(Zn_(3)(PO_(4))_(2)))in improving the MEA(monoethanolamine)-based CO_(2)absorption-desorption performance.Among the catalysts tested,AlPO_(4)demonstrated superior performance,enhancing CO_(2)absorption capacity by 4.2%to 9.3%and desorption capacity by 12.3%to 22.7%across five cycles.Notably,AlPO_(4)increased the CO_(2)desorption rate by over 104.4%at a desorption temperature of 81.3℃,simultaneously reducing the required sensible heat by 12.3%to 22.7%,compared to processes without catalysts.The improved efficiency is attributed to AlPO_(4)'s ability to effectively transfer hydrogen protons from protonated MEA to carbamate,thereby facilitating the decomposition of carbamate and regenerating CO_(2).This research introduces a viable,cost-effective,and eco-friendly solid acid catalyst strategy for CO_(2)desorption,contributing to the development of more energy-efficient CO_(2)capture technologies.
基金financially supported by the National Natural Science Foundation of China(Nos.51971162,U1933112,51671146)the Program of Shanghai Technology Research Leader(No.18XD1423800)the Fundamental Research Funds for the Central Universities(No.22120180096)。
文摘Considering a series of electromagnetic pollution problems brought by the development of electronic communication technology,more attention has been paid to the research of electromagnetic wave(EMW)absorbing materials with unique composition and structure.Herein,under the inspiration of mixeddimensional hierarchical structure,2D Ni_(2)P nanosheets anchored on 1D silk-derived carbon fiber is successfully fabricated as a gratifying resistor-dielectric type absorber.By a controllable pyrolyzation strategy and disproportionated reaction,high-density 2D Ni_(2)P nanosheets were grown vertically and cross-linked on the surface of 1D silk-derived carbon fiber.The sample exhibited superior EMW absorption performance with maximum reflection loss value of–56.9 d B at the thickness of 2.32 mm and the effective absorption bandwidth can reach to 7.2 GHz at the thickness of 1.93 mm.In addition,the pure Ni_(2)P shows remarkable dielectric characteristic and EMW absorption ability as well.The integration of dualconductive loss,enhanced polarization relaxation loss and the multiple scattering in the composites was proved to contribute to the good EMW absorption performance.Therefore,this work confirms the great potentials of Ni_(2)P as a high-efficient EMW absorbing materials and light a new way in construction of multidimensional absorber.
基金financially the National Natural Science Foundation of China(U2004175,51902086 and 62222402)China Postdoctoral Science Foundation(2022M711036)the Key Scientific Research Project plan of the University in Henan Province(22A430002)。
文摘Exploring materials with high electrochemical activity is of keen interest for electrochemistry-controlled optical and energy storage devices.However,it remains a great challenge for transition metal oxides to meet this feature due to their low electron conductivity and insufficient reaction sites.Here,we propose a type of transition metal phosphate(NiHPO_(4)·3H_(2)O,NHP)by a facile and scalable electrodeposition method,which can achieve the capability of efficient ion accommodation and injection/extraction for electrochromic energy storage applications.Specifically,the NHP film with an ultra-high transmittance(approach to 100%)achieves a large optical modulation(90.8%at 500 nm),high coloration efficiency(75.4 cm^(2)C^(-1)at 500 nm),and a high specific capacity of 47.8 mAh g^(-1)at 0.4 A g^(-1).Furthermore,the transformation mechanism of NHP upon electrochemical reaction is systematically elucidated using in situ and ex situ techniques.Ultimately,a large-area electrochromic smart window with 100 cm^(2)is constructed based on the NHP electrode,displaying superior electrochromic energy storage performance in regulating natural light and storing electrical charges.Our findings may open up new strategies for developing advanced electrochromic energy storage materials and smart windows.
基金supported by the National Key R&D Program of China(No.2022YFB2404402)the National Natural Science Foundation of China(Nos.22025507,22421001,and 22409200)the Beijing National Laboratory for Molecular Sciences(No.BNLMS-CXXM-202010).
文摘The construction of metal phosphate coating layers has been widely recognized as an effective strategy for protecting high-energy cathode materials in lithium-ion batteries(LIBs).However,due to the low solubility of metal phosphates,their precipitation in aqueous solution becomes too fast to control,making it a significant challenge to ensure a heterogeneous growth process towards surface coatings.Herein,we report a solution-based synthetic process to achieve conformal metal phosphate coating through coordination-assisted precipitation,which involved the reaction between phytic acid(PA),urea,and metal ions,particularly Nb^(5+),in ethanol solution to achieve a well-tamed coating effect.The use of PA,a plant-derived compound known as inositol hexaphosphoric acid,was facile to form soluble phytate-metal complex,which precipitated with urea to form metal-phosphate-containing coatings with thickness controlled at high precision.This proposed synthetic protocol was applied for the surface coating of high-voltage cathode materials in the form of LiNi_(0.5)Mn_(1.5)O_(4)(LNMO),leading to significantly enhanced structural and electrochemical stability for its working at 5 V.Notably,after 300 cycles,the modified LNMO was able to achieve capacity retention of 85.1%for its working at 45℃ at a current density of 1 C as compared to only 29.9%of the pristine sample.Our findings highlight the potential of solution-based processes in building conformal coatings for the stabilization of high-energy cathode materials in their LIBs application.
基金supported by the National Natural Science Foundation of China(21421001,21573115)~~
文摘The exploration of cost-effective non-noble-metal electrocatalysts is highly imperative to replace the state-of-the-art platinum-based catalysts for oxygen reduction reaction(ORR). Here, we prepared cobalt phosphonate-derived N-doped cobalt phosphate/carbon nanotube hybrids(Co Pi C-N/CNTs) by hydrothermal treatment of N-containing cobalt phosphonate and oxidized carbon nanotubes(o-CNT) followed by high-temperature calcination under nitrogen atmosphere. The resultant Co Pi C-N/CNT exhibits a superior electrocatalytic performance for the ORR in alkaline media, which is equal to the commercial Pt/C catalyst in the aspect of half-wave potential, onset potential and diffuse limiting current density. Furthermore, the excellent tolerance to methanol and strong durability outperform those of commercial Pt/C. It is found that cobalt phosphonate-derived N-doped cobalt phosphate and the in-situ formed graphitic carbons play key roles on the activity enhancement. Besides, introducing a suitable amount of CNTs enhances the electronic conductivity and further contributes to the improved ORR performance.
基金supported by the Scientific Research Funding Project of the Education Department of Liaoning Province (Grant No.LJ2020QNL002)。
文摘The design and development of new advanced superwetting porous membranes with antioil-fouling performance are still rare and highly desirable because of their potential widespread applications.A metallic phosphate nanoflower-covered mesh membrane with superhydrophilic and unprecedented antioil-fouling properties is prepared by an exceptionally simple and effective in-situ solution corrosion method.As demonstrated,the outstanding antioil-fouling property of the resulting mesh membrane is connected with the special phosphate group and the three-dimensional(3 D) nanoflower structure.Owing to the antioil-fouling property,upon to water,the oil-fouled mesh membrane can keep the surface free of various kinds of oils,including viscous crude oil to light n-hexane.Thanks to its unprecedented self-cleaning property,the superhydrophilic mesh membrane can effectively separate different oil/water mixtures without prior wetted by water,exhibiting great potential for practical spilled oil remediation.
