The development of high-performance transition metal sulfide(TMS)/carbon composites to replace conventional graphite anode remains a critical challenge for advancing lithium-ion batteries(LIBs).In this study,a facile ...The development of high-performance transition metal sulfide(TMS)/carbon composites to replace conventional graphite anode remains a critical challenge for advancing lithium-ion batteries(LIBs).In this study,a facile self-sacrifice template method is developed to prepare FeS encapsulated into N,S co-doped carbon(FeS/NSC)composite using melamine-cyanuric acid(MCA)supermolecule as a multifunctional template precursor.The function of MCA supermolecule for material synthesis is explored,revealing its special function as a dispersant,dopant and pore-forming agent.Furthermore,the effect of Fe source dosage on the morphology,structure and composition of the final products is explored.The resultant FeS/NSC-0.1(where 0.1 represents the mass of added Fe source)exhibits the most optimal proportion,characterized by a good dispersion status of FeS within the NSC matrix,effective N,S co-doping and ample porosity.Benefiting from these merits,the FeS/NSC-0.1 anode demonstrates significantly improved cycling stability and rate capability when compared to the counterparts.Undoubtedly,this work offers a universal method to produce advanced transition metal sulfide/carbon composite electrodes for energy storage and conversion systems.展开更多
Harnessing the redox potential of biochar to activate airborne O_(2)for contaminant removal is challenging.In this study,ferrihydrite(Fh)modified the boron(B),nitrogen(N)co-doped biochars(BCs)composites(Fh/B(n)NC)were...Harnessing the redox potential of biochar to activate airborne O_(2)for contaminant removal is challenging.In this study,ferrihydrite(Fh)modified the boron(B),nitrogen(N)co-doped biochars(BCs)composites(Fh/B(n)NC)were developed for enhancing the degradation of a model pollutant,tetracycline(TC),merely by airborne O_(2).Fh/B(3)NC showed excellent O_(2)activation activity for efficient TC degradation with a apparent TC degradation rate of 5.54,6.88,and 22.15 times that of B(3)NC,Fh,and raw BCs,respectively,where 1O_(2)and H_(2)O_(2)were identified as the dominant ROS for TC degradation.The B incorporation into the carbon lattice of Fh/B(3)NC promoted the generation of electron donors,sp2 C and the reductive B species,hence boosting Fe(III)reduction and 1O_(2)generation.O_(2)adsorption was enhanced due to the positively charged adsorption sites(C-B+and N-C+).And 1O_(2)was generated via Fe(II)catalyzed low-efficient successive one-electron transfer(O_(2)→O_(2)·−→1O_(2),H_(2)O_(2)),as well as biochar catalyzed high-efficient two-electron transfer(O_(2)→H_(2)O_(2)→1O_(2))that does not involve.O_(2)−as the intermediate.Moreover,Fh/B,N co-doped biochar showed a wide pH range,remarkable anti-interference capabilities,and effective detoxification.These findings shed new light on the development of environmentally benign BCs materials capable of degradading organic pollutants.展开更多
[目的]为进一步拓展单原子催化剂在亚硝酸盐还原制氨领域的应用,提出了一种铁-氮-碳(Fe-N-C)单原子催化剂电催化亚硝酸盐还原制氨的新体系.[方法]以二氧化硅为硬模板,2,6-二氨基吡啶为碳氮前驱体,硝酸铁为金属盐,通过“热解-刻蚀”策略...[目的]为进一步拓展单原子催化剂在亚硝酸盐还原制氨领域的应用,提出了一种铁-氮-碳(Fe-N-C)单原子催化剂电催化亚硝酸盐还原制氨的新体系.[方法]以二氧化硅为硬模板,2,6-二氨基吡啶为碳氮前驱体,硝酸铁为金属盐,通过“热解-刻蚀”策略制备了Fe-N-C单原子催化剂,并将其应用于亚硝酸盐制氨反应.[结果]多种结构表征结果显示,Fe-N-C催化剂表面的Fe物种呈现高度分散特征并以单原子形式存在.此外,Fe物种的化学环境主要是+2和+3价混合态,且通过与4个吡啶氮配位而稳定存在,即Fe-N-C催化剂的金属中心微观配位环境为Fe-N4结构.与纯氮碳(N-C)载体相比,本研究制备的Fe-N-C催化剂具有优异的亚硝酸盐还原性能,不仅表现出更高的起始还原电位(0 V vs可逆氢电极),具有接近100%的产氨法拉第效率和高的氨产率[8.4 mg/(h·cm^(2))],并且在连续20次催化循环测试中显示出优异的催化稳定性.[结论]本研究制备的Fe-N-C单原子催化剂对亚硝酸盐还原制氨具有优异的电催化活性,其高活性可能来源于对NO_(2)^(-)的显著吸附,并进一步促进活性氢参与脱氧加氢过程.该Fe-N-C单原子催化亚硝酸盐还原体系可为后续合成氨的活性中心设计提供指导方向.展开更多
Doping engineering is an effective strategy for graphitic carbon nitride(g-C_(3)N_(4))to improve its photocat-alytic hydrogen evolution reaction(HER)performance.In this work,a novel nitrogen and sulfur co-doped g-C_(3...Doping engineering is an effective strategy for graphitic carbon nitride(g-C_(3)N_(4))to improve its photocat-alytic hydrogen evolution reaction(HER)performance.In this work,a novel nitrogen and sulfur co-doped g-C_(3)N_(4)(N,S-g-C_(3)N_(4))is elaborately designed on the basis of theoretical predictions of first-principle density functional theory(DFT).The calculated Gibbs free energy of adsorbed hydrogen(ΔGH∗)for N,S-g-C_(3)N_(4) at the N-doping active sites is extremely close to zero(0.01 eV).Inspired by the theoretical predictions,the N,S-g-C_(3)N_(4) is successfully fabricated through ammonia-rich pyrolysis synthesis strategy,in which ammonia is in-situ obtained by pyrolyzing melamine.Subsequent characterizations indicate that the N,S-g-C_(3)N_(4) possesses high specific surface area,outstanding light utilization,good hydrophilicity,and efficient carrier transfer efficiency.Consequently,the N,S-g-C_(3)N_(4) displays an extremely high H2 evolution rate of 8269.9μmol g−1 h−1,achieves an apparent quantum efficiency(AQE)of 3.24%,and also possesses outsatnding durability.Theoretical calculations further demonstrate that N and S dopants can not only introduce doping energy level to reduce the band gap,but also induce charge redistribution to facilitate hydrogen adsorption,thus promoting the photocatalytic HER process.Moreover,femtosecond transient absorption(fs-TA)spectroscopy further corroborates the efficient photogenerated carrier transport of N,S-g-C_(3)N_(4).This research highlights a promising and reliable strategy to achieve superior photocatalytic activity,and exhibits significant guidance for precise designing high-efficiency photocatalysts.展开更多
The practicality of electrochemical water-splitting technology relies on the development of novel and efficient bifunctional electrocatalysts capable of facilitating both the hydrogen evolution reaction(HER)and oxygen...The practicality of electrochemical water-splitting technology relies on the development of novel and efficient bifunctional electrocatalysts capable of facilitating both the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).Black phosphorus(BP)holds tremendous promise for HER and OER electrocatalysis owing to its fully exposed atoms and high carrier mobility.However,the elec-trocatalytic performance of BP is still much lower than the expected theoretical limit,presenting an exciting challenge for further advancements.Herein,we embed electrochemically exfoliated few-layer BP nanosheets in higher Fermi level(EF)of cobalt,nitrogen co-doped carbons to form a new heterojunction(CoNC-BP),as efficient bifunctional electrocatalysts toward HER and OER for the advancement overall water splitting applications.A directed interfacial electron transfer is realized from CoNC to BP,facilitated by the lowering Fermi level(EF).This interfacial electron transfer plays a crucial role in optimizing the adsorption and desorption of active intermediates,while also introducing an abundance of hypervalent Co sites.These factors collectively contribute to the remarkable electrocatalytic activities of HER and OER performance,leading to the efficient performance of the developed CoNC-BP heterojunction in water-splitting applications.This work demonstrates a promising breakthrough that can inspire the design of high-efficiency catalysts.展开更多
For rechargeable aqueous zinc-ion batteries(ZIBs),the design of nanocomposites comprised of electrochemically active materials and carbon materials with novel structures has great prom-ise in addressing the issue of e...For rechargeable aqueous zinc-ion batteries(ZIBs),the design of nanocomposites comprised of electrochemically active materials and carbon materials with novel structures has great prom-ise in addressing the issue of electrical conductivity and structural stability in the electrode materials during electrochemical cycling.We report the production of a novel flexible electrode material,by anchoring MnO_(2) nanosheets on a B,N co-doped carbon nanotube ar-ray(BNCNTs)grown on carbon cloth(BNCNTs@MnO_(2)),which was fabricated by in-situ pyrolysis and hydrothermal growth.The generated BNCNTs were strongly bonded to the surface of the car-bon fibers in the carbon cloth which provides both excellent elec-tron transport and ion diffusion,and improves the stability and dur-ability of the cathode.Importantly,the BNCNTs offer more active sites for the hydrothermal growth of MnO_(2),ensuring a uniform dis-tribution.Electrochemical tests show that BNCNTs@MnO_(2) delivers a high specific capacity of 310.7 mAh g^(−1) at 0.1 A g^(−1),along with excellent rate capability and outstanding cycling stability,with a 79.7% capacity retention after 8000 cycles at 3 A g^(−1).展开更多
Heteroatom-doped porous carbon materials have been widely studied due to their high specific surface area and high heteroatom content,but it is difficult to achieve high specific surface area and high heteroatom conte...Heteroatom-doped porous carbon materials have been widely studied due to their high specific surface area and high heteroatom content,but it is difficult to achieve high specific surface area and high heteroatom content at the same time.Herein,a simple method is introduced to prepare N/O co-doped hierarchical porous carbon materials(DNZKs).Phthalonitrile resins(DNZs)were prepared by using 1,3-bis(3,4-dicyanophenoxy)benzene as raw material and ZnCl_(2)/urea as composite curing agent,and then using KOH as activator to successfully prepare DNZKs with high specific surface area,developed pores and high N/O content.The porous carbon material(DNZK@400)obtained at a curing temperature of 400℃ has the highest N content(4.97%(mass)),a large specific surface area(2026 m^(2)·g^(-1)),a high micropore proportion(0.9),a high O content(7.53%(mass)),and the best specific capacitance(up to 567 F·g^(-1) at 0.1 A·g^(-1)),which can be attribute to the high temperature resistance of the nitrogencontaining aromatic heterocyclic structure in DNZs.When the mass ratio of resin and KOH is 1:1,the specific capacitance of the sample tested by the acid three-electrode system is obtained,and it is found that the material has high cycling stability(119%specific capacitance retention after 100,000 cycle tests).This work proposes a simple and easy-to-operate method for the preparation of multifunctional porous carbon.展开更多
Aqueous zinc-based energy storage devices(ZESDs)have garnered considerable interest because of their high specific capacity,abundant zinc reserves,excellent safety,and environmental friendliness.In recent years,variou...Aqueous zinc-based energy storage devices(ZESDs)have garnered considerable interest because of their high specific capacity,abundant zinc reserves,excellent safety,and environmental friendliness.In recent years,various types of boron,nitrogen co-doped carbon(BNC)materials have been developed to improve electrochemical performance of ZESDs.To promote the advancement of these technologies,we herein give a comprehensive review of the progress in BNC materials for ZESDs.The different synthetic methods employed in the preparation of BNC materials,including direct carbonization,template method,chemical vapor deposition,hydrothermal method,etc.,are summarized.These methods play a vital role in tailoring the structure,composition,and properties of BNC materials to optimize their performance in energy storage applications.Furthermore,some key achievements of BNC materials in zinc-air batteries and zinc-ion hybrid supercapacitors are elaborated.Lastly,future challenges and development directions of BNC materials in ZESDs are prospected.This comprehensive review could serve as a valuable resource in the energy storage field,providing insights into the potential of BNC materials in zinc-based energy storage technologies.展开更多
Proton exchange membrane fuel cells(PEMFCs)constitute a promising avenue for environmentally friendly power generation.However,the reliance on unsustainable platinum-based electrocatalysts used at the electrodes poses...Proton exchange membrane fuel cells(PEMFCs)constitute a promising avenue for environmentally friendly power generation.However,the reliance on unsustainable platinum-based electrocatalysts used at the electrodes poses challenges to the commercial viability of PEMFCs.Non-platinum group metal(non-PGM)alternatives,like nitrogen-coordinated transition metals in atomic dispersion(M–N–C catalysts),show significant potential.This work presents a comparative study of two distinct sets of Fe–N–C materials,prepared by pyrolyzing hybrid composites of polyaniline(PANI)and iron(Ⅱ)chloride on a hard template.One set uses bipyridine(BPy)as an additional nitrogen source and iron ligand,offering an innovative approach.The findings reveal that the choice of pyrolysis temperature and atmosphere influences the catalyst properties.The use of ammonia in pyrolysis emerges as a crucial parameter for promoting atomic dispersion of iron,as well as increasing surface area and porosity.The optimal catalyst,prepared using BPy and ammonia,exhibits a half-wave potential of 0.834 V in 0.5 M H_(2)SO_(4)(catalyst loading of 0.6 mg cm^(-2)),a mass activity exceeding 3 A g^(-1)and high stability in acidic electrolyte,positioning it as a promising non-PGM structure in the field.展开更多
Sodium-ion batteries(SIBs) and hybrid capacitors(SIHCs) have garnered significant attention in energy storage due to their inherent advantages,including high energy density,cost-effectiveness,and enhanced safety.Howev...Sodium-ion batteries(SIBs) and hybrid capacitors(SIHCs) have garnered significant attention in energy storage due to their inherent advantages,including high energy density,cost-effectiveness,and enhanced safety.However,developing high-performance anode materials to improve sodium storage performa nce still remains a major challenge.Here,a facile one-pot method has been developed to fabricate a hybrid of MoSeTe nanosheets implanted within the N,F co-doped honeycomb carbon skeleton(MoSeTe/N,F@C).Experimental results demonstrate that the incorporation of large-sized Te atoms into MoSeTe nanosheets enlarges the layer spacing and creates abundant anion vacancies,which effectively facilitate the insertion/extraction of Na^(+) and provide numerous ion adsorption sites for rapid surface capacitive behavior.Additionally,the heteroatoms N,F co-doped honeycomb carbon skeleton with a highly conductive network can restrain the volume expansion and boost reaction kinetics within the electrode.As anticipated,the MoSeTe/N,F@C anode exhibits high reversible capacities along with exceptional cycle stability.When coupled with Na_(3)V_(2)(PO_(4))_(3)@C(NVPF@C) to form SIB full cells,the anode delivers a reversible specific capacity of 126 mA h g^(-1) after 100 cycles at 0.1 A g^(-1).Furthermore,when combined with AC to form SIHC full cells,the anode demonstrates excellent cycling stability with a reversible specific capacity of50 mA h g^(-1) keeping over 3700 cycles at 1.0 A g^(-1).In situ XRD,ex situ TEM characterization,and theoretical calculations(DFT) further confirm the reversibility of sodium storage in MoSeTe/N,F@C anode materials during electrochemical reactions,highlighting their potential for widespread practical application.This work provides new insights into the promising utilization of advanced transition metal dichalcogenides as anode materials for Na^(+)-based energy storage devices.展开更多
A series of photocatalysts of un-doped, single-doped and co-doped nanometer titanium diox- ide （TiO2） have been successfully prepared by template method using Fe（NO3）3.9H2O, La（NO3）3.6H2O, and tetrabutyl titanat...A series of photocatalysts of un-doped, single-doped and co-doped nanometer titanium diox- ide （TiO2） have been successfully prepared by template method using Fe（NO3）3.9H2O, La（NO3）3.6H2O, and tetrabutyl titanate as precursors and glucan as template. Scanning electron microscopy, X-ray diffraction, and N2 adsorption-desorption measurement were employed to characterize the morphology, crystal structure and surface structure of the samples. The photo-absorbance of the obtained catalysts was measured by UV-Vis absorption spectroscopy, and the photocatalytic activities of the prepared samples under UV and visible light were estimated by measuring the degradation rate of methyl orange in an aqueous solution. The characterizations indicated that the prepared photocatalysts consisted of anatase phase and possessed high surface area of ca. 163-176 m2/g. It was shown that the Fe and La co-doped nano-TiO2 could be activated by visible light and could thus be used as an effective catalyst in photo-oxidation reactions. The synergistic effect of Fe and La co-doping played an important role in improving the photocatalytic activity. In addition, the possibility of cyclic usage of co-doped nano-TiO2 was also confirmed, the photocatalytic activity of codoped nano-TiO2 remained above 89.6% of the fresh sample after being used four times.展开更多
基金supported by the Science Technology Talents Lifting Project of Hunan Province(No.2022TJ-N16)the Natural Science Foundation of Hunan Province(Nos.2024JJ4022,2023JJ30277,2025JJ60382)+3 种基金the China Postdoctoral Fellowship Program(GZC20233205)the Scientifc Research Fund of Hunan Provincial Education Department,China(No.24B0270)the National Natural Science Foundation of China(No.32201646)the Key Project of Jiangxi Provincial Research and Development Program(No.20243BBI91001).
文摘The development of high-performance transition metal sulfide(TMS)/carbon composites to replace conventional graphite anode remains a critical challenge for advancing lithium-ion batteries(LIBs).In this study,a facile self-sacrifice template method is developed to prepare FeS encapsulated into N,S co-doped carbon(FeS/NSC)composite using melamine-cyanuric acid(MCA)supermolecule as a multifunctional template precursor.The function of MCA supermolecule for material synthesis is explored,revealing its special function as a dispersant,dopant and pore-forming agent.Furthermore,the effect of Fe source dosage on the morphology,structure and composition of the final products is explored.The resultant FeS/NSC-0.1(where 0.1 represents the mass of added Fe source)exhibits the most optimal proportion,characterized by a good dispersion status of FeS within the NSC matrix,effective N,S co-doping and ample porosity.Benefiting from these merits,the FeS/NSC-0.1 anode demonstrates significantly improved cycling stability and rate capability when compared to the counterparts.Undoubtedly,this work offers a universal method to produce advanced transition metal sulfide/carbon composite electrodes for energy storage and conversion systems.
基金supported by the National Natural Science Foundation of China(No.U21A20293).
文摘Harnessing the redox potential of biochar to activate airborne O_(2)for contaminant removal is challenging.In this study,ferrihydrite(Fh)modified the boron(B),nitrogen(N)co-doped biochars(BCs)composites(Fh/B(n)NC)were developed for enhancing the degradation of a model pollutant,tetracycline(TC),merely by airborne O_(2).Fh/B(3)NC showed excellent O_(2)activation activity for efficient TC degradation with a apparent TC degradation rate of 5.54,6.88,and 22.15 times that of B(3)NC,Fh,and raw BCs,respectively,where 1O_(2)and H_(2)O_(2)were identified as the dominant ROS for TC degradation.The B incorporation into the carbon lattice of Fh/B(3)NC promoted the generation of electron donors,sp2 C and the reductive B species,hence boosting Fe(III)reduction and 1O_(2)generation.O_(2)adsorption was enhanced due to the positively charged adsorption sites(C-B+and N-C+).And 1O_(2)was generated via Fe(II)catalyzed low-efficient successive one-electron transfer(O_(2)→O_(2)·−→1O_(2),H_(2)O_(2)),as well as biochar catalyzed high-efficient two-electron transfer(O_(2)→H_(2)O_(2)→1O_(2))that does not involve.O_(2)−as the intermediate.Moreover,Fh/B,N co-doped biochar showed a wide pH range,remarkable anti-interference capabilities,and effective detoxification.These findings shed new light on the development of environmentally benign BCs materials capable of degradading organic pollutants.
文摘[目的]为进一步拓展单原子催化剂在亚硝酸盐还原制氨领域的应用,提出了一种铁-氮-碳(Fe-N-C)单原子催化剂电催化亚硝酸盐还原制氨的新体系.[方法]以二氧化硅为硬模板,2,6-二氨基吡啶为碳氮前驱体,硝酸铁为金属盐,通过“热解-刻蚀”策略制备了Fe-N-C单原子催化剂,并将其应用于亚硝酸盐制氨反应.[结果]多种结构表征结果显示,Fe-N-C催化剂表面的Fe物种呈现高度分散特征并以单原子形式存在.此外,Fe物种的化学环境主要是+2和+3价混合态,且通过与4个吡啶氮配位而稳定存在,即Fe-N-C催化剂的金属中心微观配位环境为Fe-N4结构.与纯氮碳(N-C)载体相比,本研究制备的Fe-N-C催化剂具有优异的亚硝酸盐还原性能,不仅表现出更高的起始还原电位(0 V vs可逆氢电极),具有接近100%的产氨法拉第效率和高的氨产率[8.4 mg/(h·cm^(2))],并且在连续20次催化循环测试中显示出优异的催化稳定性.[结论]本研究制备的Fe-N-C单原子催化剂对亚硝酸盐还原制氨具有优异的电催化活性,其高活性可能来源于对NO_(2)^(-)的显著吸附,并进一步促进活性氢参与脱氧加氢过程.该Fe-N-C单原子催化亚硝酸盐还原体系可为后续合成氨的活性中心设计提供指导方向.
基金supported by the National Natural Science Foun-dation of China(No.62004143)the Key R&D Program of Hubei Province(No.2022BAA084)the Natural Science Foundation of Hubei Province(No.2021CFB133).
文摘Doping engineering is an effective strategy for graphitic carbon nitride(g-C_(3)N_(4))to improve its photocat-alytic hydrogen evolution reaction(HER)performance.In this work,a novel nitrogen and sulfur co-doped g-C_(3)N_(4)(N,S-g-C_(3)N_(4))is elaborately designed on the basis of theoretical predictions of first-principle density functional theory(DFT).The calculated Gibbs free energy of adsorbed hydrogen(ΔGH∗)for N,S-g-C_(3)N_(4) at the N-doping active sites is extremely close to zero(0.01 eV).Inspired by the theoretical predictions,the N,S-g-C_(3)N_(4) is successfully fabricated through ammonia-rich pyrolysis synthesis strategy,in which ammonia is in-situ obtained by pyrolyzing melamine.Subsequent characterizations indicate that the N,S-g-C_(3)N_(4) possesses high specific surface area,outstanding light utilization,good hydrophilicity,and efficient carrier transfer efficiency.Consequently,the N,S-g-C_(3)N_(4) displays an extremely high H2 evolution rate of 8269.9μmol g−1 h−1,achieves an apparent quantum efficiency(AQE)of 3.24%,and also possesses outsatnding durability.Theoretical calculations further demonstrate that N and S dopants can not only introduce doping energy level to reduce the band gap,but also induce charge redistribution to facilitate hydrogen adsorption,thus promoting the photocatalytic HER process.Moreover,femtosecond transient absorption(fs-TA)spectroscopy further corroborates the efficient photogenerated carrier transport of N,S-g-C_(3)N_(4).This research highlights a promising and reliable strategy to achieve superior photocatalytic activity,and exhibits significant guidance for precise designing high-efficiency photocatalysts.
基金National Natural Science Foundation of China(Grant No.62004143)Key R&D Program of Hubei Province(Grant No.2022BAA084)+4 种基金Natural Science Foundation of Hubei Province(Grant No.2021CFB133)National Key R&D Program of China(Grant No.2022YFC3902703)Innovation Project of Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education(Grant No.LCX2021003)Open Research Fund of Key Laboratory of Material Chemistry for Energy Conversion and Storage(HUST),Ministry of Education(Grant No.2021JYBKF05)14th Graduate Ed-ucation Innovation Fund of Wuhan Institute of Technology(Grant Nos.CX2022564 and CX2022451).
文摘The practicality of electrochemical water-splitting technology relies on the development of novel and efficient bifunctional electrocatalysts capable of facilitating both the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).Black phosphorus(BP)holds tremendous promise for HER and OER electrocatalysis owing to its fully exposed atoms and high carrier mobility.However,the elec-trocatalytic performance of BP is still much lower than the expected theoretical limit,presenting an exciting challenge for further advancements.Herein,we embed electrochemically exfoliated few-layer BP nanosheets in higher Fermi level(EF)of cobalt,nitrogen co-doped carbons to form a new heterojunction(CoNC-BP),as efficient bifunctional electrocatalysts toward HER and OER for the advancement overall water splitting applications.A directed interfacial electron transfer is realized from CoNC to BP,facilitated by the lowering Fermi level(EF).This interfacial electron transfer plays a crucial role in optimizing the adsorption and desorption of active intermediates,while also introducing an abundance of hypervalent Co sites.These factors collectively contribute to the remarkable electrocatalytic activities of HER and OER performance,leading to the efficient performance of the developed CoNC-BP heterojunction in water-splitting applications.This work demonstrates a promising breakthrough that can inspire the design of high-efficiency catalysts.
基金financial support from projects funded by the National Natural Science Foundation of China(52172038,22179017)the National Key Research and Development Program of China(2022YFB4101600,2022YFB4101601)。
文摘For rechargeable aqueous zinc-ion batteries(ZIBs),the design of nanocomposites comprised of electrochemically active materials and carbon materials with novel structures has great prom-ise in addressing the issue of electrical conductivity and structural stability in the electrode materials during electrochemical cycling.We report the production of a novel flexible electrode material,by anchoring MnO_(2) nanosheets on a B,N co-doped carbon nanotube ar-ray(BNCNTs)grown on carbon cloth(BNCNTs@MnO_(2)),which was fabricated by in-situ pyrolysis and hydrothermal growth.The generated BNCNTs were strongly bonded to the surface of the car-bon fibers in the carbon cloth which provides both excellent elec-tron transport and ion diffusion,and improves the stability and dur-ability of the cathode.Importantly,the BNCNTs offer more active sites for the hydrothermal growth of MnO_(2),ensuring a uniform dis-tribution.Electrochemical tests show that BNCNTs@MnO_(2) delivers a high specific capacity of 310.7 mAh g^(−1) at 0.1 A g^(−1),along with excellent rate capability and outstanding cycling stability,with a 79.7% capacity retention after 8000 cycles at 3 A g^(−1).
基金supported by the National Natural Science Foundation of China(51673033 and 52073038)the Fundamental Research Funds for the Central Universities(DUT22LAB605).
文摘Heteroatom-doped porous carbon materials have been widely studied due to their high specific surface area and high heteroatom content,but it is difficult to achieve high specific surface area and high heteroatom content at the same time.Herein,a simple method is introduced to prepare N/O co-doped hierarchical porous carbon materials(DNZKs).Phthalonitrile resins(DNZs)were prepared by using 1,3-bis(3,4-dicyanophenoxy)benzene as raw material and ZnCl_(2)/urea as composite curing agent,and then using KOH as activator to successfully prepare DNZKs with high specific surface area,developed pores and high N/O content.The porous carbon material(DNZK@400)obtained at a curing temperature of 400℃ has the highest N content(4.97%(mass)),a large specific surface area(2026 m^(2)·g^(-1)),a high micropore proportion(0.9),a high O content(7.53%(mass)),and the best specific capacitance(up to 567 F·g^(-1) at 0.1 A·g^(-1)),which can be attribute to the high temperature resistance of the nitrogencontaining aromatic heterocyclic structure in DNZs.When the mass ratio of resin and KOH is 1:1,the specific capacitance of the sample tested by the acid three-electrode system is obtained,and it is found that the material has high cycling stability(119%specific capacitance retention after 100,000 cycle tests).This work proposes a simple and easy-to-operate method for the preparation of multifunctional porous carbon.
基金financially supported by the National Natural Science Foundation of China(No.22302177)the Public Technology Application Project of Jinhua City(No.2022–4-067)the Self Designed Scientific Research of Zhejiang Normal University(No.2021ZS0604)。
文摘Aqueous zinc-based energy storage devices(ZESDs)have garnered considerable interest because of their high specific capacity,abundant zinc reserves,excellent safety,and environmental friendliness.In recent years,various types of boron,nitrogen co-doped carbon(BNC)materials have been developed to improve electrochemical performance of ZESDs.To promote the advancement of these technologies,we herein give a comprehensive review of the progress in BNC materials for ZESDs.The different synthetic methods employed in the preparation of BNC materials,including direct carbonization,template method,chemical vapor deposition,hydrothermal method,etc.,are summarized.These methods play a vital role in tailoring the structure,composition,and properties of BNC materials to optimize their performance in energy storage applications.Furthermore,some key achievements of BNC materials in zinc-air batteries and zinc-ion hybrid supercapacitors are elaborated.Lastly,future challenges and development directions of BNC materials in ZESDs are prospected.This comprehensive review could serve as a valuable resource in the energy storage field,providing insights into the potential of BNC materials in zinc-based energy storage technologies.
基金funding from the Hellenic Foundation for Research and Innovation(HFRI)under grant agreement No 3655.
文摘Proton exchange membrane fuel cells(PEMFCs)constitute a promising avenue for environmentally friendly power generation.However,the reliance on unsustainable platinum-based electrocatalysts used at the electrodes poses challenges to the commercial viability of PEMFCs.Non-platinum group metal(non-PGM)alternatives,like nitrogen-coordinated transition metals in atomic dispersion(M–N–C catalysts),show significant potential.This work presents a comparative study of two distinct sets of Fe–N–C materials,prepared by pyrolyzing hybrid composites of polyaniline(PANI)and iron(Ⅱ)chloride on a hard template.One set uses bipyridine(BPy)as an additional nitrogen source and iron ligand,offering an innovative approach.The findings reveal that the choice of pyrolysis temperature and atmosphere influences the catalyst properties.The use of ammonia in pyrolysis emerges as a crucial parameter for promoting atomic dispersion of iron,as well as increasing surface area and porosity.The optimal catalyst,prepared using BPy and ammonia,exhibits a half-wave potential of 0.834 V in 0.5 M H_(2)SO_(4)(catalyst loading of 0.6 mg cm^(-2)),a mass activity exceeding 3 A g^(-1)and high stability in acidic electrolyte,positioning it as a promising non-PGM structure in the field.
基金supported by the National Natural Science Foundation of China(No.52002320,and 51972267)the China Postdoctoral Science Foundation(No.2022M712574)+3 种基金the Science Foundation of Shaanxi Province(2022GD-TSLD-18,No.2023-JCZD-03)Natural Science Foundation of Shaanxi Province(No.2022GY-372,2021GY-153)Industrial Projects Foundation of Ankang Science and Technology Bureau(No.AK2020-GY02-2)the Platform Construction Projects and Technology Service Teams of Ankang University(No.2021AYPT12 and 2022TD07)。
文摘Sodium-ion batteries(SIBs) and hybrid capacitors(SIHCs) have garnered significant attention in energy storage due to their inherent advantages,including high energy density,cost-effectiveness,and enhanced safety.However,developing high-performance anode materials to improve sodium storage performa nce still remains a major challenge.Here,a facile one-pot method has been developed to fabricate a hybrid of MoSeTe nanosheets implanted within the N,F co-doped honeycomb carbon skeleton(MoSeTe/N,F@C).Experimental results demonstrate that the incorporation of large-sized Te atoms into MoSeTe nanosheets enlarges the layer spacing and creates abundant anion vacancies,which effectively facilitate the insertion/extraction of Na^(+) and provide numerous ion adsorption sites for rapid surface capacitive behavior.Additionally,the heteroatoms N,F co-doped honeycomb carbon skeleton with a highly conductive network can restrain the volume expansion and boost reaction kinetics within the electrode.As anticipated,the MoSeTe/N,F@C anode exhibits high reversible capacities along with exceptional cycle stability.When coupled with Na_(3)V_(2)(PO_(4))_(3)@C(NVPF@C) to form SIB full cells,the anode delivers a reversible specific capacity of 126 mA h g^(-1) after 100 cycles at 0.1 A g^(-1).Furthermore,when combined with AC to form SIHC full cells,the anode demonstrates excellent cycling stability with a reversible specific capacity of50 mA h g^(-1) keeping over 3700 cycles at 1.0 A g^(-1).In situ XRD,ex situ TEM characterization,and theoretical calculations(DFT) further confirm the reversibility of sodium storage in MoSeTe/N,F@C anode materials during electrochemical reactions,highlighting their potential for widespread practical application.This work provides new insights into the promising utilization of advanced transition metal dichalcogenides as anode materials for Na^(+)-based energy storage devices.
文摘A series of photocatalysts of un-doped, single-doped and co-doped nanometer titanium diox- ide （TiO2） have been successfully prepared by template method using Fe（NO3）3.9H2O, La（NO3）3.6H2O, and tetrabutyl titanate as precursors and glucan as template. Scanning electron microscopy, X-ray diffraction, and N2 adsorption-desorption measurement were employed to characterize the morphology, crystal structure and surface structure of the samples. The photo-absorbance of the obtained catalysts was measured by UV-Vis absorption spectroscopy, and the photocatalytic activities of the prepared samples under UV and visible light were estimated by measuring the degradation rate of methyl orange in an aqueous solution. The characterizations indicated that the prepared photocatalysts consisted of anatase phase and possessed high surface area of ca. 163-176 m2/g. It was shown that the Fe and La co-doped nano-TiO2 could be activated by visible light and could thus be used as an effective catalyst in photo-oxidation reactions. The synergistic effect of Fe and La co-doping played an important role in improving the photocatalytic activity. In addition, the possibility of cyclic usage of co-doped nano-TiO2 was also confirmed, the photocatalytic activity of codoped nano-TiO2 remained above 89.6% of the fresh sample after being used four times.
