Organic small structure quinones go with ionic liquids electrolytes would exhibit ultrastable electrochemical properties.In this study,calix[6]quinone(C6Q) cathode was matched with ionic liquid electrolyte Li[TFSI]/[P...Organic small structure quinones go with ionic liquids electrolytes would exhibit ultrastable electrochemical properties.In this study,calix[6]quinone(C6Q) cathode was matched with ionic liquid electrolyte Li[TFSI]/[PY13][TFSI](bis(trifluoromethane)sulfonimide lithium salt/N-methyl-N-pro pylpyrrolidinium bis(trifluoromethanesulfonyl)amide) to assemble lithium-ion batteries(LIBs).The electrochemical performance of LIBs was systematically studied.The capacity retention rates of C6Q through 1000 cycles at current densities of 0.2 C and 0.5 C were 70% and 72%,respectively.At 5 C, the capacity was maintained at 190 mAh g^(-1) after 1000 cycles,and 155 mAh g^(-1) even after 10,000 cycles,comparable to inorganic materials.This work would give a big push to the practical process of organic electrode materials in energy storage.展开更多
Solid-state electrolytes with high oxidation stability are crucial for achieving high power density allsolid-state lithium batteries.Halide electrolytes are promising candidates due to their outstanding compatibility ...Solid-state electrolytes with high oxidation stability are crucial for achieving high power density allsolid-state lithium batteries.Halide electrolytes are promising candidates due to their outstanding compatibility with cathode materials and high Li^(+)conductivity.However,the electrochemical stability of chloride electrolytes is still limited,leaving them unsuitable for ultrahigh voltage operation.Besides,chemical compatibility issue between sulfide and halide electrolytes affects the electrochemical performance of all-solid-state batteries.Herein,Li-ion conductor Li_(3+x)InCl_(6-x)O_(x) is designed to address these challenges.Li_(3.25)InCl_(5.75)O_(0.25)shows a Li-ion conductivity of 0.90 mS cm^(-1)at room temperature,a high onset oxidation voltage of 3.84 V,fewer by-products at ultrahigh operation voltage,and good chemical compatibility with Li_(5.5)PS_(4.5)Cl_(1.5).The Li_(3.25)InCl_(5.75)O_(0.25)@LiNi_(0.7)Co_(0.1)Mn_(0.2)O_(2)-Li_(3.25)InCl_(5.75)O_(0.25)-VGCF/Li_(3.25)InCl_(5.75)O_(0.25)/Li_(5.5)PS_(4.5)Cl_(1.5)/Li-In battery delivers good electrochemical performances at high operating voltage.This work provides a simple,economical,and effective strategy for designing high-voltage all-solid-state electrolytes.展开更多
Layered ammonium vanadate has become a promising cathode material for aqueous zinc ion batteries(ZIBs)due to its small mass and large ionic radius of ammonium ions as well as the consequent large layer spacing and hig...Layered ammonium vanadate has become a promising cathode material for aqueous zinc ion batteries(ZIBs)due to its small mass and large ionic radius of ammonium ions as well as the consequent large layer spacing and high specific capacity.However,the irreversible de-ammoniation caused by N·H···O bonds damaged would impair cycle life of ZIBs and the strong electrostatic interaction between Zn^(2+)and V-O frame could slower the mobility of Zn^(2+).Furthermore,the thermal instability of ammonium vanadate also limits the use of common carbon coating modification method to solve the problem.Herein,V_(2)CT_(X)MXene was innovatively selected as a bifunctional source to in-situ derivatized(NH_(4))_(2)V_(8)O_(20)·x H_(2)O with amorphous carbon-coated(NHVO@C)via one-step hydrothermal method in relatively moderate temperature.The amorphous carbon shell derived from the V_(2)CT_(X)MXene as a conductive framework to effectively improve the diffusion kinetics of Zn^(2+)and the robust carbon skeleton could alleviate the ammonium dissolution during long-term cycling.As a result,zinc ion batteries using NHVO@C as cathode exhibit superior electrochemical performance.Moreover,the assembled foldable or high loading(10.2 mg/cm^(2))soft-packed ZIBs further demonstrates its practical application.This study provided new insights into the development of the carbon cladding process for thermally unstable materials in moderate temperatures.展开更多
Developing advanced battery-type materials with abundant active sites,high conductivity,versatile morphologies,and hierarchically porous structures is crucial for realizing high-quality hybrid supercapacitors.Herein,h...Developing advanced battery-type materials with abundant active sites,high conductivity,versatile morphologies,and hierarchically porous structures is crucial for realizing high-quality hybrid supercapacitors.Herein,heterogeneous FeS@NiS is synthesized by cationic Co doping via surface-structure engineering.The density functional theory(DFT)theoretical calculations are firstly performed to predict the advantages of Co dopant by improving the OH^(−)adsorption properties and adjusting electronic structure,benefiting ions/electron transfer.The dynamic surface evolution is further explored which demonstrates that CoFeS@CoNiS could be quickly reconstructed to Ni(Co)Fe_(2)O_(4)during the charging process,while the unstable structure of the amorphous Ni(Co)Fe_(2)O_(4)results in partial conversion to Ni/Co/FeOOH at high potentials,which contributes to the more reactive active site and good structural stability.Thus,the free-standing electrode reveals excellent electrochemical performance with a superior capacity(335.6 mA h g^(−1),2684 F g^(−1))at 3 A g^(−1).Furthermore,the as-fabricated device shows a quality energy density of 78.1 W h kg^(−1)at a power density of 750 W kg^(−1)and excellent cycle life of 92.1%capacitance retention after 5000 cycles.This work offers a facile strategy to construct versatile morphological structures using electrochemical activation and holds promising applications in energy-related fields.展开更多
Pt-based materials are the benchmarked catalysts in the cathodic hydrogen evolution reaction(HER)of water splitting;the prohibitive cost and scarcity of Pt immensely impede the commercialization of hydrogen energy.Ru ...Pt-based materials are the benchmarked catalysts in the cathodic hydrogen evolution reaction(HER)of water splitting;the prohibitive cost and scarcity of Pt immensely impede the commercialization of hydrogen energy.Ru has aroused significant concern because of its Pt-like activity and much lower price.However,it’s still a top priority to minimize the Ru loading and pursue the most superior cost performance.展开更多
Molybdenum carbide(MO_(2)C)materials are promising electrocatalysts with potential applications in hydrogen evolution reaction(HER)due to low cost and Pt-like electronic structures.Nevertheless,their HER activity is u...Molybdenum carbide(MO_(2)C)materials are promising electrocatalysts with potential applications in hydrogen evolution reaction(HER)due to low cost and Pt-like electronic structures.Nevertheless,their HER activity is usually hindered by the strong hydrogen binding energy.Moreover,the lack of water-cleaving site's makes it difficult for the catalysts to work in alkaline solutions.Here,we designed and synthesized a B and N dual-doped carbon layer that encapsulated on MO_(2)C nanocrystals(MO_(2)C@BNC)for accelerating HER under alkaline condition.The electronic interactions between the MO_(2)C nanocrystals and the multiple-doped carbon layer endow a near-zero H adsorption Gibbs free energy on the defective C atoms over the carbon shell.Meanwhile,the introduced B atoms afford optimal H_2O adsorption sites for the water-cleaving step.Accordingly,the dual-doped MO_(2)C catalyst with synergistic effect of non-metal sites delivers superior HER performances of a low overpotential(99 mV@10 mA cm^(-2))and a small Tafel slope(58.1 mV dec^(-1))in 1 M KOH solution.Furthermore,it presents a remarkable activity that outperforming the commercial 10%Pt/C catalyst at large current density,demonstrating its applicability in industrial water splitting.This study provides a reasonable design strategy towards noble-metal-free HER catalysts with high activity.展开更多
In this study,acrylic acid was used as a neutralizer to prepare bio-based WPU with an interpenetrating polymer network structure by thermally induced free radical emulsion polymerization.The effects of the content of ...In this study,acrylic acid was used as a neutralizer to prepare bio-based WPU with an interpenetrating polymer network structure by thermally induced free radical emulsion polymerization.The effects of the content of acrylic acid on the properties of the resulting waterborne polyurethane-poly(acrylic acid)(WPU-PAA)dispersion and the films were systematically investigated.The results showed that the cross-linking density of the interpenetrating network polymers was increased and the interlocking structure of the soft and hard phase dislocations in the molecular segments of the double networks was tailored with increasing the content of acrylic acid,leading to enhancement of the mechanical properties and water resistance of WPU-PAA films.Notably,with the increase in content of acrylic acid,the tensile strength,Young’s modulus,and toughness of the WPU-PAA-110 film increased by 3 times,and 8 times,and 2.4 times compared with WPU-PAA-80,respectively.The WPU-PAA-100 film showed the best water resistance,and the water absorption rate at 96 h was only 3.27%.This work provided a new design scheme for constructing bio-based WPU materials with excellent properties.展开更多
TiNb2O7 anode materials(TNO)have unique potential for applications in Li-ion capacitors(LICs)due to their high specific capacity of ca.280 mA h g^-1 over a wide anodic Li-insertion potential window.However,their highr...TiNb2O7 anode materials(TNO)have unique potential for applications in Li-ion capacitors(LICs)due to their high specific capacity of ca.280 mA h g^-1 over a wide anodic Li-insertion potential window.However,their highrate capability is limited by their poor electronic and ionic conductivity.In particular,studies on TNO for LICs are lacking and that for flexible LICs have not yet been reported.Herein,a unique TNO porous electrode with cross-linked nanorods tailored by post-annealing and its application in flexible LICs are reported.This binder-free TNO anode exhibits superior rate performance(~66.3%capacity retention as the rate increases from 1 to 40 C),which is ascribed to the greatly shortened ion-diffusion length in TNO nanorods,facile electrolyte penetration and fast electron transport along the continuous single-crystalline nanorod network.Furthermore,the TNO anode shows an excellent cycling stability up to 2000 cycles and good flexibility(no capacity loss after continuous bending for 500 times).Model flexible LIC assembled with the TNO anode and activated carbon cathode exhibits increased gravimetric and volumetric energy/power densities(~100.6 W h kg^-1/4108.8 W kg^-1;10.7 mW h cm^-3/419.3 mW cm^-3),more superior to previously reported hybrid supercapacitors.The device also efficiently powers an LED light upon 180°bending.展开更多
Selenium sulfide(SeS2)cathodes have attracted much concern as an optimized choice comparing to sulfur and selenium for lithium and sodium storage.However,it also suffers from poor cycling stability due to the dissolut...Selenium sulfide(SeS2)cathodes have attracted much concern as an optimized choice comparing to sulfur and selenium for lithium and sodium storage.However,it also suffers from poor cycling stability due to the dissolution of reaction intermediate products.In this study,N-doped Interconnected carbon aerogels was applied as an efficient SeS2 host by infiltrating selenium sulfide into its microporous structure(denoted as SeS2@NCAs),which could effectively accommodate the volume change of SeS2 during cycling and alleviate the dissolution of reaction intermediate products.Therefore,as for Na storage,the SeS2@NCAs cathode delivers a superior long-term cycling performance of 536 mA·h·g^-1 at a current density of 0.5 A·g^-1 after 1,000 cycles with only 0.04%capacity decline per cycle and a high rate performance(524 mA·h·g^-1 at 2 A·g^-1 and 745 mA·h·g^-1 at 0.1 A·g^-1 retained),indicating the remarkable cycling stability of SeS2@NCAs cathodes.展开更多
Iron-based nanostructures represent an emerging class of catalysts with high electroactivity for oxygen reduction reaction(ORR)in energy storage and conversion technologies.However,current practical applications have ...Iron-based nanostructures represent an emerging class of catalysts with high electroactivity for oxygen reduction reaction(ORR)in energy storage and conversion technologies.However,current practical applications have been limited by insufficient durability in both alkaline and acidic environments.In particular,limited attention has been paid to stabilizing iron-based catalysts by introducing additional metal by the alloying effect.Herein,we report bimetallic Fe_(2)Mo nanoparticles on N-doped carbon(Fe_(2)Mo/NC)as an efficient and ultra-stable ORR electrocatalyst for the first time.The Fe_(2)Mo/NC catalyst shows high selectivity for a four-electron pathway of ORR and remarkable electrocatalytic activity with high kinetics current density and half-wave potential as well as low Tafel slope in both acidic and alkaline medias.It demonstrates excellent long-term durability with no activity loss even after 10,000 potential cycles.Density functional theory(DFT)calculations have confirmed the modulated electronic structure of formed Fe_(2)Mo,which supports the electron-rich structure for the ORR process.Meanwhile,the mutual protection between Fe and Mo sites guarantees efficient electron transfer and long-term stability,especially under the alkaline environment.This work has supplied an effective strategy to solve the dilemma between high electroactivity and long-term durability for the Fe-based electrocatalysts,which opens a new direction of developing novel electrocatalyst systems for future research.展开更多
基金supported by the National Natural Science Foundation of China (Nos. 21875206 and 21403187)the Natural Science Foundation of Hebei Province (B2019203487)。
文摘Organic small structure quinones go with ionic liquids electrolytes would exhibit ultrastable electrochemical properties.In this study,calix[6]quinone(C6Q) cathode was matched with ionic liquid electrolyte Li[TFSI]/[PY13][TFSI](bis(trifluoromethane)sulfonimide lithium salt/N-methyl-N-pro pylpyrrolidinium bis(trifluoromethanesulfonyl)amide) to assemble lithium-ion batteries(LIBs).The electrochemical performance of LIBs was systematically studied.The capacity retention rates of C6Q through 1000 cycles at current densities of 0.2 C and 0.5 C were 70% and 72%,respectively.At 5 C, the capacity was maintained at 190 mAh g^(-1) after 1000 cycles,and 155 mAh g^(-1) even after 10,000 cycles,comparable to inorganic materials.This work would give a big push to the practical process of organic electrode materials in energy storage.
基金supported by the National Key Research and Development Program of China(2021YFB2500200)the National Natural Science Foundation of China(52177214,52222703)for supporting our workJiangsu Funding Program for Excellent Postdoctoral Talent for the support。
文摘Solid-state electrolytes with high oxidation stability are crucial for achieving high power density allsolid-state lithium batteries.Halide electrolytes are promising candidates due to their outstanding compatibility with cathode materials and high Li^(+)conductivity.However,the electrochemical stability of chloride electrolytes is still limited,leaving them unsuitable for ultrahigh voltage operation.Besides,chemical compatibility issue between sulfide and halide electrolytes affects the electrochemical performance of all-solid-state batteries.Herein,Li-ion conductor Li_(3+x)InCl_(6-x)O_(x) is designed to address these challenges.Li_(3.25)InCl_(5.75)O_(0.25)shows a Li-ion conductivity of 0.90 mS cm^(-1)at room temperature,a high onset oxidation voltage of 3.84 V,fewer by-products at ultrahigh operation voltage,and good chemical compatibility with Li_(5.5)PS_(4.5)Cl_(1.5).The Li_(3.25)InCl_(5.75)O_(0.25)@LiNi_(0.7)Co_(0.1)Mn_(0.2)O_(2)-Li_(3.25)InCl_(5.75)O_(0.25)-VGCF/Li_(3.25)InCl_(5.75)O_(0.25)/Li_(5.5)PS_(4.5)Cl_(1.5)/Li-In battery delivers good electrochemical performances at high operating voltage.This work provides a simple,economical,and effective strategy for designing high-voltage all-solid-state electrolytes.
基金financially supported by the National Natural Science Foundation of China(Nos.52402271,22005167 and52302273)the Youth Innovation Team Project for Talent Introduction and Cultivation in Universities of Shandong Province(No.2024KJH129)+2 种基金the Taishan Scholar Project of Shandong Provinceof China(Nos.tsqn202211160,tsqn202312199)Shandong Provincial Natural Science Foundation of China(Nos.ZR2022QE003 and ZR2023QE176)China Postdoctoral Science Foundation(No.2023M741810)。
文摘Layered ammonium vanadate has become a promising cathode material for aqueous zinc ion batteries(ZIBs)due to its small mass and large ionic radius of ammonium ions as well as the consequent large layer spacing and high specific capacity.However,the irreversible de-ammoniation caused by N·H···O bonds damaged would impair cycle life of ZIBs and the strong electrostatic interaction between Zn^(2+)and V-O frame could slower the mobility of Zn^(2+).Furthermore,the thermal instability of ammonium vanadate also limits the use of common carbon coating modification method to solve the problem.Herein,V_(2)CT_(X)MXene was innovatively selected as a bifunctional source to in-situ derivatized(NH_(4))_(2)V_(8)O_(20)·x H_(2)O with amorphous carbon-coated(NHVO@C)via one-step hydrothermal method in relatively moderate temperature.The amorphous carbon shell derived from the V_(2)CT_(X)MXene as a conductive framework to effectively improve the diffusion kinetics of Zn^(2+)and the robust carbon skeleton could alleviate the ammonium dissolution during long-term cycling.As a result,zinc ion batteries using NHVO@C as cathode exhibit superior electrochemical performance.Moreover,the assembled foldable or high loading(10.2 mg/cm^(2))soft-packed ZIBs further demonstrates its practical application.This study provided new insights into the development of the carbon cladding process for thermally unstable materials in moderate temperatures.
基金financial support from the Chang Jiang Scholars Program (51073047)the National Natural Science Foundation of China (51773049)+5 种基金the China Aerospace Science and Technology Corporation-Harbin Institute of Technology Joint Center for Technology Innovation Fund (HIT15-1A01)the Harbin City Science and Technology Projects (2013DB4BP031 and RC2014QN017035)the Natural Science Foundation of Shandong Province of China (ZR2023QE071)the College Students’ Innovation and Entrepreneurship Training Program Projects of Shandong Province (S202211065048)the Scientific Research Foundation of Qingdao University (DC1900009425)the China Postdoctoral Science Foundation (2022TQ0282)
文摘Developing advanced battery-type materials with abundant active sites,high conductivity,versatile morphologies,and hierarchically porous structures is crucial for realizing high-quality hybrid supercapacitors.Herein,heterogeneous FeS@NiS is synthesized by cationic Co doping via surface-structure engineering.The density functional theory(DFT)theoretical calculations are firstly performed to predict the advantages of Co dopant by improving the OH^(−)adsorption properties and adjusting electronic structure,benefiting ions/electron transfer.The dynamic surface evolution is further explored which demonstrates that CoFeS@CoNiS could be quickly reconstructed to Ni(Co)Fe_(2)O_(4)during the charging process,while the unstable structure of the amorphous Ni(Co)Fe_(2)O_(4)results in partial conversion to Ni/Co/FeOOH at high potentials,which contributes to the more reactive active site and good structural stability.Thus,the free-standing electrode reveals excellent electrochemical performance with a superior capacity(335.6 mA h g^(−1),2684 F g^(−1))at 3 A g^(−1).Furthermore,the as-fabricated device shows a quality energy density of 78.1 W h kg^(−1)at a power density of 750 W kg^(−1)and excellent cycle life of 92.1%capacitance retention after 5000 cycles.This work offers a facile strategy to construct versatile morphological structures using electrochemical activation and holds promising applications in energy-related fields.
基金supported by the Development Project of Youth Innovation Team in Shandong Colleges and Universities(No.2019KJC031)the Natural Science Foundation of Shandong Province(Nos.ZR2019MB064,ZR2021MB122 and ZR2022MB137)the Doctoral Program of Liaocheng University(No.318051608).
文摘Pt-based materials are the benchmarked catalysts in the cathodic hydrogen evolution reaction(HER)of water splitting;the prohibitive cost and scarcity of Pt immensely impede the commercialization of hydrogen energy.Ru has aroused significant concern because of its Pt-like activity and much lower price.However,it’s still a top priority to minimize the Ru loading and pursue the most superior cost performance.
基金supported by the National Natural Science Foundation of China(Grant No.52202310)Natural Science Foundation of Jiangsu Province(Grant No.BK20191443)+7 种基金the Qinglan ProjectYouth Hundred Talents Programthe Toptalent Program of Yangzhou Universitythe Innovation technology platform project(YZ2020268)jointly built by Yangzhou City and Yangzhou UniversityPostgraduate Research&Practice Innovation Program of Jiangsu Province(SJCX22_1703)the Key Research and Development Projects of Sichuan Province(23ZDYF0466)“Tianfu Emei”Science and Technology Innovation Leader Program in Sichuan ProvinceUniversity of Electronic Science and Technology of China Talent Start-up Funds(A1098531023601208)。
文摘Molybdenum carbide(MO_(2)C)materials are promising electrocatalysts with potential applications in hydrogen evolution reaction(HER)due to low cost and Pt-like electronic structures.Nevertheless,their HER activity is usually hindered by the strong hydrogen binding energy.Moreover,the lack of water-cleaving site's makes it difficult for the catalysts to work in alkaline solutions.Here,we designed and synthesized a B and N dual-doped carbon layer that encapsulated on MO_(2)C nanocrystals(MO_(2)C@BNC)for accelerating HER under alkaline condition.The electronic interactions between the MO_(2)C nanocrystals and the multiple-doped carbon layer endow a near-zero H adsorption Gibbs free energy on the defective C atoms over the carbon shell.Meanwhile,the introduced B atoms afford optimal H_2O adsorption sites for the water-cleaving step.Accordingly,the dual-doped MO_(2)C catalyst with synergistic effect of non-metal sites delivers superior HER performances of a low overpotential(99 mV@10 mA cm^(-2))and a small Tafel slope(58.1 mV dec^(-1))in 1 M KOH solution.Furthermore,it presents a remarkable activity that outperforming the commercial 10%Pt/C catalyst at large current density,demonstrating its applicability in industrial water splitting.This study provides a reasonable design strategy towards noble-metal-free HER catalysts with high activity.
基金by the Research and Development Program in Key Areas of Guangdong Province(Grant No.2020B0202010008)Guangdong Province Science&Technology Program(2018B030306016)+1 种基金Guangdong Provincial Innovation Team for General Key Technologies in Modern Agricultural Industry(2019KJ133)Key Projects of Basic Research and Applied Basic Research of the Higher Education Institutions of Guangdong Province(2018KZDXM014).
文摘In this study,acrylic acid was used as a neutralizer to prepare bio-based WPU with an interpenetrating polymer network structure by thermally induced free radical emulsion polymerization.The effects of the content of acrylic acid on the properties of the resulting waterborne polyurethane-poly(acrylic acid)(WPU-PAA)dispersion and the films were systematically investigated.The results showed that the cross-linking density of the interpenetrating network polymers was increased and the interlocking structure of the soft and hard phase dislocations in the molecular segments of the double networks was tailored with increasing the content of acrylic acid,leading to enhancement of the mechanical properties and water resistance of WPU-PAA films.Notably,with the increase in content of acrylic acid,the tensile strength,Young’s modulus,and toughness of the WPU-PAA-110 film increased by 3 times,and 8 times,and 2.4 times compared with WPU-PAA-80,respectively.The WPU-PAA-100 film showed the best water resistance,and the water absorption rate at 96 h was only 3.27%.This work provided a new design scheme for constructing bio-based WPU materials with excellent properties.
基金supported by the National Natural Science Foundation of China (51672205, 21673169 and 51972257)the National Key R&D Program of China (2016YFA0202602)the Natural Science Foundation of Hubei Province (2018CFB581)
文摘TiNb2O7 anode materials(TNO)have unique potential for applications in Li-ion capacitors(LICs)due to their high specific capacity of ca.280 mA h g^-1 over a wide anodic Li-insertion potential window.However,their highrate capability is limited by their poor electronic and ionic conductivity.In particular,studies on TNO for LICs are lacking and that for flexible LICs have not yet been reported.Herein,a unique TNO porous electrode with cross-linked nanorods tailored by post-annealing and its application in flexible LICs are reported.This binder-free TNO anode exhibits superior rate performance(~66.3%capacity retention as the rate increases from 1 to 40 C),which is ascribed to the greatly shortened ion-diffusion length in TNO nanorods,facile electrolyte penetration and fast electron transport along the continuous single-crystalline nanorod network.Furthermore,the TNO anode shows an excellent cycling stability up to 2000 cycles and good flexibility(no capacity loss after continuous bending for 500 times).Model flexible LIC assembled with the TNO anode and activated carbon cathode exhibits increased gravimetric and volumetric energy/power densities(~100.6 W h kg^-1/4108.8 W kg^-1;10.7 mW h cm^-3/419.3 mW cm^-3),more superior to previously reported hybrid supercapacitors.The device also efficiently powers an LED light upon 180°bending.
基金The work supported by the National Key Research and Development Program of China(No.2018YFC0807600)Fundam ental Research Funds for the Central Universities(No.WK2320000035).
文摘Selenium sulfide(SeS2)cathodes have attracted much concern as an optimized choice comparing to sulfur and selenium for lithium and sodium storage.However,it also suffers from poor cycling stability due to the dissolution of reaction intermediate products.In this study,N-doped Interconnected carbon aerogels was applied as an efficient SeS2 host by infiltrating selenium sulfide into its microporous structure(denoted as SeS2@NCAs),which could effectively accommodate the volume change of SeS2 during cycling and alleviate the dissolution of reaction intermediate products.Therefore,as for Na storage,the SeS2@NCAs cathode delivers a superior long-term cycling performance of 536 mA·h·g^-1 at a current density of 0.5 A·g^-1 after 1,000 cycles with only 0.04%capacity decline per cycle and a high rate performance(524 mA·h·g^-1 at 2 A·g^-1 and 745 mA·h·g^-1 at 0.1 A·g^-1 retained),indicating the remarkable cycling stability of SeS2@NCAs cathodes.
基金supported by the National Key R&D Program of China(No.2021YFA1501101)the National Nature Science Foundation of China(Nos.21862011,21771156,and 51864024)+4 种基金Yunnan province(No.2019FI003)the Shenzhen Knowledge Innovation Program(Basic Research,No.JCYJ20190808181205752)the Research Grants Council(RGC)of the Hong Kong Special Administrative Region,China(Project No.CityU 11206520)the National Natural Science Foundation of China/RGC Joint Research Scheme(No.N_PolyU502/21)the funding for Projects of Strategic Importance of The Hong Kong Polytechnic University(Project Code:1-ZE2V).
文摘Iron-based nanostructures represent an emerging class of catalysts with high electroactivity for oxygen reduction reaction(ORR)in energy storage and conversion technologies.However,current practical applications have been limited by insufficient durability in both alkaline and acidic environments.In particular,limited attention has been paid to stabilizing iron-based catalysts by introducing additional metal by the alloying effect.Herein,we report bimetallic Fe_(2)Mo nanoparticles on N-doped carbon(Fe_(2)Mo/NC)as an efficient and ultra-stable ORR electrocatalyst for the first time.The Fe_(2)Mo/NC catalyst shows high selectivity for a four-electron pathway of ORR and remarkable electrocatalytic activity with high kinetics current density and half-wave potential as well as low Tafel slope in both acidic and alkaline medias.It demonstrates excellent long-term durability with no activity loss even after 10,000 potential cycles.Density functional theory(DFT)calculations have confirmed the modulated electronic structure of formed Fe_(2)Mo,which supports the electron-rich structure for the ORR process.Meanwhile,the mutual protection between Fe and Mo sites guarantees efficient electron transfer and long-term stability,especially under the alkaline environment.This work has supplied an effective strategy to solve the dilemma between high electroactivity and long-term durability for the Fe-based electrocatalysts,which opens a new direction of developing novel electrocatalyst systems for future research.
