Ovarian follicle development is associated with the physiological functions of granulosa cells(GCs),including proliferation and apoptosis.The level of miR-24-3p in ovarian tissue of high-yielding Yorkshire×Landra...Ovarian follicle development is associated with the physiological functions of granulosa cells(GCs),including proliferation and apoptosis.The level of miR-24-3p in ovarian tissue of high-yielding Yorkshire×Landrace sows was significantly higher than that of low-yielding sows.However,the functions of miR-24-3p on GCs are unclear.In this study,using flow cytometry,5-ethynyl-2′-de-oxyuridine(EdU)staining,and cell count,we showed that miR-24-3p promoted the proliferation of GCs increasing the proportion of cells in the S phase and upregulating the expression of cell cycle genes,moreover,miR-24-3p inhibited GC apoptosis.Mechanistically,on-line prediction,bioinformatics analysis,a luciferase reporter assay,RT-qPCR,and Western blot results showed that the target gene of miR-24-3p in proliferation and apoptosis is cyclin-dependent kinase inhibitor 1B(P27/CDKN1B).Furthermore,the effect of miR-24-3p on GC proliferation and apoptosis was attenuated by P27 overexpression.These findings suggest that miR-24-3p regulates the physiological functions of GCs.展开更多
Lithium-sulfur batteries with liquid electrolytes have been obstructed by severe shuttle effects and intrinsic safety concerns.Introducing inorganic solid-state electrolytes into lithium-sulfur systems is believed as ...Lithium-sulfur batteries with liquid electrolytes have been obstructed by severe shuttle effects and intrinsic safety concerns.Introducing inorganic solid-state electrolytes into lithium-sulfur systems is believed as an effective approach to eliminate these issues without sacrificing the high-energy density,which determines sulfidebased all-solid-state lithium-sulfur batteries.However,the lack of design principles for high-performance composite sulfur cathodes limits their further application.The sulfur cathode regulation should take several factors including the intrinsic insulation of sulfur,well-designed conductive networks,integrated sulfur-electrolyte interfaces,and porous structure for volume expansion,and the correlation between these factors into account.Here,we summarize the challenges of regulating composite sulfur cathodes with respect to ionic/electronic diffusions and put forward the corresponding solutions for obtaining stable positive electrodes.In the last section,we also outlook the future research pathways of architecture sulfur cathode to guide the develop high-performance all-solid-state lithium-sulfur batteries.展开更多
Li-metal batteries(LMBs)regain research prominence owing to the ever-increasing high-energy requirements.Commercially available carbonate electrolytes exhibit unfavourable parasitic reactions with Limetal anode(LMA),l...Li-metal batteries(LMBs)regain research prominence owing to the ever-increasing high-energy requirements.Commercially available carbonate electrolytes exhibit unfavourable parasitic reactions with Limetal anode(LMA),leading to the formation of unstable solid electrolyte interphase(SEI)and the breed of Li dendrites/dead Li.Significantly,lithium nitrate(LiNO_(3)),an excellent film-forming additive,proves crucial to construct a robust Li_(3)N/Li_(2)O/Li_(x)NO_(y)-rich SEI after combining with ether-based electrolytes.Thus,the given challenge leads to natural ideas which suggest the incorporation of LiNO_(3) into commercial carbonate for practical LMBs.Regrettably,LiNO_(3) demonstrates limited solubility(~800 ppm)in commercial carbonate electrolytes.Thence,developing stable SEI and dendrite-free LMA with the incorporation of LiNO_(3) into carbonate electrolytes is an efficacious strategy to realize robust LMBs via a scalable and cost-effective route.Therefore,this review unravels the grievances between LMA,LiNO_(3)and carbonate electrolytes,and enables a comprehensive analysis of LMA stabilizing mechanism with LiNO_(3),dissolution principle of LiNO_(3) in carbonate electrolytes,and LiNO_(3) introduction strategies.This review converges attention on a point that the LiNO_(3)-introduction into commercial carbonate electrolytes is an imperious choice to realize practical LMBs with commercial 4 V layered cathode.展开更多
It is challenging to efficiently and economically recycle many lithium-ion batteries(LIBs)because of the low valuation of commodity metals and materials,such as LiFePO_(4).There are millions of tons of spent LIBs wher...It is challenging to efficiently and economically recycle many lithium-ion batteries(LIBs)because of the low valuation of commodity metals and materials,such as LiFePO_(4).There are millions of tons of spent LIBs where the barrier to recycling is economical,and to make recycling more feasible,it is required that the value of the processed recycled material exceeds the value of raw commodity materials.The presented research illustrates improved profitability and economics for recycling spent LIBs by utilizing the surplus energy in lithiated graphite to drive the preparation of organolithiums to add value to the recycled lithium materials.This study methodology demonstrates that the surplus energy of lithiated graphite obtained from spent LIBs can be utilized to prepare high-value organolithiums,thereby significantly improving the economic profitability of LIB recycling.Organolithiums(R-O-Li and R-Li)were prepared using alkyl alcohol(R-OH)and alkyl bromide(R-Br)as substrates,where R includes varying hindered alkyl hydrocarbons.The organolithiums extracted from per kilogram of recycled LIBs can increase the economic value between$29.5 and$226.5 kg^(−1) cell.The value of the organolithiums is at least 5.4 times the total theoretical value of spent materials,improving the profitability of recycling LIBs over traditional pyrometallurgical($0.86 kg^(−1) cell),hydrometallurgical($1.00 kg^(−1) cell),and physical direct recycling methods($5.40 kg^(−1) cell).展开更多
The secretory activities of meibomian glands are regulated by the autonomic nervous system, The change in density and activity of autonomic nerves in meibomian glands during menopause play an important role in the pat...The secretory activities of meibomian glands are regulated by the autonomic nervous system, The change in density and activity of autonomic nerves in meibomian glands during menopause play an important role in the pathogenesis of dry eye. In view of this, we established a dry eye rat model by removing the bilateral ovaries. We used neuropeptide Y and vasoactive intestinal polypeptide as markers of autonomic neurotransmitters. Our results showed that the concentration of estradiol in serum significantly decreased, the density of neuropeptide Y immunoreactivity in nerve fibers significantly increased, the density of vasoactive intestinal polypeptide immunoreactivity in nerve fibers significantly decreased, and the ratio of vasoactive intestinal polypeptide/neuropeptide Y positive staining significantly decreased. These results suggest that a decrease in ovary activity may lead to autonomic nervous system dysfunction, thereby affecting the secretory activity of the meibomian gland, which participates in sexual hormone imbalance-induced dry eye.展开更多
Background:Oleic acid is an abundant free fatty acid present in livestock that are in a negative energy-balance state,and it may have detrimental effects on female reproduction and fertility.Oleic acid induces lipid a...Background:Oleic acid is an abundant free fatty acid present in livestock that are in a negative energy-balance state,and it may have detrimental effects on female reproduction and fertility.Oleic acid induces lipid accumulation in bovine granulosa cells,which leads to a foam cell-like morphology and reduced steroidogenesis.However,why oleic acid increases lipid accumulation but decreases steroidogenesis remains unclear.This study focused on oleic acid’s effects on lipid type and steroidogenesis.Results:Oleic acid increased the lipid accumulation in a concentration-dependent manner and mainly increased the triglyceride level and decreased the cholesterol ester level.Oleic acid also led to a decline in estradiol and progesterone production in porcine granulosa cells in vitro.In addition,oleic acid up-regulated the expression of CD36 and diacylglycerol acyltransferase 2,but down-regulated the expression of 3-hydroxy-3-methylglutarylcoenzyme A reductase,scavenger receptor class B member 1 and acetyl-Coenzyme A acetyltransferase 2,as well as steroidogenesis-related genes,including cytochrome P450 family 11 subfamily A member 1,cytochrome P450family 19 subfamily A member 1 and 3 as well as steroidogenic acute regulatory protein at the mRNA and protein levels.An oleic acid-rich diet also enhanced the triglyceride levels and reduced the cholesterol levels in ovarian tissues of female mice,which resulted in lower estradiol levels than in control-fed mice.Compared with the control,decreases in estrus days and the numbers of antral follicles and corpora lutea,as well as an increase in the numbers of the atretic follicles,were found in the oleic acid-fed female mice.Conclusions:Oleic acid changed the lipid type stored in lipid droplets of ovarian granulosa cells,and led to a decrease in steroidogenesis.These results improve our understanding of fertility decline in livestock that are in a negative energy-balance state.展开更多
The random step maneuver with uniformly distributed starting times has the disadvantage that it cannot focus the starting time on the more efficiency time. It decreases the penetration probability. To resolve this pro...The random step maneuver with uniformly distributed starting times has the disadvantage that it cannot focus the starting time on the more efficiency time. It decreases the penetration probability. To resolve this problem, a random step penetration algorithm with normal distribution starting time is proposed. Using the shaping filters and adjoint system method, the miss distance with different starting times can be acquired. According to the penetration standard, the time window ensuring successful penetration can be calculated and it is used as the 3σ bound of the normally distributed random maneuver. Simulation results indicate that the normally distributed random maneuver has higher penetration probability than the uniformly distributed random maneuver.展开更多
Iron-based electrodes have attracted great attention for sodium storage because of the distinct cost effectiveness.However,exploring suitable iron-based electrodes with high power density and long duration remains a b...Iron-based electrodes have attracted great attention for sodium storage because of the distinct cost effectiveness.However,exploring suitable iron-based electrodes with high power density and long duration remains a big challenge.Herein,a spray-drying strategy is adopted to construct graphene-coated Na_(2.4)Fe_(1.8)(SO_(4))_(3) nanograins in a 3D graphene microsphere network.The unique structural and compositional advantages endow these electrodes to exhibit outstanding electrochemical properties with remarkable rate performance and long cycle life.Mechanism analyses further explain the outstanding electrochemical properties from the structural aspect.展开更多
We consider maps on positive definite cones of von Neumann algebras preserving unitarily invariant norms of the spectral geometric means. The main results concern Jordan *-isomorphisms between <em>C</em>*-...We consider maps on positive definite cones of von Neumann algebras preserving unitarily invariant norms of the spectral geometric means. The main results concern Jordan *-isomorphisms between <em>C</em>*-algebras, and show that they are characterized by the preservation of unitarily invariant norms of those operations.展开更多
Perturbation problem of operator algebras was first introduced by Kadison and Kastler. In this short note, we consider the uniform perturbation of two classes of operator algebras, i.e., MF algebras and quasidiagonal ...Perturbation problem of operator algebras was first introduced by Kadison and Kastler. In this short note, we consider the uniform perturbation of two classes of operator algebras, i.e., MF algebras and quasidiagonal C*-algebras. We show that the sets of MF algebras and quasidiagonal C*-algebras of a given C*-algebra are closed under the perturbation of uniform norm.展开更多
Sodium(Na)ion batteries(SIBs)promise low-cost energy storage systems but are still restricted by insufficient energy density.Introducing oxygen(O)redox into the design of the Na-storage cathode is presently considered...Sodium(Na)ion batteries(SIBs)promise low-cost energy storage systems but are still restricted by insufficient energy density.Introducing oxygen(O)redox into the design of the Na-storage cathode is presently considered an effective avenue to generate extra capacity in solving the energy density bottleneck.The succeeding issues are how to overcome the irreversible electrochemical behavior accompanied by O release.Meanwhile,the O redox chemistry and subsequent structural evolution remain ambiguous so far.Here,we deliberate on the O redox mechanism in Na-storage transition metal oxides.Challenges associated with the reaction irreversibility and structural collapse are summarized by virtue of the advanced characterization techniques.Beyond that,strategies that potentially enhance the electrochemical properties of O redox and future research perspectives on exploring useable O redox cathode materials are outlined.展开更多
The Fe–N–C material is a promising non-noblemetal electrocatalyst for oxygen reduction reaction(ORR).Further improvement on the ORR activity is highly desired in order to replace Pt/C in acidic media.Herein,we devel...The Fe–N–C material is a promising non-noblemetal electrocatalyst for oxygen reduction reaction(ORR).Further improvement on the ORR activity is highly desired in order to replace Pt/C in acidic media.Herein,we developed a new-type of single-atom Fe–N–C electrocatalyst,in which Fe–Nxactive sites were modified by P atoms.The half-wave potential of the optimized material reached 0.858 V,which is 23 mV higher than that of the pristine one in a 0.1 mol L-1 HClO4 solution.Density functional theory(DFT)calculations revealed that P-doping can reduce the thermodynamic overpotential of the rate determining step and consequently improve the ORR activity.展开更多
Mass production of highly efficient,durable,and inexpensive single atomic catalysts is currently the major challenge associated with the oxygen reduction reaction(ORR)for fuel cells.In this study,we develop a general ...Mass production of highly efficient,durable,and inexpensive single atomic catalysts is currently the major challenge associated with the oxygen reduction reaction(ORR)for fuel cells.In this study,we develop a general strategy that uses a simple ultrasonic atomization coupling with pyrolysis and calcination process to synthesize single atomic FeNC catalysts(FeNC SACs)at large scale.The microstructure characterizations confirm that the active centers root in the single atomic Fe sites chelating to the four-fold pyridinic N atoms.The identified specific Fe active sites with the variable valence states facilitate the transfer of electrons,endowing the FeNC SACs with excellent electrochemical ORR activity.The FeNC SACs were used as cathode catalysts in a homemade Zn-air battery,giving an open-circuit voltage(OCV)of 1.43 V,which is substantially higher than that of commercial Pt/C catalysts.This study provides a simple approach to the synthesis of single atomic catalysts at large scale.展开更多
基金supported by the National Natural Science Foundation of China(32272849)the National Key R&D Program of China(2021YFF1000602)the earmarked fund for CARS-35-PIG。
文摘Ovarian follicle development is associated with the physiological functions of granulosa cells(GCs),including proliferation and apoptosis.The level of miR-24-3p in ovarian tissue of high-yielding Yorkshire×Landrace sows was significantly higher than that of low-yielding sows.However,the functions of miR-24-3p on GCs are unclear.In this study,using flow cytometry,5-ethynyl-2′-de-oxyuridine(EdU)staining,and cell count,we showed that miR-24-3p promoted the proliferation of GCs increasing the proportion of cells in the S phase and upregulating the expression of cell cycle genes,moreover,miR-24-3p inhibited GC apoptosis.Mechanistically,on-line prediction,bioinformatics analysis,a luciferase reporter assay,RT-qPCR,and Western blot results showed that the target gene of miR-24-3p in proliferation and apoptosis is cyclin-dependent kinase inhibitor 1B(P27/CDKN1B).Furthermore,the effect of miR-24-3p on GC proliferation and apoptosis was attenuated by P27 overexpression.These findings suggest that miR-24-3p regulates the physiological functions of GCs.
基金supported by the National Natural Science Foundation of China(No.52272241)the start-up funding from Zhejiang University。
文摘Lithium-sulfur batteries with liquid electrolytes have been obstructed by severe shuttle effects and intrinsic safety concerns.Introducing inorganic solid-state electrolytes into lithium-sulfur systems is believed as an effective approach to eliminate these issues without sacrificing the high-energy density,which determines sulfidebased all-solid-state lithium-sulfur batteries.However,the lack of design principles for high-performance composite sulfur cathodes limits their further application.The sulfur cathode regulation should take several factors including the intrinsic insulation of sulfur,well-designed conductive networks,integrated sulfur-electrolyte interfaces,and porous structure for volume expansion,and the correlation between these factors into account.Here,we summarize the challenges of regulating composite sulfur cathodes with respect to ionic/electronic diffusions and put forward the corresponding solutions for obtaining stable positive electrodes.In the last section,we also outlook the future research pathways of architecture sulfur cathode to guide the develop high-performance all-solid-state lithium-sulfur batteries.
基金the support by the Leading Innovative and Entrepreneur Team Introduction Program of Zhejiang(2019R01006)the National Natural Science Foundation of China(NSFC:12205252)+3 种基金A Project Supported by Scientific Research Fund of Zhejiang Provincial Education Department(Y202250795)the Research Funds of Institute of Zhejiang University-Quzhou,the Basic Public Welfare Research Special Project of Zhejiang Province(LZY22B040001)the Science and Technology Project of Quzhou Research Institute,Zhejiang University(IZQ2021KJ2032)the Independent Scientific Research Project of Quzhou Research Institute,Zhejiang University(IZQ2021RCZX007)。
文摘Li-metal batteries(LMBs)regain research prominence owing to the ever-increasing high-energy requirements.Commercially available carbonate electrolytes exhibit unfavourable parasitic reactions with Limetal anode(LMA),leading to the formation of unstable solid electrolyte interphase(SEI)and the breed of Li dendrites/dead Li.Significantly,lithium nitrate(LiNO_(3)),an excellent film-forming additive,proves crucial to construct a robust Li_(3)N/Li_(2)O/Li_(x)NO_(y)-rich SEI after combining with ether-based electrolytes.Thus,the given challenge leads to natural ideas which suggest the incorporation of LiNO_(3) into commercial carbonate for practical LMBs.Regrettably,LiNO_(3) demonstrates limited solubility(~800 ppm)in commercial carbonate electrolytes.Thence,developing stable SEI and dendrite-free LMA with the incorporation of LiNO_(3) into carbonate electrolytes is an efficacious strategy to realize robust LMBs via a scalable and cost-effective route.Therefore,this review unravels the grievances between LMA,LiNO_(3)and carbonate electrolytes,and enables a comprehensive analysis of LMA stabilizing mechanism with LiNO_(3),dissolution principle of LiNO_(3) in carbonate electrolytes,and LiNO_(3) introduction strategies.This review converges attention on a point that the LiNO_(3)-introduction into commercial carbonate electrolytes is an imperious choice to realize practical LMBs with commercial 4 V layered cathode.
基金National Natural Science Foundation of China,Grant/Award Number:51232005Key-Area Research and Development Program of Guangdong Province,Grant/Award Number:2020B090919003+1 种基金Joint Fund of the National Natural Science Foundation of China,Grant/Award Number:U1401243Shenzhen Technical Plan Project,Grant/Award Number:CYJ20170412170911187。
文摘It is challenging to efficiently and economically recycle many lithium-ion batteries(LIBs)because of the low valuation of commodity metals and materials,such as LiFePO_(4).There are millions of tons of spent LIBs where the barrier to recycling is economical,and to make recycling more feasible,it is required that the value of the processed recycled material exceeds the value of raw commodity materials.The presented research illustrates improved profitability and economics for recycling spent LIBs by utilizing the surplus energy in lithiated graphite to drive the preparation of organolithiums to add value to the recycled lithium materials.This study methodology demonstrates that the surplus energy of lithiated graphite obtained from spent LIBs can be utilized to prepare high-value organolithiums,thereby significantly improving the economic profitability of LIB recycling.Organolithiums(R-O-Li and R-Li)were prepared using alkyl alcohol(R-OH)and alkyl bromide(R-Br)as substrates,where R includes varying hindered alkyl hydrocarbons.The organolithiums extracted from per kilogram of recycled LIBs can increase the economic value between$29.5 and$226.5 kg^(−1) cell.The value of the organolithiums is at least 5.4 times the total theoretical value of spent materials,improving the profitability of recycling LIBs over traditional pyrometallurgical($0.86 kg^(−1) cell),hydrometallurgical($1.00 kg^(−1) cell),and physical direct recycling methods($5.40 kg^(−1) cell).
基金supported by the Key Technology Research & Development Program of Hebei Province,No.10276105D-3the Key Project of Hebei Province Health Department of Medical Science,No.20120154the Key Technology Research & Development Program of Hebei Province Handan City,No.1023108101-2
文摘The secretory activities of meibomian glands are regulated by the autonomic nervous system, The change in density and activity of autonomic nerves in meibomian glands during menopause play an important role in the pathogenesis of dry eye. In view of this, we established a dry eye rat model by removing the bilateral ovaries. We used neuropeptide Y and vasoactive intestinal polypeptide as markers of autonomic neurotransmitters. Our results showed that the concentration of estradiol in serum significantly decreased, the density of neuropeptide Y immunoreactivity in nerve fibers significantly increased, the density of vasoactive intestinal polypeptide immunoreactivity in nerve fibers significantly decreased, and the ratio of vasoactive intestinal polypeptide/neuropeptide Y positive staining significantly decreased. These results suggest that a decrease in ovary activity may lead to autonomic nervous system dysfunction, thereby affecting the secretory activity of the meibomian gland, which participates in sexual hormone imbalance-induced dry eye.
基金supported by grants from the National Natural Science Foundation(No.31802047)the National Science and Technology Major Project of China(No.2016ZX08006003)。
文摘Background:Oleic acid is an abundant free fatty acid present in livestock that are in a negative energy-balance state,and it may have detrimental effects on female reproduction and fertility.Oleic acid induces lipid accumulation in bovine granulosa cells,which leads to a foam cell-like morphology and reduced steroidogenesis.However,why oleic acid increases lipid accumulation but decreases steroidogenesis remains unclear.This study focused on oleic acid’s effects on lipid type and steroidogenesis.Results:Oleic acid increased the lipid accumulation in a concentration-dependent manner and mainly increased the triglyceride level and decreased the cholesterol ester level.Oleic acid also led to a decline in estradiol and progesterone production in porcine granulosa cells in vitro.In addition,oleic acid up-regulated the expression of CD36 and diacylglycerol acyltransferase 2,but down-regulated the expression of 3-hydroxy-3-methylglutarylcoenzyme A reductase,scavenger receptor class B member 1 and acetyl-Coenzyme A acetyltransferase 2,as well as steroidogenesis-related genes,including cytochrome P450 family 11 subfamily A member 1,cytochrome P450family 19 subfamily A member 1 and 3 as well as steroidogenic acute regulatory protein at the mRNA and protein levels.An oleic acid-rich diet also enhanced the triglyceride levels and reduced the cholesterol levels in ovarian tissues of female mice,which resulted in lower estradiol levels than in control-fed mice.Compared with the control,decreases in estrus days and the numbers of antral follicles and corpora lutea,as well as an increase in the numbers of the atretic follicles,were found in the oleic acid-fed female mice.Conclusions:Oleic acid changed the lipid type stored in lipid droplets of ovarian granulosa cells,and led to a decrease in steroidogenesis.These results improve our understanding of fertility decline in livestock that are in a negative energy-balance state.
文摘The random step maneuver with uniformly distributed starting times has the disadvantage that it cannot focus the starting time on the more efficiency time. It decreases the penetration probability. To resolve this problem, a random step penetration algorithm with normal distribution starting time is proposed. Using the shaping filters and adjoint system method, the miss distance with different starting times can be acquired. According to the penetration standard, the time window ensuring successful penetration can be calculated and it is used as the 3σ bound of the normally distributed random maneuver. Simulation results indicate that the normally distributed random maneuver has higher penetration probability than the uniformly distributed random maneuver.
基金financial support by the National Natural Science Foundation of China(Nos.21673165 and 21972108)National Key Research Program of China(No.2016YFB0901500)the supercomputing system in the Supercomputing Center of Wuhan University。
文摘Iron-based electrodes have attracted great attention for sodium storage because of the distinct cost effectiveness.However,exploring suitable iron-based electrodes with high power density and long duration remains a big challenge.Herein,a spray-drying strategy is adopted to construct graphene-coated Na_(2.4)Fe_(1.8)(SO_(4))_(3) nanograins in a 3D graphene microsphere network.The unique structural and compositional advantages endow these electrodes to exhibit outstanding electrochemical properties with remarkable rate performance and long cycle life.Mechanism analyses further explain the outstanding electrochemical properties from the structural aspect.
文摘We consider maps on positive definite cones of von Neumann algebras preserving unitarily invariant norms of the spectral geometric means. The main results concern Jordan *-isomorphisms between <em>C</em>*-algebras, and show that they are characterized by the preservation of unitarily invariant norms of those operations.
文摘Perturbation problem of operator algebras was first introduced by Kadison and Kastler. In this short note, we consider the uniform perturbation of two classes of operator algebras, i.e., MF algebras and quasidiagonal C*-algebras. We show that the sets of MF algebras and quasidiagonal C*-algebras of a given C*-algebra are closed under the perturbation of uniform norm.
基金National Natural Science Foundation of China,Grant/Award Numbers:52002352,52071295。
文摘Sodium(Na)ion batteries(SIBs)promise low-cost energy storage systems but are still restricted by insufficient energy density.Introducing oxygen(O)redox into the design of the Na-storage cathode is presently considered an effective avenue to generate extra capacity in solving the energy density bottleneck.The succeeding issues are how to overcome the irreversible electrochemical behavior accompanied by O release.Meanwhile,the O redox chemistry and subsequent structural evolution remain ambiguous so far.Here,we deliberate on the O redox mechanism in Na-storage transition metal oxides.Challenges associated with the reaction irreversibility and structural collapse are summarized by virtue of the advanced characterization techniques.Beyond that,strategies that potentially enhance the electrochemical properties of O redox and future research perspectives on exploring useable O redox cathode materials are outlined.
基金This work was supported by the National Key R&D Program of China(2017YFB0102900)the Research Grant Council(N一HKUST610/17)of Hong Kong Special Administrative Region.It used resources of the Advanced Photon Source,Office of Science user facilities,supported by the U.S.Department of Energy,Office of Science,Office of Basic Energy Sciences(DE-AC02-06CH11357).
文摘The Fe–N–C material is a promising non-noblemetal electrocatalyst for oxygen reduction reaction(ORR).Further improvement on the ORR activity is highly desired in order to replace Pt/C in acidic media.Herein,we developed a new-type of single-atom Fe–N–C electrocatalyst,in which Fe–Nxactive sites were modified by P atoms.The half-wave potential of the optimized material reached 0.858 V,which is 23 mV higher than that of the pristine one in a 0.1 mol L-1 HClO4 solution.Density functional theory(DFT)calculations revealed that P-doping can reduce the thermodynamic overpotential of the rate determining step and consequently improve the ORR activity.
基金the National Natural Science Foundation of China(NSFC,51971029)the NSFC-BRICS STI Framework Program(51861145309)+4 种基金the National S&T Major Project(2018ZX10301201)the Joint Research Project of University of Science and Technology Beijing&Taipei University of Technology(TW2018007)the“1125”Zhihui Zhengzhou Talent Project of Henan Province(39080070)the Fundamental Research Funds for the Central Universities(FRF-BR-15-027A)the fund supports from the“100 talent plan”fund of Fujian province(Contract No:2017-802)。
文摘Mass production of highly efficient,durable,and inexpensive single atomic catalysts is currently the major challenge associated with the oxygen reduction reaction(ORR)for fuel cells.In this study,we develop a general strategy that uses a simple ultrasonic atomization coupling with pyrolysis and calcination process to synthesize single atomic FeNC catalysts(FeNC SACs)at large scale.The microstructure characterizations confirm that the active centers root in the single atomic Fe sites chelating to the four-fold pyridinic N atoms.The identified specific Fe active sites with the variable valence states facilitate the transfer of electrons,endowing the FeNC SACs with excellent electrochemical ORR activity.The FeNC SACs were used as cathode catalysts in a homemade Zn-air battery,giving an open-circuit voltage(OCV)of 1.43 V,which is substantially higher than that of commercial Pt/C catalysts.This study provides a simple approach to the synthesis of single atomic catalysts at large scale.