To obtain intrinsic overcharge boundary and investigate overcharge mechanism,here we propose an innovative method,the step overcharge test,to reduce the thermal crossover and distinguish the overcharge thermal behavio...To obtain intrinsic overcharge boundary and investigate overcharge mechanism,here we propose an innovative method,the step overcharge test,to reduce the thermal crossover and distinguish the overcharge thermal behavior,including 5%state of charge(SOC)with small current overcharge and resting until the temperature equilibrium under adiabatic conditions.The intrinsic thermal response and the self-excitation behaviour are analysed through temperature and voltage changes during the step overcharge period.Experimental results show that the deintercalated state of the cathode is highly correlated to self-heating parasitic reactions.Before reaching the upper limit of Negative/Positive(N/P)ratio,the temperature changes little,the heat generation is significantly induced by the reversible heat(endothermic)and ohmic heat,which could balance each other.Following that the lithium metal is gradually deposited on the surface of the anode and reacts with electrolyte upon overcharge,inducing selfheating side reaction.However,this spontaneous thermal reaction could be“self-extinguished”.When the lithium in cathode is completely deintercalated,the boundary point of overcharge is about 4.7 V(~148%SOC,>40℃),and from this point,the self-heating behaviour could be continuously triggered until thermal runaway(TR)without additional overcharge.The whole static and spontaneous process lasts for 115 h and the side reaction heat is beyond 320,000 J.The continuous self-excitation behavior inside the battery is attributed to the interaction between the highly oxidized cathode and the solvent,which leads to the dissolution of metal ions.The dissolved metal ions destroy the SEI(solid electrolyte interphase)film on the surface of the deposited Li of anode,which induces the thermal reaction between lithium metal and the solvent.The interaction between cathode,the deposited Li of anode,and solvent promotes the temperature of the battery to rise slowly.When the temperature of the battery reaches more than 60℃,the reaction between lithium metal and solvent is accelerated.After the temperature rises rapidly to the melting point of the separator,it triggers the thermal runaway of the battery due to the short circuit of the battery.展开更多
The pathophysiology of osteoarthritis(OA)is multifactorial,with the primary risk factors being obesity,age,environmental variables,and genetic predisposition.The available evidence suggests that genetic diversity does...The pathophysiology of osteoarthritis(OA)is multifactorial,with the primary risk factors being obesity,age,environmental variables,and genetic predisposition.The available evidence suggests that genetic diversity does not adequately account for all clinical characteristics and heterogeneity of OA.Genetics has emerged as a nascent and crucial area of research in OA.The epigenetic module presents a potential link between genetic and environmental risk factors and the susceptibility and pathogenesis of OA.As a critical epigenetic alteration,DNA methylation has been shown to have an important role in the etiology of OA and is a viable biomarker for predicting disease progression and medication response,as shown in this research.This review aims to update knowledge in the field of DNA methylation associated with OA to better identify the essential features of OA subtypes and pathological conditions,hence accelerating individualized treatment and precision medicine.展开更多
In this study,a detailed analysis of the combustion behaviors of the lithium iron phosphate(LFP)and lithium manganese oxide(LMO)batteries used in electric bicycles was conducted.This research included quantitative mea...In this study,a detailed analysis of the combustion behaviors of the lithium iron phosphate(LFP)and lithium manganese oxide(LMO)batteries used in electric bicycles was conducted.This research included quantitative measurements of the combustion duration,flame height,combustion temperature,heat release rate,and total heat release.The results indicated that LMO batteries exhibited higher combustion temperatures of 600–700°C,flame heights of 70–75 cm,a significantly higher heat release rate of40.1 k W(12 Ah),and a total heat release of 1.04 MJ(12 Ah)compared to LFP batteries with the same capacity.Based on these experimental results,a normalized total heat release(NORTHR)parameter was proposed,demonstrating good universality for batteries with different capacities.Utilizing this parameter,quantitative calculations and optimization of the extinguishing agent dosage were conducted for fires involving these two types of batteries,and the method was validated by extinguishing fires for these two types of battery packs with water-based extinguishing fluids.展开更多
Nitrogen reduction reaction(NRR)under ambient conditions is always a long-standing challenge in science,due to the extreme difficulty in breaking the strong N≡N triple bond.The key to resolving this issue undoubtedly...Nitrogen reduction reaction(NRR)under ambient conditions is always a long-standing challenge in science,due to the extreme difficulty in breaking the strong N≡N triple bond.The key to resolving this issue undoubtedly lies in searching superior catalysts to efficiently activate and hydrogenate the stable nitrogen molecules.We herein evaluate the feasibility of WP_(2) for N2 activation and reduction,and first demonstrate WP_(2) with an impressive ammonia yield rate of 7.13 lg h^(-1)cm^(-2),representing a promising W-based catalyst for NRR.DFT analysis further reveals that the NRR catalysis on WP_(2) proceeds in a distal reaction pathway,and the exceptional NRR activity is originated from superior surface electron energy level matching between WP_(2) and NRR potential which facilitates the interfacial proton-coupled electron transfer dynamics.The successfully unraveling the intrinsic catalytic mechanism of WP_(2) for NRR could offer a powerful platform to manipulate the NRR activity by tuning the electron energy levels.展开更多
On the basis of data mining,systematic pharmacology,molecular docking,and experiment validation,the oxidative-inflammatory molecular targets of Coicis Semen in the therapy of osteoarthritis(OA)were explored.Methods:Th...On the basis of data mining,systematic pharmacology,molecular docking,and experiment validation,the oxidative-inflammatory molecular targets of Coicis Semen in the therapy of osteoarthritis(OA)were explored.Methods:The association rule analysis was effectively applied to highlight the correlation between Coicis Semen and oxidative inflammation indices.The random walk model was subsequently used to evaluate the clinical efficacy of Coicis Semen.Network pharmacology was used to predict network targets.The binding affinity of the active ingredient in Coicis Semen to the key target of OA was also successfully predicted.Results:Coicis Semen showed a significant reduction in oxidative-inflammatory indicators of OA.A total of 108 promising targets were predicted for the 24 bioactive compounds in Coicis Semen.Eight target genes were considered core target genes.The enrichment analysis predicts that Coicis Semen may activate the interleukin(IL)-17,mitogen-activated protein kinase(MAPK),and nuclear factor kappa B(NF-kappa B)signaling pathways.Molecular docking demonstrated that stigmasterol,2-monoolein,sitosterol,and sitosterol alpha1 had free binding energies to oxidative and inflammatory targets(MAPK1,Estrogen Receptor 1[ESR1],and Peroxisome Proliferator-Activated Receptor Alpha[PPARA]).Both clinical trials and in vitro cell experiments revealed that Coicis Semen could increase ESR1 and PPAR-αlevels while decreasing MAPK1 levels.Conclusions:Coicis Semen has a remarkable anti-OA effect.Precisely,the major components of Coicis Semen,including stigmasterol,sitosterol alpha1,sitosterol,and 2-monoolein,specifically inhibit MAPK1,ESR1,and PPARA to reduce the inflammatory response and oxidative damage in OA.展开更多
Interfacial H_(2)release severely limits the reversibility and feasibility of aqueous Zn metal batteries for large-scale energy storage.Different from the conventional perception that H_(2)release mainly originates fr...Interfacial H_(2)release severely limits the reversibility and feasibility of aqueous Zn metal batteries for large-scale energy storage.Different from the conventional perception that H_(2)release mainly originates from the competition between hydrogen evolution reaction and Zn plating process,we herein surprisingly find that non-negligible H_(2)is also generated during stripping due to the accelerated chemical corrosion of the newly exposed Zn surface.To address this issue,we systematically screened the organic additives with different molecular structures and functional groups.Interestingly,a positive correlation between the adsorption strength of additives and the ability to inhibit the interfacial hydrogen release is found.Taking cysteamine(MEA)as a model additive,a gradient solid electrolyte interphase(SEI)is in situ formed at the Zn surface,acting as a chemical“barrier”to isolate interfacial water molecules from electrode surface consequently enable a higher Coulombic efficiency(>99.5%,4000 cycles)compared with that of MEA-free electrolyte(98.1%,189 cycles).This work provides a new understanding of the interfacial hydrogen release mechanism and the criteria for selecting additives for aqueous Zn metal anodes.展开更多
The high unoccupied d band energy of Ni_(3)N basically results in weak orbital coupling with water molecule,consequently leading to slow water dissociation kinetics.Herein,we demonstrate Cr doping can downshift the un...The high unoccupied d band energy of Ni_(3)N basically results in weak orbital coupling with water molecule,consequently leading to slow water dissociation kinetics.Herein,we demonstrate Cr doping can downshift the unoccupied d orbitals and strengthen the interfacial orbital coupling to boost the water dissociation kinetics.The prepared Cr-Ni_(3)N/Ni displays an impressive overpotential of 37 mV at 10 mA·cmgeo-2,close to the benchmark Pt/C in 1.0 M KOH solution.Refined structural analysis reveals the Cr dopant exists as the Cr-N_(6)states and the average d band energy of Ni_(3)N is also lowered.Density functional theory calculation further confirms the downshifted d band energy can strengthen the orbital coupling between the unpaired electrons in O 2p and the unoccupied state of Ni 3d,which thus facilitates the water adsorption and dissociation.The work provides a new concept to achieve on-demand functions for hydrogen evolution catalysis and beyond,by regulating the interfacial orbital coupling.展开更多
The interstitial structure and weak Ni-N interaction of Ni3N lead to high unoccupied d orbital energy and unsuitable orbital orientation,which consequently results in weak orbital coupling with H2O and slow water diss...The interstitial structure and weak Ni-N interaction of Ni3N lead to high unoccupied d orbital energy and unsuitable orbital orientation,which consequently results in weak orbital coupling with H2O and slow water dissociation kinetics for alkaline hydrogen evolution catalysis.Herein,we successfully lower the unoccupied d orbital energy of Ni3N to strengthen the interfacial electronic coupling by employing the strong electron pulling capability of oxygen dopants.The prepared O-Ni3N catalyst delivers an overpotential of 55 mV at 10 mA cm−2,very close to the commercial Pt/C.Refined structural characterization indicates the oxygen incorporation can decrease the electron densities around the Ni sites.Moreover,density functional theory calculation further proves the oxygen incorporation can create more unoccupied orbitals with lower energy and superior orientation for water adsorption and dissociation.The concept of orbital-regulated interfacial electronic coupling could offer a unique approach for the rational design of hydrogen evolution catalysts and beyond.展开更多
With the gradual reduction of fossil fuel and the growing environmental concerns over the climate change associated with the use of fossil fuel,renewable energy sources such as solar,wind,biomass,geothermal and hydroe...With the gradual reduction of fossil fuel and the growing environmental concerns over the climate change associated with the use of fossil fuel,renewable energy sources such as solar,wind,biomass,geothermal and hydroelectric are becoming increasingly important.In particular,solar power generation has emerged as the most rapidly growing renewable source.As a result,solar cells of different types have been intensively studied.展开更多
基金funded by the National Key Research and Development Program of China(2018YFB0104400)supported by the Beijing Natural Science Foundation(2214066)。
文摘To obtain intrinsic overcharge boundary and investigate overcharge mechanism,here we propose an innovative method,the step overcharge test,to reduce the thermal crossover and distinguish the overcharge thermal behavior,including 5%state of charge(SOC)with small current overcharge and resting until the temperature equilibrium under adiabatic conditions.The intrinsic thermal response and the self-excitation behaviour are analysed through temperature and voltage changes during the step overcharge period.Experimental results show that the deintercalated state of the cathode is highly correlated to self-heating parasitic reactions.Before reaching the upper limit of Negative/Positive(N/P)ratio,the temperature changes little,the heat generation is significantly induced by the reversible heat(endothermic)and ohmic heat,which could balance each other.Following that the lithium metal is gradually deposited on the surface of the anode and reacts with electrolyte upon overcharge,inducing selfheating side reaction.However,this spontaneous thermal reaction could be“self-extinguished”.When the lithium in cathode is completely deintercalated,the boundary point of overcharge is about 4.7 V(~148%SOC,>40℃),and from this point,the self-heating behaviour could be continuously triggered until thermal runaway(TR)without additional overcharge.The whole static and spontaneous process lasts for 115 h and the side reaction heat is beyond 320,000 J.The continuous self-excitation behavior inside the battery is attributed to the interaction between the highly oxidized cathode and the solvent,which leads to the dissolution of metal ions.The dissolved metal ions destroy the SEI(solid electrolyte interphase)film on the surface of the deposited Li of anode,which induces the thermal reaction between lithium metal and the solvent.The interaction between cathode,the deposited Li of anode,and solvent promotes the temperature of the battery to rise slowly.When the temperature of the battery reaches more than 60℃,the reaction between lithium metal and solvent is accelerated.After the temperature rises rapidly to the melting point of the separator,it triggers the thermal runaway of the battery due to the short circuit of the battery.
基金supported by the Anhui Famous Traditional Chinese Medicine Liu Jian Studio Construction Project(Traditional Chinese Medicine Development Secret[2018]No.11)the Ministry of Science and Technology National Key Research and Development Program Chinese Medicine Modernization Research Key Project(No.2018YFC1705204)+1 种基金Anhui Province Traditional Chinese Medicine Leading Talent Project(Traditional Chinese Medicine Development Secret[2018]No.23)the Anhui Key Research and Development Program Foreign Science and Technology Cooperation Project(No.201904b11020011).
文摘The pathophysiology of osteoarthritis(OA)is multifactorial,with the primary risk factors being obesity,age,environmental variables,and genetic predisposition.The available evidence suggests that genetic diversity does not adequately account for all clinical characteristics and heterogeneity of OA.Genetics has emerged as a nascent and crucial area of research in OA.The epigenetic module presents a potential link between genetic and environmental risk factors and the susceptibility and pathogenesis of OA.As a critical epigenetic alteration,DNA methylation has been shown to have an important role in the etiology of OA and is a viable biomarker for predicting disease progression and medication response,as shown in this research.This review aims to update knowledge in the field of DNA methylation associated with OA to better identify the essential features of OA subtypes and pathological conditions,hence accelerating individualized treatment and precision medicine.
基金supported by the New Energy Vehicle Power Battery Life Cycle Testing and Verification Public Service Platform Project[2022-235-224]the Beijing Science and Technology Planning Project[Z221100005222004]+1 种基金the Key Technologies Research and Development Program[2021YFB2012504]the Beijing Goldenbridge Project[ZZ2023002]。
文摘In this study,a detailed analysis of the combustion behaviors of the lithium iron phosphate(LFP)and lithium manganese oxide(LMO)batteries used in electric bicycles was conducted.This research included quantitative measurements of the combustion duration,flame height,combustion temperature,heat release rate,and total heat release.The results indicated that LMO batteries exhibited higher combustion temperatures of 600–700°C,flame heights of 70–75 cm,a significantly higher heat release rate of40.1 k W(12 Ah),and a total heat release of 1.04 MJ(12 Ah)compared to LFP batteries with the same capacity.Based on these experimental results,a normalized total heat release(NORTHR)parameter was proposed,demonstrating good universality for batteries with different capacities.Utilizing this parameter,quantitative calculations and optimization of the extinguishing agent dosage were conducted for fires involving these two types of batteries,and the method was validated by extinguishing fires for these two types of battery packs with water-based extinguishing fluids.
基金financial support from the National Natural Science Foundation of China(Nos.21771169,11804325,11722543,11875258,11505187)the National Key Research and Development Program of China(2017YFA0206703)+3 种基金Anhui Provincial Natural Science Foundation(BJ2060190077)USTC start-up fundingRecruitment Program of Global Expertthe Fundamental Research Funds for the Central Universities(WK2060190074,WK2060190081,WK2310000066)。
文摘Nitrogen reduction reaction(NRR)under ambient conditions is always a long-standing challenge in science,due to the extreme difficulty in breaking the strong N≡N triple bond.The key to resolving this issue undoubtedly lies in searching superior catalysts to efficiently activate and hydrogenate the stable nitrogen molecules.We herein evaluate the feasibility of WP_(2) for N2 activation and reduction,and first demonstrate WP_(2) with an impressive ammonia yield rate of 7.13 lg h^(-1)cm^(-2),representing a promising W-based catalyst for NRR.DFT analysis further reveals that the NRR catalysis on WP_(2) proceeds in a distal reaction pathway,and the exceptional NRR activity is originated from superior surface electron energy level matching between WP_(2) and NRR potential which facilitates the interfacial proton-coupled electron transfer dynamics.The successfully unraveling the intrinsic catalytic mechanism of WP_(2) for NRR could offer a powerful platform to manipulate the NRR activity by tuning the electron energy levels.
基金supported by the Anhui Famous Traditional Chinese Medicine Liu Jian Studio Construction Project(Traditional Chinese Medicine Development Secret[2018]No.11)the Ministry of Science and Technology National Key Research and Development Program Chinese Medicine Modernization Research Key Project(No.2018YFC1705204)+2 种基金Anhui Province Traditional Chinese Medicine Leading Talent Project(Traditional Chinese Medicine Development Secret[2018]No.23)the Anhui key Research and Development Program Foreign Science and Technology Cooperation Project(No.201904b11020011)the Anhui Provincial Education Department Project(No.2022AH050449).
文摘On the basis of data mining,systematic pharmacology,molecular docking,and experiment validation,the oxidative-inflammatory molecular targets of Coicis Semen in the therapy of osteoarthritis(OA)were explored.Methods:The association rule analysis was effectively applied to highlight the correlation between Coicis Semen and oxidative inflammation indices.The random walk model was subsequently used to evaluate the clinical efficacy of Coicis Semen.Network pharmacology was used to predict network targets.The binding affinity of the active ingredient in Coicis Semen to the key target of OA was also successfully predicted.Results:Coicis Semen showed a significant reduction in oxidative-inflammatory indicators of OA.A total of 108 promising targets were predicted for the 24 bioactive compounds in Coicis Semen.Eight target genes were considered core target genes.The enrichment analysis predicts that Coicis Semen may activate the interleukin(IL)-17,mitogen-activated protein kinase(MAPK),and nuclear factor kappa B(NF-kappa B)signaling pathways.Molecular docking demonstrated that stigmasterol,2-monoolein,sitosterol,and sitosterol alpha1 had free binding energies to oxidative and inflammatory targets(MAPK1,Estrogen Receptor 1[ESR1],and Peroxisome Proliferator-Activated Receptor Alpha[PPARA]).Both clinical trials and in vitro cell experiments revealed that Coicis Semen could increase ESR1 and PPAR-αlevels while decreasing MAPK1 levels.Conclusions:Coicis Semen has a remarkable anti-OA effect.Precisely,the major components of Coicis Semen,including stigmasterol,sitosterol alpha1,sitosterol,and 2-monoolein,specifically inhibit MAPK1,ESR1,and PPARA to reduce the inflammatory response and oxidative damage in OA.
基金support by the Fundamental Research Funds for the National Natural Science Foundation of China(22379135)the Fundamental Research Funds for the Central Universities(WK2060000016)the Collaborative Innovation program of Hefei Science Center,CAS.
文摘Interfacial H_(2)release severely limits the reversibility and feasibility of aqueous Zn metal batteries for large-scale energy storage.Different from the conventional perception that H_(2)release mainly originates from the competition between hydrogen evolution reaction and Zn plating process,we herein surprisingly find that non-negligible H_(2)is also generated during stripping due to the accelerated chemical corrosion of the newly exposed Zn surface.To address this issue,we systematically screened the organic additives with different molecular structures and functional groups.Interestingly,a positive correlation between the adsorption strength of additives and the ability to inhibit the interfacial hydrogen release is found.Taking cysteamine(MEA)as a model additive,a gradient solid electrolyte interphase(SEI)is in situ formed at the Zn surface,acting as a chemical“barrier”to isolate interfacial water molecules from electrode surface consequently enable a higher Coulombic efficiency(>99.5%,4000 cycles)compared with that of MEA-free electrolyte(98.1%,189 cycles).This work provides a new understanding of the interfacial hydrogen release mechanism and the criteria for selecting additives for aqueous Zn metal anodes.
基金The work was supported by the National Natural Science Foundation of China(Nos.21771169 and 11722543)the National Key Research and Development Program of China(No.2017YFA0206703)+1 种基金Anhui Provincial Natural Science Foundation(No.BJ2060190077)Collaborative Innovation Program of Hefei Science Center,CAS,and the Fundamental Research Funds for the Central Universities(Nos.WK2060190074,WK2060190081,WK2310000066,and WK2060000015).
文摘The high unoccupied d band energy of Ni_(3)N basically results in weak orbital coupling with water molecule,consequently leading to slow water dissociation kinetics.Herein,we demonstrate Cr doping can downshift the unoccupied d orbitals and strengthen the interfacial orbital coupling to boost the water dissociation kinetics.The prepared Cr-Ni_(3)N/Ni displays an impressive overpotential of 37 mV at 10 mA·cmgeo-2,close to the benchmark Pt/C in 1.0 M KOH solution.Refined structural analysis reveals the Cr dopant exists as the Cr-N_(6)states and the average d band energy of Ni_(3)N is also lowered.Density functional theory calculation further confirms the downshifted d band energy can strengthen the orbital coupling between the unpaired electrons in O 2p and the unoccupied state of Ni 3d,which thus facilitates the water adsorption and dissociation.The work provides a new concept to achieve on-demand functions for hydrogen evolution catalysis and beyond,by regulating the interfacial orbital coupling.
基金This work was supported by the National Natural Science Foundation of China(21771169,51801075,11722543)the National Key Research and Development Program of China(2017YFA0206703)+1 种基金Anhui Provincial Natural Science Foundation(BJ2060190077)Recruitment Program of Global Expert,and the Fundamental Research Funds for the Central Universities(WK2060190074,WK2060190081,WK2310000066).
文摘The interstitial structure and weak Ni-N interaction of Ni3N lead to high unoccupied d orbital energy and unsuitable orbital orientation,which consequently results in weak orbital coupling with H2O and slow water dissociation kinetics for alkaline hydrogen evolution catalysis.Herein,we successfully lower the unoccupied d orbital energy of Ni3N to strengthen the interfacial electronic coupling by employing the strong electron pulling capability of oxygen dopants.The prepared O-Ni3N catalyst delivers an overpotential of 55 mV at 10 mA cm−2,very close to the commercial Pt/C.Refined structural characterization indicates the oxygen incorporation can decrease the electron densities around the Ni sites.Moreover,density functional theory calculation further proves the oxygen incorporation can create more unoccupied orbitals with lower energy and superior orientation for water adsorption and dissociation.The concept of orbital-regulated interfacial electronic coupling could offer a unique approach for the rational design of hydrogen evolution catalysts and beyond.
文摘With the gradual reduction of fossil fuel and the growing environmental concerns over the climate change associated with the use of fossil fuel,renewable energy sources such as solar,wind,biomass,geothermal and hydroelectric are becoming increasingly important.In particular,solar power generation has emerged as the most rapidly growing renewable source.As a result,solar cells of different types have been intensively studied.
