With the continuing boost in the demand for energy storage,there is an increasing requirement for batteries to be capable of operation in extreme environmental conditions.Sodium-ion batteries(SIBs) have emerged as a h...With the continuing boost in the demand for energy storage,there is an increasing requirement for batteries to be capable of operation in extreme environmental conditions.Sodium-ion batteries(SIBs) have emerged as a highly promising energy storage solution due to their promising performance over a wide range of temperatures and the abundance of sodium resources in the earth's crust.Compared to lithiumion batteries(LIBs),although sodium ions possess a larger ionic radius,they are more easily desolvated than lithium ions.Fu rthermore,SIBs have a smaller Stokes radius than lithium ions,resulting in improved sodium-ion mobility in the electrolyte.Nevertheless,SIBs demonstrate a significant decrease in performance at low temperatures(LT),which constrains their operation in harsh weather conditions.Despite the increasing interest in SIBs,there is a notable scarcity of research focusing specifically on their mechanism under LT conditions.This review explores recent research that considers the thermal tolerance of SIBs from an inner chemistry process perspective,spanning a wide temperature spectrum(-70 to100℃),particularly at LT conditions.In addition,the enhancement of electrochemical performance in LT SIBs is based on improvements in reaction kinetics and cycling stability achieved through the utilization of effective electrode materials and electrolyte components.Furthermore,the safety concerns associated with SIBs are addressed and effective strategies are proposed for mitigating these issues.Finally,prospects conducted to extend the environmental frontiers of commercial SIBs are discussed mainly from three viewpoints including innovations in materials,development and research of relevant theoretical mechanisms,and intelligent safety management system establishment for larger-scale energy storage SIBs.展开更多
A lead-free base glaze suitable for pearlescent pigments was prepared by a low-temperature solid-phase reaction with alkali waste.Tests were performed to evaluate the effects of the sintering conditions and alkali was...A lead-free base glaze suitable for pearlescent pigments was prepared by a low-temperature solid-phase reaction with alkali waste.Tests were performed to evaluate the effects of the sintering conditions and alkali waste composition on the prepared base glaze and pearlescent glaze.The experimental results show that partially replacing SiO_(2) with B_(2)O_(3) effectively reduced the sintering temperature and time to form a glass network,but the network structure becomes disconnected as the B_(2)O_(3) content increases.An amorphous base glaze was obtained when soda ash was replaced with a small amount of alkali waste,but increasing the addition of NaCl further was adverse to base glaze formation by resulting in crystallization of the base glaze and a decrease in the bridging oxygen content.The pearlescent pigment was thermally stable in the glaze at 750℃,while higher temperatures caused the crystalline phase of NaAlSiO_(4) to appear and adhere to the surface of pigment granules,which degraded the pearlescent effect of the glaze.展开更多
The cognition of active sites in the Ni-based catalysts plays a vital role and remains a huge challenge in improving catalytic performance of low temperature CO_(2) dry reforming of methane(LTDRM).In this work,typical...The cognition of active sites in the Ni-based catalysts plays a vital role and remains a huge challenge in improving catalytic performance of low temperature CO_(2) dry reforming of methane(LTDRM).In this work,typical catalysts of SiO_(2) and γ-Al_(2)O_(3) supported Ni and Ni-Ce were designed and prepared.Importantly,the difference in the chemical speciations of active sites on the Ni-based catalysts is revealed by advanced characterizations and further estimates respective catalytic performance for LTDRM.Results show that larger[Ni0-]particles mixed with[Ni-O-Sin])species on the Ni/SiO_(2)(R)make CH_(4) excessive decomposition,leading to poor activity and stability.Once the Ce species is doped,however,superior activity(59.0%CH_(4) and 59.8%CO_(2) conversions),stability and high H_(2)/CO ratio(0.96)at 600℃ can be achieved on the Ni-Ce/SiO_(2)(R),in comparison with other catalysts and even reported studies.The improved performance can be ascribed to the formation of integral([Ni0_(n))]-[CeⅢ-□-CeⅢ])species on the Ni-Ce/SiO_(2)(R)catalyst,containing highly dispersed[Ni]particles and rich oxygen vacancies,which can synergistically establish a new stable balance between gasification of carbon species and CO_(2) dissocia-tion.With respect to Ni-Ce/γ-Al_(2)O_(3)(R),the Ni and Ce precursors are easily captured by extra-framework Al_(n)-OH groups and further form stable isolated([Ni0_(n))]-[Ni-O-Al_(n)])and[CeⅢ-O-Al_(n)]species.In such a case,both of them preferentially accelerate CO_(2) adsorption and dissociation,causing more car-bon deposition due to the disproportionation of superfuous CO product.This deep distinguishment of chemical speciations of active sites can guide us to further develop new efficient Ni-based catalysts for LTDRM in the future.展开更多
The direct synthesis of C2 hydrocarbons （ethylene, acetylene and ethane） from methane is one of the most important task in C1 chemistry. Higher conversion of methane and selectivity to C2 hydrocarbons can be real-iz...The direct synthesis of C2 hydrocarbons （ethylene, acetylene and ethane） from methane is one of the most important task in C1 chemistry. Higher conversion of methane and selectivity to C2 hydrocarbons can be real-ized through plasma reaction. In order to explore the reaction process and mechanism, the possible reaction paths （1）—（4） were proposed on coupling reaction of methane through plasma and studied theoretically using semi-PM3 method [PM3 is parameterization method of modified neglect of diatomic overlap （MNDO）] including determining the transition state, calculating the activation energy and thermodynamic state functions and analyzing the bond or-der and intrinsic reaction coordinate. The reaction heat results indicate that the reactions （2） and （4） are exothermic, while reactions of （1） and （3） are endothermic. The activation energy results show that activation energy for reac-tions （1） and （2） was much lower than that of reaction paths （3） and （4）. Therefore, paths （1） and （2） is the favorable reaction path energetically. More interestingly by comparing the intrinsic reaction coordinated （IRC） of the reaction paths （1） and （2）, it is found that the variations of bond lengths in reaction path （1） has a crucial effect on the poten-tial energy, while in reaction path （2）, the adjustment of the system geometry also contributes to the whole potential energy of the system.展开更多
The mercury sulfidation experiments were conducted in the pH range from 1 to 13.The results show that Hg(Ⅱ) reacted with equimolar S(Ⅱ) has the lowest remained Hg(Ⅱ) concentration(9.7 μg/L) at pH 1.0 and the highe...The mercury sulfidation experiments were conducted in the pH range from 1 to 13.The results show that Hg(Ⅱ) reacted with equimolar S(Ⅱ) has the lowest remained Hg(Ⅱ) concentration(9.7 μg/L) at pH 1.0 and the highest remained concentration(940.8 μg/L) at pH 13.0.Meanwhile,the changes of pH values were monitored exactly,which reveal that solution pH values change when mixing the same pH value solutions of HgCl2 and Na2S.In order to explain the phenomena and determine the reaction paths of Hg(Ⅱ) reacting with S(Ⅱ) in the solution,the concerned thermodynamics was studied.Species of S(Ⅱ)-H2O system and Hg(Ⅱ)-H2O system at different pH values were calculated,and then the species distribution diagrams of S(Ⅱ)-H2O system,Hg(Ⅱ)-H2O system and Hg(Ⅱ)-Cl--OH--H2O system were drawn.Combining the experimental data and thermodynamic calculation,the mechanism of Hg(Ⅱ) reacting with S(Ⅱ) was deduced.The results indicate that different species of S(Ⅱ) and Hg(Ⅱ) have the diverse reaction paths to form HgS precipitate at different pH values and the standard Gibbs free energies change(△r GmΘ)of those equations are also calculated,which can provide a guidance for mercury-containing wastewater treatment with Na2S.展开更多
The stereodynamics of the C^NO reaction is investigated at O.06eV by means of the quasi-classical trajectory method on a recent ab initio 4^A＂ potential energy surface （PES）. The influences of rotation excitation ...The stereodynamics of the C^NO reaction is investigated at O.06eV by means of the quasi-classical trajectory method on a recent ab initio 4^A＂ potential energy surface （PES）. The influences of rotation excitation （j = 0 -3） on stereodynamics are discussed. The obtained stereodynamical information is compared with the previously reported results on the 2A′ and 2^A＂ PESs to give a full insight into the chemical stereodynamics of the title reaction.展开更多
Active soldering of 5A06 Al alloy was performed at 300 ℃ by using Sn-1Ti and Sn-1Ti-0.3Ga active solders, respectively. Theeffects of soldering time on the microstructure and mechanical properties of the joints were ...Active soldering of 5A06 Al alloy was performed at 300 ℃ by using Sn-1Ti and Sn-1Ti-0.3Ga active solders, respectively. Theeffects of soldering time on the microstructure and mechanical properties of the joints were investigated. The results showed that the Sn-1Tisolder broke the oxide film on the surface of the Al substrate and induced intergranular diffusion in the Al substrate. When Ga was added tothe solder, severe dissolution pits appeared in the Al substrate due to the action of Sn-1Ti-0.3Ga solder, and many Al particles were flakedfrom the matrix into the solder seam. Under thermal stress and the Ti adsorption effect, the oxide film cracked. With increasing solderingtime, the shear strength of 5A06 Al alloy joints soldered with Sn-1Ti and Sn-1Ti-0.3Ga active solders increased. When soldered for 90 min,the joint soldered with Sn-1Ti-0.3Ga solder had a higher shear strength of 22.12 MPa when compared to Sn-1Ti solder.展开更多
基金supported by the Natural Science Foundation of Jiangsu Province(No.BK20220618)the National Natural Science Foundation of China(Nos.22078028 and 21978026)。
文摘With the continuing boost in the demand for energy storage,there is an increasing requirement for batteries to be capable of operation in extreme environmental conditions.Sodium-ion batteries(SIBs) have emerged as a highly promising energy storage solution due to their promising performance over a wide range of temperatures and the abundance of sodium resources in the earth's crust.Compared to lithiumion batteries(LIBs),although sodium ions possess a larger ionic radius,they are more easily desolvated than lithium ions.Fu rthermore,SIBs have a smaller Stokes radius than lithium ions,resulting in improved sodium-ion mobility in the electrolyte.Nevertheless,SIBs demonstrate a significant decrease in performance at low temperatures(LT),which constrains their operation in harsh weather conditions.Despite the increasing interest in SIBs,there is a notable scarcity of research focusing specifically on their mechanism under LT conditions.This review explores recent research that considers the thermal tolerance of SIBs from an inner chemistry process perspective,spanning a wide temperature spectrum(-70 to100℃),particularly at LT conditions.In addition,the enhancement of electrochemical performance in LT SIBs is based on improvements in reaction kinetics and cycling stability achieved through the utilization of effective electrode materials and electrolyte components.Furthermore,the safety concerns associated with SIBs are addressed and effective strategies are proposed for mitigating these issues.Finally,prospects conducted to extend the environmental frontiers of commercial SIBs are discussed mainly from three viewpoints including innovations in materials,development and research of relevant theoretical mechanisms,and intelligent safety management system establishment for larger-scale energy storage SIBs.
基金by the National Natural Science Foundation of China(No.51402097)the College Students Innovation and Entrepreneurship Training Program of Hubei University of Technology(No.202010500045)。
文摘A lead-free base glaze suitable for pearlescent pigments was prepared by a low-temperature solid-phase reaction with alkali waste.Tests were performed to evaluate the effects of the sintering conditions and alkali waste composition on the prepared base glaze and pearlescent glaze.The experimental results show that partially replacing SiO_(2) with B_(2)O_(3) effectively reduced the sintering temperature and time to form a glass network,but the network structure becomes disconnected as the B_(2)O_(3) content increases.An amorphous base glaze was obtained when soda ash was replaced with a small amount of alkali waste,but increasing the addition of NaCl further was adverse to base glaze formation by resulting in crystallization of the base glaze and a decrease in the bridging oxygen content.The pearlescent pigment was thermally stable in the glaze at 750℃,while higher temperatures caused the crystalline phase of NaAlSiO_(4) to appear and adhere to the surface of pigment granules,which degraded the pearlescent effect of the glaze.
基金financially supported by the National Natural Science Foundation of China (22006059, 21968015)National Engineering Laboratory for Flue Gas Pollutants Control Technology and Equipment (NEL-KF-201905)+1 种基金Applied Basic Research Program of Yunnan Province, China (202101AU070154, 2019FD034)Analysis and Testing Fund of Kunming University of Science and Technology (2020 T20200006)
文摘The cognition of active sites in the Ni-based catalysts plays a vital role and remains a huge challenge in improving catalytic performance of low temperature CO_(2) dry reforming of methane(LTDRM).In this work,typical catalysts of SiO_(2) and γ-Al_(2)O_(3) supported Ni and Ni-Ce were designed and prepared.Importantly,the difference in the chemical speciations of active sites on the Ni-based catalysts is revealed by advanced characterizations and further estimates respective catalytic performance for LTDRM.Results show that larger[Ni0-]particles mixed with[Ni-O-Sin])species on the Ni/SiO_(2)(R)make CH_(4) excessive decomposition,leading to poor activity and stability.Once the Ce species is doped,however,superior activity(59.0%CH_(4) and 59.8%CO_(2) conversions),stability and high H_(2)/CO ratio(0.96)at 600℃ can be achieved on the Ni-Ce/SiO_(2)(R),in comparison with other catalysts and even reported studies.The improved performance can be ascribed to the formation of integral([Ni0_(n))]-[CeⅢ-□-CeⅢ])species on the Ni-Ce/SiO_(2)(R)catalyst,containing highly dispersed[Ni]particles and rich oxygen vacancies,which can synergistically establish a new stable balance between gasification of carbon species and CO_(2) dissocia-tion.With respect to Ni-Ce/γ-Al_(2)O_(3)(R),the Ni and Ce precursors are easily captured by extra-framework Al_(n)-OH groups and further form stable isolated([Ni0_(n))]-[Ni-O-Al_(n)])and[CeⅢ-O-Al_(n)]species.In such a case,both of them preferentially accelerate CO_(2) adsorption and dissociation,causing more car-bon deposition due to the disproportionation of superfuous CO product.This deep distinguishment of chemical speciations of active sites can guide us to further develop new efficient Ni-based catalysts for LTDRM in the future.
基金Supported by the National Natural Science Foundation of China (No.20606023).
文摘The direct synthesis of C2 hydrocarbons （ethylene, acetylene and ethane） from methane is one of the most important task in C1 chemistry. Higher conversion of methane and selectivity to C2 hydrocarbons can be real-ized through plasma reaction. In order to explore the reaction process and mechanism, the possible reaction paths （1）—（4） were proposed on coupling reaction of methane through plasma and studied theoretically using semi-PM3 method [PM3 is parameterization method of modified neglect of diatomic overlap （MNDO）] including determining the transition state, calculating the activation energy and thermodynamic state functions and analyzing the bond or-der and intrinsic reaction coordinate. The reaction heat results indicate that the reactions （2） and （4） are exothermic, while reactions of （1） and （3） are endothermic. The activation energy results show that activation energy for reac-tions （1） and （2） was much lower than that of reaction paths （3） and （4）. Therefore, paths （1） and （2） is the favorable reaction path energetically. More interestingly by comparing the intrinsic reaction coordinated （IRC） of the reaction paths （1） and （2）, it is found that the variations of bond lengths in reaction path （1） has a crucial effect on the poten-tial energy, while in reaction path （2）, the adjustment of the system geometry also contributes to the whole potential energy of the system.
基金Project(50925417) supported by China National Funds for Distinguished Young ScientistsProject(50830301) supported by the Key Project of the National Natural Science Foundation of China+2 种基金Project(308019) supported by the Key Science and Technical Project of Ministry of Science and Technology of ChinaProject(2007BAC25B01) supported by the National Key Project of Science and Technical Supporting Programs Funded by Ministry of Science and Technology of China during the 11th Five-Year PlanProject(08JJ3020) supported by the Natural Science Foundation of Hunan Province, China
文摘The mercury sulfidation experiments were conducted in the pH range from 1 to 13.The results show that Hg(Ⅱ) reacted with equimolar S(Ⅱ) has the lowest remained Hg(Ⅱ) concentration(9.7 μg/L) at pH 1.0 and the highest remained concentration(940.8 μg/L) at pH 13.0.Meanwhile,the changes of pH values were monitored exactly,which reveal that solution pH values change when mixing the same pH value solutions of HgCl2 and Na2S.In order to explain the phenomena and determine the reaction paths of Hg(Ⅱ) reacting with S(Ⅱ) in the solution,the concerned thermodynamics was studied.Species of S(Ⅱ)-H2O system and Hg(Ⅱ)-H2O system at different pH values were calculated,and then the species distribution diagrams of S(Ⅱ)-H2O system,Hg(Ⅱ)-H2O system and Hg(Ⅱ)-Cl--OH--H2O system were drawn.Combining the experimental data and thermodynamic calculation,the mechanism of Hg(Ⅱ) reacting with S(Ⅱ) was deduced.The results indicate that different species of S(Ⅱ) and Hg(Ⅱ) have the diverse reaction paths to form HgS precipitate at different pH values and the standard Gibbs free energies change(△r GmΘ)of those equations are also calculated,which can provide a guidance for mercury-containing wastewater treatment with Na2S.
基金Supported by the National Natural Science Foundation of China under Grant No 11204392the Scientific and Technological Research Program of Chongqing Municipal Education Commission under Grant Nos KJ1400920 and KJ130821
文摘The stereodynamics of the C^NO reaction is investigated at O.06eV by means of the quasi-classical trajectory method on a recent ab initio 4^A＂ potential energy surface （PES）. The influences of rotation excitation （j = 0 -3） on stereodynamics are discussed. The obtained stereodynamical information is compared with the previously reported results on the 2A′ and 2^A＂ PESs to give a full insight into the chemical stereodynamics of the title reaction.
基金the National Natural Science Foundation of China(No.52171045).
文摘Active soldering of 5A06 Al alloy was performed at 300 ℃ by using Sn-1Ti and Sn-1Ti-0.3Ga active solders, respectively. Theeffects of soldering time on the microstructure and mechanical properties of the joints were investigated. The results showed that the Sn-1Tisolder broke the oxide film on the surface of the Al substrate and induced intergranular diffusion in the Al substrate. When Ga was added tothe solder, severe dissolution pits appeared in the Al substrate due to the action of Sn-1Ti-0.3Ga solder, and many Al particles were flakedfrom the matrix into the solder seam. Under thermal stress and the Ti adsorption effect, the oxide film cracked. With increasing solderingtime, the shear strength of 5A06 Al alloy joints soldered with Sn-1Ti and Sn-1Ti-0.3Ga active solders increased. When soldered for 90 min,the joint soldered with Sn-1Ti-0.3Ga solder had a higher shear strength of 22.12 MPa when compared to Sn-1Ti solder.
