The development of reliable and affordable all-solid-state sodium metal batteries(ASS-SMBs)requires suitable solid-state electrolytes with cost-efficient processing and stabilized electrode/electrolyte interfaces.Here...The development of reliable and affordable all-solid-state sodium metal batteries(ASS-SMBs)requires suitable solid-state electrolytes with cost-efficient processing and stabilized electrode/electrolyte interfaces.Here,an integrated porous/dense/porous Na_(5)YSi_(4)O_(12)(NYS)trilayered scaffold is designed and fabricated by tape casting using aqueous slurries.In this template-based NYS scaffold,the dense layer in the middle serves as a separator and the porous layers on both sides accommodate the active materials with their volume changes during the charge/discharge processes,increasing the contact area and thus enhancing the utilization rate and homogenizing the current distribution.The Na/NYS/Na symmetric cells with the Pb-coated NYS scaffold exhibit significantly reduced interfacial impedance and superior critical current density of up to 3.0 mA cm^(-2)against Na metal owing to enhanced wettability.Furthermore,the assembled Na/NYS/S full cells operated without external pressure at room temperature showed a high initial discharge capacity of 970 mAh g^(-1)and good cycling stability with a capacity of 600 mAh g^(-1)after 150 cycles(based on the mass of sulfur).This approach paves the way for the realization of economical and practical ASS-SMBs from the perspective of ceramic manufacturing.展开更多
Thermodynamic diagrams of Na−S−Fe−H_(2)O system were constructed to analyze the behavior of sulfur and iron in the Bayer process.After digestion,iron mainly exists as Fe_(3)O_(4) and Fe_(2)O_(3) in red mud,and partial...Thermodynamic diagrams of Na−S−Fe−H_(2)O system were constructed to analyze the behavior of sulfur and iron in the Bayer process.After digestion,iron mainly exists as Fe_(3)O_(4) and Fe_(2)O_(3) in red mud,and partial iron transfers into solution as Fe(OH)_(3)^(−),HFeO_(2)^(−),Fe(OH)_(4)^(−)and Fe(OH)_(4)^(2−).The dominant species of sulfur is S^(2−),followed by SO_(4)^(2−),and then SO_(3)^(2−)and S_(2)O_(3)^(2−).The thermodynamic analysis is consistent with the iron and sulfur species distribution in the solution obtained by experiments.When the temperature decreases,sulfur and iron can combine and precipitate.Controlling low potential and reducing temperature are beneficial to removing them from the solution.XRD patterns show that NaFeS_(2)·2H_(2)O,FeS and FeS_(2) widely appear in red mud and precipitates of pyrite and high-sulfur bauxite digestion solution.Thermodynamic analysis can be utilized to guide the simultaneous removal of sulfur and iron in the Bayer process.展开更多
A series of Na-W-Mn-Zr/SiO2 catalysts promoted by different contents of S or/and P were prepared and their catalytic performance for oxidative coupling of methane was investigated to clarify the effect of S and P on t...A series of Na-W-Mn-Zr/SiO2 catalysts promoted by different contents of S or/and P were prepared and their catalytic performance for oxidative coupling of methane was investigated to clarify the effect of S and P on the Na-W-Mn-Zr/SiO2 catalyst. The catalysts were characterized by X-ray diffraction （XRD） and X-ray photoelectron spectroscopy （XPS）. From the characterization results, it is found that the addition of S and P to the Na-W-Mn-ZffSiO2 catalyst helps the formation of active phases, such as α-cristobalite, Na2WO4, ZrO2, and Na2SO4. Moreover, the addition of S and P increases the concentration of surface-active oxygen species by improving the migration of active components from the bulk phase to the surface of the catalyst. According to the activity test, impressive methane conversion and C2 hydrocarbons yield were obtained at a low temperature of 1023 K over the six-component Na-W-Mn-Zr-S-P/SiO2 catalyst, which contained 2 wt% S and 0.4 wt% P simultaneously. The deactivation of Na-W-Mn-Zr-S-P/SiO2 was due to the loss of surface active components.展开更多
Na-W-Mn-Zr-S-P/SiO2 catalysts for oxidative coupling of methane （OCM） were prepared by incipient wetness impregnation, sol-gel and mixture slurry methods. The catalyst prepared by mixture slurry method showed the be...Na-W-Mn-Zr-S-P/SiO2 catalysts for oxidative coupling of methane （OCM） were prepared by incipient wetness impregnation, sol-gel and mixture slurry methods. The catalyst prepared by mixture slurry method showed the best catalytic performance among all samples. In addition, the effects of different addition sequences of Na, W, Mn, Zr, S and P on the catalytic performance were studied. The absence of Na before the addition of Mn and Zr in the catalysts preparation depressed the formation of the active phases of Mn2O3 and ZrO2 and decreased the activities of the catalysts significantly.展开更多
Na-ion batteries(NIBs)have attracted considerable attention in recent years owing to the high abundance and low cost of Na.It is well known that S doping can improve the electrochemical performance of carbon materials...Na-ion batteries(NIBs)have attracted considerable attention in recent years owing to the high abundance and low cost of Na.It is well known that S doping can improve the electrochemical performance of carbon materials for NIBs.However,the current methods for S doping in carbons normally involve toxic precursors or rigorous conditions.In this work,we report a creative and facile strategy for preparing S-doped porous carbons(SCs)via the pyrolysis of conjugated microporous polymers(CMPs).Briefly,thiophene-based CMPs served as the precursors and doping sources simultaneously.Simple direct carbonization of CMPs produced S-doped carbon materials with highly porous structures.When used as an anode for NIBs,the SCs exhibited a high reversible capacity of 440 mAh g?1 at 50 mA g?1 after 100 cycles,superior rate capability,and excellent cycling stability(297 mAh g?1 after 1000 cycles at 500 mA g?1),outperforming most S-doped carbon materials reported thus far.The excellent performance of the SCs is attributed to the expanded lattice distance after S doping.Furthermore,we employed ex situ X-ray photoelectron spectroscopy to investigate the electrochemical reaction mechanism of the SCs during sodiation-desodiation,which can highlight the role of doped S for Na-ion storage.展开更多
For double arrays of constants {a ni, 1≤i≤k n, n≥1} and NA r.v. 's {X n, n≥1}, conditions for almost sure convergence of are given. Both casesk n ↑ ∞ andk n=∞ are treated. A Marcinkiewicz-type theorem for ...For double arrays of constants {a ni, 1≤i≤k n, n≥1} and NA r.v. 's {X n, n≥1}, conditions for almost sure convergence of are given. Both casesk n ↑ ∞ andk n=∞ are treated. A Marcinkiewicz-type theorem for i. d. NA sequences is obtained as a special case.展开更多
以拌合液为KOH和NaOH混合溶液的C_3S-纳米SiO_2浆体为对象,研究了液固比对浆体在去离子水中释放K^+和Na^+的影响以及浆体对K^+和Na^+的滞留能力;并采用29Si MAS NMR分析讨论了K^+和Na^+在C_3S-纳米SiO_2浆体上的存在形式。结果表明:随...以拌合液为KOH和NaOH混合溶液的C_3S-纳米SiO_2浆体为对象,研究了液固比对浆体在去离子水中释放K^+和Na^+的影响以及浆体对K^+和Na^+的滞留能力;并采用29Si MAS NMR分析讨论了K^+和Na^+在C_3S-纳米SiO_2浆体上的存在形式。结果表明:随着液固比的增大,浆体释放的K^+和Na^+的百分数逐渐增大;经去离子水充分洗涤后仍有一部分K^+和Na^+存在于浆体中,且浆体对K^+和Na^+的滞留能力随着纳米SiO_2掺量的增加以及拌合液碱浓度的增大而增强。29Si MAS NMR分析证实了K^+和Na^+能够进入C-S-H凝胶层间形成不可逆的化学结合。K^+和Na^+通过取代C-S-H凝胶层间≡SiOCa+中的Ca2+,缩短了C-S-H凝胶中[SiO4]4-四面体链长,从而使凝胶中Q1和Q2峰向左移动。展开更多
基金the China Scholarship Council(CSC,No.201906200023)the MatKat Foundation.Aikai Yang,whose CSC grant application is affiliated with Nankai University(Tianjin,China)the Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education)at Nankai University.Partial financial support from the German Federal Ministry of Education and Research(BMBF)within the project“HeNa”(support code 13XP0390B)is also gratefully acknowledged.
文摘The development of reliable and affordable all-solid-state sodium metal batteries(ASS-SMBs)requires suitable solid-state electrolytes with cost-efficient processing and stabilized electrode/electrolyte interfaces.Here,an integrated porous/dense/porous Na_(5)YSi_(4)O_(12)(NYS)trilayered scaffold is designed and fabricated by tape casting using aqueous slurries.In this template-based NYS scaffold,the dense layer in the middle serves as a separator and the porous layers on both sides accommodate the active materials with their volume changes during the charge/discharge processes,increasing the contact area and thus enhancing the utilization rate and homogenizing the current distribution.The Na/NYS/Na symmetric cells with the Pb-coated NYS scaffold exhibit significantly reduced interfacial impedance and superior critical current density of up to 3.0 mA cm^(-2)against Na metal owing to enhanced wettability.Furthermore,the assembled Na/NYS/S full cells operated without external pressure at room temperature showed a high initial discharge capacity of 970 mAh g^(-1)and good cycling stability with a capacity of 600 mAh g^(-1)after 150 cycles(based on the mass of sulfur).This approach paves the way for the realization of economical and practical ASS-SMBs from the perspective of ceramic manufacturing.
基金the financial supports from the National Natural Science Foundation of China(No.51904052)the Chongqing Research Program of Basic Research and Frontier Technology,China(No.cstc2020jcyjmsxm X0476)+1 种基金the Science and Technology Research Program of Chongqing Municipal Education Commission,China(No.KJQN201901508)the Graduate Science and Technology Innovation Training Program of Chongqing University of Science and Technology,China(No.YKJCX2020201)。
文摘Thermodynamic diagrams of Na−S−Fe−H_(2)O system were constructed to analyze the behavior of sulfur and iron in the Bayer process.After digestion,iron mainly exists as Fe_(3)O_(4) and Fe_(2)O_(3) in red mud,and partial iron transfers into solution as Fe(OH)_(3)^(−),HFeO_(2)^(−),Fe(OH)_(4)^(−)and Fe(OH)_(4)^(2−).The dominant species of sulfur is S^(2−),followed by SO_(4)^(2−),and then SO_(3)^(2−)and S_(2)O_(3)^(2−).The thermodynamic analysis is consistent with the iron and sulfur species distribution in the solution obtained by experiments.When the temperature decreases,sulfur and iron can combine and precipitate.Controlling low potential and reducing temperature are beneficial to removing them from the solution.XRD patterns show that NaFeS_(2)·2H_(2)O,FeS and FeS_(2) widely appear in red mud and precipitates of pyrite and high-sulfur bauxite digestion solution.Thermodynamic analysis can be utilized to guide the simultaneous removal of sulfur and iron in the Bayer process.
基金supported by the National Natural Science Foundation of China (20676116)
文摘A series of Na-W-Mn-Zr/SiO2 catalysts promoted by different contents of S or/and P were prepared and their catalytic performance for oxidative coupling of methane was investigated to clarify the effect of S and P on the Na-W-Mn-Zr/SiO2 catalyst. The catalysts were characterized by X-ray diffraction （XRD） and X-ray photoelectron spectroscopy （XPS）. From the characterization results, it is found that the addition of S and P to the Na-W-Mn-ZffSiO2 catalyst helps the formation of active phases, such as α-cristobalite, Na2WO4, ZrO2, and Na2SO4. Moreover, the addition of S and P increases the concentration of surface-active oxygen species by improving the migration of active components from the bulk phase to the surface of the catalyst. According to the activity test, impressive methane conversion and C2 hydrocarbons yield were obtained at a low temperature of 1023 K over the six-component Na-W-Mn-Zr-S-P/SiO2 catalyst, which contained 2 wt% S and 0.4 wt% P simultaneously. The deactivation of Na-W-Mn-Zr-S-P/SiO2 was due to the loss of surface active components.
基金supported by the financial support from National Natural Science Foundation of China (20676116)
文摘Na-W-Mn-Zr-S-P/SiO2 catalysts for oxidative coupling of methane （OCM） were prepared by incipient wetness impregnation, sol-gel and mixture slurry methods. The catalyst prepared by mixture slurry method showed the best catalytic performance among all samples. In addition, the effects of different addition sequences of Na, W, Mn, Zr, S and P on the catalytic performance were studied. The absence of Na before the addition of Mn and Zr in the catalysts preparation depressed the formation of the active phases of Mn2O3 and ZrO2 and decreased the activities of the catalysts significantly.
基金Financial support from National Natural Science Foundation of China(Nos.51702056 and 51772135)the Ministry of Education of China(6141A02022516)China Postdoctoral Science Foundation(2017M622902 and 2019T120790).
文摘Na-ion batteries(NIBs)have attracted considerable attention in recent years owing to the high abundance and low cost of Na.It is well known that S doping can improve the electrochemical performance of carbon materials for NIBs.However,the current methods for S doping in carbons normally involve toxic precursors or rigorous conditions.In this work,we report a creative and facile strategy for preparing S-doped porous carbons(SCs)via the pyrolysis of conjugated microporous polymers(CMPs).Briefly,thiophene-based CMPs served as the precursors and doping sources simultaneously.Simple direct carbonization of CMPs produced S-doped carbon materials with highly porous structures.When used as an anode for NIBs,the SCs exhibited a high reversible capacity of 440 mAh g?1 at 50 mA g?1 after 100 cycles,superior rate capability,and excellent cycling stability(297 mAh g?1 after 1000 cycles at 500 mA g?1),outperforming most S-doped carbon materials reported thus far.The excellent performance of the SCs is attributed to the expanded lattice distance after S doping.Furthermore,we employed ex situ X-ray photoelectron spectroscopy to investigate the electrochemical reaction mechanism of the SCs during sodiation-desodiation,which can highlight the role of doped S for Na-ion storage.
文摘For double arrays of constants {a ni, 1≤i≤k n, n≥1} and NA r.v. 's {X n, n≥1}, conditions for almost sure convergence of are given. Both casesk n ↑ ∞ andk n=∞ are treated. A Marcinkiewicz-type theorem for i. d. NA sequences is obtained as a special case.
文摘以拌合液为KOH和NaOH混合溶液的C_3S-纳米SiO_2浆体为对象,研究了液固比对浆体在去离子水中释放K^+和Na^+的影响以及浆体对K^+和Na^+的滞留能力;并采用29Si MAS NMR分析讨论了K^+和Na^+在C_3S-纳米SiO_2浆体上的存在形式。结果表明:随着液固比的增大,浆体释放的K^+和Na^+的百分数逐渐增大;经去离子水充分洗涤后仍有一部分K^+和Na^+存在于浆体中,且浆体对K^+和Na^+的滞留能力随着纳米SiO_2掺量的增加以及拌合液碱浓度的增大而增强。29Si MAS NMR分析证实了K^+和Na^+能够进入C-S-H凝胶层间形成不可逆的化学结合。K^+和Na^+通过取代C-S-H凝胶层间≡SiOCa+中的Ca2+,缩短了C-S-H凝胶中[SiO4]4-四面体链长,从而使凝胶中Q1和Q2峰向左移动。
