Aqueous zinc-ion batteries exhibit significant promise for practical energy storage owing to their costeffective materials and inherent safety.However,the practical application at low temperatures is hindered by the s...Aqueous zinc-ion batteries exhibit significant promise for practical energy storage owing to their costeffective materials and inherent safety.However,the practical application at low temperatures is hindered by the sluggish interfacial kinetics at the Zn electrode.Here,a localized cation-anion clustering chemistry is developed by introducing cyclopentyl methyl ether(CPME)as a diluent to improve the low-temperature interface kinetics at the Zn anode.In this configuration,CPME does not participate in solvation shell formation but instead facilitates the selective integration of trifluoro-methane-sulfonate anions(OTF^(-))into the solvation sheaths of Zn^(2+)ions,accelerating desolvation kinetics at the zinc metal interface.Furthermore,the enhanced interaction between Zn^(2+)and OTF^(-)anions drives preferential anion decomposition,yielding a ZnF_(2)-rich interfacial layer,which enhances Zn^(2+)diffusion at the Zn electrode interface under cryogenic conditions.Notably,Zn//Cu cells employing this optimized electrolyte achieve corrosion-resistant zinc stripping/plating of over 1200 cycles at-40℃,with an average Coulombic efficiency of 99.74%.Moreover,Zn//NaV_(3)O_(8)·1.5H_(2)O(NVO)full cells demonstrate exceptional stability,retaining 90.91%of their initial capacity after 2000 cycles at-40℃.This work offers new insights into the rational regulation of interfacial kinetics in aqueous zinc-ion batteries at low temperatures.展开更多
Layered V_(2)O_(5) cathode holds the merits of high theoretical specific capacity(589 mA h g^(-1))in aqueous zinc-ion batteries(AZIBs),yet it still suffers from inferior bulk conductivity and structure degradation not...Layered V_(2)O_(5) cathode holds the merits of high theoretical specific capacity(589 mA h g^(-1))in aqueous zinc-ion batteries(AZIBs),yet it still suffers from inferior bulk conductivity and structure degradation notably during prolonged cycling.Herein,we ingeniously design cations(Na^(+)/Co^(2+)/Al^(3+))and anion(F^(-))synergistic-doped hydrated V_(2)O_(5)·0.48H_(2)O cathode(VNACOF)to enhance the electronic and spatial effects in the bulk.A range of in-situ,ex-situ characterizations,and DFT calculations profoundly clarify the strengthened ionic/electronic conductivities,structural stability,and Zn^(2+)diffusion kinetics.As a result,the VNACOF displays a superior discharge capacity(529 mA h g^(-1)@0.1 C),rate capabilities(488 mA h g^(-1)@0.5 C,437 mA h g^(-1)@1C),and cycling stability(301 mA h g^(-1)@10 C@5000 cycles@93%)with sufficient energy density(393 W h kg^(-1)),Furthermore,the pouch-cells with high-load(60 mg)also deliver superior cyclic(2 C@178 mA h g^(-1)@1000 cycles@90%)and rate performance(132 mA h g^(-1)@5 C),revealing great application potential for high-energy-density and high-stability AZIBs.展开更多
Reducing dietary cation-anion difference (DCAD) has been proved an effective way to prevent milk fever in dairy cows. Based on the similar physiological gastro-intestinal tract anatomy and metabolic process between ...Reducing dietary cation-anion difference (DCAD) has been proved an effective way to prevent milk fever in dairy cows. Based on the similar physiological gastro-intestinal tract anatomy and metabolic process between female goats and dairy cows, this study was conducted to evaluate the effects of varying DCAD on fluid acid-base status, plasma minerals concentration and anti-oxidative stress capacity of female goats. Urinary pH, plasma Ca, P and Mg; and anti-oxidative stress indices of total superoxide dismutase (T-SOD), hydrogen peroxide (HzO2), glutathione peroxidase (GSH-Px) and malondialdehyde (MDA) were determined to evaluate the effect. Forty-eight Guizhou black female goats ((15±1.9) mon of old, (22.3±3.75) kg of BW) were randomly allocated to 4 blocks of 12 goats each and were fed 1 of 4 diets differed in DCAD level (calculated as Na+K-C1-S, mEq kg-1 DM). Levels of DCAD were preliminarily designed to be control (+ 150 mEq kg^-1 DM, CON), high DCAD (+300 mEq kg^-1 DM, HD), low DCAD (0 mEq kg^-1 DM, LD) and negative DCAD (-150 mEq kg^-1 DM, ND), respectively. A commercial anionic salts (Animate) and sodium bicarbonate (NaHCO3) were supplemented to reduce and increase DCAD level, respectively. There was no difference in dry matter intake for 4 groups of goats. Urine pH was aggressively decreased (P〈0.0001) with reduced DCAD and there was a strong association between DCAD and urine pH (R2=0.793, P〈0.0001). Compared with CON and HD feeding of LD and ND resulted in greater (P〈0.05) plasma Ca concentration. Plasma P level was increased (P〈0.05) when anionic salts were supplemented. The DCAD alteration did not affected (P〉0.05) plasma Mg level. There was no significant (P〉0.05) difference in plasma GSH-Px activity and H202, but anionic salts supplementation in LD and ND significantly increased (P〈0.05) plasma T-SOD activity and tended to reduce MDA (P〈0.1) over HD and CON. Results from this study indicated that reducing DCAD could decrease urine pH and increase plasma Ca concentration of female goats. Additionally, reducing DCAD was helpful to enhance anti-oxidative stress capability of female goats.展开更多
Finding suitable strategies to effectively enhance the optical properties of materials are the goal being pursued by researchers.Herein,cation-anion synergetic interactions strategy was proposed to develop two novel o...Finding suitable strategies to effectively enhance the optical properties of materials are the goal being pursued by researchers.Herein,cation-anion synergetic interactions strategy was proposed to develop two novel organic-inorganic hybrid antimony-based optical materials,(C_(3)H_(5)N_(2))Sb F_(2)SO_(4)(I)and(C_(5)H_(6)N)Sb F_(2)SO_(4)(Ⅱ),which were obtained by introducing Sb^(3+)cation containing stereochemically active lone-pair(SCALP)and organicπ-conjugated cations into sulphate system.The synergistic interactions of the organicπ-conjugated cations,the inorganic[SbO_(2)F_(2)]^(3-)seesaw anions and the[SO_(4)]^(2-)distorted tetrahedra anions make their ultraviolet(UV)absorption edges approach 297 and 283 nm,respectively,and raise their birefringence up to 0.193@546 nm and 0.179@546 nm,respectively.Interestingly,although the two compounds have the same stoichiometric ratio and similar one-dimensional(1D)chain structure,they show opposite macroscopic symmetry,where the NCS compound(Ⅱ)exhibits a large secondharmonic generation(SHG)response(1.6 times that of KH_(2)PO_(4)).The two reported compounds are found to be promising UV optical materials in the experimental tests.展开更多
Cultivated tea(Camellia sinensis) plants acidify the rhizosphere, and Aluminum(Al) toxicity is recognized as a major limiting factor for plant growth in acidic soils. However, the mechanisms responsible for rhizospher...Cultivated tea(Camellia sinensis) plants acidify the rhizosphere, and Aluminum(Al) toxicity is recognized as a major limiting factor for plant growth in acidic soils. However, the mechanisms responsible for rhizosphere acidification associated with Al have not been fully elucidated. The present study examined the effect of Al on root-induced rhizosphere acidification, plasma membrane H^+-adenosine triphosphatase(H^+-ATPase) activity, and cation-anion balance in tea plant roots. The exudation of H^+from tea plant roots with or without Al treatment was visualized using an agar sheet with bromocresol purple. The H^+-ATPase activity of plasma membranes isolated from the roots was measured after hydrolysis using the two-phase partition system. The Al treatment strongly enhanced the exudation of H^+, and the acidification of tea plant roots by Al was closely associated with plasma membrane H^+-ATPase activity. The root plasma membrane H^+-ATPase activity increased with Al concentration. The Al content, amount of protons released, and H^+-ATPase activity were significantly higher in roots treated with Al than in those untreated. The results of the cation-anion balance in roots showed an excess of cations relative to anions, with the amount of excess cation uptake increasing with increasing Al concentrations. These suggest that Al-enhanced proton release is associated with plasma membrane H^+-ATPase activity and excess cation uptake. Findings of this study would provide insights into the contributing factors of soil acidification in tea plantations.展开更多
The high-nickel layered cathodes Li[Ni_(x)Co_(y)Mn_(1-x-y)]O_(2)(x≥0.8)with high specific capacity and long cycle life are considered as prospective cathodes for lithium-ion batteries.However,the microcrack formation...The high-nickel layered cathodes Li[Ni_(x)Co_(y)Mn_(1-x-y)]O_(2)(x≥0.8)with high specific capacity and long cycle life are considered as prospective cathodes for lithium-ion batteries.However,the microcrack formation and poor structural stability give rise to inferior rate performance and undesirable cycling life.Herein,we propose a dual modification strategy combining primary particle structure design and element doping to modify Li[Ni_(0.95)Co_(0.025)Mn_(0.025)]O_(2) cathode by tungsten and fluorine co-doped(W-F-NCM95).The doping of W can convert the microstructure of primary particles to the unique rod-like shape,which is beneficial to enhance the reversibility of phase transition and alleviate the generation of microcracks.F doping is conducive to alleviating the surface side reactions.Thus,due to the synergistic effect of W,F codoping,the obtained W-F-NCM95 cathodes deliver a high initial capacity of 236.1 mA h g^(-1) at 0.1 C and superior capacity retention of 88.7%over 100 cycles at 0.5 C.Moreover,the capacity still maintains73.8%after 500 cycles at 0.5 C and the texture of primary particle is intact.This work provides an available strategy by W and F co-doping to enhance the electrochemistry performance of high-nickel cathodes for practical application.展开更多
The rational design and optimization of noble-metal-free semiconductor photocatalysts aim to increase the number of active sites and accelerate the separation and transfer of charges,thereby achieving high-performance...The rational design and optimization of noble-metal-free semiconductor photocatalysts aim to increase the number of active sites and accelerate the separation and transfer of charges,thereby achieving high-performance hydrogen evolution reactions(HER).In this study,we innovatively designed an S-scheme heterojunction catalyst composed of CdS nanoparticles rich in cationic Cd vacancies(VCCS)and ZnWO4nanorods rich in anionic O vacancies(VOZWO)that regulate the surface electronic states of the catalyst through dual vacancies engineering.Specifically,the introduction of vacancy engineering effectively adjusted the energy level structure of the catalyst,achieving bandgap narrowing,enhancing light absorption capacity,providing hole trapping sites,and creating more active sites.As expected,the optimized VOZWO@VCCS heterojunction exhibited exceptional photocatalytic H_(2)production rates of 11.55 mmol g^(-1)h^(-1)in the absence of noble-metal cocatalysts,which are approximately 462 times and4 times higher than those of pure VOZWO(0.025 mmol g^(-1)h^(-1))and VCCS(2.89 mmol g^(-1)h^(-1)),respectively.In-depth characterization tests and density functional theory(DFT)calculations revealed that the introduction of vacancies significantly reduced the bandgap,improved the transfer efficiency of photoinduced carriers,and validated the charge transfer mechanism of the S-scheme heterojunction.展开更多
Conventional gel polymer electrolytes based on polymers such as poly(ethylene oxide) face inherent limitations in enhancing ionic conductivity and electrochemical stability.Introducing diverse functional groups into t...Conventional gel polymer electrolytes based on polymers such as poly(ethylene oxide) face inherent limitations in enhancing ionic conductivity and electrochemical stability.Introducing diverse functional groups into the polymer framework enables the precise modulation of its physicochemical properties,thereby influencing the performance of lithium metal batteries.Herein,an in situ dual-crosslinked gel polymer electrolyte based on polyester and polyamide is proposed.This design enables synergistic cation-anion regulation,facilitating continuous Li^(+) transport by abundant ester groups while anchoring the anions by N–H groups.The resulting gel polymer electrolyte exhibits a high ionic conductivity of 0.58 mS cm^(-1)and an elevated Li^(+) transference number of 0.6.The assembled Li||LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2) coin cells achieve 400 cycles at 0.5 C and 300 cycles at 1 C.Furthermore,a 4-layer stacked Li||LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(active material mass loading of 26.7 mg cm^(-2)) pouch cell in lean electrolyte conditions(1.7 g Ah^(-1)) is assembled and sustains 45 cycles without obvious decay.This study provides a strategy of synergistic cationanion regulation in gel polymer electrolytes,offering insights for stable lithium metal batteries.展开更多
It used to be held that the cloud point phenomenon was only a characteris-tic of nonionic surfactants alone. Such phenomenon is rarely observed in ionicsurfactants. The present study shows that the mixture of cationic...It used to be held that the cloud point phenomenon was only a characteris-tic of nonionic surfactants alone. Such phenomenon is rarely observed in ionicsurfactants. The present study shows that the mixture of cationic-anionic surfac-tants not only has a krafft point which is the characteristic of an ionic surfactant,but also exhibits the cloud point phenomenon obviously at certain concentrations.展开更多
Cobait(Ⅱ) nitrate reacted with 1,10-phenanthroline (phen) and 5-sulfosaiicylic acid (H3ssal) to yield the cobait(Ⅰ) complex [Co(phen)2(H2O)2](Hssal)o4H2O (1) and the reaction of 1 with copper acetate...Cobait(Ⅱ) nitrate reacted with 1,10-phenanthroline (phen) and 5-sulfosaiicylic acid (H3ssal) to yield the cobait(Ⅰ) complex [Co(phen)2(H2O)2](Hssal)o4H2O (1) and the reaction of 1 with copper acetate led to a novel complex [Co(phen)(H2O)4][Cu2(ssal)2(phen)2]·5H2O (2). These two complexes were cationanion species and the cationic motif [Co(phen)2(H2O)2]^2+of 1 could be converted to [Co(phen)(H2O)4]^2+ in the formation process of new anion [Cu2(phen)2(ssal)2]^2- of 2. In both complexes abundant hydrogen bonds construct different supramolecular architectures, thus the conversion reaction can provide a new path to create novel supramolecular network.展开更多
基金This research was financially supported by the National Natural Science Foundation of China(22209071,22309081)the Natural Science Foundation of Jiangsu Province(BK20220339,BK20230320)+2 种基金the Natural Science Research in Colleges and Universities of Jiangsu Province(22KJB150006,22KJB430005)the China Postdoctoral Science Foundation funded project(2023M731641)the Open Project Fund from Jiangsu Province Large Scientific Instruments。
文摘Aqueous zinc-ion batteries exhibit significant promise for practical energy storage owing to their costeffective materials and inherent safety.However,the practical application at low temperatures is hindered by the sluggish interfacial kinetics at the Zn electrode.Here,a localized cation-anion clustering chemistry is developed by introducing cyclopentyl methyl ether(CPME)as a diluent to improve the low-temperature interface kinetics at the Zn anode.In this configuration,CPME does not participate in solvation shell formation but instead facilitates the selective integration of trifluoro-methane-sulfonate anions(OTF^(-))into the solvation sheaths of Zn^(2+)ions,accelerating desolvation kinetics at the zinc metal interface.Furthermore,the enhanced interaction between Zn^(2+)and OTF^(-)anions drives preferential anion decomposition,yielding a ZnF_(2)-rich interfacial layer,which enhances Zn^(2+)diffusion at the Zn electrode interface under cryogenic conditions.Notably,Zn//Cu cells employing this optimized electrolyte achieve corrosion-resistant zinc stripping/plating of over 1200 cycles at-40℃,with an average Coulombic efficiency of 99.74%.Moreover,Zn//NaV_(3)O_(8)·1.5H_(2)O(NVO)full cells demonstrate exceptional stability,retaining 90.91%of their initial capacity after 2000 cycles at-40℃.This work offers new insights into the rational regulation of interfacial kinetics in aqueous zinc-ion batteries at low temperatures.
基金financially supported by the National Key Research and Development Program of China(2022YFA1505700,2019YFA0210403)the National Natural Science Foundation of China(52102216)+4 种基金the Natural Science Foundation of Fujian Province(2022J01625,2022-S-002)the Anhui Key Laboratory of Nanomaterials and Nanotechnology,the Major Science and Technology Projects in Anhui Province(202305a12020006)the Open Project of State Key Laboratory of Inorganic Synthesis and Preparative Chemistry(2025-22)the Innovation Training Program for College Students(cxxl-2024131,cxxl-2024136)support by Transmission Electron Microscope Platform and High-performance Computing Platform of Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China。
文摘Layered V_(2)O_(5) cathode holds the merits of high theoretical specific capacity(589 mA h g^(-1))in aqueous zinc-ion batteries(AZIBs),yet it still suffers from inferior bulk conductivity and structure degradation notably during prolonged cycling.Herein,we ingeniously design cations(Na^(+)/Co^(2+)/Al^(3+))and anion(F^(-))synergistic-doped hydrated V_(2)O_(5)·0.48H_(2)O cathode(VNACOF)to enhance the electronic and spatial effects in the bulk.A range of in-situ,ex-situ characterizations,and DFT calculations profoundly clarify the strengthened ionic/electronic conductivities,structural stability,and Zn^(2+)diffusion kinetics.As a result,the VNACOF displays a superior discharge capacity(529 mA h g^(-1)@0.1 C),rate capabilities(488 mA h g^(-1)@0.5 C,437 mA h g^(-1)@1C),and cycling stability(301 mA h g^(-1)@10 C@5000 cycles@93%)with sufficient energy density(393 W h kg^(-1)),Furthermore,the pouch-cells with high-load(60 mg)also deliver superior cyclic(2 C@178 mA h g^(-1)@1000 cycles@90%)and rate performance(132 mA h g^(-1)@5 C),revealing great application potential for high-energy-density and high-stability AZIBs.
基金funded by the National Natural Science Foundation of China (30901038, 31160468)the State Key Laboratory of Animal Nutrition, Ministry of Science and Technology, China (2004DA125184F1115)the Key Technology Research and Development Program of Guizhou Province, China ([2009]3085)
文摘Reducing dietary cation-anion difference (DCAD) has been proved an effective way to prevent milk fever in dairy cows. Based on the similar physiological gastro-intestinal tract anatomy and metabolic process between female goats and dairy cows, this study was conducted to evaluate the effects of varying DCAD on fluid acid-base status, plasma minerals concentration and anti-oxidative stress capacity of female goats. Urinary pH, plasma Ca, P and Mg; and anti-oxidative stress indices of total superoxide dismutase (T-SOD), hydrogen peroxide (HzO2), glutathione peroxidase (GSH-Px) and malondialdehyde (MDA) were determined to evaluate the effect. Forty-eight Guizhou black female goats ((15±1.9) mon of old, (22.3±3.75) kg of BW) were randomly allocated to 4 blocks of 12 goats each and were fed 1 of 4 diets differed in DCAD level (calculated as Na+K-C1-S, mEq kg-1 DM). Levels of DCAD were preliminarily designed to be control (+ 150 mEq kg^-1 DM, CON), high DCAD (+300 mEq kg^-1 DM, HD), low DCAD (0 mEq kg^-1 DM, LD) and negative DCAD (-150 mEq kg^-1 DM, ND), respectively. A commercial anionic salts (Animate) and sodium bicarbonate (NaHCO3) were supplemented to reduce and increase DCAD level, respectively. There was no difference in dry matter intake for 4 groups of goats. Urine pH was aggressively decreased (P〈0.0001) with reduced DCAD and there was a strong association between DCAD and urine pH (R2=0.793, P〈0.0001). Compared with CON and HD feeding of LD and ND resulted in greater (P〈0.05) plasma Ca concentration. Plasma P level was increased (P〈0.05) when anionic salts were supplemented. The DCAD alteration did not affected (P〉0.05) plasma Mg level. There was no significant (P〉0.05) difference in plasma GSH-Px activity and H202, but anionic salts supplementation in LD and ND significantly increased (P〈0.05) plasma T-SOD activity and tended to reduce MDA (P〈0.1) over HD and CON. Results from this study indicated that reducing DCAD could decrease urine pH and increase plasma Ca concentration of female goats. Additionally, reducing DCAD was helpful to enhance anti-oxidative stress capability of female goats.
基金supported by the National Natural Science Foundation of China(Nos.22122106,22071158,21971171,22305166)the Fundamental Research Funds from Sichuan University(No.2021SCUNL101)the Natural Science Foundation of Sichuan Province(No.2023NSFC1066)。
文摘Finding suitable strategies to effectively enhance the optical properties of materials are the goal being pursued by researchers.Herein,cation-anion synergetic interactions strategy was proposed to develop two novel organic-inorganic hybrid antimony-based optical materials,(C_(3)H_(5)N_(2))Sb F_(2)SO_(4)(I)and(C_(5)H_(6)N)Sb F_(2)SO_(4)(Ⅱ),which were obtained by introducing Sb^(3+)cation containing stereochemically active lone-pair(SCALP)and organicπ-conjugated cations into sulphate system.The synergistic interactions of the organicπ-conjugated cations,the inorganic[SbO_(2)F_(2)]^(3-)seesaw anions and the[SO_(4)]^(2-)distorted tetrahedra anions make their ultraviolet(UV)absorption edges approach 297 and 283 nm,respectively,and raise their birefringence up to 0.193@546 nm and 0.179@546 nm,respectively.Interestingly,although the two compounds have the same stoichiometric ratio and similar one-dimensional(1D)chain structure,they show opposite macroscopic symmetry,where the NCS compound(Ⅱ)exhibits a large secondharmonic generation(SHG)response(1.6 times that of KH_(2)PO_(4)).The two reported compounds are found to be promising UV optical materials in the experimental tests.
基金supported by the National Natural Science Foundation of China (Nos. 31600558 and 31400587)the Natural Science Foundation of Jiangsu, China (No. BK20160590)+1 种基金the Earmarked Fund for Modern Agro-industry Technology Research System of China (No. CARS-19)the Agricultural Science and Technology Innovation Fund of Jiangsu, China (No. CX(13)5016)
文摘Cultivated tea(Camellia sinensis) plants acidify the rhizosphere, and Aluminum(Al) toxicity is recognized as a major limiting factor for plant growth in acidic soils. However, the mechanisms responsible for rhizosphere acidification associated with Al have not been fully elucidated. The present study examined the effect of Al on root-induced rhizosphere acidification, plasma membrane H^+-adenosine triphosphatase(H^+-ATPase) activity, and cation-anion balance in tea plant roots. The exudation of H^+from tea plant roots with or without Al treatment was visualized using an agar sheet with bromocresol purple. The H^+-ATPase activity of plasma membranes isolated from the roots was measured after hydrolysis using the two-phase partition system. The Al treatment strongly enhanced the exudation of H^+, and the acidification of tea plant roots by Al was closely associated with plasma membrane H^+-ATPase activity. The root plasma membrane H^+-ATPase activity increased with Al concentration. The Al content, amount of protons released, and H^+-ATPase activity were significantly higher in roots treated with Al than in those untreated. The results of the cation-anion balance in roots showed an excess of cations relative to anions, with the amount of excess cation uptake increasing with increasing Al concentrations. These suggest that Al-enhanced proton release is associated with plasma membrane H^+-ATPase activity and excess cation uptake. Findings of this study would provide insights into the contributing factors of soil acidification in tea plantations.
基金supported by the National Key R&D Program of China(2018YFB0905600)。
文摘The high-nickel layered cathodes Li[Ni_(x)Co_(y)Mn_(1-x-y)]O_(2)(x≥0.8)with high specific capacity and long cycle life are considered as prospective cathodes for lithium-ion batteries.However,the microcrack formation and poor structural stability give rise to inferior rate performance and undesirable cycling life.Herein,we propose a dual modification strategy combining primary particle structure design and element doping to modify Li[Ni_(0.95)Co_(0.025)Mn_(0.025)]O_(2) cathode by tungsten and fluorine co-doped(W-F-NCM95).The doping of W can convert the microstructure of primary particles to the unique rod-like shape,which is beneficial to enhance the reversibility of phase transition and alleviate the generation of microcracks.F doping is conducive to alleviating the surface side reactions.Thus,due to the synergistic effect of W,F codoping,the obtained W-F-NCM95 cathodes deliver a high initial capacity of 236.1 mA h g^(-1) at 0.1 C and superior capacity retention of 88.7%over 100 cycles at 0.5 C.Moreover,the capacity still maintains73.8%after 500 cycles at 0.5 C and the texture of primary particle is intact.This work provides an available strategy by W and F co-doping to enhance the electrochemistry performance of high-nickel cathodes for practical application.
基金supported by the National Natural Science Foundation of China(22271106,52073286)the Natural Science Foundation of Fujian Province(2006 L2005)。
文摘The rational design and optimization of noble-metal-free semiconductor photocatalysts aim to increase the number of active sites and accelerate the separation and transfer of charges,thereby achieving high-performance hydrogen evolution reactions(HER).In this study,we innovatively designed an S-scheme heterojunction catalyst composed of CdS nanoparticles rich in cationic Cd vacancies(VCCS)and ZnWO4nanorods rich in anionic O vacancies(VOZWO)that regulate the surface electronic states of the catalyst through dual vacancies engineering.Specifically,the introduction of vacancy engineering effectively adjusted the energy level structure of the catalyst,achieving bandgap narrowing,enhancing light absorption capacity,providing hole trapping sites,and creating more active sites.As expected,the optimized VOZWO@VCCS heterojunction exhibited exceptional photocatalytic H_(2)production rates of 11.55 mmol g^(-1)h^(-1)in the absence of noble-metal cocatalysts,which are approximately 462 times and4 times higher than those of pure VOZWO(0.025 mmol g^(-1)h^(-1))and VCCS(2.89 mmol g^(-1)h^(-1)),respectively.In-depth characterization tests and density functional theory(DFT)calculations revealed that the introduction of vacancies significantly reduced the bandgap,improved the transfer efficiency of photoinduced carriers,and validated the charge transfer mechanism of the S-scheme heterojunction.
基金supported by the National Natural Science Foundation of China (92372111,22179070,22279126)the Fundamental Research Funds for the Central Universities (RF1028623157)the Anhui Science Fund for Distinguished Young Scholars(2408085J009)。
文摘Conventional gel polymer electrolytes based on polymers such as poly(ethylene oxide) face inherent limitations in enhancing ionic conductivity and electrochemical stability.Introducing diverse functional groups into the polymer framework enables the precise modulation of its physicochemical properties,thereby influencing the performance of lithium metal batteries.Herein,an in situ dual-crosslinked gel polymer electrolyte based on polyester and polyamide is proposed.This design enables synergistic cation-anion regulation,facilitating continuous Li^(+) transport by abundant ester groups while anchoring the anions by N–H groups.The resulting gel polymer electrolyte exhibits a high ionic conductivity of 0.58 mS cm^(-1)and an elevated Li^(+) transference number of 0.6.The assembled Li||LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2) coin cells achieve 400 cycles at 0.5 C and 300 cycles at 1 C.Furthermore,a 4-layer stacked Li||LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(active material mass loading of 26.7 mg cm^(-2)) pouch cell in lean electrolyte conditions(1.7 g Ah^(-1)) is assembled and sustains 45 cycles without obvious decay.This study provides a strategy of synergistic cationanion regulation in gel polymer electrolytes,offering insights for stable lithium metal batteries.
文摘It used to be held that the cloud point phenomenon was only a characteris-tic of nonionic surfactants alone. Such phenomenon is rarely observed in ionicsurfactants. The present study shows that the mixture of cationic-anionic surfac-tants not only has a krafft point which is the characteristic of an ionic surfactant,but also exhibits the cloud point phenomenon obviously at certain concentrations.
基金Project supported by the National Natural Science Foundation of China (No. 50073019).
文摘Cobait(Ⅱ) nitrate reacted with 1,10-phenanthroline (phen) and 5-sulfosaiicylic acid (H3ssal) to yield the cobait(Ⅰ) complex [Co(phen)2(H2O)2](Hssal)o4H2O (1) and the reaction of 1 with copper acetate led to a novel complex [Co(phen)(H2O)4][Cu2(ssal)2(phen)2]·5H2O (2). These two complexes were cationanion species and the cationic motif [Co(phen)2(H2O)2]^2+of 1 could be converted to [Co(phen)(H2O)4]^2+ in the formation process of new anion [Cu2(phen)2(ssal)2]^2- of 2. In both complexes abundant hydrogen bonds construct different supramolecular architectures, thus the conversion reaction can provide a new path to create novel supramolecular network.