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
Nonflammable gel polymer electrolytes(GPEs)are intriguing owing to their flame-retardancy,high ionic conductivity and nonleakage properties.However,their application is critically hindered by unfavorable interfacial c...Nonflammable gel polymer electrolytes(GPEs)are intriguing owing to their flame-retardancy,high ionic conductivity and nonleakage properties.However,their application is critically hindered by unfavorable interfacial compatibility due to the incorporation of high-reactive solvents.Herein,we present an innovative solvent anchoring strategy to remold Li^(+)solvation structure,thus inducing an effective interfacial protective layer to alleviate adverse solvents decomposition.A nonflammable eutectic GPE(DIPE)is synthesized by in situ incorporating poly-ethoxylated trimethylolpropane triacrylate(PETPTA)polymer skeleton to flame-retardant LiTFSI-sulfolane(SL)-based deep eutectic solvent(DES).The “SL solvent anchoring”strategy is validated to rely on dipole-dipole intermolecular interaction between ACH_(2)groups on the PETPTA polymer skeleton and AO@S groups on SL solvents,which breaks the solvation dominance of SL solvents and directly suppresses their decomposition.It simultaneously facilitates reconstruction of a TFSI--dominated Li^(+)solvation sheath without increasing LiTFSI concentration,thereby fostering anion-derived SEI and CEI protective layers.Dynamic interfacial resistance evolution reveals accelerated interfacial Li^(+)transport kinetics in DIPE.Therefore,Li|DIPE|Li cell delivers remarkably enhanced Li reversibility with cycle life over 1000 h at 0.1 mA cm^(-2)and Li|DIPE|LCO cell achieves 90.7%capacity retention over 700 cycles at 0.3 C.This study opens an emerging avenue to remold Li^(+)solvation environment and enhance interfacial compatibility in GPE by manipulating the solvent-anchoring effect.展开更多
Uncontrolled dendrite growth,sluggish reaction kinetics,and drastic side reactions on the anodeelectrolyte interface are the main obstacles that restrict the application prospect of aqueous zinc-ion batteries.Traditio...Uncontrolled dendrite growth,sluggish reaction kinetics,and drastic side reactions on the anodeelectrolyte interface are the main obstacles that restrict the application prospect of aqueous zinc-ion batteries.Traditional glass fiber(GF)separator with chemical inertness is almost ineffective in restricting these challenges.Herein,inspired by the ionic enrichment behavior of seaweed plants,a facile biomass species,anionic sodium alginate(SA),is purposely decorated on the commercial GF separator to tackle these issues towards Zn anode.Benefiting from the abundant zincophilic functional groups and superior mechanical strength properties,the as-obtained SA@GF separator could act as ion pump to boost the Zn^(2+)transference number(0.68),reduce the de-solvation energy barrier of hydrated Zn^(2+),and eliminate the undesired concentration polarization effect,which are verified by experimental tests,theoretical calculations,and finite element simulation,respectively.Based on these efficient modulation mechanisms,the SA@GF separator can synchronously achieve well-aligned Zn deposition and the suppression of parasitic side-reactions.Therefore,the Zn‖Zn coin cell integrated with SA@GF separator could yield a prolonged calendar lifespan over 1230 h(1 mA cm^(-2)and 1 mAh cm^(-2)),exhibiting favorable competitiveness with previously reported separator modification strategies.Impressively,the Zn-MnO_(2)full and pouch cell assembled with the SA@GF separator also delivered superior cycling stability and rate performance,further verifying its practical application effect.This work provides a new design philosophy to stabilize the Zn anode from the aspect of separator.展开更多
The interfacial kinetics,micellization and interfacial characteristics of the synergetic extrac- tion system,D_2EHPA-H_2RPA-Al^(3+),have been studied.H_2RPA is a single long chain alkyl phosphate.We have found that H_...The interfacial kinetics,micellization and interfacial characteristics of the synergetic extrac- tion system,D_2EHPA-H_2RPA-Al^(3+),have been studied.H_2RPA is a single long chain alkyl phosphate.We have found that H_2RPA in the mixed extractant system strongly exhibits the characteristics of micellization and interfacial activity.As the concentration of D_2EHPA in- creases,the micellization and interracial activity of H_2RPA decrease.The interfacial adsorption behaviour of H_2RPA is opposite to that of D_2EHPA.It was proved that the kine- tics of non-micella mixed extraction system was controlled by the chemical reaction at inter- face,and the reaction rate equation was obtained.This non-micella mixed extraction system is expected to be used in the future.展开更多
The kinetics of solvent.extraction of aluminum with di-2-ethylhexyl phosphoric acid(DEHPA)in n-heptane have been studied in a constant interfacial area cell.A HC1-KHC8H404(potassium biphthalate.KHL)buffer solution was...The kinetics of solvent.extraction of aluminum with di-2-ethylhexyl phosphoric acid(DEHPA)in n-heptane have been studied in a constant interfacial area cell.A HC1-KHC8H404(potassium biphthalate.KHL)buffer solution was used to maintain a constant pH during extraction.The effects of the concentration of aluminum,pH,the concentration of the extractant,the interfacial area and the temperature on the extraction rate were investigated.A method has been invented to determine amont of the extracted aluminum in the organic phase with 8-hydroxyquinoline.Based on calculation of the coordination states of the aluminum ions and their contribution to the reaction rate,a raaction mechanism which includes two main reaction paths,has been proposed to describe the process.One path starts from Al(H_(2)O)6^(+).and the other starts from Al(H_(2)O)6^(+).The reaction could take place both in the aqueous phase and at the interface.The main reaction region could be changed as the conditions of extraction were changed.When[HA]<0.03 mol/L the process was controlled by the interfacial reaction,and when[HA]>0.03 mol/L it was shifted to a homogeneous aqueous solution reaction.展开更多
Achieving simultaneous fast-charging capabilities and low-temperature adaptability in graphite-based lithium-ion batteries(LIBs)with an acceptable cycle life remains challenging.Herein,an ether-based electrolyte with ...Achieving simultaneous fast-charging capabilities and low-temperature adaptability in graphite-based lithium-ion batteries(LIBs)with an acceptable cycle life remains challenging.Herein,an ether-based electrolyte with temperature-adaptive Li^(+)solvation structure is designed for graphite,and stable Li^(+)/solvent co-intercalation has been achieved at subzero.As revealed by in-situ variable temperature(-20℃)X-ray diffraction(XRD),the poor compatibility of graphite in ether-based electrolyte at 25℃is mainly due to the continuous electrolyte decomposition and the in-plane rearrangement below0.5 V.Former results in a significant irreversible capacity,while latter maintains graphite in a prolonged state of extreme expansion,ultimately leading to its exfoliation and failure.In contrast,low temperature triggers the rearra ngement of Li^(+)solvation structu re with stronger Li^(+)/solvent binding energy and sho rter Li^(+)-O bond length,which is conducive for reversible Li^(+)/solvent co-intercalation and reducing the time of graphite in an extreme expansion state.In addition,the co-intercalation of solvents minimizes the interaction between Li-ions and host graphite,endowing graphite with fast diffusion kinetics.As expected,the graphite anode delivers about 84%of the capacity at room temperature at-20℃.Moreover,within6 min,about 83%,73%,and 43%of the capacity could be charged at 25,-20,and-40℃,respectively.展开更多
Sodium-ion batteries stand a chance of enabling fast charging ability and long lifespan while operating at low temperature(low-T).However,sluggish kinetics and aggravated dendrites present two major challenges for ano...Sodium-ion batteries stand a chance of enabling fast charging ability and long lifespan while operating at low temperature(low-T).However,sluggish kinetics and aggravated dendrites present two major challenges for anodes to achieve the goal at low-T.Herein,we propose an interlayer confined strategy for tailoring nitrogen terminals on Ti_(3)C_(2) MXene(Ti_(3)C_(2)-N_(funct)) to address these issues.The introduction of nitrogen terminals endows Ti_(3)C_(2)-N_(funct) with large interlayer space and charge redistribution,improved conductivity and sufficient adsorption sites for Na^(+),which improves the possibility of Ti_(3)C_(2) for accommodating more Na atoms,further enhancing the Na^(+) storage capability of Ti_(3)C_(2).As revealed,Ti_(3)C_(2)-N_(funct) not only possesses a lower Na-ion diffusion energy barrier and charge trans-fer activation energy,but also exhibits Na^(+)-solvent co-intercalation behavior to circumvent a high de-solvation energy barrier at low-T.Besides,the solid electrolyte interface dominated by inorganic com-pounds is more beneficial for the Na^(+)transfer at the electrode/electrolyte interface.Compared with of the unmodified sample,Ti_(3)C_(2)-Nfunct exhibits a twofold capacity(201 mAh g^(-1)),fast-charging ability(18 min at 80% capacity retention),and great superiority in cycle life(80.9%@5000 cycles)at -25℃.When coupling with Na_(3)V_(2)(PO_(4))_(2)F_(3) cathode,the Ti_(3)C_(2)-N_(funct)//NVPF exhibits high energy density and cycle stability at -25℃.展开更多
Photocatalytic water oxidation based on semiconductors usually suffers from poor charge transfer from the bulk to the interface,which is necessary for oxygen generation.Here,we construct a hybrid artificial photosynth...Photocatalytic water oxidation based on semiconductors usually suffers from poor charge transfer from the bulk to the interface,which is necessary for oxygen generation.Here,we construct a hybrid artificial photosynthesis system for photocatalytic water oxidation.The system consists of BiVO4as the light harvester,a transitional metal complex(M(dca)2,M=Co,Ni,dca:dicyanamide)as the water oxidation catalyst,and S2O82?as a sacrificial electron acceptor.The system exhibits enhanced oxygen evolution activity when M(dca)2is introduced.The BiVO4/Co(dca)2and Bi‐VO4/Ni(dca)2systems exhibit excellent oxygen evolution rates of508.1and297.7μmol/(h·g)compared to the pure BiVO4which shows a photocatalytic oxygen evolution rate of252.2μmol/(h·g)during6h of photocatalytic reaction.Co(dca)2is found to be more effective than Ni(dca)2as a water oxidation catalyst.The enhanced photocatalytic performance is ascribed to the M(dca)2‐engineered BiVO4/electrolyte interface energetics,and to the M(dca)2‐catalyzed surface water oxidation.These two factors lead to a decrease in the energy barrier for hole transfer from the bulk to the surface of BiVO4,which promotes the water oxidation kinetics.展开更多
Low temperature aqueous batteries(LT-ABs)have attracted extensive attention recent years.The LT-ABs suffer from electrolyte freezing,slow ionic diffusion and sluggish interfacial redox kinetics at low temperature.In t...Low temperature aqueous batteries(LT-ABs)have attracted extensive attention recent years.The LT-ABs suffer from electrolyte freezing,slow ionic diffusion and sluggish interfacial redox kinetics at low temperature.In this review,we discuss physicochemical properties of aqueous electrolytes in terms of phase diagram,ion diffusion and interfacial redox kinetics to guide the design of low temperature aqueous electrolytes(LT-AEs).Firstly,the characteristics of equilibrium and non equilibrium phase diagrams are introduced to analyze the antifreezing mechanisms and propose design strategies for LT-AEs.Then,the temperature/concentration/charge carrier dependence conductivity characteristics in aqueous electrolytes are reviewed to comprehend and regulate the ion diffusion kinetics.Moreover,we introduce interfacial studies in aqueous and non-aqueous batteries and propose potential improvement strategies for interfacial redox kinetics in LT-ABs.Finally,we summarize design strategies of LT-AEs for developing high performance LT-ABs.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supported by the National Natural Science Foundation of China(52172214,52472220,52272221,52171182)Postdoctoral Innovation Project of Shandong Province(202102003)+2 种基金The“New 20 Clauses about Colleges and Universities”Program of Jinan(202228107)the Qilu Young Scholar Programthe HPC Cloud Platform of Shandong University are also acknowledged。
文摘Nonflammable gel polymer electrolytes(GPEs)are intriguing owing to their flame-retardancy,high ionic conductivity and nonleakage properties.However,their application is critically hindered by unfavorable interfacial compatibility due to the incorporation of high-reactive solvents.Herein,we present an innovative solvent anchoring strategy to remold Li^(+)solvation structure,thus inducing an effective interfacial protective layer to alleviate adverse solvents decomposition.A nonflammable eutectic GPE(DIPE)is synthesized by in situ incorporating poly-ethoxylated trimethylolpropane triacrylate(PETPTA)polymer skeleton to flame-retardant LiTFSI-sulfolane(SL)-based deep eutectic solvent(DES).The “SL solvent anchoring”strategy is validated to rely on dipole-dipole intermolecular interaction between ACH_(2)groups on the PETPTA polymer skeleton and AO@S groups on SL solvents,which breaks the solvation dominance of SL solvents and directly suppresses their decomposition.It simultaneously facilitates reconstruction of a TFSI--dominated Li^(+)solvation sheath without increasing LiTFSI concentration,thereby fostering anion-derived SEI and CEI protective layers.Dynamic interfacial resistance evolution reveals accelerated interfacial Li^(+)transport kinetics in DIPE.Therefore,Li|DIPE|Li cell delivers remarkably enhanced Li reversibility with cycle life over 1000 h at 0.1 mA cm^(-2)and Li|DIPE|LCO cell achieves 90.7%capacity retention over 700 cycles at 0.3 C.This study opens an emerging avenue to remold Li^(+)solvation environment and enhance interfacial compatibility in GPE by manipulating the solvent-anchoring effect.
基金supported by research grants from the National Natural Science Foundation of China(52173235,22008193,52106110)the Key Research and Development Project of Hainan Province(ZDYF2024SHFZ038)+2 种基金Venture&Innovation Support Program for Chongqing Overseas Returnees(CX2021018)Research Foundation of Chongqing University of Science and Technology(ckrc2021071)Numerical computations were performed on Hefei Advanced Computing Center.
文摘Uncontrolled dendrite growth,sluggish reaction kinetics,and drastic side reactions on the anodeelectrolyte interface are the main obstacles that restrict the application prospect of aqueous zinc-ion batteries.Traditional glass fiber(GF)separator with chemical inertness is almost ineffective in restricting these challenges.Herein,inspired by the ionic enrichment behavior of seaweed plants,a facile biomass species,anionic sodium alginate(SA),is purposely decorated on the commercial GF separator to tackle these issues towards Zn anode.Benefiting from the abundant zincophilic functional groups and superior mechanical strength properties,the as-obtained SA@GF separator could act as ion pump to boost the Zn^(2+)transference number(0.68),reduce the de-solvation energy barrier of hydrated Zn^(2+),and eliminate the undesired concentration polarization effect,which are verified by experimental tests,theoretical calculations,and finite element simulation,respectively.Based on these efficient modulation mechanisms,the SA@GF separator can synchronously achieve well-aligned Zn deposition and the suppression of parasitic side-reactions.Therefore,the Zn‖Zn coin cell integrated with SA@GF separator could yield a prolonged calendar lifespan over 1230 h(1 mA cm^(-2)and 1 mAh cm^(-2)),exhibiting favorable competitiveness with previously reported separator modification strategies.Impressively,the Zn-MnO_(2)full and pouch cell assembled with the SA@GF separator also delivered superior cycling stability and rate performance,further verifying its practical application effect.This work provides a new design philosophy to stabilize the Zn anode from the aspect of separator.
文摘The interfacial kinetics,micellization and interfacial characteristics of the synergetic extrac- tion system,D_2EHPA-H_2RPA-Al^(3+),have been studied.H_2RPA is a single long chain alkyl phosphate.We have found that H_2RPA in the mixed extractant system strongly exhibits the characteristics of micellization and interfacial activity.As the concentration of D_2EHPA in- creases,the micellization and interracial activity of H_2RPA decrease.The interfacial adsorption behaviour of H_2RPA is opposite to that of D_2EHPA.It was proved that the kine- tics of non-micella mixed extraction system was controlled by the chemical reaction at inter- face,and the reaction rate equation was obtained.This non-micella mixed extraction system is expected to be used in the future.
基金supported by China National Natural Science Foundation。
文摘The kinetics of solvent.extraction of aluminum with di-2-ethylhexyl phosphoric acid(DEHPA)in n-heptane have been studied in a constant interfacial area cell.A HC1-KHC8H404(potassium biphthalate.KHL)buffer solution was used to maintain a constant pH during extraction.The effects of the concentration of aluminum,pH,the concentration of the extractant,the interfacial area and the temperature on the extraction rate were investigated.A method has been invented to determine amont of the extracted aluminum in the organic phase with 8-hydroxyquinoline.Based on calculation of the coordination states of the aluminum ions and their contribution to the reaction rate,a raaction mechanism which includes two main reaction paths,has been proposed to describe the process.One path starts from Al(H_(2)O)6^(+).and the other starts from Al(H_(2)O)6^(+).The reaction could take place both in the aqueous phase and at the interface.The main reaction region could be changed as the conditions of extraction were changed.When[HA]<0.03 mol/L the process was controlled by the interfacial reaction,and when[HA]>0.03 mol/L it was shifted to a homogeneous aqueous solution reaction.
基金financially supported by the National Natural Science Foundation of China(52372191)the Natural Science Foundation of Fujian Province(2023J05047)+1 种基金the Natural Science Foundation of Xiamen,China(3502Z202372036)the support of the High-Performance Computing Center(HPCC)at Harbin Institute of Technology on first-principles calculations.
文摘Achieving simultaneous fast-charging capabilities and low-temperature adaptability in graphite-based lithium-ion batteries(LIBs)with an acceptable cycle life remains challenging.Herein,an ether-based electrolyte with temperature-adaptive Li^(+)solvation structure is designed for graphite,and stable Li^(+)/solvent co-intercalation has been achieved at subzero.As revealed by in-situ variable temperature(-20℃)X-ray diffraction(XRD),the poor compatibility of graphite in ether-based electrolyte at 25℃is mainly due to the continuous electrolyte decomposition and the in-plane rearrangement below0.5 V.Former results in a significant irreversible capacity,while latter maintains graphite in a prolonged state of extreme expansion,ultimately leading to its exfoliation and failure.In contrast,low temperature triggers the rearra ngement of Li^(+)solvation structu re with stronger Li^(+)/solvent binding energy and sho rter Li^(+)-O bond length,which is conducive for reversible Li^(+)/solvent co-intercalation and reducing the time of graphite in an extreme expansion state.In addition,the co-intercalation of solvents minimizes the interaction between Li-ions and host graphite,endowing graphite with fast diffusion kinetics.As expected,the graphite anode delivers about 84%of the capacity at room temperature at-20℃.Moreover,within6 min,about 83%,73%,and 43%of the capacity could be charged at 25,-20,and-40℃,respectively.
基金the National Natural Sci-ence Foundation of China(Grant Nos.21673064,51902072 and 22109033)Heilongjiang Touyan Team(Grant No.HITTY-20190033)+1 种基金Fundamental Research Funds for the Central Universities(Grant Nos.HIT.NSRIF.2019040 and 2019041)State Key Laboratory of Urban Water Resource and Environment(Harbin Institute of Technology)(Grant No.2020 DX11).
文摘Sodium-ion batteries stand a chance of enabling fast charging ability and long lifespan while operating at low temperature(low-T).However,sluggish kinetics and aggravated dendrites present two major challenges for anodes to achieve the goal at low-T.Herein,we propose an interlayer confined strategy for tailoring nitrogen terminals on Ti_(3)C_(2) MXene(Ti_(3)C_(2)-N_(funct)) to address these issues.The introduction of nitrogen terminals endows Ti_(3)C_(2)-N_(funct) with large interlayer space and charge redistribution,improved conductivity and sufficient adsorption sites for Na^(+),which improves the possibility of Ti_(3)C_(2) for accommodating more Na atoms,further enhancing the Na^(+) storage capability of Ti_(3)C_(2).As revealed,Ti_(3)C_(2)-N_(funct) not only possesses a lower Na-ion diffusion energy barrier and charge trans-fer activation energy,but also exhibits Na^(+)-solvent co-intercalation behavior to circumvent a high de-solvation energy barrier at low-T.Besides,the solid electrolyte interface dominated by inorganic com-pounds is more beneficial for the Na^(+)transfer at the electrode/electrolyte interface.Compared with of the unmodified sample,Ti_(3)C_(2)-Nfunct exhibits a twofold capacity(201 mAh g^(-1)),fast-charging ability(18 min at 80% capacity retention),and great superiority in cycle life(80.9%@5000 cycles)at -25℃.When coupling with Na_(3)V_(2)(PO_(4))_(2)F_(3) cathode,the Ti_(3)C_(2)-N_(funct)//NVPF exhibits high energy density and cycle stability at -25℃.
基金supported by the National Natural Science Foundation of China (51672210, 51323011, 51236007)~~
文摘Photocatalytic water oxidation based on semiconductors usually suffers from poor charge transfer from the bulk to the interface,which is necessary for oxygen generation.Here,we construct a hybrid artificial photosynthesis system for photocatalytic water oxidation.The system consists of BiVO4as the light harvester,a transitional metal complex(M(dca)2,M=Co,Ni,dca:dicyanamide)as the water oxidation catalyst,and S2O82?as a sacrificial electron acceptor.The system exhibits enhanced oxygen evolution activity when M(dca)2is introduced.The BiVO4/Co(dca)2and Bi‐VO4/Ni(dca)2systems exhibit excellent oxygen evolution rates of508.1and297.7μmol/(h·g)compared to the pure BiVO4which shows a photocatalytic oxygen evolution rate of252.2μmol/(h·g)during6h of photocatalytic reaction.Co(dca)2is found to be more effective than Ni(dca)2as a water oxidation catalyst.The enhanced photocatalytic performance is ascribed to the M(dca)2‐engineered BiVO4/electrolyte interface energetics,and to the M(dca)2‐catalyzed surface water oxidation.These two factors lead to a decrease in the energy barrier for hole transfer from the bulk to the surface of BiVO4,which promotes the water oxidation kinetics.
基金The work described in this paper was fully supported by a grant from the Research Grant Council of the Hong Kong Special Administrative Region,China(No.CUHK14304520).
文摘Low temperature aqueous batteries(LT-ABs)have attracted extensive attention recent years.The LT-ABs suffer from electrolyte freezing,slow ionic diffusion and sluggish interfacial redox kinetics at low temperature.In this review,we discuss physicochemical properties of aqueous electrolytes in terms of phase diagram,ion diffusion and interfacial redox kinetics to guide the design of low temperature aqueous electrolytes(LT-AEs).Firstly,the characteristics of equilibrium and non equilibrium phase diagrams are introduced to analyze the antifreezing mechanisms and propose design strategies for LT-AEs.Then,the temperature/concentration/charge carrier dependence conductivity characteristics in aqueous electrolytes are reviewed to comprehend and regulate the ion diffusion kinetics.Moreover,we introduce interfacial studies in aqueous and non-aqueous batteries and propose potential improvement strategies for interfacial redox kinetics in LT-ABs.Finally,we summarize design strategies of LT-AEs for developing high performance LT-ABs.
