（R）-2-hydroxy-3-phenylpropionic acid （PIP,） is an ideal antimicrobial compound with broad-spectrum activity against a wide range of Gram-positive bacteria, some Gram-negative bacteria, and fungi. We studied the bi...（R）-2-hydroxy-3-phenylpropionic acid （PIP,） is an ideal antimicrobial compound with broad-spectrum activity against a wide range of Gram-positive bacteria, some Gram-negative bacteria, and fungi. We studied the bioconversion of phenylpyruvate （PPA） to PLA using whole recombinant Escherichia coli cells in a series of buffer/organic solvent systems. Octane was found to be the best organic solvent. The optimum volume ratio of the water phase to the n-octane phase, conversion temperature, substrate concentration, and cell concentration were 6：4, 40 ℃, 12.5 g/L, and 30 g/L wet cells, respectively. Under the optimized conditions, the average PLA productivity in the aqueous/ n-octane system was 30.69% higher than that in the aqueous system, and 32.31 g/L PLA was obtained with the use of a stirred reactor （2-L scale）. Taken together, our findings indicated that PLA biosynthesis was more efficient in an aqueous/n-octane biphasic system than in a monophasic aqueous system. The proposed biphasic system is an effective strategy for enhancing PLA yield and the biosynthesis of its analogues.展开更多
Aqueous alkali metal-ion batteries(AAMIBs)have been recognized as emerging electrochemical energy storage technologies for grid-scale applications owning to their intrinsic safety,cost-effectiveness,and environmental ...Aqueous alkali metal-ion batteries(AAMIBs)have been recognized as emerging electrochemical energy storage technologies for grid-scale applications owning to their intrinsic safety,cost-effectiveness,and environmental sustainability.However,the practical application of AAMIBs is still severely constrained by the tendency of aqueous electrolytes to freeze at low temperatures and decompose at high temperatures,limiting their operational temperature range.Considering the urgent need for energy systems with higher adaptability and resilience at various application scenarios,designing novel electrolytes via structure modulation has increasingly emerged as a feasible and economical strategy for the performance optimization of wide-temperature AAMIBs.In this review,the latest advancement of wide-temperature electrolytes for AAMIBs is systematically and comprehensively summarized.Specifically,the key challenges,failure mechanisms,correlations between hydrogen bond behaviors and physicochemical properties,and thermodynamic and kinetic interpretations in aqueous electrolytes are discussed firstly.Additionally,we offer forward-looking insights and innovative design principles for developing aqueous electrolytes capable of operating across a broad temperature range.This review is expected to provide some guidance and reference for the rational design and regulation of widetemperature electrolytes for AAMIBs and promote their future development.展开更多
Aqueous zinc-ion batteries(AZIBs)have garnered considerable attention as promising post-lithium energy storage technologies owing to their intrinsic safety,cost-effectiveness,and competitive gravimetric energy density...Aqueous zinc-ion batteries(AZIBs)have garnered considerable attention as promising post-lithium energy storage technologies owing to their intrinsic safety,cost-effectiveness,and competitive gravimetric energy density.However,their practical commercialization is hindered by critical challenges on the anode side,including dendrite growth and parasitic reactions at the anode/electrolyte interface.Recent studies highlight that rational electrolyte structure engineering offers an effective route to mitigate these issues and strengthen the electrochemical performance of the zinc metal anode.In this review,we systematically summarize state-of-the-art strategies for electrolyte optimization,with a particular focus on the zinc salts regulation,electrolyte additives,and the construction of novel electrolytes,while elucidating the underlying design principles.We further discuss the key structure–property relationships governing electrolyte behavior to provide guidance for the development of next-generation electrolytes.Finally,future perspectives on advanced electrolyte design are proposed.This review aims to serve as a comprehensive reference for researchers exploring high-performance electrolyte engineering in AZIBs.展开更多
Aqueous zinc metal batteries(AZMBs)face significant challenges in achieving reversibility and cycling stability,primarily due to hydrogen evolution reactions(HER)and zinc dendrite growth.In this study,by employing car...Aqueous zinc metal batteries(AZMBs)face significant challenges in achieving reversibility and cycling stability,primarily due to hydrogen evolution reactions(HER)and zinc dendrite growth.In this study,by employing carefully designed cells that approximate the structural characteristics of practical batteries,we revisit this widely held view through in-operando X-ray radiography to examine zinc dendrite formation and HER under nearpractical operating conditions.While conventional understanding emphasizes the severity of these processes,our findings suggest that zinc dendrites and HER are noticeably less pronounced in dense,real-operation configurations compared to modified cells,possibly due to a more uniform electric field and the suppression of triple-phase boundaries.This study indicates that other components,such as degradation at the cathode current collector interface and configuration mismatches within the full cell,may also represent important barriers to the practical application of AZMBs,particularly during the early stages of electrodeposition.展开更多
The bimetallic NiCu/SAPO-11 catalysts were prepared by co-impregnation, sequential impregnation, coprecipitation, and mechanical mixing methods. Powder X-ray diffraction, nitrogen adsorption-desorption,temperature-pro...The bimetallic NiCu/SAPO-11 catalysts were prepared by co-impregnation, sequential impregnation, coprecipitation, and mechanical mixing methods. Powder X-ray diffraction, nitrogen adsorption-desorption,temperature-programmed desorption of ammonia, transmission electron microscopy, temperatureprogrammed reduction of hydrogen, and X-ray photoelectron spectroscopy were used to characterize the physicochemical properties of the catalysts. The catalytic performance of the catalysts was assessed by the hydroisomerization of n-octane. Results indicated that the conversion of n-octane and selectivity to n-octane isomers were related to the preparation methods of the catalysts. The catalysts with Ni-Cu alloy effectively restrained the hydrogenolysis reaction that decreases the selectivity of isomerization. The catalyst prepared by the mechanical mixing of NiO and CuO hardly formed Ni-Cu alloy, showing obvious hydrogenolysis and low selectivity to n-octane isomers. The unbalance between the metal and acid sites resulted in the low conversion of n-octane and selectivity to n-octane isomers. Among all the catalysts,the catalyst prepared by the co-impregnation method exhibited high catalytic activity and selectivity to n-octane isomers.展开更多
SAPO-11 molecular sieves were synthesized using silica sol, hydrophilic fumed silica, and tetraethyl orthosilicate（TEOS） as silicon precursors. Their physicochemical properties were characterized using XRD,SEM, nitr...SAPO-11 molecular sieves were synthesized using silica sol, hydrophilic fumed silica, and tetraethyl orthosilicate（TEOS） as silicon precursors. Their physicochemical properties were characterized using XRD,SEM, nitrogen adsorption-desorption, Py-IR, NH;-TPD, EDS, and;Al,;P,;Si MAS NMR techniques. The catalytic performance was assessed in the hydroisomerization of n-octane. The results showed that the silicon precursors influenced the physicochemical properties and catalytic performance of SAPO-11. SAPO-11 synthesized using hydrophilic fumed silica as silicon precursor showed higher silicon distribution and had more medium acid sites. SAPO-11 synthesized using TEOS as silicon precursor had more silicon content, but more silicon islands formed in its framework. The depolymerization of silicon precursors might affect the silicon content and distribution in SAPO-11. In the hydroisomerization of n-octane, the catalytic activity strongly depended on the number of medium acid sites instead of the number of total acid sites.SAPO-11 synthesized using hydrophilic fumed silica as silicon precursor exhibited higher catalytic activity than the other samples because it has more medium acid sites.展开更多
The catalyst NiW/HSAPO-11 was prepared by impregnating Ni and W onto HSAPO-11 zeolite with two different methods. The isomerization and aromatization properties were investigated with an microreactor using n-octane ...The catalyst NiW/HSAPO-11 was prepared by impregnating Ni and W onto HSAPO-11 zeolite with two different methods. The isomerization and aromatization properties were investigated with an microreactor using n-octane as a feedstock. NiW/HSAPO-11 shows a high hydroconversion activity of n-octane, and the optimum operating parameters for the catalyst to produce high octane number products were: 400℃, 2.0MPa, VH2:Vn-octane= 400:1, liquid hourly space velocity LHSV=1.0h-1. Under the optimum reaction condition, the conversion efficiency, C5 liquid + product selectivity, isomerization and aromatization product selectivity were 69.80%, 56.95%, 79.73% and 1.29% respectively. The catalyst (S1) impregnated with Ni and W after the HSAPO-11 zeolite was combined with Al2O3 matrix, performed better than the catalyst (S2) impregnated with Ni and W before combining with the Al2O3 matrix.展开更多
A bifunctional catalyst Pt/HY-β was prepared from a bimicroporous composite zeolite Y-β. Characterization results showed that the specific surface area, pore volume, and acid amount of the catalyst Pt/HY-β all decr...A bifunctional catalyst Pt/HY-β was prepared from a bimicroporous composite zeolite Y-β. Characterization results showed that the specific surface area, pore volume, and acid amount of the catalyst Pt/HY-β all decreased compared to the original zeolite. The catalytic performance of this catalyst in n-octane hydroisomerization was investigated in a fixed bed stainless steel tubular reactor. The results showed that at a hydrogen/n-octane volume ratio of 1000, pressure of 0.6 MPa, temperature of 230 ℃ and LHSV of 3 h^-1, the conversion of n-octane, yield of liquid, hydrocracking rate and yield of iso-octane were 52.32%, 88.66%, 12.60%, 39.51%, respectively.展开更多
Optimized calculations of 75 PCDDs and their parent DD were carded out at the B3LYP/6-31G＊ level by density functional theory （DFT） method. The structural parameters were obtained and significant correlation betwee...Optimized calculations of 75 PCDDs and their parent DD were carded out at the B3LYP/6-31G＊ level by density functional theory （DFT） method. The structural parameters were obtained and significant correlation between the C1 substitution position and some structural parameters was found. Consequently, the number of C1 substitution positions was taken as theoretical descriptors to establish two novel QSPR models for predicting lgKow and -lgSw of all PCDD congeners. The two models achieved in this work contain two variables （Na and Nβ）, of which r = 0.9312, 0.9965 and SD = 0.27, 0.12 respectively, and t values are all large. The variation inflation factors （VIF） of variables in the two models herein are both less than 5.0, suggesting high accuracy of the lgKow and -lgSw predicting models, and the results of cross-validation test also show that the two models exhibit optimum stability and good predictive power. By comparison, the correlation and predictive ability of the present work are more advantageous than those obtained using semi-empirical AM1 and GC-RI methods.展开更多
A seed-directed approach to synthesizing Fe ZSM-22 zeolite without organic structure directing agent(OSDA)was developed by using Fe-rich diatomite as all aluminum and iron sources.The Fe ZSM-22zeolite with optimal cry...A seed-directed approach to synthesizing Fe ZSM-22 zeolite without organic structure directing agent(OSDA)was developed by using Fe-rich diatomite as all aluminum and iron sources.The Fe ZSM-22zeolite with optimal crystallinity and purity can be obtained by systematically adjusting feed composition and synthesis conditions.Characterizations show that Fe ZSM-22 zeolite synthesized with OSDA-free owns high crystallinity,obvious thin needle-shaped morphology and high Bronsted/Lewis acid ratio.Significantly,when used for n-octane hydroisomerization reaction,its derived catalyst exhibits the best catalytic performance reflected by the highest selectivity to C_(8)isomers compared to the two reference catalysts prepared based on a Fe-containing and a Fe-free ZSM-22 synthesized through an OSDA-directed route from natural diatomite and conventional chemicals,respectively.This work provides an alternative route to sustainably synthesizing heteroatomic zeolites with high performance.展开更多
Aqueous zinc-ion electrochromic(EC)technology,boasting the capability to fulfill both safety and cost-ef⁃fectiveness requirements,is garnering extensive attention in various application areas including smart windows,t...Aqueous zinc-ion electrochromic(EC)technology,boasting the capability to fulfill both safety and cost-ef⁃fectiveness requirements,is garnering extensive attention in various application areas including smart windows,thermal management,displays,and camouflage.However,typical inorganic EC materials,such as tungsten oxides(WO_(3)),of⁃ten suffer from slow ion diffusion kinetics and limited optical contrast within the aqueous Zn^(2+)electrolyte because of the large size and strong Coulombic interactions of the Zn^(2+),which limits their wide applicability.Here,ordered WO_(3)nanowire films,constructed by a one-step grazing angle deposition method,is demonstrated to boost the response speed and optical contrast during EC phenomena.Compared with dense films,the ordered WO_(3)nanowire films with a porosity of 44.6%demonstrate anti-reflective property and excellent comprehensive EC performance,including fast response time(3.6 s and 1.2 s for coloring and bleaching,respectively),large optical contrast(66.6%at 700 nm)and high col⁃oration efficiency(64.3 cm^(2)·C^(-1)).A large-area prototype EC device(17 cm×12 cm)with fast color-switching is also successfully achieved.Mechanistic studies show that the improved performance is mainly due to the ordered porous nanowire structures,which provides direct electron transfer paths and sufficient interfacial contacts,thus simultaneously enhancing the electrochemical activity and fast redox kinetics.This study provides a simple and effective strategy to im⁃prove the performance of tungsten oxide-based aqueous zinc ion EC materials and devices.展开更多
As battery technology evolves and demand for efficient energy storage solutions,aqueous zinc ion batteries(AZIBs)have garnered significant attention due to their safety and environmental benefits.However,the stability...As battery technology evolves and demand for efficient energy storage solutions,aqueous zinc ion batteries(AZIBs)have garnered significant attention due to their safety and environmental benefits.However,the stability of cathode materials under high-voltage conditions remains a critical challenge in improving its energy density.This review systematically explores the failure mechanisms of high-voltage cathode materials in AZIBs,including hydrogen evolution reaction,phase transformation and dissolution phenomena.To address these challenges,we propose a range of advanced strategies aimed at improving the stability of cathode materials.These strategies include surface coating and doping techniques designed to fortify the surface properties and structure integrity of the cathode materials under high-voltage conditions.Additionally,we emphasize the importance of designing antioxidant electrolytes,with a focus on understanding and optimizing electrolyte decomposition mechanisms.The review also highlights the significance of modifying conductive agents and employing innovative separators to further enhance the stability of AZIBs.By integrating these cutting-edge approaches,this review anticipates substantial advancements in the stability of high-voltage cathode materials,paving the way for the broader application and development of AZIBs in energy storage.展开更多
Optimized calculation of dibenzofuran （DF） and 135 polychlorinated dibenzofurans （PCDFs） was carried out at the B3LYP/6-31G＊ level in GAUSSIAN 98 program. Based on the theoretical linear solvation energy relation...Optimized calculation of dibenzofuran （DF） and 135 polychlorinated dibenzofurans （PCDFs） was carried out at the B3LYP/6-31G＊ level in GAUSSIAN 98 program. Based on the theoretical linear solvation energy relationship （TLSER） model, the obtained structural parameters were taken as theoretical descriptors to establish the novel quantitative structureproperty relationship （QSPR） model for predicting n-octanol/water partition coefficients （lgKow） of PCDFs. The new model of lgKow achieved in this work contains three variables： energy of the highest occupied molecular orbital （EHOMO）, the most negative atomic partial charge （q^-） and average molecular polarizability （a）, of which R^2= 0.9011 and SD = 0,17 with larger t values. In addition, the variation inflation factors （VIF） of variables in the present model are all less than 5.5, suggesting high accuracy of the lgKow model. And the results of cross-validation test （q^2 = 0.8688） and method validation also show this model exhibits optimum stability and better predictive power than semi-empirical method. At the same time, it is found that the aqueous solubility （-lgSw） has high relative correlation with constant volume molar heat capacity （Cv^0）, of which R^2 = 0.9777 and SD = 0.22. Moreover, lgKow and -lgSw values of all PCDF congeners were predicted respectively.展开更多
To achieve the target of carbon neutrality,it is crucial to develop an efficient and green synthesis methodology with good atomic economy to achieve sufficient utilization of energy and sustainable development.Photoin...To achieve the target of carbon neutrality,it is crucial to develop an efficient and green synthesis methodology with good atomic economy to achieve sufficient utilization of energy and sustainable development.Photoinduced electron transfer reversible addition-fragmentation chain-transfer(PET-RAFT)polymerization is a precise methodology for constructing polymers with well-defined structures.However,conventional semiconductor-mediated PET-RAFT polymerization still has considerable limitations in terms of efficiency as well as the polymerization environment.Herein,sulfur-doped carbonized polymer dots(CPDs)were hydrothermally synthesized for catalysis of aqueous PET-RAFT polymerization at unprecedented efficiency with a highest propagation rate of 5.05 h-1.The resulting polymers have well-controlled molecular weight and narrow molecular weight dispersion(Ð<1.10).Based on the optoelectronic characterizations,we obtained insights into the photoinduced electron transfer process and proposed the mechanism for CPD-mediated PET-RAFT polymerization.In addition,as-synthesized CPDs for PET-RAFT polymerization were also demonstrated to be suitable for a wide range of light sources(blue/green/solar irradiation),numerous monomers,low catalyst loading(low as 0.01 mg mL^(-1)),and multiple polar solvent environments,all of which allowed to achieve efficiencies much higher than those of existing semiconductor-mediated methods.Finally,the CPDs were confirmed to be non-cytotoxic and catalyzed PET-RAFT polymerization successfully in cell culture media,indicating broad prospects in biomedical fields.展开更多
Aqueous zinc-ion batteries(AZIBs)are gaining attention owing to their affordability,high safety,and high energy density,making them a promising solution for large-scale energy storage.However,their performance is hamp...Aqueous zinc-ion batteries(AZIBs)are gaining attention owing to their affordability,high safety,and high energy density,making them a promising solution for large-scale energy storage.However,their performance is hampered by the instability of both the anode-electrolyte interface and the cathode-electrolyte interface.The use of sodium gluconate(SG),an organic sodium salt with multiple hydroxyl groups,as an electrolyte additive is suggested.Experimental and theoretical analyses demonstrate that Na^(+)from SG can intercalate and deintercalate within the associated V_(2)O_(5) cathode during in situ electrochemical processes.This action supports the layered structure of V_(2)O_(5),prevents structural collapse and phase transitions,and enhances Zn^(2+)diffusion kinetics.Additionally,the gluconate anion disrupts the original Zn^(2+)solvation structure,mitigates water-induced side reactions,and suppresses Zn dendrite growth.The synchronous regulation of both the V_(2)O_(5) cathode and Zn anode by the SG additive leads to considerable performance improvements.Zn‖Zn symmetric batteries demonstrate a cycle life exceeding 2800 h at 0.5 mA cm^(-2)and 1 mAh cm^(-2).In Zn‖V_(2)O_(5) full batteries,a high specific capacity of 288.92 mAh g^(-1)and capacity retention of 82.29%are maintained over 1000 cycles at a current density of 2 A g^(-1).This multifunctional additive strategy offers a new pathway for the practical application of AZIBs.展开更多
The Jahn-Teller effect of Mn^(3+)brings drastic structural changes to MnO_(2)-based materials and accelerates the destruction and deactivation of the internal structure of the materials,thus leading to severe capacity...The Jahn-Teller effect of Mn^(3+)brings drastic structural changes to MnO_(2)-based materials and accelerates the destruction and deactivation of the internal structure of the materials,thus leading to severe capacity fading and phase change of MnO_(2)-based materials in aqueous zinc ion batteries(AZIBs).Here,this study doped high valent vanadium ions into MnO_(2)(VMO-x)to inhibit manganese's Jahn-Teller effect.Through a series of characterizations,such as X-ray diffraction(XRD),Raman spectroscopy,and scanning electron microscopy(SEM),it was discovered that the introduction of vanadium ions effectively increased the interlayer spacing of MnO_(2),facilitating the transport of ions into the interlayer.Additionally,Fourier transform infrared spectroscopy(FTIR)and X-ray photoelectron spectroscopy(XPS)demonstrated vanadium doped could effectively adjust the electronic structure,decreasing the average oxidation state of manganese,thereby inhibiting the Jahn-Teller effect and significantly enhancing the stability of the VMO-x cathode.The theoretical calculation showed that introducing vanadium ions enhanced the interaction between the main material and Zn^(2+),optimized its electron transport capacity,and led to better electrical conductivity and reaction kinetics of the VMO-5.Benefiting from this,the VMO-5 cathode exhibited an outstanding capacity of 283 mAh/g and maintained a capacity retention rate of 79%after 2000 cycles,demonstrating excellent electrochemical performance.Furthermore,the mechanism of H^(+)/Zn^(2+)co-intercalation/deintercalation was demonstrated through mechanism analysis.Finally,the test results of the pouch cell demonstrated the excellent flexibility and safety exhibited by the VMO-5 make it have great potential in flexible devices.This work presented a novel approach to doping high valence metal ions into manganese-based electrodes for AZIBs.展开更多
Aqueous aluminum ion batteries(AAIBs)have garnered extensive attention due to their environmental friendliness,high theoretical capacity,and low cost.However,the sluggish reaction kinetics and severe structural collap...Aqueous aluminum ion batteries(AAIBs)have garnered extensive attention due to their environmental friendliness,high theoretical capacity,and low cost.However,the sluggish reaction kinetics and severe structural collapse of the cathode material,especially manganese oxide,during the cycling process have hindered its further application.Herein,Cu^(2+)pre-interca la ted layeredδ-MnO_(2)was synthesized via a hydrothermal method.The pre-intercalated Cu^(2+)ions not only improve the conductivity of MnO_(2)cathode but also stabilize the structure to enhance stability.X-ray absorption fine structure(XAFS)combined with density functional theory(DFT)calculations confirm the formation of the covalent bond between Cu and O,increasing the electronegativity of O atoms and enhancing the H^(+)adsorption energy.Moreover,ex-situ measurements not only elucidate the Al^(3+)/H^(+)co-insertion energy storage mechanism but also demonstrate the high reversibility of the Cu-MnO_(2)cathode during cycling.This work provides a promising modification approach for the application of manganese oxides in AAIBs.展开更多
The iron and steel industries generate large amounts of unavoidable CO_(2)emissions as well as considerable quantities of slags.More than one-half of the emitted CO_(2)is produced in blast furnaces during ironmaking,a...The iron and steel industries generate large amounts of unavoidable CO_(2)emissions as well as considerable quantities of slags.More than one-half of the emitted CO_(2)is produced in blast furnaces during ironmaking,and thus it is meaningful to use blast furnace slags to capture CO_(2)while addressing the byproducts and flue gas of ironmaking.Mineral carbonation of slags is a promising route to achieve carbon neutrality and effective slag utilization.To exploit slag more effectively and capture CO_(2)in flue gas,an in-depth investigation into the carbonation of blast furnace slags generated with different cooling methods was conducted.The effects of the solid–liquid ratio and introduced CO_(2)concentration on carbonation were determined.The CO_(2)uptake capacity of air-cooled slag(0.04 g/g)was greater than that of water-quenched slag.The CO_(2)uptake capacities of the two slags were comparable with those of slags in previous works,indicating the potential of the two slags for CO_(2)sequestration and utilization even with low-energy input and this fact suggests that this process is feasible.展开更多
V_(2)O_(5)·nH_(2)O has been widely studied for aqueous zinc-ion batteries.The intercalation of inorganic ions has been used as a feasible method to improve the capacity of vanadium pentoxide.To further improve th...V_(2)O_(5)·nH_(2)O has been widely studied for aqueous zinc-ion batteries.The intercalation of inorganic ions has been used as a feasible method to improve the capacity of vanadium pentoxide.To further improve the stability,organic small molecule choline chloride intercalation is used to expand the spacing of the vanadium pentoxide layers and increase the cycling stability.Therefore,we consider the introduction of Sr^(2+)to cointercalate with choline chloride.Here,we synthes-ized vanadium pentoxide cointercalated with Sr^(2+)and choline ions(Ch^(+))via a simple hydrothermal method.The electro-chemical performance shows an enhanced cathode capacitance contribution of Sr&Ch-V_(2)O_(5),with a discharge capacity of 526 mAh·g^(-1)at 0.1 A·g^(-1)and a retention rate of 78.9%after 2000 cycles at 5 A·g^(-1).This work offers a novel strategy for the design of organic‒inorganic hybrid materials for use as cathodes in aqueous zinc-ion batteries.展开更多
Aqueous zinc-halogen batteries are promising candidates for large-scale energy storage due to their abundant resources,intrinsic safety,and high theoretical capacity.Nevertheless,the uncontrollable zinc dendrite growt...Aqueous zinc-halogen batteries are promising candidates for large-scale energy storage due to their abundant resources,intrinsic safety,and high theoretical capacity.Nevertheless,the uncontrollable zinc dendrite growth and spontaneous shuttle effect of active species have prohibited their practical implementation.Herein,a double-layered protective film based on zinc-ethylenediamine tetramethylene phosphonic acid(ZEA)artificial film and ZnF2-rich solid electrolyte interphase(SEI)layer has been successfully fabricated on the zinc metal anode via electrode/electrolyte synergistic optimization.The ZEA-based artificial film shows strong affinity for the ZnF2-rich SEI layer,therefore effectively suppressing the SEI breakage and facilitating the construction of double-layered protective film on the zinc metal anode.Such double-layered architecture not only modulates Zn2+flux and suppresses the zinc dendrite growth,but also blocks the direct contact between the metal anode and electrolyte,thus mitigating the corrosion from the active species.When employing optimized metal anodes and electrolytes,the as-developed zinc-(dual)halogen batteries present high areal capacity and satisfactory cycling stability.This work provides a new avenue for developing aqueous zinc-(dual)halogen batteries.展开更多
基金Project supported by the National Natural Science Foundation of China(Nos.31470092 and 31501459)the Natural Science Youth Foundation of Jiangsu Province(No.BK20130380)China
文摘（R）-2-hydroxy-3-phenylpropionic acid （PIP,） is an ideal antimicrobial compound with broad-spectrum activity against a wide range of Gram-positive bacteria, some Gram-negative bacteria, and fungi. We studied the bioconversion of phenylpyruvate （PPA） to PLA using whole recombinant Escherichia coli cells in a series of buffer/organic solvent systems. Octane was found to be the best organic solvent. The optimum volume ratio of the water phase to the n-octane phase, conversion temperature, substrate concentration, and cell concentration were 6：4, 40 ℃, 12.5 g/L, and 30 g/L wet cells, respectively. Under the optimized conditions, the average PLA productivity in the aqueous/ n-octane system was 30.69% higher than that in the aqueous system, and 32.31 g/L PLA was obtained with the use of a stirred reactor （2-L scale）. Taken together, our findings indicated that PLA biosynthesis was more efficient in an aqueous/n-octane biphasic system than in a monophasic aqueous system. The proposed biphasic system is an effective strategy for enhancing PLA yield and the biosynthesis of its analogues.
基金supported by the National Natural Science Foundation of China(52002297)National Key R&D Program of China(2022VFB2404800)+1 种基金Wuhan Yellow Crane Talents Program,China Postdoctoral Science Foundation(No.2024M752495)the Postdoctoral Fellowship Program of CPSF(No.GZB20230552).
文摘Aqueous alkali metal-ion batteries(AAMIBs)have been recognized as emerging electrochemical energy storage technologies for grid-scale applications owning to their intrinsic safety,cost-effectiveness,and environmental sustainability.However,the practical application of AAMIBs is still severely constrained by the tendency of aqueous electrolytes to freeze at low temperatures and decompose at high temperatures,limiting their operational temperature range.Considering the urgent need for energy systems with higher adaptability and resilience at various application scenarios,designing novel electrolytes via structure modulation has increasingly emerged as a feasible and economical strategy for the performance optimization of wide-temperature AAMIBs.In this review,the latest advancement of wide-temperature electrolytes for AAMIBs is systematically and comprehensively summarized.Specifically,the key challenges,failure mechanisms,correlations between hydrogen bond behaviors and physicochemical properties,and thermodynamic and kinetic interpretations in aqueous electrolytes are discussed firstly.Additionally,we offer forward-looking insights and innovative design principles for developing aqueous electrolytes capable of operating across a broad temperature range.This review is expected to provide some guidance and reference for the rational design and regulation of widetemperature electrolytes for AAMIBs and promote their future development.
基金supported by the Natural Science Foundation of China(Nos.52125202,52202100,and U24A2065)the Natural Science Foundation of Jiangsu Province(BK20243016)Fundamental Research Funds for the Central Universities,China Postdoctoral Science Foundation(No.2024T171166).
文摘Aqueous zinc-ion batteries(AZIBs)have garnered considerable attention as promising post-lithium energy storage technologies owing to their intrinsic safety,cost-effectiveness,and competitive gravimetric energy density.However,their practical commercialization is hindered by critical challenges on the anode side,including dendrite growth and parasitic reactions at the anode/electrolyte interface.Recent studies highlight that rational electrolyte structure engineering offers an effective route to mitigate these issues and strengthen the electrochemical performance of the zinc metal anode.In this review,we systematically summarize state-of-the-art strategies for electrolyte optimization,with a particular focus on the zinc salts regulation,electrolyte additives,and the construction of novel electrolytes,while elucidating the underlying design principles.We further discuss the key structure–property relationships governing electrolyte behavior to provide guidance for the development of next-generation electrolytes.Finally,future perspectives on advanced electrolyte design are proposed.This review aims to serve as a comprehensive reference for researchers exploring high-performance electrolyte engineering in AZIBs.
基金the fundamental Research Funds for the central Universities(x2wjD2240360)for the funding supportMeanwhile,Engineering and Physical Sciences Research Council(EPSRC,EP/V027433/3)+2 种基金UK Research and Innovation(UKRI)under the UK government’s Horizon Europe funding(101077226,EP/Y008707/1)Faraday Institution(EP/S003053/1)Degradation project(FIRG001),Royal Society(IEC\NSFC\233361),QUB Agility Fund and Wright Technology and Research Centre(W-Tech,R5240MEE)Funding from UK aid from the UK Government through the Faraday Institution and the Transforming Energy Access Programme(Grant number FIRG050-Device engineering of Zn-based hybrid micro-flow batteries and by-product H2 collection for Emerging Economies)。
文摘Aqueous zinc metal batteries(AZMBs)face significant challenges in achieving reversibility and cycling stability,primarily due to hydrogen evolution reactions(HER)and zinc dendrite growth.In this study,by employing carefully designed cells that approximate the structural characteristics of practical batteries,we revisit this widely held view through in-operando X-ray radiography to examine zinc dendrite formation and HER under nearpractical operating conditions.While conventional understanding emphasizes the severity of these processes,our findings suggest that zinc dendrites and HER are noticeably less pronounced in dense,real-operation configurations compared to modified cells,possibly due to a more uniform electric field and the suppression of triple-phase boundaries.This study indicates that other components,such as degradation at the cathode current collector interface and configuration mismatches within the full cell,may also represent important barriers to the practical application of AZMBs,particularly during the early stages of electrodeposition.
基金supported by the National Natural Science Foundation of China (No. 21676300)
文摘The bimetallic NiCu/SAPO-11 catalysts were prepared by co-impregnation, sequential impregnation, coprecipitation, and mechanical mixing methods. Powder X-ray diffraction, nitrogen adsorption-desorption,temperature-programmed desorption of ammonia, transmission electron microscopy, temperatureprogrammed reduction of hydrogen, and X-ray photoelectron spectroscopy were used to characterize the physicochemical properties of the catalysts. The catalytic performance of the catalysts was assessed by the hydroisomerization of n-octane. Results indicated that the conversion of n-octane and selectivity to n-octane isomers were related to the preparation methods of the catalysts. The catalysts with Ni-Cu alloy effectively restrained the hydrogenolysis reaction that decreases the selectivity of isomerization. The catalyst prepared by the mechanical mixing of NiO and CuO hardly formed Ni-Cu alloy, showing obvious hydrogenolysis and low selectivity to n-octane isomers. The unbalance between the metal and acid sites resulted in the low conversion of n-octane and selectivity to n-octane isomers. Among all the catalysts,the catalyst prepared by the co-impregnation method exhibited high catalytic activity and selectivity to n-octane isomers.
基金supported by the National Natural Science Foundation,China(no.21676300)
文摘SAPO-11 molecular sieves were synthesized using silica sol, hydrophilic fumed silica, and tetraethyl orthosilicate（TEOS） as silicon precursors. Their physicochemical properties were characterized using XRD,SEM, nitrogen adsorption-desorption, Py-IR, NH;-TPD, EDS, and;Al,;P,;Si MAS NMR techniques. The catalytic performance was assessed in the hydroisomerization of n-octane. The results showed that the silicon precursors influenced the physicochemical properties and catalytic performance of SAPO-11. SAPO-11 synthesized using hydrophilic fumed silica as silicon precursor showed higher silicon distribution and had more medium acid sites. SAPO-11 synthesized using TEOS as silicon precursor had more silicon content, but more silicon islands formed in its framework. The depolymerization of silicon precursors might affect the silicon content and distribution in SAPO-11. In the hydroisomerization of n-octane, the catalytic activity strongly depended on the number of medium acid sites instead of the number of total acid sites.SAPO-11 synthesized using hydrophilic fumed silica as silicon precursor exhibited higher catalytic activity than the other samples because it has more medium acid sites.
文摘The catalyst NiW/HSAPO-11 was prepared by impregnating Ni and W onto HSAPO-11 zeolite with two different methods. The isomerization and aromatization properties were investigated with an microreactor using n-octane as a feedstock. NiW/HSAPO-11 shows a high hydroconversion activity of n-octane, and the optimum operating parameters for the catalyst to produce high octane number products were: 400℃, 2.0MPa, VH2:Vn-octane= 400:1, liquid hourly space velocity LHSV=1.0h-1. Under the optimum reaction condition, the conversion efficiency, C5 liquid + product selectivity, isomerization and aromatization product selectivity were 69.80%, 56.95%, 79.73% and 1.29% respectively. The catalyst (S1) impregnated with Ni and W after the HSAPO-11 zeolite was combined with Al2O3 matrix, performed better than the catalyst (S2) impregnated with Ni and W before combining with the Al2O3 matrix.
基金sponsored by China Petroleumand Chemical Corporation(No.:090701)
文摘A bifunctional catalyst Pt/HY-β was prepared from a bimicroporous composite zeolite Y-β. Characterization results showed that the specific surface area, pore volume, and acid amount of the catalyst Pt/HY-β all decreased compared to the original zeolite. The catalytic performance of this catalyst in n-octane hydroisomerization was investigated in a fixed bed stainless steel tubular reactor. The results showed that at a hydrogen/n-octane volume ratio of 1000, pressure of 0.6 MPa, temperature of 230 ℃ and LHSV of 3 h^-1, the conversion of n-octane, yield of liquid, hydrocracking rate and yield of iso-octane were 52.32%, 88.66%, 12.60%, 39.51%, respectively.
基金This work was supported by the National Natural Science Foundation of China (No. 20737001)(2003CB415002)China Postdoctoral Science Foundation (No. 2003033486)
文摘Optimized calculations of 75 PCDDs and their parent DD were carded out at the B3LYP/6-31G＊ level by density functional theory （DFT） method. The structural parameters were obtained and significant correlation between the C1 substitution position and some structural parameters was found. Consequently, the number of C1 substitution positions was taken as theoretical descriptors to establish two novel QSPR models for predicting lgKow and -lgSw of all PCDD congeners. The two models achieved in this work contain two variables （Na and Nβ）, of which r = 0.9312, 0.9965 and SD = 0.27, 0.12 respectively, and t values are all large. The variation inflation factors （VIF） of variables in the two models herein are both less than 5.0, suggesting high accuracy of the lgKow and -lgSw predicting models, and the results of cross-validation test also show that the two models exhibit optimum stability and good predictive power. By comparison, the correlation and predictive ability of the present work are more advantageous than those obtained using semi-empirical AM1 and GC-RI methods.
基金the financial supports from the National Natural Science Foundation of China(22322803,22178059,22208054,22221005,22072019)Key Technologies Innovation and Industrialization Projects of Fujian Province(2022G031)Qingyuan Innovation Laboratory(00121002,00523005)。
文摘A seed-directed approach to synthesizing Fe ZSM-22 zeolite without organic structure directing agent(OSDA)was developed by using Fe-rich diatomite as all aluminum and iron sources.The Fe ZSM-22zeolite with optimal crystallinity and purity can be obtained by systematically adjusting feed composition and synthesis conditions.Characterizations show that Fe ZSM-22 zeolite synthesized with OSDA-free owns high crystallinity,obvious thin needle-shaped morphology and high Bronsted/Lewis acid ratio.Significantly,when used for n-octane hydroisomerization reaction,its derived catalyst exhibits the best catalytic performance reflected by the highest selectivity to C_(8)isomers compared to the two reference catalysts prepared based on a Fe-containing and a Fe-free ZSM-22 synthesized through an OSDA-directed route from natural diatomite and conventional chemicals,respectively.This work provides an alternative route to sustainably synthesizing heteroatomic zeolites with high performance.
基金Supported by Jilin Provincial Scientific and Technological Development Program(20230508109RC,20230201051GX,20220201091GX)National Natural Science Foundation of China(62035013,61275235)。
文摘Aqueous zinc-ion electrochromic(EC)technology,boasting the capability to fulfill both safety and cost-ef⁃fectiveness requirements,is garnering extensive attention in various application areas including smart windows,thermal management,displays,and camouflage.However,typical inorganic EC materials,such as tungsten oxides(WO_(3)),of⁃ten suffer from slow ion diffusion kinetics and limited optical contrast within the aqueous Zn^(2+)electrolyte because of the large size and strong Coulombic interactions of the Zn^(2+),which limits their wide applicability.Here,ordered WO_(3)nanowire films,constructed by a one-step grazing angle deposition method,is demonstrated to boost the response speed and optical contrast during EC phenomena.Compared with dense films,the ordered WO_(3)nanowire films with a porosity of 44.6%demonstrate anti-reflective property and excellent comprehensive EC performance,including fast response time(3.6 s and 1.2 s for coloring and bleaching,respectively),large optical contrast(66.6%at 700 nm)and high col⁃oration efficiency(64.3 cm^(2)·C^(-1)).A large-area prototype EC device(17 cm×12 cm)with fast color-switching is also successfully achieved.Mechanistic studies show that the improved performance is mainly due to the ordered porous nanowire structures,which provides direct electron transfer paths and sufficient interfacial contacts,thus simultaneously enhancing the electrochemical activity and fast redox kinetics.This study provides a simple and effective strategy to im⁃prove the performance of tungsten oxide-based aqueous zinc ion EC materials and devices.
基金supported by the Exchange Program of Highend Foreign Experts of Ministry of Science and Technology of People’s Republic of China(No.G2023041003L)the Natural Science Foundation of Shaanxi Provincial Department of Education(No.23JK0367)+1 种基金the Scientific Research Startup Program for Introduced Talents of Shaanxi University of Technology(Nos.SLGRCQD2208,SLGRCQD2306,SLGRCQD2133)Contaminated Soil Remediation and Resource Utilization Innovation Team at Shaanxi University of Technology。
文摘As battery technology evolves and demand for efficient energy storage solutions,aqueous zinc ion batteries(AZIBs)have garnered significant attention due to their safety and environmental benefits.However,the stability of cathode materials under high-voltage conditions remains a critical challenge in improving its energy density.This review systematically explores the failure mechanisms of high-voltage cathode materials in AZIBs,including hydrogen evolution reaction,phase transformation and dissolution phenomena.To address these challenges,we propose a range of advanced strategies aimed at improving the stability of cathode materials.These strategies include surface coating and doping techniques designed to fortify the surface properties and structure integrity of the cathode materials under high-voltage conditions.Additionally,we emphasize the importance of designing antioxidant electrolytes,with a focus on understanding and optimizing electrolyte decomposition mechanisms.The review also highlights the significance of modifying conductive agents and employing innovative separators to further enhance the stability of AZIBs.By integrating these cutting-edge approaches,this review anticipates substantial advancements in the stability of high-voltage cathode materials,paving the way for the broader application and development of AZIBs in energy storage.
基金This work was supported by the China Postdoctoral Science Foundation (No. 2003033486)
文摘Optimized calculation of dibenzofuran （DF） and 135 polychlorinated dibenzofurans （PCDFs） was carried out at the B3LYP/6-31G＊ level in GAUSSIAN 98 program. Based on the theoretical linear solvation energy relationship （TLSER） model, the obtained structural parameters were taken as theoretical descriptors to establish the novel quantitative structureproperty relationship （QSPR） model for predicting n-octanol/water partition coefficients （lgKow） of PCDFs. The new model of lgKow achieved in this work contains three variables： energy of the highest occupied molecular orbital （EHOMO）, the most negative atomic partial charge （q^-） and average molecular polarizability （a）, of which R^2= 0.9011 and SD = 0,17 with larger t values. In addition, the variation inflation factors （VIF） of variables in the present model are all less than 5.5, suggesting high accuracy of the lgKow model. And the results of cross-validation test （q^2 = 0.8688） and method validation also show this model exhibits optimum stability and better predictive power than semi-empirical method. At the same time, it is found that the aqueous solubility （-lgSw） has high relative correlation with constant volume molar heat capacity （Cv^0）, of which R^2 = 0.9777 and SD = 0.22. Moreover, lgKow and -lgSw values of all PCDF congeners were predicted respectively.
基金supported by the National Natural Science Foundation of China(NSFC)under Grant No.22035001 and No.52233005.
文摘To achieve the target of carbon neutrality,it is crucial to develop an efficient and green synthesis methodology with good atomic economy to achieve sufficient utilization of energy and sustainable development.Photoinduced electron transfer reversible addition-fragmentation chain-transfer(PET-RAFT)polymerization is a precise methodology for constructing polymers with well-defined structures.However,conventional semiconductor-mediated PET-RAFT polymerization still has considerable limitations in terms of efficiency as well as the polymerization environment.Herein,sulfur-doped carbonized polymer dots(CPDs)were hydrothermally synthesized for catalysis of aqueous PET-RAFT polymerization at unprecedented efficiency with a highest propagation rate of 5.05 h-1.The resulting polymers have well-controlled molecular weight and narrow molecular weight dispersion(Ð<1.10).Based on the optoelectronic characterizations,we obtained insights into the photoinduced electron transfer process and proposed the mechanism for CPD-mediated PET-RAFT polymerization.In addition,as-synthesized CPDs for PET-RAFT polymerization were also demonstrated to be suitable for a wide range of light sources(blue/green/solar irradiation),numerous monomers,low catalyst loading(low as 0.01 mg mL^(-1)),and multiple polar solvent environments,all of which allowed to achieve efficiencies much higher than those of existing semiconductor-mediated methods.Finally,the CPDs were confirmed to be non-cytotoxic and catalyzed PET-RAFT polymerization successfully in cell culture media,indicating broad prospects in biomedical fields.
基金supported by the Battery Energy Storage Testing Center of Chongqing through their provision of testing support and technical assistance。
文摘Aqueous zinc-ion batteries(AZIBs)are gaining attention owing to their affordability,high safety,and high energy density,making them a promising solution for large-scale energy storage.However,their performance is hampered by the instability of both the anode-electrolyte interface and the cathode-electrolyte interface.The use of sodium gluconate(SG),an organic sodium salt with multiple hydroxyl groups,as an electrolyte additive is suggested.Experimental and theoretical analyses demonstrate that Na^(+)from SG can intercalate and deintercalate within the associated V_(2)O_(5) cathode during in situ electrochemical processes.This action supports the layered structure of V_(2)O_(5),prevents structural collapse and phase transitions,and enhances Zn^(2+)diffusion kinetics.Additionally,the gluconate anion disrupts the original Zn^(2+)solvation structure,mitigates water-induced side reactions,and suppresses Zn dendrite growth.The synchronous regulation of both the V_(2)O_(5) cathode and Zn anode by the SG additive leads to considerable performance improvements.Zn‖Zn symmetric batteries demonstrate a cycle life exceeding 2800 h at 0.5 mA cm^(-2)and 1 mAh cm^(-2).In Zn‖V_(2)O_(5) full batteries,a high specific capacity of 288.92 mAh g^(-1)and capacity retention of 82.29%are maintained over 1000 cycles at a current density of 2 A g^(-1).This multifunctional additive strategy offers a new pathway for the practical application of AZIBs.
基金supported the National Key Research and Development Program of China(No.2024YFA1409900)the National Natural Science Foundation of China(Nos.62101296 and 52303335)+2 种基金the China Postdoctoral Science Foundation(Nos.2021M702656 and 2023M730099)the Natural Science Foundation of Shaanxi Province(Nos.2021JQ-756 and 2021M702656)the Graduate Innovation Fund of the School of Mechanical Engineering,Shaanxi University of Technology(No.SLGJX202404)。
文摘The Jahn-Teller effect of Mn^(3+)brings drastic structural changes to MnO_(2)-based materials and accelerates the destruction and deactivation of the internal structure of the materials,thus leading to severe capacity fading and phase change of MnO_(2)-based materials in aqueous zinc ion batteries(AZIBs).Here,this study doped high valent vanadium ions into MnO_(2)(VMO-x)to inhibit manganese's Jahn-Teller effect.Through a series of characterizations,such as X-ray diffraction(XRD),Raman spectroscopy,and scanning electron microscopy(SEM),it was discovered that the introduction of vanadium ions effectively increased the interlayer spacing of MnO_(2),facilitating the transport of ions into the interlayer.Additionally,Fourier transform infrared spectroscopy(FTIR)and X-ray photoelectron spectroscopy(XPS)demonstrated vanadium doped could effectively adjust the electronic structure,decreasing the average oxidation state of manganese,thereby inhibiting the Jahn-Teller effect and significantly enhancing the stability of the VMO-x cathode.The theoretical calculation showed that introducing vanadium ions enhanced the interaction between the main material and Zn^(2+),optimized its electron transport capacity,and led to better electrical conductivity and reaction kinetics of the VMO-5.Benefiting from this,the VMO-5 cathode exhibited an outstanding capacity of 283 mAh/g and maintained a capacity retention rate of 79%after 2000 cycles,demonstrating excellent electrochemical performance.Furthermore,the mechanism of H^(+)/Zn^(2+)co-intercalation/deintercalation was demonstrated through mechanism analysis.Finally,the test results of the pouch cell demonstrated the excellent flexibility and safety exhibited by the VMO-5 make it have great potential in flexible devices.This work presented a novel approach to doping high valence metal ions into manganese-based electrodes for AZIBs.
基金financially supported by the National Natural Science Foundation of China(52102233)Science and Technology Project of Hebei Education Department(QN2023019)。
文摘Aqueous aluminum ion batteries(AAIBs)have garnered extensive attention due to their environmental friendliness,high theoretical capacity,and low cost.However,the sluggish reaction kinetics and severe structural collapse of the cathode material,especially manganese oxide,during the cycling process have hindered its further application.Herein,Cu^(2+)pre-interca la ted layeredδ-MnO_(2)was synthesized via a hydrothermal method.The pre-intercalated Cu^(2+)ions not only improve the conductivity of MnO_(2)cathode but also stabilize the structure to enhance stability.X-ray absorption fine structure(XAFS)combined with density functional theory(DFT)calculations confirm the formation of the covalent bond between Cu and O,increasing the electronegativity of O atoms and enhancing the H^(+)adsorption energy.Moreover,ex-situ measurements not only elucidate the Al^(3+)/H^(+)co-insertion energy storage mechanism but also demonstrate the high reversibility of the Cu-MnO_(2)cathode during cycling.This work provides a promising modification approach for the application of manganese oxides in AAIBs.
基金supported by the Science and Technology Research Partnership for Sustainable Development(SATREPS)。
文摘The iron and steel industries generate large amounts of unavoidable CO_(2)emissions as well as considerable quantities of slags.More than one-half of the emitted CO_(2)is produced in blast furnaces during ironmaking,and thus it is meaningful to use blast furnace slags to capture CO_(2)while addressing the byproducts and flue gas of ironmaking.Mineral carbonation of slags is a promising route to achieve carbon neutrality and effective slag utilization.To exploit slag more effectively and capture CO_(2)in flue gas,an in-depth investigation into the carbonation of blast furnace slags generated with different cooling methods was conducted.The effects of the solid–liquid ratio and introduced CO_(2)concentration on carbonation were determined.The CO_(2)uptake capacity of air-cooled slag(0.04 g/g)was greater than that of water-quenched slag.The CO_(2)uptake capacities of the two slags were comparable with those of slags in previous works,indicating the potential of the two slags for CO_(2)sequestration and utilization even with low-energy input and this fact suggests that this process is feasible.
文摘V_(2)O_(5)·nH_(2)O has been widely studied for aqueous zinc-ion batteries.The intercalation of inorganic ions has been used as a feasible method to improve the capacity of vanadium pentoxide.To further improve the stability,organic small molecule choline chloride intercalation is used to expand the spacing of the vanadium pentoxide layers and increase the cycling stability.Therefore,we consider the introduction of Sr^(2+)to cointercalate with choline chloride.Here,we synthes-ized vanadium pentoxide cointercalated with Sr^(2+)and choline ions(Ch^(+))via a simple hydrothermal method.The electro-chemical performance shows an enhanced cathode capacitance contribution of Sr&Ch-V_(2)O_(5),with a discharge capacity of 526 mAh·g^(-1)at 0.1 A·g^(-1)and a retention rate of 78.9%after 2000 cycles at 5 A·g^(-1).This work offers a novel strategy for the design of organic‒inorganic hybrid materials for use as cathodes in aqueous zinc-ion batteries.
基金support from the National Natural Science Foundation of China(22209089,22178187)Natural Science Foundation of Shandong Province(ZR2022QB048,ZR2021MB006)+2 种基金Excellent Youth Science Foundation of Shandong Province(Overseas)(2023HWYQ-089)the Taishan Scholars Program of Shandong Province(tsqn201909091)Open Research Fund of School of Chemistry and Chemical Engineering,Henan Normal University.
文摘Aqueous zinc-halogen batteries are promising candidates for large-scale energy storage due to their abundant resources,intrinsic safety,and high theoretical capacity.Nevertheless,the uncontrollable zinc dendrite growth and spontaneous shuttle effect of active species have prohibited their practical implementation.Herein,a double-layered protective film based on zinc-ethylenediamine tetramethylene phosphonic acid(ZEA)artificial film and ZnF2-rich solid electrolyte interphase(SEI)layer has been successfully fabricated on the zinc metal anode via electrode/electrolyte synergistic optimization.The ZEA-based artificial film shows strong affinity for the ZnF2-rich SEI layer,therefore effectively suppressing the SEI breakage and facilitating the construction of double-layered protective film on the zinc metal anode.Such double-layered architecture not only modulates Zn2+flux and suppresses the zinc dendrite growth,but also blocks the direct contact between the metal anode and electrolyte,thus mitigating the corrosion from the active species.When employing optimized metal anodes and electrolytes,the as-developed zinc-(dual)halogen batteries present high areal capacity and satisfactory cycling stability.This work provides a new avenue for developing aqueous zinc-(dual)halogen batteries.
