High theoretical capacity and unique layered structures make MoS_(2)a promising lithium-ion battery anode material.However,the anisotropic ion transport in layered structures and the poor intrinsic conductivity of MoS...High theoretical capacity and unique layered structures make MoS_(2)a promising lithium-ion battery anode material.However,the anisotropic ion transport in layered structures and the poor intrinsic conductivity of MoS_(2)lead to unacceptable ion transport capability.Here,we propose in-situ construction of interlayer electrostatic repulsion caused by Co^(2+)substituting Mo^(4+)between MoS_(2)layers,which can break the limitation of interlayer van der Waals forces to fabricate monolayer MoS_(2),thus establishing isotropic ion transport paths.Simultaneously,the doped Co atoms change the electronic structure of monolayer MoS_(2),thus improving its intrinsic conductivity.Importantly,the doped Co atoms can be converted into Co nanoparticles to create a space charge region to accelerate ion transport.Hence,the Co-doped monolayer MoS_(2)shows ultrafast lithium ion transport capability in half/full cells.This work presents a novel route for the preparation of monolayer MoS_(2)and demonstrates its potential for application in fast-charging lithium-ion batteries.展开更多
Nanofiltration separation has become a popular technique for removing largeorganic molecules and inorganic substances from water. It is achieved by a combination of threemechanisms: electrostatic repulsion, sieving an...Nanofiltration separation has become a popular technique for removing largeorganic molecules and inorganic substances from water. It is achieved by a combination of threemechanisms: electrostatic repulsion, sieving and diffusion. In the present work, a model based onirreversible thermodynamics is extended and used to estimate rejection of inorganic salts andorganic substances. Binary systems are modeled, where the feed contains an ion that is much lesspermeable to the membrane as compared with the other ion. The two model parameters are estimated byfitting the model to the experimental data. Variation of these parameters with the composition ofthe feed is described by an empirical correlation. This work attempts to describe transport throughthe nanofiltration membranes by a simple model.展开更多
Seawater electrolysis,especially in coastlines,is widely considered as a sustainable way of making clean and high-purity H2 from renewable energy;however,the practical viability is challenged severely by the limited a...Seawater electrolysis,especially in coastlines,is widely considered as a sustainable way of making clean and high-purity H2 from renewable energy;however,the practical viability is challenged severely by the limited anode durability resulting from side reactions of chlorine species.Herein,we report an effective Cl^(−) blocking barrier of NiFe-layer double hydroxide(NiFe-LDH)to harmful chlorine chemistry during alkaline seawater oxidation(ASO),a pre-formed surface-derived NiFe-phosphate(Pi)outerlayer.Specifically,the PO_(4)^(3−)-enriched outer-layer is capable of physically and electrostatically inhibiting Cl−adsorption,which protects active Ni^(3+)sites during ASO.The NiFe-LDH with the NiFe-Pi outer-layer(NiFe-LDH@NiFe-Pi)exhibits higher current densities(j)and lower overpotentials to afford 1 A·cm^(−2)(η1000 of 370 mV versusη1000 of 420 mV)than the NiFe-LDH in 1 M KOH+seawater.Notably,the NiFe-LDH@NiFe-Pi also demonstrates longer-term electrochemical durability than NiFe-LDH,attaining 100-h duration at the j of 1 A·cm^(−2).Additionally,the importance of surface-derived PO_(4)^(3−)-enriched outer-layer in protecting the active centers,γ-NiOOH,is explained by ex situ characterizations and in situ electrochemical spectroscopic studies.展开更多
The impeded mass transfer rate by on-site-generated gas bubbles at both cathode and anode dramatically reduces the energy conversion efficiency of the proton exchange membrane water electrolyzer(PEMWE).Herein,we repor...The impeded mass transfer rate by on-site-generated gas bubbles at both cathode and anode dramatically reduces the energy conversion efficiency of the proton exchange membrane water electrolyzer(PEMWE).Herein,we report a surfactant-assistant method to accelerate the nano/micro-bubble detachment and the mass transfer rate by reducing the surface tension,resulting in an increase in overall efficiency.Four kinds of surfactants are studied in this work.Only potassium perfluorobutyl sulfonate(PPFBS),which has the structural similarity to Nafion,shows a significant promotion of activity and stability for both hygrogen evolution reaction(HER)and oxygen evolution reaction(OER)in the acidic medium at the high current density region.The HER overpotential at 0.1 A·cm−2 decreased 22%,and the current density at−0.4 V increased 31%by adding PPFBS.The promotion of overall efficiency by PPFBS on a homemade PEMWE was also proven.The reduced surface tension and electrostatic repulsion were the probable origins of the accelerated bubble detachment.展开更多
Although lithium metal has become a promising anode material for high-energy batteries owing to its high specific capacity and the lowest reduction potential,the continuous side reactions with electrolyte as well as t...Although lithium metal has become a promising anode material for high-energy batteries owing to its high specific capacity and the lowest reduction potential,the continuous side reactions with electrolyte as well as the safety problem caused by Li dendrite growth restrict Li anode’s practical application.Herein,we demonstrate that N-fluoropyridinium(ArF^(+))bis(trifluoromethane)sulfonimide(TFSI-)as an electrolyte additive can protect the lithium metal by both solid electrolyte interphase(SEI)protection and electrostatic repulsion mechanisms.The ArF+cations not only participate in forming F,Ncontaining SEI protective layer on Li surface,but also act as a cationic repellent during Li deposition to inhibit Li dendrite growth.As a result,the cycle performance of Li symmetric cells and Li||LiFePO_(4)full cells were significantly improved by using ArFTFSIadded electrolyte.This study provides an electrolyte additive strategy for Li anode realizing SEI protection and electrostatic repulsion simultaneously.展开更多
The history of antiparallel coiled coil dimer design is briefly reviewed and the main principles governing the successful designs are explained. They include analysis of the inter subunit electrostatic repulsion for ...The history of antiparallel coiled coil dimer design is briefly reviewed and the main principles governing the successful designs are explained. They include analysis of the inter subunit electrostatic repulsion for determining partners for dimerization and of the buried polar interaction for determining the relative orientation of the partners. A theory is proposed to explain the lack of antiparallel coiled coil homodimers in nature.展开更多
Surfactants are widely used to improve the solubility of oil in water in petrochemical,making it more difficult to remove oil–water emulsions during the water treatment process.Electrocoagulation(EC) is an appropriat...Surfactants are widely used to improve the solubility of oil in water in petrochemical,making it more difficult to remove oil–water emulsions during the water treatment process.Electrocoagulation(EC) is an appropriate method for treating oily wastewater and destabilizing emulsions. However, the demulsification mechanism of oil–water droplets emulsified by surfactants with different charges have not been investigated systematically. The demulsification performance of electrocoagulation on emulsions wastewater containing cationic,non-ionic, and anionic surfactants was studied. The results showed that the removal rate of total organic carbon(TOC) in oily wastewater with anionic surfactant by EC reached92.98% ± 0.40% at a current density of 1 mA/cm^(2), while that of the non-ionic surfactant was 84.88% ± 0.63%. The characterization of flocs showed that EC has the highest coagulation and demulsification of oil droplets with a negative charge on the surface(-70.50 ± 10.25mV), which indicated that the charge neutralization of oil droplets was beneficial for the destabilization of the formed oily flocs. However, when the zeta potential of the oil droplets reached 75.50 ± 1.25 mV, the TOC removal efficiency was only 11.80% ± 1.43%. The TOC removal could achieve 33.23% ± 3.21% when the current density improved from 1 mA/cm^(2)to 10 mA/cm^(2). The enhanced removal was due to the sweep coagulation rather than charge neutralization. This study provides a fundamental basis for the electrochemical treatment of oily wastewater.展开更多
基金financially supported by Shenzhen Key Laboratory of Advanced Energy Storage(No.ZDSYS20220401141000001)the Research Grants Council of the Hong Kong Special Administrative Region,China(Project No.R6005-20)。
文摘High theoretical capacity and unique layered structures make MoS_(2)a promising lithium-ion battery anode material.However,the anisotropic ion transport in layered structures and the poor intrinsic conductivity of MoS_(2)lead to unacceptable ion transport capability.Here,we propose in-situ construction of interlayer electrostatic repulsion caused by Co^(2+)substituting Mo^(4+)between MoS_(2)layers,which can break the limitation of interlayer van der Waals forces to fabricate monolayer MoS_(2),thus establishing isotropic ion transport paths.Simultaneously,the doped Co atoms change the electronic structure of monolayer MoS_(2),thus improving its intrinsic conductivity.Importantly,the doped Co atoms can be converted into Co nanoparticles to create a space charge region to accelerate ion transport.Hence,the Co-doped monolayer MoS_(2)shows ultrafast lithium ion transport capability in half/full cells.This work presents a novel route for the preparation of monolayer MoS_(2)and demonstrates its potential for application in fast-charging lithium-ion batteries.
文摘Nanofiltration separation has become a popular technique for removing largeorganic molecules and inorganic substances from water. It is achieved by a combination of threemechanisms: electrostatic repulsion, sieving and diffusion. In the present work, a model based onirreversible thermodynamics is extended and used to estimate rejection of inorganic salts andorganic substances. Binary systems are modeled, where the feed contains an ion that is much lesspermeable to the membrane as compared with the other ion. The two model parameters are estimated byfitting the model to the experimental data. Variation of these parameters with the composition ofthe feed is described by an empirical correlation. This work attempts to describe transport throughthe nanofiltration membranes by a simple model.
基金supported by the Free Exploration Project of Frontier Technology for Laoshan Laboratory(No.16-02)the National Natural Science Foundation of China(Nos.22072015 and 21927811).
文摘Seawater electrolysis,especially in coastlines,is widely considered as a sustainable way of making clean and high-purity H2 from renewable energy;however,the practical viability is challenged severely by the limited anode durability resulting from side reactions of chlorine species.Herein,we report an effective Cl^(−) blocking barrier of NiFe-layer double hydroxide(NiFe-LDH)to harmful chlorine chemistry during alkaline seawater oxidation(ASO),a pre-formed surface-derived NiFe-phosphate(Pi)outerlayer.Specifically,the PO_(4)^(3−)-enriched outer-layer is capable of physically and electrostatically inhibiting Cl−adsorption,which protects active Ni^(3+)sites during ASO.The NiFe-LDH with the NiFe-Pi outer-layer(NiFe-LDH@NiFe-Pi)exhibits higher current densities(j)and lower overpotentials to afford 1 A·cm^(−2)(η1000 of 370 mV versusη1000 of 420 mV)than the NiFe-LDH in 1 M KOH+seawater.Notably,the NiFe-LDH@NiFe-Pi also demonstrates longer-term electrochemical durability than NiFe-LDH,attaining 100-h duration at the j of 1 A·cm^(−2).Additionally,the importance of surface-derived PO_(4)^(3−)-enriched outer-layer in protecting the active centers,γ-NiOOH,is explained by ex situ characterizations and in situ electrochemical spectroscopic studies.
基金This work was supported by the National Natural Science Foundation of China(Nos.21971008 and 22101016)Fundamental Research Funds for the Central Universities(buctrc201916,buctrc201823)China Petroleum&Chemical Corporation(SINOPEC,120052-2).
文摘The impeded mass transfer rate by on-site-generated gas bubbles at both cathode and anode dramatically reduces the energy conversion efficiency of the proton exchange membrane water electrolyzer(PEMWE).Herein,we report a surfactant-assistant method to accelerate the nano/micro-bubble detachment and the mass transfer rate by reducing the surface tension,resulting in an increase in overall efficiency.Four kinds of surfactants are studied in this work.Only potassium perfluorobutyl sulfonate(PPFBS),which has the structural similarity to Nafion,shows a significant promotion of activity and stability for both hygrogen evolution reaction(HER)and oxygen evolution reaction(OER)in the acidic medium at the high current density region.The HER overpotential at 0.1 A·cm−2 decreased 22%,and the current density at−0.4 V increased 31%by adding PPFBS.The promotion of overall efficiency by PPFBS on a homemade PEMWE was also proven.The reduced surface tension and electrostatic repulsion were the probable origins of the accelerated bubble detachment.
基金This work was financially supported by the National Key R&D Program of China(No.2022YFB2402600)National Natural Science Foundation of China(No.22279166)+1 种基金Basic and Applied Basic Research Foundation of Guangdong Province-Regional joint fund project(No.2022B1515120019)the Fundamental Research Funds for the Central Universities,Sun Yat-Sen University(Nos.22qntd0101 and 22dfx01).
文摘Although lithium metal has become a promising anode material for high-energy batteries owing to its high specific capacity and the lowest reduction potential,the continuous side reactions with electrolyte as well as the safety problem caused by Li dendrite growth restrict Li anode’s practical application.Herein,we demonstrate that N-fluoropyridinium(ArF^(+))bis(trifluoromethane)sulfonimide(TFSI-)as an electrolyte additive can protect the lithium metal by both solid electrolyte interphase(SEI)protection and electrostatic repulsion mechanisms.The ArF+cations not only participate in forming F,Ncontaining SEI protective layer on Li surface,but also act as a cationic repellent during Li deposition to inhibit Li dendrite growth.As a result,the cycle performance of Li symmetric cells and Li||LiFePO_(4)full cells were significantly improved by using ArFTFSIadded electrolyte.This study provides an electrolyte additive strategy for Li anode realizing SEI protection and electrostatic repulsion simultaneously.
基金the"973" Projectthe Natural ScienceFoundation of Guangdongthe Research Foundationfor Returned Overseas Scholars of the Ministry ofEducationthe State Key L ab of Biomembrane &Membrane Biotechnology
文摘The history of antiparallel coiled coil dimer design is briefly reviewed and the main principles governing the successful designs are explained. They include analysis of the inter subunit electrostatic repulsion for determining partners for dimerization and of the buried polar interaction for determining the relative orientation of the partners. A theory is proposed to explain the lack of antiparallel coiled coil homodimers in nature.
基金the financial support from the National Key R&D Program of China (No. 2019YFC0408400)the Young Scientists Fund of the National Natural Science Foundation of China (No. 52000174)the Key Research Program of Frontier Sciences, CAS (No. ZDBS-LYDQC014)。
文摘Surfactants are widely used to improve the solubility of oil in water in petrochemical,making it more difficult to remove oil–water emulsions during the water treatment process.Electrocoagulation(EC) is an appropriate method for treating oily wastewater and destabilizing emulsions. However, the demulsification mechanism of oil–water droplets emulsified by surfactants with different charges have not been investigated systematically. The demulsification performance of electrocoagulation on emulsions wastewater containing cationic,non-ionic, and anionic surfactants was studied. The results showed that the removal rate of total organic carbon(TOC) in oily wastewater with anionic surfactant by EC reached92.98% ± 0.40% at a current density of 1 mA/cm^(2), while that of the non-ionic surfactant was 84.88% ± 0.63%. The characterization of flocs showed that EC has the highest coagulation and demulsification of oil droplets with a negative charge on the surface(-70.50 ± 10.25mV), which indicated that the charge neutralization of oil droplets was beneficial for the destabilization of the formed oily flocs. However, when the zeta potential of the oil droplets reached 75.50 ± 1.25 mV, the TOC removal efficiency was only 11.80% ± 1.43%. The TOC removal could achieve 33.23% ± 3.21% when the current density improved from 1 mA/cm^(2)to 10 mA/cm^(2). The enhanced removal was due to the sweep coagulation rather than charge neutralization. This study provides a fundamental basis for the electrochemical treatment of oily wastewater.