Antimony is more than an emerging pollutant in water but a scare resource.In this study,we report an adsorbent with the record capacity so far from the balanced view of Sb(Ⅲ) and Sb(Ⅴ).The composite adsorbent was fa...Antimony is more than an emerging pollutant in water but a scare resource.In this study,we report an adsorbent with the record capacity so far from the balanced view of Sb(Ⅲ) and Sb(Ⅴ).The composite adsorbent was fabricated by encapsulating hollow Fe_(3)O_(4)nanosphere with the EDTA grafted chitosan,and it has superhigh adsorption capacity of for 657.1 mg/g for Sb(Ⅲ) and 467.3 mg/g for Sb(Ⅴ),respectively.The mechanism study reveals that the adsorption of Sb initializes from the Fe_(3)O_(4),propagates along the chitosan with hydrogen bond,and terminates at the inner sphere complex with the EDTA moiety in the adsorbent.In view of the ultra-high adsorption capacity of the adsorbent,the recovered adsorbent that contains abundant (>36.4%) highly dispersed antimony nanoparticles (600-FCSE-Sb) is applied to Li-ion battery anode after reduction.This article provides a new idea for connecting water treatment and electric energy storage.展开更多
An anion-rich electric double layer(EDL)region is favorable for fabricating an inorganic-rich solid-electrolyte interphase(SEI)towards stable lithium metal anode in ester electrolyte.Herein,cetyltrimethylammonium brom...An anion-rich electric double layer(EDL)region is favorable for fabricating an inorganic-rich solid-electrolyte interphase(SEI)towards stable lithium metal anode in ester electrolyte.Herein,cetyltrimethylammonium bromide(CTAB),a cationic surfactant,is adopted to draw more anions into EDL by ionic interactions that shield the repelling force on anions during lithium plating.In situ electrochemical surface-enhanced Raman spectroscopy results combined with molecular dynamics simulations validate the enrichment of NO_(3)^(−)/FSI−anions in the EDL region due to the positively charged CTA^(+).In-depth analysis of SEI structure by X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry results confirmed the formation of the inorganic-rich SEI,which helps improve the kinetics of Li^(+)transfer,lower the charge transfer activation energy,and homogenize Li deposition.As a result,the Li||Li symmetric cell in the designed electrolyte displays a prolongated cycling time from 500 to 1300 h compared to that in the blank electrolyte at 0.5 mA cm^(-2) with a capacity of 1 mAh cm^(-2).Moreover,Li||LiFePO_(4) and Li||LiCoO_(2) with a high cathode mass loading of>10 mg cm^(-2) can be stably cycled over 180 cycles.展开更多
The synchronous construction of metal phosphate and phosphorus-doped carbon structures is of great significance to innovate the design,synthesis,and application of catalysts,as these phosphoruscontaining composite mat...The synchronous construction of metal phosphate and phosphorus-doped carbon structures is of great significance to innovate the design,synthesis,and application of catalysts,as these phosphoruscontaining composite materials have shown a remarkable contribution to electrocatalysts.However,their preparation procedure generally involves using large amounts of excess phosphorus sources for phosphorization,which inevitably release poisonous PH_(3) or dangerous phosphorus vapor.Here,a strategy for in-situ formation of FePO_(4) embedded in P-doped carbon 2D nano film(FePO_(4)/PdC)is developed using a highly integrated precursor,which is a small molecular organophosphine ligand,1,1’bis(diphenylphosphine)ferrocene(DPPF).The multi-source precursor DPPF that contains Fe,P,and C is molecular-vapor-deposited on the nickel foam(NF)supported ZIF-67 nanosheets to obtain the composite catalyst,namely DPPF-500/ZIF-67/NF.FePO_(4)/PdC encapsulated the ZIF-67 derived Co/N-doped carbon matrix(Co NC)to form a sandwich structure FePO_(4)/PdC@CoNC.The constructed catalyst shows good performance for OER,requiring an overpotential of only 297 m V to deliver 600 m A/cm^(2) with a Tafel slope of 42.7 m V dec^(-1).DFT calculations demonstrate that the synergistic effects between the metal active center and P-doped carbon film reduce the energy barriers and improve electron transport.This method of constructing P-containing catalysts overcomes the demand for additional P sources to realize eco-friendly fabrication and yields a unique structure with good catalytic activity.展开更多
Various forms of intelligent light-controlled soft actuators and robots rely on advanced material architectures and bionic systems to enable programmable remote actuation and multifunctionality.Despite advancements,si...Various forms of intelligent light-controlled soft actuators and robots rely on advanced material architectures and bionic systems to enable programmable remote actuation and multifunctionality.Despite advancements,significant challenges remain in developing actuators and robots that can effectively mimic the low-intensity,wide-wavelength light signal sensing and processing functions observed in living organisms.Herein,we report a design strategy that integrates light-responsive artificial synapses(AS)with liquid crystal networks(LCNs)to create bionic light-controlled LCN soft actuators(AS-LCNs).Remarkably,AS-LCNs can be controlled with light intensities as low as 0.68 mW cm^(-2),a value comparable to the light intensity perceivable by the human eye.These AS-LCNs can perform programmable intelligent sensing,learning,and memory within a wide wavelength range from 365 nm to 808 nm.Additionally,our system demonstrates time-related proofs of concept for a tachycardia alarm and a porcupine defense behavior simulation.Overall,this work addresses the limitations of traditional light-controlled soft actuators and robots in signal reception and processing,paving the way for the development of intelligent soft actuators and robots that emulate the cognitive abilities of living organisms.展开更多
Li-O_(2)batteries with an ultrahigh theoretical energy density of up to 3500 W·h/kg have drawn extensive attention as future energy storage technologies.However,large discharge/charge overpotentials(>1 V)and u...Li-O_(2)batteries with an ultrahigh theoretical energy density of up to 3500 W·h/kg have drawn extensive attention as future energy storage technologies.However,large discharge/charge overpotentials(>1 V)and unsatisfactory cycling performance are the main obstacles for practical applications.Recently,integrating photocatalysis into Li-O_(2)batteries has emerged as a promising method to mitigate overpotentials,but the rational design of photocathodes with excellent photoelectrochemical activity and stability remains challenging.This review focuses on recent research progress on the reaction mechanisms in photo-assisted Li-O_(2)batteries and the development of photocathodes.We present several strategies for tailoring catalytic materials from the perspectives of material selection and its catalytic performance optimization,aiming to provide a fundamental understanding and insights into the design of efficient photocathodes.The key challenges in constructing highperformance photocathodes and potential strategies were also discussed,offering insights for the development and application of efficient photocathodes in photo-assisted Li-O_(2)batteries.展开更多
van der Waals heterostructures stacked by transition metal dichalcogenides and graphene provide a new opportunity for exploring superlubricity.However,the further reduction of friction is limited by the unavoidable ch...van der Waals heterostructures stacked by transition metal dichalcogenides and graphene provide a new opportunity for exploring superlubricity.However,the further reduction of friction is limited by the unavoidable charge transfer in the heterostructures.The dynamics of charge transfer occur at picosecond time scale,which cannot be detected by traditional friction instruments,making the friction mechanism of charge transfer unclear.Here,we investigate friction-induced charge transfer in WS_(2)/graphene heterostructures with ultrafast friction energy dissipation detecting technique.The observed friction exhibits a strong linear relationship with the dissipation rate of interlayer charge transfer.By modulating the band structure of heterostructures,the dissipation rate of interlayer charge transfer can be efficiently tuned from 0.72 to 0.17 ps^(−1),resulting in a~35%reduction in friction.This work gives the direct explanation of friction-induced charge transfer,which enables the high-performance micro-electro-mechanical systems and new insight into the origin of friction from the perspective of ultrafast electron dynamics.展开更多
基金supported by the National Natural Science Foundation of China (No.21872020)。
文摘Antimony is more than an emerging pollutant in water but a scare resource.In this study,we report an adsorbent with the record capacity so far from the balanced view of Sb(Ⅲ) and Sb(Ⅴ).The composite adsorbent was fabricated by encapsulating hollow Fe_(3)O_(4)nanosphere with the EDTA grafted chitosan,and it has superhigh adsorption capacity of for 657.1 mg/g for Sb(Ⅲ) and 467.3 mg/g for Sb(Ⅴ),respectively.The mechanism study reveals that the adsorption of Sb initializes from the Fe_(3)O_(4),propagates along the chitosan with hydrogen bond,and terminates at the inner sphere complex with the EDTA moiety in the adsorbent.In view of the ultra-high adsorption capacity of the adsorbent,the recovered adsorbent that contains abundant (>36.4%) highly dispersed antimony nanoparticles (600-FCSE-Sb) is applied to Li-ion battery anode after reduction.This article provides a new idea for connecting water treatment and electric energy storage.
基金financial support from Singapore Ministry of Education under its AcRF Tier 2 Grant No MOE-T2EP10123-0001Singapore National Research Foundation Investigatorship under Grant No NRF-NRFI08-2022-0009Academic Excellence Foundation of BUAA for PhD Students(applicant:Hongfei Xu).
文摘An anion-rich electric double layer(EDL)region is favorable for fabricating an inorganic-rich solid-electrolyte interphase(SEI)towards stable lithium metal anode in ester electrolyte.Herein,cetyltrimethylammonium bromide(CTAB),a cationic surfactant,is adopted to draw more anions into EDL by ionic interactions that shield the repelling force on anions during lithium plating.In situ electrochemical surface-enhanced Raman spectroscopy results combined with molecular dynamics simulations validate the enrichment of NO_(3)^(−)/FSI−anions in the EDL region due to the positively charged CTA^(+).In-depth analysis of SEI structure by X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry results confirmed the formation of the inorganic-rich SEI,which helps improve the kinetics of Li^(+)transfer,lower the charge transfer activation energy,and homogenize Li deposition.As a result,the Li||Li symmetric cell in the designed electrolyte displays a prolongated cycling time from 500 to 1300 h compared to that in the blank electrolyte at 0.5 mA cm^(-2) with a capacity of 1 mAh cm^(-2).Moreover,Li||LiFePO_(4) and Li||LiCoO_(2) with a high cathode mass loading of>10 mg cm^(-2) can be stably cycled over 180 cycles.
基金financially supported by the National Natural Science Foundation of China(21872020)the 1226 Engineering Health Major Project(BWS17J028,AWS16J018)the Fundamental Research Funds for the Central Universities(N180705004)。
文摘The synchronous construction of metal phosphate and phosphorus-doped carbon structures is of great significance to innovate the design,synthesis,and application of catalysts,as these phosphoruscontaining composite materials have shown a remarkable contribution to electrocatalysts.However,their preparation procedure generally involves using large amounts of excess phosphorus sources for phosphorization,which inevitably release poisonous PH_(3) or dangerous phosphorus vapor.Here,a strategy for in-situ formation of FePO_(4) embedded in P-doped carbon 2D nano film(FePO_(4)/PdC)is developed using a highly integrated precursor,which is a small molecular organophosphine ligand,1,1’bis(diphenylphosphine)ferrocene(DPPF).The multi-source precursor DPPF that contains Fe,P,and C is molecular-vapor-deposited on the nickel foam(NF)supported ZIF-67 nanosheets to obtain the composite catalyst,namely DPPF-500/ZIF-67/NF.FePO_(4)/PdC encapsulated the ZIF-67 derived Co/N-doped carbon matrix(Co NC)to form a sandwich structure FePO_(4)/PdC@CoNC.The constructed catalyst shows good performance for OER,requiring an overpotential of only 297 m V to deliver 600 m A/cm^(2) with a Tafel slope of 42.7 m V dec^(-1).DFT calculations demonstrate that the synergistic effects between the metal active center and P-doped carbon film reduce the energy barriers and improve electron transport.This method of constructing P-containing catalysts overcomes the demand for additional P sources to realize eco-friendly fabrication and yields a unique structure with good catalytic activity.
基金National Key Research and Development Program of China,Grant/Award Numbers:2021YFA1101303,2022YFB3203502National Natural Science Foundation of China,Grant/Award Numbers:22105043,22305175,62074111+1 种基金Innovation Program of Shanghai Municipal Education Commission,Grant/Award Number:2021-01-07-00-07-E00096Fundamental Research Funds for the Central Universities。
文摘Various forms of intelligent light-controlled soft actuators and robots rely on advanced material architectures and bionic systems to enable programmable remote actuation and multifunctionality.Despite advancements,significant challenges remain in developing actuators and robots that can effectively mimic the low-intensity,wide-wavelength light signal sensing and processing functions observed in living organisms.Herein,we report a design strategy that integrates light-responsive artificial synapses(AS)with liquid crystal networks(LCNs)to create bionic light-controlled LCN soft actuators(AS-LCNs).Remarkably,AS-LCNs can be controlled with light intensities as low as 0.68 mW cm^(-2),a value comparable to the light intensity perceivable by the human eye.These AS-LCNs can perform programmable intelligent sensing,learning,and memory within a wide wavelength range from 365 nm to 808 nm.Additionally,our system demonstrates time-related proofs of concept for a tachycardia alarm and a porcupine defense behavior simulation.Overall,this work addresses the limitations of traditional light-controlled soft actuators and robots in signal reception and processing,paving the way for the development of intelligent soft actuators and robots that emulate the cognitive abilities of living organisms.
基金supported by Singapore Ministry of Education under its AcRF Tier 2(MOE-T2EP10123-0001)Singapore National Research Foundation Investigatorship(NRF-NRFI08-2022-0009).
文摘Li-O_(2)batteries with an ultrahigh theoretical energy density of up to 3500 W·h/kg have drawn extensive attention as future energy storage technologies.However,large discharge/charge overpotentials(>1 V)and unsatisfactory cycling performance are the main obstacles for practical applications.Recently,integrating photocatalysis into Li-O_(2)batteries has emerged as a promising method to mitigate overpotentials,but the rational design of photocathodes with excellent photoelectrochemical activity and stability remains challenging.This review focuses on recent research progress on the reaction mechanisms in photo-assisted Li-O_(2)batteries and the development of photocathodes.We present several strategies for tailoring catalytic materials from the perspectives of material selection and its catalytic performance optimization,aiming to provide a fundamental understanding and insights into the design of efficient photocathodes.The key challenges in constructing highperformance photocathodes and potential strategies were also discussed,offering insights for the development and application of efficient photocathodes in photo-assisted Li-O_(2)batteries.
基金supported by the National Natural Science Foundation of China(Nos.52425503,52475199,52105195,52075284,and 52350380).
文摘van der Waals heterostructures stacked by transition metal dichalcogenides and graphene provide a new opportunity for exploring superlubricity.However,the further reduction of friction is limited by the unavoidable charge transfer in the heterostructures.The dynamics of charge transfer occur at picosecond time scale,which cannot be detected by traditional friction instruments,making the friction mechanism of charge transfer unclear.Here,we investigate friction-induced charge transfer in WS_(2)/graphene heterostructures with ultrafast friction energy dissipation detecting technique.The observed friction exhibits a strong linear relationship with the dissipation rate of interlayer charge transfer.By modulating the band structure of heterostructures,the dissipation rate of interlayer charge transfer can be efficiently tuned from 0.72 to 0.17 ps^(−1),resulting in a~35%reduction in friction.This work gives the direct explanation of friction-induced charge transfer,which enables the high-performance micro-electro-mechanical systems and new insight into the origin of friction from the perspective of ultrafast electron dynamics.
