It is significant to develop highly efficient electrocatalysts for energy conversion systems.Interface engineering is one of the most feasible approaches to effectively enhance the electrocatalytic activity.Herein,the...It is significant to develop highly efficient electrocatalysts for energy conversion systems.Interface engineering is one of the most feasible approaches to effectively enhance the electrocatalytic activity.Herein,the density functional theory(DFT)calculations predict that the potential barriers of Fe sites at the interface of FeP–CoP heterostructures are lower than that of Fe sites in FeP nanoparticles(NPs),Co sites in CoP NPs,or Co sites in heterostructures.Motivated by the DFT calculation results,FeP–CoP heterostructures have been designed and synthesized by a metal–organic frameworks(MOFs)confined-phosphorization method.The FeP–CoP exhibits the lowest overpotential of 230 mV at the current density of 10 mA·cm^(−2)for oxygen evolution reaction(OER),compared with FeP(470 mV)and CoP(340 mV),which outperforms most of transition metal-based catalysts.The Tafel analysis of FeP–CoP heterostructures shows an improved reaction kinetic pathway with the smallest slope of 90.3 mV·dec^(−1),as compared to the Tafel slopes of FeP NPs(137 mV·dec^(−1))and CoP NPs(114 mV·dec^(−1)).And the FeP–CoP shows extraordinary long-term stability over 24 h.The excellent activity and long-term stability of FeP–CoP derive from the synergistic effect between FeP and CoP.展开更多
It is important and challenging to analyze nanocluster structure with atomic precision.Herein,α-hemolysin nanopore was used to identify nanoclusters at the single molecule level by providing two-dimensional(2D)dwell ...It is important and challenging to analyze nanocluster structure with atomic precision.Herein,α-hemolysin nanopore was used to identify nanoclusters at the single molecule level by providing two-dimensional(2D)dwell time–current blockage spectra and translocation event frequency which sensitively depended on their structures.Nanoclusters such as Anderson,Keggin,Dawson,and a few lacunary Dawson polyoxometalates with very similar structures,even with only a two-atom difference,could be discriminated.This nanopore device could simultaneously measure multiple nanoclusters in a mixture qualitatively and quantitatively.Furthermore,molecular dynamics(MD)simulations provided microscopic understandings of the nanocluster translocation dynamics and yielded 2D dwell time–current blockage spectra in close agreement with experiments.The nanopore platform provides a novel powerful tool for nanocluster characterization.展开更多
As more than 60%of worldwide consumed energy is unused and becomes waste heat every year,high-efficiency waste heat to power technologies are highly demanded for the conversion of wasted heat to electricity.Thermoelec...As more than 60%of worldwide consumed energy is unused and becomes waste heat every year,high-efficiency waste heat to power technologies are highly demanded for the conversion of wasted heat to electricity.Thermoelectrics which can convert the wasted heat directly into electricity represent a promising approach for energy recovery.Thermoelectric technology has existed for several decades,but its usage has been limited due to low efficiencies.Recent advances in nanotechnology have enabled the improving of thermoelectric properties which open up the thermoelectrics’feasibility in industry.In this paper,we present an overview of recent progress in increasing the porosity of thermoelectric materials from atomic scale to microscale,leading to the enhancement of figure of merit.展开更多
The development of cost-effective electrocatalysts for overall water splitting is highly desirable,remaining a critical challenge at current stage.Herein,a class of composite FeNi@MXene(Mo_(2)TiC_(2)T_(x))@nickel foam...The development of cost-effective electrocatalysts for overall water splitting is highly desirable,remaining a critical challenge at current stage.Herein,a class of composite FeNi@MXene(Mo_(2)TiC_(2)T_(x))@nickel foam(NF)has been synthesized through introducing Fe2+ions and in-situ combining with surface nickel atoms on nickel foam.The obtained FeNi@Mo_(2)TiC_(2)T_(x)@NF exhibited high activity with overpotentials of 165 and 190 mV for the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)at a current density of 10 mA·cm^(-2),respectively.The synergetic effects of Mo_(2)TiC_(2)T_(x)and FeNi nanoalloys lead to increasing catalytic activities,where MXene provides high active surface area and rich active sites for HER,and FeNi nanoalloys promote the OER.Theoretical simulation of electron exchange capacity between FeNi and MXene in FeNi@Mo_(2)TiC_(2)T_(x)catalyst shows that electrons transferred from surface Mo atoms to the interface between FeNi and MXene,indicating that the electrons are accumulated near the FeNi nanoparticles.This kind of electronic distribution facilitates the formation of intermediate of NiOOH.Correspondingly,(H++e-)is more inclined onto Mo-Ni interfaces for HER.The Gibbs free energy changes for H*to HER and potential-limiting step for-OOH intermediate in OER over FeNi@Mo_(2)TiC_(2)T_(x)are much less than those on bare MXene.The catalyst can be further used for overall water splitting in alkaline solution,realizing a current density of 50 mA·cm^(-2)at 1.74 V.This work provides a facile strategy to achieve efficient and cheap catalysts for new energy production.展开更多
基金the National Natural Science Foundation of China(Nos.22101289 and 22275138)the Hundred Talents Programs in Chinese Academy of Science,the National Key Research and Development Project(No.2021YFA1502200)+1 种基金the Bellwethers Project of Zhejiang Research and Development Plan(No.2022C01158)the Ningbo Yongjiang Talent Introduction Programme(No.2021A-111-G).
文摘It is significant to develop highly efficient electrocatalysts for energy conversion systems.Interface engineering is one of the most feasible approaches to effectively enhance the electrocatalytic activity.Herein,the density functional theory(DFT)calculations predict that the potential barriers of Fe sites at the interface of FeP–CoP heterostructures are lower than that of Fe sites in FeP nanoparticles(NPs),Co sites in CoP NPs,or Co sites in heterostructures.Motivated by the DFT calculation results,FeP–CoP heterostructures have been designed and synthesized by a metal–organic frameworks(MOFs)confined-phosphorization method.The FeP–CoP exhibits the lowest overpotential of 230 mV at the current density of 10 mA·cm^(−2)for oxygen evolution reaction(OER),compared with FeP(470 mV)and CoP(340 mV),which outperforms most of transition metal-based catalysts.The Tafel analysis of FeP–CoP heterostructures shows an improved reaction kinetic pathway with the smallest slope of 90.3 mV·dec^(−1),as compared to the Tafel slopes of FeP NPs(137 mV·dec^(−1))and CoP NPs(114 mV·dec^(−1)).And the FeP–CoP shows extraordinary long-term stability over 24 h.The excellent activity and long-term stability of FeP–CoP derive from the synergistic effect between FeP and CoP.
基金supported by the National Key Research and Development Program of China(No.2021YFA1200104)New Cornerstone Science Foundation,the National Natural Science Foundation of China(Nos.22027807,22034004,and 22078104)+1 种基金the Strategic Priority Research Program of Chinese Academy of Sciences(No.XDB36000000)Tsinghua-Vanke Special Fund for Public Health and Health Discipline Development(No.2022Z82WKJ003).
文摘It is important and challenging to analyze nanocluster structure with atomic precision.Herein,α-hemolysin nanopore was used to identify nanoclusters at the single molecule level by providing two-dimensional(2D)dwell time–current blockage spectra and translocation event frequency which sensitively depended on their structures.Nanoclusters such as Anderson,Keggin,Dawson,and a few lacunary Dawson polyoxometalates with very similar structures,even with only a two-atom difference,could be discriminated.This nanopore device could simultaneously measure multiple nanoclusters in a mixture qualitatively and quantitatively.Furthermore,molecular dynamics(MD)simulations provided microscopic understandings of the nanocluster translocation dynamics and yielded 2D dwell time–current blockage spectra in close agreement with experiments.The nanopore platform provides a novel powerful tool for nanocluster characterization.
基金The work documented is supported under a research grant from the US Navy,Mr.Peter A.Morrison at the Office of Naval Research(Award Number N000141912518)located in Arlington,Virginia,USA.
文摘As more than 60%of worldwide consumed energy is unused and becomes waste heat every year,high-efficiency waste heat to power technologies are highly demanded for the conversion of wasted heat to electricity.Thermoelectrics which can convert the wasted heat directly into electricity represent a promising approach for energy recovery.Thermoelectric technology has existed for several decades,but its usage has been limited due to low efficiencies.Recent advances in nanotechnology have enabled the improving of thermoelectric properties which open up the thermoelectrics’feasibility in industry.In this paper,we present an overview of recent progress in increasing the porosity of thermoelectric materials from atomic scale to microscale,leading to the enhancement of figure of merit.
基金the financial support by the National Natural Science Foundation of China(Nos.21771137,21773288,and 21722104)the Training Project of Innovation Team of Colleges and Universities in Tianjin(No.TD13-5020)the Natural Science Foundation of Tianjin City of China(No.18JCJQJC47700).
文摘The development of cost-effective electrocatalysts for overall water splitting is highly desirable,remaining a critical challenge at current stage.Herein,a class of composite FeNi@MXene(Mo_(2)TiC_(2)T_(x))@nickel foam(NF)has been synthesized through introducing Fe2+ions and in-situ combining with surface nickel atoms on nickel foam.The obtained FeNi@Mo_(2)TiC_(2)T_(x)@NF exhibited high activity with overpotentials of 165 and 190 mV for the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)at a current density of 10 mA·cm^(-2),respectively.The synergetic effects of Mo_(2)TiC_(2)T_(x)and FeNi nanoalloys lead to increasing catalytic activities,where MXene provides high active surface area and rich active sites for HER,and FeNi nanoalloys promote the OER.Theoretical simulation of electron exchange capacity between FeNi and MXene in FeNi@Mo_(2)TiC_(2)T_(x)catalyst shows that electrons transferred from surface Mo atoms to the interface between FeNi and MXene,indicating that the electrons are accumulated near the FeNi nanoparticles.This kind of electronic distribution facilitates the formation of intermediate of NiOOH.Correspondingly,(H++e-)is more inclined onto Mo-Ni interfaces for HER.The Gibbs free energy changes for H*to HER and potential-limiting step for-OOH intermediate in OER over FeNi@Mo_(2)TiC_(2)T_(x)are much less than those on bare MXene.The catalyst can be further used for overall water splitting in alkaline solution,realizing a current density of 50 mA·cm^(-2)at 1.74 V.This work provides a facile strategy to achieve efficient and cheap catalysts for new energy production.