Stable and efficient single atom catalysts(SACs)are highly desirable yet challenging in catalyzing acidic oxygen evolution reaction(OER).Herein,we report a novel iridium single atom catalyst structure,with atomic Ir d...Stable and efficient single atom catalysts(SACs)are highly desirable yet challenging in catalyzing acidic oxygen evolution reaction(OER).Herein,we report a novel iridium single atom catalyst structure,with atomic Ir doped in tetragonal PdO matrix(IrSAs-PdO)via a lattice-confined strategy.The optimized IrSAs-PdO-0.10 exhibited remarkable OER activity with an overpotential of 277 mV at 10 mA·cm^(-2) and long-term stability of 1000 h in 0.5 M H_(2)SO_(4).Furthermore,the turnover frequency attains 1.6 s^(-1) at an overpotential of 300 mV with a 24-fold increase in the intrinsic activity.The high activity originates from isolated iridium sites with low valence states and decreased Ir–O bonding covalency,and the excellent stability is a result of the effective confinement of iridium sites by Ir–O–Pd motifs.Moreover,we demonstrated for the first time that SACs have great potential in realizing ultralow loading of iridium(as low as microgram per square center meter level)in a practical water electrolyzer.展开更多
The scale-up deployment of ruthenium(Ru)-based oxygen evolution reaction(OER)electrocatalysts in proton exchange membrane water electrolysis(PEMWE)is greatly restricted by the poor stability.As the lattice-oxygen-medi...The scale-up deployment of ruthenium(Ru)-based oxygen evolution reaction(OER)electrocatalysts in proton exchange membrane water electrolysis(PEMWE)is greatly restricted by the poor stability.As the lattice-oxygen-mediated mechanism(LOM)has been identified as the major contributor to the fast performance degradation,impeding lattice oxygen diffusion to inhibit lattice oxygen participation is imperative,yet remains challenging due to the lack of efficient approaches.Herein,we strategically regulate the bonding nature of Ru–O towards suppressed LOM via Ru-based high-entropy oxide(HEO)construction.The lattice disorder in HEOs is believed to increase migration energy barrier of lattice oxygen.As a result,the screened Ti_(23)Nb_(9)Hf_(13)W_(12)Ru_(43)O_(x) exhibits 11.7 times slower lattice oxygen diffusion rate,84%reduction in LOM ratio,and 29 times lifespan extension compared with the state-of-the-art RuO_(2) catalyst.Our work opens up a feasible avenue to constructing stabilized Ru-based OER catalysts towards scalable application.展开更多
Cell identification and sorting have been hot topics recently.However,most conventional approaches can only predict the category of a single target,and lack the ability to perform multitarget tasks to provide coordina...Cell identification and sorting have been hot topics recently.However,most conventional approaches can only predict the category of a single target,and lack the ability to perform multitarget tasks to provide coordinate information of the targets.This limits the development of high-throughput cell screening technologies.Fortunately,artificial intelligence(AI)systems based on deep-learning algorithms provide the possibility to extract hidden features of cells from original image information.Here,we demonstrate an AI-assisted multitarget processing system for cell identification and sorting.With this system,each target cell can be swiftly and accurately identified in a mixture by extracting cell morphological features,whereafter accurate cell sorting is achieved through noninvasive manipulation by optical tweezers.The AI-assisted model shows promise in guiding the precise manipulation and intelligent detection of high-flux cells,thereby realizing semiautomatic cell research.展开更多
Sn-based materials are considered as a kind of potential anode materials for lithium-ion batteries(LIBs)owing to their high theoretical capacity.However,their use is limited by large volume expansion deriving from the...Sn-based materials are considered as a kind of potential anode materials for lithium-ion batteries(LIBs)owing to their high theoretical capacity.However,their use is limited by large volume expansion deriving from the lithiation/delithiation process.In this work,amorphous Sn modified nitrogen-doped porous carbon nanosheets(ASnNPCNs)are obtained.The synergistic effect of amorphous Sn and high edge-nitrogendoped level porous carbon nanosheets provides ASn-NPCNs with multiple advantages containing abundant defect sites,high specific surface area(214.9 m^(2)·g^(−1)),and rich hierarchical pores,which can promote the lithium-ion storage.Serving as the LIB anode,the as-prepared ASn-NPCNs-750 electrode exhibits an ultrahigh capacity of 1643 mAh·g^(−1) at 0.1 A·g^(−1),ultrafast rate performance of 490 mAh·g^(−1) at 10 A·g^(−1),and superior long-term cycling performance of 988 mAh·g^(−1) at 1 A·g^(−1) after 2000 cycles with a capacity retention of 98.9%.Furthermore,the in-depth electrochemical kinetic test confirms that the ultrahigh-capacity and fast-charging performance of the ASn-NPCNs750 electrode is ascribed to the rapid capacitive mechanism.These impressive results indicate that ASn-NPCNs-750 can be a potential anode material for high-capacity and fast-charging LIBs.展开更多
Morphotropic phase boundary(MPB)plays a key role in tuning piezoelectric responses of ferroelectric ceramics.Here,Bi_(0.5)Na_(0.5)TiO_(3)modified BiFeO_(3)-BaTiO_(3)ternary solid solutions of 0.7BiFeO_(3)-(0.3-x)BaTiO...Morphotropic phase boundary(MPB)plays a key role in tuning piezoelectric responses of ferroelectric ceramics.Here,Bi_(0.5)Na_(0.5)TiO_(3)modified BiFeO_(3)-BaTiO_(3)ternary solid solutions of 0.7BiFeO_(3)-(0.3-x)BaTiO_(3)-xBi_(0.5)Na_(0.5)TiO_(3)(referred to as BF-BT-xBNT,0.00≤x≤0.04)were prepared for lead-free piezo-electrics.All the ceramics exhibit an MPB with coexisting rhombohedral(R)and tetragonal(T)phases,and the R/T phase ratio decreases upon increasing x.The increment of BNT promotes the grain growth,lowers the leakage current and Curie temperature(TC),and gradually drives the ferroelectric to relaxor transition.Because of the MPB with appropriate R/T phase ratio,increased grain size and density,and decreased leakage current,the well-balanced performance between d_(33)=206 pC/N and TC=488℃is obtained in x=0.01 case.In addition,the further enhanced in-situ d_(33)=286e347 pC/N is obtained in BF-BT-xBNT ceramics along with the improved depolarization temperature T_(d)from 280 to 312℃,showing a potential application for lead-free piezoceramics at high temperature.展开更多
The creation of universal strategies to affect the reaction route of the electroreduction of CO_(2) is critical.Here,we report the first work to introduce cations into diverse metals such as Cu,Bi,In,and Sn via the el...The creation of universal strategies to affect the reaction route of the electroreduction of CO_(2) is critical.Here,we report the first work to introduce cations into diverse metals such as Cu,Bi,In,and Sn via the electroreduction of related metallic oxides in quaternary ammonium surfactant solutions.Compared to their physical adsorption,cations embedded into the electrodes have a more pronounced impact on the electrical field,which effectively influences the adsorption state of intermediates.With the increase of surface field,the hydrogen evolution reaction and*COOH route are significantly reduced,favouring the*OCHO pathway instead.As a result,hydrogen,CO,and C_(2+)products almost completely vanish at−0.5 V versus RHE in 0.1 M Na_(2)SO_(4)in an H-type cell after enough cations are embedded into the Cu electrode,and the faradaic efficiency of formate rises from 18.0%to 99.5%simultaneously.展开更多
基金supported by the National Key R&D Program of China(No.2022YFB4002000)the National Natural Science Foundation of China(No.22232004)+2 种基金the Strategic priority research program of CAS(No.XDA21090400)the Jilin Province Science and Technology Development Program(NOs.20210301008GX and 20210502002ZP)the Jilin Province Development and Reform Commission Program(No.2023C032-6).
文摘Stable and efficient single atom catalysts(SACs)are highly desirable yet challenging in catalyzing acidic oxygen evolution reaction(OER).Herein,we report a novel iridium single atom catalyst structure,with atomic Ir doped in tetragonal PdO matrix(IrSAs-PdO)via a lattice-confined strategy.The optimized IrSAs-PdO-0.10 exhibited remarkable OER activity with an overpotential of 277 mV at 10 mA·cm^(-2) and long-term stability of 1000 h in 0.5 M H_(2)SO_(4).Furthermore,the turnover frequency attains 1.6 s^(-1) at an overpotential of 300 mV with a 24-fold increase in the intrinsic activity.The high activity originates from isolated iridium sites with low valence states and decreased Ir–O bonding covalency,and the excellent stability is a result of the effective confinement of iridium sites by Ir–O–Pd motifs.Moreover,we demonstrated for the first time that SACs have great potential in realizing ultralow loading of iridium(as low as microgram per square center meter level)in a practical water electrolyzer.
基金The authors thank the National Key R&D Program of China(No.2021YFB4000200)the National Natural Science Foundation of China(No.22232004)+1 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDA21090400)the Jilin Province Science and Technology Development Program(Nos.20210301008GX,YDZJ202202CXJD011,and 20210502002ZP)for financial support.
文摘The scale-up deployment of ruthenium(Ru)-based oxygen evolution reaction(OER)electrocatalysts in proton exchange membrane water electrolysis(PEMWE)is greatly restricted by the poor stability.As the lattice-oxygen-mediated mechanism(LOM)has been identified as the major contributor to the fast performance degradation,impeding lattice oxygen diffusion to inhibit lattice oxygen participation is imperative,yet remains challenging due to the lack of efficient approaches.Herein,we strategically regulate the bonding nature of Ru–O towards suppressed LOM via Ru-based high-entropy oxide(HEO)construction.The lattice disorder in HEOs is believed to increase migration energy barrier of lattice oxygen.As a result,the screened Ti_(23)Nb_(9)Hf_(13)W_(12)Ru_(43)O_(x) exhibits 11.7 times slower lattice oxygen diffusion rate,84%reduction in LOM ratio,and 29 times lifespan extension compared with the state-of-the-art RuO_(2) catalyst.Our work opens up a feasible avenue to constructing stabilized Ru-based OER catalysts towards scalable application.
基金supported by the National Natural Science Foundation of China(Nos.61975128,62175157,92150301,and 62375177)the Shenzhen Science and Technology Program(Nos.JCYJ20210324120403011 and RCJC20210609103232046)the Guangdong Major Project of Basic and Applied Basic Research(No.2020B0301030009)。
文摘Cell identification and sorting have been hot topics recently.However,most conventional approaches can only predict the category of a single target,and lack the ability to perform multitarget tasks to provide coordinate information of the targets.This limits the development of high-throughput cell screening technologies.Fortunately,artificial intelligence(AI)systems based on deep-learning algorithms provide the possibility to extract hidden features of cells from original image information.Here,we demonstrate an AI-assisted multitarget processing system for cell identification and sorting.With this system,each target cell can be swiftly and accurately identified in a mixture by extracting cell morphological features,whereafter accurate cell sorting is achieved through noninvasive manipulation by optical tweezers.The AI-assisted model shows promise in guiding the precise manipulation and intelligent detection of high-flux cells,thereby realizing semiautomatic cell research.
基金supports from the National Natural Science Foundation of China(Grant Nos.22238012,22178384,and 21908245)the Science Foundation of China University of Petroleum,Beijing(Grant No.ZX20220079).
文摘Sn-based materials are considered as a kind of potential anode materials for lithium-ion batteries(LIBs)owing to their high theoretical capacity.However,their use is limited by large volume expansion deriving from the lithiation/delithiation process.In this work,amorphous Sn modified nitrogen-doped porous carbon nanosheets(ASnNPCNs)are obtained.The synergistic effect of amorphous Sn and high edge-nitrogendoped level porous carbon nanosheets provides ASn-NPCNs with multiple advantages containing abundant defect sites,high specific surface area(214.9 m^(2)·g^(−1)),and rich hierarchical pores,which can promote the lithium-ion storage.Serving as the LIB anode,the as-prepared ASn-NPCNs-750 electrode exhibits an ultrahigh capacity of 1643 mAh·g^(−1) at 0.1 A·g^(−1),ultrafast rate performance of 490 mAh·g^(−1) at 10 A·g^(−1),and superior long-term cycling performance of 988 mAh·g^(−1) at 1 A·g^(−1) after 2000 cycles with a capacity retention of 98.9%.Furthermore,the in-depth electrochemical kinetic test confirms that the ultrahigh-capacity and fast-charging performance of the ASn-NPCNs750 electrode is ascribed to the rapid capacitive mechanism.These impressive results indicate that ASn-NPCNs-750 can be a potential anode material for high-capacity and fast-charging LIBs.
基金supported by Natural Science Foundation of Guangxi,China(2022GXNSFBA03561219245084)Guangdong Basic and Applied Basic Research Foundation(2020A1515111004)National Natural Science Foundation of China(52032007,52072028),and Foundation for Guangxi Bagui scholars.
文摘Morphotropic phase boundary(MPB)plays a key role in tuning piezoelectric responses of ferroelectric ceramics.Here,Bi_(0.5)Na_(0.5)TiO_(3)modified BiFeO_(3)-BaTiO_(3)ternary solid solutions of 0.7BiFeO_(3)-(0.3-x)BaTiO_(3)-xBi_(0.5)Na_(0.5)TiO_(3)(referred to as BF-BT-xBNT,0.00≤x≤0.04)were prepared for lead-free piezo-electrics.All the ceramics exhibit an MPB with coexisting rhombohedral(R)and tetragonal(T)phases,and the R/T phase ratio decreases upon increasing x.The increment of BNT promotes the grain growth,lowers the leakage current and Curie temperature(TC),and gradually drives the ferroelectric to relaxor transition.Because of the MPB with appropriate R/T phase ratio,increased grain size and density,and decreased leakage current,the well-balanced performance between d_(33)=206 pC/N and TC=488℃is obtained in x=0.01 case.In addition,the further enhanced in-situ d_(33)=286e347 pC/N is obtained in BF-BT-xBNT ceramics along with the improved depolarization temperature T_(d)from 280 to 312℃,showing a potential application for lead-free piezoceramics at high temperature.
基金the National Natural Science Foundation of China(grant nos.22073104,22273108,22293015,22072156,and 22121002)the Beijing Natural Science Foundation(grant no.2222043)+1 种基金the CAS Project for Young Scientists in Basic Research(grant no.YSBR-050)the Innovation Program of the IHEP(grant no.2023000034)for their financial support of this research。
文摘The creation of universal strategies to affect the reaction route of the electroreduction of CO_(2) is critical.Here,we report the first work to introduce cations into diverse metals such as Cu,Bi,In,and Sn via the electroreduction of related metallic oxides in quaternary ammonium surfactant solutions.Compared to their physical adsorption,cations embedded into the electrodes have a more pronounced impact on the electrical field,which effectively influences the adsorption state of intermediates.With the increase of surface field,the hydrogen evolution reaction and*COOH route are significantly reduced,favouring the*OCHO pathway instead.As a result,hydrogen,CO,and C_(2+)products almost completely vanish at−0.5 V versus RHE in 0.1 M Na_(2)SO_(4)in an H-type cell after enough cations are embedded into the Cu electrode,and the faradaic efficiency of formate rises from 18.0%to 99.5%simultaneously.
