Electrocatalytic N2 reduction to NH3 under ambient conditions is an eco-friendly and sustainable alternative to the traditional Haber-Bosch process. However, inhibited by the high activation barrier of N2, this proces...Electrocatalytic N2 reduction to NH3 under ambient conditions is an eco-friendly and sustainable alternative to the traditional Haber-Bosch process. However, inhibited by the high activation barrier of N2, this process needs efficient electrocatalysts to adsorb and activate the N2, enabling the N2 reduction reaction(NRR). Herein, we report that porous LaFeO3 nanofiber with oxygen vacancies acts as an efficient NRR electrocatalyst with abundant active sites to enhance the adsorption and activation of N2. When tested in 0.1 M HCl, such electrocatalyst achieves a high Faradaic efficiency of 8.77% and a large NH3 yield rate of 18.59 μg h–1 mgcat–1.at-0.55 V versus reversible hydrogen electrode. This catalyst also shows high long-term electrochemical stability and excellent selectivity for NH3 formation. Density functional theory calculations reveal that, by introducing oxygen vacancy on LaFeO3, the subsurface metallic ions are exposed with newly localized electronic states near the Fermi level, which facilitates the adsorption and activation of N2 molecules as well as the subsequent hydrogenation reactions.展开更多
The electrocatalytic synthesis of C-N coupling compounds from CO_(2) and nitrogenous species not only offers an effective avenue to achieve carbon neutral-ity and reduce environmental pollution,but also establishes a ...The electrocatalytic synthesis of C-N coupling compounds from CO_(2) and nitrogenous species not only offers an effective avenue to achieve carbon neutral-ity and reduce environmental pollution,but also establishes a route to synthesize valuable chemicals,such as urea,amide,and amine.This innovative approach expands the application range and product categories beyond simple carbona-ceous species in electrocatalytic CO_(2) reduction,which is becoming a rapidly advancing field.This review summarizes the research progress in electrocatalytic urea synthesis,using N_(2),NO_(2)^(-),and NO_(3)^(-)as nitrogenous species,and explores emerging trends in the electrosynthesis of amide and amine from CO_(2) and nitro-gen species.Additionally,the future opportunities in this field are highlighted,including electrosynthesis of amino acids and other compounds containing C-N bonds,anodic C-N coupling reactions beyond water oxidation,and the catalytic mechanism of corresponding reactions.This critical review also captures the insights aimed at accelerating the development of electrochemical C-N coupling reactions,confirming the superiority of this electrochemical method over the traditional techniques.展开更多
The integrated perception capable of detecting and monitoring varieties of activities is one of the ultimate purposes of wearable electronics and intelligent robots.Limited by the space occupation,it lacks practical f...The integrated perception capable of detecting and monitoring varieties of activities is one of the ultimate purposes of wearable electronics and intelligent robots.Limited by the space occupation,it lacks practical feasibility to stack multiple types of single sensors on each other.Herein,a high-sensitivity dual-function capacitive sensor with proximity sensing and pressure sensing is proposed.The fringing electric field can be confined in the proximity-sensitive area by fibrous loop-patterned electrode,leading to more stolen charges when object approaching and thus a high proximity sensitivity.The high-permittivity doped structured dielectric layer reduces the compressive stiffness and enhances the rate of compression-caused increase in the equivalent relative permittivity of the dielectric layer,resulting in a larger increase in capacitance and thus a high pressure sensitivity.The electrodes and dielectric layer together compose the capacitor and act as the sensor without taking up additional space.The decoupling of proximity-sensing and pressure-sensing modes can be achieved by decrease or increase in capacitance.Combined with array distribution and sequential scanning,the sensors can be used for detection of motion trajectory,contour recognition,pressure distribution.展开更多
Electrochemical nitrogen reduction reaction(NRR)is considered as an alternative to the industrial Haber-Bosch process for NH3 production due to both low energy consumption and environment friendliness.However,the majo...Electrochemical nitrogen reduction reaction(NRR)is considered as an alternative to the industrial Haber-Bosch process for NH3 production due to both low energy consumption and environment friendliness.However,the major problem of electrochemical NRR is the unsatisfied efficiency and selectivity of electrocatalyst.As one group of the cheapest and most abundant transition metals,iron-group(Fe,Co,Ni and Cu)electrocatalysts show promising potential on cost and performance advantages as ideal substitute for traditional noble-metal catalysts.In this minireview,we summarize recent advances of iron-group-based materials(including their oxides,hydroxides,nitrides,sulfides and phosphides,etc.)as non-noble metal electrocatalysts towards ambient N2-to-NH3 conversion in aqueous media.Strategies to boost NRR performances and perspectives for future developments are discussed to provide guidance for the field of NRR studies.展开更多
As a carbon-neutral alternative to the Haber-Bosch process,electrochemical N2 reduction enables environment-friendly NH3 synthesis at ambient conditions but needs active electrocatalysts for the N2 reduction reaction....As a carbon-neutral alternative to the Haber-Bosch process,electrochemical N2 reduction enables environment-friendly NH3 synthesis at ambient conditions but needs active electrocatalysts for the N2 reduction reaction.Here,we report that conductive metal-organic framework CO3(hexahydroxytriphenylene)2(Co3 HHTP2)nanoparticles act as an efficient catalyst for ambient electrochemical N2-to-NH3 fixation.When tested in 0.5 M LiClO4,such Co3 HHTP2 achieves a large NH3 yield of 22.14μg·h^-1·mg^-1 cat.with a faradaic efficiency of 3.34%at-0.40 V versus the reversible hydrogen electrode.This catalyst also shows high electrochemical stability and excellent selectivity toward NH3 synthesis.展开更多
Design and development of high-efficiency and durable oxygen evolution reaction(OER)electrocatalysts is crucial for hydrogen production from seawater splitting.Herein,we report the in situ electrochemical conversion o...Design and development of high-efficiency and durable oxygen evolution reaction(OER)electrocatalysts is crucial for hydrogen production from seawater splitting.Herein,we report the in situ electrochemical conversion of a nanoarray of Ni(TCNQ)2(TCNQ=tetracyanoquinodimethane)on graphite paper into Ni(OH)_(2) nanoparticles confined in a conductive TCNQ nanoarray(Ni(OH)_(2)-TCNQ/GP)by anode oxidation.The Ni(OH)_(2)-TCNQ/GP exhibits high OER performance and demands overpotentials of 340 and 382 mV to deliver 100 mA·cm^(−2) in alkaline freshwater and alkaline seawater,respectively.Meanwhile,the Ni(OH)_(2)-TCNQ/GP also demonstrates steady long-term electrochemical durability for at least 80 h under alkaline seawater.展开更多
To develop highly efficient electrochemical catalysts for N2 fixation is important to sustainable ambient NH_(3) production through the N_(2) reduction reaction(NRR).Herein,we demonstrate the development of vanadium p...To develop highly efficient electrochemical catalysts for N2 fixation is important to sustainable ambient NH_(3) production through the N_(2) reduction reaction(NRR).Herein,we demonstrate the development of vanadium phosphide nanoparticle on V foil as a high-efficiency and stable catalyst for ambient NH3 production with excellent selectivity.The high Faradaic efficiency of 22%with a large NH3 yield of 8.35×10^(−11) mol·s^(−1)·cm^(−2)was obtained at 0 V vs.the reversible hydrogen electrode in acid solution,superior to all previously studied V-based NRR catalysts.Density functional theory calculations are also utilized to have an insight into the catalytic mechanism.展开更多
Seawater electrolysis is the most promising technology for large scale hydrogen production due to the abundance and low cost of seawater in nature.However,compared with the traditional freshwater electrolysis,the issu...Seawater electrolysis is the most promising technology for large scale hydrogen production due to the abundance and low cost of seawater in nature.However,compared with the traditional freshwater electrolysis,the issues of electrode poisoning and corrosion will occur during the seawater electrolysis process,and active and stable electrocatalysts for the hydrogen evolution reaction(HER)are thus highly desired.In this work,N,O-doped carbon foam in-situ derived from commercial melamine foam is proposed as a high-active metal-free HER electrocatalyst for seawater splitting.In acidic seawater,our catalyst shows high hydrogen generation performance with small overpotential of 161 mV at 10 mA·cm^(−2),a low Tafel slop of 97.5 mV·dec^(−1),and outstanding stability.展开更多
Ambient electroreduction of nitrogen(N_(2))is considered as a green and feasible approach for ammonia(NH_(3))synthesis,which urgently demands for efficient electrocatalyst.Morphology has close relationship with cataly...Ambient electroreduction of nitrogen(N_(2))is considered as a green and feasible approach for ammonia(NH_(3))synthesis,which urgently demands for efficient electrocatalyst.Morphology has close relationship with catalytic activity of heterogeneous catalysts.Nanoribbon is attractive nanostructure,which possesses the flexibility of one-dimensional nanomaterials,the large surface area of two-dimensional nanomaterials,and lateral size confinement effects.In this work,Cu_(3)P nanoribbon is proposed as a highly efficient electrocatalyst for N_(2)-to-NH_(3)conversion under benign conditions.When measured in N_(2)-saturated 0.1 M HCl,such Cu_(3)P nanoribbon achieves high performance with an excellent Faradaic efficiency as high as 37.8%and a large yield of 18.9μg·h^(−1)·mgcat.−1 at−0.2 V.It also demonstrates outstanding stability in long-term electrolysis test at least for 45 h.展开更多
An asymmetrical supercapacitor （ASC）, comprising reduced graphene oxide （rGO）-encapsulated nickel phosphite hollow microspheres （NPOH-0.5@rGO） as positive electrode, and porous nitrogen/sulfur co-doped rGO aerog...An asymmetrical supercapacitor （ASC）, comprising reduced graphene oxide （rGO）-encapsulated nickel phosphite hollow microspheres （NPOH-0.5@rGO） as positive electrode, and porous nitrogen/sulfur co-doped rGO aerogel （NS-3D rGO） as negative electrode has been prepared. The NPOH-0.5@rGO electrode combines the advantages of the NPOH hollow microspheres and the conductive rGO layers giving rise to a large specific capacitance, high cycling reversibility, and excellent rate performance. The NS-3D rGO electrode with abundant porosity and active sites promotes electrolyte infiltration and broadens the working voltage range. The ASC （NPOH-0.5@rGO//NS-3D rGO） shows a maximum voltage of up to 1.4 V, outstanding cycling ability （capacitance retention of 95.5% after 10,000 cycles）, and excellent rate capability （capacitance retention of 77% as the current density is increased ten times）. The ASC can light up an light-emitting diodes （LED） for more than 20 min after charging for 20 s. The fabrication technique and device architecture can be extended to other active oxide and carbon-based materials for next-generation high-performance electrochemical storage devices.展开更多
Seawater electrolysis is an extremely attractive approach for harvesting clean hydrogen energy,but detrimental chlorine species(i.e.,chloride and hypochlorite)cause severe corrosion at the anode.Here,we report our rec...Seawater electrolysis is an extremely attractive approach for harvesting clean hydrogen energy,but detrimental chlorine species(i.e.,chloride and hypochlorite)cause severe corrosion at the anode.Here,we report our recent finding that benzoate anions-intercalated NiFe-layered double hydroxide nanosheet on carbon cloth(BZ-NiFe-LDH/CC)behaves as a highly efficient and durable monolithic catalyst for alkaline seawater oxidation,affords enlarged interlayer spacing of LDH,inhibits chlorine(electro)chemistry,and alleviates local pH drop of the electrode.It only needs an overpotential of 320 mV to reach a current density of 500 mA·cm^(−2)in 1 M KOH.In contrast to the fast activity decay of NiFe-LDH/CC counterpart during long-term electrolysis,BZ-NiFe-LDH/CC achieves stable 100-h electrolysis at an industrial-level current density of 500 mA·cm^(−2)in alkaline seawater.Operando Raman spectroscopy studies further identify structural changes of disorderedδ(NiIII-O)during the seawater oxidation process.展开更多
Sustainable mitigation of the continuously rising concentration of NO contaminants is among the most urgent issues of this century.Ambient electrocatalytic conversion of NO into useful NH_(3)offers an attractive path ...Sustainable mitigation of the continuously rising concentration of NO contaminants is among the most urgent issues of this century.Ambient electrocatalytic conversion of NO into useful NH_(3)offers an attractive path toward achieving sustainable NO abatement and NH_(3)production simultaneously.However,its efficiency is challenged by the intense competition from hydrogen evolution reaction and relatively high energy barriers of NO activation.It is thus highly desirable to explore active electrocatalyst for NO reduction reaction and investigate the mechanisms on relevant surfaces.Herein,we introduce an FeP nanorod array on carbon cloth as a high-efficiency catalyst for NO electroreduction to NH3.In 0.2 M phosphate-buffered solution,this catalyst exhibits a low onset potential of-0.014 V.Moreover,it achieves a remarkable Faradaic efficiency of 88.49%and a large NH_(3)yield of 85.62μmol·h^(-1)cm^(-2),with durability for stable NO conversion over 12 h of electrolysis.The catalytic mechanism on FeP is investigated further by theoretical calculations.展开更多
Electrochemical reduction of NO offers us an attractive alternative to traditional selective catalytic reduction process for harmful NO removal and simultaneous NH_(3)production,but it requires efficient electrocataly...Electrochemical reduction of NO offers us an attractive alternative to traditional selective catalytic reduction process for harmful NO removal and simultaneous NH_(3)production,but it requires efficient electrocatalyst to enable the NO reduction reaction with high selectivity.Here,we report on the development of Bi nanoparticles/carbon nanosheet composite(Bi@C)for highly effective NO reduction electrocatalysis toward selective NH_(3)formation.Such Bi@C catalyst attains an impressive NH_(3)yield of 1,592.5μg·h^(−1)·mgcat.^(−1)and a high Faradaic efficiency as high as 93%in 0.1 M Na_(2)SO_(4)electrolyte.Additionally,it can be applied as efficient cathode materials for Zn–NO battery to reduce NO to NH_(3)with high electricity generation.展开更多
Highly sensitive flexible pressure sensors play an important role to ensure the safety and friendliness during the human-robot interaction process.Microengineering the active layer has been shown to improve performanc...Highly sensitive flexible pressure sensors play an important role to ensure the safety and friendliness during the human-robot interaction process.Microengineering the active layer has been shown to improve performance of pressure sensors.However,the current structural strategy almost relying on axial compression deformation suffers structural stifening,and together with the limited area growth efficiency of conformal interface,essentially limiting the maximum sensitivity.Here,inspired by the interface contact behavior of gecko's feet,we design a slant hierarchical microstructure to act as an electrode contacting with an ionic gel layer,fundamentally eliminating the pressure resistance and maximizing functional interface expansion to achieving ultrasensitive sensitivity.Such a structuring strategy dramatically improves the relative capacitance change both in the low-and high-pressure region,thereby boosting the sensitivity up to 36000kPa^(-1) and effective measurement range up to 30okPa.To verify the advantages of high sensitivity,the sensor is integrated with a soft magnetic robot to demonstrate a biomimetic Venus flytrap.The ability to perceive weak stimuli allows the sensor to be used as a sensory and feedback window,realizing the capture of small live insects and the transportation of fragile objects.展开更多
基金the National Natural Science Foundation of China(Nos.21575137 and 11704005)。
文摘Electrocatalytic N2 reduction to NH3 under ambient conditions is an eco-friendly and sustainable alternative to the traditional Haber-Bosch process. However, inhibited by the high activation barrier of N2, this process needs efficient electrocatalysts to adsorb and activate the N2, enabling the N2 reduction reaction(NRR). Herein, we report that porous LaFeO3 nanofiber with oxygen vacancies acts as an efficient NRR electrocatalyst with abundant active sites to enhance the adsorption and activation of N2. When tested in 0.1 M HCl, such electrocatalyst achieves a high Faradaic efficiency of 8.77% and a large NH3 yield rate of 18.59 μg h–1 mgcat–1.at-0.55 V versus reversible hydrogen electrode. This catalyst also shows high long-term electrochemical stability and excellent selectivity for NH3 formation. Density functional theory calculations reveal that, by introducing oxygen vacancy on LaFeO3, the subsurface metallic ions are exposed with newly localized electronic states near the Fermi level, which facilitates the adsorption and activation of N2 molecules as well as the subsequent hydrogenation reactions.
基金National Natural Science Foundation of China,Grant/Award Numbers:42277485,21976141,22272197,22102184,22102136,U22A20392Natural Science Foundation of Hubei Province,Grant/Award Numbers:2022CFB1001,2021CFA034+1 种基金Department of Education of Hubei Province,Grant/Award Numbers:Q20221701,Q20221704Joint Fund of Yulin University and Dalian National Laboratory for Clean Energy,Grant/Award Number:YLU-DNL Fund 2022008。
文摘The electrocatalytic synthesis of C-N coupling compounds from CO_(2) and nitrogenous species not only offers an effective avenue to achieve carbon neutral-ity and reduce environmental pollution,but also establishes a route to synthesize valuable chemicals,such as urea,amide,and amine.This innovative approach expands the application range and product categories beyond simple carbona-ceous species in electrocatalytic CO_(2) reduction,which is becoming a rapidly advancing field.This review summarizes the research progress in electrocatalytic urea synthesis,using N_(2),NO_(2)^(-),and NO_(3)^(-)as nitrogenous species,and explores emerging trends in the electrosynthesis of amide and amine from CO_(2) and nitro-gen species.Additionally,the future opportunities in this field are highlighted,including electrosynthesis of amino acids and other compounds containing C-N bonds,anodic C-N coupling reactions beyond water oxidation,and the catalytic mechanism of corresponding reactions.This critical review also captures the insights aimed at accelerating the development of electrochemical C-N coupling reactions,confirming the superiority of this electrochemical method over the traditional techniques.
基金the National Key Research and Development Program of China(No.2021YFB2011500)the National Natural Science Foundation of China(Nos.52025055 and 51905415)+4 种基金Institutional Foundation of The First Affiliated Hospital of Xi’an Jiaotong University,the China Gas Turbine Establishment of Aero Engine Corporation of China(No.GJCZ-2019-0039)the National Postdoctoral Program for Innovative Talents(No.BX20180251)Young Talent Fund of University Association for Science and Technology in Shaanxi,China(No.20200404)Basic Research Program of Natural Science of Shaanxi Province of China(Nos.2019JLM-5 and 2021JLM-42)Shaanxi University Youth Innovation Team.
文摘The integrated perception capable of detecting and monitoring varieties of activities is one of the ultimate purposes of wearable electronics and intelligent robots.Limited by the space occupation,it lacks practical feasibility to stack multiple types of single sensors on each other.Herein,a high-sensitivity dual-function capacitive sensor with proximity sensing and pressure sensing is proposed.The fringing electric field can be confined in the proximity-sensitive area by fibrous loop-patterned electrode,leading to more stolen charges when object approaching and thus a high proximity sensitivity.The high-permittivity doped structured dielectric layer reduces the compressive stiffness and enhances the rate of compression-caused increase in the equivalent relative permittivity of the dielectric layer,resulting in a larger increase in capacitance and thus a high pressure sensitivity.The electrodes and dielectric layer together compose the capacitor and act as the sensor without taking up additional space.The decoupling of proximity-sensing and pressure-sensing modes can be achieved by decrease or increase in capacitance.Combined with array distribution and sequential scanning,the sensors can be used for detection of motion trajectory,contour recognition,pressure distribution.
文摘Electrochemical nitrogen reduction reaction(NRR)is considered as an alternative to the industrial Haber-Bosch process for NH3 production due to both low energy consumption and environment friendliness.However,the major problem of electrochemical NRR is the unsatisfied efficiency and selectivity of electrocatalyst.As one group of the cheapest and most abundant transition metals,iron-group(Fe,Co,Ni and Cu)electrocatalysts show promising potential on cost and performance advantages as ideal substitute for traditional noble-metal catalysts.In this minireview,we summarize recent advances of iron-group-based materials(including their oxides,hydroxides,nitrides,sulfides and phosphides,etc.)as non-noble metal electrocatalysts towards ambient N2-to-NH3 conversion in aqueous media.Strategies to boost NRR performances and perspectives for future developments are discussed to provide guidance for the field of NRR studies.
文摘As a carbon-neutral alternative to the Haber-Bosch process,electrochemical N2 reduction enables environment-friendly NH3 synthesis at ambient conditions but needs active electrocatalysts for the N2 reduction reaction.Here,we report that conductive metal-organic framework CO3(hexahydroxytriphenylene)2(Co3 HHTP2)nanoparticles act as an efficient catalyst for ambient electrochemical N2-to-NH3 fixation.When tested in 0.5 M LiClO4,such Co3 HHTP2 achieves a large NH3 yield of 22.14μg·h^-1·mg^-1 cat.with a faradaic efficiency of 3.34%at-0.40 V versus the reversible hydrogen electrode.This catalyst also shows high electrochemical stability and excellent selectivity toward NH3 synthesis.
基金supported by the National Natural Science Foundation of China(No.22072015)the Opening Fund of Key Laboratory of Chemical Biology and Traditional Chinese Medicine Research(Hunan Normal University)Ministry of Education(2020-02).
文摘Design and development of high-efficiency and durable oxygen evolution reaction(OER)electrocatalysts is crucial for hydrogen production from seawater splitting.Herein,we report the in situ electrochemical conversion of a nanoarray of Ni(TCNQ)2(TCNQ=tetracyanoquinodimethane)on graphite paper into Ni(OH)_(2) nanoparticles confined in a conductive TCNQ nanoarray(Ni(OH)_(2)-TCNQ/GP)by anode oxidation.The Ni(OH)_(2)-TCNQ/GP exhibits high OER performance and demands overpotentials of 340 and 382 mV to deliver 100 mA·cm^(−2) in alkaline freshwater and alkaline seawater,respectively.Meanwhile,the Ni(OH)_(2)-TCNQ/GP also demonstrates steady long-term electrochemical durability for at least 80 h under alkaline seawater.
基金This work is financially supported by the National Natural Science Foundation of China （Nos. 61574122, 51502257, 21373107 and U1304108）, the Innovative Research Team （in Science and Technology） in Universities in Henan Province （No. 13IRTSTHN018）, the Key Project of Henan Educational Committee （No. 15A140035）, and the program for Science ＆ Technology Innovation Talents in Universities of Henan Province （No. 15HASTIT018）.
文摘为在便携电子学的申请的灵活、容易可配置的 supercapacitors 表演伟人诺言。在这研究， multiwall C nanotubes (CNT ) 与层次 ultrathin 装饰了锌硫化物(ZnS ) nanosheets (ZnS@CNT ) 经由一个灵巧的方法被综合。产生 ZnS@CNT 电极，它交付 347.3 F
基金supported by the National Natural Science Foundation of China(No.21575137).
文摘To develop highly efficient electrochemical catalysts for N2 fixation is important to sustainable ambient NH_(3) production through the N_(2) reduction reaction(NRR).Herein,we demonstrate the development of vanadium phosphide nanoparticle on V foil as a high-efficiency and stable catalyst for ambient NH3 production with excellent selectivity.The high Faradaic efficiency of 22%with a large NH3 yield of 8.35×10^(−11) mol·s^(−1)·cm^(−2)was obtained at 0 V vs.the reversible hydrogen electrode in acid solution,superior to all previously studied V-based NRR catalysts.Density functional theory calculations are also utilized to have an insight into the catalytic mechanism.
基金supported by the National Natural Science Foundation of China(No.22072015).
文摘Seawater electrolysis is the most promising technology for large scale hydrogen production due to the abundance and low cost of seawater in nature.However,compared with the traditional freshwater electrolysis,the issues of electrode poisoning and corrosion will occur during the seawater electrolysis process,and active and stable electrocatalysts for the hydrogen evolution reaction(HER)are thus highly desired.In this work,N,O-doped carbon foam in-situ derived from commercial melamine foam is proposed as a high-active metal-free HER electrocatalyst for seawater splitting.In acidic seawater,our catalyst shows high hydrogen generation performance with small overpotential of 161 mV at 10 mA·cm^(−2),a low Tafel slop of 97.5 mV·dec^(−1),and outstanding stability.
基金the National Natural Science Foundation of China(No.22072015)the Opening Fund of Key Laboratory of Chemical Biology and Traditional Chinese Medicine Research(Hunan Normal University),Ministry of Education(No.2020-02)+2 种基金Young Elite Scientist Sponsorship Program by CAST(No.YESS20210226)the Youth Innovation Promotion Association of the Chinese Academy of Sciences(No.2020354)Deanship of Scientific Research at King Khalid University,Abha,Saudi Arabia for funding this work through the Research Group Program under No.RGP.2/79/43.
文摘Ambient electroreduction of nitrogen(N_(2))is considered as a green and feasible approach for ammonia(NH_(3))synthesis,which urgently demands for efficient electrocatalyst.Morphology has close relationship with catalytic activity of heterogeneous catalysts.Nanoribbon is attractive nanostructure,which possesses the flexibility of one-dimensional nanomaterials,the large surface area of two-dimensional nanomaterials,and lateral size confinement effects.In this work,Cu_(3)P nanoribbon is proposed as a highly efficient electrocatalyst for N_(2)-to-NH_(3)conversion under benign conditions.When measured in N_(2)-saturated 0.1 M HCl,such Cu_(3)P nanoribbon achieves high performance with an excellent Faradaic efficiency as high as 37.8%and a large yield of 18.9μg·h^(−1)·mgcat.−1 at−0.2 V.It also demonstrates outstanding stability in long-term electrolysis test at least for 45 h.
基金This work was jointly supported by the National Natural Science Foundation of China （No. 51572246）, Fundamental Research Funds for the Central Universi- ties （Nos. 53200859565, 53200859500 and 2652015425）, as well as City University of Hong Kong Applied Research Grant （ARG） （No. 9667122） and Strategic Research Grant （SRG） （No. 7004644）.
文摘An asymmetrical supercapacitor （ASC）, comprising reduced graphene oxide （rGO）-encapsulated nickel phosphite hollow microspheres （NPOH-0.5@rGO） as positive electrode, and porous nitrogen/sulfur co-doped rGO aerogel （NS-3D rGO） as negative electrode has been prepared. The NPOH-0.5@rGO electrode combines the advantages of the NPOH hollow microspheres and the conductive rGO layers giving rise to a large specific capacitance, high cycling reversibility, and excellent rate performance. The NS-3D rGO electrode with abundant porosity and active sites promotes electrolyte infiltration and broadens the working voltage range. The ASC （NPOH-0.5@rGO//NS-3D rGO） shows a maximum voltage of up to 1.4 V, outstanding cycling ability （capacitance retention of 95.5% after 10,000 cycles）, and excellent rate capability （capacitance retention of 77% as the current density is increased ten times）. The ASC can light up an light-emitting diodes （LED） for more than 20 min after charging for 20 s. The fabrication technique and device architecture can be extended to other active oxide and carbon-based materials for next-generation high-performance electrochemical storage devices.
基金supported by the National Natural Science Foundation of China(No.21575137).
文摘Seawater electrolysis is an extremely attractive approach for harvesting clean hydrogen energy,but detrimental chlorine species(i.e.,chloride and hypochlorite)cause severe corrosion at the anode.Here,we report our recent finding that benzoate anions-intercalated NiFe-layered double hydroxide nanosheet on carbon cloth(BZ-NiFe-LDH/CC)behaves as a highly efficient and durable monolithic catalyst for alkaline seawater oxidation,affords enlarged interlayer spacing of LDH,inhibits chlorine(electro)chemistry,and alleviates local pH drop of the electrode.It only needs an overpotential of 320 mV to reach a current density of 500 mA·cm^(−2)in 1 M KOH.In contrast to the fast activity decay of NiFe-LDH/CC counterpart during long-term electrolysis,BZ-NiFe-LDH/CC achieves stable 100-h electrolysis at an industrial-level current density of 500 mA·cm^(−2)in alkaline seawater.Operando Raman spectroscopy studies further identify structural changes of disorderedδ(NiIII-O)during the seawater oxidation process.
基金This work was supported by the National Natural Science Foundation of China(Nos.52076045 and 22072015)。
文摘Sustainable mitigation of the continuously rising concentration of NO contaminants is among the most urgent issues of this century.Ambient electrocatalytic conversion of NO into useful NH_(3)offers an attractive path toward achieving sustainable NO abatement and NH_(3)production simultaneously.However,its efficiency is challenged by the intense competition from hydrogen evolution reaction and relatively high energy barriers of NO activation.It is thus highly desirable to explore active electrocatalyst for NO reduction reaction and investigate the mechanisms on relevant surfaces.Herein,we introduce an FeP nanorod array on carbon cloth as a high-efficiency catalyst for NO electroreduction to NH3.In 0.2 M phosphate-buffered solution,this catalyst exhibits a low onset potential of-0.014 V.Moreover,it achieves a remarkable Faradaic efficiency of 88.49%and a large NH_(3)yield of 85.62μmol·h^(-1)cm^(-2),with durability for stable NO conversion over 12 h of electrolysis.The catalytic mechanism on FeP is investigated further by theoretical calculations.
基金supported by the National Natural Science Foundation of China(No.22072015)the Opening Fund of Key Laboratory of Chemical Biology and Traditional Chinese Medicine Research(Hunan Normal University),Ministry of Education(2020-02).
文摘Electrochemical reduction of NO offers us an attractive alternative to traditional selective catalytic reduction process for harmful NO removal and simultaneous NH_(3)production,but it requires efficient electrocatalyst to enable the NO reduction reaction with high selectivity.Here,we report on the development of Bi nanoparticles/carbon nanosheet composite(Bi@C)for highly effective NO reduction electrocatalysis toward selective NH_(3)formation.Such Bi@C catalyst attains an impressive NH_(3)yield of 1,592.5μg·h^(−1)·mgcat.^(−1)and a high Faradaic efficiency as high as 93%in 0.1 M Na_(2)SO_(4)electrolyte.Additionally,it can be applied as efficient cathode materials for Zn–NO battery to reduce NO to NH_(3)with high electricity generation.
基金This work was supported by the National Key Research and Development Programof China(Grant No.2021YFB2011500)National Natural Science Foundation of China(Grant Nos.52025055 and 51905415)+4 种基金Natural ScienceFoundationofShaanxiProvince,China(2019JLM-5)Institutional Foundation of the First Affiliated Hospital of Xi'an Jiaotong University,China Gas Turbine Establishment of Aero Engine Corporation of China(GJCZ-2019-0039)National Postdoctoral Program for InnovativeTalents(No.BX20180251)hina Postdoctoral ScienceFoundation(No.2019M653588)YoungTalent Fund of UniversityAssociationfor ScienceandTechnology in Shaanxi,China(20200404).
文摘Highly sensitive flexible pressure sensors play an important role to ensure the safety and friendliness during the human-robot interaction process.Microengineering the active layer has been shown to improve performance of pressure sensors.However,the current structural strategy almost relying on axial compression deformation suffers structural stifening,and together with the limited area growth efficiency of conformal interface,essentially limiting the maximum sensitivity.Here,inspired by the interface contact behavior of gecko's feet,we design a slant hierarchical microstructure to act as an electrode contacting with an ionic gel layer,fundamentally eliminating the pressure resistance and maximizing functional interface expansion to achieving ultrasensitive sensitivity.Such a structuring strategy dramatically improves the relative capacitance change both in the low-and high-pressure region,thereby boosting the sensitivity up to 36000kPa^(-1) and effective measurement range up to 30okPa.To verify the advantages of high sensitivity,the sensor is integrated with a soft magnetic robot to demonstrate a biomimetic Venus flytrap.The ability to perceive weak stimuli allows the sensor to be used as a sensory and feedback window,realizing the capture of small live insects and the transportation of fragile objects.
