Nitric oxide(NO),which generally originates from vehicle exhaust and industrial flue gases,is one of the most serious air pollutants.In this case,the electrochemical NO reduction reaction(NORR)not only removes the atm...Nitric oxide(NO),which generally originates from vehicle exhaust and industrial flue gases,is one of the most serious air pollutants.In this case,the electrochemical NO reduction reaction(NORR)not only removes the atmospheric pollutant NO but also produces valuable ammonia(NH_(3)).Hence,through the synthesis and modification of Fe_(3)C nanocrystal cata-lysts,the as-obtained optimal sample of Fe_(3)C/C-900 was adopted as the NORR catalyst at ambient conditions.As a result,the Fe_(3)C/C-900 catalyst showed an NH_(3)Faraday efficiency of 76.5%and an NH_(3)yield rate of 177.5μmol·h^(-1)·cm^(-2)at the working potentials of-0.8 and-1.2 V versus reversible hydrogen electrode(vs.RHE),respectively.And it delivered a stable NORR activity during the electrolysis.Moreover,we attribute the high NORR properties of Fe_(3)C/C-900 to two aspects:one is the enhanced intrinsic activity of Fe_(3)C nanocrystals,including the lowering of the energy barrier of rate-limiting step(*NOH→*N)and the inhibition of hydrogen evolution;on the other hand,the favorable dispersion of active components,the effective adsorption of gaseous NO,and the release of liquid NH_(3)products facilitated by the porous carbon substrate.展开更多
The practical applications of carbon anode for lithium-ion batteries(LIBs)are largely obstructed by their moderate rate capability and cyclic stability.Herein,we report a N,S-codoped porous carbon nanosheet(NSC)decora...The practical applications of carbon anode for lithium-ion batteries(LIBs)are largely obstructed by their moderate rate capability and cyclic stability.Herein,we report a N,S-codoped porous carbon nanosheet(NSC)decorated with Fe_(3)C nanoparticles(Fe_(3)C/NSC)by a one-pot pyrolysis process.The high surface area and abundant defects of NSC can not only promote electrons and ions transfer,but also induce high pseudocapacitive contribution.More importantly,the synergistic catalysis effect of Fe-Nx and Fe_(3)C can catalyze the reversible conversion of some solid electrolyte interface(SEI)components to offer excess capacity during cycling.As expected,the Fe_(3)C-NSC anode delivers a discharge capacity of750 mAh·g^(-1)under a current density of 0.5 A·g^(-1)through 500 cycles and retains a dis-charge capacity of 366 mAh·g^(-1)at 4 A·g^(-1)after 1600 cycles,respectively.Most importantly,the lithium-ion capacitors based on Fe_(3)C/NSC anode demonstrate a high energy density of 249.5 Wh·kg^(-1)at 560 W·kg^(-1).展开更多
Iron-based anodes for lithium-ion batteries(LIBs)with higher theoretical capacity,natural abundance and cheapness have received considerable attention,but they still suffer from the fast capacity fading.To address thi...Iron-based anodes for lithium-ion batteries(LIBs)with higher theoretical capacity,natural abundance and cheapness have received considerable attention,but they still suffer from the fast capacity fading.To address this issue,we report a facile synthesis of plate-like carbonsupported Fe_(3)C nanoparticles through chemical blowing/carbonization under calcination.The ultrafine Fe_(3)C nanoparticles are prone to be oxidized when exposing in air;thus,Fe_(3)C/C with mild oxidization and the fully oxidized product of Fe_(2)O_(3)/C are successfully prepared by controlling the oxidization condition.When applied as an anode material in LIB,the Fe_(3)C/C electrode demonstrates excellent cycle stability(826 mAh·g^(-1)after 120 cycles under 500 mA·g^(-1))and rate performance(410.6 mAh·g^(-1) under 2 A·g^(-1)),compared with the Fe_(2)O_(3)/C counterpart.The enhanced electrochemical performance can be ascribed to the synergetic effect of the Fe_(3)C with mild oxidation and the unique hierarchical structure of plate-like carbon decorated with Fe_(3)C catalyst.More importantly,this work may offer new approaches to synthesize other transition metal(e.g.,Co,Ni)-based anode material by replacing the precursor ingredient.展开更多
Efficient bifunctional oxygen electrocatalysts for ORR and OER are fundamental to the development of high performance metal-air batteries.Herein,a facile cost-efficient two-step pyrolysis strategy for the fabrication ...Efficient bifunctional oxygen electrocatalysts for ORR and OER are fundamental to the development of high performance metal-air batteries.Herein,a facile cost-efficient two-step pyrolysis strategy for the fabrication of a bifunctional oxygen electrocatalyst has been proposed.The efficient non-preciousmetal-based electrocatalyst,Fe/Fe_(3)C@Fe-N_(x)-C consists of highly curved onion-like carbon shells that encapsulate Fe/Fe_(3)C nanoparticles,distributed on an extensively porous graphitic carbon aerogel.The obtained Fe/Fe_(3)C@Fe-N_(x)-C aerogel exhibited superb electrochemical activity,excellent durability,and high methanol tolerance.The experimental results indicated that the assembly of onion-like carbon shells with encapsulated Fe/Fe_(3)C yielded highly curved carbon surfaces with abundant Fe-Nxactive sites,a porous structure,and enhanced electrocatalytic activity towards ORR and OER,hence displaying promising potential for application as an air cathode in rechargeable Zn-air batteries.The constructed Zn-air battery possessed an exceptional peak power density of~147 mW cm^(-2),outstanding cycling stability(200 cycles,1 h per cycle),and a small voltage gap of 0.87 V.This study offers valuable insights regarding the construction of low-cost and highly active bifunctional oxygen electrocatalysts for efficient air batteries.展开更多
The improvement of catalysts’stability under harsh reaction conditions is vital for their practical applica-bility.Herein,iron carbide(Fe_(3)C)nanoparticles were encapsulated in graphitic carbon in situ and a carbon ...The improvement of catalysts’stability under harsh reaction conditions is vital for their practical applica-bility.Herein,iron carbide(Fe_(3)C)nanoparticles were encapsulated in graphitic carbon in situ and a carbon ball served as the carrier.The synthesized Fe_(3)C@C/C was first utilized to treat an m-cresol wastewater containing Si via catalytic ozonation.Compared with the commercial Fe/Al_(2)O_(3)catalyst,the resistance to Si of the Fe_(3)C@C/C was improved 22.68 times,while the TOC removal rate increased by a factor of 2.9,and it remained stable during 10 cycles and 12000 min of continuous reaction,which further demon-strated its potential for diverse applications.The catalyst exhibits improved resistance to Si because of the dual protection from the carbon-encapsulated structure and carbon carrier.Density functional theory calculations show that the encapsulation of Fe_(3)C using carbon significantly increases the resistance to adsorption of Si on its active sites.In addition,the activation of O_(3)is unimpeded on the Fe_(3)C adsorption sites by the protection from C,thus the generation of reactive oxygen species(ROS)by ozone is largely promoted.The mechanism associated with the resistance of the Fe_(3)C@C/C catalyst to Si and its elevated activity are also elucidated.展开更多
基金supported by the Guangxi Natural Science Fund for Distinguished Young Scholars(2024GXNSFFA010008)Shenzhen Science and Technology Program(JCYJ20230807112503008).
文摘Nitric oxide(NO),which generally originates from vehicle exhaust and industrial flue gases,is one of the most serious air pollutants.In this case,the electrochemical NO reduction reaction(NORR)not only removes the atmospheric pollutant NO but also produces valuable ammonia(NH_(3)).Hence,through the synthesis and modification of Fe_(3)C nanocrystal cata-lysts,the as-obtained optimal sample of Fe_(3)C/C-900 was adopted as the NORR catalyst at ambient conditions.As a result,the Fe_(3)C/C-900 catalyst showed an NH_(3)Faraday efficiency of 76.5%and an NH_(3)yield rate of 177.5μmol·h^(-1)·cm^(-2)at the working potentials of-0.8 and-1.2 V versus reversible hydrogen electrode(vs.RHE),respectively.And it delivered a stable NORR activity during the electrolysis.Moreover,we attribute the high NORR properties of Fe_(3)C/C-900 to two aspects:one is the enhanced intrinsic activity of Fe_(3)C nanocrystals,including the lowering of the energy barrier of rate-limiting step(*NOH→*N)and the inhibition of hydrogen evolution;on the other hand,the favorable dispersion of active components,the effective adsorption of gaseous NO,and the release of liquid NH_(3)products facilitated by the porous carbon substrate.
基金financially supported by the National Science Foundation of China (Nos. 51772169, 52072217 and 51802261)the National Key R&D Program of China (No. 2018YFB0905400)+2 种基金the Major Technological Innovation Project of Hubei Science and Technology Department (No. 2019AAA164)the Natural Science Foundation of Hubei Province of China (No. 2019CFB337)the Natural Science Foundation of Hubei Provincial Department of Education (No. Q20191204)
文摘The practical applications of carbon anode for lithium-ion batteries(LIBs)are largely obstructed by their moderate rate capability and cyclic stability.Herein,we report a N,S-codoped porous carbon nanosheet(NSC)decorated with Fe_(3)C nanoparticles(Fe_(3)C/NSC)by a one-pot pyrolysis process.The high surface area and abundant defects of NSC can not only promote electrons and ions transfer,but also induce high pseudocapacitive contribution.More importantly,the synergistic catalysis effect of Fe-Nx and Fe_(3)C can catalyze the reversible conversion of some solid electrolyte interface(SEI)components to offer excess capacity during cycling.As expected,the Fe_(3)C-NSC anode delivers a discharge capacity of750 mAh·g^(-1)under a current density of 0.5 A·g^(-1)through 500 cycles and retains a dis-charge capacity of 366 mAh·g^(-1)at 4 A·g^(-1)after 1600 cycles,respectively.Most importantly,the lithium-ion capacitors based on Fe_(3)C/NSC anode demonstrate a high energy density of 249.5 Wh·kg^(-1)at 560 W·kg^(-1).
基金financially supported by State Grid Corporation of China(No.5202011600TY)。
文摘Iron-based anodes for lithium-ion batteries(LIBs)with higher theoretical capacity,natural abundance and cheapness have received considerable attention,but they still suffer from the fast capacity fading.To address this issue,we report a facile synthesis of plate-like carbonsupported Fe_(3)C nanoparticles through chemical blowing/carbonization under calcination.The ultrafine Fe_(3)C nanoparticles are prone to be oxidized when exposing in air;thus,Fe_(3)C/C with mild oxidization and the fully oxidized product of Fe_(2)O_(3)/C are successfully prepared by controlling the oxidization condition.When applied as an anode material in LIB,the Fe_(3)C/C electrode demonstrates excellent cycle stability(826 mAh·g^(-1)after 120 cycles under 500 mA·g^(-1))and rate performance(410.6 mAh·g^(-1) under 2 A·g^(-1)),compared with the Fe_(2)O_(3)/C counterpart.The enhanced electrochemical performance can be ascribed to the synergetic effect of the Fe_(3)C with mild oxidation and the unique hierarchical structure of plate-like carbon decorated with Fe_(3)C catalyst.More importantly,this work may offer new approaches to synthesize other transition metal(e.g.,Co,Ni)-based anode material by replacing the precursor ingredient.
基金supported financially by the National Natural Science Foundation of China,China(Grant No.51702180,51572136,91963113,21703116,51372127,51873096)The Scientific and Technical Development Project of Qingdao,China(Grant No.18-2-2-52-jch)+1 种基金The Taishan Scholar Advantage and Characteristic Discipline Team of Eco Chemical Process and TechnologyThe Natural Science Foundation of Hebei Province(B2019204009)。
文摘Efficient bifunctional oxygen electrocatalysts for ORR and OER are fundamental to the development of high performance metal-air batteries.Herein,a facile cost-efficient two-step pyrolysis strategy for the fabrication of a bifunctional oxygen electrocatalyst has been proposed.The efficient non-preciousmetal-based electrocatalyst,Fe/Fe_(3)C@Fe-N_(x)-C consists of highly curved onion-like carbon shells that encapsulate Fe/Fe_(3)C nanoparticles,distributed on an extensively porous graphitic carbon aerogel.The obtained Fe/Fe_(3)C@Fe-N_(x)-C aerogel exhibited superb electrochemical activity,excellent durability,and high methanol tolerance.The experimental results indicated that the assembly of onion-like carbon shells with encapsulated Fe/Fe_(3)C yielded highly curved carbon surfaces with abundant Fe-Nxactive sites,a porous structure,and enhanced electrocatalytic activity towards ORR and OER,hence displaying promising potential for application as an air cathode in rechargeable Zn-air batteries.The constructed Zn-air battery possessed an exceptional peak power density of~147 mW cm^(-2),outstanding cycling stability(200 cycles,1 h per cycle),and a small voltage gap of 0.87 V.This study offers valuable insights regarding the construction of low-cost and highly active bifunctional oxygen electrocatalysts for efficient air batteries.
基金This work was financially supported by the Youth Innovation Promotion Association CAS(No.2020190)the National Natural Science Foundation of China(No.52100072)+1 种基金the Scientific Research Common Program of Beijing Municipal,Commission of Education(No.KM202010017006)the Beijing Natural Science Foundation(No.8214056).
文摘The improvement of catalysts’stability under harsh reaction conditions is vital for their practical applica-bility.Herein,iron carbide(Fe_(3)C)nanoparticles were encapsulated in graphitic carbon in situ and a carbon ball served as the carrier.The synthesized Fe_(3)C@C/C was first utilized to treat an m-cresol wastewater containing Si via catalytic ozonation.Compared with the commercial Fe/Al_(2)O_(3)catalyst,the resistance to Si of the Fe_(3)C@C/C was improved 22.68 times,while the TOC removal rate increased by a factor of 2.9,and it remained stable during 10 cycles and 12000 min of continuous reaction,which further demon-strated its potential for diverse applications.The catalyst exhibits improved resistance to Si because of the dual protection from the carbon-encapsulated structure and carbon carrier.Density functional theory calculations show that the encapsulation of Fe_(3)C using carbon significantly increases the resistance to adsorption of Si on its active sites.In addition,the activation of O_(3)is unimpeded on the Fe_(3)C adsorption sites by the protection from C,thus the generation of reactive oxygen species(ROS)by ozone is largely promoted.The mechanism associated with the resistance of the Fe_(3)C@C/C catalyst to Si and its elevated activity are also elucidated.
