The graphitic carbon nitride(g-C_3N_4) which is a two-dimensional conjugated polymer has drawn broad interdisciplinary attention as a low-cost, metal-free, and visible-light-responsive photocatalyst in the area of env...The graphitic carbon nitride(g-C_3N_4) which is a two-dimensional conjugated polymer has drawn broad interdisciplinary attention as a low-cost, metal-free, and visible-light-responsive photocatalyst in the area of environmental remediation. The g-C_3N_4-based materials have excellent electronic band structures, electron-rich properties, basic surface functionalities, high physicochemical stabilities and are ‘‘earth-abundant.'' This review summarizes the latest progress related to the design and construction of g-C_3N_4-based materials and their applications including catalysis, sensing,imaging, and white-light-emitting diodes. An outlook on possible further developments in g-C_3N_4-based research for emerging properties and applications is also included.展开更多
Clean energy and a sustainable environment are grand challenges that the world is facing which can be addressed by converting solar energy into transportable and storable fuels(chemical fuel).The main scientific and t...Clean energy and a sustainable environment are grand challenges that the world is facing which can be addressed by converting solar energy into transportable and storable fuels(chemical fuel).The main scientific and technological challenges for efficient solar energy conversion,energy storage,and environmental applications are the stability,durability,and performance of low-cost functional materials.Among different nanomaterials,perovskite type LaFeO_(3)has been extensively investigated as a photocatalyst due to its abundance,high stability,compositional and structural fexibility,high electrocatalytic activity,efficient sunlight absorption,and tunable band gap and band edges.Hence,it is urgent to write a comprehensive review to highlight the trend,challenges,and prospects of LaFeO_(3)in the field of photocatalytic solar energy conversion and environment purification.This critical review summarizes the history and basic principles of photocatalysis.Further,it reviews in detail the LaFeO_(3),applications,shortcomings,and activity enhancement strategies including the design of nanostructures,elemental doping,and heterojunctions construction such as Type-I,Type-II,Z-Type,and uncommon heterojunctions.Besides,the optical and electronic properties,charge carriers separation,electron transport phenomenon and alignment of the band gaps in LaFeO_(3)-based heterostructures are comprehensively discussed.展开更多
The dynamic phase transition properties for ferroelectric nanotube under a spin-1/2 transverse Ising model are studied under the effective field theory(EFT)with correlations.The temperature effects on the pseudo-spin ...The dynamic phase transition properties for ferroelectric nanotube under a spin-1/2 transverse Ising model are studied under the effective field theory(EFT)with correlations.The temperature effects on the pseudo-spin systems are unveiled in three-dimensional(3-D)and two-dimensional(2-D)phase diagrams.Moreover,the dynamic behaviors of exchange interactions on the 3-D and 2-D phase transitions under high temperature are exhibited.The results present that it is hard to obtain pure ferroelectric phase under high temperature;that is,the vibration of orderly pseudo-spins cannot be eliminated completely.展开更多
Spin engineering is recognized as a promising strategy that modulates the association between d‐orbital electrons and the oxygenated species,and enhances the catalytic kinetics.However,few efforts have been made to c...Spin engineering is recognized as a promising strategy that modulates the association between d‐orbital electrons and the oxygenated species,and enhances the catalytic kinetics.However,few efforts have been made to clarify whether spin engineering could make a considerable enhancement for electrocatalytic water oxidation.Herein,we report the spin engineering of a nanocage‐structured(Co,Ni)Se_(2)/C@FeOOH,that showed significant oxygen evolution reaction(OER)activity.Magnetization measurement presented that the(Co,Ni)Se_(2)/C@FeOOH sample possesses higher polarization spin number(μb=6.966μB/f.u.)compared with that of the(Co,Ni)Se_(2)/C sample(μb=6.398μB/f.u.),for which the enlarged spin polarization number favors the adsorption and desorption energy of the intermediate oxygenated species,as confirmed by surface valance band spectra.Consequently,the(Co,Ni)Se_(2)/C@FeOOH affords remarkable OER product with a low overpotential of 241 mV at a current of 10 mA cm^(-2) and small Tafel slope of 44 mV dec^(-1) in 1.0 mol/L KOH alkaline solution,significantly surpassing the parent(Co,Ni)Se_(2)/C catalyst.This work will trigger a solid step for the design of highly‐efficient OER electrocatalysts.展开更多
In this paper, an advanced distributed energy-efficient clustering (ADEEC) protocol was proposed with the aim of balancing energy consumption across the nodes to achieve longer network lifetime for In-Vehicle Wireless...In this paper, an advanced distributed energy-efficient clustering (ADEEC) protocol was proposed with the aim of balancing energy consumption across the nodes to achieve longer network lifetime for In-Vehicle Wireless Sensor Networks (IVWSNs). The algorithm changes the cluster head selection probability based on residual energy and location distribution of nodes. Then node associate with the cluster head with least communication cost and high residual energy. Simulation results show that ADEEC achieves longer stability period, network lifetime,and throughput than the other classical clustering algorithms.展开更多
Highly active and low-cost oxygen evolution reaction(OER)catalytic electrodes are extremely essential for exploration of green hydrogen via water splitting.Herein,an advanced Fe-Ni-F electrocatalyst is fabricated by a...Highly active and low-cost oxygen evolution reaction(OER)catalytic electrodes are extremely essential for exploration of green hydrogen via water splitting.Herein,an advanced Fe-Ni-F electrocatalyst is fabricated by a facile annealing strategy using ammonium fluoride,of which the structure feature is unveiled by XRD,FESEM,TEM,EDS,BET,and XPS measurements.The as-prepared Fe-Ni-F addresses a low overpotential of 277 mV and a small Tafel slope of 49 mV dec^(-1)at a current density of 10 mA cm^(-2),significantly outperforming other control samples as well as the state-of-the-art RuO_(2).The advanced nature of our Fe-Ni-F catalyst could also be further evidenced from the robust stability in KOH alkaline solution,showing as 5.41%degradation after 24 h continuous working.Upon analysis,it suggests that the decent catalytic activity should be attributed to the formed bimetallic(oxy)hydroxides because of the introduction of fluoride and the synergistic effect of iron and nickel towards oxygen generation.This work represents the potential of Fe-and/or Ni-based fluoride as efficient catalyst for low-energy consumption oxygen generation.展开更多
The release of anthropogenic CO_(2)emissions into the atmosphere has significantly accelerated global warming within the past few decades.According to the latest data,it is predicted that the concentration of CO_(2)wi...The release of anthropogenic CO_(2)emissions into the atmosphere has significantly accelerated global warming within the past few decades.According to the latest data,it is predicted that the concentration of CO_(2)will rise to 800 ppm over this century,and could reach 2000 ppm by 2300.Such high level of CO_(2)is expected to result in significant increase in global temperature as well as ocean acidification[1].展开更多
Anodic urea oxidation reaction(UOR)is an intriguing half reaction that can replace oxygen evolution reaction(OER)and work together with hydrogen evolution reaction(HER)toward simultaneous hydrogen fuel generation and ...Anodic urea oxidation reaction(UOR)is an intriguing half reaction that can replace oxygen evolution reaction(OER)and work together with hydrogen evolution reaction(HER)toward simultaneous hydrogen fuel generation and urea-rich wastewater purification;however,it remains a challenge to achieve overall urea electrolysis with high efficiency.Herein,we report a multifunctional electrocatalyst termed as Rh/Ni V-LDH,through integration of nickel-vanadium layered double hydroxide(LDH)with rhodium single-atom catalyst(SAC),to achieve this goal.The electrocatalyst delivers high HER mass activity of0.262 A mg^(-1) and exceptionally high turnover frequency(TOF)of 2.125 s^(-1) at an overpotential of100 m V.Moreover,exceptional activity toward urea oxidation is addressed,which requires a potential of 1.33 V to yield 10 mA cm^(-2),endorsing the potential to surmount the sluggish OER.The splendid catalytic activity is enabled by the synergy of the Ni V-LDH support and the atomically dispersed Rh sites(located on the Ni-V hollow sites)as evidenced both experimentally and theoretically.The selfsupported Rh/Ni V-LDH catalyst serving as the anode and cathode for overall urea electrolysis(1 mol L^(-1) KOH with 0.33 mol L^(-1) urea as electrolyte)only requires a small voltage of 1.47 V to deliver 100 mA cm^(-2) with excellent stability.This work provides important insights into multifunctional SAC design from the perspective of support sites toward overall electrolysis applications.展开更多
Highly active and low-cost catalytic electrodes for urea oxidation reaction(UOR)are always crucial for exploration of urea fuel cells.Herein,novel york-shell-structural Ni_(2)P/C na nosphere hybrids(Ni_(2)P/C-YS)are r...Highly active and low-cost catalytic electrodes for urea oxidation reaction(UOR)are always crucial for exploration of urea fuel cells.Herein,novel york-shell-structural Ni_(2)P/C na nosphere hybrids(Ni_(2)P/C-YS)are rationally constructed via a hydrothermal method and subsequent phosphidation treatment under different temperature ranging from 250℃to 450℃for UOR applications.In the in-situ constructed hollow york-shell structure,the coupling of conductive carbon materials and active Ni_(2)P allows numerous interfaces facilitating the electron transfer and thereby accelerating the catalytic kinetics.The results demonstrate that Ni_(2)P/C-YS-350 nanocomposite can boost the UOR process with a low potential of 1.366 V vs.RHE at a current density of 50 mA/cm^(2) in alkaline electrolyte and afford the superior durability with negligible potential decay after 23 h.This study presents that the carbon coated Ni_(2)P hybrid with the optimized crystallinities and hollow york-shell configurations can be a promising candidate for application in urea fuel cells.展开更多
Electrocatalytic urea oxidation reaction(UOR)is regarded as an effective yet challenging approach for the degradation of urea in wastewater into harmless N2 and CO_(2).To overcome the sluggish kinetics,catalytically a...Electrocatalytic urea oxidation reaction(UOR)is regarded as an effective yet challenging approach for the degradation of urea in wastewater into harmless N2 and CO_(2).To overcome the sluggish kinetics,catalytically active sites should be rationally designed to maneuver the multiple key steps of intermediate adsorption and desorption.Herein,we demonstrate that metal-organic frameworks(MOFs)can provide an ideal platform for tailoring binary active sites to facilitate the rate-determining steps,achieving remarkable electrocatalytic activity toward UOR.Specifically,the MOF(namely,NiMn_(0.14)-BDC)based on Ni/Mn sites and terephthalic acid(BDC)ligands exhibits a low voltage of 1.317 V to deliver a current density of 10 mA cm^(-2).As a result,a high turnover frequency(TOF)of 0.15 s^(-1) is achieved at a voltage of 1.4 V,which enables a urea degradation rate of 81.87%in 0.33 M urea solution.The combination of experimental characterization with theoretical calculation reveals that the Ni and Mn sites play synergistic roles in maneuvering the evolution of urea molecules and key reaction intermediates during the UOR,while the binary Ni/Mn sites in MOF offer the tunability for electronic structure and d-band center impacting on the intermediate evolution.This work provides important insights into active site design by leveraging MOF platform and represents a solid step toward highly efficient UOR with MOF-based electrocatalysts.展开更多
文摘The graphitic carbon nitride(g-C_3N_4) which is a two-dimensional conjugated polymer has drawn broad interdisciplinary attention as a low-cost, metal-free, and visible-light-responsive photocatalyst in the area of environmental remediation. The g-C_3N_4-based materials have excellent electronic band structures, electron-rich properties, basic surface functionalities, high physicochemical stabilities and are ‘‘earth-abundant.'' This review summarizes the latest progress related to the design and construction of g-C_3N_4-based materials and their applications including catalysis, sensing,imaging, and white-light-emitting diodes. An outlook on possible further developments in g-C_3N_4-based research for emerging properties and applications is also included.
基金financially supported by the Ministry of Science and Technology of China(Grant No.2018YFA0702100)the National Natural Science Foundation of China(Grant Nos.11874169,51972129)+3 种基金the National Key R&D Program of China(Grant No.2017YFE0120500)the Key Research and Development Program of Hubei(Grant No.2020BAB079)the South Xinjiang Innovation and Development Program of Key Industries of Xinjiang Production and Construction Corps(Grants No.2020DB002)the Hubei‘‘Chu-Tian Young Scholar”program.
文摘Clean energy and a sustainable environment are grand challenges that the world is facing which can be addressed by converting solar energy into transportable and storable fuels(chemical fuel).The main scientific and technological challenges for efficient solar energy conversion,energy storage,and environmental applications are the stability,durability,and performance of low-cost functional materials.Among different nanomaterials,perovskite type LaFeO_(3)has been extensively investigated as a photocatalyst due to its abundance,high stability,compositional and structural fexibility,high electrocatalytic activity,efficient sunlight absorption,and tunable band gap and band edges.Hence,it is urgent to write a comprehensive review to highlight the trend,challenges,and prospects of LaFeO_(3)in the field of photocatalytic solar energy conversion and environment purification.This critical review summarizes the history and basic principles of photocatalysis.Further,it reviews in detail the LaFeO_(3),applications,shortcomings,and activity enhancement strategies including the design of nanostructures,elemental doping,and heterojunctions construction such as Type-I,Type-II,Z-Type,and uncommon heterojunctions.Besides,the optical and electronic properties,charge carriers separation,electron transport phenomenon and alignment of the band gaps in LaFeO_(3)-based heterostructures are comprehensively discussed.
基金Project supported by the National Key R&D Program of China(Grant No.2017YFE0120500)the National Natural Science Foundation of China(Grant No.51972129)+3 种基金the South Xinjiang Innovation and Development Program of Key Industries of Xinjiang Production and Construction Corps(Grant No.2020DB002)the Fundamental Research Funds for the Central Universities,China(Grant Nos.HUST 2018KFYYXJJ051 and 2019KFYXMBZ076)Shenzhen Fundamental Research Fund(Grant No.JCYJ20190813172609404)the Hubei“Chu-Tian Young Scholar”Program。
文摘The dynamic phase transition properties for ferroelectric nanotube under a spin-1/2 transverse Ising model are studied under the effective field theory(EFT)with correlations.The temperature effects on the pseudo-spin systems are unveiled in three-dimensional(3-D)and two-dimensional(2-D)phase diagrams.Moreover,the dynamic behaviors of exchange interactions on the 3-D and 2-D phase transitions under high temperature are exhibited.The results present that it is hard to obtain pure ferroelectric phase under high temperature;that is,the vibration of orderly pseudo-spins cannot be eliminated completely.
文摘Spin engineering is recognized as a promising strategy that modulates the association between d‐orbital electrons and the oxygenated species,and enhances the catalytic kinetics.However,few efforts have been made to clarify whether spin engineering could make a considerable enhancement for electrocatalytic water oxidation.Herein,we report the spin engineering of a nanocage‐structured(Co,Ni)Se_(2)/C@FeOOH,that showed significant oxygen evolution reaction(OER)activity.Magnetization measurement presented that the(Co,Ni)Se_(2)/C@FeOOH sample possesses higher polarization spin number(μb=6.966μB/f.u.)compared with that of the(Co,Ni)Se_(2)/C sample(μb=6.398μB/f.u.),for which the enlarged spin polarization number favors the adsorption and desorption energy of the intermediate oxygenated species,as confirmed by surface valance band spectra.Consequently,the(Co,Ni)Se_(2)/C@FeOOH affords remarkable OER product with a low overpotential of 241 mV at a current of 10 mA cm^(-2) and small Tafel slope of 44 mV dec^(-1) in 1.0 mol/L KOH alkaline solution,significantly surpassing the parent(Co,Ni)Se_(2)/C catalyst.This work will trigger a solid step for the design of highly‐efficient OER electrocatalysts.
文摘In this paper, an advanced distributed energy-efficient clustering (ADEEC) protocol was proposed with the aim of balancing energy consumption across the nodes to achieve longer network lifetime for In-Vehicle Wireless Sensor Networks (IVWSNs). The algorithm changes the cluster head selection probability based on residual energy and location distribution of nodes. Then node associate with the cluster head with least communication cost and high residual energy. Simulation results show that ADEEC achieves longer stability period, network lifetime,and throughput than the other classical clustering algorithms.
基金supported by the National Natural Science Foundation of China(No.51804223,52272202)the Innovation Foundation of Key Laboratory of Green Chemical Process of Ministry of Education(No.GCX202113)+1 种基金Bintuan Science and Technology Program(No.2020DB002,2022DB009)the Shenzhen Science and Technology Innovation Committee(No.JCYJ20200109141412308).
文摘Highly active and low-cost oxygen evolution reaction(OER)catalytic electrodes are extremely essential for exploration of green hydrogen via water splitting.Herein,an advanced Fe-Ni-F electrocatalyst is fabricated by a facile annealing strategy using ammonium fluoride,of which the structure feature is unveiled by XRD,FESEM,TEM,EDS,BET,and XPS measurements.The as-prepared Fe-Ni-F addresses a low overpotential of 277 mV and a small Tafel slope of 49 mV dec^(-1)at a current density of 10 mA cm^(-2),significantly outperforming other control samples as well as the state-of-the-art RuO_(2).The advanced nature of our Fe-Ni-F catalyst could also be further evidenced from the robust stability in KOH alkaline solution,showing as 5.41%degradation after 24 h continuous working.Upon analysis,it suggests that the decent catalytic activity should be attributed to the formed bimetallic(oxy)hydroxides because of the introduction of fluoride and the synergistic effect of iron and nickel towards oxygen generation.This work represents the potential of Fe-and/or Ni-based fluoride as efficient catalyst for low-energy consumption oxygen generation.
基金supported by National Natural Science Foundation of China(Nos.51972129,52272202)the National Key R&D Program of China(No.2022YFB3807201)Bintuan Science and Technology Program(Nos.2020DB002,2022DB009).
文摘The release of anthropogenic CO_(2)emissions into the atmosphere has significantly accelerated global warming within the past few decades.According to the latest data,it is predicted that the concentration of CO_(2)will rise to 800 ppm over this century,and could reach 2000 ppm by 2300.Such high level of CO_(2)is expected to result in significant increase in global temperature as well as ocean acidification[1].
基金finically supported by the National Key R&D Program of China(2017YFE0120500)the National Natural Science Foundation of China(51972129,51702150,and 21725102)+2 种基金the Key Research and Development Program of Hubei(2020BAB079)Bintuan Science and Technology Program(2020DB002,and 2022DB009)the Science and Technology Innovation Committee Foundation of Shenzhen(JCYJ20210324141613032 and JCYJ20190809142019365)。
文摘Anodic urea oxidation reaction(UOR)is an intriguing half reaction that can replace oxygen evolution reaction(OER)and work together with hydrogen evolution reaction(HER)toward simultaneous hydrogen fuel generation and urea-rich wastewater purification;however,it remains a challenge to achieve overall urea electrolysis with high efficiency.Herein,we report a multifunctional electrocatalyst termed as Rh/Ni V-LDH,through integration of nickel-vanadium layered double hydroxide(LDH)with rhodium single-atom catalyst(SAC),to achieve this goal.The electrocatalyst delivers high HER mass activity of0.262 A mg^(-1) and exceptionally high turnover frequency(TOF)of 2.125 s^(-1) at an overpotential of100 m V.Moreover,exceptional activity toward urea oxidation is addressed,which requires a potential of 1.33 V to yield 10 mA cm^(-2),endorsing the potential to surmount the sluggish OER.The splendid catalytic activity is enabled by the synergy of the Ni V-LDH support and the atomically dispersed Rh sites(located on the Ni-V hollow sites)as evidenced both experimentally and theoretically.The selfsupported Rh/Ni V-LDH catalyst serving as the anode and cathode for overall urea electrolysis(1 mol L^(-1) KOH with 0.33 mol L^(-1) urea as electrolyte)only requires a small voltage of 1.47 V to deliver 100 mA cm^(-2) with excellent stability.This work provides important insights into multifunctional SAC design from the perspective of support sites toward overall electrolysis applications.
基金financially supported by the National Key Research and Development Program of China(No.2017YFE0120500)the National Natural Science Foundation of China(Nos.51804223 and 51972129)+4 种基金CAS Key Laboratory of Nano-Bio Interface(No.19ZY01)the South Xinjiang Innovation and Development Program of Key Industries of Xinjiang Production and Construction Corps(No.2020DB002)the Scientific Research Foundation of Wuhan Institute of Technology(No.K201761)the Fundamental Research Funds for the Central Universities(Nos.HUST 2018KFYYXJJ051,2019KFYXMBZ076)the Hubei"Chu-Tian Young Scholar"Program。
文摘Highly active and low-cost catalytic electrodes for urea oxidation reaction(UOR)are always crucial for exploration of urea fuel cells.Herein,novel york-shell-structural Ni_(2)P/C na nosphere hybrids(Ni_(2)P/C-YS)are rationally constructed via a hydrothermal method and subsequent phosphidation treatment under different temperature ranging from 250℃to 450℃for UOR applications.In the in-situ constructed hollow york-shell structure,the coupling of conductive carbon materials and active Ni_(2)P allows numerous interfaces facilitating the electron transfer and thereby accelerating the catalytic kinetics.The results demonstrate that Ni_(2)P/C-YS-350 nanocomposite can boost the UOR process with a low potential of 1.366 V vs.RHE at a current density of 50 mA/cm^(2) in alkaline electrolyte and afford the superior durability with negligible potential decay after 23 h.This study presents that the carbon coated Ni_(2)P hybrid with the optimized crystallinities and hollow york-shell configurations can be a promising candidate for application in urea fuel cells.
基金This work is finically supported by the National Key R&D Program of China(Grant No.2017YFE0120500)the National Natural Science Foundation of China(Grant Nos.51972129,21725102)+3 种基金the Bintuan Science and Technology Program(Grant Nos.2020DB002,2022DB009)the Key Research and Development Program of Hubei(Grant No.2020BAB079)the Science and Technology Innovation Committee Foundation of Shenzhen(Grant No.JCYJ20210324141613032)the Natural Science Foundation of Jiangsu Province of China(BK20211609).
文摘Electrocatalytic urea oxidation reaction(UOR)is regarded as an effective yet challenging approach for the degradation of urea in wastewater into harmless N2 and CO_(2).To overcome the sluggish kinetics,catalytically active sites should be rationally designed to maneuver the multiple key steps of intermediate adsorption and desorption.Herein,we demonstrate that metal-organic frameworks(MOFs)can provide an ideal platform for tailoring binary active sites to facilitate the rate-determining steps,achieving remarkable electrocatalytic activity toward UOR.Specifically,the MOF(namely,NiMn_(0.14)-BDC)based on Ni/Mn sites and terephthalic acid(BDC)ligands exhibits a low voltage of 1.317 V to deliver a current density of 10 mA cm^(-2).As a result,a high turnover frequency(TOF)of 0.15 s^(-1) is achieved at a voltage of 1.4 V,which enables a urea degradation rate of 81.87%in 0.33 M urea solution.The combination of experimental characterization with theoretical calculation reveals that the Ni and Mn sites play synergistic roles in maneuvering the evolution of urea molecules and key reaction intermediates during the UOR,while the binary Ni/Mn sites in MOF offer the tunability for electronic structure and d-band center impacting on the intermediate evolution.This work provides important insights into active site design by leveraging MOF platform and represents a solid step toward highly efficient UOR with MOF-based electrocatalysts.