Seawater electrolysis is a promising approach for sustainable energy without relying on precious freshwater.However,the large-scale seawater electrolysis is hindered by low catalytic efficiency and severe anode corros...Seawater electrolysis is a promising approach for sustainable energy without relying on precious freshwater.However,the large-scale seawater electrolysis is hindered by low catalytic efficiency and severe anode corrosion caused by the harmful chlorine.In contrast to the oxygen evolution reaction (OER)and chlorin ion oxidation reaction (ClOR),glycerol oxidation reaction (GOR) is more thermodynamically and kinetically favorable alternative.Herein,a Ru doping cobalt phosphide (Ru-CoP_(2)) is proposed as a robust bifunctional electrocatalyst for seawater electrolysis and GOR,for the concurrent productions of hydrogen and value-added formate.The in situ and ex situ characterization analyses demonstrated that Ru doping featured in the dynamic reconstruction process from Ru-CoP_(2)to Ru-CoOOH,accounting for the superior GOR performance.Further coupling GOR with hydrogen evolution was realized by employing Ru-CoP_(2)as both anode and cathode,requiring only a low voltage of 1.43 V at 100 mA cm^(-2),which was 250 m V lower than that in alkaline seawater.This work guides the design of bifunctional electrocatalysts for energy-efficient seawater electrolysis coupled with biomass resource upcycling.展开更多
Nitrogen dioxide(NO_(2))is a significant air pollutant with harmful effects on human health and the environment.Timely and accurate monitoring of NO_(2)concentrations is crucial for improving air quality and protectin...Nitrogen dioxide(NO_(2))is a significant air pollutant with harmful effects on human health and the environment.Timely and accurate monitoring of NO_(2)concentrations is crucial for improving air quality and protecting public health.However,quantifying NO_(2)in the presence of other gases remains challenging.Herein,we integrate Ru onto the MoS_(2)surface to form Ru-S-Mo active sites,thereby tuning the electronic structure of MoS_(2)for enhanced NO_(2)detection.This sensor shows excellent sensitivity(29.7%at 100×10^(-6)NO_(2)and 25℃),with a linear response to NO_(2)ranging from 0.5 to 200×10^(-6),and a significantly reduced response/recovery time from 160/3636 s for pure MoS_(2)to 58/427 s for Ru@MoS_(2)at 100×10^(-6)NO_(2).Additionally,the sensor is highly selective for NO_(2),exhibiting a response 14 times higher than for other gases,and possesses strong anti-interference capabilities,accurately quantifying NO_(2)in the presence of varying H_(2)concentrations(10×10^(-6)-200×10^(-6))with a low RSD of 5.34%.A portable wireless NO_(2)monitoring system was successfully constructed using Ru@MoS_(2),enabling real-time gas leak detection(10×10^(-6)-50×10^(-6))with hazard warnings and maintaining a stable response to NO_(2)over a 4-week period.This work extends the gas sensing applications of MoS_(2)and provides a portable,wireless,and high-selectivity NO_(2)sensing method for environmental monitoring and safety assurance.展开更多
We successfully synthesize a series of polycrystalline CeRuxFe1-xCe3(0≤x≤0.5)samples,which are characterized using powder x-ray diffraction,resistivity and specific heat measurements.The expansion of the lattice c...We successfully synthesize a series of polycrystalline CeRuxFe1-xCe3(0≤x≤0.5)samples,which are characterized using powder x-ray diffraction,resistivity and specific heat measurements.The expansion of the lattice constants with increasing x demonstrates the successful doping of Ru into the CeFeGe3 lattice.Upon doping,it is found that the temperature up to which Landau-Fermi liquid behavior is observed in the resistivity is reduced.Meanwhile,there is also a pronounced increase in the resistivity coefficient and residual resistivity,as well as a clear upturn in C/T at low temperatures,suggesting that Ru doping may tune the system towards a quantum critical point.展开更多
At present,Ru dopants mainly enhance electrocatalytic performance by inducing strain,vacancy,local electron difference,and synergy.Surprisingly,this work innovatively proposes that trace Ru atoms induce dual-reconstru...At present,Ru dopants mainly enhance electrocatalytic performance by inducing strain,vacancy,local electron difference,and synergy.Surprisingly,this work innovatively proposes that trace Ru atoms induce dual-reconstruction of phosphide by regulating the electronic configuration and proportion of Co–P/Co–O species,and ultimately activate superb electrocatalytic performance.Specifically,Ru-CoFeP@C/nickel foam(NF)is reconstructed to generate hydrophilic Co(OH)_(2)nanosheets during the hydrogen evolution reaction(HER)process,further accelerating the alkaline HER kinetics of phosphide.And the as-formed CoOOH during the oxygen evolution reaction(OER)process directly accelerates the oxygen overflow efficiency.As expected,the overpotential at 100 mA·cm^(−2)(η100)values of the reconstructed Ru-CoFeP@C/NF are 0.104 and 0.257 V for HER and OER,which are greatly lower than that of Pt/C-NF and RuO_(2)-NF benchmarks,respectively.This work provides guidance for the construction of highperformance catalysts for HER and OER dual reconstruction.This work provides a new idea for the optimization of catalyst structure and electrocatalytic performance.展开更多
基金National Natural Science Foundation of China (Nos. 42276035, 22309030)Guangdong Basic and Applied Basic Research Foundation (Nos. 2023A1515012589,2020A1515110473)Key Plat Form Programs and Technology Innovation Team Project of Guangdong Provincial Department of Education (Nos. 2019GCZX002, 2020KCXTD011)。
文摘Seawater electrolysis is a promising approach for sustainable energy without relying on precious freshwater.However,the large-scale seawater electrolysis is hindered by low catalytic efficiency and severe anode corrosion caused by the harmful chlorine.In contrast to the oxygen evolution reaction (OER)and chlorin ion oxidation reaction (ClOR),glycerol oxidation reaction (GOR) is more thermodynamically and kinetically favorable alternative.Herein,a Ru doping cobalt phosphide (Ru-CoP_(2)) is proposed as a robust bifunctional electrocatalyst for seawater electrolysis and GOR,for the concurrent productions of hydrogen and value-added formate.The in situ and ex situ characterization analyses demonstrated that Ru doping featured in the dynamic reconstruction process from Ru-CoP_(2)to Ru-CoOOH,accounting for the superior GOR performance.Further coupling GOR with hydrogen evolution was realized by employing Ru-CoP_(2)as both anode and cathode,requiring only a low voltage of 1.43 V at 100 mA cm^(-2),which was 250 m V lower than that in alkaline seawater.This work guides the design of bifunctional electrocatalysts for energy-efficient seawater electrolysis coupled with biomass resource upcycling.
基金supported by the Natural Science Foundation of Henan Province,China(No.242300421226)the scientific research program of innovation platform in State Tobacco Monopoly Administration.
文摘Nitrogen dioxide(NO_(2))is a significant air pollutant with harmful effects on human health and the environment.Timely and accurate monitoring of NO_(2)concentrations is crucial for improving air quality and protecting public health.However,quantifying NO_(2)in the presence of other gases remains challenging.Herein,we integrate Ru onto the MoS_(2)surface to form Ru-S-Mo active sites,thereby tuning the electronic structure of MoS_(2)for enhanced NO_(2)detection.This sensor shows excellent sensitivity(29.7%at 100×10^(-6)NO_(2)and 25℃),with a linear response to NO_(2)ranging from 0.5 to 200×10^(-6),and a significantly reduced response/recovery time from 160/3636 s for pure MoS_(2)to 58/427 s for Ru@MoS_(2)at 100×10^(-6)NO_(2).Additionally,the sensor is highly selective for NO_(2),exhibiting a response 14 times higher than for other gases,and possesses strong anti-interference capabilities,accurately quantifying NO_(2)in the presence of varying H_(2)concentrations(10×10^(-6)-200×10^(-6))with a low RSD of 5.34%.A portable wireless NO_(2)monitoring system was successfully constructed using Ru@MoS_(2),enabling real-time gas leak detection(10×10^(-6)-50×10^(-6))with hazard warnings and maintaining a stable response to NO_(2)over a 4-week period.This work extends the gas sensing applications of MoS_(2)and provides a portable,wireless,and high-selectivity NO_(2)sensing method for environmental monitoring and safety assurance.
基金Supported by the National Natural Science Foundation of China under Grant Nos 11474251,11604291 and U1632275the National Key Research and Development Program of China under Grant Nos 2017YFA0303100 and 2016YFA0300202the Science Challenge Project of China under Grant No TZ2016004
文摘We successfully synthesize a series of polycrystalline CeRuxFe1-xCe3(0≤x≤0.5)samples,which are characterized using powder x-ray diffraction,resistivity and specific heat measurements.The expansion of the lattice constants with increasing x demonstrates the successful doping of Ru into the CeFeGe3 lattice.Upon doping,it is found that the temperature up to which Landau-Fermi liquid behavior is observed in the resistivity is reduced.Meanwhile,there is also a pronounced increase in the resistivity coefficient and residual resistivity,as well as a clear upturn in C/T at low temperatures,suggesting that Ru doping may tune the system towards a quantum critical point.
基金supported by the National Natural Science Foundation of China(Nos.52072197 and 21971132)the 111 Project of China(No.D20017)+5 种基金Outstanding Youth Foundation of Shandong Province,China(No.ZR2019JQ14)Natural Science Foundation of Shandong Province,China(No.ZR2022QE098)Major Scientific and Technological Innovation Project(No.2019JZZY020405)Major Basic Research Program of Natural Science Foundation of Shandong Province under Grant(No.ZR2020ZD09)Qingdao Postdoctoral Researcher Applied Research Project(No.04030431060100)Postdoctoral Innovation Project of Shandong Province(No.SDCX-ZG-20220307).
文摘At present,Ru dopants mainly enhance electrocatalytic performance by inducing strain,vacancy,local electron difference,and synergy.Surprisingly,this work innovatively proposes that trace Ru atoms induce dual-reconstruction of phosphide by regulating the electronic configuration and proportion of Co–P/Co–O species,and ultimately activate superb electrocatalytic performance.Specifically,Ru-CoFeP@C/nickel foam(NF)is reconstructed to generate hydrophilic Co(OH)_(2)nanosheets during the hydrogen evolution reaction(HER)process,further accelerating the alkaline HER kinetics of phosphide.And the as-formed CoOOH during the oxygen evolution reaction(OER)process directly accelerates the oxygen overflow efficiency.As expected,the overpotential at 100 mA·cm^(−2)(η100)values of the reconstructed Ru-CoFeP@C/NF are 0.104 and 0.257 V for HER and OER,which are greatly lower than that of Pt/C-NF and RuO_(2)-NF benchmarks,respectively.This work provides guidance for the construction of highperformance catalysts for HER and OER dual reconstruction.This work provides a new idea for the optimization of catalyst structure and electrocatalytic performance.