Rechargeable lithium-oxygen(Li-O_(2))batteries have attracted wide attention due to their high energy density.However,the sluggish cathode kinetics results in high overvoltage and poor cycling performance.Ruthenium(Ru...Rechargeable lithium-oxygen(Li-O_(2))batteries have attracted wide attention due to their high energy density.However,the sluggish cathode kinetics results in high overvoltage and poor cycling performance.Ruthenium(Ru)-based electrocatalysts have been demonstrated to be promising cathode catalysts to promote oxygen evolution reaction(OER).It facilitates decomposition of lithium peroxide(Li_(2)O_(2))by adjusting Li_(2)O_(2) morphologies,which is due to the strong interaction between Ru-based catalyst and superoxide anion(O_(2))intermediate.In this review,the design strategies of Ru-based electrocatalysts are introduced to enhance their OER catalytic kinetics in Li-O_(2) batteries.Different configurations of Ru-based catalysts,including metal particles(Ru metal and alloys),single-atom catalysts,and Ru-loaded compounds with various substrates(carbon materials,metal oxides/sulfides),have been summarized to regulate the electronic structure and the matrix architecture of the Ru-based electrocatalysts.The structure-property relationship of Ru-based catalysts is discussed for a better understanding of the Li_(2)O_(2) decomposition mechanism at the cathode interface.Finally,the challenges of Ru-based electrocatalysts are proposed for the future development of Li-O_(2) batteries.展开更多
The investigation of highly effective,durable,and cost-effective electrocatalysts for the hydrogen evolution reaction(HER)is a prerequisite for the upcoming hydrogen energy society.To establish a new hydrogen energy s...The investigation of highly effective,durable,and cost-effective electrocatalysts for the hydrogen evolution reaction(HER)is a prerequisite for the upcoming hydrogen energy society.To establish a new hydrogen energy system and gradually replace the traditional fossil-based energy,electrochemical water-splitting is considered the most promising,environmentally friendly,and efficient way to produce pure hydrogen.Compared with the commonly used platinum(Pt)-based catalysts,ruthenium(Ru)is expected to be a good alternative because of its similar hydrogen bonding energy,lower water decomposition barrier,and considerably lower price.Analyzing and revealing the HER mechanisms,as well as identifying a rational design of Ru-based HER catalysts with desirable activity and stability is indispensable.In this review,the research progress on HER electrocatalysts and the relevant describing parameters for HER performance are briefly introduced.Moreover,four major strategies to improve the performance of Ru-based electrocatalysts,including electronic effect modulation,support engineering,structure design,and maximum utilization(single atom)are discussed.Finally,the challenges,solutions and prospects are highlighted to prompt the practical applications of Rubased electrocatalysts for HER.展开更多
Supported Ru-based catalysts, prepared by a surfactant-stabilized colloidal method, exhibited a good selectivity to bis（4-aminocyclohexyl）methane via the hydrogenation of 4,4′-methylenedianiline. Transmission elect...Supported Ru-based catalysts, prepared by a surfactant-stabilized colloidal method, exhibited a good selectivity to bis（4-aminocyclohexyl）methane via the hydrogenation of 4,4′-methylenedianiline. Transmission electron microscopy（TEM） and X-ray diffraction（XRD） characterization showed Ru nanoparticles were well-dispersed on activated carbon, leading to the high activity and selectivity to the product.展开更多
The highly dispersed supported ruthenium-yttrium (Ru-Y) bimetallic catalysts were prepared by impregnation method and their catalytic performance for hydrogenation of ester was fully investigated. The catalyst was cha...The highly dispersed supported ruthenium-yttrium (Ru-Y) bimetallic catalysts were prepared by impregnation method and their catalytic performance for hydrogenation of ester was fully investigated. The catalyst was characterized by X-ray diffraction and field emission scanning electron microscopy. The results show that the average particle diameter of the bimetallic crystallites was less than 10 nm. The effects of the reaction temperature, the hydrogen pressure, the amount of catalyst and the proportion of yttrium in catalyst on the hydrogenation of ester were studied. The experimental results show that the introduction of yttrium not only changed the chemical and textural properties of ruthenium-based catalyst but also controlled the formation of Ru-Y alloy. The Ru-Y catalyst (Ru-2%Y/TiO2) exhibited high catalytic activity and good selectivity towards the higher alcohols. Under optimal reaction conditions of 240°C and 5 MPa hydrogen pressure, the conversion of palm oil esters was above 93.4% while the selectivity towards alcohol was above 99.0%.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
Engineering the internal structure and chemical composition of nanomaterials in a cost-effective way has been challenging, especially for enhancing their performance for a given application. Herein, we report a genera...Engineering the internal structure and chemical composition of nanomaterials in a cost-effective way has been challenging, especially for enhancing their performance for a given application. Herein, we report a general strategy to fabricate hollow nanostructures of ruthenium-based binary or ternary oxides via a galvanic replacement process together with a subsequent thermal treatment. In particular,the as-prepared NiO-RuO_2 hollow nanostructures loaded on carbon nanotubes(hNiO-RuO_2/CNT) with RuO_2 mass ratio at 19.6% for a supercapacitor adopting the KOH electrolyte exhibit high specific capacitances of 740 F g^(-1) at a constant current density of 1 A g^(-1) with good cycle stability. The specific capacitance for hNiO-RuO_2/CNT electrodes maintains638.4 F g^(-1) at a current density of 5 A g^(-1). This simple approach may shed some light on the way for making a wide range of metal oxides with tunable nanostructures and compositions for a variety of applications.展开更多
基金the National Natural Science Foundation of China(22325902 and 51671107)Haihe Laboratory of Sustainable Chemical Transformations.
文摘Rechargeable lithium-oxygen(Li-O_(2))batteries have attracted wide attention due to their high energy density.However,the sluggish cathode kinetics results in high overvoltage and poor cycling performance.Ruthenium(Ru)-based electrocatalysts have been demonstrated to be promising cathode catalysts to promote oxygen evolution reaction(OER).It facilitates decomposition of lithium peroxide(Li_(2)O_(2))by adjusting Li_(2)O_(2) morphologies,which is due to the strong interaction between Ru-based catalyst and superoxide anion(O_(2))intermediate.In this review,the design strategies of Ru-based electrocatalysts are introduced to enhance their OER catalytic kinetics in Li-O_(2) batteries.Different configurations of Ru-based catalysts,including metal particles(Ru metal and alloys),single-atom catalysts,and Ru-loaded compounds with various substrates(carbon materials,metal oxides/sulfides),have been summarized to regulate the electronic structure and the matrix architecture of the Ru-based electrocatalysts.The structure-property relationship of Ru-based catalysts is discussed for a better understanding of the Li_(2)O_(2) decomposition mechanism at the cathode interface.Finally,the challenges of Ru-based electrocatalysts are proposed for the future development of Li-O_(2) batteries.
基金supported by the Key Research and Development Project of Hainan Province(ZDYF2020037,ZDYF2020207)the National Natural Science Foundation of China(21805104)+1 种基金Innovative Research Projects for Graduate Students of Hainan Province(Hyb2020-05)the Start-up Research Foundation of Hainan University(KYQD(ZR)-20008,20083,20084)。
文摘The investigation of highly effective,durable,and cost-effective electrocatalysts for the hydrogen evolution reaction(HER)is a prerequisite for the upcoming hydrogen energy society.To establish a new hydrogen energy system and gradually replace the traditional fossil-based energy,electrochemical water-splitting is considered the most promising,environmentally friendly,and efficient way to produce pure hydrogen.Compared with the commonly used platinum(Pt)-based catalysts,ruthenium(Ru)is expected to be a good alternative because of its similar hydrogen bonding energy,lower water decomposition barrier,and considerably lower price.Analyzing and revealing the HER mechanisms,as well as identifying a rational design of Ru-based HER catalysts with desirable activity and stability is indispensable.In this review,the research progress on HER electrocatalysts and the relevant describing parameters for HER performance are briefly introduced.Moreover,four major strategies to improve the performance of Ru-based electrocatalysts,including electronic effect modulation,support engineering,structure design,and maximum utilization(single atom)are discussed.Finally,the challenges,solutions and prospects are highlighted to prompt the practical applications of Rubased electrocatalysts for HER.
基金Supported by the National High Technology Research and Development Program of China(No.2007AA03Z345)
文摘Supported Ru-based catalysts, prepared by a surfactant-stabilized colloidal method, exhibited a good selectivity to bis（4-aminocyclohexyl）methane via the hydrogenation of 4,4′-methylenedianiline. Transmission electron microscopy（TEM） and X-ray diffraction（XRD） characterization showed Ru nanoparticles were well-dispersed on activated carbon, leading to the high activity and selectivity to the product.
文摘The highly dispersed supported ruthenium-yttrium (Ru-Y) bimetallic catalysts were prepared by impregnation method and their catalytic performance for hydrogenation of ester was fully investigated. The catalyst was characterized by X-ray diffraction and field emission scanning electron microscopy. The results show that the average particle diameter of the bimetallic crystallites was less than 10 nm. The effects of the reaction temperature, the hydrogen pressure, the amount of catalyst and the proportion of yttrium in catalyst on the hydrogenation of ester were studied. The experimental results show that the introduction of yttrium not only changed the chemical and textural properties of ruthenium-based catalyst but also controlled the formation of Ru-Y alloy. The Ru-Y catalyst (Ru-2%Y/TiO2) exhibited high catalytic activity and good selectivity towards the higher alcohols. Under optimal reaction conditions of 240°C and 5 MPa hydrogen pressure, the conversion of palm oil esters was above 93.4% while the selectivity towards alcohol was above 99.0%.
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(2117322621376247+4 种基金21573240and 21506225)Center for MesoscienceInstitute of Process EngineeringChinese Academy of Sciences(COM2015A001)the Knowledge Innovation Program of the Chinese Academy of Sciences(KGCX2-YW-341)
文摘Engineering the internal structure and chemical composition of nanomaterials in a cost-effective way has been challenging, especially for enhancing their performance for a given application. Herein, we report a general strategy to fabricate hollow nanostructures of ruthenium-based binary or ternary oxides via a galvanic replacement process together with a subsequent thermal treatment. In particular,the as-prepared NiO-RuO_2 hollow nanostructures loaded on carbon nanotubes(hNiO-RuO_2/CNT) with RuO_2 mass ratio at 19.6% for a supercapacitor adopting the KOH electrolyte exhibit high specific capacitances of 740 F g^(-1) at a constant current density of 1 A g^(-1) with good cycle stability. The specific capacitance for hNiO-RuO_2/CNT electrodes maintains638.4 F g^(-1) at a current density of 5 A g^(-1). This simple approach may shed some light on the way for making a wide range of metal oxides with tunable nanostructures and compositions for a variety of applications.
