Hydrogen peroxide(H_(2)O_(2))oxidation and reduction reactions(HPOR/HPRR)are pivotal in various innovative electrochemical energy conversion devices.A comprehensive understanding of these mechanisms is critical for ca...Hydrogen peroxide(H_(2)O_(2))oxidation and reduction reactions(HPOR/HPRR)are pivotal in various innovative electrochemical energy conversion devices.A comprehensive understanding of these mechanisms is critical for catalyst design and performance improvement in these applications.In this work,we systematically investigate the HPOR/HPRR mechanisms on low-index Pt surfaces,specifically Pt(111),Pt(100)and Pt(110),through density functional theory(DFT)calculations combined with the computational hydrogen electrode(CHE)model.For HPOR,all the low-index Pt surfaces exhibit a unified potential-determining step(PDS)involving the electrochemical oxidation of hydroperoxyl intermediates(HOO*).The binding free energy of HOO*(Δ_(GHOO*))emerges as an activity descriptor,with Pt(110)exhibiting the highest HPOR activity.The HPRR mechanism follows a chem-electrochemical(C-EC)pathway.The rate-determining step(RDS)of HPRR is either the cleavage of the HO-OH bond(chemical)or the reduction of HO(electrochemical),depending on their respective activation energies.These activation energies are functions of the HO*binding free energy,Δ_(GHO*),establishingΔ_(GHO*)as the descriptor for HPRR activity prediction.Pt(111)and Pt(100)are identified as the most active HPRR catalysts among the studied metal surfaces,although they still experience a significant overpotential.The scaling relationship betweenΔ_(GHOO*)andΔ_(GHO*)reveals a thermodynamic coupling of HPOR and HPRR,explaining their occurrence on Pt surfaces.These findings provide important insights and activity descriptors for both HPOR and HPRR,providing valuable guidance for the design of electrocatalysts in H_(2)O_(2)-related energy applications and fuel cells.展开更多
We used hydrodynamic simulations and shock wave propagation theories to analyze the behavior of shock waves within Ti/Pt periodically modulated graded structures and their integration layers.The effects of the total n...We used hydrodynamic simulations and shock wave propagation theories to analyze the behavior of shock waves within Ti/Pt periodically modulated graded structures and their integration layers.The effects of the total number of periodic layers,the total thickness of graded materials and loading velocity on the integration layer thickness and behavior of pressure-strain rate were systematically investigated.The results reveal that,by adjusting the total number of periodically modulated layers,the total thickness of graded materials and loading velocity the pressure amplitudes of the reflected compressive and rarefaction waves at different interfaces of Ti/Pt periodically modulated graded materials can be precisely controlled.Furthermore,empirical structural design criteria for Ti/Pt periodically modulated graded materials are established.The thickness ratio variation between adjacent Ti/Pt layers in the periodic structure must exceed 0.32.After the collaborative design of the integration layer,Ti/Pt periodically modulated graded materials can achieve a controllable loading function with pressures ranging from 1.4 to 144 GPa and strain rates from 3.8×10^(4) to 1.7×10^(7) s^(–1).The outcomes of this research provide a theoretical and simulation basis for the optimized design of periodically modulated graded materials to be utilized in ramp compression experiments.展开更多
We report on the growth of CoFe_(2)O_(4)/Pt heterostructure and their magnetotransport properties.The magnetoresistance under high magnetic fields exhibits a sign change when the temperature increases from 5 K to 10 K...We report on the growth of CoFe_(2)O_(4)/Pt heterostructure and their magnetotransport properties.The magnetoresistance under high magnetic fields exhibits a sign change when the temperature increases from 5 K to 10 K.The anomalous Hall resistance decreases as the temperature increases.Furthermore,angle-dependent magnetoresistance indicates that the observed magnetotransport behaviors originate from the competition between the spin Hall magnetoresistance and magnetic proximity effect.展开更多
基金Supported by the Shanxi Province Grant(202203021212007,2023SHB003).
文摘Hydrogen peroxide(H_(2)O_(2))oxidation and reduction reactions(HPOR/HPRR)are pivotal in various innovative electrochemical energy conversion devices.A comprehensive understanding of these mechanisms is critical for catalyst design and performance improvement in these applications.In this work,we systematically investigate the HPOR/HPRR mechanisms on low-index Pt surfaces,specifically Pt(111),Pt(100)and Pt(110),through density functional theory(DFT)calculations combined with the computational hydrogen electrode(CHE)model.For HPOR,all the low-index Pt surfaces exhibit a unified potential-determining step(PDS)involving the electrochemical oxidation of hydroperoxyl intermediates(HOO*).The binding free energy of HOO*(Δ_(GHOO*))emerges as an activity descriptor,with Pt(110)exhibiting the highest HPOR activity.The HPRR mechanism follows a chem-electrochemical(C-EC)pathway.The rate-determining step(RDS)of HPRR is either the cleavage of the HO-OH bond(chemical)or the reduction of HO(electrochemical),depending on their respective activation energies.These activation energies are functions of the HO*binding free energy,Δ_(GHO*),establishingΔ_(GHO*)as the descriptor for HPRR activity prediction.Pt(111)and Pt(100)are identified as the most active HPRR catalysts among the studied metal surfaces,although they still experience a significant overpotential.The scaling relationship betweenΔ_(GHOO*)andΔ_(GHO*)reveals a thermodynamic coupling of HPOR and HPRR,explaining their occurrence on Pt surfaces.These findings provide important insights and activity descriptors for both HPOR and HPRR,providing valuable guidance for the design of electrocatalysts in H_(2)O_(2)-related energy applications and fuel cells.
基金Funded by the Guangdong Major Project of Basic and Applied Basic Research(No.2021B0301030001)the Foundation of National Key Laboratory of Shock Wave and Detonation Physics(No.JCKYS2022212004)。
文摘We used hydrodynamic simulations and shock wave propagation theories to analyze the behavior of shock waves within Ti/Pt periodically modulated graded structures and their integration layers.The effects of the total number of periodic layers,the total thickness of graded materials and loading velocity on the integration layer thickness and behavior of pressure-strain rate were systematically investigated.The results reveal that,by adjusting the total number of periodically modulated layers,the total thickness of graded materials and loading velocity the pressure amplitudes of the reflected compressive and rarefaction waves at different interfaces of Ti/Pt periodically modulated graded materials can be precisely controlled.Furthermore,empirical structural design criteria for Ti/Pt periodically modulated graded materials are established.The thickness ratio variation between adjacent Ti/Pt layers in the periodic structure must exceed 0.32.After the collaborative design of the integration layer,Ti/Pt periodically modulated graded materials can achieve a controllable loading function with pressures ranging from 1.4 to 144 GPa and strain rates from 3.8×10^(4) to 1.7×10^(7) s^(–1).The outcomes of this research provide a theoretical and simulation basis for the optimized design of periodically modulated graded materials to be utilized in ramp compression experiments.
基金supported by the National Natural Science Foundation of China(Grant Nos.62525406,T2394473,624B2070,and 62274085)the National Key Research and Development Program of China(Grant No.2022YFA1402404)the Innovation Program for Quantum Science and Technology of China(Grant No.2024ZD0301300)。
文摘We report on the growth of CoFe_(2)O_(4)/Pt heterostructure and their magnetotransport properties.The magnetoresistance under high magnetic fields exhibits a sign change when the temperature increases from 5 K to 10 K.The anomalous Hall resistance decreases as the temperature increases.Furthermore,angle-dependent magnetoresistance indicates that the observed magnetotransport behaviors originate from the competition between the spin Hall magnetoresistance and magnetic proximity effect.
