The rational design of a novel catalytic center with a sound basis remains both challenging and rewarding for the electrochemical reduction of N2(e NRR),which has provided a feasible route for achieving clean and sust...The rational design of a novel catalytic center with a sound basis remains both challenging and rewarding for the electrochemical reduction of N2(e NRR),which has provided a feasible route for achieving clean and sustainable NH3production under ambient conditions.Herein,using density functional theory calculations,we demonstrate that hybrid metal(M)-boron(B)double-atom catalysts(DACs)embedded in gC_(2)N substrate(M-B@C_(2)N,M=3d,4d and 5d transition metals)can achieve both high catalytic activity and high selectivity in e NRR.The proposed M-B@C_(2)N DACs have exhibited impressive feasibility and stability thanks to the resilient and robust C_(2)N substrate with abundant pyridinic N atoms distributed among right-sized pore structures.Our results reveal that like the metal center,the embedded B atom can actively involve in N≡N bond activation viaπ*-backdonation mechanism concomitant with the substantial charge transfer to adsorbed*N2,leading to sizable NAN bond elongation.Accordingly,both adsorption energy and NAN bond length of*N2can be employed as catalytic descriptors for predicting e NRR activity in terms of the limiting potentials(UL).Using high-throughput screening method,we found that six M-B@C_(2)N candidates have stood out as the outstanding electrocatalysts for driving e NRR,namely,M=Ti(UL=0 V),Mo(UL=0 V),Nb(UL=-0.04 V),W(UL=-0.23 V),Zr(UL=-0.26 V),V(UL=-0.28 V).The underlying origin is attributed to the balanced and constrained N-affinity of M-B dual site working in synergy,which can thus be used as one important guide of catalyst design.展开更多
Reducing the aerodynamic drag and noise levels of high-speed pantographs is important for promoting environmentally friendly,energy efficient and rapid advances in train technology.Using computational fluid dynamics t...Reducing the aerodynamic drag and noise levels of high-speed pantographs is important for promoting environmentally friendly,energy efficient and rapid advances in train technology.Using computational fluid dynamics theory and the K-FWH acoustic equation,a numerical simulation is conducted to investigate the aerodynamic characteristics of high-speed pantographs.A component optimization method is proposed as a possible solution to the problemof aerodynamic drag and noise in high-speed pantographs.The results of the study indicate that the panhead,base and insulator are the main contributors to aerodynamic drag and noise in high-speed pantographs.Therefore,a gradual optimization process is implemented to improve the most significant components that cause aerodynamic drag and noise.By optimizing the cross-sectional shape of the strips and insulators,the drag and noise caused by airflow separation and vortex shedding can be reduced.The aerodynamic drag of insulator with circular cross section and strips with rectangular cross section is the largest.Ellipsifying insulators and optimizing the chamfer angle and height of the windward surface of the strips can improve the aerodynamic performance of the pantograph.In addition,the streamlined fairing attached to the base can eliminate the complex flow and shield the radiated noise.In contrast to the original pantograph design,the improved pantograph shows a 21.1%reduction in aerodynamic drag and a 1.65 dBA reduction in aerodynamic noise.展开更多
基金supported by the National Natural Science Foundation of China(21673137)the support from the Program for Top Talents in Songjiang District of Shanghai。
文摘The rational design of a novel catalytic center with a sound basis remains both challenging and rewarding for the electrochemical reduction of N2(e NRR),which has provided a feasible route for achieving clean and sustainable NH3production under ambient conditions.Herein,using density functional theory calculations,we demonstrate that hybrid metal(M)-boron(B)double-atom catalysts(DACs)embedded in gC_(2)N substrate(M-B@C_(2)N,M=3d,4d and 5d transition metals)can achieve both high catalytic activity and high selectivity in e NRR.The proposed M-B@C_(2)N DACs have exhibited impressive feasibility and stability thanks to the resilient and robust C_(2)N substrate with abundant pyridinic N atoms distributed among right-sized pore structures.Our results reveal that like the metal center,the embedded B atom can actively involve in N≡N bond activation viaπ*-backdonation mechanism concomitant with the substantial charge transfer to adsorbed*N2,leading to sizable NAN bond elongation.Accordingly,both adsorption energy and NAN bond length of*N2can be employed as catalytic descriptors for predicting e NRR activity in terms of the limiting potentials(UL).Using high-throughput screening method,we found that six M-B@C_(2)N candidates have stood out as the outstanding electrocatalysts for driving e NRR,namely,M=Ti(UL=0 V),Mo(UL=0 V),Nb(UL=-0.04 V),W(UL=-0.23 V),Zr(UL=-0.26 V),V(UL=-0.28 V).The underlying origin is attributed to the balanced and constrained N-affinity of M-B dual site working in synergy,which can thus be used as one important guide of catalyst design.
基金supported by National Natural Science Foundation of China(12372049)Science and Technology Program of China National Accreditation Service for Confor-mity Assessment(2022CNAS15)+1 种基金Sichuan Science and Technology Program(2023JDRC0062)Independent Project of State Key Laboratory of Rail Transit Vehicle System(2023TPL-T06).
文摘Reducing the aerodynamic drag and noise levels of high-speed pantographs is important for promoting environmentally friendly,energy efficient and rapid advances in train technology.Using computational fluid dynamics theory and the K-FWH acoustic equation,a numerical simulation is conducted to investigate the aerodynamic characteristics of high-speed pantographs.A component optimization method is proposed as a possible solution to the problemof aerodynamic drag and noise in high-speed pantographs.The results of the study indicate that the panhead,base and insulator are the main contributors to aerodynamic drag and noise in high-speed pantographs.Therefore,a gradual optimization process is implemented to improve the most significant components that cause aerodynamic drag and noise.By optimizing the cross-sectional shape of the strips and insulators,the drag and noise caused by airflow separation and vortex shedding can be reduced.The aerodynamic drag of insulator with circular cross section and strips with rectangular cross section is the largest.Ellipsifying insulators and optimizing the chamfer angle and height of the windward surface of the strips can improve the aerodynamic performance of the pantograph.In addition,the streamlined fairing attached to the base can eliminate the complex flow and shield the radiated noise.In contrast to the original pantograph design,the improved pantograph shows a 21.1%reduction in aerodynamic drag and a 1.65 dBA reduction in aerodynamic noise.
