Atom-level modulation of the coordination environment for single-atom catalysts(SACs)is considered as an effective strategy for elevating the catalytic performance.For the MNxsite,breaking the symmetrical geometry and...Atom-level modulation of the coordination environment for single-atom catalysts(SACs)is considered as an effective strategy for elevating the catalytic performance.For the MNxsite,breaking the symmetrical geometry and charge distribution by introducing relatively weak electronegative atoms into the first/second shell is an efficient way,but it remains challenging for elucidating the underlying mechanism of interaction.Herein,a practical strategy was reported to rationally design single cobalt atoms coordinated with both phosphorus and nitrogen atoms in a hierarchically porous carbon derived from metal-organic frameworks.X-ray absorption spectrum reveals that atomically dispersed Co sites are coordinated with four N atoms in the first shell and varying numbers of P atoms in the second shell(denoted as Co-N/P-C).The prepared catalyst exhibits excellent oxygen reduction reaction(ORR)activity as well as zinc-air battery performance.The introduction of P atoms in the Co-SACs weakens the interaction between Co and N,significantly promoting the adsorption process of ^(*)OOH,resulting in the acceleration of reaction kinetics and reduction of thermodynamic barrier,responsible for the increased intrinsic activity.Our discovery provides insights into an ultimate design of single-atom catalysts with adjustable electrocatalytic activities for efficient electrochemical energy conversion.展开更多
In an integrated energy system(IES) composed of multiple subsystems, energy coupling causes an energy supply blockage or shutdown in one subsystem, thereby affecting the energy flow distribution optimization of other ...In an integrated energy system(IES) composed of multiple subsystems, energy coupling causes an energy supply blockage or shutdown in one subsystem, thereby affecting the energy flow distribution optimization of other subsystems.The energy supply should be globally optimized during the IES energy supply restoration process to produce the highest restoration net income. Mobile emergency sources can be quickly and flexibly connected to supply energy after an energy outage to ensure a reliable supply to the system, which adds complexity to the decision. This study focuses on a powergas IES with mobile emergency sources and analyzes the coupling relationship between the gas distribution system and the power distribution system in terms of sources, networks, and loads, and the influence of mobile emergency source transportation. The influence of the transient process caused by the restoration operation of the gas distribution system on the power distribution system is also discussed. An optimization model for power-gas IES restoration was established with the objective of maximizing the net income. The coordinated restoration optimization decision-making process was also built to realize the decoupling iteration of the power-gas IES, including system status recognition, mobile emergency source dispatching optimization, gas-to-power gas flow optimization, and parallel intra-partition restoration scheme optimization for both the power and gas distribution systems. A simulation test power-gas IES consisting of an 81-node medium-voltage power distribution network, an 89-node medium-pressure gas distribution network, and four mobile emergency sources was constructed. The simulation analysis verified the efficiency of the proposed coordinated restoration optimization method.展开更多
基金supported by the National Natural Science Foundation of China(51872115,12234018 and 52101256)Beijing Synchrotron Radiation Facility(BSRF,4B9A)。
文摘Atom-level modulation of the coordination environment for single-atom catalysts(SACs)is considered as an effective strategy for elevating the catalytic performance.For the MNxsite,breaking the symmetrical geometry and charge distribution by introducing relatively weak electronegative atoms into the first/second shell is an efficient way,but it remains challenging for elucidating the underlying mechanism of interaction.Herein,a practical strategy was reported to rationally design single cobalt atoms coordinated with both phosphorus and nitrogen atoms in a hierarchically porous carbon derived from metal-organic frameworks.X-ray absorption spectrum reveals that atomically dispersed Co sites are coordinated with four N atoms in the first shell and varying numbers of P atoms in the second shell(denoted as Co-N/P-C).The prepared catalyst exhibits excellent oxygen reduction reaction(ORR)activity as well as zinc-air battery performance.The introduction of P atoms in the Co-SACs weakens the interaction between Co and N,significantly promoting the adsorption process of ^(*)OOH,resulting in the acceleration of reaction kinetics and reduction of thermodynamic barrier,responsible for the increased intrinsic activity.Our discovery provides insights into an ultimate design of single-atom catalysts with adjustable electrocatalytic activities for efficient electrochemical energy conversion.
基金supported by the Open Research Fund of Jiangsu Collaborative Innovation Center for Smart Distribution Network (XTCX202001)National Natural Science Foundation of China (52077061)。
文摘In an integrated energy system(IES) composed of multiple subsystems, energy coupling causes an energy supply blockage or shutdown in one subsystem, thereby affecting the energy flow distribution optimization of other subsystems.The energy supply should be globally optimized during the IES energy supply restoration process to produce the highest restoration net income. Mobile emergency sources can be quickly and flexibly connected to supply energy after an energy outage to ensure a reliable supply to the system, which adds complexity to the decision. This study focuses on a powergas IES with mobile emergency sources and analyzes the coupling relationship between the gas distribution system and the power distribution system in terms of sources, networks, and loads, and the influence of mobile emergency source transportation. The influence of the transient process caused by the restoration operation of the gas distribution system on the power distribution system is also discussed. An optimization model for power-gas IES restoration was established with the objective of maximizing the net income. The coordinated restoration optimization decision-making process was also built to realize the decoupling iteration of the power-gas IES, including system status recognition, mobile emergency source dispatching optimization, gas-to-power gas flow optimization, and parallel intra-partition restoration scheme optimization for both the power and gas distribution systems. A simulation test power-gas IES consisting of an 81-node medium-voltage power distribution network, an 89-node medium-pressure gas distribution network, and four mobile emergency sources was constructed. The simulation analysis verified the efficiency of the proposed coordinated restoration optimization method.
