Inspired by MXene nanosheets and their regulation of surface functional groups,a series of Ti_(2)C‐based single‐atom electrocatalysts(TM@Ti_(2)CT_(x),TM=V,Cr,Mn,Fe,Co,and Ni)with two dif‐ferent functional groups(T=...Inspired by MXene nanosheets and their regulation of surface functional groups,a series of Ti_(2)C‐based single‐atom electrocatalysts(TM@Ti_(2)CT_(x),TM=V,Cr,Mn,Fe,Co,and Ni)with two dif‐ferent functional groups(T=–O and–S)was designed.The CO_(2)RR catalytic performance was stud‐ied using well‐defined ab initio calculations.Our results show that the CO_(2) molecule can be more readily activated on TM@Ti_(2)CO_(2) than the TM@Ti_(2)CS_(2) surface.Bader charge analysis reveals that the Ti_(2)CO_(2) substrate is involved in the adsorption reaction,and enough electrons are injected into the 2π*u orbital of CO_(2),leading to a V‐shaped CO_(2) molecular configuration and partial negative charge distribution.The V‐shaped CO_(2) further reduces the difficulty of the first hydrogenation reac‐tion step.The calculatedΔG of the first hydrogenation reaction on TM@Ti_(2)CO_(2) was significantly lower than that of the TM@Ti_(2)CS_(2) counterpart.However,the subsequent CO_(2) reduction pathways show that the UL of the potential determining step on TM@Ti_(2)CS_(2) is smaller than that of TM@Ti_(2)CO_(2).Combining the advantages of both TM@Ti_(2)CS_(2) and TM@Ti_(2)CO_(2),we designed a mixed functional group surface with–O and–S to anchor TM atoms.The results show that Cr atoms an‐chored on the surface of mixed functional groups exhibit high catalytic activity for the selective production of CH4.This study opens an exciting new avenue for the rational design of highly selec‐tive MXene‐based single‐atom CO_(2)RR electrocatalysts.展开更多
A novel hybrid self-reconfigurable modular robot is designed to finish the morphing action from line shape to hexagon shape. The robot is composed of many basic modules,each of which consists of a master module and a ...A novel hybrid self-reconfigurable modular robot is designed to finish the morphing action from line shape to hexagon shape. The robot is composed of many basic modules,each of which consists of a master module and a slave module in the shape of triangular prism. There are four connection ports on each basic module. For the master module there are two holes on each connection port,and for the slave one there are two pegs on each connection. The docking process between two neighboring basic modules is analyzed with a peg-in-hole mechanical structure. A small motion's method is presented and the contact forces are derived. According to the force/moment,the pose of a motion module should be adjusted to make two neighboring modules align and finish the docking process.Finally,a simulation of 3 basic modules is shown to finish the morphing and docking process effectively. The system can finish the morphing task from the line shape to the hexagon shape.展开更多
文摘Inspired by MXene nanosheets and their regulation of surface functional groups,a series of Ti_(2)C‐based single‐atom electrocatalysts(TM@Ti_(2)CT_(x),TM=V,Cr,Mn,Fe,Co,and Ni)with two dif‐ferent functional groups(T=–O and–S)was designed.The CO_(2)RR catalytic performance was stud‐ied using well‐defined ab initio calculations.Our results show that the CO_(2) molecule can be more readily activated on TM@Ti_(2)CO_(2) than the TM@Ti_(2)CS_(2) surface.Bader charge analysis reveals that the Ti_(2)CO_(2) substrate is involved in the adsorption reaction,and enough electrons are injected into the 2π*u orbital of CO_(2),leading to a V‐shaped CO_(2) molecular configuration and partial negative charge distribution.The V‐shaped CO_(2) further reduces the difficulty of the first hydrogenation reac‐tion step.The calculatedΔG of the first hydrogenation reaction on TM@Ti_(2)CO_(2) was significantly lower than that of the TM@Ti_(2)CS_(2) counterpart.However,the subsequent CO_(2) reduction pathways show that the UL of the potential determining step on TM@Ti_(2)CS_(2) is smaller than that of TM@Ti_(2)CO_(2).Combining the advantages of both TM@Ti_(2)CS_(2) and TM@Ti_(2)CO_(2),we designed a mixed functional group surface with–O and–S to anchor TM atoms.The results show that Cr atoms an‐chored on the surface of mixed functional groups exhibit high catalytic activity for the selective production of CH4.This study opens an exciting new avenue for the rational design of highly selec‐tive MXene‐based single‐atom CO_(2)RR electrocatalysts.
基金Supported by the National Natural Science Foundation of China(No.61175069,51075272,51475300)
文摘A novel hybrid self-reconfigurable modular robot is designed to finish the morphing action from line shape to hexagon shape. The robot is composed of many basic modules,each of which consists of a master module and a slave module in the shape of triangular prism. There are four connection ports on each basic module. For the master module there are two holes on each connection port,and for the slave one there are two pegs on each connection. The docking process between two neighboring basic modules is analyzed with a peg-in-hole mechanical structure. A small motion's method is presented and the contact forces are derived. According to the force/moment,the pose of a motion module should be adjusted to make two neighboring modules align and finish the docking process.Finally,a simulation of 3 basic modules is shown to finish the morphing and docking process effectively. The system can finish the morphing task from the line shape to the hexagon shape.
