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
For the first time the low-lying J = 1/2 pentaquark states are investigated in the pseudoscalar-vector Skyrme model. Once the conventional baryon properties are fit, other states are predicted without any more adjusta...For the first time the low-lying J = 1/2 pentaquark states are investigated in the pseudoscalar-vector Skyrme model. Once the conventional baryon properties are fit, other states are predicted without any more adjustable parameters. Furthermore, both symmetry-breaking and decay operators are treated in full. In particular, we focus on the calculations of mass and decay width, and compare them with the experimental data available and relevant theoretical results obtained in other pictures. We recognize that the higher-order contributions, such as the 35 and/or 35 representation admixtures, are not negligible. Our analysis provides some valuable clues to the physical mechanisms, and the oncoming experimental search and/or confirmation could provide a sharp test of our proposal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The project partially supported by National Natural Science Foundation of China under Grant Nos. 10375039 and 90503008, the Doctoral Program Funds of the Ministry of Education, and the Research Fund of the Nuclear Theory Center of Heavy Ion Research Facility at Lanzhou of China.Acknowledgments We are grateful to Prof. H. Weigel for his useful program from E-mail exchanges.
文摘For the first time the low-lying J = 1/2 pentaquark states are investigated in the pseudoscalar-vector Skyrme model. Once the conventional baryon properties are fit, other states are predicted without any more adjustable parameters. Furthermore, both symmetry-breaking and decay operators are treated in full. In particular, we focus on the calculations of mass and decay width, and compare them with the experimental data available and relevant theoretical results obtained in other pictures. We recognize that the higher-order contributions, such as the 35 and/or 35 representation admixtures, are not negligible. Our analysis provides some valuable clues to the physical mechanisms, and the oncoming experimental search and/or confirmation could provide a sharp test of our proposal
