Luo Heng, Wang Xiaoxu, Wan Chubin, Xie Lu, Song Minhui, Qian Ping
Department of Physics, University of Science and Technology Beijing, Beijing 100083, China.
Beijing Advanced Innovation Center for Materials Genome Engineering, University of Science and Technology Beijing, Beijing 100083, China.
Nanomaterials (Basel). 2022 Mar 25;12(7):1081. doi: 10.3390/nano12071081.
The possibility of using transition metal (TM)/MXene as a catalyst for the nitrogen reduction reaction (NRR) was studied by density functional theory, in which TM is an Fe atom, and MXene is pure TiCO or TiCO doped with N/F/P/S/Cl. The adsorption energy and Gibbs free energy were calculated to describe the limiting potentials of N activation and reduction, respectively. N activation was spontaneous, and the reduction potential-limiting step may be the hydrogenation of N to *NNH and the desorption of *NH to NH. The charge transfer of the adsorbed Fe atoms to N molecules weakened the interaction of N≡N, which indicates that Fe/MXene is a potential catalytic material for the NRR. In particular, doping with nonmetals F and S reduced the limiting potential of the two potential-limiting steps in the reduction reaction, compared with the undoped pure structure. Thus, Fe/MXenes doped with these nonmetals are the best candidates among these structures.
采用密度泛函理论研究了过渡金属（TM）/MXene作为氮还原反应（NRR）催化剂的可能性，其中TM为Fe原子，MXene为纯TiCO或掺杂N/F/P/S/Cl的TiCO。计算了吸附能和吉布斯自由能，分别描述了N活化和还原的极限电位。N活化是自发的，还原电位限制步骤可能是N加氢生成NNH以及NH脱附生成NH。吸附的Fe原子向N分子的电荷转移削弱了N≡N的相互作用，这表明Fe/MXene是一种潜在的NRR催化材料。特别是，与未掺杂的纯结构相比，掺杂非金属F和S降低了还原反应中两个电位限制步骤的极限电位。因此，掺杂这些非金属的Fe/MXenes是这些结构中最佳的候选材料。
