The electrochemical nitrogen reduction reaction(NRR)to directly produce NH3 from N_(2) and H_(2)O under ambient conditions has attracted significant attention due to its ecofriendliness.Nevertheless,the electrochemica...The electrochemical nitrogen reduction reaction(NRR)to directly produce NH3 from N_(2) and H_(2)O under ambient conditions has attracted significant attention due to its ecofriendliness.Nevertheless,the electrochemical NRR presents several practical challenges,including sluggish reaction and low selectivity.Here,bi-atom catalysts have been proposed to achieve excellent activity and high selectivity toward the electrochemical NRR by Ma and his co-workers.It could accelerate the kinetics of N_(2)-to-NH_(3) electrochemical conversion and possess better electrochemical NRR selectivity.This work sheds light on the introduction of bi-atom catalysts to enhance the performance of the electrochemical NRR.展开更多
Designing providential catalyst is the key to drive the electrochemical nitrogen reduction reactions(NRR),which is referring to multiple intermediates and products. By means of density functional theory(DFT)calculatio...Designing providential catalyst is the key to drive the electrochemical nitrogen reduction reactions(NRR),which is referring to multiple intermediates and products. By means of density functional theory(DFT)calculations, we studied heteronuclear bi-atom electrocatalyst(HBEC) for NRR. Our results revealed that compared to homonuclear bi-atom electrocatalyst(Fe_2@C_2N, V_2@C_2N), Fe, V-co-doped C_2N(Fe V@C_2N)had a smaller limiting potential of-0.17 V and could accelerate N_2-to-NH_3 conversion through the enzymatic pathway of NRR. Importantly, N–N bond length monotonically increases with increasing the Bader charges of adsorbed N_2 molecule but decreases with increasing the Bader charge difference of two adsorbed N atoms. Additionally, the Fe V@C_2N could suppress the production of H_2 by the preferential adsorption and reduction of N_2 molecule. Thus, the as-designed HBEC may have the outstanding electrochemical NRR performance. This work opens a new perspective for NRR by HBECs under mild conditions.展开更多
The proposed method was studied with NiNO3,PdCl2,PdCl2-NiNO3 or PdCl2-Mg(NO3)2 as chemical modifier.The bismuth solution modified by the addition of palladium chloride is found to be better than the other three chemic...The proposed method was studied with NiNO3,PdCl2,PdCl2-NiNO3 or PdCl2-Mg(NO3)2 as chemical modifier.The bismuth solution modified by the addition of palladium chloride is found to be better than the other three chemical modifier.The result shows that temperature is increased by 300℃ after the addition of PdCl2.By XRD and EXD,we also studied the atomization mechanism of Bi with PdCl2 as chemical modifier in this experiment.It is probable that the chemical modifier catalyzes and reduces the atomization of Bi regarding as activated center.展开更多
文摘The electrochemical nitrogen reduction reaction(NRR)to directly produce NH3 from N_(2) and H_(2)O under ambient conditions has attracted significant attention due to its ecofriendliness.Nevertheless,the electrochemical NRR presents several practical challenges,including sluggish reaction and low selectivity.Here,bi-atom catalysts have been proposed to achieve excellent activity and high selectivity toward the electrochemical NRR by Ma and his co-workers.It could accelerate the kinetics of N_(2)-to-NH_(3) electrochemical conversion and possess better electrochemical NRR selectivity.This work sheds light on the introduction of bi-atom catalysts to enhance the performance of the electrochemical NRR.
基金supported by the National Natural Science Foundation of China (Grant no. 51302079)the National Natural Science Foundation of Hunan Province (Grant no. 2017JJ1008)。
文摘Designing providential catalyst is the key to drive the electrochemical nitrogen reduction reactions(NRR),which is referring to multiple intermediates and products. By means of density functional theory(DFT)calculations, we studied heteronuclear bi-atom electrocatalyst(HBEC) for NRR. Our results revealed that compared to homonuclear bi-atom electrocatalyst(Fe_2@C_2N, V_2@C_2N), Fe, V-co-doped C_2N(Fe V@C_2N)had a smaller limiting potential of-0.17 V and could accelerate N_2-to-NH_3 conversion through the enzymatic pathway of NRR. Importantly, N–N bond length monotonically increases with increasing the Bader charges of adsorbed N_2 molecule but decreases with increasing the Bader charge difference of two adsorbed N atoms. Additionally, the Fe V@C_2N could suppress the production of H_2 by the preferential adsorption and reduction of N_2 molecule. Thus, the as-designed HBEC may have the outstanding electrochemical NRR performance. This work opens a new perspective for NRR by HBECs under mild conditions.
文摘The proposed method was studied with NiNO3,PdCl2,PdCl2-NiNO3 or PdCl2-Mg(NO3)2 as chemical modifier.The bismuth solution modified by the addition of palladium chloride is found to be better than the other three chemical modifier.The result shows that temperature is increased by 300℃ after the addition of PdCl2.By XRD and EXD,we also studied the atomization mechanism of Bi with PdCl2 as chemical modifier in this experiment.It is probable that the chemical modifier catalyzes and reduces the atomization of Bi regarding as activated center.
