Boosting Electroreduction Kinetics of Nitrogen to Ammonia via Tuning Electron Distribution of Single‐Atomic Iron Sites

Abstract

Electrocatalytic nitrogen reduction reaction (NRR) playsavital role for next-generation electrochemical energy conversion technologies.H owever,t he NRR kinetics is still limited by the sluggish hydrogenation process on noble-metalfree electrocatalyst. Herein, we report the rational design and synthesis of ah ybrid catalyst with atomic iron sites anchored on aN ,O-doped porous carbon (Fe SA-NO-C) matrix of an inverse opal structure,leading to aremarkably high NH 3 yield rate of 31.9 mg NH 3 h À1 mg À1 cat. and Faradaic efficiency of 11.8 % at À0.4 Vf or NRR electrocatalysis,o utperformed almost all previously reported atomically dispersed metal-nitrogen-carbon catalysts.T heoretical calculations revealed that the observed high NRR catalytic activity for the Fe SA-NO-C catalyst stemmed mainly from the optimizedc harge-transfer between the adjacent Oa nd Fe atoms homogenously distributed on the porous carbon support, which could not only significantly facilitate the transportation of N 2 and ions but also effectively decrease the binding energy between the isolated Fe atom and *N 2 intermediate and the thermodynamic Gibbsfree energy of the rate-determining step (*N 2 ! *NNH).

High Capacity and Fast Kinetics of Potassium-Ion Batteries Boosted by Nitrogen-Doped Mesoporous Carbon Spheres

“…For the purpose of obtaining better electrochemical performances, it is necessary to further modify hard carbon materials. It is a proved fact that porosity structure is beneficial to enhance the contact between electrolyte and anode material, providing more active sites, shortening K-ion diffusion distance and accommodating volumetric expansion [14,[20][21][22][23]. In addition, heteroatom doping, especially N doping, has been applied to increase active sites of carbon materials, so as to promote K-ion adsorption and increase their electronic conductivity [24][25][26][27][28][29][30].…”

P‐Block Atomically Dispersed Antimony Catalyst for Highly Efficient Oxygen Reduction Reaction

“…The charge density of Sb SAC is shown in Figure 1 a, the visible charge transfers from Sb to N atoms, resulting in the decreased electron density of Sb atom. The positively charged Sb atoms are conducive to adsorb O 2 and reaction intermediates, may act as active centers and facilitate electron transfer [8b, 10] . As shown in Figure 1 b, the O 2 adsorption energy of Sb NPs is only −0.067 eV, which is much lower than that of Sb SAC (−0.571 eV), indicating a weaker interaction with O 2 on Sb NPs than Sb SAC.…”

Progress in Mo/W-based electrocatalysts for nitrogen reduction to ammonia under ambient conditions

“…After releasing one NH 3 molecule, the process continues to hydrogenate the left N atom (close to the surface of the catalyst) to produce the second NH 3 . 40 While in Fig. 1(c), the generated H atoms alternately are adsorbed on these two N atoms, and then two NH 3 molecules are released.…”