Fe-doped phosphorene for the nitrogen reduction reaction

Abstract

The nitrogen-to-ammonia conversion is one of the most important and challenging processes in chemistry.

A Biomass‐Derived Carbon‐Based Electrocatalyst for Efficient N2 Fixation to NH3 under Ambient Conditions

“…Electrochemical N 2 reduction is regarded as a sustainable alternative for ambient NH 3 production, but efficient electrocatalysts are needed to meet the challenge to break the strong N≡N triple bond of N 2 . Up till now, great efforts have been made to explore earth‐abundant transition‐metal‐based catalyst materials . Nevertheless, transition metals that bind N 2 too weakly have poor capability for activating N 2 .…”

“…[9][10][11] Up till now,g reat efforts have been made to explore earth-abundantt ransition-metal-based catalyst materials. [12][13][14][15][16][17][18][19][20][21] Nevertheless, transition metals that bind N 2 too weakly have poor capability for activating N 2 . [22,23] Additionally,t he inherentc orrosion and oxidation susceptibility of a wide variety of transition-metal-based materials largely restricts their application in acidic proton-exchange membrane-based electrochemical devices.…”

Transition Metal‐dinitrogen Complex Embedded Graphene for Nitrogen Reduction Reaction

“…The whole catalytic process needs six protons and six electrons, which follows the three possible pathways: distal, alternating and enzyme mechanisms. [2,6,[25][26][27][28][29] The manner of nitrogen molecule absorbed on the catalytic active site is the influence factor of NRR pathway. Both the distal and alternating mechanisms are following the "end-on" pattern of nitrogen molecule absorption, while the enzyme mechanism is along with the "side on" pattern.…”

Atomic Structure Modification for Electrochemical Nitrogen Reduction to Ammonia

“…Meanwhile, Ma and co-workers predicted that the Fe-doped monolayer phosphorene (Fe@P) SMAC could exhibit better catalytic performance than the original matrix using the spin-polarized DFT. [27] In their results, the Fe@P complex exhibited an exotherm when N 2 is absorbed, indicating the sufficient activation of N 2 . Importantly, the doped Fe atom not only reduced the bandgap of the complex to 0.65 eV, quickening the charge-transfer process, but also acted as the catalytic active center for NRR as evidenced by the asymmetric charge and spin-density distribution (Figure 2a).…”

“…In addition, existing challenges and future development directions are proposed to obtain more credible NRR catalysts with high catalytic performance and selectivity. and high pressure (15)(16)(17)(18)(19)(20)(21)(22)(23)(24)(25)(26)(27)(28)(29)(30), [1,2] which consumes more than 1% of the energy generated in the world each year. [3] This is due to the high bond energy of NN bond (941 kJ mol −1 ), especially the first step cleavage that requires thermodynamically strong energy barrier of 410 kJ mol −1 .…”