Single-atom catalysts based on two-dimensional metalloporphyrin monolayers for ammonia synthesis under ambient conditions

Dual transition metal atoms embedded in N-doped graphene for electrochemical nitrogen fixation under ambient conditions

“…Aer the N 2 molecule is spontaneously attached to the catalyst's surface, the follow-up nitrogen reduction reaction will experience six proton-electron pair (H + + e À ) transfer processes. On the basis of a comprehensive literature search and from our own experience; [18][19][20][21][22][23][24][25] the rst protonation step (*N 2 + H + + e À / *N 2 H) and the last protonation step (*NH 2 + H + + e À / *NH 3 ) will usually show a large uphill in the free energy and require sufficient energy input, [18][19][20][21][22][23][24][25] thus, the free energy changes of these two steps (DG *N 2 / *N 2 H and DG *NH 2 /*NH 3 ) are usually considered as the potential determining step and can be used as criteria for high throughput screening. On the basis of our experience, we set up the criteria (DG *N 2 /*N 2 H < 0.45 and DG *NH 2 /*NH 3 < 0.45 eV) for the follow-up procedures for screening.…”

“…Single-atom catalysis has attracted considerable attention due to its maximum atomic utilization, high activity and selectivity. [13][14][15][16][17][18][19][20][21][22][23][24][25][26][27][28] Nitrogen-doped graphene is a large class of fascinating substrates to anchor transition metal atoms for electrocatalytic nitrogen reduction reaction with good performance. [29][30][31] Compared with single active site, dual transition metal atoms provide more opportunities for NRR with two active sites and synergistic effects.…”

Multi-level Descriptor Construction for Screening Eligible Single-Atom-Embedded Ternary B3C2P3 Monolayers as Nitrogen Fixation Catalysts

“…Owing to the characteristics of high specific surface area, excellent mechanical properties, and desirable carrier mobility, two-dimensional (2D) materials are generally adopted as the substrates for metal atom anchoring. In previous studies, the MoS 2 monolayer, phosphorene, 2D nitrides or phosphides (BN, BP, and g-C 3 N 4 ), ,, macrocyclic organic-conjugated monolayer, − and graphene as well as its derivatives , have also been widely adopted as potential electrocatalyst supports for NRR. However, to our best knowledge, the low activity and selectivity dilemma still exists in experiments, and designing novel efficient NRR electrocatalysts is an ideal scenario for removing the two stumbling blocks.…”

Porphyrins and Phthalocyanines on Solid-State Mesoporous Matrices as Catalysts in Oxidation Reactions

“…In the MOF a porphyrin molecule is intact and becomes a part of 3D structure, capable of catalytic action [ 33 ]. While SAC often are focused on the processing of the small molecules such as CO 2 reduction [ 30 ], ammonia synthesis [ 34 ] and O 2 reduction [ 35 ], while organic reactions are studied to a lesser extent [ 31 ].…”