Unveiling the underlying mechanism of nitrogen fixation by a new class of electrocatalysts two-dimensional TM@g-C4N3 monosheets

In silico design of single transition metal atom anchored defective boron carbide monolayers as high-performance electrocatalysts for the nitrogen reduction reaction

“…As shown in Table 2, systems Ta@V B and W@V B have Δ G max NRR larger than 0.55 eV and are not suitable for the NRR, while the others exhibit efficient catalytic activity. Re@V B shows the highest catalytic performance, with a low Δ G max NRR of 0.28 eV, which is comparable (or lower) to those of other recently reported efficient NRR catalysts, such as experimentally a certain percentage of B-doped graphene (0.50 eV), 51 V-doped g-C 4 N 3 (0.37 eV), 52 carbon-bound boron nitride nanoribbon edges (0.39 eV) 53 and Mo atom-bound defective boron nitride (0.35 eV). 30…”

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.…”

Theoretical studies of MXene-supported single-atom catalysts: Os1/Ti2CS2 for low-temperature CO oxidation

“…Over the past decade, SAC has expanded rapidly and the concept of SAC has been further developed into dynamic SACs [24] and single-cluster catalysts (SCCs) [25,26]. Many studies [27][28][29][30][31][32][33][34][35][36] have been devoted to obtaining SACs with high stability, high selectivity and high reactivity [37][38][39] for thermocatalysis, photocatalysis, electrocatalysis, and photoelectrocatalysis reactions [15,[40][41][42][43], such as CO oxidation, water gas shift reaction, activation of C-H bonds, photo-and electro-catalytic water splitting, and CO 2 reduction reaction, oxygen reduction reaction, hydrogen evolution reaction, oxygen evolution reaction, hydrogenation reactions, and nitrogen reduction reaction [5,15,[43][44][45][46][47][48][49][50][51][52][53][54].…”