Efficient modulation of the catalytic performance of electrocatalytic nitrogen reduction with transition metals anchored on N/O-codoped graphene by coordination engineering

Abstract

We for the first time report the discovery of a series of highly efficient electrocatalysts, i.e., transition metal anchored N/O-codoped graphene, for nitrogen fixation via high-throughput screening combined with first-principles...

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

“…Since the concept of single-atom catalysis was firstly proposed by Zhang, Li, Liu et al in 2011 [1], considerable attention has been paid to this area because of its unique homogeneous structural characteristics of a single-atom (SA) active center and the excellent catalytic performance in heterogeneous catalysis [2][3][4][5][6][7][8][9][10]. Several reviews [11][12][13][14][15] have summarized the development of single-atom catalysts (SACs), the structure-function relationship between SACs and their catalytic performance, and the diverse applications of SACs in heterogeneous catalysis [16][17][18][19][20][21][22][23]. 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].…”

A composite approach to synthesize a high-performance Pt/WO3–carbon catalyst for optical and electrocatalytic applications

“…To overcome the challenges of stability and decrease the cost of the Pt catalyst, several efforts have been made for methanol oxidation reactions. Single site catalysts have wide applications in diverse reactions, 1,2 such as the oxygen reduction reaction (ORR), [3][4][5][6] nitrogen reduction reaction (NRR), [7][8][9][10] and CO 2 reduction reaction (CRR), [11][12][13] and the catalysts mostly comprise metallic NPs (Pt, Au, Ag, Ni, Co, etc.) dispersed on a suitable support.…”