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

Abstract

The development of low−cost and high−efficiency single atom catalysts (SACs) is essential for catalyzing nitrogen reduction reactions (NRR) under ambient conditions. Current SACs suffer from low selectivity and poor activity,...

Construction of a BC3-based TM single-atom catalyst for efficient reduction of CO2 to CH4: a computational study

“…In our previous work, a structural descriptor φ was proposed as a symbol of catalyst performance for various inherent properties, including the active center. 34 The descriptor φ is defined as follows: φ = θ d × ( χ TM + 2 × χ C + χ B )/ χ O , where χ TM , χ C , χ B and χ O represent the electronegativity of the TM, C, B, and O elements, respectively, and θ d denotes the d-electron number of the TM atom. The calculated φ -values and the corresponding catalytic performances are depicted as points in Fig.…”

“…Previous studies have reported that carbon vacancies are more likely to form on a BC 3 monolayer than boron vacancies. 33,34 Thus, for CO 2 RR, 12 TM atoms are doped into carbon vacancies to create SACs denoted as TM@BC 3 , as shown in Fig. 1(a).…”

“…[30][31][32] Rh-and Re-doped BC 3 monolayers have been shown to be efficient catalysts for the ORR, OER, and NRR, respectively. 33,34 In this work, the CO 2 RR catalytic properties and dominant products of 12 transition metal (TM) atoms (V, Mn, Fe, Co, Ni, Cu, Mo, Ru, Rh, Pd, Ag, and Pt) doped on BC 3 are systematically investigated using density functional theory (DFT) calculations. We find that Pt@BC 3 is the most efficient CO 2 RR catalyst with high selectivity for CH 4 at a limiting potential of À0.36 V. We also identify a volcanic relationship between the DG *OCHO , as well as the descriptor j, and the limiting potential, which provides guidance for tuning the active site to improve catalytic performance.…”

Curvature effects on the bifunctional oxygen catalytic performance of single atom metal–N–C

“…Non-noble metal single-atom catalysts (SACs) with their metal-nitrogen-carbon coordination, namely, the so-called MN 4 structure have attracted the attention of many researchers in recent years, due to their full metal utilization, superior catalytic activity, and affordable price. [8][9][10][11][12] A similar local coordination environment in such MN 4 catalysts makes it easier to identify the active sites for accurate and insightful theoretical predictions. 13 On the other hand, a similar coordination environment also underlies the intrinsic electronic structure of the active sites-this makes it difficult to break the linear relationship between the catalytic activity and the adsorption energies of reaction intermediates in multi-step reactions, thus further hindering the possibility of improving their activities.…”

Interlayer electronic coupling regulates the performance of FeN MXenes and Fe2B2 MBenes as high-performance Li- and Al-ion batteries

“…[10][11][12][13] Many 2D materials show excellent performance as anode materials, for example nonmetallic element-based materials, like carbon, [14][15][16] boron, [17][18][19][20] phosphorus, 21,22 and binary compounds formed by the main group elements. 23,24 The stabilities and electronic conductivities of these compounds are improved by the addition of special metal ions. 25,26 Early transition metal carbides and carbonitrides (called MXenes) and orthorhombic transition metal borides (MBenes) have remarkable applications in electrode materials.…”