Selective catalytic oxidation of formaldehyde on single V- and Cr-atom decorated magnetic C4N3 substrate: A first principles study

The regulatory function of the d-orbital structure in TM@g-t-C4N3 for bifunctional catalysis of the oxygen evolution/reduction reaction

“…[40][41][42][43][44] Many reports have already shown that the single-ring g-C 4 N 3 (g-s-C 4 N 3 ) is appropriate to provide support for SACs, which can efficiently catalyze many reaction processes, such as the NRR, 45 OER/ORR 46 and oxidation reaction of formaldehyde (HCHO). 47 On the other side, another structure of g-C 4 N 3 with tri-ring units ((g-t-C 4 N 3 ) was reported theoretically in 2013. 41 Furthermore, Sakshi Agarwal et al found that the g-t-C 4 N 3 doped with single TM atoms can catalyze the NRR process with high performance, 48 clarifying that the g-t-C 4 N 3 has broad prospects in catalysis.…”

Unraveling the Activity and Mechanism of TM@g-C4N3 Electrocatalysts in the Oxygen Reduction Reaction

“…The remarkable catalytic performance exhibited by SACs can be attributed to tunable active sites and electronic structure. ,− For instance, the maintenance of isolated TM atoms and incorporated nitrogen atoms contribute to the enhancement of activity. − Nevertheless, the strong electronegativity of nitrogen atoms may result in a strong binding strength with intermediates, which is not favorable for the ORR. − In order to adjust the adsorption strength between active site and intermediates, various strategies have been employed, including adjusting coordination atoms ,, and utilizing different kinds of carbon supports. , For instance, g-C 3 N 4 has a variety of active sites with different coordination environments according to different TM loading sites, thus exhibiting excellent catalytic performance. , Similar to g-C 3 N 4 , the experimentally synthesized g-C 4 N 3 monolayer is also a promising graphitic carbon nitride material . g-C 4 N 3 is a half-metal material with suitable vacancies, as well as abundant nitrogen ligands and electron pairs near the vacancy, which indicates that g-C 4 N 3 may have better conductivity, thus becoming a promising electrocatalyst material. , It has shown excellent catalytic ability in nitrogen reduction reaction and HCHO oxidation reaction. , Advanced DFT techniques, such as computational hydrogen electrode (CHE) model and constant potential model (CPM) DFT schemes, , are commonly used to describe ORR and other electrochemical reaction pathways.…”

“…36,37 reaction. 38,39 Advanced DFT techniques, such as computational hydrogen electrode (CHE) model and constant potential model (CPM) DFT schemes, 40,41 are commonly used to describe ORR and other electrochemical reaction pathways.…”