Activation and Conversion of Molecular Nitrogen to the Precursor of Ammonia on Silicon Substituted Cyclo[18]Carbon: a DFT Design

Abstract

Recent synthesis of sp-hybridized cyclo [18]carbon allotrope has attracted immense curiosity. Since then, a generous amount of theoretical studies concerning aromaticity, adsorption, and spectra of the molecule have been performed. However, very few stuides have been carried out concerning its reactivities and catalytic behaviour. In this article, a DFT-based inquisition has been reported regarding the reactivity of Si substituted cyclo [18]carbon molecule towards molecular N 2 . Results show that the Si substituted derivative is effective in producing adducts with molecular nitrogen. Charge calculations and IRC trapping methods indicate that only the Si center of C 17 Si and its (HOMO-1) level participate in N 2 addition. The N-adduct so formed, is then found to spontaneously react with molecular H 2 . The addition of two H 2 molecules to the activated nitrogen molecule to give respective amine derivatives have also been studied. The successful generation of the precursor of NH 3 by C 17 Si lays a clear emphasis on its potentiality.

Mechanistic Inquisition on the Reduction of C17Si(NH2)2 to NH3: A DFT Study

“…The C 17 Si-N 2 adduct, so formed, was also seen to bear a strong affinity towards H 2 molecules and reacted with them, producing two amine derivatives. [62] However, the complete catalytic cycle of the formation of NH 3 and the regeneration of the catalyst, i. e., C 17 Si, were the two most important outcomes that were unanswered in the previous findings. Therefore, in this work, we attempted to address the same, starting from the C 17 Si-(NH 2 ) 2 adduct.…”

Probing the structural, electronic and optical properties of pure and B, N, or Li substituted Cyclo-18 ring: density functional theory investigations

“…To check the reliability of our method, we have calculated C-C, C≡C, C-B, C-N, and C-Li bond length for D 9h polyynic C-18 ring. We have compared our data with the existing reported values [23][24][25]…”

“…To understand the ground state properties of Cyclo-18, several theoretical simulations have been reported using MP2 [23][24][25][26][27], HF [28,29], SCF [25], DFT [30][31][32][33], and Quantum Monte carlo [34] techniques. In this direction, researchers have produced reliable DFT results for linear and non-linear small carbon C n molecules [12][13][14] with ring and chain structures.…”

Host–guest cooperative bridged bicyclopolyynic (BBP) open-molecular cages with optical-switching properties

“…[49][50][51][52][53][54] Appraisal on sensing and catalytic properties of C n rings has also received the utmost research attention. [55][56][57][58][59][60][61] Likewise, understanding the interaction behaviour of metal atoms with C n rings is the heart of several studies. [62][63][64][65][66][67] Research has also been conducted to scrutinize these molecular rings for applications in electronics, optoelectronics, and other functional device engineering.…”