Molecular N2 Research Articles

First-principles molecular dynamics of exciton-driven initial stage of plasma phase transition in warm dense molecular nitrogen.

Understanding the properties of molecular nitrogen N2 at extreme conditions is the fundamental problem for atomistic theory and the important benchmark for the capabilities of first-principles molecular dynamics (FPMD) methods. In this work, we focus on the connection between the dynamics of ions and electronic excitations in warm dense N2. The restricted open-shell Kohn-Sham method gives us the possibility to reach relevant time and length scales for FPMD modeling of an isolated exciton dynamics in warm dense N2. Wannier localization sheds light on the corresponding mechanisms of covalent bond network rearrangements that stand behind polymerization kinetics. FPMD results suggest a concept of energy transfer from the thermal energy of ions into the internal energy of polymeric structures that form in warm dense N2 at extreme conditions. Our findings agree with the thermobaric conditions for the onset of absorption in the optical spectroscopy study of Jiang et al. [Nat. Commun. 9, 2624 (2018)].

SMILES-based QSAR virtual screening to identify potential therapeutics for COVID-19 by targeting 3CLpro and RdRp viral proteins

The COVID-19 pandemic has prompted the medical systems of many countries to develop effective treatments to combat the high rate of infection and death caused by the disease. Within the array of proteins found in SARS-CoV-2, the 3 chymotrypsin-like protease (3CLpro) holds significance as it plays a crucial role in cleaving polyprotein peptides into distinct functional nonstructural proteins. Meanwhile, RNA-dependent RNA polymerase (RdRp) takes center stage as the key enzyme tasked with replicating the viral genomic RNA within host cells. These proteins, 3CLpro and RdRp, are deemed optimal subjects for QSAR modeling due to their pivotal functions in the viral lifecycle. In this study, SMILES-based QSAR classification models were developed for a dataset of 2377 compounds that were defined as either active or inactive against 3CLpro and RdRp. Pharmacophore (PH4) and QSAR modeling were used for the virtual screening on 60.2 million compounds including ZINC, ChEMBL, Molport, and MCULE databases to identify new potent inhibitors against 3CLpro and RdRp. Then, a filter was established based on typical molecular characteristics to identify drug-like molecules. The molecular docking was also performed to evaluate the binding affinity of 156 AND 51 potential inhibitors to 3CLpro and RdRp, respectively. Among the 15 hits identified based on molecular docking scores, M3, N2, and N4 were identified as promising inhibitors due to their good synthetic accessibility scores (3.07, 3.11, and 3.29 out of 10 for M3, N2, and N4 respectively). These compounds contain amine functional groups, which are known for their crucial role in the binding interactions between drugs and their targets. Consequently, these hits have been chosen for further biological assay studies to validate their activity. They may represent novel 3CLpro and RdRp inhibitors possessing drug-like properties suitable for COVID-19 therapy.

Combining PSMA-PET and PROMISE to re-define disease stage and risk in patients with prostate cancer: a multicentre retrospective study

Prostate-specific membrane antigen (PSMA)-PET was introduced into clinical practice in 2012 and has since transformed the staging of prostate cancer. Prostate Cancer Molecular Imaging Standardized Evaluation (PROMISE) criteria were proposed to standardise PSMA-PET reporting. We aimed to compare the prognostic value of PSMA-PET by PROMISE (PPP) stage with established clinical nomograms in a large prostate cancer dataset with follow-up data for overall survival. In this multicentre retrospective study, we used data from patients of any age with histologically proven prostate cancer who underwent PSMA-PET at the University Hospitals in Essen, Münster, Freiburg, and Dresden, Germany, between Oct 30, 2014, and Dec 27, 2021. We linked a subset of patient hospital records with patient data, including mortality data, from the Cancer Registry North-Rhine Westphalia, Germany. Patients from Essen University Hospital were randomly assigned to the development or internal validation cohorts (2:1). Patients from Münster, Freiburg, and Dresden University Hospitals were included in an external validation cohort. Using the development cohort, we created quantitative and visual PPP nomograms based on Cox regression models, assessing potential PPP predictors for overall survival, with least absolute shrinkage and selection operator penalty for overall survival as the primary endpoint. Performance was measured using Harrell's C-index in the internal and external validation cohorts and compared with established clinical risk scores (International Staging Collaboration for Cancer of the Prostate [STARCAP], European Association of Urology [EAU], and National Comprehensive Cancer Network [NCCN] risk scores) and a previous nomogram defined by Gafita et al (hereafter referred to as GAFITA) using receiver operating characteristic (ROC) curves and area under the ROC curve (AUC) estimates. We analysed 2414 male patients (1110 included in the development cohort, 502 in the internal cohort, and 802 in the external validation cohort), among whom 901 (37%) had died as of data cutoff (June 30, 2023; median follow-up of 52·9 months [IQR 33·9-79·0]). Predictors in the quantitative PPP nomogram were locoregional lymph node metastases (molecular imaging N2), distant metastases (extrapelvic nodal metastases, bone metastases [disseminated or diffuse marrow involvement], and organ metastases), tumour volume (in L), and tumour mean standardised uptake value. Predictors in the visual PPP nomogram were distant metastases (extrapelvic nodal metastases, bone metastases [disseminated or diffuse marrow involvement], and organ metastases) and total tumour lesion count. In the internal and external validation cohorts, C-indices were 0·80 (95% CI 0·77-0·84) and 0·77 (0·75-0·78) for the quantitative nomogram, respectively, and 0·78 (0·75-0·82) and 0·77 (0·75-0·78) for the visual nomogram, respectively. In the combined development and internal validation cohort, the quantitative PPP nomogram was superior to STARCAP risk score for patients at initial staging (n=139 with available staging data; AUC 0·73 vs 0·54; p=0·018), EAU risk score at biochemical recurrence (n=412; 0·69 vs 0·52; p<0·0001), and NCCN pan-stage risk score (n=1534; 0·81 vs 0·74; p<0·0001) for the prediction of overall survival, but was similar to GAFITA nomogram for metastatic hormone-sensitive prostate cancer (mHSPC; n=122; 0·76 vs 0·72; p=0·49) and metastatic castration-resistant prostate cancer (mCRPC; n=270; 0·67 vs 0·75; p=0·20). The visual PPP nomogram was superior to EAU at biochemical recurrence (n=414; 0·64 vs 0·52; p=0·0004) and NCCN across all stages (n=1544; 0·79 vs 0·73; p<0·0001), but similar to STARCAP for initial staging (n=140; 0·56 vs 0·53; p=0·74) and GAFITA for mHSPC (n=122; 0·74 vs 0·72; p=0·66) and mCRPC (n=270; 0·71 vs 0·75; p=0·23). Our PPP nomograms accurately stratify high-risk and low-risk groups for overall survival in early and late stages of prostate cancer and yield equal or superior prediction accuracy compared with established clinical risk tools. Validation and improvement of the nomograms with long-term follow-up is ongoing (NCT06320223). Cancer Registry North-Rhine Westphalia.

Genesis of Polynitrogen Compounds Employing Silicon Substituted cyclo[18]carbon: A DFT Investigation.

Activation of molecular N2 and its catalytic ability to form NH3 using C17Si has been already reported. This current study reports the formation of exclusive polynitrogen clusters (N4 and N5) on the C17Si ring. The clusters are generated using N2 and N3 respectively. Physical and chemical property analyses of the clusters show that the N5 cluster exhibits greater stability than N4. The former is seen to experience reduced molecular strain compared to the latter owing to its co-planar geometry. The thermodynamic calculations of the systems further show that the formation of the N5 cluster is spontaneous compared to N4 on the C17Si ring.

Enhanced Activity and Selectivity for Nitrogen Reduction Reaction in Electrode-based Heterostructures: A DFT Computational Study.

Developing sustainable and efficient catalysts for ammonia synthesis from atmospheric molecular N2 under ambient conditions presents a significant 21st-century challenge. Two-dimensional heterostructures, particularly single-atom catalysts (SACs) supported on two-dimensional materials, have emerged as a promising avenue due to their remarkable catalytic activity and selectivity. Electrides, characterized by an abundance of free electrons and high surface activity, have attracted substantial attention in this context. Through density functional theory (DFT) calculations, this study proposes electride-graphene heterostructures (EGHS) as catalysts to effectively regulate charge distribution at the catalytic center, facilitating the optimization of catalytic performance. The EGHS model addresses challenges related to excessive adsorbate binding, mitigating electron transfer compared to electride monolayer adsorption. This novel approach utilizes heterogeneous heterostructures to finely tune the catalytic site, optimizing electron input for enhanced catalysis.Based on the optimized charge transfer for N2 activation, the Cr-doped EGHS (Cr@EGHS) exhibits a promising performance in the nitrogen reduction reaction, leading to, a relatively low limiting potential of -0.85 V and high selectivity. The hypothesis charge transfer depend on N2 activation is further supported by modulating the distance between component layers of heterostructure. These findings contribute to design principles for 2D heterostructure catalysts and offer a reference for experimental synthesis.

Two-dimensional nonlinear spectroscopy in the extreme ultraviolet to study dynamics of atomic and molecular gases

We present a two-dimensional (2D) nonlinear four-wave mixing scheme in the extreme ultraviolet (XUV) to investigate ultrafast electronic wave-packets dynamics of multi-electron states in the above-threshold ionization region, using atomic argon and molecular nitrogen as examples. Coherent light sources in the range between 24 and 45 eV is generated by phase-matched cascaded four-wave mixing processes with a collinear configuration of laser fields 800 nm and 1400 nm. Motion of the electrons involving the excited states 3s3p6np (1P10) of argon gas, theF2Σg+ state and the predissociation state C2Σu+ of molecular nitrogen ion N2+ are unravelled through the ‘on-axis’ and ‘off-axis’ features of the two-dimensional spectra. Interpretation of the experimental data is supported by a theoretical dipole control model. Hence, results of this study may be promising for studies of dynamics of electrons in more complex systems.

Comparative study on the molecular evolution of changqing petroleum coke during air and pure oxygen combustion: A ReaxFF method analysis

Based on reactive force field (ReaxFF) simulation, the molecular evolution mechanism of air combustion simulation and pure oxygen combustion simulation of Changqing petroleum coke was studied. On the basis of the original petroleum coke molecular model, N2 and O2 molecules were added to construct the air combustion simulation model and the pure oxygen combustion simulation model respectively. The number of molecules, main products, and typical hydrocarbon gases in the two simulation results were analyzed by setting up the LAMMPS in. file. Finally, the molecular changes of pyrrole and pyridine were described. The results show that the main reaction interval of pure oxygen combustion is earlier than that of air combustion. In the main reaction temperature range, the reaction rate of pure oxygen combustion is higher than that of simulated air combustion. At 170 ps, the two simulations reaction speed is the fastest time point; Pyridine is more stable than pyrrole. The research on the distinction and comparison of two kinds of simulation has certain guiding significance for the clean utilization of petroleum coke combustion process in industry.

Engineering of local electron properties optimization in single-atom catalysts enabling sustainable photocatalytic conversion of N2 into NH3

Photocatalytic synthesis of ammonia (NH3) from nitrogen (N2) offers a promising strategy for carbon neutrality, as it avoids the energy-intensive and carbon-emitting industrial processes. The exploration of high-efficiency N2 photofixation systems for photocatalytic N2 reduction reaction (pNRR) is critical but it remains a challenge since the lack of rational structural design and atomic-level insights into molecular N2 activation mechanism. Herein, an atomically dispersed single-atom palladium (Pd) active sites decorated oxygen-deficient molybdenum oxide (Pd/MoO3-x) was creatively designed for assessing pNRR performance. Interestingly, the integration of single-atom Pd active sites in MoO3-x can significantly weaken the N≡N bond of adsorbed N2 and effectively lower the activation energy barrier during the pNRR process. This is attributed to the fact that the modified Pd single-atom sites of Pd/MoO3-x play a dominant role in the N2 spontaneous adsorption process as well as possess a remarkable photogenerated electron trapping ability, which could be assisted to inject electrons into N2 antibonding orbital, thus significantly accelerates the reaction kinetics. Consequently, the Pd/MoO3-x photocatalyst reaches an impressive NH3 yield rate of 103.2 μggcat.−1h−1, which is superior to that of pristine MoO3-x (21.2 μggcat.−1h−1) and commercial MoO3 (6.5 μggcat.−1h−1), respectively. The present study not only creates a reliable approach to expand efficient N2 photofixation system under mild conditions through the fabrication of atomically dispersed monometallic active sites, but also offers atomic-level insights into the underlying mechanism of pNRR catalytic process.

A new look at N[formula omitted] electronic transitions: An experimental and theoretical study

Neutral and ionic N2 species exhibit a rich spectrum as a result of the large density of couplings between states with different multiplicities. In this sense, spectra of the molecular ion N2+ are investigated combining Fourier transform spectroscopy and ab initio methods. We have reanalyzed the First Negative band System (B2Σu+→ X2Σg+) including five bands not reported previously by Fourier spectroscopy. The spectra were recorded using a resolution of 0.6 cm−1 and accuracy of 0.005 cm−1. These results are then compared with new MRCI+Q/AV6Z calculations. For the first time, transition probabilities are computed for the previously observed 22Πg-A2Πu band system. The 22Πg state (Te = 67,029 cm−1) has a dissociation energy of 24,787 cm−1 at Re = 2.7332 a0. The predicted lifetimes for the 22Πg-A2Πu emissions are of the order of 170 ns. The calculated transition probabilities A(v′=0, v′′=0) for the B2Σu+-X2Σg+ and 22Πg-A2Πu bands are 1.156 × 107 and 1.716 × 103 s−1, respectively. The role of spin–orbit (SO) matrix elements in the spectroscopic data of N2+ is discussed, including results for SO constants as a function of vibrational level of A2Πu state. Our theoretical SO constant A0(A2Πu) = −73.40 cm−1 reproduces well the experimental one (−74.67 cm−1). SO calculations are also used to investigate spin-forbidden transitions on N2+. The obtained <A2Πu|HˆSO|a4Σu+>≈ 30 cm−1. Following a sum-over-states (SOS) methodology, the best estimate for the spin-rotation constant γ0 of the X2Σg+ and B2Σu+ states are 0.0096 and 0.0211 cm−1, respectively, in quantitative agreement with the present experimental data of 0.00917(36) and 0.0206(9).

Tailoring the efficiency of porphyrin molecular frameworks for the electroactivation of molecular N2.

The combination of compositional versatility and topological diversity for the integration of electroactive species into high-porosity molecular architectures is perhaps one of the main appeals of metal-organic frameworks (MOFs) in the field of electrocatalysis. This premise has attracted much interest in recent years, and the results generated have also revealed one of the main limitations of molecular materials in this context: low stability under electrocatalytic conditions. Using zirconium MOFs as a starting point, in this work, we use this stability as a variable to discriminate between the most suitable electrocatalytic reaction and specific topologies within this family. Our results revealed that the PCN-224 family is particularly suitable for the electroreduction of molecular nitrogen for the formation of ammonia with faradaic efficiencies above 30% in the presence of Ni2+ sites, an activity that improves most of the catalysts described. We also introduce the fluorination of porphyrin at the meso position as a good alternative to improve both the activity and stability of this material under electrocatalytic conditions.

Recent Developments of Dual Single-Atom Catalysts for Nitrogen Reduction Reaction.

Ammonia is vital for fertilizer production, hydrogen storage, and alternative fuels. The conventional Haber-Bosch process for ammonia production is energy-intensive and environmentally harmful. Designing environmentally friendly and low-energy consumption strategies for electrocatalytic N2 reduction reaction (ENRR) in mild conditions is meaningful. Single-atom catalysts (SACs) have been studied extensively for NRR due to their high atomic utilization and unique electronic structure but are limited by their poor faradic efficiency and low ammonia formation yield. Dual single-atom catalysts (DSACs) have recently emerged as a promising solution for the effective activation of molecular N2 , providing diverse active sites and synergistic interactions between adjacent atoms. In this review, we summarize the latest advances in metal DSACs for electrochemical ENRR based on both theoretical calculations and experimental studies, including aspects such as their variety, coordination, support, N2 adsorption and activity mechanisms, the characterization of NRR and electrochemical cell Configuration. We also address challenges and prospects in this rapidly evolving field, providing a comprehensive overview of DSACs for ENRR.

Raman scattering in the Earth’s atmosphere, Part II: Radiative transfer modeling for remote sensing applications

Raman scattering in the Earth’s atmosphere is caused predominantly by its most abundant molecular components, N2 and O2. After the computation of the optical properties that govern the spectral and angular redistribution of light due to various inelastic scattering events, viz. rotational Raman scattering (RRS), vibrational Raman scattering (VRS), and rovibrational Raman scattering (RVRS), covered in Part I of this series, the next challenge in the simulation of inelastic scattering in the Earth’s atmosphere is to carry out radiative transfer (RT) computations across several wavelengths simultaneously.In this part of our work, we provide the RT formulation for fully polarized simulations of inelastic scattering using the matrix-operator-method-based RT model vSmartMOM. The formalism is optimized for easy use with GPUs, allowing an unprecedented speedup of accurate multi-wavelength RT computations of inelastic scattering using the full Stokes-vector, thus allowing its operational use without coarse spectral binning (Rozanov and Vountas, 2014), or single scattering approximations (Sioris and Evans, 1999) at longer wavelengths.After comparing our model against the current state-of-the-art, we demonstrate the use of vSmartMOM to simulate Raman lidar measurements, the Ring effect, the ghosting of Fraunhofer lines due to vibrational Raman scattering and spectral corrections due to inelastic scattering in the O2 A-band in the Earth’s atmosphere. We use our model (1.) to validate the convention of neglecting the contribution of VRS and RVRS, and (2.) to quantify the speed and accuracy of the single scattering approximation in the O2 A-band.

Влияние колебательно-возбужденного молекулярного азота на инфракрасное свечение газов O3 и N2O на высотах средней атмосферы Земли

The concentrations of N2(X1g+, v' = 1) and the emission intensities of infrared bands of ozone O3 and nitrous oxide N2O are calculated at altitudes of 30–70 km of the Earth's middle atmosphere during precipitation of electrons with energies E = 2, 4, 10 MeV. It is shown that for a given relativistic electron flux of 105 e/cm2·s·ster, the concentrations of vibrationally excited molecular nitrogen N2(X1g+, v' = 1) are about 105–106 cm–3 at altitudes of 50–70 km of the middle atmosphere. The emission profiles of the infrared bands of ozone at 4.7 µm and 9,9 µm, as well as the infrared band of nitrous oxide at 4.5 µm, are calculated for precipitation of high-energy electrons with energies E = 2, 4, 10 MeV. It has been shown for the first time that vibrationally excited nitrogen N2(X1g+, v' = 1) plays an important role in changing the infrared balance of the middle atmosphere as a result of inelastic molecular collisions with O3 and N2O molecules during precipitation of high-energy electrons.

The study of electronic kinetics of molecular nitrogen in the Titan’s middle atmosphere during the precipitation of cosmic rays

The kinetics of the \({{{\text{A}}}^{3}}\Sigma _{u}^{ + },\) B3Πg, W3Δu, \({{{\text{B}}}^{{{\text{'}}3}}}\Sigma _{u}^{ - },\) and C3Πu triplet states of molecular nitrogen at the heights of the middle atmosphere of Titan during action of cosmic rays into the atmosphere has been studied. The calculations consider the intramolecular and intermolecular electron energy transfer during inelastic collisions of electronically excited molecular nitrogen with N2, CH4, and CO molecules. The interaction of electronically excited N2 molecules with molecules of acetylene C2H2 and ethylene C2H4 in the middle atmosphere of Titan at altitudes of 50–250 km has been studied. For the first time, the dominance of reactions with metastable molecular nitrogen N2(\({{{\text{A}}}^{3}}\Sigma _{u}^{ + }\)) in the formation of C2H and C2H3 radicals at these heights has been shown.

Long-Term Degradation Mechanisms in Application-Implemented Radical Thin Films.

Blatter radical derivatives are very attractive due to their potential applications, ranging from batteries to quantum technologies. In this work, we focus on the latest insights regarding the fundamental mechanisms of radical thin film (long-term) degradation, by comparing two Blatter radical derivatives. We find that the interaction with different contaminants (such as atomic H, Ar, N, and O and molecular H2, N2, O2, H2O, and NH2) affects the chemical and magnetic properties of the thin films upon air exposure. Also, the radical-specific site, where the contaminant interaction takes place, plays a role. Atomic H and NH2 are detrimental to the magnetic properties of Blatter radicals, while the presence of molecular water influences more specifically the magnetic properties of the diradical thin films, and it is believed to be the major cause of the shorter diradical thin film lifetime in air.

New carbon–nitrogen–oxygen compounds as high energy density materials

Molecular crystals are complex systems exhibiting various crystal structures, and accurately modeling the crystal structures is essential for understanding their physical behaviors under high pressure. Here, we perform an extensive structure search of ternary carbon-nitrogen-oxygen (CNO) compound under high pressure with the CALYPSO method and first principles calculations, and successfully identify three polymeric CNO compounds with Pbam, C2/m and symmetries under 100 GPa. More interestingly, these structures are also dynamically stable at ambient pressure, and are potential high energy density materials (HEDMs). The energy densities of Pbam, C2/m and phases of CNO are about 2.30 kJ/g, 1.37 kJ/g and 2.70 kJ/g, respectively, with the decompositions of graphitic carbon and molecular carbon dioxide and α-N (molecular N2) at ambient pressure. The present results provide in-depth insights into the structural evolution and physical properties of CNO compounds under high pressures, which offer crucial insights for designs and syntheses of novel HEDMs.

Mechanistic understanding of N2 activation: a comparison of unsupported and supported Ru catalysts.

N2 dissociative adsorption is commonly the rate-determining step in thermal ammonia synthesis. Herein, we performed density functional theory (DFT) calculations to understand the N2 dissociation mechanism on models of unsupported Ru(0001) terraces, Ru B5 sites, and polar MgO(111)-supported Ru8 cluster mimicking a B5 site geometry, denoted (Ru8(B5-like)/MgO(111)). The activation energy of N2 dissociative adsorption on the Ru8(B5-like)/MgO(111) model (Ea = 0.33 eV) is much lower than that on the unsupported Ru(0001) terrace (Ea = 1.74 eV) and Ru B5 (Ea = 0.62 eV) models. The lower N2 dissociation barrier on Ru B5 sites is facilitated by the enhanced σ donation and π* back-donation between N2(σ, π*) and Ru(d) orbitals resulting in the stronger activation of the molecular side-on N2* dissociation precursor. The Ru8(B5-like)/MgO(111) also exhibits enhanced σ donation because of the B5-like cluster geometry. Furthermore, the Ru cluster of the bare Ru8(B5-like)/MgO(111) model is positively charged. This induced an unusual π donation from N2(π) to Ru(d) orbitals as revealed by analyses of the density of states and partial charge densities. The combined σ and π donation resulted in an increased synergistic π* back-donation. The total interactions between N2(σ, π, π*) and Ru(d) resulted in an overall electron transfer to the adsorbed N2 from the Ru atoms in the B5-like site with no direct involvement of the MgO(111) substrate. Analyses of bond stretching vibrations and bond lengths show that the N2(σ, π, π*) and Ru(d) interactions lead to a weaker N-N bond and stronger Ru-N bonds. These correspond to a lower barrier of N2 dissociation on the Ru8(B5-like)/MgO(111) model, where the highest red-shift of N-N vibration and the longest N-N bond length were observed after side-on N2* adsorption. These results demonstrate that an electron-deficient Ru catalyst are not always inhibited from donating electrons to adsorbed N2. Rather, this study shows that the electron deficiency of Ru can promote π* back-donation and N2 activation. These new insights may therefore open new avenues to design supported Ru catalysts for nitrogen activation.

Computational Insight into Defective Boron Nitride Supported Double-Atom Catalysts for Electrochemical Nitrogen Reduction

Designing highly selective and efficient double-atom electrocatalysts (DACs) is essential for achieving a superior nitrogen-reduction reaction (NRR) performance. Herein, we explored the defective boron nitride–supported cage-like double-atom catalysts to rummage the qualified NRR catalysts. Based on a systematic evaluation of the stability, N2 adsorption, NRR selectivity and activity of 10 DACs of TM1-TM2@VB-BN, we predicted Ru-Ti@VB-BN to be the NRR candidate with a limiting potential of −0.40 V. Compared to the corresponding single-atom catalysts, the introduction of Ti/Mo modulates the d-band center of the active metal atom, which improves the NRR performance. Moreover, the magnetic Ru-Ti dimer can facilitate the transfer of charge to molecular N2, ensuring a significant activation of the inert N≡N bond. This research not only opens up new avenues for designing boron nitride–supported DACs for NRR, but also deepens the understanding of DACs in N2 activation.

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

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 N2 . 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 C17 Si and its (HOMO-1) level participate in N2 addition. The N-adduct so formed, is then found to spontaneously react with molecular H2 . The addition of two H2 molecules to the activated nitrogen molecule to give respective amine derivatives have also been studied. The successful generation of the precursor of NH3 by C17 Si lays a clear emphasis on its potentiality.

Color and spectral characteristics of long-lived meteor trail formed by the Tunka bolide

The paper addresses color characteristics and possible spectral composition of emission of a long-lived (~40 min) meteor trail of uncommon geometry, which was formed due to the bolide passage in the Tunka Valley on November 17, 2017. Analysis of dynamics of RGB channels of the meteor trail colored image shows that during the first ~8 minutes the meteor trail emission might have been contributed by the ionization trail. The ionization trail was formed by particles of the meteor matter neutral and ionized components that were heated to high temperatures on the surface of the main meteoroid and separated from it. We also examine the discussed mechanism of heterogeneous chemical reactions occurring on the surface of meteoric dust (FeS, FeO, etc.) with participation of atoms and molecules of atmospheric gases. The yellowish color of the Tunka bolide meteor trail was assumed to be determined, first of all, by the emission of molecular nitrogen N₂ band within the 570–750 nm spectral range (the first positive system) and/or enhancement of NO*₂ continuum in heterogeneous chemical reactions. The meteor trail emission spectrum should also include relatively bright atomic lines and molecular bands of the meteoric matter and atmospheric gases FeI, MgI, CaI, SiI, NaI, FeO and SO₂, OI, OH, etc.