Journal of Chemical Sciences最新文献

{"title":"Design and synthesis of hexahydro pyrene containing unusual α-amino acid derivatives","authors":"Sambasivarao Kotha,&nbsp;Vidyasagar Gaikwad,&nbsp;Saima Ansari","doi":"10.1007/s12039-023-02170-5","DOIUrl":"10.1007/s12039-023-02170-5","url":null,"abstract":"<div><p>We report constrained α-amino acid derivatives containing hexahydro pyrene unit using ethyl isocyanoacetate as a glycine equivalent. The required precursor 1,4,5,8-tetrakis(bromomethyl)naphthalene <b>3</b> was prepared from commercially available naphthalene-1,4,5,8-tetracarboxylic anhydride <b>4</b> in a three-step sequence.</p><h3>Graphical abstract</h3><p>Herein, we have developed a facile synthetic strategy to hexahydro pyrene bearing unusual amino acid derivative through the coupling of 1,4,5,8-tetrakis(bromomethyl)naphthalene with ethyl isocyanoacetate (EICA) as a glycine equivalent.</p><figure><div><div><div><picture><source><img></source></picture></div></div></div></figure></div>","PeriodicalId":50242,"journal":{"name":"Journal of Chemical Sciences","volume":"135 2","pages":""},"PeriodicalIF":1.7,"publicationDate":"2023-05-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"4433963","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"External electric field as a catalyst for ammonia formation via reaction of N(_2) and N-heterocyclic carbene","authors":"Priyanka Yadav,&nbsp;Pradeep Kumar","doi":"10.1007/s12039-023-02162-5","DOIUrl":"10.1007/s12039-023-02162-5","url":null,"abstract":"<div><p>Based on quantum chemical calculations, we have investigated an external electric field (EEF) as a potential catalyst for ammonia formation from the reaction of N<span>(_2)</span> with 3,5-di-tert-butyl-2-oxopiperidine-1-carbonitrile carbene. It is shown that by choosing the EEF at suitable direction and strength, the barrier for the reaction can be reduced from <span>(sim)</span> 17.10 kcal mol<span>(^{-1})</span> to <span>(sim)</span> 0.97 kcal mol<span>(^{-1})</span>. It was also shown by computing the reaction rate that in the presence of EEF, the rate of title reaction can be increased by trillionfold. Therefore, N<span>(_2)</span> with N-heterocyclic carbene (NHC) in the presence of an external electric field gives the possibility of a very efficient way of making ammonia from nitrogen.</p><h3>Graphical abstract</h3><p>In the present work, we have shown that without any catalyst, the reaction of N₂ with N-heterocyclic carbene is a high barrier reaction, but by choosing an external electric field at a\u0000suitable direction and strength, the rate of N₂ with NHC can be increased by a trillionfold.\u0000Therefore, N₂ with NHC in the presence of an external electric field gives the possibility of\u0000a very efficient way of making ammonia from nitrogen.</p><figure><div><div><div><picture><source><img></source></picture></div></div></div></figure></div>","PeriodicalId":50242,"journal":{"name":"Journal of Chemical Sciences","volume":"135 2","pages":""},"PeriodicalIF":1.7,"publicationDate":"2023-05-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"4431094","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Futuristic storage devices: Single molecular magnets of rare earths versus spin crossover systems of earth-abundant metals","authors":"Gargi Bhatt,&nbsp;Aheli Ghatak,&nbsp;Ramaswamy Murugavel","doi":"10.1007/s12039-023-02163-4","DOIUrl":"10.1007/s12039-023-02163-4","url":null,"abstract":"<div><p>Molecular toolkit is a crucial part of futuristic spintronics and quantum information technologies. Magnetic bistability is the basis for such applications, which can be achieved by spin crossover (SCO) systems and single molecular magnets (SMMs). The SCO phenomenon relies on cooperativity, while the latter defies it. For the first time, a recent report by Galán-Mascarós and coworkers outlined the occurrence of memory effect in a trinuclear iron spin crossover system through its incorporation in a solid-state diamagnetic matrix or as a dilute solution. The fact that this molecule can show a memory effect on dilution, almost at a molecular level, opens up new possibilities for SCO systems doubling up as single-molecule magnets at elevated temperatures in the foreseeable future.</p><h3>Graphical abstract</h3><p>Memory effect in a trinuclear iron spin crossover system by incorporating it in a solid-state diamagnetic matrix or as a dilute solution opens up new vistas in molecular magnetism is detailed in this article.</p>\u0000 <figure><div><div><div><picture><source><img></source></picture></div></div></div></figure>\u0000 </div>","PeriodicalId":50242,"journal":{"name":"Journal of Chemical Sciences","volume":"135 2","pages":""},"PeriodicalIF":1.7,"publicationDate":"2023-05-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"4224458","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Structure and diffusion of active-passive binary mixtures in a single-file","authors":"Tanwi Debnath,&nbsp;Shubhadip Nayak,&nbsp;Poulami Bag,&nbsp;Debajyoti Debnath,&nbsp;Pulak Kumar Ghosh","doi":"10.1007/s12039-023-02158-1","DOIUrl":"10.1007/s12039-023-02158-1","url":null,"abstract":"<div><p>We numerically study structure and dynamics of single files composed of active particles, as well as, active-passive binary mixtures. Our simulation results show that when the persistent length of self-propelled particles is much larger than the average inter-particle separation and the self-propulsion velocity is larger than the thermal velocity, particles in the file exist as clusters of various sizes. Average cluster size and structures of the file are very sensitive to self-propulsion properties, thermal fluctuations and composition of the mixture. In addition to the variation of file composition, our study considers two sorts of mixture configurations. One corresponds to the uniform distribution of active passive throughout the mixture in the single file. In the other configuration, active particles are on one side of the file. For the both configurations, even a little fraction of active particles produces a large impact on the structure and dynamics of the file.</p><h3>Graphical abstract</h3><p>When persistent length of active species is much larger than average inter-particle separation, active-species in a single-file exist as clusters of various sizes. Due to the motility transfer mechanism, little fractions of active  particles have great impacts on the structure and dynamics of single-files composed of active-passive binary mixtures. </p><figure><div><div><div><picture><source><img></source></picture></div></div></div></figure></div>","PeriodicalId":50242,"journal":{"name":"Journal of Chemical Sciences","volume":"135 2","pages":""},"PeriodicalIF":1.7,"publicationDate":"2023-04-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"5072890","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Impurity effects on phase change in Lennard-Jones atomic clusters","authors":"Sankar Ghorai,&nbsp;Mintu Nandi,&nbsp;Pinaki Chaudhury","doi":"10.1007/s12039-023-02156-3","DOIUrl":"10.1007/s12039-023-02156-3","url":null,"abstract":"<div><p>In this work, we would like to explore the possibility of studying phase change behaviour in pure Lennard-Jones clusters as well as the effect of introducing a heteroatom. The system studied are <span>({textrm{Ar}}_{10})</span>, <span>({textrm{Xe}}_{10})</span> and <span>({textrm{Ar}}_{10-1}{textrm{Xe}}_1)</span> as well as <span>({textrm{Ar}}_{10-9}{textrm{Xe}}_{9})</span>. The phase change is followed by the temperature variation in classical configuration heat capacity. As the heat capacity is calculated by evaluating the variance in the energy of the isomers possible, an important aspect is to sample the Lennard-Jones surface effectively and pick out as many isomers which are possible for this system. The sampling at various temperatures has been done using the replica exchange Monte Carlo or Parallel tempering procedure. The main focus of the present work is to see how the phase change behaviour is affected on going from the pure Lennard-Jones systems to the once possessing dopants. To further aid in the understanding bond length fluctuation parameter has also been calculated for all the systems with changing temperature along with the classical configuration.</p><h3>Graphical abstract</h3><p>Synopsis: The phase change behavior of pure Lennard-Jones clusters and the effect of introducing a heteroatom was studied using replica exchange Monte Carlo or parallel tempering techniques and examining the classical configuration heat capacity and bond length fluctuation parameter. The systems studied were Ar₁₀ , Xe₁₀ and Ar₁₀₋₁ Xe₁ as well as Ar₁₀₋₉ Xe₉.\u0000</p><figure><div><div><div><picture><img></picture></div></div></div></figure></div>","PeriodicalId":50242,"journal":{"name":"Journal of Chemical Sciences","volume":"135 2","pages":""},"PeriodicalIF":1.7,"publicationDate":"2023-04-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s12039-023-02156-3.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"4484608","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Details of ozonolysis of catechol at high temperature and product energy distribution","authors":"Ankita Agarwal,&nbsp;Amit Kumar Paul","doi":"10.1007/s12039-023-02152-7","DOIUrl":"10.1007/s12039-023-02152-7","url":null,"abstract":"<div><p>On-the-fly classical dynamics simulation is performed for the post-transition state dynamics of ozonolysis of catechol at an internal (rotational + vibrational) excitation temperature of 1000 K. The results are compared to the same obtained at lower internal temperatures of 400 and 500 K. The product energy distributions are obtained for the products CO₂, H₂O, and CO obtained from the simulations at 400, 500, and 1000 K. O₂ channel, which was an insignificant channel at 400/500 K, becomes one of the major channels at 1000 K. Moreover, the CO₂ channel is seen to follow a different path at 1000 K than at lower temperatures. The potential energy profiles of these new CO₂ and O₂ channels are reported. Center-of-mass translational, rotational, and vibrational energy distributions of the products suggest that the product molecules are significantly hot in all degrees of freedom, and the dynamics is non-statistical.</p><h3>Graphical abstract</h3><p>The on-the-fly classical dynamics simulation of the ozonolysis of catechol was done at internal (rotational + vibrational) excitation temperatures of 400, 500, and 1000 K and four product channels namely; CO, CO₂, H₂O, and SCA. At 1000K a different path for the CO₂ channel was observed and an O₂ channel was also observed. The product energy distributions are obtained for the products, CO₂, H₂O, and CO obtained from the simulations at 400, 500, and 1000 K.</p>\u0000 <figure><div><div><div><picture><source><img></source></picture></div></div></div></figure>\u0000 </div>","PeriodicalId":50242,"journal":{"name":"Journal of Chemical Sciences","volume":"135 2","pages":""},"PeriodicalIF":1.7,"publicationDate":"2023-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"4442062","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Benzoxanthones derivatives: insight into oxalic acid catalyzed synthesis, crystallographic analysis and potential application in dye-sensitized solar cell","authors":"Pooja Bedi,&nbsp;Anil Kumar Behera,&nbsp;Abdullah K Alanazi,&nbsp;Manas Roy,&nbsp;Suvadra Das,&nbsp;Rahul Shukla,&nbsp;Tanay Pramanik,&nbsp;Anik Sen","doi":"10.1007/s12039-023-02151-8","DOIUrl":"10.1007/s12039-023-02151-8","url":null,"abstract":"<div><p>This study reports the synthesis of benzoxanthone derivatives by employing oxalic acid as a catalyst under ultrasonic irradiations and grinding techniques. Results show that the ultra-sonication method is much more reliable and gives better yields in lesser time. A detailed crystallographic analysis of the previously reported structures reveals that dispersive forces primarily drive crystal packing. Additionally, a theoretical understanding of the mechanism was performed, followed by applying such benzoxanthones as donor moieties for Donor-π-spacer-Acceptor type dye sensitizers for Dye Sensitizer solar cells.</p><h3>Graphical abstract</h3><p>The article describes a novel way of synthesizing Benzoxanthones Derivatives using: Oxalic Acid Catalyst. The work also sheds light on the energetics associated with the crystal structure of Benzoxanthones Derivatives along with their potential application in Dye-Sensitized Solar Cells (DSSC).\u0000</p><figure><div><div><div><picture><source><img></source></picture></div></div></div></figure></div>","PeriodicalId":50242,"journal":{"name":"Journal of Chemical Sciences","volume":"135 2","pages":""},"PeriodicalIF":1.7,"publicationDate":"2023-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s12039-023-02151-8.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"4443968","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Highly selective in-situ prepared g-C3N4/P-B composite photocatalyst for direct C-H bond arylation and NADH regeneration cofactor under solar light","authors":"Neetika Swarnkar,&nbsp;Rajesh K Yadav,&nbsp;Satyam Singh,&nbsp;Rehana Shahin,&nbsp;Ravindra K Shukla,&nbsp;Santosh K Tripathi,&nbsp;Dilip K Dwivedi,&nbsp;Satya Nath,&nbsp;Chandani Singh,&nbsp;Jin-O Baeg","doi":"10.1007/s12039-023-02150-9","DOIUrl":"10.1007/s12039-023-02150-9","url":null,"abstract":"<div><p>Metal-free photocatalysis is a sustainable and environmentally friendly method of transforming solar energy into molecules with added value. A light-harvesting photocatalyst without metal Phloxin-B (P-B) <i>in-situ</i> edge functionalized graphitic carbon nitride (g-C₃N₄) was assembled to enable the solar-light responsive photocatalytic C-H bond arylation and NADH regeneration cofactor. The photocatalytic performance was examined to estimate the C-H bond arylation and NADH regeneration efficiency by g-C₃N₄/P-B composite photocatalyst. The charge carrier transfer of g-C₃N₄ was found to be stimulated by the light harvester P-B layer, increasing the efficiency of chemical synthesis under solar light irradiation. In light of this, the g-C₃N₄/P-B composite photocatalyst exhibits high photocatalytic activity for the successful C-H bond arylation (98.6%) and regeneration of NADH (70.7%). This composite photocatalyst was characterized by FTIR and UV-visible spectrum along with particle size analysis, and cyclic voltammetry (CV). This effort offers a new and superficial technique to synthesize a highly efficient g-C₃N₄/P-B composite photocatalyst and afford a greener path for renewable energy and photocatalytic reactions.</p><h3>Graphical abstract</h3><p>The graphical abstract represents the highly selective g-C₃N₄/P-B photocatalyst for the C-H bond activation of 4-bromoaryldiazonium salts with furan and regeneration of NADH under solar light irradiation. The g-C₃N₄/P-B photocatalyst has been effective photocatalytic property due stacking of Phloxin-B dye (P-B) on the g-C₃N₄ sheet. NADH regenerated and C-H bond arylated products are used as substrates in the pharma industries.</p>\u0000 <figure><div><div><div><picture><source><img></source></picture></div></div></div></figure>\u0000 </div>","PeriodicalId":50242,"journal":{"name":"Journal of Chemical Sciences","volume":"135 2","pages":""},"PeriodicalIF":1.7,"publicationDate":"2023-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"4107431","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Synthesis and structural characterization of unsymmetrical Schiff base 2-(1-(2-aminophenylimino)ethyl)phenol (LH3) and its Pd(II) complex [Pd3(LH)3]: catalysis of Suzuki–Miyaura cross-coupling reaction","authors":"Uday Chand Mandal,&nbsp;Arnab Chatterjee,&nbsp;Taraknath Chattopadhyay,&nbsp;Aparajita Mukherjee,&nbsp;Rajarshi Ghosh","doi":"10.1007/s12039-023-02142-9","DOIUrl":"10.1007/s12039-023-02142-9","url":null,"abstract":"<div><p>An unsymmetrical Schiff base 2-(1-(2-aminophenylimino)ethyl)phenol (LH₃) and its trinuclear Pd(II) complex [Pd^II₃(LH)₃] (<b>1</b>) were successfully synthesized and X-ray crystallographically characterized. <b>1</b> effectively catalyzed Suzuki-Miyaura coupling on reaction between each of bromobenzene and substituted bromobenzenes with phenylboronic acid resulting biphenyl and substituted biphenyls, respectively. The catalyzed products were characterized gas chromatographically.</p><h3>Graphical abstract</h3><p>An unsymmetrical Schiff base 2-(1-(2-aminophenylimino)ethyl)phenol (LH₃) and its trinuclear Pd(II) complex [Pd^II₃(LH)₃] (<b>1</b>) were synthesized, and characterized both spectroscopically and X-ray crystallographically. LH₃ and <b>1</b> were found to had Cc and P-1 space groups with monoclinic and triclinic crystal systems. <b>1</b> was found to catalyze Suzuki-Miyaura cross coupling reactions to produce biphenyl and p-nitrobipheenyl from respective bromobenzene and p-nitrobromobenzene.</p>\u0000 <figure><div><div><div><picture><source><img></source></picture></div></div></div></figure>\u0000 </div>","PeriodicalId":50242,"journal":{"name":"Journal of Chemical Sciences","volume":"135 2","pages":""},"PeriodicalIF":1.7,"publicationDate":"2023-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"4108370","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Understanding the correlation of microscopic structure and macroscopic properties of multi-component glass through atomistic simulations","authors":"Pooja Sahu,&nbsp;S K Musharaf Ali,&nbsp;K T Shenoy,&nbsp;A Arvind,&nbsp;D Banerjee,&nbsp;Sanjay Kumar,&nbsp;S Manohar,&nbsp;Kislay Bhatt","doi":"10.1007/s12039-023-02143-8","DOIUrl":"10.1007/s12039-023-02143-8","url":null,"abstract":"<div><p>Nuclear power is attracting renewed interest as an alternative power source because it is climate friendly with low greenhouse gas emissions, but its acceptance depends on the safe containment of nuclear waste under geological repositories. For the immobilization of high-level liquid waste (HLLW), borosilicate glass has been considered to be the preferred choice. Selecting suitable glass composition for the vitrification of HLLW is one of the major challenges in nuclear waste reprocessing. The fusion of valuable material properties has led to the acceptance of sodium borosilicate (NBS) glasses for nuclear waste immobilization. The mechanisms associated with these properties are only partially exposed and need further exploration. In that perspective, ZnO doping in borosilicate glasses was studied by performing experiments, classical molecular dynamics (MD), and <i>ab-initio</i> MD (AIMD) simulations. A significant change in glass structure was monitored from short-range order parameters (pair correlation function) and intermediate-range order parameters (angle distribution profiles). Order of connectivity illustrated that the hydrolysis of glass would slow down with the addition of ZnO in the glass matrix. Successively, the effect of microscopic structure on observable glass properties: chemical durability, mechanical strength, and thermal stability, was analyzed. Results show a good match of MD estimated trend for Young Modulus, glass transition temperature, and leaching data with the experimental observations, confirming the transferability of applied potential parameters for multi-component (n≥4) glasses. Both the experiments and MD simulations report the enhanced chemical durability of glass with ZnO addition. The enhanced chemical resistivity of Zn-NBS was also established from the increasing activation energy for the diffusion of Na ions. The combined studies from experiments and atomistic simulations disclose many fascinating microstructures and dynamics due to the presence of ZnO in the glass. The results presented here can be exploited to construe the experimental results and plan future experiments.</p><h3>Graphical abstract</h3><p>The chemical, mechanical, and thermal strength of ZnO-incorporated sodium borosilicate glass was demonstrated by combined experiments and molecular dynamics (MD) simulations. The BKS interatomic potential was validated by <i>ab-initio</i> MD (AIMD) simulation. The results show the good mapping of MD-generated radial and angle distribution functions with the AIMD results.\u0000</p><figure><div><div><div><picture><source><img></source></picture></div></div></div></figure></div>","PeriodicalId":50242,"journal":{"name":"Journal of Chemical Sciences","volume":"135 2","pages":""},"PeriodicalIF":1.7,"publicationDate":"2023-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"4107987","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}