Article
Chemistry, Organic
Du Ding, Lian-Feng Fan, Zhi-Yong Han, Pu-Sheng Wang
Summary: In this article, a three-component and redox-neutral synthesis of homoallyl amines and homoallylic alcohols is described. This reaction involves readily available C=X compounds, 1,3-butadiene, and various nucleophiles, and is catalyzed by the combination of photoredox and nickel catalysts.
Article
Chemistry, Multidisciplinary
Huimin Yu, Qinglong Zhang, Weiwei Zi
Summary: In this study, the use of synergistic Pd/Cu catalysis in the photochemical 1,4-bisalkylation reactions was reported, resulting in the efficient synthesis of α-amino acid esters bearing quaternary stereocenters. Experimental and computational investigation confirmed a radical pathway involving catalysis by an excited-state palladium species, with the stereochemistry mainly controlled by the chiral Cu catalyst.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Environmental Sciences
Monika Bhattu, Meenakshi Verma, Aabid A. Wani, P. V. Bharatam, Shweta Sareen, Deepika Kathuria
Summary: This study demonstrates a simple method for synthesizing organic nanoparticles (ONPs) and blue fluorescent Quantum Dots (QDs) with potential applications in pesticide sensing. The synthesized QDs show selective sensing potential towards imidacloprid and exhibit a good linear response within a certain concentration range.
ENVIRONMENTAL RESEARCH
(2023)
Article
Chemistry, Physical
Asami Matsuda, Yoshitaka Matsumura, Yasuhiro Yamada, Satoshi Sato
Summary: This study focused on the vapor-phase catalytic dehydration of 1,4-butanediol over Y2O3-ZrO2 catalysts, producing different products depending on reaction conditions. Y2Zr2O7 with an equimolar ratio of Y/Zr exhibited high selectivity for 3B1OL. Calcination at 700 degrees Celsius showed the highest catalytic activity for BD formation. The reactivity of 3B1OL was found to be higher than that of saturated alcohols, suggesting a probable one-step dehydration mechanism for 1,4-BDO to BD conversion.
MOLECULAR CATALYSIS
(2021)
Article
Engineering, Environmental
Juan V. Alegre-Requena, Glenn R. Hafenstine, Xiangchen Huo, Yanfei Guan, Jim Stunkel, Frederick G. Baddour, Kinga A. Unocic, Bruno C. Klein, Ryan E. Davis, Robert S. Paton, Derek R. Vardon, Seonah Kim
Summary: This study investigated the production of 1,3-butadiene (BDE) from 2,3-butanediol (2,3-BDO) using silica-supported phosphoric acid and metal phosphate catalysts. Experimental tests demonstrated that the catalyst achieved a maximum BDE yield of 63% when commercially available 2,3-BDO was used. Quantum chemical mechanistic studies revealed the involvement of 1,2-epoxybutane as a kinetically viable and thermodynamically stable intermediate in the production of BDE.
CHEMICAL ENGINEERING JOURNAL
(2023)
Review
Chemistry, Physical
Meena Devi, Parvin Kumar, Rahul Singh, Laxmi Narayan, Ashwani Kumar, Jayant Sindhu, Sohan Lal, Khalid Hussain, Devender Singh
Summary: The 1,4-naphthoquinone skeleton is an important component found in many biologically active natural products and chemotherapy agents. 1,4-naphthoquinones with electron donor amino substituents on specific positions have the potential to act as anion sensors and have various biological and industrial applications. 2,3-diamino-1,4-naphthoquinone is a promising bacteriostatic agent.
JOURNAL OF MOLECULAR STRUCTURE
(2022)
Article
Chemistry, Physical
Kairi Onodera, Yosuke Nakaji, Mizuho Yabushita, Yoshinao Nakagawa, Keiichi Tomishige
Summary: The dehydration of biomass-derived 1,4-butanediol (1,4-BDO) to 1,3-butadiene (BD) can be efficiently catalyzed by cerium oxide (CeO2) with weak acid-base bifunctionality, leading to a yield of 66% and a selectivity of 80% under optimized conditions. However, catalysts with strong acid sites, such as SiO2-Al2O3 and H-type mordenite (H-MOR), are not suitable for this reaction as they produce tetrahydrofuran as the major product.
APPLIED CATALYSIS A-GENERAL
(2023)
Article
Chemistry, Organic
Zhenqiang Chen, Yingying Sun, Shoufeng Wang, Qing-Wei Zhang
Summary: A base-promoted tandem Michael addition of malonates to 2,3-bis(diarylphosphinyl)-1,3-butadienes was developed for the synthesis of cyclopentyl 1,2-bisphosphine compounds. This method enables rapid construction of various 1,2-bis(diarylphosphinyl)cyclopentanes, and features readily accessible reactants, mild conditions and good functional group tolerance. The product could be easily transformed to the corresponding transition metal complexes, which may find broad applications in asymmetric catalysis.
EUROPEAN JOURNAL OF ORGANIC CHEMISTRY
(2023)
Article
Polymer Science
Beibei Wang, Heng Liu, Tao Tang, Xuequan Zhang
Summary: Highly cis-1,4 selective polymerization of 1,3-butadiene using specific cobalt complexes has been achieved with high thermal stability and yield. The molecular weight distribution of the resulting polymers is narrow and can be finely tuned by adjusting polymerization parameters. Additionally, the successful copolymerization with a polar monomer significantly improves the surface properties of the polymer.
Article
Chemistry, Multidisciplinary
Makoto Shimizu, Toshihiro Yamamoto, Hiroaki Shindo, Isao Mizota, Yusong Zhu
Summary: The compound 2,3-dimethoxy-2,3-dimethyl-1,4-dioxane serves as a stable precursor to functionalized cyclohexene derivatives through a [4+2] cycloaddition reaction, which can be transformed into potentially useful intermediates for biologically important materials.
Article
Chemistry, Physical
Kazuki Nakazono, Ryoji Takahashi, Yasuhiro Yamada, Satoshi Sato
Summary: The study showed that Sc2O3 catalyst prepared and aged under specific conditions exhibits excellent catalytic activity for the dehydration of 2,3-butanediol, leading to high purity 3-buten-2-ol and 1,3-butadiene production.
MOLECULAR CATALYSIS
(2021)
Article
Chemistry, Physical
Jianhui Jin, Cheng Xie, Jiao Gao, Hong Wang, Jinyang Zhang, Yujie Zhao, Min Gao, Jiabi Ma, Zhandong Wang, Jiwen Guan
Summary: This study investigates the reactions of 1,3-butadiene with cycloheptatriene and 5-methylene-1,3-cyclohexadiene in a SiC microreactor, leading to the formation of toluene. Experimental evidence and theoretical calculations suggest that 5-methylene-1,3-cyclohexadiene is a key intermediate in the primary reaction, and secondary reactions play a role in enhancing toluene formation. These findings provide insights into the mechanism of toluene-promoted molecular growth of PAHs in combustion environments.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Lijia Liu, Feng Wang, Chunyu Zhang, Heng Liu, Guangfeng Wu, Xuequan Zhang
Summary: A series of high thermal stability alpha-diimine nickel and cobalt complexes were revealed in this study, suitable for high-temperature polymerization of 1,3-butadiene. Increasing temperature can enhance the yield but decrease the molecular weight and cis-1,4- content of the resultant polymers.
MOLECULAR CATALYSIS
(2022)
Article
Chemistry, Multidisciplinary
Qi-Chen Wei, Ya Chen, Zhao Wang, Da-Zhuang Yu, Wei-Hao Wang, Jian-Quan Li, Li-Hua Chen, Yu Li, Bao-Lian Su
Summary: A light-assisted semi-hydrogenation process using water as the hydrogen atom source and in situ photocatalysis was developed, showing excellent catalytic performance and selectivity for 1,3-butadiene semi-hydrogenation at ambient temperature. This H-2-free process has the potential to bring advancements in industrial hydrogenation technology in terms of economic and safe operations.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Asami Matsuda, Fumiya Sato, Yasuhiro Yamada, Satoshi Sato
Summary: This study investigated the vapor-phase catalytic dehydration of 1,4-butanediol using rare earth metal oxide catalysts, resulting in the production of 1,3-butadiene. Yb2O3 exhibited the highest catalytic activity, which was further enhanced by hydrothermal aging. The results also indicated that the morphology of Yb2O3 and its catalytic activity were influenced by the hydrothermal aging conditions.
BULLETIN OF THE CHEMICAL SOCIETY OF JAPAN
(2022)
Review
Chemistry, Multidisciplinary
Saroj Kumar Kushvaha, Ankush Mishra, Herbert W. Roesky, Kartik Chandra Mondal
Summary: The isolation of cyclic (alkyl) amino carbenes (cAACs) in 2005 was a significant breakthrough in the field of stable carbenes. Their excellent electronic properties have led to their utilization in various areas of chemistry, including catalysis.
CHEMISTRY-AN ASIAN JOURNAL
(2022)
Article
Chemistry, Inorganic & Nuclear
Ekta Nag, Aditya Kulkarni, Sai Manoj N. V. T. Gorantla, Nico Graw, Maria Francis, Regine Herbst-Irmer, Dietmar Stalke, Herbert W. Roesky, Kartik Chandra Mondal, Sudipta Roy
Summary: The precursor SbCl (Top) has been used for the synthesis of a distibane compound via one-electron reduction using KC8. Different alkali metals were used as reducing agents to isolate corresponding stable dimeric alkali metal antimonides. The synthesized compounds were characterized using various analytical techniques and their catalytic activity and luminescent properties were studied.
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Inorganic & Nuclear
Kavita Devi, Sai Manoj N. V. T. Gorantla, Kartik Chandra Mondal
Summary: This study provides a deeper insight into the N-2 binding and the influence of carbon atoms in previously reported Fe complexes through energy decomposition analysis and natural orbital for chemical valence calculations/analyses. The role of carbon atoms in the iron-carbon site is studied using deformation electron densities, and the interaction energy between Fe and N-2 as well as the orbital interactions between them are quantitatively estimated. The sigma-donation effects of three phosphine ligands and their effects on the Fe-N-2 bond are thoroughly studied.
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Physical
Saroj Kumar Kushvaha, Sai Manoj N. V. T. Gorantla, Kartik Chandra Mondal
Summary: The structure and properties of donor ligands with bent Si2C units have been revealed through theoretical calculations. The results suggest that the Si2C unit can be stabilized by a pair of donor base ligands, with electrostatic and covalent orbital interactions playing a major role in the interaction energy.
JOURNAL OF PHYSICAL CHEMISTRY A
(2022)
Article
Chemistry, Multidisciplinary
Sai Manoj N. V. T. Gorantla, Kartik Chandra Mondal
Summary: Metal complexes containing low valence iron atoms can bind with dinitrogen molecules and produce ammonia under suitable conditions. The higher affinity between iron atoms and dinitrogen compared to other transition metal atoms is explored in this study. The analysis of the interacting orbitals and energy in the metal complexes provides insights into the mechanism of interaction between dinitrogen and iron atoms.
Article
Chemistry, Multidisciplinary
Harsha S. Karnamkkott, Sai Manoj N. V. T. Gorantla, Kavita Devi, Geetika Tiwari, Kartik Chandra Mondal
Summary: Recent advances in non-metal compounds have successfully achieved dinitrogen binding and activation, attracting scientific attention for its potential in reducing N-2 into ammonia. The study demonstrates the stability and bonding of cAAC-E bonded N-2-complex, suggesting the synthesis of elusive species may be possible with cAAC ligands and bulky substitutions. The thermodynamic favorability of E=E bond formation over N-2 binding energy between two cAAC-E units is highlighted in the research.
Article
Chemistry, Multidisciplinary
Robert Izsak, Christoph Riplinger, Nick S. Blunt, Bernardo de Souza, Nicole Holzmann, Ophelia Crawford, Joan Camps, Frank Neese, Patrick Schopf
Summary: Quantum computers are expected to be useful in simulating strongly correlated chemical systems, but careful selection of orbital spaces is crucial. This study presents a scheme for automatically selecting an active space and combines quantum phase estimation and variational quantum eigensolver algorithms to accurately describe the environment. The protocol outlined here can be applied to chemical systems of any size, including those beyond the capabilities of classical computation.
JOURNAL OF COMPUTATIONAL CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Sai Manoj N. V. T. Gorantla, Harsha S. Karnamkkott, Selvakumar Arumugam, Sangita Mondal, Kartik Chandra Mondal
Summary: The factors influencing the binding, activation, and reduction of N-2 by FeMoco of nitrogenase are not completely understood. Model complexes have been synthesized and studied, but they differ from the real Fe-sites of FeMoco. This study focuses on a series of complexes containing a weak field ligand and investigates their effect on Fe-centers and N-2 binding.
JOURNAL OF COMPUTATIONAL CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Selvakumar Arumugam, Madhuri Bhattacharya, Sai Manoj N. V. T. Gorantla, Kartik Chandra Mondal
Summary: Two new series of air stable compounds containing cAAC(X)= fluorene/indene groups were isolated and characterized. These compounds showed green light emission and solvatochromism in solution, and exhibited a quasi-reversible electron transfer process as confirmed by cyclic voltammogram and electron paramagnetic resonance studies. DFT/TDDFT calculations and energy decomposition analysis were performed to study their bonding and electronic transitions. These redox active and thermally stable organic molecules may have potential applications in molecule based spin memory devices.
CHEMISTRY-AN ASIAN JOURNAL
(2023)
Article
Chemistry, Medicinal
Markus R. Hermann, Christofer S. Tautermann, Peter Sieger, Marc A. Grundl, Alexander Weber
Summary: We conducted a comprehensive study on predicting the reactivity of propynamides. Covalent inhibitors like propynamides have improved potency, selectivity, and unique pharmacologic properties compared to non-covalent counterparts. By using three different in silico methods, we were able to predict the in vitro properties of propynamides, a covalent warhead class found in approved drugs. While the electrophilicity index only applies to specific subclasses, adduct formation and transition state energies are good predictors of in vitro reactivity with glutathione (GSH). Overall, these methods are suitable for estimating the reactivity of propynamides, allowing for the fine tuning of reactivity and speeding up the design process of covalent drugs.
Article
Chemistry, Inorganic & Nuclear
Sunil Kumar, Selvakumar Arumugam, Bjoern Schwarz, Helmut Ehrenberg, Kartik Chandra Mondal
Summary: A representative Co(II) based single ion magnet (SIM) with N2O2 donor set and distorted pseudo-tetrahedral geometry has been synthesized and characterized. The atomic and electronic structure have been studied through DC magnetometry, ab-initio multi-reference CASSCF calculations, and qualitative ligand field theory. AC magnetometry has been used for the investigation of spin-lattice relaxation with temperature and magnetic field variations.
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Physical
Robert Izsak, Aleksei V. Ivanov, Nick S. Blunt, Nicole Holzmann, Frank Neese
Summary: In this article, the different measures of electron correlation in wave function theory, density functional theory, and quantum information theory are briefly reviewed. The focus is then placed on a more traditional metric based on dominant weights in the full configuration solution and its behavior regarding the choice of N-electron and one-electron basis. The impact of symmetry is discussed, and the usefulness of distinguishing between determinants, configuration state functions, and configurations as reference functions is emphasized.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Multidisciplinary
Sonam Suthar, Kartik Chandra Mondal
Summary: In this study, energy decomposition analysis and natural orbital for chemical valence (EDA-NOCV) were used to investigate the bonding in cyclopropane rings of 49 different organic compounds. The majority of compounds (37/49) were found to preferentially form two dative covalent C-C bonds, while a smaller portion (7/49) favored two covalent electron sharing bonds. A few compounds (5/49) showed flexibility to adopt either bonding mode. The effects of functional groups on the bonding were also studied. The bonding analyses were supported by QTAIM analyses, which revealed distinct parameters for C-3 rings compared to normal hydrocarbons. The bonding in most cyclopropane rings was found to be similar to metal-olefin systems.
JOURNAL OF COMPUTATIONAL CHEMISTRY
(2023)
Article
Chemistry, Inorganic & Nuclear
Selvakumar Arumugam, Bjoern Schwarz, Prathap Ravichandran, Sunil Kumar, Liviu Ungur, Kartik Chandra Mondal
Summary: This work investigates the dynamic magnetic properties of a complex [(Cp-Ar3)(4)(Dy2Cl4K2)-Cl-III]& BULL;3.5(C7H8) synthesized using a tri-aryl-substituted cyclopentadienyl ligand (Cp-Ar3). The Dy(III)-metallocene weakly couples via K2Cl4 and exhibits slow relaxation of magnetization below 14.5 K under zero applied dc field through KD3 energy levels with an energy barrier of 136.9/133.7 cm(-1) at the Dy sites. The coordination of two chloride ions at each Dy centre leads to geometrical distortion and reduction of the single-ion axial anisotropy energy barrier.
DALTON TRANSACTIONS
(2023)
Article
Physics, Multidisciplinary
Aleksei Ivanov, Christoph Sunderhauf, Nicole Holzmann, Tom Ellaby, Rachel N. Kerber, Glenn Jones, Joan Camps
Summary: In this work, a quantum algorithm based on sparse qubitization approach is presented for ground-state energy calculations of periodic solids on error-corrected quantum computers. It is shown that the use of Wannier functions reduces computational resources compared to Bloch functions due to lower Hamiltonian norm and exploitability of translational symmetry. The resource requirements of the algorithm are estimated for industrially relevant transition metal oxides and found to be substantial in terms of gates and qubits.
PHYSICAL REVIEW RESEARCH
(2023)
