Article
Chemistry, Inorganic & Nuclear
Kgauhelo Mentoor, Linette Twigge, J. W. Hans Niemantsverdriet, Jannie C. Swarts, Elizabeth Erasmus
Summary: The treatment of silica nanopowders resulted in the generation of supported Lewis acids and Lewis bases, forming a series of frustrated Lewis pairs (FLPs) that successfully captured CO2 and converted it to formic acid. Spectroscopic characterization of the synthesized products was performed to analyze the reaction outcomes.
INORGANIC CHEMISTRY
(2021)
Article
Chemistry, Physical
Rafal Kusy, Marcin Lindner, Jakub Wagner, Karol Grela
Summary: In this study, (E)-selective semihydrogenation of alkynes using an iridium complex and an unsymmetrical phosphine ligand was achieved with formic acid as a hydrogen donor. The stereoselectivity of the reaction was controlled by the ligand-to-metal ratio, with a 1:2 ratio giving exclusively (E)-alkene. The catalytic system exhibited high chemoselectivity and exceptional stereoselectivity, and was effective for a wide range of substrates. The difference in catalytic activity between unsymmetrical and symmetrical ferrocene-based ligands was attributed to divergent coordination and steric hindrance.
Article
Chemistry, Inorganic & Nuclear
Kyle D. Spielvogel, Nathan C. Stumme, Taylor Fetrow, Li Wang, Javier A. Luna, Jason M. Keith, Scott K. Shaw, Scott R. Daly
Summary: Metal-ligand cooperativity (MLC) is a powerful approach to achieve new chemical transformations with metal complexes by leveraging reactive ligands. However, quantifying the effect of ligand modifications on MLC binding strength remains a challenge. In this study, cyclic voltammetry (CV) was used to quantify the differences in MLC binding strength in a series of square-pyramidal Ru complexes.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Inorganic & Nuclear
David Decker, Zhihong Wei, Jabor Rabeah, Hans-Joachim Drexler, Angelika Brueckner, Haijun Jiao, Torsten Beweries
Summary: In this study, a Co(ii) PNNH pincer catalyst system was applied for the highly E-selective transfer semihydrogenation of internal diaryl alkynes. The catalyst system showed high activity, short reaction times, and operated under mild conditions.
INORGANIC CHEMISTRY FRONTIERS
(2022)
Article
Chemistry, Physical
Yong Cheng, Dan Wang, Xiuxiu Wang, Ying-Hua Zhou
Summary: In this study, a high-efficiency tandem catalyst CuO-Ru-0.3@Co3O4 was synthesized for the hydrolytic dehydrogenation of ammonia borane (AB) and the hydrogenation of nitrobenzenes (NBs). The catalyst showed high activity and good cyclic stability.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2022)
Article
Chemistry, Physical
Yi Wang, Xiang Liu
Summary: The research team enhanced the catalytic activity of CoFe2O4 by reducing it, leading to superior performance in the hydrolytic dehydrogenation of ammonia borane. The reduced CoFe2O4 showed increased catalytic activity in the presence of NaOH, and could be reused multiple times without any loss of catalytic activity.
JOURNAL OF MOLECULAR LIQUIDS
(2021)
Article
Chemistry, Physical
Zheng-Wang Qu, Hui Zhu, Rainer Streubel, Stefan Grimme
Summary: Extensive DFT calculations demonstrate that BH3NH3 can transfer hydrogen to CO2 as separated hydride and proton rather than HCO3- in water, with a barrier energy of 25.9 kcal mol(-1). Subsequently, borate anions facilitate faster hydrogen transfer to electrophilic CO2, protic H2O, or HCO2H, resulting in competitive formate production and H-2 release.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Inorganic & Nuclear
Ignacio Chamorro-Mena, Noemi Linares, Javier Garcia-Martinez
Summary: This study describes the optimization of Cu2O/CuO heterostructures for enhanced (photo)catalytic performance. The evaluation of catalysts with different Cu2O/CuO molar ratios revealed that a ratio of 0.15 resulted in significantly higher rate constants under blue-LED light. Furthermore, this photocatalyst exhibited good stability and excellent chemoselectivity in the presence of other functionalities.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Inorganic & Nuclear
Ignacio Chamorro-Mena, Noemi Linares, Javier Garcia-Martinez
Summary: This study explores the optimization of Cu2O/CuO heterostructures for enhancing their (photo)catalytic performance. By evaluating catalysts with different Cu2O/CuO molar ratios, the researchers found that a ratio of 0.15 resulted in significantly higher reaction rate constants under blue LED light compared to lower (0.01) or higher (0.42) ratios. The photocatalyst also demonstrated good stability (>70% after 5 cycles) and excellent chemoselectivity in the selective reduction of the nitro group in the presence of other functionalities, such as -COOH, -CONH2, and -OH.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Inorganic & Nuclear
Orhi Esarte Palomero, Richard A. Jones
Summary: The synthesis of novel ferrocene tethered boramidinate frustrated Lewis pairs (FLPs) capable of sequentially capturing small molecules is reported. The reactivity of the boramidinate moieties can be tuned by altering the substituents and borane used in the reduction. Independent small molecule capture by each FLP has been demonstrated, allowing for sequential capture of different gaseous small molecules.
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Physical
Dapeng Wu, Jing Guo, Hongju Wang, Xilin Zhang, Yonggang Yang, Can Yang, Zhiyong Gao, Zichun Wang, Kai Jiang
Summary: Boron and nitrogen co-doped titanium dioxide nanosheets with high surface area were synthesized using ammonia borane as the green regent, achieving excellent performance in photocatalytic reduction of carbon dioxide. Transient optical measurements indicated that the samples with rich defect states and elevated conduction band position could enhance light harvesting efficiency. It was suggested that Lewis acid-base pairs on the material could substantially increase the activation of inert CO2, facilitating its photoreduction with hydrogen.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2021)
Article
Multidisciplinary Sciences
Yuzhu Zhou, Quan Zhou, Hengjie Liu, Wenjie Xu, Zhouxin Wang, Sicong Qiao, Honghe Ding, Dongliang Chen, Junfa Zhu, Zeming Qi, Xiaojun Wu, Qun He, Li Song
Summary: Developing efficient electrocatalysts for selective CO2 conversion is important. In this study, the authors demonstrate that a Ni single-atom catalyst coordinated with pyrrolic nitrogen and pyridinic nitrogen efficiently converts CO2 to CO. The catalyst shows high CO partial current density and turnover frequency, as well as excellent Faradaic efficiency of CO. The study also provides insights into the origin of the catalyst's catalytic activity.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Bowen Li, Jianzhong Chen, Dan Liu, Ilya D. Gridnev, Wanbin Zhang
Summary: In this study, an environmentally friendly and efficient method for the synthesis of chiral hydroxylamines through nickel-catalysed asymmetric hydrogenation was reported.
Article
Chemistry, Multidisciplinary
Qin Zhu, Shuoqi Zhang, Jing Ma, Jun Zhu, Shuhua Li, Guixiang Zeng
Summary: The transfer hydrogenation of azobenzene with ammonia borane mediated by pincer bismuth complex 1 was studied using density functional theory calculations. The study revealed an unusual metal-ligand cooperation mechanism involving the saturation/regeneration of the C=N functional group on the pincer ligand. The reaction proceeds through the hydrogenation of the C=N bond, followed by the conversion of 3(CN) to a Bi-H intermediate, and eventually results in the production of N,N'-diphenylhydrazine and regeneration of the catalyst. The substitution of the phenyl group with a tert-butyl group on the pincer ligand improves the catalyst's performance.
CHEMISTRY-AN ASIAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Rimeh Mighri, Kevin Turani-I-Belloto, Umit B. Demirci, Johan G. Alauzun
Summary: Carbon-doped boron nitride (BN/C) was synthesized by pyrolysis of a nanostructured mixture of alkyl amine borane adduct and ammonia borane at 1100 C-?. The use of alkyl amine borane adduct as a soft template enabled the formation of nanospheres. The resulting BN/C materials exhibited a microporous structure with interconnected pores in the nanometer range, a high specific surface area, and excellent gas sorption properties.
Article
Materials Science, Multidisciplinary
Subrata Santra, Arpan Ghosh, Arun Mondal, Sk. Mursed Ali, Dishan Das, Kishor Sarkar, Lisa Roy, Mijanur Rahaman Molla
Summary: This study focused on the controlled synthesis of polyurethanes with recycled plastic waste to investigate the impact of polymer molar mass on the thermodynamics of self-assembly. The stable micellar nanostructure with environment-specific surface charge modulation and controlled guest release can significantly contribute to the development of robust chemotherapeutics.
ACS APPLIED POLYMER MATERIALS
(2022)
Article
Chemistry, Organic
Subhajit Chakraborty, Rakesh Mondal, Subhasree Pal, Amit Kumar Guin, Lisa Roy, Nanda D. Paul
Summary: We developed a sustainable and eco-friendly method for selective N-alkylation of various amines using a well-defined Zn(II)-catalyst with a tridentate arylazo scaffold. A total of 57 N-alkylated amines were synthesized with good to excellent yields, including 17 new examples. The Zn(II)-catalyst demonstrated wide functional group tolerance and compatibility for the synthesis of dialkylated amines, providing high yields for the precursors of tripelennamine and thonzonium bromide drugs.
JOURNAL OF ORGANIC CHEMISTRY
(2023)
Article
Chemistry, Physical
Souvik Misra, Pijush Singh, Ajeet Kumar Singh, Lisa Roy, Soumen Kuila, Sukantha Dey, Ajit K. Mahapatra, Jayanta Nanda
Summary: Supramolecular chirality of self-assembled biomaterials can be tuned by altering the methylene units in achiral amino acids, as demonstrated in this study. The inversion of supramolecular helicity was extensively studied through CD spectroscopy and morphological analysis. Density functional theory study revealed that the methylene spacers influence the orientation of n-n stacking interactions of naphthalimide units in the self-assembled structure, which regulates the helicity.
JOURNAL OF PHYSICAL CHEMISTRY B
(2022)
Article
Chemistry, Organic
Samrat Kundu, Lisa Roy, Modhu Sudan Maji
Summary: In this study, a unique carbazole-based organophotocatalyst, benzoperylenocarbazole (BPC), is reported as a potent organo-photoreductant. BPC exhibits a lower excited state oxidation potential and a reasonable excited state lifetime, making it an effective photosensitizer. With low catalyst loading and irradiation of blue light, a variety of vicinal diols and diamines can be synthesized in excellent yields through reductive coupling of carbonyls and imines. DFT calculations provide insight into the electronic structure of BPC.
Article
Chemistry, Organic
Sudhir Kumar Hota, Satya Prakash Panda, Sanju Das, Sanat Kumar Mahapatra, Lisa Roy, Suman De Sarkar, Sandip Murarka
Summary: We proposed a novel disconnection approach to synthesize fused tetrahydroquinolines through a visible light-mediated radical (4 + 2) annulation reaction between alkyl N-(acyloxy)-phthalimides and N-substituted maleimides using DIPEA as an additive. The reaction involves a photoactivated electron donor-acceptor complex between alkyl NHPI esters and DIPEA, and regioselective tetrahydroquinolines were obtained. This metal-and catalyst-free methodology exhibits a wide scope, good functional group tolerance, and detailed mechanistic investigations were performed.
JOURNAL OF ORGANIC CHEMISTRY
(2023)
Article
Chemistry, Physical
Soumen Kuila, Ajeet Kumar Singh, Akash Shrivastava, Sukantha Dey, Tukai Singha, Lisa Roy, Biswarup Satpati, Jayanta Nanda
Summary: In this work, three hybrid dipeptides, consisting of a beta-amino acid and an alpha-amino acid conjugated with 1,8-naphthalimide (NMI), were designed, synthesized, and purified. The effect of molecular chirality on supramolecular assembly was studied by varying the chirality of the alpha-amino acid. Self-assembly and gelation of the NMI conjugates were investigated in mixed solvent systems. The results showed that the chirality of the alpha-amino acid influenced the formation of self-supporting gels and chiral assembled structures.
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Article
Chemistry, Multidisciplinary
Payel Khanra, Ajeet Kumar Singh, Lisa Roy, Anindita Das
Summary: This study explores the complex kinetic and thermodynamic pathways involved in the supramolecular copolymerization of two chiral dipolar NMI building blocks. O-NMI forms distinct nanotapes and helical fibers, while S-NMI only forms stable spherical assemblies. The study also shows that O-NMI and S-NMI can evolve into star-shaped copolymers with controllable length.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Organic
Satya Prakash Panda, Sudhir Kumar Hota, Rupashri Dash, Lisa Roy, Sandip Murarka
Summary: In this study, a transition-metal-free NaI/PPh3-mediated direct C-H alkylation of azauracils using N-(acyloxy)-pthalimides (NHPIs) as alkyl surrogates was developed under visible light irradiation. Mechanistic studies revealed the formation of a photoactivated electron donor-acceptor (EDA) complex between NaI/PPh3, TMEDA, and alkyl NHPI ester, and the crucial role of TMEDA in enhancing the activity of the photoredox system. This reaction demonstrated a wide scope, scalability, and good functional group tolerance, allowing for the alkylation of various azauracils with primary, secondary, and tertiary NHPI esters under mild conditions to afford the desired products in good to excellent yields.
Article
Chemistry, Organic
Satabdi Bera, Aniruddha Biswas, Juthi Pal, Lisa Roy, Supriya Mondal, Rajarshi Samanta
Summary: A Pd(II)-catalyzed oxidative naphthylation of unmasked 2-pyridone derivatives using a twofold internal alkyne as coupling partner is described. The reaction involves N-H/C-H activation and leads to polyarylated N-naphthyl 2-pyridones. Mechanistic studies suggest a plausible mechanism based on N-H/C-H activation. The photophysical properties of the N-naphthyl 2-pyridone derivatives are explored and show promising results.
Article
Chemistry, Inorganic & Nuclear
Ajeet Kumar Singh, Lisa Roy
Summary: This study investigates the catalytic activity of two nickel and copper complexes in the water splitting reaction through density functional theory. The nickel complexes exhibit complex borderline chemistry, with competition between water oxidation and molecular species degradation, while the copper complexes display robust and efficient molecular water oxidation behavior. The disparity is primarily attributed to the reversible O-O bond formation in nickel complexes, which provide a platform for direct attack and ligand deactivation, whereas the copper complexes exhibit radical character on the hydroxyl ligand, accelerating O-O interaction and leading to predominant homogeneous water oxidation under all conditions.
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Organic
Satabdi Bera, Aniruddha Biswas, Juthi Pal, Lisa Roy, Supriya Mondal, Rajarshi Samanta
Summary: In this paper, a Pd(II)-catalyzed oxidative naphthylation of unmasked 2-pyridone derivatives using a twofold internal alkyne as a coupling partner is described. The reaction proceeds through N-H/C-H activation to provide polyarylated N-naphthyl 2-pyridones. Mechanistic studies and DFT calculations suggest a plausible mechanism based on N-H/C-H activation. The photophysical properties of the N-naphthyl 2-pyridone derivatives were also studied.
Article
Chemistry, Multidisciplinary
Saurajit Ghosh, Himanshi Bhambri, Ajeet Kumar Singh, Sanjay K. Mandal, Lisa Roy, Partha Sarathi Addy
Summary: In this study, a convenient two-step synthesis method was used to obtain luminescent molecules, and a comparative study was conducted to demonstrate the importance of weak π-π interactions in aggregation-induced emission (AIE) and solid-state mechanochromic luminescence. The most fascinating finding is the observation of switchable fluorescent dark and bright states of the solid AIEgen. Furthermore, the AIEgen was demonstrated to be useful for detecting volatile organic compounds.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Organic
Prahallad Meher, Satya Prakash Panda, Sanat Kumar Mahapatra, Karan Ramdas Thombare, Lisa Roy, Sandip Murarka
Summary: We report a photoredox system that can form a self-assembled complex and activate diaryliodonium reagents for arylation of heterocycles under mild conditions.
Article
Chemistry, Multidisciplinary
Rupkumar Khuntia, Sanat Kumar Mahapatra, Lisa Roy, Subhas Chandra Pan
Summary: In this study, a new method has been developed to rapidly synthesize structurally diverse and complex molecules from easily available starting materials through catalytic reactions. Through the analysis of the mechanistic intricacies, the roles of chiral and Lewis base catalysts in the reaction have been investigated.
Article
Chemistry, Physical
Souvik Misra, Pijush Singh, Ajeet Kumar Singh, Lisa Roy, Soumen Kuila, Sukantha Dey, Ajit K. Mahapatra, Jayanta Nanda
Summary: This study demonstrates a new approach to tune the supramolecular chirality of self-assembled biomaterials by altering the methylene units in the achiral amino acids of naphthalimide-capped peptide-based gel nanofibers. The research provides a detailed analysis of the inversion of supramolecular helicity and its underlying mechanisms using CD spectroscopy and morphological analysis.
JOURNAL OF PHYSICAL CHEMISTRY B
(2022)
