Article
Biochemistry & Molecular Biology
Homa Mousavi, Maria Eugenia Garcia-Rubino, Duane Choquesillo-Lazarte, Alfonso Castineiras, Luis Lezama, Antonio Frontera, Juan Niclos-Gutierrez
Summary: The reaction in water leads to the formation of a ternary copper compound, which has been characterized using various physical methods and theoretical calculations. The compound exhibits a specific molecular structure and dimensionality.
Article
Multidisciplinary Sciences
Jian-Hua Wang, Yu-Liang Tang, Zhou Gong, Rohit Jain, Fan Xiao, Yu Zhou, Dan Tan, Qiang Li, Niu Huang, Shu-Qun Liu, Keqiong Ye, Chun Tang, Meng-Qiu Dong, Xiaoguang Lei
Summary: This study develops a new cross-linker called DOPA2 for rapid chemical cross-linking mass spectrometry analysis, which captures the conformations of protein unfolding intermediates. Compared with traditional cross-linkers, DOPA2 shows unique advantages in terms of speed, structural agreement, and adaptability. Additionally, this method allows for time-course analysis of protein conformational changes during denaturant-induced unfolding.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Physical
Snehasish Thakur, Antonio Frontera, Shouvik Chattopadhyay
Summary: Two polymeric [VO3](n)(n-) metavanadate chain complexes have been synthesized and characterized in this study, with complex 2 having a unique crystal lattice structure. Strong N-H···O hydrogen bonding interactions were observed in both complexes, with complex 2 also exhibiting phenoxazinone synthase-like activity.
JOURNAL OF MOLECULAR STRUCTURE
(2021)
Article
Chemistry, Physical
Pratidnya Shendge, Shailza Sharma, Minati Baral, B. K. Kanungo
Summary: The study focused on a catechol-thiosemicarbazone based tridentate NOS chelator and its octahedral pincer complexes with trivalent aluminum, chromium, iron and gallium. The coordination of metal-ligands in the complexes resulted in two planar pincer type arrangements with meridional configuration, maintaining a perpendicular profile. Quantum mechanical studies at DFT level were conducted to explore the structure, reactivity and spectroscopic properties of the compounds. The fluorescence behavior of the chelator was found to exhibit a significant alteration in the emission spectrum in the presence of zinc ion, indicating a ten-fold enhancement.
JOURNAL OF MOLECULAR STRUCTURE
(2021)
Article
Chemistry, Organic
Qian Tao, Ya-Nan Li, Wen-Jun Tang, Peng-Yu Liu, Fang Yu, Yu-Peng He
Summary: The direct di-ortho-arylation of substituted phenylalanines has been achieved via methoxyiminoacyl (MIA)-mediated Pd-catalyzed C-H functionalization, providing a diverse array of phenylalanine derivatives with good to high efficiency. Computational results showed a bimetallic interaction between Pd(IV)-Ag(I) through localized orbital, which favored the reductive elimination step of the arylation process.
TETRAHEDRON LETTERS
(2021)
Article
Multidisciplinary Sciences
Abhay K. Patel, Neetu Patel, R. N. Patel, Rajendra N. Jadeja
Summary: A series of copper(II) mu-alkoxo-mu-carboxylato complexes were synthesized and characterized. These complexes were designed as structural and functional models of catechol oxidase enzymes. The catecholase activity and superoxide dismutase activity of the complexes were evaluated.
Article
Engineering, Electrical & Electronic
Abhishek Mishra, Atanu Betal, Ravi Kumar, Prem Lama, Satyajit Sahu, Ramesh K. Metre
Summary: Compound 1, synthesized from the reaction of 2-phenylazophenyl tin chloride and sodium hydroxide, exhibits various supramolecular structures in its crystal lattice and demonstrates NDR behavior in I-V characteristic studies.
ACS APPLIED ELECTRONIC MATERIALS
(2021)
Article
Chemistry, Inorganic & Nuclear
Jiurong Hu, Wenjie Dong, Jihong Wang
Summary: This study investigates the reaction of complex (p-cymene)Ru(S2C2B10H10) with HC=CC(OH)(CH3)2, resulting in the formation of isomers and corresponding complexes. The structures of these complexes were analyzed by various characterization methods. Furthermore, the formation mechanisms of these complexes were studied.
INORGANIC CHEMISTRY COMMUNICATIONS
(2022)
Article
Chemistry, Physical
Svetlana A. Katkova, Alexander S. Mikherdov, Elina Sokolova, Alexander S. Novikov, Galina L. Starova, Mikhail A. Kinzhalov
Summary: A series of platinum(II) isocyanide complexes were synthesized and characterized in this study. Noncovalent interactions between the isocyanide group and platinum atom were identified using X-ray diffraction analysis and confirmed by DFT calculations and analysis of the electron density distribution. The contacts between the isocyanide moiety and various metal centers were also verified.
JOURNAL OF MOLECULAR STRUCTURE
(2022)
Article
Chemistry, Multidisciplinary
Kousik Ghosh, Antonio Frontera, Shouvik Chattopadhyay
Summary: A heteronuclear cobalt/potassium complex has been synthesized and characterized, forming discrete I-3(-) dimers in the solid state with anti-electrostatic halogen-halogen interaction, which is energetically favorable in solution.
Article
Chemistry, Inorganic & Nuclear
Yufang Xie, Qiyi Miao, Wenhao Deng, Yilei Lu, Yinuo Yang, Xiaohui Chen, Rong-Zhen Liao, Shengfa Ye, Chen-Ho Tung, Wenguang Wang
Summary: A diamido-bridged dicobalt complex supported by a diamidonaphthalene ligand, Cp*Co2(2)(mu-1,8-C10H8(NH)(2)) (1), was synthesized and its reactivity towards redox transformations of the Co2N2 core was investigated. It was found that the Co(II)-Co(II) bond can be protonated, resulting in the formation of a bridging hydride [1H](+). The diamidonaphthalene ligand stabilizes the Co(II)Co(III) mixed-valent state (1(+)), which can bind CO to form [1-CO](+). Surprisingly, the mixed-valent complex also activates H2O to give a Co(III)Co(III) hydroxy complex [1-OH](+), accompanied by the release of H2.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Physical
Konstantin V. Bozhenko, Andrey N. Utenyshev, Alyona A. Starikova, Anatoly V. Metelitsa, Andrey G. Starikov, Vladimir I. Minkin, Sergey M. Aldoshin
Summary: A DFT study revealed characteristic structural features of monomeric fragments of 1D-polymer chains consisting of cobalt complexes with TPDO ligands. The elongation of donor-acceptor Co-N bonds can be attributed to the bulky tert-butyl groups in TPDO and repulsive interactions between N-donor ligands' hydrogen atoms and oxygen diketonate atoms. The unusual Co-O distances in Co(acac)2TPDO2 may be caused by the possible presence of the low-spin doublet state at higher temperature.
CHEMICAL PHYSICS LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Prasanta Kumar Bhaumik, Rosa M. Gomila, Antonio Frontera, Samia Benmansour, Carlos J. Gomez-Garcia, Shouvik Chattopadhyay
Summary: The hooked cross-shaped anion participates in strong CH center dot center dot center dot[Cu(N-3)(4)](2-) interactions in the pentanuclear hetero-metallic copper(II)-sodium complex. DFT calculations, MEP analysis, and NCI plot index analysis were used to analyze and characterize these interactions. Cation-pi interactions between the pentacoordinated Na-atom and the aromatic ring of the Schiff base ligand were described and compared with existing X-ray structures.
NEW JOURNAL OF CHEMISTRY
(2022)
Article
Chemistry, Physical
Huifang Xing, Qiyu Meng, Liangrong Yang, Congmei Chen, Huizhou Liu
Summary: The study employed the PWPB95-D3 double-hybrid functional with precise dispersion description to calculate the thermodynamic properties of complexes formed by 1,3-Diisopropoxycalix[4]arenecrown-6 (BPC6) and alkali metal cations (Li', Na', K', Rb', and Cs') in gas phase and various solutions. Symmetry-adapted perturbation theory (SAPT) and IGM based on Hirshfeld partition of molecular density (IGMH) were used for the first time to analyze the interactions of these complexes. The results showed that the electrostatic energy dominated the interaction energy in the gas phase, while the dielectric screen of solvents and the presence of protic solvents influenced the binding Gibbs free energy. The dispersion interaction also played a significant role in the complexation with large cations in solvents.
JOURNAL OF MOLECULAR LIQUIDS
(2023)
Article
Chemistry, Physical
Takanori Iwasaki, Wataru Ishiga, Shrinwantu Pal, Kyoko Nozaki, Nobuaki Kambe
Summary: This study reports the mechanistic investigation of the Rh-catalyzed cross-coupling reaction between vinylic ethers and aryl Grignard reagents. The presence of olefinic ligands significantly affects the catalytic activity of Rh precatalysts. Computational studies reveal that the reaction proceeds through Mg cation-assisted insertion/anti-beta-oxygen elimination, with the Mg countercation coordinating to the ethereal oxygen atom in the transition state.
Article
Chemistry, Inorganic & Nuclear
Jose Luis Serrano, Sujeet Gaware, Jose Antonio Perez, Jose Perez, Pedro Lozano, Santosh Kori, Rambabu Dandela, Yogesh S. Sanghvi, Anant R. Kapdi
Summary: Commercially available Quadrol has been used as a neutral hydrophilic ligand in the synthesis and characterization of water soluble palladium(ii) complexes. These complexes show high solubility in water and are effective catalysts for the synthesis of functionalized nucleoside analogues at room temperature.
DALTON TRANSACTIONS
(2022)
Review
Chemistry, Physical
Rosario M. P. Colodrero, Pascual Olivera-Pastor, Aurelio Cabeza, Montse Bazaga-Garcia
Summary: This article reviews the progress in metal phosphate structural chemistry, with a focus on proton conductivity properties and applications. It discusses the relationship between structure and property, the origins of conducting properties, and the classification of metal phosphates. It also emphasizes the outstanding properties of certain materials for their application in fuel cells.
Article
Nanoscience & Nanotechnology
Alvaro Vilchez-Cozar, Eirini Armakola, Maria Gjika, Aurelia Visa, Montse Bazaga-Garcia, Pascual Olivera-Pastor, Duane Choquesillo-Lazarte, David Marrero-Lopez, Aurelio Cabeza, Rosario M. P. Colodrero, Konstantinos D. Demadis
Summary: This article focuses on the synthesis and characterization of one-dimensional imidazole-containing etidronates and their solid solutions, and evaluates their properties as multipurpose materials for energy conversion processes. The study finds that one of the catalysts exhibits the best catalytic performance in the oxygen reduction reaction and shows potential applications in overall water splitting and zinc-air batteries.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Multidisciplinary
Jose Luis Serrano
Summary: Modification of unprotected nucleosides has been attracting continuous interest, with Pd-catalyzed cross-coupling reactions playing an important role, while the team's synthesis of water-soluble Pd-imidates complexes has yielded interesting results.
Article
Construction & Building Technology
Isabel M. R. Bernal, Miguel A. G. Aranda, Isabel Santacruz, Angeles G. De la Torre, Ana Cuesta
Summary: Limestone Calcined Clay Cements (LC3) is a material that can achieve up to 40% CO2 emissions savings and has competitive mechanical performances after one week. However, the initial reactivity of LC3 needs improvement. In this study, a multitechnique approach was used to understand the early age reactivities of LC3, and it was found that the Al-O interatomic correlation position and intensity in the synchrotron pair distribution function (sPDF) could be a good descriptor for early age reactivity. The results were complemented by Al-27 MAS-NMR studies, which showed that the rate of pozzolanic reaction at early ages is influenced by the particle size, surface area, and local disorder of metakaolin.
JOURNAL OF SUSTAINABLE CEMENT-BASED MATERIALS
(2023)
Article
Construction & Building Technology
Cinthya Redondo-Soto, Alejandro Morales-Cantero, Ana Cuesta, Isabel Santacruz, Daniela Gastaldi, Fulvio Canonico, Miguel A. G. Aranda
Summary: LC3 is a type of concrete material that can reduce the CO2 footprint by 40%. It has high content of belite and exhibits excellent durability performance.
CEMENT AND CONCRETE RESEARCH
(2023)
Article
Chemistry, Multidisciplinary
Jan Fassbender, Niklas Volk, Antonio Garcia Alcaraz, Selvakumar Balasubramaniam, Arturo Espinosa Ferao, Rainer Streubel
Summary: After more than 160 years of research, scientists have finally synthesized an oxaphosphirane, a phosphorus analogue derivative of oxirane. Reactions with various compounds have shown that increasing the coordination number at phosphorus causes destabilization, which supports previous findings. Theoretical studies have provided insights into ring strain energy, ring/ring interconversion, and oxidation pathways.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Applied
Miriam Mas-Montoya, Antonio Garcia Alcaraz, Arturo Espinosa Ferao, Delia Bautista, David Curiel
Summary: Two four-coordinate boron complexes, compounds 5 and 7, were synthesized using similar benzophenanthridine-based ligands but with different conformational constraints, and their optical properties were investigated. Ligand design considering expansion of pi-conjugation and structural desymmetrization was found to be effective in obtaining fluorophores with large Stokes shifts. The incorporation of a conformationally free substructure increased the geometry relaxation in the first excited state (S1) and the ground state (S0), resulting in enhanced Stokes shift. Solvatochromism showed divergent behavior in emission and absorption spectra, attributed to the different stabilization degrees of the S0 and S1 states compared to the Franck-Condon states. Aggregation-induced emission (AIE) was observed in molecule 7, which was attributed to blocking the motion of peripheral rotor based on solid state packing determined by X-ray diffraction.
Article
Construction & Building Technology
Raquel Perez-Bravo, Alejandro Morales-Cantero, Ana Cuesta, Miguel A. G. Aranda, Isabel Santacruz, Angeles G. de la Torre
Summary: The effect of TIPA and CaCl2 on early hydration of B-BYF cement was investigated. TIPA reduced paste viscosity during the initial minutes but promoted the formation of AFt after the induction period, resulting in a 169% increase in 1-day mechanical strengths. CaCl2 accelerated the dissolution rate of ye'elimite, leading to the early precipitation of ettringite and a 181% improvement in 1-day mechanical strengths. The reactivity of ferrite and alpha'H-belite was not affected by either admixture during the first 24 hours of hydration.
CONSTRUCTION AND BUILDING MATERIALS
(2023)
Article
Multidisciplinary Sciences
Shiva Shirani, Ana Cuesta, Alejandro Morales-Cantero, Isabel Santacruz, Ana Diaz, Pavel Trtik, Mirko Holler, Alexander Rack, Bratislav Lukic, Emmanuel Brun, Ines R. Salcedo, Miguel A. G. Aranda
Summary: Despite decades of research, our understanding of cement dissolution and precipitation processes at early stages is still limited due to the lack of suitable imaging methods. In this study, near-field ptychographic nanotomography was used to visualize the hydration of commercial Portland cement in a thick capillary. The results show the formation of a porous C-S-H gel shell with a thickness of 500 nm after 19 hours, covering all the alite grains with a water gap. The dissolution rate of smaller alite grains was found to be approximately four times faster than that of larger grains in the deceleration stage. The study also mapped out the development of etch pits and measured particle size distributions over time. This work lays the foundation for mechanistic studies of dissolution-precipitation processes in cement using advanced nanoimaging techniques.
NATURE COMMUNICATIONS
(2023)
Review
Chemistry, Physical
Ana Cuesta, Alejandro Morales-Cantero, Angeles G. G. De la Torre, Miguel A. G. Aranda
Summary: Reducing the CO2 emissions from cement production is important, and this can be achieved by using supplementary cementitious materials instead of Portland clinker. However, this can lead to lower early-age mechanical strengths due to slow pozzolanic reactions. To address this issue, accelerator admixtures can be used. Calcium silicate hydrate nucleation seeding shows promise in accelerating cement reactions without compromising late strength and durability performances. Other benefits include low temperature concreting, precasting, and shotconcrete.
Article
Chemistry, Multidisciplinary
Sujeet Gaware, Santosh Kori, Jose Luis Serrano, Rambabu Dandela, Stephen Hilton, Yogesh S. Sanghvi, Anant R. Kapdi
Summary: A rapid flow-based cross-coupling synthesis protocol was developed for C5-pyrimidine substituted nucleosides, allowing for facile access to multiple nucleoside analogues in a few minutes compared to conventional batch chemistry.
JOURNAL OF FLOW CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Arturo Espinosa Ferao, Alicia Rey Planells
Summary: Accurate ring strain energy (RSE) values were reported for sixty-six parent pnictogeniranes with two other identical p-block elements, El(2)Pn. A decrease in RSE was found to be correlated with an increase in the p character of the AO used in endocyclic bonds, particularly in groups 15 and 16. The higher -NICS(1) values also parallel the presence of atom-centred diatropic currents, mostly arising from the lone pairs. Only in the case of pnictogenaditrieliranes Tr(2)Pn (Tr=B, Al, Ga), the decrease of -NICS(1) is related to lower Huckel-type 2 pi-electron aromaticity in group 13.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Arturo Espinosa Ferao
Summary: This study explores the deoxygenation of parent and substituted oxiranes using lambda(3)sigma(3)-phosphorus reagents and reveals mechanistic aspects, as well as regio- and stereochemical consequences. It shows that attack to a ring C atom is usually preferred over direct P-to-O attack for one-step deoxygenation. The study also investigates the use of heavier derivatives AsMe3 and SbMe3 as oxirane deoxygenating reagents. The thermodynamic tendencies of lambda(3)sigma(3)-phosphorus reagents to act as oxygen or carbene acceptors are theoretically studied.
Article
Chemistry, Inorganic & Nuclear
Arif Ali Khan, Tim Kalisch, Arturo Espinosa Ferao, Rainer Streubel
Summary: The reaction of a transient terminal phosphinidene complex with triethylamine resulted in the formation of an sp(3) C-H insertion product, as confirmed by P-31 NMR spectroscopy. The product was isolated as a semi-solid compound. However, after 24 hours of reaction, a primary phosphane complex was obtained. The compounds were characterized using NMR spectroscopy and mass spectrometry. Formation of the final products is explained by a mechanistic proposal based on DFT calculations.
DALTON TRANSACTIONS
(2023)
