Article
Chemistry, Multidisciplinary
Ziyan Zhang, Nikita Kvasovs, Anastasiia Dubrovina, Vladimir Gevorgyan
Summary: This method utilizes visible light-induced and Bronsted acid-assisted generation of hybrid palladium C(sp(3))-centered radical intermediate, enabling efficient transformation of a wide range of vinyl arenes, heteroarenes, and diazo compounds.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Xue-Gong Jia, Qi-Wei Yao, Xing-Zhong Shu
Summary: This study presents a new method for the preparation of enantioenriched heterocycles through N-cyclization-alkylation reaction, addressing a long-standing challenge in the synthetic community and achieving highly enantioenriched pyrrolines under mild conditions.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Xue-Gong Jia, Qi-Wei Yao, Xing-Zhong Shu
Summary: This study reports a novel N-cyclization-alkylation reaction, showcasing the potential of heterocyclization for accessing enantioenriched cyclic architectures and solving a long-standing challenge in synthetic chemistry.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Review
Chemistry, Applied
Antonio Mourino
Summary: 1α,25-dihydroxyvitamin D3 (1,25D3), the active form of vitamin D3, plays a crucial role in regulating mineral homeostasis, cell growth, and immune responses. However, its clinical applications are limited due to hypercalcemic effects. Therefore, there has been a focus on synthesizing highly active and non-calcemic analogs of 1,25D3 for the treatment of hyperproliferative diseases.
ADVANCED SYNTHESIS & CATALYSIS
(2023)
Article
Engineering, Environmental
Goutham Rangarajan, Ramin Farnood
Summary: This study reports the synthesis of H2SO4-modified biochars as solid-acid catalysts to activate H2O2 under visible light radiation. Results showed that under photo-Fenton conditions, SBC500 can achieve complete MO removal and a TOC reduction.
JOURNAL OF HAZARDOUS MATERIALS
(2022)
Article
Chemistry, Physical
Jisoo Kim, Jeongah Lim, Ji Dang Kim, Myong Yong Choi, Sunwoo Lee, Hyun Chul Choi
Summary: Pd-graphene quantum dot (Pd-GQD) catalysts were prepared and characterized for their properties and catalytic activity. The study found that Pd-GQD catalyst exhibited higher catalytic activity in the Heck and decarboxylative cross-coupling reactions, and GQD was an effective support material for preparing new catalysts.
Article
Chemistry, Physical
Fukun Lei, Yu Jiang, Yangsheng Ma, Deng Xiang, Jie Wang, Zhanglong Guo, Tao Dai, Maofei Ran
Summary: The electron transfer effects of different nitrogen functional groups on Pd/N-CNT catalysts for the Heck reaction were investigated. Pd/N-CNTs were synthesized to control the percentage of different N species. The synthesis temperature significantly affected the structure of Pd/N-CNT, and the Pd-graphitic N complex was identified as the active-site in the Heck reaction.
CHEMICAL PHYSICS LETTERS
(2023)
Article
Chemistry, Physical
Masoumeh Beiranvand, Davood Habibi
Summary: In this study, the mesoporous silica SBA-15 (SBA) was modified by a tetra-urea (TU) ligand to prepare the SBA@TU@Pd(0) nano-structured reduced catalyst. The catalytic activity of SBA@TU@Pd(0) was successfully studied in the Mizoroki-Heck and Suzuki-Miyaura cross-coupling reactions, showing short reaction times and high yields. The non-reduced nano-catalyst SBA@TU@Pd(II) also exhibited similar reaction yields but longer reaction times.
JOURNAL OF MOLECULAR STRUCTURE
(2023)
Article
Chemistry, Multidisciplinary
Alexey S. Galushko, Daniil A. Boiko, Evgeniy O. Pentsak, Dmitry B. Eremin, Valentine P. Ananikov
Summary: A method for characterizing supported catalysts in a spatially localized manner has been proposed. This approach utilizes various microscopes to track the evolution of metal particles, including individual atoms, in catalytic reactions. By studying the behavior of palladium atoms and nanoparticles, it was discovered that single atoms leach out into solution and exhibit higher catalytic activity compared to surface nanoparticles. These findings challenge the assumption that the superior catalytic activity comes from the operation of single atomic catalytic centers on the surface of the support.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Engineering, Environmental
Yuting Yuan, Shikha Garg, Jinxing Ma, T. David Waite
Summary: In this study, copper aluminum layered hydroxides and copper oxide were used as catalysts for heterogeneous catalytic ozonation, targeting the removal of oxalate and formate contaminants. The role of the catalyst in contaminant removal was elucidated, with Cu-Al LDHs facilitating slow decay of O-3 to form surface hydroxyl radicals, while CuO rapidly transforms O-3 into surface-located hydroxyl radicals and/or other oxidants. Futile consumption of surface-located oxidants via interaction with the catalyst surface was minimal for Cu-Al LDHs, but becomes significant with higher CuO dosages.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2021)
Article
Chemistry, Physical
Zahid Nawaz, Nevin Gurbuz, Muhammad Naveed Zafar, Namik Ozdemir, Uzma Habib, Kalsoom Jan, Ismail Ozdemir
Summary: The research aims to synthesize homogeneous catalysts by starting from novel precursors to form N-heterocyclic carbene (NHC) ligands, and subsequently synthesizing Pd(NHC)-PEPPSI type complexes. The structure of all synthesized ligands and complexes was confirmed using various spectroscopic techniques, with some compounds confirmed by X-ray. These complexes were found to be significantly active as catalysts in the C-C cross-coupling reaction.
JOURNAL OF MOLECULAR STRUCTURE
(2021)
Article
Engineering, Environmental
Weilai Wang, Yuanzheng Zhang, Lei Xu, Yuansheng Pei, Junfeng Niu
Summary: This study explores safer and more efficient hydrogen sources by using hydrogen rich balls for catalytic hydrogenation of specific contaminants in water. The results show that hydrogen rich balls can sustainably release hydrogen, improving the adsorption and activation of hydrogen molecules on the catalyst and effectively removing p-chlorophenol and Cr(VI).
JOURNAL OF HAZARDOUS MATERIALS
(2022)
Article
Engineering, Chemical
Clement G. A. Morisse, Annelouise M. McCullagh, James W. Campbell, Chris Mitchell, Robert H. Carr, David Lennon
Summary: Two Pd/gamma-Al2O3 catalysts were studied for the vapor phase hydrogenation of nitrobenzene. It was found that the catalyst with higher metal loading exhibited higher selectivity towards aniline, while the catalyst with lower metal loading minimized product overhydrogenation. A global reaction scheme was proposed based on the experimental results to define the accessible by-product distribution of the examined catalysts. This is important for defining the product purification procedures required in heat recovery scenarios connected with large-scale aniline production.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2022)
Article
Engineering, Chemical
Jian Xiao, Lu Wang, Haonan Zhang, Ning Ma, Minli Tao, Wenqin Zhang
Summary: The study immobilized palladium salts and Pd(0) nanoparticles on amine and quaternary ammonium functionalized polyacrylonitrile fibers to prepare functionalized fiber catalysts, with Gemini quaternary ammonium fiber immobilized Pd(0) nanoparticles showing the best catalytic activity. The catalyst demonstrated high efficiency in catalyzing Heck reaction and 4-nitrophenol reduction with high yields, also exhibiting good substrate tolerance and recyclability. Experimental results confirmed the conversion of Pd(II) to Pd(0) during coupling reactions, contributing to the enhanced catalytic activity of PANF-immobilized Pd(0) compared to Pd(II).
CHEMICAL ENGINEERING SCIENCE
(2022)
Article
Chemistry, Multidisciplinary
Assefa Aschenaki, Fangfang Ren, Jia Liu, Wenqing Zheng, Qianyi Song, Wenhui Jia, James Jianmin Bao, Youxin Li
Summary: A novel magnetic nanoparticle catalyst with Pd was prepared in this study for the synthesis of unsymmetrical biaryl compounds through Suzuki cross-coupling reaction. The catalyst showed promising catalytic activity with high TOF and TON values, indicating an efficient reaction efficiency and reusability for up to seven times without significant loss in activity.
Review
Chemistry, Multidisciplinary
Lauren G. O'Neil, John F. Bower
Summary: Classical amination methods involve the reaction of a nitrogen nucleophile with an electrophilic carbon center; however, in recent years, umpoled strategies have gained traction where the nitrogen source acts as an electrophile. A wide range of electrophilic aminating agents are now available, and these underpin a range of powerful C-N bond-forming processes. In this Review, we highlight the strategic use of electrophilic aminating agents in total synthesis.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Jamie A. Cadge, John F. Bower, Christopher A. Russell
Summary: A combined theoretical and experimental investigation revealed an unusual mechanism of aryl iodide oxidative addition to gold complexes. The comparison between gold and palladium demonstrated significant differences in reaction rates and mechanisms, suggesting that gold could potentially facilitate a broad range of new or complementary transformations.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Guilherme A. M. Jardim, Renato L. de Carvalho, Mateus P. Nunes, Luana A. Machado, Leandro D. Almeida, Karim A. Bahou, John F. Bower, Eufranio N. da Silva Junior
Summary: Metal catalyzed C-H functionalization is widely used in organic chemistry for selective functionalization. Understanding the synthesis of transition metal Cp-type catalysts is crucial for modifying the catalyst structure for different applications.
CHEMICAL COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Atanu Modak, Juan Alegre-Requena, Louis de Lescure, Kathryn J. Rynders, Robert S. Paton, Nicholas J. Race
Summary: The ability to manipulate C-C bonds for selective chemical transformations is a challenging and growing area of research. The study reported a formal insertion of diazo compounds into unactivated C-C bonds of benzyl bromide derivatives catalyzed by a simple Lewis acid, resulting in products containing benzylic quaternary centers and alkyl bromides amenable to further derivatization. Computational analysis provided insight into the reaction mechanism, particularly the key selectivity-determining step.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Organic
Hannah M. Holst, Jack T. Floreancig, Casey B. Ritts, Nicholas J. Race
Summary: This study demonstrates the synthesis of beta-phenethylamine products through the treatment of unsymmetrical 2,3-disubstituted aziridines with TiCl4, involving the intermediacy of a phenonium ion. Computational analysis provides insight into the reaction mechanism, especially the selectivity of phenonium opening.
Article
Chemistry, Multidisciplinary
Olga O. Sokolova, John F. Bower
Summary: An enantioselective (3+1+2) cycloaddition reaction triggered by carbonylative C-C bond activation of cyclopropanes is achieved using an endo-directing group strategy. This reaction represents a rare example where C-C bond oxidative addition determines the enantiomeric outcome, and it is the first time this has been achieved within the context of a multicomponent reaction design.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Adam D. J. Calow, David Dailler, John F. Bower
Summary: Under Rh-catalyzed conditions, secondary amines and anilines serve as directing groups, enabling regioselective C-C bond activation of nonactivated cydopropanes. The resulting amino-stabilized rhodacydes undergo carbonylative C-N bond formation to yield challenging seven- and eight-membered lactams, exploiting the rare oxidative addition of C-C bonds of nonactivated cyclopropanes in reaction design.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Jamie A. Cadge, Paul J. Gates, John F. Bower, Christopher A. Russell
Summary: This research reports a newly discovered gold(III) metallafluorene complex that can be used for the synthesis of stable 9-fluorenone products through migratory insertion of CO. This finding expands the potential of using gold chemistry for product synthesis.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Changcheng Jing, Benjamin T. Jones, Ross J. Adams, John F. Bower
Summary: Unique examples of aza-Heck-based C(sp3)-H functionalization cascades are described, where alkyl-Pd(II) intermediates generated from the aza-Heck-type cyclization of N-(pentafluorobenzoyloxy)carbamates undergo C(sp(3))-H palladation to form cyclopropanes. The key factors controlling the site selectivity of the cyclopropanation process have been elucidated, enabling selective access to a wide range of ring- or spiro-fused systems.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Organic
Sangyun Kim, Annika D. S. Richardson, Atanu Modak, Nicholas J. Race
Summary: We report a dual-catalytic enantioselective allylic alkylation reaction that allows for the synthesis of alpha-amino heteroaryl benzylamine stereocenters with high yield and enantioselectivity.
JOURNAL OF ORGANIC CHEMISTRY
(2022)
Article
Chemistry, Organic
Olga O. Sokolova, Andrew G. Dalling, John F. Bower
Summary: This Account focuses on C-C bond activation based methodologies using minimally activated cyclopropanes, which allow for the atom economical assembly of complex scaffolds.
Article
Chemistry, Multidisciplinary
Samuel C. Scott, Jamie A. Cadge, Grace K. Boden, John F. Bower, Christopher A. Russell
Summary: We presented a Au-I complex of a hemi-labile (C boolean AND N) N-heterocyclic carbene ligand which can catalyze the oxidative addition of aryl iodides. Extensive computational and experimental investigations were performed to confirm and rationalize the oxidative addition process. The application of this initiation mode led to the first examples of exogenous oxidant-free Au-I/Au-III catalyzed 1,2-oxyarylations of ethylene and propylene. These challenging yet powerful processes establish these commodity chemicals as nucleophilic-electrophilic building blocks in catalytic reaction design.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Yuxiang Zhu, Matthew J. S. Smith, Wenbin Tu, John F. Bower
Summary: TFA promotes deprotection of O-Ts activated N-Boc hydroxylamines, leading to aminofunctionalization-based polycyclizations of tethered alkenes. The method enables a range of intramolecular alkene anti-1,2-difunctionalizations, including diamination, amino-oxygenation, and amino-arylation. It offers a predictable platform for accessing diverse C(sp(3))-rich polyheterocycles relevant to medicinal chemistry.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Matthew J. S. Smith, Wenbin Tu, Craig M. Robertson, John F. Bower
Summary: This article introduces an aminative cyclization reaction under acidic conditions, which is triggered by the deprotection of BocNR(OSO2R) reagents and carried out on alkenes equipped with pendant nucleophiles. The method offers flexibility in terms of choosing nucleophiles, alkenes, and cyclization modes, and enables the construction of consecutive stereocenters under operationally simple conditions.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Phillippa Cooper, Andrew G. Dalling, Elliot H. E. Farrar, Timothy P. Aldhous, Simon Grelaud, Eleanor Lester, Lyman J. Feron, Paul D. Kemmitt, Matthew N. Grayson, John F. Bower
Summary: The Ir-catalyzed alkene hydroarylation allows for the efficient synthesis of quaternary benzylic centers, and the structural features of the ligand play a crucial role in the reaction efficiency.
Article
Chemistry, Multidisciplinary
Alexander M. Prophet, Kritanjan Polley, Gary J. Van Berkel, David T. Limmer, Kevin R. Wilson
Summary: The oxidation kinetics of iodide by ozone at the air-water interface is studied in single microdroplets. Molecular simulations and kinetic modeling are used to understand the underlying multiphase mechanism.
Article
Chemistry, Multidisciplinary
Rong Zhang, Jiajing Lan, Fei Wang, Shumei Chen, Jian Zhang
Summary: By utilizing 1,1'-ferrocene dicarboxylic acid as a chelating and surface protection ligand, we have synthesized multi-nuclear indium oxide clusters with varying nuclear sizes, including heptanuclear and thirteen-nuclear clusters. These clusters possess labile coordination sites, allowing for structural modification and self-assembly, resulting in the formation of various cluster structures.
Article
Chemistry, Multidisciplinary
Hui Wang, Hui Liu, Mingsen Wang, Jiaheng Hou, Yongjun Li, Yuancheng Wang, Yingjie Zhao
Summary: Two supramolecular complexes were prepared using CBs and M1, and their single-crystal structures were analyzed by SCXRD. The unexpected 1:2 self-assembly structure between M1 and CB[8] was discovered for the first time. These complexes exhibit unique photophysical properties and provide valuable information about the structure and photophysical properties of supramolecular complexes.
Article
Chemistry, Multidisciplinary
Chang-Hee Lee, Sookil Park, Sanggil Kim, Ji Young Hyun, Hyun Soo Lee, Injae Shin
Summary: The epidermal growth factor receptor (EGFR) is a cell-surface glycoprotein involved in cell proliferation and tumor development. This study used a fluorescently labeled EGFR to investigate its time-dependent endocytosis in live cells and found that appended glycans affect EGFR internalization. Additionally, the study detected sialic acid residues attached to EGFR on the live cell surface using FRET-based imaging. This research provides valuable insights into the cellular functions of EGFR.
Article
Chemistry, Multidisciplinary
Subhankar Sahu, Lokesh Kumar, Sumita Das, Dipti Gupta, Ruchi Anand
Summary: This study proposes a strategy that combines organic electronics with biosensor scaffolds to create a compact device for monitoring environmental aromatic pollution. By coupling biosensing protein MopR with an organic electrochemical transistor (OECT), a sensor module capable of efficient detection of phenol was designed. Exclusive phenol detection with minimal loss of sensitivity could be achieved in complex pollutant mixtures and real environmental samples.
Review
Chemistry, Multidisciplinary
Changseok Lee, Hyung-Joon Kang, Sungwoo Hong
Summary: The formation of C-N bonds through hydroamination reactions catalyzed by nickel hydrides has been a topic of recent interest. This approach offers a way to efficiently transform a variety of alkene and alkyne substrates into compounds enriched with C-N bonds. The review provides a concise overview of the underlying reaction mechanisms and aims to stimulate further progress in NiH-catalytic techniques and catalyst design.
Article
Chemistry, Multidisciplinary
Yueci Wu, Lu-Lu Sun, Hai-Hao Han, Xiao-Peng He, Weiguo Cao, Tony D. James
Summary: Drug-induced liver injury (DILI) is a common cause of acute liver failure in the USA and Europe, but most cases can be recovered or prevented by discontinuing the offending drug. Recent research has found that peroxynitrite (ONOO-) can be used as a potential indicator for early diagnosis of DILI, and there is an urgent need to establish a method to detect and track peroxynitrite in DILI cases. In this study, a FRET-based nano fluorescent probe CD-N-I was developed, which showed high selectivity and sensitivity in detecting peroxynitrite. The probe successfully detected exogenous peroxynitrite in live cells and endogenous peroxynitrite in APAP-induced liver injury of HepG2 cells.
Article
Chemistry, Multidisciplinary
Dmitry L. Lipilin, Mikhail O. Zubkov, Mikhail D. Kosobokov, Alexander D. Dilman
Summary: This article describes a direct photocatalytic method for the thiolation of unprotected acids, which was previously challenging. By using a thionocarbonate reagent with an N-O bond, the efficient conversion of carboxylic acids to thiols is achieved.
Article
Chemistry, Multidisciplinary
Jason Malenfant, Lucille Kuster, Yohann Gagne, Kouassi Signo, Maxime Denis, Sylvain Canesi, Mathieu Frenette
Summary: Raman microscopy can reveal compound-specific vibrational fingerprints without sample preparation. The combination of efficient theoretical calculations and a user-friendly software can accurately predict peak positions and provide match scores to assist with structure determination.
Article
Chemistry, Multidisciplinary
Jayoh A. Hernandez, Paul S. Micus, Sean Alec Lois Sunga, Luca Mazzei, Stefano Ciurli, Gabriele Meloni
Summary: Essential trace metals play crucial roles in the survival and virulence of bacterial pathogens. Helicobacter pylori requires nickel for colonization and persistence in the stomach, and NixA is an essential nickel transporter in this process. This study characterizes the selectivity and electrogenic nature of NixA-mediated nickel transport.
Article
Chemistry, Multidisciplinary
Tarali Devi, Kuheli Dutta, Jennifer Deutscher, Stefan Mebs, Uwe Kuhlmann, Michael Haumann, Beatrice Cula, Holger Dau, Peter Hildebrandt, Kallol Ray
Summary: This study emphasizes the importance of subtle electronic changes and secondary interactions in the stability of biologically relevant metal-dioxygen intermediates. It also shows that the role of the chloride ligand in stabilizing the Fe-III-(OOBu)-Bu-t moiety can extend to other anions, including the thiolate ligand.
Article
Chemistry, Multidisciplinary
Jacqueline R. Santhouse, Jeremy M. G. Leung, Lillian T. Chong, W. Seth Horne
Summary: By studying the folding kinetics and mechanism of the BdpA sequence, researchers found that altering the backbone connectivity can affect protein folding. This suggests that protein mimetic chains have a significant degree of plasticity in transitioning between unfolded and folded states.
Article
Chemistry, Multidisciplinary
Divanshu Gupta, Ralf Einholz, Holger F. Bettinger
Summary: This study presents the first direct spectroscopic evidence of a cyclic seven-membered iminoborane. Compared to linear amino-iminoboranes, this cyclic iminoborane exhibits weakened bond strength and lower Lewis acidity value. The study suggests that the reduced ring strain of cyclic iminoborane prevents nitrogen fixation but allows facile (2 + 2) cycloaddition reaction with C2H4.
Article
Chemistry, Multidisciplinary
Renny Mathew, Aniruddha Mazumder, Praveen Kumar, Julie Matula, Sharmarke Mohamed, Petr Brazda, Mahesh Hariharan, Brijith Thomas
Summary: This study reveals the packing arrangement of partially disordered nitro-perylenediimide (NO2-PDI) using a synergistic approach that combines 3D ED, ssNMR, and DFT techniques. By overcoming these challenges, this methodology opens up new avenues for material characterization, driving exciting advancements in the field.