Article
Multidisciplinary Sciences
Dawei Cao, Chen-Chen Li, Huiying Zeng, Yong Peng, Chao-Jun Li
Summary: The study presents a method for constructing C(sp(3))-C(sp(3)) bonds using a nickel-catalyzed reductive coupling of moisture and air-stable hydrazones, with broad substrate scope and harmless by-products. The method demonstrates high functional group compatibility and practicality in the application to biological molecules.
NATURE COMMUNICATIONS
(2021)
Article
Chemistry, Inorganic & Nuclear
Gyorgy Hanko, Richard Marton, Antal Udvardy, Mihaly Purgel, Agnes Katho, Ferenc Joo, Gabor Papp
Summary: The water-soluble cis,mer-[IrH2Cl(mtppms)3] was an effective catalyst for the reduction of terminal alkynes by hydrogen transfer, with the highest rate observed at pH 3. The reactions exclusively yielded corresponding alkenes as products, with excess mtppms ligand inhibiting the reaction by forming a less active complex. The joint mechanism for both hydrogenation and transfer hydrogenation pathways was suggested based on experimental results and DFT calculations.
INORGANICA CHIMICA ACTA
(2021)
Article
Engineering, Environmental
Edgar S. Duran-Uribe, Antonio Sepulveda-Escribano, Enrique V. Ramos-Fernandez
Summary: Transition metal phosphides have attracted great interest as catalysts for hydrogenation reactions. In this study, cobalt phosphide nanoparticles supported on carbon were synthesized using microwave assistance and applied in the hydrogenation of 1-chloro-4-nitrobenzene. The catalytic activity was found to depend on the reduction temperature, with the phosphorus-rich cobalt phosphide obtained at low temperatures exhibiting the highest activity.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Organic
Daniel Timelthaler, Christoph Topf
Summary: This catalytic method allows for the pressure hydrogenation of quinolines in aqueous solution using a cobalt-based catalyst prepared from Co(OAc)(2)center dot 4H(2)O and zinc powder. The synthesis process is time-saving and operationally simple, with all reagents readily available from commercial sources. The reaction setup and autoclave charging are conducted outside an inert-gas-operated containment system for convenience.
SYNTHESIS-STUTTGART
(2022)
Review
Biochemistry & Molecular Biology
Qiang Wan, Sen Lin, Hua Guo
Summary: This article reviews recent theoretical advances in understanding FLP-based heterogeneous catalysis in various applications, such as metal oxides, functionalized surfaces, and two-dimensional materials. It emphasizes the importance of a better understanding of the catalytic mechanism for the experimental design of novel heterogeneous FLP catalysts.
Article
Chemistry, Multidisciplinary
Yuki Saito, Shu Kobayashi
Summary: The application of heterogeneous catalysts in continuous-flow enantioselective hydroacylation reactions was studied. Catalysts were prepared by mixing supports and rhodium complexes, and showed excellent activity and enantioselectivity. Under optimized conditions, the catalysts exhibited high turnover numbers and could be applied to various substrates. Furthermore, sequential-flow reactions with other heterogeneous catalysts were demonstrated for the synthesis of biologically active molecules and functional materials.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Meiling Zhu, Haitao Tian, Sanxia Chen, Wenxuan Xue, Yanhong Wang, Hongcheng Lu, Ting Li, Feng Chen, Conghui Tang
Summary: Herein, we report a cobalt N,N-bidentate complex catalyzed reductive formylation of N-heteroarenes for the generation of N-formyltetrahydroquinoline (FTHQ) derivatives. Formic acid was used as a transfer hydrogenation reagent, which is safe, abundant, and easy to handle. This work represents the first homogeneous system for the reductive formylation of N-heteroarenes, where the metal ligand cooperated dehydrogenation is crucial for the success of this transformation. Deuteration labeling experiments and Hammett analysis were conducted, suggesting a plausible mechanism.
JOURNAL OF CATALYSIS
(2022)
Article
Chemistry, Multidisciplinary
Zhaoyang Cheng, Jun Guo, Yufeng Sun, Yushan Zheng, Zhehong Zhou, Zhan Lu
Summary: This study presents a controllable cobalt-catalyzed sequential hydrosilylation/hydroboration reaction of arylacetylenes, achieving high regioselectivities for all possible regio-outcomes. Adjusting the ligands of cobalt catalysts combined with dual catalysis relay strategy is crucial for achieving regio-chemistry control, which may inspire further exploration in diversity-oriented synthesis involving multiple additions.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Sophie W. Anferov, Alexander S. Filatov, John S. Anderson
Summary: The use of supporting ligands that can store either protons or electrons has emerged as a powerful strategy in catalysis. This strategy allows for the storage of both protons and electrons in the secondary coordination sphere, resulting in remarkable transformations. This article describes the application of this strategy in Co-based hydrogenation catalysis, showing that ancillary ligands can alter the classic organometallic mechanisms for catalysis.
Article
Chemistry, Physical
Bingxue Liu, Qiang Liu
Summary: Cobalt-catalyzed hydroalkylation of alkenes and alkynes is an efficient method for selective formation of C-C bonds. Significant progress has been made in the past five years, covering different reaction mechanisms.
Article
Chemistry, Multidisciplinary
Emilia Paone, Mariachiara Miceli, Angela Malara, Guozhu Ye, Elsayed Mousa, Elza Bontempi, Patrizia Frontera, Francesco Mauriello
Summary: After appropriate thermal treatments, spent Li-ion batteries can be directly used as catalysts for selective hydrogenation, showing the potential of using and recycling the batteries as precious catalytic materials.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2022)
Article
Chemistry, Multidisciplinary
Soumyadeep Chakrabortty, Katharina Konieczny, Felix J. de Zwart, Eduard. O. Bobylev, Eszter Barath, Sergey Tin, Bernd H. Mueller, Joost N. H. Reek, Bas de Bruin, Johannes G. de Vries
Summary: Researchers achieved enantioselective hydrogenation of cyclic enamides using an earth-abundant cobalt-bisphosphine catalyst. The catalytic system, CoCl2/(S,S)-Ph-BPE, reduced trisubstituted carbocyclic enamides to saturated amides with high activity and excellent enantioselectivity (up to 99%). The methodology can be extended to the synthesis of chiral amines by base hydrolysis of the hydrogenation products. Preliminary mechanistic investigations suggested a sigma-bond-metathesis pathway for the hydrogenation of the carbon-carbon double bond, involving a high spin cobalt (II) species.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Yan-Dong Zhang, Xiao-Yu Li, Qian-Kun Mo, Wen-Bin Shi, Jia-Bao Zhao, Shou-Fei Zhu
Summary: In this study, we developed new Co complexes with cyclopropane-based diphosphine ligands that can catalyze highly chemo-, regio-, and stereoselective hydroboration reactions of unsymmetrical internal alkynes. These reactions exhibit unusual regioselectivity, leading to the synthesis of trisubstituted alkenylborates and alkenes with different stereochemistry.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Connor S. MacNeil, Hongyu Zhong, Tyler P. Pabst, Michael Shevlin, Paul J. Chirik
Summary: The cobalt-catalyzed asymmetric hydrogenation of dehydro-sitagliptin was studied and applied to the synthesis of sitagliptin. The discovery of catalysts was accelerated by the synthesis of cationic bis(phosphine) cobalt eta 6-arene complexes. The optimal catalyst showed high yield and enantioselectivity, and maintained excellent activity and selectivity after standing in air for 2 weeks.
Article
Chemistry, Multidisciplinary
Chuncheng Lin, Weihao Wan, Xueting Wei, Jinzhu Chen
Summary: Co nanoparticles encapsulated in N-doped carbon nanotubes (Co@NC900) have been investigated as a potential substitute for precious Pt-group catalysts in hydrogenative heterocyclization reactions. Co@NC900 demonstrates efficient catalytic activity for the hydrogenative coupling of 2-nitroaniline to benzaldehyde, with >99% yield at ambient temperature in a single step. The catalyst is easily recoverable and recyclable, with kinetic experiments suggesting that hydrogenation is the rate-determining step, with an apparent activation energy of 41 +/- 1 kJ mol(-1). Theoretical investigations reveal the mechanism by which Co@NC900 activates both H-2 and the nitro group of 2-nitroaniline, providing insights for the green and efficient synthesis of heterocyclic compounds.
Review
Chemistry, Multidisciplinary
Maomao Xie, Meng Gao, Yang Yun, Martin Malmsten, Vincent M. M. Rotello, Radek Zboril, Omid Akhavan, Aliaksandr Kraskouski, John Amalraj, Xiaoming Cai, Jianmei Lu, Huizhen Zheng, Ruibin Li
Summary: Antimicrobial resistance (AMR) is a major threat to the environment and health, and antimicrobial nanomaterials are being explored as alternatives to conventional antibiotics. Some antimicrobial nanomaterials show AMR-independent antimicrobial effects, while others trigger the evolution of AMR. This review compares the mechanisms and relationships of antibiotics and antimicrobial nanomaterials, examines nano-microbe interactions, and provides an outlook on future antimicrobial nanomaterials.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Nanoscience & Nanotechnology
Rahul P. Gaikwad, Dhanaji R. Naikwadi, Ankush V. Biradar, Manoj B. Gawande
Summary: This study investigates the role of mesoporous graphitic carbon nitride (mpg-C3N4) photocatalyst in the esterification of substituted benzaldehyde under visible light irradiation at room temperature without any additives. The mpg-C3N4 material, characterized by various techniques, exhibits high surface area, porosity, medium band gap, and nanowire-like shape. These properties enhance the photocatalytic activity of mpg-C3N4 towards the esterification reaction.
ACS APPLIED NANO MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Olivier Henrotte, Eva Yazmin Santiago, Artur Movsesyan, Luca Mascaretti, Morteza Afshar, Alessandro Minguzzi, Alberto Vertova, Zhiming M. Wang, Radek Zboril, Stepan Kment, Alexander O. Govorov, Alberto Naldoni
Summary: The investigation of photocatalytic systems at the nanoscale is crucial for understanding their fundamental principles, improving their design, and enhancing their applicability. A photochemical nanoscopy technique has been developed to detect the molecular products of plasmonic hot-carrier-driven photocatalytic reactions with nanometric precision. Applying this methodology to Au/TiO2 plasmonic photocatalysts, it was discovered that smaller and denser Au nanoparticle arrays have lower optical contribution but higher quantum efficiency in hot-hole-driven photocatalysis, which is closely related to population heterogeneity. This study also revealed the areas of oxidation and reduction product evolution in a single plasmonic nanodiode, demonstrating the bipolar behavior of such nanosystems. These findings enable quantitative investigations at the nanoscale to evaluate the photocatalytic reactivity of low-dimensional materials in various chemical reactions.
Review
Chemistry, Multidisciplinary
Iosif Tantis, Smita Talande, Vasileios Tzitzios, Georgia Basina, Vishal Shrivastav, Aristides Bakandritsos, Radek Zboril
Summary: This review focuses on recent advances in electrochemical energy storage (EES) technologies related to 2D crystals originating from non-layered 3D solids (non-van der Waals; nvdW) and their influence on the materials' features. The methods and challenges in top-down and bottom-up strategies towards nvdW 2D sheets and their applications in EES are discussed. Moreover, the opportunities and challenges of nvdW 2D systems in various applications are highlighted.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Physical
Tomas Malina, Cordula Hirsch, Alexandra Rippl, David Panacek, Katerina Polakova, Veronika Sedajova, Magdalena Scheibe, Radek Zboril, Peter Wick
Summary: Graphene oxide (GO) is a promising delivery nanoplatform, but its non-specific surface properties and heterogeneity in stability limit its commercial application. Evaluating the interaction of emerging graphene derivatives with endothelial and immune cells is important. The study demonstrated that graphene acid (GA) and cyanographene (GCN) have better biocompatibility and potential for drug/gene delivery compared to GO.
Article
Chemistry, Organic
Vishakha Goyal, Tarun Bhatt, Chitrarekha Dewangan, Anand Narani, Ganesh Naik, Ekambaram Balaraman, Kishore Natte, Rajenahally V. Jagadeesh
Summary: This study reports the catalytic utilization of methanol as a hydrogen source for the reduction of various functional organic compounds. The use of a commercially available Pt/C catalyst enables the transfer hydrogenation of nitroarenes, olefins, and carbonyl compounds. The Pt/C catalytic system shows practicability in terms of catalyst recycling and reusability, as well as reaction upscaling, along with the N-methylation and N-alkylation of anilines.
JOURNAL OF ORGANIC CHEMISTRY
(2023)
Review
Chemistry, Physical
En Zhao, Wenjun Zhang, Lin Dong, Radek Zboril, Zupeng Chen
Summary: Transfer hydrogenation using liquid hydrogen carriersas the direct proton sources under mild conditions has attracted considerable attention in the field of organic synthesis. Photocatalytic water-donating transfer hydrogenation (PWDTH) has emerged as an eco-friendly alternative to conventional hydrogenation technology. This paper discusses recent advances in PWDTH reactions, including the mechanism of hydrogen transfer and the design principles of efficient photocatalysts. It also explores the current challenges and future opportunities in this rapidly developing field.
Article
Chemistry, Multidisciplinary
Reshma Babu, Subarna Sukanya Padhy, Rohit Kumar, Ekambaram Balaraman
Summary: Sustainable chemical production requires the development of coherent and robust catalytic systems based on earth-abundant transition metals. This study explores a novel tandem reaction that converts cyclic and acyclic diazo compounds into valuable amines using a single-site molecular manganese complex as the catalyst. The reaction involves dehydrogenation, transfer hydrogenation, and borrowing hydrogenation strategies, and utilizes renewable feedstocks such as alcohols. The synthetic application of this approach in pharmaceutical synthesis and the production of N-CH3/CD3 derivatives is also demonstrated.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Organic
Olutayo N. Farinde, Vanaparthi Satheesh, Kendra K. Shrestha, Carmen R. Rhinehalt, Vinod G. Landge, Michael C. Young
Summary: Cinnamylamines are important components of many drugs targeting G protein-coupled receptors. Existing methods for synthesizing 3,3-diarylallylamines often involve a multistep process that includes poorly-selective Wittig addition and direct aryl addition to N-protected cinnamylamines using aryl iodides which leads to decreased selectivity. However, by using aryl boronic acids, the yield and selectivity can be improved.
ORGANIC CHEMISTRY FRONTIERS
(2023)
Article
Chemistry, Multidisciplinary
Madhu Nallagangula, Murugan Subaramanian, Rohit Kumar, Ekambaram Balaraman
Summary: In recent years, the borrowing hydrogen (BH) and interrupted borrowing hydrogen (IBH) strategies have gained significant attention for their efficient and sustainable synthesis of diverse building blocks. These approaches offer advantages such as use of feedstock chemicals, high atom economy, no pre-activation of substrates, and water as the only by-product. This review article focuses on the recent advances in the IBH strategy and its application in sustainable chemical synthesis, particularly in C-C bond formation, synthesis of 3,3'-bisindolylmethanes, alpha-branched ketones/diketones, and regioselective alkylation of N-heterocycles.
CHEMICAL COMMUNICATIONS
(2023)
Review
Chemistry, Physical
Babak Jaleh, Atefeh Nasri, Mahtab Eslamipanah, Mahmoud Nasrollahzadeh, Jacky H. Advani, Paolo Fornasiero, Manoj B. Gawande
Summary: Industrialization has led to increased demand for clean energy storage and conversion systems to reduce the use of environmentally harmful substances. Nature-inspired materials, with their extended porous architectures, high surface areas, and low cost, show great potential as catalysts and nanofillers in energy storage and conversion. This review summarizes the structure and classification of natural materials suitable for energy devices, focusing on their applications and advancements in fuel cells.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
Reshma Babu, Subarna S. Padhy, Ganesan Sivakumar, Ekambaram Balaraman
Summary: Sustainable chemical production requires new catalysts and technologies, and the development of robust catalytic systems based on plentiful transition metals is crucial.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Review
Chemistry, Inorganic & Nuclear
Harsh R. Darji, Hanumant B. Kale, Farhan F. Shaikh, Manoj B. Gawande
Summary: This review focuses on the utilization of CO2 for methanol synthesis and various reactor systems. The technology discussed in this review is expected to support and advance research on selective methanol synthesis from CO2 as a fuel, providing sustainable solutions for climate change and rising energy demands.
COORDINATION CHEMISTRY REVIEWS
(2023)
Review
Chemistry, Multidisciplinary
Virender K. Sharma, Xingmao Ma, Radek Zboril
Summary: Water is a crucial component of the United Nations' sustainable development goals, and water reuse is becoming increasingly accepted in response to global water scarcity. However, traditional treatment processes face challenges in treating low concentrations of pollutants in the presence of other chemicals. Advanced oxidation processes and the use of single atom catalysts offer promising solutions to these challenges.
CHEMICAL SOCIETY REVIEWS
(2023)
Article
Chemistry, Multidisciplinary
Priti Sharma, Debdyuti Mukherjee, Sujoy Sarkar, Daniel Mandler, Rajender S. Varma, Manoj B. Gawande, Radek Zboril, Yoel Sasson
Summary: A straightforward and mild protocol for photochemical in situ selective hydrogenation was achieved using an Al-H2O system as a hydrogen donor and a Pd-g-C3N4 photocatalyst. This method showed excellent yield and selectivity for a wide range of olefins and nitro compounds (>99%) under visible light and ambient conditions. The Pd-g-C3N4 photocatalyst also demonstrated efficient bifunctional electrocatalytic activity for overall water splitting.