Article
Chemistry, Organic
Jinghao Zhang, Yang Chen, Jing Sun, Jingyun Wang, Mingdong Zhou
Summary: A palladium-catalyzed direct alkenylation method for alkyl chain-substituted tetrathienoacenes has been developed under mild conditions. This efficient and viable approach allows for the synthesis of various dialkenylated tetrathienoacenes using different functionalized alkenes as coupling substrates.
Article
Chemistry, Multidisciplinary
Francesco Ferlin, Ioannis Anastasiou, Nihad Salameh, Takeru Miyakoshi, Olivier Baudoin, Luigi Vaccaro
Summary: A heterogeneous catalyst has been prepared for the intramolecular activation/cyclization reaction to synthesize indolines. The catalyst showed high efficiency through a release and catch mechanism, facilitated by iodide ligands. The heterogeneous nature of the catalyst was further utilized in the design of a continuous-flow protocol, enabling efficient recovery and reuse.
Article
Chemistry, Physical
Qing-Shan Kong, Xing-Long Li, Hong-Bo Shen, Hua-Jian Xu, Yao Fu
Summary: This study presents an eco-friendly and efficient heterogeneous sodium-doped porous sodium manganese oxide catalyst for the oxidative cleavage of furanic 1,2-diols into medium-chain furanic aldehyde compounds. Various high value-added chemicals were synthesized using this catalytic approach, demonstrating its broad applicability and high selectivity.
GREEN ENERGY & ENVIRONMENT
(2022)
Review
Chemistry, Multidisciplinary
Bogdan Y. Karlinskii, Valentine P. Ananikov
Summary: C-H functionalization is a convenient and powerful tool in modern chemistry, but its harsh reaction conditions limit its use for modifying unstable substrates. Biomass-derived furan platform chemicals are promising organic molecules, but their sensitivity to acids, oxidants, and high temperatures hinders traditional methods of C-H functionalization. New catalytic methods are urgently needed to modify non-reactive furan cores and obtain materials with controlled properties.
Article
Chemistry, Multidisciplinary
Andrea Vassoi, Tommaso Tabanelli, Annalisa Sacchetti, Francesca Di Gioia, Luigi Capuzzi, Fabrizio Cavani
Summary: This study introduces a new heterogeneous catalyst for the oxidative cleavage of unsaturated fatty acids triglycerides derived from vegetable oil, providing a promising alternative to current ozonization processes. The catalyst based on Cu2+ showed efficient recovery, regeneration, and recycling capabilities, offering potential for further industrial exploitation.
Article
Engineering, Environmental
Zathang Laldinpuii, Samson Lalhmangaihzuala, Zodinpuia Pachuau, Khiangte Vanlaldinpuia
Summary: PET, as one of the most widely used polymeric materials, can be depolymerized using BLA derived catalyst, which is cost-free, environmentally friendly, and reusable for multiple cycles, making it an efficient and sustainable solution for plastic waste management.
Article
Chemistry, Physical
Dolores Bourbiaux, Yu Xu, Laurence Burel, Firat Goc, Pascal Fongarland, Regis Philippe, Guillaume Aubert, Cyril Aymonier, Franck Rataboul, Laurent Djakovitch
Summary: Lignin is a major component of lignocellulosic biomass and can be depolymerized under mild oxidizing conditions with the Pd catalyst to produce oxygenated aromatic compounds. The richness of functional groups in lignin makes it an attractive precursor for a wide variety of aromatic compounds. Differences in selectivity in aromatic monomers may arise depending on the catalyst nature and synthetic methods used.
Article
Energy & Fuels
Hind Al-shaikh, Jamal Lasri, Julian G. Knight, Soha T. Al-Goul
Summary: Ordered mesoporous silica supported Pd NPs were synthesized and showed notable efficiencies in the hydrolytic production of H2 from NaBH4. The catalyst stabilized by PEG and imidazolium ionic liquid based-[KIT-6] exhibited higher activity compared to its [KIT-6] counterpart.
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
Nanoscience & Nanotechnology
Jyoti Rohilla, Sahil Thakur, Keshav Kumar, Raghubir Singh, Varinder Kaur
Summary: The present study synthesized Sn-NaMOF using solvothermal method and used it as a support for Pd nanoparticles. The resulting Pd NPs/Sn-Na MOF showed excellent catalytic activity for the conversion of fructose to 5-HMF. The catalyst exhibited fast conversion, recyclability, and high yield of 5-HMF in aqueous medium without the formation of side products.
ACS APPLIED NANO MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Bo Zhou, Fan Song, Xinyue Ma, Lijun Wang
Summary: In this study, TiO2 nanoparticles supported on exfoliated montmorillonite were used as catalysts to efficiently catalyze the acetalization reactions of biomass-derived furfural and alcohols. The catalyst achieved equilibrium in a short time with high catalytic performance, showing stable product output in continuous-flow reactions. Both Lewis and Bronsted acid sites on the catalyst were essential for maximizing the catalytic performance by simultaneously activating both furfural and alcohol.
Article
Green & Sustainable Science & Technology
Danilo Gualberto Zavarize, Heder Braun, Jorge Diniz de Oliveira
Summary: A novel acid heterogeneous catalyst derived from Amazon acai berry seeds showed excellent performance in the methanolysis of waste cooking oil, with optimized conditions leading to a maximum conversion rate of 89%. The catalyst exhibited low cost, high stability, and outperformed traditional homogenous acid catalysts and activated carbon-derived catalysts in terms of performance and reusability.
Article
Chemistry, Organic
Gredy Kiala Kinkutu, Catherine Louis, Myriam Roy, Juliette Blanchard, Julie Oble
Summary: In order to develop a continuous flow process for the C3-alkylation of furfural, we optimized the reaction conditions using a pulsed-flow system and then successfully transferred them to a continuous flow reactor. This allowed for the C3-alkylation of furfural to be carried out in a safer and more efficient manner.
BEILSTEIN JOURNAL OF ORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Harsh Vardhan, Abdullah M. Al-Enizi, Ayman Nafady, Yanxiong Pan, Zhongyu Yang, Humberto R. Gutierrez, Xiaolong Han, Shengqian Ma
Summary: The exponential growth in the field of covalent-organic frameworks (COFs) is attributed to the direct correlation between designing principles and desired properties. The comparison of catalytic activity between single-pore and dual-pore COFs is crucial for establishing a structure-function relationship. By synthesizing imine-linked dual-pore COFs with controllable bipyridine content, this study demonstrates efficient catalytic active sites for selective functionalization of sp(2)C-H bonds to C-X (X = Br, Cl) or C-O bonds. The comparison between palladium decorated dual-pore frameworks and single-pore imine-linked Pd(II) @ Py-2,2'-BPyDC framework provides insights into the relationship between catalytic activity and core properties of rationally designed frameworks.
Review
Chemistry, Physical
Apoorva Shetty, Vandana Molahalli, Aman Sharma, Gurumurthy Hegde
Summary: Biomass-derived carbons have unique physical and chemical properties, such as tunable surface, chemical inertness, and hydrophobicity, which make them ideal candidates to be used as heterogeneous catalysts and catalytic supports. The wide range of reactions that can be compatible with biomass-derived carbon materials includes organic transformations, electrocatalytic reactions, and photocatalytic reactions. This review discusses the uses of biomass-derived materials in the field of heterogeneous catalysis, highlighting the importance and unique properties of carbon materials derived from biomass as potential catalysts.
Article
Chemistry, Organic
Tian Sang, Chuntian Li, Fan Jia, Jing He, Yan Liu, Luigi Vaccaro, Jichang Liu, Ping Liu
Summary: This study has developed a series of halogenated systems for pyrazolo[1,5-a]pyrimidines, achieving selective transformations by mono- and di-iodination using varying ratios of pyrazolo[1,5-a]pyrimidines and NIS. Additionally, the reaction with NBS or NCS produces unique dibrominated or dichlorinated products. The wide range of substrates, good functional group tolerance, and gram-scale synthesis demonstrate the potential application of this reaction.
POLYCYCLIC AROMATIC COMPOUNDS
(2023)
Review
Chemistry, Multidisciplinary
Yan Zhang, Zhenzhi Cai, Svenja Warratz, Chanchan Ma, Lutz Ackermann
Summary: In recent years, electrochemical oxidative reactions using radical intermediates have become an environmentally friendly and powerful method for the formation of C-E (E = C, N, S, Se, O and Hal) bonds through single-electron transfer processes at the electrodes. This minireview focuses on the recent advances in electrooxidation and radical reactions, particularly concerning radical additions onto alkynes, until June 2022.
SCIENCE CHINA-CHEMISTRY
(2023)
Review
Chemistry, Physical
Federica Valentini, Oriana Piermatti, Luigi Vaccaro
Summary: The direct functionalization of inactivated C-H bonds has gained attention as a method for step-economy, atom-efficient, and environmentally sustainable processes. The design and preparation of highly active metal nanoparticles as catalysts for C-H bond activation under mild reaction conditions is still being investigated. This review focuses on the functionalization of un-activated C(sp3)-H, C(sp2)-H, and C(sp)-H bonds using metal and metal oxide nanoparticles for C-O and C-X (X = Halogen, B, P, S, Se) bond formation, leading to more sustainable access to industrial production.
Article
Chemistry, Multidisciplinary
Xinran Chen, Hasret Can Guelen, Jun Wu, Zi-Jing Zhang, Xin Hong, Lutz Ackermann
Summary: Ruthenium-catalyzed sigma-bond activation-assisted meta-C-H functionalization has gained significance in the formation of distal C-C bonds. However, the lack of mechanistic studies has hindered a complete understanding of the site-selectivity and reaction pattern. In this study, computational investigations were conducted on ruthenium-catalyzed C-H functionalization using alkyl bromides and aryl bromides. Monocyclometalated ruthenium(II) complexes were identified as the active species, with inner-sphere single electron transfer (ISET) facilitating the activation of organic bromides. The competition between reductive elimination and radical coupling determines the site-selectivity, which was further predicted using a multilinear regression model validated by experiments.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Yan Zhang, Chunhang Zhao, Chanchan Ma, Zhenzhi Cai, Lutz Ackermann, Sven Trienes
Summary: We describe a mechanistically distinct approach using photoinduced carbon-carbon (C-C) activation/ring-opening to access gamma,delta-unsaturated aldehydes from methylenecyclobutanols and sulfonyl chlorides by strain release. The sulfonyl motif on the products was easily removed by another photocatalytic process, enabling the concise assembly of the natural product alatanone A. Our approach demonstrates versatile functional group tolerance, ample substrate scope, and scalability, and represents a conceptually distinct alternative to existing approaches for remote 1,4-diversifications, with a double bond remaining in the obtained products.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Shan Chen, Binbin Yuan, Yulei Wang, Lutz Ackermann
Summary: By difunctionalization of nonactivated alkenes, twofold distal C-H functionalization was achieved, allowing rapid access to multifunctionalized molecules. The multicomponent ruthenium-catalyzed remote 1,n-difunctionalization (n=6,7) of nonactivated alkenes with fluoroalkyl halides and heteroarenes in a modular manner was reported. This method provided mild conditions, unique selectivity, and broad substrate scope, and featured a domino process for twofold remote C(sp(2))-H/C(sp(3))-H activation with the sequential formation of three different carbon-centered radicals. A plausible mechanism was proposed based on detailed experimental and computational studies.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Jun Wu, Wen Wei, Julia Poehlmann, Rajeshwaran Purushothaman, Lutz Ackermann
Summary: In this study, a ruthenium(II)-catalyzed multicomponent Domino reaction was reported, which enables the efficient synthesis of structurally diversified C-alkyl glycosides in a single step.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Dingyi Wang, Binbin Yuan, Jiawei Xu, Lutz Ackermann
Summary: In this study, an electrochemical strategy was used to achieve the dual functionalization of unactivated alkenes through an intramolecular migration process. This strategy eliminated the need for sacrificial chemical oxidants and noble-metal catalysts, and the reactions were carried out under mild conditions. The electrochemistry enabled the migration of (hetero)aryl groups, leading to the formation of alkenyl/alkynyl-migration products. The reaction mechanism was established through experiments and computations.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Editorial Material
Chemistry, Organic
Lutz Ackermann, Song Lin
Summary: The field of organic electrosynthesis and electrocatalysis has experienced a remarkable revival in recent years. Electrochemistry, as an unconventional reaction tool, has allowed synthetic chemists to innovate novel transformations, advance new synthetic strategies, and enhance the sustainability of organic synthesis.
EUROPEAN JOURNAL OF ORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Kui Zeng, Ruhuai Mei, Sebastian Dechert, Lutz Ackermann, Kai Zhang
Summary: This study reports a recyclable stereoauxiliary aminocatalytic approach for the efficient one-pot synthesis of desired trisubstituted indolizine-2-carbaldehydes via [3+2] annulations of acyl pyridines and alpha,beta-unsaturated aldehydes, using aminosugars derived from biomass. Control experiments confirm the stereoauxiliary effect favored by the beta-anomer of D-glucosamine. Moreover, polymeric chitosan containing predominantly beta-D-anhydroglucosamine units shows excellent catalytic performance and can be used for large-scale synthesis and catalytic cycling experiments. Thus, this approach advances the existing methodologies and provides a rich library of indolizine-2-aldehydes, which can be used for late-stage diversification and targeted modifications of bioactive molecules or drugs.
COMMUNICATIONS CHEMISTRY
(2023)
Review
Chemistry, Multidisciplinary
Yulei Wang, Suman Dana, Hao Long, Yang Xu, Yanjun Li, Nikolaos Kaplaneris, Lutz Ackermann
Summary: Late-stage functionalization (LSF) is a powerful strategy to accelerate the development of medicinally relevant compounds, crop protecting agents, and functional materials. Electrochemical late-stage functionalization (eLSF) has emerged as an environmentally friendly platform and has gained significant momentum in the past decade.
Article
Chemistry, Multidisciplinary
Elisa Y. Lai, Binbin Yuan, Lutz Ackermann, Magnus J. Johansson
Summary: In this study, a new method for directed ruthenium-catalyzed C-H aminocarbonylation has been developed under mild conditions through high-throughput experimentation. This method allows the introduction of special amide functional groups and is applicable to various substitution patterns and different weakly Lewis basic directing groups in anilides.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Nihad Salameh, Federica Valentini, Olivier Baudoin, Luigi Vaccaro
Summary: We report a general and efficient enantioselective C-H arylation of aryl bromides using BozPhos as the bisphosphine ligand and SP-NHC-PdII as recoverable heterogeneous catalyst. By exploiting the release and catch mechanism of action, high enantioselectivities were achieved across different substrates containing methyl, cyclopropyl and aryl C-H bonds. The developed catalytic system provides a more sustainable solution for the synthesis of high added-value chiral products through recycling of the precious metal.
Article
Meteorology & Atmospheric Sciences
S. P. Alexander, A. Protat, A. Berne, L. Ackermann
Summary: Antarctic precipitation, especially within the boundary layer, is poorly characterized and understood due to limited surface-based remote sensing observations. This study used cloud and precipitation remote-sensing instruments to characterize snowfall over Davis. The results reveal the relationship between virga and wind conditions, particle aggregation at certain temperatures, and the sublimation of snowfall mass at different altitudes. These findings contribute to a better understanding of snowfall in the Antarctic region.
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES
(2023)
Article
Chemistry, Physical
Julia Struwe, Lutz Ackermann
Summary: In recent years, photoelectrocatalysis has become more and more viable for molecular synthesis. However, there is still a lack of detailed comparison among different catalysts for the undirected C-H functionalization of arenes. To address this, more than a dozen different mediators were utilized to compare their efficacies in the trifluoromethylation of (hetero-)arenes.
FARADAY DISCUSSIONS
(2023)
Article
Chemistry, Multidisciplinary
Xuemei Liu, Chaonan Cui, Shuoshuo Wei, Jinyu Han, Xinli Zhu, Qingfeng Ge, Hua Wang
Summary: This study presents a new strategy for designing efficient photocatalysts that can convert CO2 into hydrocarbons by utilizing synergistic catalytic sites. The findings provide a solution for the selective photocatalytic reduction of CO2 to CH4.
Article
Chemistry, Multidisciplinary
Chengxian Hu, Dan Wang, Lu Wang, Ying Fu, Zhengyin Du
Summary: A novel one-pot, three-component reaction conducted under electrochemical conditions was studied. The reaction involved 2-aminothiophenols, aldehydes, and malononitrile, using TBABF4 as an electrolyte and CuI as a catalyst. The proposed reaction mechanism suggested that CuI served as an electron relay. This method offers simplified operation, high atom economy, and mild reaction conditions.
Article
Chemistry, Multidisciplinary
Zhi Yang, Yu Chen, Linxi Wan, Yuxiao Li, Dan Chen, Jianlin Tao, Pei Tang, Fen-Er Chen
Summary: A highly enantioselective method for the complete hydrogenation of pyrimidinium salts using Ir/(S,S)-f-Binaphane complex as the catalyst was developed. This method provides easy access to fully saturated chiral hexahydropyrimidines, which are prevalent in many bioactive molecules. The reactions exhibit high yields and enantioselectivities under mild reaction conditions without additives. Successful application of this methodology in a continuous flow fashion further extends its practical utility.
Article
Chemistry, Multidisciplinary
Tina Jeoh, Jennifer Danger Nill, Wujun Zhao, Sankar Raju Narayanasamy, Liang Chen, Hoi-Ying N. Holman
Summary: In this study, the enzymatic hydrolysis of cellulose was investigated using real-time infrared spectromicroscopy. The spatial heterogeneity of cellulose was found to impact the hydrolysis kinetics. Hydration affected cellulose ordering, and Cel7A preferentially removed less extensively hydrogen bonded cellulose.
Article
Chemistry, Multidisciplinary
Tiphaine Richard, Walid Abdallah, Xavier Trivelli, Mathieu Sauthier, Clement Dumont
Summary: An effective method of grafting functionalities onto lignin based on glycerol carbonate has been developed using an efficient nickel-catalysed telomerisation reaction. This method allows lignin to have new reactive functions and reduces the glass transition temperatures of modified lignins, thereby expanding the application range of lignin-based resins.
Article
Chemistry, Multidisciplinary
Jing Qi, Xiyan Wang, Gan Wang, Srinivas Reddy Dubbaka, Patrick ONeill, Hwee Ting Ang, Jie Wu
Summary: This study presents a green and environmentally friendly approach for the synthesis of imides using electrocatalytic oxidation with H2O as the oxygen source. The method eliminates the need for toxic or expensive oxidants and achieves high yields under mild reaction conditions. It shows broad substrate compatibility and potential for industrial applications.
Article
Chemistry, Multidisciplinary
Babasaheb Sopan Gore, Lin-Wei Pan, Jun-Hao Lin, Yi-Chi Luo, Jeh-Jeng Wang
Summary: Here, we report a visible light-promoted intramolecular radical cascade reaction for the construction of fluorenol and naphthalene-fused cyclopropyl carbaldehyde derivatives. This method offers mild reaction conditions, a broad substrate scope, excellent step efficiency, and scalability, without the need for external chemical oxidants. The novelty of this protocol was demonstrated by synthesizing chrysene analogs and performing late-stage functionalizations.
Article
Chemistry, Multidisciplinary
Juho Antti Sirvio, Idamaria Romakkaniemi, Juha Ahola, Svitlana Filonenko, Juha P. Heiskanen, Ari Ammala
Summary: This article discusses the method of using supramolecular interaction between an aromatic hydrogen bond donor and lignin to achieve rapid delignification of softwood at low temperatures.
Article
Chemistry, Multidisciplinary
Yunyan Meng, Chunxiang Pan, Na Liu, Hongjiang Li, Zixiu Liu, Yao Deng, Zixiang Wei, Jianbin Xu, Baomin Fan
Summary: A novel visible light-driven synthesis method for 2,3-diamines has been developed, which has mild conditions, avoids the use of metal reagents, and can synthesize diamines and diols in one pot.
Article
Chemistry, Multidisciplinary
Mingqing Huang, Haiyang Huang, Mengyao You, Xinxin Zhang, Longgen Sun, Chao Chen, Zhichao Mei, Ruchun Yang, Qiang Xiao
Summary: A direct air-oxidized strategy for the synthesis of benzo[b]phosphole oxides was developed in this study. Arylphosphine oxides were transformed into phosphinoyl radicals, which were further combined with various alkynes to achieve the desired products. DFT calculations revealed the mechanism of phosphinoyl radical formation.
Article
Chemistry, Multidisciplinary
Anwei Wang, Jiayin Huang, Chunsheng Zhao, Yu Fan, Junfeng Qian, Qun Chen, Mingyang He, Weiyou Zhou
Summary: This study demonstrates an innovative strategy for the aerobic oxidation of C(sp(3))-H bonds using gamma-valerolactone. By optimizing the reaction conditions and utilizing specific catalysts, efficient oxidation of C(sp(3))-H bonds is achieved with good chemoselectivity in certain cases.
Article
Chemistry, Multidisciplinary
Shun Li, Likai Tong, Zhijian Peng, Bo Zhang, Xiuli Fu
Summary: Sulfide compounds show promise as electrocatalysts for water splitting, but their performance is limited by factors such as limited active sites and hindered substance transport. This study successfully prepared a high-entropy sulfide (ZnCoMnFeAlMg)(9)S-8, which reduced grain size and increased specific surface area, enabling the realization of a dual-functional catalyst with multiple catalytic sites. High entropy also modulated the electronic properties of sulfides, reducing the potential energy barrier for hydrolysis. This research introduces a new approach for functionalizing high entropy nanomaterials and improves the performance of water splitting catalysts.
