Review
Chemistry, Organic
Da-Liang Zhu, Jie Li, David James Young, Yanqing Wang, Hong-Xi Li
Summary: Organic transformations using carbonyl-photoredox/metal dual catalysis have gained significant attention lately. Carbonyl photosensitizers, which are abundant and inexpensive, act as effective agents for single electron, energy, or hydrogen atom transfer to induce metal-catalyzed cross-coupling and dicarbofunctionalization of olefins. This review summarizes literature reports on metal-catalyzed photocatalytic coupling reactions from 2020 to mid-2023, focusing on C-C and C-heteroatom bond forming reactions.
ASIAN JOURNAL OF ORGANIC CHEMISTRY
(2023)
Article
Chemistry, Physical
Alberto Lopez-Magano, Borja Ortin-Rubio, Inhar Imaz, Daniel Maspoch, Jose Aleman, Ruben Mas-Balleste
Summary: The functionalization of an imine-based layered covalent organic framework has allowed the obtention of a heterobimetallated material with photoactive Ir and Ni fragments immobilized within the porous structure. These heterogeneous light-mediated reactions showed enhanced activity and stability compared to analogous homogeneous systems.
Article
Nanoscience & Nanotechnology
Yefei Wang, Zhen Zhou, Liang Zhao, Cheng He, Wenlong Sun, Chunying Duan
Summary: By stabilizing highly active carbenes in metal-organic frameworks, efficient acceleration of carbene migratory insertion and C-H bond activation was achieved, leading to inert alkane functionalization. The first-time isolation and structural characterization of Ir-III-carbene intermediates were successfully conducted.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Review
Biochemistry & Molecular Biology
Alejandro Torregrosa-Chinillach, Rafael Chinchilla
Summary: This review summarizes the recent advances in oxidative dehydrogenation of C-N and C-O bonds, leading to C=N and C=O bonds, respectively, using air or pure oxygen as oxidants and metal-free homogeneous or recyclable heterogeneous photocatalysts under visible light irradiation.
Review
Chemistry, Multidisciplinary
Qian-Yu Li, Yuhang He, Yu-Mei Lin, Lei Gong
Summary: Photo-induced methylation is a valuable method for introducing methyl groups into organic molecules, especially in pharmaceutical chemistry. This article provides a comprehensive review of photochemical strategies for direct and selective methylation of different types of C-H bonds. These advancements are expected to drive progress in organic synthesis, photocatalysis, and pharmaceutical development.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Review
Chemistry, Physical
DeGuang Liu, ZheYuan Xu, HaiZhu Yu, Yao Fu
Summary: In recent decades, density functional theory (DFT) calculations have been extensively used to investigate the mechanisms of transition metal-catalyzed C-O activation reactions. These studies provide valuable insights into the structure-reactivity/selectivity correlations through theoretical simulations and energy profile analysis. Alcohols, derived from biomass and affordable, have been extensively studied in organic synthesis. This review provides a brief overview of DFT studies conducted since 2017 on C-OH bond activation of alcohols catalyzed by transition metals, covering four main categories: free radical cleavage, metal insertion, nucleophilic attack, and β-OH elimination. Promising strategies and future research directions in this field are also discussed.
Article
Chemistry, Multidisciplinary
Cheng Huang, Jia Qiao, Rui-Nan Ci, Xu-Zhe Wang, Yang Wang, Jing-Hao Wang, Bin Chen, Chen-Ho Tung, Li-Zhu Wu
Summary: The study presents a method using semiconductor quantum dots as photocatalysts to directly couple allylic C(sp(3))-H bonds with alpha-amino C-H bonds or heteroarenes under sunlight irradiation. The protocol does not require additional oxidants or reductants, pre-functionalization of coupling partners, and produces hydrogen as a byproduct. This represents the first direct alkylation and arylation of allylic C(sp(3))-H bonds with hydrogen evolution powered by solar energy, showcasing outstanding efficiency, selectivity, step- and atom-economy.
Article
Chemistry, Physical
Conor Waldt, Hansel Montalvo-Castro, Abdulrahman Almithn, Alvaro Loaiza-Orduz, Craig Plaisance, David Hibbitts
Summary: C-O hydrogenolysis can be selectively activated by transition metal phosphides, such as Ni2P and Ni12P5, which show higher selectivities toward hindered C-O bonds compared to pure Ni catalysts. In this study, DFT calculations were used to investigate other transition metal phosphides' selectivity towards hindered C-O activation. Results showed a nearly ubiquitous shift in selectivity towards hindered C-O activation for all the phosphides compared to their pure metal counterparts, with Ni2P and Pd2P predicted to exhibit high selectivity towards 3C-O activation. The selectivity shifts can be attributed to the electronegativity of the metal and charge transfer between P and nearby metal atoms.
JOURNAL OF CATALYSIS
(2023)
Article
Chemistry, Organic
Valeriia Iziumchenko, Vladimir Gevorgyan
Summary: This review summarizes recent developments in the field of dual light-excited ketone/transition-metal catalysis, which enables versatile functionalizations of C-H or C-X bonds through the use of triplet ketone as a hydrogen-atom-abstracting agent, a single-electron acceptor, or a photosensitizer.
Article
Chemistry, Multidisciplinary
Bhushan A. Baviskar, Prashant V. Ajmire, Deshraj S. Chumbhale, Mohammad Sadat Khan, Vitthal G. Kuchake, Madhavi Singupuram, Purushottam R. Laddha
Summary: Research on transition metal catalysis, specifically exploring the applications of abundant first row transition elements for C-C coupling reactions, is rapidly advancing. The Suzuki-Miyaura coupling reaction, particularly catalyzed by nickel, has attracted significant interest from organic chemists in recent decades. However, the environmental concern of halogen waste has prompted the exploration of alternative electrophiles, such as carboxylic acid derivatives, phenol derivatives, and amides, to replace organic halides in traditional Suzuki coupling reactions. This strategy involves activating C-O and C-N bonds to form C-C coupling products. The current focus is on developing various Ni-based catalytic systems that activate C-O and C-N bonds to achieve successful Suzuki coupling reactions, with a recent emphasis on green metrics.
SUSTAINABLE CHEMISTRY AND PHARMACY
(2023)
Review
Chemistry, Applied
Guodong Zhang, Yihan Cheng, Matthias Beller, Feng Chen
Summary: The recent research focus on utilizing carbon dioxide for organic synthesis has led to advancements in carboxylations using visible light photoredox and transition-metal dual catalysis, creating new pathways for constructing carboxylates.
ADVANCED SYNTHESIS & CATALYSIS
(2021)
Article
Chemistry, Physical
Qigang Li, Xiaoqiang Li, Yifei Ling, Jiaxin Liu, Jun Yang
Summary: An activation paradigm for the sp3-C-Si bond of silanols via a visible-light photoinduced open-shell pathway has been developed. It proceeded through base metal catalyzed ligand-to-metal charge-transfer (LMCT) and subsequent beta-scission process. Various alkyl radicals can be generated under mild conditions.
Article
Chemistry, Multidisciplinary
Guanfeng Ji, Liang Zhao, Jianwei Wei, Junkai Cai, Cheng He, Zenggang Du, Wei Cai, Chunying Duan
Summary: The article introduces a novel multiphoton excitation approach to activate inert C(sp(3))-H bonds and oxygen, which enables oxidation reactions and the development of sustainable synthetic strategies through integration of various events.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Review
Chemistry, Inorganic & Nuclear
Siva Sankar Murthy Bandaru, Jagrut Shah, Shatrughn Bhilare, Carola Schulzke, Anant R. Kapdi, Julien Roger, Jean-Cyrille Hierso
Summary: This review focuses on the applications of different ferrocenylphosphine ligands in transition metal-catalyzed cross-coupling strategies, including the asymmetric synthesis using chiral ferrocenyl phosphines. It also discusses the latest advances in the chemistry of symmetric achiral di- and polyphosphine ferrocene-based ligands related to metal-catalyzed bond-forming reactions. A cumulative table compiling significant work in this field is provided.
COORDINATION CHEMISTRY REVIEWS
(2023)
Review
Chemistry, Applied
Xiaofan Cui, Remi Chauvin, Chao Pi, Yangjie Wu, Xiuling Cui
Summary: This review presents recent progress in the use of vinylene carbonate as a reactant in transition metal-catalyzed C-H bond activation/cyclization reactions. By analyzing and comparing different reaction models, it highlights the advantages of using vinylene carbonate as a surrogate for ethynol and other reactants, and discusses related mechanisms and synthetic applications.
ADVANCED SYNTHESIS & CATALYSIS
(2023)
Article
Public, Environmental & Occupational Health
Allyson J. Gallant, Paul Flowers, Karen Deakin, Nicola Cogan, Susan Rasmussen, David Young, Lynn Williams
Summary: This study aimed to enhance influenza vaccination uptake among adults with chronic respiratory conditions by using the Behaviour Change Wheel (BCW) to specify intervention content. The study identified barriers and enablers to vaccination through focus groups, interviews, and surveys. Factors such as perceptions of vaccine side effects, time constraints, and fear of needles were found to be common barriers, while enablers included protection from influenza, reminders, and support from others. Based on the findings, the study proposed a suite of multi-level intervention components involving diverse actors, recipients, and settings to enhance vaccination uptake.
PSYCHOLOGY & HEALTH
(2023)
Article
Pediatrics
Elizabeth M. A. Henderson, David Tappin, David Young, Donata Favretto, Helen Mactier
Summary: This study aimed to examine the correlation between postnatal maternal self-report of alcohol consumption during pregnancy and PEth concentration measured from dried blood spot (DBS) obtained on day 5 of life. However, the study found that PEth concentration measured from DBS obtained on day 5 of life does not reliably identify modest prenatal alcohol exposure (PAE) after 36 weeks' gestation from maternal self-report.
ARCHIVES OF DISEASE IN CHILDHOOD
(2023)
Article
Chemistry, Organic
Da-Liang Zhu, Jie Li, Qi Wu, Yanqing Wang, David J. Young, Hong-Xi Li
Summary: The efficient etherification of alcohols with aryl bromides can be promoted by sodium tert-butoxide at room temperature. This simple procedure offers a practical pathway to aryl alkyl ethers in good yields without the need for any transition metal species.
SYNTHESIS-STUTTGART
(2023)
Article
Chemistry, Medicinal
Mengyao Feng, Fuyuan Liu, Ningwen Yang, Jiayao Yu, Wei Yang, David James Young, Xiang-Qian Cao, Hong-Xi Li, Zhi-Gang Ren
Summary: A heterobimetallic coordination polymer [Au4(dppmt)4(AgCl)2]n (1) incorporating an in situ generated P-S ligand (dppmtH) was synthesized. The structure of 1 contains a one-dimensional helical Au-Au chain. Coordination polymer 1 exhibited a rapid, selective, reversible, and visible vapor chromic response on exposure to methanol (MeOH) vapor.
ACS MEDICINAL CHEMISTRY LETTERS
(2023)
Article
Biochemistry & Molecular Biology
Qing Li, Bo-Wei Xu, Yi-Ming Zou, Ru-Jie Niu, Jin-Xiang Chen, Wen-Hua Zhang, David James. Young
Summary: In this study, nanoscale two-dimensional Fe-II- and Co-II-based metal-organic frameworks (NMOFs) were shown to have an anticancer effect in the tumor microenvironment. These NMOFs can catalyze the production of hydroxyl radicals (center dot OH) and O-2 in the presence of H2O2, and consume O-2 to produce singlet oxygen (O-1(2)) through photodynamic therapy. Both center dot OH and O-1(2) are reactive oxygen species (ROS) that inhibit cancer cell proliferation.
Article
Biochemistry & Molecular Biology
Kiyoshi Fujisawa, Yui Kobayashi, Mitsuki Okano, Ryota Iwabuchi, Shiori Kondo, David James Young
Summary: Coordination polymers of transition metal ions, such as silver(I), are important in coordination chemistry. Silver(I) coordination polymers are often insoluble in common solvents, making it difficult to analyze them in solution. However, by using a tetramethyl-substituted bipyrazole ligand, we have synthesized more soluble silver(I) complexes with coordinated ions CF3CO2- and CF3SO3-. We determined the structures of these complexes and studied their solution behavior using various spectroscopic techniques.
Article
Chemistry, Inorganic & Nuclear
Kiyoshi Fujisawa, Aoba Yamada, Moeka Koyama, David James Young
Summary: Tridentate, planar nitrogen containing ligands based on pyridine and pyrazoles were synthesized and their solid-state structures were analyzed. Copper(II) chlorido and trifluoromethanesulfonato complexes were formed with these ligands and their coordination geometries were studied. The UV-Vis spectra of the complexes showed pi-pi* transition band red-shift and d-d transition bands at similar energy, indicating structural changes in the solution-state. EPR spectroscopy supported the findings.
INORGANICA CHIMICA ACTA
(2023)
Article
Chemistry, Organic
Da-Liang Zhu, Jie Li, David James Young, Yanqing Wang, Hong-Xi Li
Summary: This paper presents a mild strategy for aminating aryl halides with anilines using dual photoredox and nickel catalysis. Thioxanthen-9-one, an inexpensive and readily available compound, greatly enhanced this cross-coupling reaction, yielding a diverse range of diarylamines in good yields (41-93%) at room temperature. The reaction could be performed under compact fluorescent lamp light or sunlight and was tolerant of various functional groups. It was successfully applied to the synthesis of natural products and drug molecules, even at a gram-scale. The mechanism involves several steps including oxidative addition, transmetalation, energy transfer, and reductive elimination.
ORGANIC CHEMISTRY FRONTIERS
(2023)
Article
Chemistry, Inorganic & Nuclear
Shengnan Hu, Sisi Yan, Yuanyuan Hu, David James Young, Hong-Xi Li, Chengrong Lu, Jing-Hui He, Zhi-Gang Ren
Summary: Reliable and sensitive detection of sub-ppm level, ultra-low humidity is critical for a number of important technologies. We report a heteronuclear Au2Cu2 cluster complex that can undergo reversible transformations and has photoluminescent properties in different environments. The crystals of the complex can detect ultralow humidity of 0.21 ppm (w/w).
INORGANIC CHEMISTRY FRONTIERS
(2023)
Article
Chemistry, Inorganic & Nuclear
You-Hui Zhao, Hai-Yan Li, David James Young, Xiangqian Cao, Da-Liang Zhu, Zhi-Gang Ren, Hong-Xi Li
Summary: Earth-abundant copper(I) coordination complexes have been developed as visible-light photocatalysts for the intermolecular atom-transfer radical addition reactions. Four heteroleptic bis-chelate Cu(I) complexes were synthesized and showed broad absorption in the visible spectrum. These complexes facilitated efficient reactions with CBr4, CCl3Br, and CHI3, yielding high product yields up to 91%. The substitution on the phpz ligand had a significant impact on the absorption, emission, redox potential, and photocatalytic activity.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Inorganic & Nuclear
Mengyao Feng, Fuyuan Liu, Ningwen Yang, Jiayao Yu, Wei Yang, David James Young, Xiang-Qian Cao, Hong -Xi Li, Zhi-Gang Ren
Summary: A heterobimetallic coordination polymer [Au-4(dppmt)(4)(AgCl)2(]) n (1) with an in situ generated P-S ligand (dppmtH) was synthesized. The structure of 1 contains a helical Au-Au chain connected by [Au(2()dppmt)(2)] dimers. Upon excitation at 343 nm, 1 exhibited cyan phosphorescent emission at QY = 22.3% and t = 0.78 μs. Coordination polymer 1 exhibited a rapid, selective, reversible, and visible vaporchromic response on exposure to methanol vapor, with its emission shifting to a more intense green at QY = 46.8% and t = 1.24 μs.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Zhi-Hao Zhang, Jia-Lu Ge, Yan Li, Qing Li, Pin-Pin Ma, Xiao-Yan Tang, Wen-Hua Zhang, David J. Young
Summary: Developing porous materials for efficient capture of I-2 is important for the sequestration and storage of radioactive iodine towards clean nuclear energy. In this study, three structurally identical two-dimensional (2D) metal-organic frameworks (MOFs) were prepared, and one of the MOFs showed the highest adsorption capacity for I-2.
Article
Biochemistry & Molecular Biology
Shan He, Yixiao Wu, Yang Zhang, Xuan Luo, Christopher T. Gibson d Jingrong Gao, Jingrong Gao, Matt Jellicoe, Hao Wang, David J. Young, Colin L. Raston
Summary: Biodegradable cellulose films derived from kombucha, processed using a vortex fluidic device, show increased mechanical strength due to intense micromixing and high shear stress of the liquid film. The films retain their biodegradability and degrade within 5 days.
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
(2023)
