Article
Chemistry, Multidisciplinary
Tianze Zhang, Hanmin Huang
Summary: The catalytic C(sp(3))-C(sp(3)) coupling of alkyl halides and tertiary amines offers a promising tool for the rapid decoration of amine skeletons. We developed a metal-free photocatalytic system for the aminomethylation of alkyl halides through radical-involved C(sp(3))-C(sp(3)) bond formation, allowing for the synthesis of sterically congested tertiary amines that are of interest in organic synthesis but not easily prepared by other methods.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Wongyu Lee, Dongwook Kim, Sangwon Seo, Sukbok Chang
Summary: In this study, a polar-radical relay strategy is reported for the alpha-C-H amination of cyclic amines using N-chloro-N-sodio-carbamates. The strategy involves the in situ generation of a cyclic iminium intermediate using N-iodosuccinimide (NIS) as an oxidant, followed by a series of polar and radical reactions to achieve controlled C-N bond formation. The method provides a facile and regioselective access to a broad range of alpha-amino cyclic amines and demonstrates excellent applicability for functionalization of biologically relevant compounds.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Mikhail Feofanov, Vladimir Akhmetov, Ryo Takayama, Konstantin Amsharov
Summary: A novel catalyst-free approach to benzoannulated oxygen-containing heterocycles from fluorinated oligophenylenes is reported, utilizing potassium tert-butoxide as an O2- synthon. The radical nature of the reaction enables nucleophilic substitution and facilitates de-tert-butylation, allowing for multiple annulations and the synthesis of ladder-type O-heteroacenes and oligodibenzofurans.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Prithwish Ghosh, Na Yeon Kwon, Youjung Byun, Neeraj Kumar Mishra, Jung Su Park, In Su Kim
Summary: In this study, a cobalt(II)-catalyzed method for C-H alkylation and acylation of N-heterocycles using 1,4-dihydropyridines (DHPs) as alkylating and acylating agents was reported. The combination of KBrO3 and a Co(II) catalyst successfully generated alkyl and acyl radicals from DHPs. This method was applicable to various heterocycles and demonstrated selectivity in modifying drug candidates and synthesizing bioactive molecules on a gram scale.
Article
Chemistry, Multidisciplinary
Byeongseok Kweon, Changha Kim, Seonyul Kim, Sungwoo Hong
Summary: An efficient strategy for remote C-H pyridylation of hydroxamates with excellent ortho-selectivity has been developed by designing new photon-absorbing O-aryl oxime pyridinium salts. The photoexcitation of oxime pyridinium intermediates generates iminyl radicals via photolytic N-O bond cleavage, allowing for the installation of pyridyl rings at the gamma-CN position. This novel synthetic approach offers advantages in terms of efficiency, simplicity, and broad functional group tolerance under mild and metal-free conditions.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Myojeong Kim, Euna You, Jieun Kim, Sungwoo Hong
Summary: An efficient method for functionalizing pyridines and quinolines through radical-mediated reactions has been developed, allowing for selective modification of heteroatom positions.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Huaipu Yan, Qian Liao, Yuqing Chen, Gagik G. G. Gurzadyan, Binghui Lu, Chao Wu, Lei Shi
Summary: Co-porphines were discovered to be highly efficient MHAT catalysts for chemoselective allene functionalization under photoirradiation with a loading of only 0.01 mol %. The combination of photo Co-MHAT and Ti catalysis enabled successful carbonyl allylation, providing expedient access to beta-functionalized homoallylic alcohols in over 100 examples with exceptional regio- and diastereoselectivity. Mechanism studies supported the key role of selectively transferring hydrogen atoms from cobalt hydride to allenes and generating allyl radicals in the catalytic cycle.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Allen F. Prusinowski, Henry C. Sise, Taylor N. Bednar, David A. Nagib
Summary: A radical aza-Heck cyclization strategy has been developed to synthesize functionally rich products with four contiguous C-heteroatom bonds. This multicatalytic strategy enables rapid synthesis of medicinally relevant motifs and the mechanistic insights reveal the cooperation of three distinct photocatalytic cycles.
Article
Chemistry, Multidisciplinary
Timon Kurzawa, Reinhold Zimmer, Ernst-Ulrich Wuerthwein, Hans-Ulrich Reissig
Summary: In this study, the acetic anhydride-promoted reaction of a model pyrimidine N-oxide to a 4-acetoxymethyl-substituted pyrimidine derivative was investigated. The experiments and quantum chemical calculations revealed that a (pyrimidin-4-yl)methyl radical is a key species in the rearrangement and that the reaction proceeds through radical intermediates. The calculations also showed that both concerted [3,3]-sigmatropic rearrangements and stepwise processes are energetically feasible.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Environmental Sciences
Yanhui Sun, Lin Liu, Ming Li, Xiaoxiao Chen, Fei Xu
Summary: Vanillin and vanillic acid are two lignin pyrolysis products generated by biomass combustion. The gas-phase oxidation mechanisms of vanillin and vanillic acid initiated by OH/NO3 radicals were investigated using density functional theory. The primary reactions involve OH/NO3 addition and H-atom abstraction, leading to the formation of various oxidation products. The total rate constants and atmospheric lifetimes of the oxidation processes were calculated, providing valuable information for further experimental research.
Article
Chemistry, Multidisciplinary
Chang-Yin Tan, Myojeong Kim, Inyoung Park, Yuhyun Kim, Sungwoo Hong
Summary: A unified strategy for the deoxygenative or desulfurative pyridylation of various alcohols and thiols has been developed using a single-electron transfer (SET) process mediated by frustrated Lewis pairs (FLPs). The method involves the formation of FLPs between pyridinium salts and PtBu3, and the generation of alkyl radicals through the ionic coupling of phosphine radical cations with in situ generated xanthates. Visible-light irradiation enhances the reaction efficiency. This method offers a previously unrecognized opportunity for the selective heteroarylation of alcohols and thiols with diverse functional groups.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Jingyang Qin, Manuel Barday, Samikshan Jana, Nil Sanosa, Ignacio Funes-Ardoiz, Christopher J. Teskey
Summary: A mild and selective hydropyridylation method for dienes was reported, allowing for traceless coupling of dienes on a wide range of pyridine substrates. The method showed good functional group tolerance, making it suitable for late-stage functionalization. The mechanistic pathway involved non-reversible hydrogen atom transfer, resulting in a reaction that was uniquely selective for dienes in the presence of other olefins.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Jinping Liang, Ling Fu, Kai Gao, Xiaoguang Duan
Summary: This study investigates the activation mechanism of peroxymonosulfate (PMS) through the synthesis of Co-K-N-O-C composites. The results show that the low-valent cobalt species, especially Co0, greatly enhance the generation of radicals, thereby improving the degradation efficiency of recalcitrant contaminants.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Chemistry, Multidisciplinary
Franz-Lucas Haut, Riccardo S. Mega, Joan V. Estornell, Ruben Martin
Summary: We describe a catalytic intramolecular decarboxylative/desulfonylative sp(3) allylation triggered by sulfinate salts under light irradiation. The reaction likely proceeds through a non-classical, radical-polar crossover mechanism, providing a rapid and reliable method to access valuable allyl architectures from readily available precursors. The protocol is characterized by its simplicity, scalability, and the use of abundant, commercially available catalysts.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Maximilian Scheruebl, Constantin G. Daniliuc, Armido Studer
Summary: The article introduces the application of arynes as radical acceptors, showing how the stable radical TEMPO can react with different ortho-substituted benzynes to generate aryl radicals for subsequent cyclizations, eventually being trapped by TEMPO. This method provides a novel approach for the convenient synthesis of various dihydrobenzofurans, oxindoles, and sultones.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Gastroenterology & Hepatology
Lihong Mao, Chaoqun Li, Xiaoyu Wang, Mingyu Sun, Yifan Li, Zihan Yu, Binxin Cui, Gaoyue Guo, Wanting Yang, Yangyang Hui, Xiaofei Fan, Jie Zhang, Kui Jiang, Chao Sun
Summary: This study found that in decompensated cirrhosis, low subcutaneous adipose tissue index (SATI) and concurrent total adipose tissue index (TATI) were associated with an increased risk of frailty.
JOURNAL OF CLINICAL AND TRANSLATIONAL HEPATOLOGY
(2023)
Article
Allergy
Qiuyan Liang, Jinrong Fu, Xiang Wang, Lijuan Liu, Wenfeng Xiao, Yajing Gao, Lan Yang, Hongmiao Yu, Xueru Xie, Zikun Tu, Saihua Huang, Xiao Han, Liling Qian, Yufeng Zhou
Summary: This study identified 372 differentially expressed circRNAs in peripheral blood mononuclear cells (PBMCs) of children with asthma. Among them, a circRNA called circS100A11 was highly expressed in monocytes and significantly upregulated in children with asthma. Further experiments demonstrated that circS100A11 promoted M2a macrophage activation by enhancing translation of its host gene, S100A11, and exacerbated lung inflammation in a mouse model of asthma. The study also found that circS100A11 competitively bound to CAPRIN1 to promote S100A11 translation, thereby enhancing M2a macrophage activation.
Article
Limnology
Xu Yan, Min Cao, Qiang Fu, Ning Yang, Ningning Wang, Lin Song, Chao Li
Summary: In this study, lncRNAs in the intestine of black rockfish after Edwardsiella tarda infection were identified and analyzed. Results showed that these lncRNAs were significantly regulated and involved in metabolic and immune-related pathways. Co-expression of lncRNAs and mRNAs with metabolic and immunity functions were also found. This research provides a foundation for further investigation of the regulatory roles of lncRNAs in the intestinal immune response of black rockfish.
JOURNAL OF OCEANOLOGY AND LIMNOLOGY
(2023)
Article
Pediatrics
Lingyu Lai, Yong Lu, Zhimin Xi, Fang Liu, Liling Qian, Libo Wang, Quming Zhao
Summary: This study presented two cases of Bronchial Dieulafoy's disease (BDD) in children, diagnosed by bronchial arteriography and CTA. Both patients underwent successful bronchial artery embolization (BAE) and no recurrence of hemoptysis was observed during the follow-up period. It highlights the importance of considering BDD in children with hemoptysis and endobronchial protrusion.
TRANSLATIONAL PEDIATRICS
(2023)
Article
Fisheries
Chengbin Gao, Xin Cai, Alan J. Lymbery, Le Ma, Min Cao, Chao Li
Summary: An integrative analysis was conducted in black rockfish intestine and spleen after bacterial infection, revealing a cooperation between the immune genes of the two organs. Two key immune genes and their related non-coding RNAs were identified in the regulation mechanism of the intestine-spleen axis during different bacterial infections. These findings provide insights into the immune response in black rockfish.
Article
Fisheries
Zhe Liu, Peng Liu, Tong Cui, Xuan Chen, Beibei Wang, Chengbin Gao, Zhongyi Wang, Chao Li, Ning Yang
Summary: Six IKK genes were identified in turbot, and they were widely expressed in various tissues. After bacterial infection, these genes showed different expression patterns in mucosal tissues, indicating their potential roles in maintaining mucosal barrier integrity. Protein-protein interaction network analysis revealed that most interacting proteins of IKK genes were related to the NF-kappa B signaling pathway. Functional experiments confirmed the involvement of SmIKK alpha/SmIKK alpha 2/SmIKK beta in the activation of NF-kappa B in turbot.
FISH & SHELLFISH IMMUNOLOGY
(2023)
Article
Fisheries
Chengbin Gao, Xin Cai, Le Ma, Peng Sun, Chao Li
Summary: In this study, the regulatory roles of circRNA-related ceRNA networks in the spleen immune system of black rockfish infected with A. salmonicida were investigated. The results revealed 39 differentially expressed circRNAs during the infection, which were significantly enriched in multiple immune-related pathways. These findings suggest a potential role of circRNA in the antibacterial immune response of fish.
FISH & SHELLFISH IMMUNOLOGY
(2023)
Article
Cell Biology
Yiping Liu, Xuefeng Ge, Chao Li, Ting Xue
Summary: A continuous intestine cell line named SMI was established from turbot using tissue explant technique and had undergone more than 60 subcultures. The SMI cell line had a diploid chromosome number of 44 and showed characteristics of epidermal cells. It could be used as an ideal platform to explore gene function in vitro and exhibited immune functions similar to the intestinal epithelium in vivo.
IN VITRO CELLULAR & DEVELOPMENTAL BIOLOGY-ANIMAL
(2023)
Article
Biochemistry & Molecular Biology
Chengbin Gao, Xin Cai, Le Ma, Ting Xue, Chao Li
Summary: In this study, the TNF alpha was characterized and its roles in the immune system of black rockfish during bacterial infections were explored. The results showed that Ss_TNF alpha was significantly up-regulated in the spleen and intestine after infections, while down-regulated in PBLs. The expression patterns of other inflammatory cytokines were also observed.
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
(2023)
Article
Chemistry, Multidisciplinary
Wan-Chen Cindy Lee, Jingyi Wang, Yiling Zhu, X. Peter Zhang
Summary: Asymmetric radical bicyclization processes using metalloradical catalysis have been developed to construct chiral chromanones and chromanes with fused cyclopropanes. Through optimization of the chiral amidoporphyrin ligand platform, a Co(II)-metalloradical system can activate different alkene functionalities under mild conditions for effective radical bicyclization, delivering desired products with high yields and excellent control of stereoselectivities. Computational and experimental studies reveal the stepwise radical mechanisms involved in the Co(II)-catalyzed bicyclization processes.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Computer Science, Information Systems
Jian Cheng, Quanyuan Feng, Chao Li, Wenxiu Yang
Summary: In this paper, a new run-time monitoring technique is proposed to detect hardware Trojans (HT) on working field-programmable gate array (FPGA), which can enhance the hardware security of IoT devices. The technique places multiple temperature sensors on FPGA and collects their values at each time interval. A predictive model is constructed to estimate the real-time distribution of sensor frequency. If the difference between the predicted value and the real one exceeds a dynamically updated threshold, an HT activation is reported. The experiment results demonstrate that the technique achieves high detection accuracy (>= 98%), low false negative ratio (<= 1.5%), and zero false positive ratio under various FPGA HT benchmarks.
Article
Biochemistry & Molecular Biology
Donglei Sun, Xin Qi, Haishen Wen, Chao Li, Jianlong Li, Jiwei Chen, Zexin Tao, Mingxin Zhu, Xiaoyan Zhang, Yun Li
Summary: A new yellow-mutant northern snakehead with market-favoured yellow skin was discovered in China. It was confirmed to be an albino with a non-sense mutation in slc45a2 gene as the causation for the yellow skin. Comparative transcriptomic analysis revealed the potential involvement of fibroblasts in pigmentation in fish.
Article
Biochemistry & Molecular Biology
Min Cao, Ting Xue, Huijun Huo, Xiaoyan Zhang, Ning Ning Wang, Xu Yan, Chao Li
Summary: Spatial transcriptomes were used to study the transcriptomic landscape in the posterior intestine of Sebastes schlegelii following Edwardsiella piscicida infection. A molecular regionalization of the posterior intestine was observed in the healthy condition. After bacterial infection, immune-related genes were predominantly found in the mucosa layer. The expression of regeneration-related genes suggested the constant proliferation of new cells in response to pathogen invasion, while increasing microbiota communities indicated their role in maintaining intestinal integrity and shaping the mucosal immune system.
Article
Construction & Building Technology
Senyu Lou, Yaou Zhang, Chao Li, Jingjing Chen
Summary: This paper focuses on the Largos of the Macau Peninsula and categorizes their main functions as serving the community, facilitating traffic, and promoting religious culture through historical combing and field research. A spatial syntactic theory is applied to establish a model, using three syntactic parameters - synergy, integration, and choice - to interpret the analysis results. Based on the syntactic parameters, the results are divided into four categories, and improvement strategies are proposed for the selected spaces that require enhancements. Taking Macau's Largos as an example, this paper aims to provide a reference for the effective renewal of urban micro-spaces and small public spaces by applying space syntax analysis.
Article
Green & Sustainable Science & Technology
Chao Li, Kexin Yi, Shaogang Hu, Wulin Yang
Summary: A novel microbial separator was developed for air-breathing microbial fuel cells to protect cathodic catalytic activity. This concept effectively prevents biofouling, improves the stability of the cells, enhances chemical oxygen demand removal efficiency, prolongs lifespan, and reduces economic costs.
ENVIRONMENTAL SCIENCE AND ECOTECHNOLOGY
(2023)