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Deciphering fungal metabolon coupling tandem inverse-electrondemand Diels-Alder reaction and semipinacol rearrangement for the biosynthesis of spiro polycyclic alkaloids

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Science China Chemistry 2025年第1期68卷 288-296页

作者： Shuai Liu Wen-Qiang Xu Ying-Tong Di Man-cheng Tang Ding-Kang chen ming-ming Cao Yao-Wen Chang Hong-Yu Tang Chun-Mao Yuan Jun-Bo Yang Zhi-Li Zuo Han Guo Zi-Fei Xu Ying Zeng Yun-Dong Wu Xiao-Jiang Hao Key Laboratory of Phytochemistry and Natural Medicines (Chinese Academy of Sciences) Kunming Institute of Botany Chinese Academy of Sciences University of Chinese Academy of Sciences Lab of Computational Chemistry and Drug Design State Key Laboratory of Chemical Oncogenomics Peking University Shenzhen Graduate School Shenzhen Bay Laboratory State Key Laboratory of Microbial Metabolism School of Life Sciences & Biotechnology Shanghai Jiao Tong University State Key Laboratory of Functions and Applications of Medicinal Plants Guizhou Medical University Molecular Biology Experimental Center Germplasm Bank of Wild Species in Southwest China Kunming Institute of Botany Chinese Academy of Sciences Yunnan Key Laboratory for Wild Plant Resources Kunming Institute of Botany Chinese Academy of Sciences Research Unit of Chemical Biology of Natural Anti-Virus Products Chinese Academy of Medical Sciences

In the intricate process of natural product biosynthesis, a metabolon can enhance metabolic flux by associating sequential enzymes. A fungal metabolon, comprising of flavin-dependent monooxygenase Spe F and P450 monooxygenase Spe G, is identified in the biosynthesis of spiro polycyclic alkaloids(+)-notoamide B and its diastereomer(+)-versicolamide B. Using notoamide E as a substance, Spe F/Spe G metabolon can control the stereoselectivity of its 2,3-epoxidation, followed by hydrogen atom ion at C-17 to generate reactive epoxide tau-m A with dienyl iminium unit. Subsequently,(+)-notoamide B and(+)-versicolamide B are produced via tandem nonenzymatic inverse-electron-demand Diels-Alder reaction and semipinacol rearrangement. This provides the first example of metabolon in the biosynthesis of spiro-prenylated indole alkaloids.

关键词： metabolon Diels-Alder reaction semipinacol rearrangement biosynthesis notoamides spiro polycyclic alkaloids

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Chondroitinase ABC combined with Schwann cell transplantation enhances restoration of neural connection and functional recovery following acute and chronic spinal cord injury

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Neural Regeneration Research 2025年第5期20卷 1467-1482页

作者： Wenrui Qu Xiangbing Wu Wei Wu Ying Wang Yan Sun Lingxiao Deng Melissa Walker chen chen Heqiao Dai Qi Han Ying Ding Yongzhi Xia George Smith Rui Li Nai-Kui Liu Xiao-ming Xu Spinal Cord and Brain Injury Research Group Stark Neurosciences Research InstituteDepartment of Neurological SurgeryIndiana University School of MedicineIndianapolisINUSA Department of Hand Surgery the Second Hospital of Jilin UniversityChangchunJilin ProvinceChina Shriners Hospitals Pediatric Research Center Temple University School of MedicinePhiladelphiaPAUSA Department of Anatomy&Cell Biology Indiana University School of MedicineIndianapolisINUSA

Schwann cell transplantation is considered one of the most promising cell-based therapy to repair injured spinal cord due to its unique growth-promoting and myelin-forming properties.A the Food and Drug Administration-approved Phase I clinical trial has been conducted to evaluate the safety of transplanted human autologous Schwann cells to treat patients with spinal cord injury.A major challenge for Schwann cell transplantation is that grafted Schwann cells are confined within the lesion cavity,and they do not migrate into the host environment due to the inhibitory barrier formed by injury-induced glial scar,thus limiting axonal reentry into the host spinal *** we introduce a combinatorial strategy by suppressing the inhibitory extracellular environment with injection of lentivirus-mediated transfection of chondroitinase ABC gene at the rostral and caudal borders of the lesion site and simultaneously leveraging the repair capacity of transplanted Schwann cells in adult rats following a mid-thoracic contusive spinal cord *** report that when the glial scar was degraded by chondroitinase ABC at the rostral and caudal lesion borders,Schwann cells migrated for considerable distances in both rostral and caudal *** Schwann cell migration led to enhanced axonal regrowth,including the serotonergic and dopaminergic axons originating from supraspinal regions,and promoted recovery of locomotor and urinary bladder ***,the Schwann cell survival and axonal regrowth persisted up to 6 months after the injury,even when treatment was delayed for 3 months to mimic chronic spinal cord *** findings collectively show promising evidence for a combinatorial strategy with chondroitinase ABC and Schwann cells in promoting remodeling and recovery of function following spinal cord injury.

关键词： axonal regrowth bladder function chondroitinase ABC functional recovery glial scar lentivirus migration Schwann cell spinal cord injury transplantation

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Halogen composition and heterogeneity in the continental lithospheric mantle

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Science China Earth Sciences 2025年第1期68卷 310-314页

作者： Chunfei chen State Key Laboratory of Geological Processes and Mineral Resources School of Earth Sciences China University of Geosciences

1. Introduction Halogens, including fluorine(F), chlorine(Cl), bromine(Br), and iodine(I), are highly mobile and water-soluble elements that can become significantly enriched in melts and fluids. In fluids and melts, halogens react with nearly all metals and readily form complexes with metal cations, significantly influencing the distribution of metal elements between different phases. Therefore, halogens play a crucial role in the migration, enrichment, and mineralization of key metals in the lithosphere(Weis et al., 2012; Liu et al., 2024).

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Inter‑Skeleton Conductive Routes Tuning Multifunctional Conductive Foam for Electromagnetic Interference Shielding,Sensing and Thermal Management

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Nano-Micro Letters 2025年第3期17卷 19-36页

作者： Xufeng Li Chunyan chen Zhenyang Li Peng Yi Haihan Zou Gao Deng ming Fang Junzhe He Xin Sun Ronghai Yu Jianglan Shui Caofeng Pan Xiaofang Liu School of Materials Science and Engineering Beihang UniversityBeijing 100191People’s Republic of China Institute of Atomic Manufacturing Beihang UniversityBeijing 100191People’s Republic of China Tianmushan Laboratory Xixi Octagon CityYuhang DistrictHangzhou 310023People’s Republic of China Science and Technology On Electromagnetic Scattering Laboratory Beijing Institute of Environmental FeaturesBeijing 100854People’s Republic of China

Conductive polymer foam(CPF)with excellent compressibility and variable resistance has promising applications in electromagnetic interference(EMI)shielding and other integrated functions for wearable ***,its insufficient change amplitude of resistance with compressive strain generally leads to a degradation of shielding performance during ***,an innovative loading strategy of conductive materials on polymer foam is proposed to significantly increase the contact probability and contact area of conductive components under *** inter-skeleton conductive films are constructed by loading alginate-decorated magnetic liquid metal on the polymethacrylate films hanged between the foam skeleton(denoted as AMLM-PM foam).Traditional point contact between conductive skeletons under compression is upgraded to planar contact between conductive ***,the resistance change of AMLM-PM reaches four orders of magnitude under ***,the inter-skeleton conductive films can improve the mechanical strength of foam,prevent the leakage of liquid metal and increase the scattering area of EM ***-PM foam has strain-adaptive EMI shielding performance and shows compression-enhanced shielding effectiveness,solving the problem of traditional CPFs upon *** upgrade of resistance response also enables foam to achieve sensitive pressure sensing over a wide pressure range and compression-regulated Joule heating function.

关键词： Inter-skeleton conductive films Conductive polymer foam Liquid metal Electromagnetic interference shielding

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Cyano migration-mediated radical-polar crossover cyclopropanation

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Science China Chemistry 2025年第1期68卷 241-248页

作者： Ziqiang Wang Yasu chen Jie Li chen Zhu Key Laboratory of Organic Synthesis of Jiangsu Province College of Chemistry Chemical Engineering and Materials ScienceSoochow University Frontiers Science Center for Transformative Molecules Zhangjiang Institute for Advanced Study and Shanghai Key Laboratory for Molecular Engineering of Chiral Drugs Shanghai Jiao Tong University

We report a novel cyano migration-mediated radical-polar crossover process, whereby both the sulfonylcyanation of aliphatic alkenes and the formation of cyclopropanes are concurrently achieved. This transformation yields a diverse array of multisubstituted cyclopropanes under mild photocatalytic conditions. Mechanistic studies elucidate that the reaction proceeds via intramolecular nucleophilic substitution, leading to the formation of the cyclopropane derivatives.

关键词： cyclopropanation cyano migration radical-polar crossover radical reactions

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Self-assembled carbon monoxide nanoprodrug for chemiexcitationtriggered synergistic chemotherapy against breast cancer

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Science China Chemistry 2025年

作者： Shunfei Cui Yiyao Pan chenzhe Ma Bin Qi Qingqiang Min ming Li Huabing chen Hengte Ke Xingyue Ji Jiangsu Province Engineering Research Center of Precision Diagnostics and Therapeutics Development College of Pharmaceutical ScienceSoochow University

Carbon monoxide（CO） has recently been well-established as a promising therapeutic modality against cancer. The development of transition-metal-free and tumor-targeted delivery platforms for CO is highly demanded but remains very sporadic. Herein, we developed a polyprodrug system for the co-delivery of CO and a chemotherapeutic agent combretastin A-4（CA-4） to the tumor site based on a chemiexcitation mechanism. Such a poly-prodrug successfully achieved the co-activation of CO and CA-4 in response to H2O2at the tumor site both in vitro and in vivo. Importantly, a synergist effect between CO and CA-4 was observed in suppressing tumor growth in a mouse tumor model. It is anticipated that such a poly-prodrug system could be potentially adapted for the co-delivery of CO and another drug payload for combinational therapy for other indications.

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Peri-centrosomal localization of small interfering RNAs in C. elegans

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Science China Life Sciences 2025年

作者： Qile Jin Xuezhu Feng Minjie Hong Ke Wang Xiangyang chen Jiewei cheng Yan Kuang Xiaoyue si mingjing Xu Xinya Huang Shouhong Guang chengming Zhu Department of Obstetrics and Gynecology The First Affiliated Hospital of USTC The USTC RNA Institute Hefei National Research Center for Physical Sciences at the Microscale School of Life Sciences Division of Life Sciences and Medicine Biomedical Sciences and Health Laboratory of Anhui Province University of Science and Technology of China School of Basic Medicine Anhui Medical University

The centrosome is the microtubule-organizing center and a crucial part of cell division. Centrosomal RNAs(cnRNAs) have been reported to enable precise spatiotemporal control of gene expression during cell division in many species. Whether and how cnRNAs exist in C. elegans are unclear. Here, using the nuclear RNAi Argonaute protein NRDE-3 as a reporter, we observed potential peri-centrosome localized small interfering(si)RNAs in C. elegans. NRDE-3 was previously shown to associate with pre-mRNAs and pre-rRNAs via a process involving the presence of complementary siRNAs. We generated a GFP-NRDE-3 knock-in transgene through CRISPR/Cas9 technology and observed that NRDE-3 formed peri-centrosomal foci neighboring the tubulin protein TBB-2, other centriole proteins and pericentriolar material(PCM)components in C. elegans embryos. The peri-centrosomal accumulation of NRDE-3 depends on RNA-dependent RNA polymerase(RdRP)-synthesized 22G siRNAs and the PAZ domain of NRDE-3, which is essential for siRNA binding. Mutation of eri-1, ergo-1, or drh-3 significantly increased the percentage of pericentrosome-enriched NRDE-3. At the metaphase of the cell cycle, NRDE-3 was enriched in both the peri-centrosomal region and the spindle. Moreover, the integrity of centriole proteins and pericentriolar material(PCM) components is also required for the peri-centrosomal accumulation of NRDE-3. Therefore, we concluded that siRNAs could accumulate in the pericentrosomal region in C. elegans and suggested that the peri-centrosomal region may also be a platform for RNAi-mediated gene regulation.

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Two paths, one goal: mechanism of calcium homeostasis to balance plant growth and immunity

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Science China Life Sciences 2025年第1期68卷 306-308页

作者： Aziz Ul Ikram Yanping Jing Huan chen Jian chen International Genome Center Jiangsu University Joint Center for single Cell Biology School of Agriculture and BiologyShanghai Jiao Tong University

Calcium(Ca2+) is an essential nutrient and a cellular signal in plants. The level of free Ca2+in the apoplast is ～10,000-fold higher than that in the cytoplasm at the resting state. This large Ca2+level gradient across the membrane between the interior and exterior can cause Ca2+overload and toxicity. Plants have evolved mechanisms to export Ca2+out of the cytoplasm or store it in intracellular organelles, such as endoplasmic reticulum（ER）, mitochondria, and vacuole.

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Efficient photocatalytic reduction of CO2 to formate by a molecular noble metal-free system

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Science China Chemistry 2025年第1期68卷 152-156页

作者： Lihua Zhang Lingjing chen Huatian Shi Yue Wei Gui chen Tai-Chu Lau School of Environment and Civil Engineering Research Center for Eco-environmental Engineering Dongguan University of Technology Department of Chemistry and Institute of Molecular Functional Materials City University of Hong Kong

Reducing CO2to carbon-neutral solar fuels can not only alleviate the energy demand but also mitigate the greenhouse *** present,developing an efficient non-noble metal photo/electrocatalytic system for converting CO2to a specific product beyond CO is still a big ***,we report a new cobalt complex bearing 2,2′-bi-1,10-phenanthroline ligand that can photocatalytically reduce CO2to formate （HCOO-）.Turnover number （TON） for HCOO-up to 677 with 99%selectivity can be achieved using organic dyes purpurin as photosensitizer and 1,3-dimethyl-2-phenyl-2,3-dihydro-1H-benzo[d]imidazole （BIH） as sacrificial reductant in a CO2-saturated NMP/TEA （v/v,3:1） solution under visible light *** potential electrolysis at-1.41 V （***/Ag Cl） in the presence of 12 m M Et3NHBF4also produced HCOO-with Faradaic efficiency of 39%.Spectroscopic and electrochemical studies suggest that a[CoI-H]species is the key intermediate for CO2reduction.

关键词： photocatalysis noble metal-free CO2 reduction formate cobalt hydride

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A versatile synthetic strategy towards rare earth based metal-organic frameworks

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Science China Chemistry 2025年

作者： Quan Shi Yun-Hao Xu ming-Hui chen Peng Zhao Wen-Bo Deng Ji Xiong Kai Guo Ya-Qing Feng Bao Zhang School of Chemical Engineering and Technology Tianjin University Tianjin Collaborative Innovation Center of Chemical Science and Engineering Guangdong Laboratory Chemistry & Fine Chemical Industry Jieyang Center

Rare earth metal-organic frameworks (RE-MOFs) have drawn wide attention owing to diverse network structures and various application ***,due to the unpredictable formation of the nodes,it is still challenging to design novel RE-MOFs.A novel versatile strategy was developed employing a RE-acetate complex (RE2(CH3COO)6·4H2O) as a precursor to construct RE-MOFs.2D RE-MOFs (RE-DBP) and 3D RE-MOFs (RE-TCPP) could be obtained by using dicarboxylic porphyrin ligands H2DBP and tetracarboxylic porphyrin ligands H2TCPP,*** RE-MOFs were further synthesized to verify the universality of the *** crystalline RE-MOFs could also be prepared at room temperature via the developed strategy,which could significantly promote large-scale preparation and practical application of *** proof of the concept,the performance of porphyrin-based RE-MOFs was investigated in the photocatalytic cycloaddition of CO2with *** the RE-DBP(Co) MOFs,Tb-DBP(Co) exhibited the best photocatalytic performance,which was also greater than that of the corresponding 3D MOF Tb-TCPP(Co) due to the optimal 2D structure and thus the accelerated photogenerated charge separation and transfer *** work not only provides a novel versatile strategy to design and develop RE-MOFs,but also proposes a promising approach for the potential bulk production of RE-MOFs at room temperature.

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