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Cobalamin-dependent radical S-adenosyl-L-methionine protein functions with a partner to successively methylate tricyclic indole alkaloid for chuangxinmycin maturation and derivatization

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Science China Chemistry 2025年第1期68卷 308-316页

作者： Sili Wang Jiancheng Huang Yanan du Wei Huang Yufeng xue Xiaokun xu Guannan zhong Yuanyuan Shi Bin Hong Xiaoying Bian Wen liu State Key Laboratory of Chemical Biology Shanghai Institute of Organic Chemistry University of Chinese Academy of SciencesChinese Academy of Sciences State Key Laboratory of Microbial Technology Shandong University National Health Commission (NHC) Key Laboratory of Biotechnology for Microbial Drugs Institute of Medicinal BiotechnologyChinese Academy of Medical Science & Peking Union Medical College

Cobalamin(Cbl)-dependent radical S-adenosyl-L-methionine(SAM) proteins constitute the largest collection of the radical SAM superfamily that has hundreds of thousands of individual members. Many of these proteins are involved in the biosynthesis of pharmaceutically important natural products to catalyze chemically demanding reactions. In the biosynthetic pathway of chuangxinmycin(CXM), a unique indole alkaloid antibiotic with potent anti-infective activity, functionalization of the characteristic thiopyrano[4,3,2-cd]indole scaffold by regio-and stereoselective C3-methylation is believed to rely on a Cbl-dependent radical process, which, however, remained to be reconstituted biochemically. We here report the dissection of this enzymatic process, which requires the incorporation of Cxm8, a Cbl-dependent radical SAM protein, with Cxm9, a duF5825family protein that shares no homology to any proteins of known functions. Cxm8 and Cxm9 function together by forming an unexpected heterodimeric complex that selectively catalyzes C3-methylation of the tricyclic indole-S-hetero ring system in a successive manner, achieving CXM and a recently identified, C3-dimethylated congener. Detailed biochemical characterization,isotope labeling, structural simulation and bioinformatics analysis rationalized the catalysis of the Cxm8/Cxm9 complex and particularly the necessity of the duF5825 protein for C3-methylase activity. This is the first example that a Cbl-dependent protein acts with a partner to exhibit radical SAM activity.

关键词： cbl-dependent radical SAM protein biosynthesis chuangxinmycin stereoselective methylation

Advances in the Development of Gradient Scaffolds Made of Nano‑Micromaterials for Musculoskeletal Tissue Regeneration

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Nano-Micro Letters 2025年第3期17卷 455-500页

作者： Lei Fang Xiaoqi lin Ruian xu Lu liu Yu Zhang feng Tian Jiao Jiao li Jiajia xue Beijing Laboratory of Biomedical Materials Beijing University of Chemical TechnologyBeijing 100029People’s Republic of China State Key Laboratory of Organic‑Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029People’s Republic of China School of Biomedical Engineering Faculty of Engineering and ITUniversity of Technology SydneySydneyNSW 2007Australia

The intricate hierarchical structure of musculoskeletal tissues,including bone and interface tissues,necessitates the use of complex scaffold designs and material structures to serve as tissue-engineered *** has led to growing interest in the development of gradient bone scaffolds with hierarchical structures mimicking the extracellular matrix of native tissues to achieve improved therapeutic *** on the anatomical characteristics of bone and interfacial tissues,this review provides a summary of current strategies used to design and fabricate biomimetic gradient scaffolds for repairing musculoskeletal tissues,specifically focusing on methods used to construct compositional and structural gradients within the *** latest applications of gradient scaffolds for the regeneration of bone,osteochondral,and tendon-to-bone interfaces are ***,the current progress of testing gradient scaffolds in physiologically relevant animal models of skeletal repair is discussed,as well as the challenges and prospects of moving these scaffolds into clinical application for treating musculoskeletal injuries.

关键词： Gradient scaffolds Musculoskeletal tissues Advanced manufacturing Biomaterials Tissue regeneration

Preparation of Co/S co-doped carbon catalysts for excellent methylene blue degradation

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International Journal of Minerals,Metallurgy and Materials 2025年第1期32卷 169-181页

作者： Haixu li Haobo He Tiannan Jiang Yunfei du Zhichen Wu liang xu Xinjie Wang Xiaoguang liu Wanhua Yu Wendong xue School of Materials Science and Engineering University of Science and Technology BeijingBeijing 100083China Beijing Jinyu Tongda Refractory Technologies Co. Ltd.Beijing 100085China

S and Co co-doped carbon catalysts were prepared via pyrolysis of MOF-71 and thiourea mixtures at 800℃at a mass ratio of MOF-71 to thiourea of 1:0.1 to effectively activate peroxymonosulfate(PMS)for methylene blue(MB)*** effects of two different mixing routes were identified on the MB degradation ***,the catalyst obtained by the alcohol solvent evaporation(MOF-AEP)mixing route could degrade 95.60%MB(50 mg/L)within 4 min(degradation rate:K=0.78 min^(-1)),which was faster than that derived from the direct grinding method(MOF-DGP,80.97%,K=0.39 min^(-1)).X-ray photoelectron spectroscopy revealed that the Co-S content of MOF-AEP(43.39at%)was less than that of MOF-DGP(54.73at%),and the proportion of C-S-C in MOF-AEP(13.56at%)was higher than that of MOF-DGP(10.67at%).Density functional theory calculations revealed that the adsorption energy of Co for PMS was -2.94 eV when sulfur was doped as C-S-C on the carbon skeleton,which was higher than that when sulfur was doped next to cobalt in the form of Co-S bond(-2.86 eV).Thus,the C-S-C sites might provide more contributions to activate PMS compared with ***,the degradation parameters,including pH and MOF-AEP dosage,were ***,radical quenching experiments and electron paramagnetic resonance(EPR)measurements revealed that ^(1)O_(2)might be the primary catalytic species,whereas·O~(2-)might be the secondary one in degrading MB.

关键词： advanced oxidation process alcohol solvent evaporation hydrogen bond S and Co co-doped carbon catalysts wastewater remediation

Targets capture by distributed active swarms via bio-inspired reinforcement learning

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Science China(Physics,Mechanics & Astronomy) 2025年第1期Mechanics & Astronomy) .卷 210-221页

作者： Kun xu Yue li Jun Sun Shuyuan du Xinpeng Di Yuguang Yang Bo li Institute of Biomechanics and Medical Engineering Applied Mechanics Laboratory Department of Engineering MechanicsTsinghua University Institute of Nuclear and New Energy Technology Tsinghua University Shanghai Aerospace Control Technology Institute Shanghai Key Laboratory of Aerospace Intelligent Control Technology College of Automation Engineering Nanjing University of Aeronautics and Astronautics

Natural swarms arranged from cells to herds are usually decentralized but display intriguing collective intelligence in coordinating individuals across large scales to efficiently achieve their common goals. Learning from nature may provide new strategies for controlling collective dynamics of synthetic swarms to accomplish specific functions. Here, we present a bioinspired computational framework that steers distributed active swarms to collectively capture and merge targets via reinforcement learning. We exploit collective milling structures of natural herds to cage the targets, and adopt a switching control policy inspired by sperms' chiral dynamics to optimize the trajectories of individuals, through which the active swarms can selforganize to enclose single or multiple distant targets in a dynamical, adaptive and scalable manner. There exists a critical swarm size, beyond which the excessive competition between agents would generate large mechanical forces, leading to capture instability but enabling the transition from short-distance to long-distance merging capture of multiple targets. This work provides physical insights into distributed active swarms and could offer a multilevel, decentralized strategy toward controlling swarm robotics in wide applications such as bio-medical devices, machine immunity, and target clearance.

关键词： swarm intelligence robotics multi-tasks artificial intelligence bionics

Recent progress on photoactive nonprecious transition-metal complexes

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Science China Chemistry 2025年第1期68卷 46-95页

作者： zhong-liang Gong Hong-Jie Zhang Yan Cheng Jianxun liu Yuhan Ai Yaqin li Zhihui feng Qiong Zhang Shaolong Gong Yong Chen Chang-Jiang Yao Yuan-Yuan Zhu liang-Jin xu Yu-Wu zhong CAS Key Laboratory of Photochemistry Institute of Chemistry Chinese Academy of Sciences State Key Laboratory of Structural Cemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences School of Chemistry and Chemical Engineering Anhui Key Laboratory of Advanced Catalytic Materials and Reaction EngineeringHefei University of Technology State Key Laboratory of Explosion Science and Safety Protection School of Mechatronical Engineering Beijing Institute of Technology College of Chemistry and Molecular Sciences Hubei Key Lab on Organic and Polymeric Optoelectronic Materials Wuhan University School of Chemistry and Chemical Engineering Anhui University Key Laboratory of Photochemical Conversion and Optoelectronic Materials & CAS-HKU Joint Laboratory on New Materials Technical Institute of Physics and Chemistry Chinese Academy of Sciences

Photoactive complexes of nonprecious transition metals, mainly including those in the first-row and partially the second-row of the Periodic table of elements, have received increasing attention in view of their low cost and long-term sustainability. They are recognized as promising alternatives to noble transition metal complex congeners that have been extensively studied in optoelectronic devices, artificial photosynthesis, photocatalysis, biodiagnostics, and therapeutics, etc. This review is devoted to a comprehensive summary on the classical and recent advances on photoactive nonprecious transition metal complexes, including photoactive Zr, V, Cr, Mo, and W complexes, Mn complexes and hybrids, Fe, Co, Ni, and Cu complexes, and Zn and Cd complexes and hybrids. A particular focus is given on the molecular design, modulation of photophysical and photochemical properties, and applications of the representative and lately-developed nonprecious metal complexes. In addition, a perspective on the future development in this field is provided at the end of this review.

关键词： photoactive metal complexes earth-abundant metals nonprecious metal complexes luminescence photochemistry

Inhibitory gamma-aminobutyric acidergic neurons in the anterior cingulate cortex participate in the comorbidity of pain and emotion

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Neural Regeneration Research 2025年第10期20卷 2838-2854页

作者： Lu Guan Mengting Qiu Na li Zhengxiang Zhou Ru Ye liyan zhong Yashuang xu Junhui Ren Yi liang Xiaomei Shao Jianqiao Fang Junfan Fang Junying du Department of Neurobiology and Acupuncture Research Third School of Clinical MedicineZhejiang Chinese Medical UniversityHangzhouZhejiang ProvinceChina Key Laboratory for Research of Acupuncture Treatment and Transformation of Emotional Diseases Third School of Clinical MedicineZhejiang Chinese Medical UniversityHangzhouZhejiang ProvinceChina Fuchun Community Health Service Center of Fuyang District HangzhouZhejiang ProvinceChina

Pain is often comorbid with emotional disorders such as anxiety and *** of the anterior cingulate cortex has been implicated in pain and pain-related negative emotions that arise from impairments in inhibitory gamma-aminobutyric acid *** review primarily aims to outline the main circuitry(including the input and output connectivity)of the anterior cingulate cortex and classification and functions of different gamma-aminobutyric acidergic neurons;it also describes the neurotransmitters/neuromodulators affecting these neurons,their intercommunication with other neurons,and their importance in mental comorbidities associated with chronic pain *** understanding on their role in pain-related mental comorbidities may facilitate the development of more effective treatments for these ***,the mechanisms that regulate gamma-aminobutyric acidergic systems remain *** is also unclear as to whether the mechanisms are presynaptic or *** exploration of the complexities of this system may reveal new pathways for research and drug development.

关键词： anterior cingulate cortex anxiety chronic pain circuit communication comorbidity depression gamma-aminobutyric acidergic neurons parvalbumin neurons synaptic transmission

Mainchain conformation ordering self-assembly tailored room temperature phosphorescence emission

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Science China Chemistry 2025年第1期68卷 329-336页

作者： Yuzhu li Yumeng Gao feng Tian Yu Wang Yuan Yao Shaoliang lin Xiang Ma Binbin xu Shanghai Key Laboratory of Advanced Polymeric Materials Key Laboratory for Ultrafine Materials of Ministry of Education School of Materials Science and Engineering East China University of Science and Technology Shanghai Synchrotron Radiation Facility Shanghai Advanced Research Institute Chinese Academy of Sciences Key Laboratory for Advance Materials and Feringa Noble Prize Scientist Joint Research Centre Frontiers Science for Materiobiology and Dynamic Chemistry School of Chemistry and Molecular Engineering East China University of Science & Technology

Developing organic room-temperature phosphorescence （RTP） materials with a wide range of tunable-emission is significant in expanding the applications of RTP ***,we rationally designed amphiphilic alternating copolymers poly(1,2-bis（4-alkoxyphenyl）ethane-1,2-dione-alt-（ethylene glycol）x)(P（Bz-alt-EGx）) that combined the advantage of alternating benzil and EGxskeleton,and tunable mainchain *** a mainchain conformation ordering assembly （COA） process,P（Bz-alt-EGx） self-assembled into well-defined platelets,and such assemblies emitted blue RTP at ca.425 nm due to the ordered folded-chain conformation and confined *** contrast,traditional self-assembly （TA） of P（Bz-alt-EGx） obtained less ordered aggregates,such as asymmetric worms,vesicles,and rod-like *** resultant less ordered aggregates exhibited yellow-green RTP at ca.550 *** wide-tuning RTP emission in solution （between blue and yellow-green,over125 nm） is realized using the P（Bz-alt-EGx） alternating copolymers under the treatment of different self-assembly *** study uncovers a new strategy to tailor the RTP emission through different self-assembly pathways and holds great promise for the fabrication of advanced optical materials.

关键词： self-assembly conformation ordering alternating copolymer phosphorescence emission

Constructing 2D bismuth-based heterostructure for highly efficient photocatalytic CO2 reduction

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Tungsten 2025年第1期7卷 71-79页

作者： Ruo-Hang xu Hao-Yu Jiang Dan-Dan Cui Kun-Rong du Hong-Run Zhang Sheng-Jie xu Ya-Qi li Zhi-Zhen Ren liang Wang Wei-Chang Hao Yi du School of Physics and BUAA-UOW Joint Research Centre Beihang University Shenzhen Institute of Beihang University Centre for Catalysis and Clean Energy School of Environment and Science Griffith University

Reforming carbon dioxide（CO2） into fuels and valuable chemicals using solar energy holds significant potential for emission reduction and addressing energy supply *** recombination of photocarriers remains a major obstacle,however,to enhancing solar energy conversion efficiency in the photocatalytic reaction *** two-dimensional materials,constructing heterogeneous structures has emerged as an effective strategy to enhance the separation of photoexcited carriers by leveraging the internal electric field at the heterogeneous ***,we present a facile strategy for preparing Bi4NbO8Br/Bi2WO6plate-on-plate Z-scheme junctions with a strong internal electric field by in situ *** unique heterostructure facilitates efficient separation and transport of photoexcited charges by harnessing the internal electric field induced by chemical bonding at the lateral ***,the Bi4NbO8Br/Bi2WO6heterostructure exhibits enhanced CO2photoreduction properties,along with a CO yield rate of approximately 35 μmol·g-1·h-1under full light *** work offers novel insights into the synthesis of unique hetero structures intended to enhance the efficiency of photocatalytic CO2reduction.

关键词： Bi4NbO8Br/Bi2WO6 CO2 reduction Heterostructures Photocatalysts

The complex roles of m^(6)A modifications in neural stem cell proliferation, differentiation, and self-renewal and implications for memory and neurodegenerative diseases

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Neural Regeneration Research 2025年第6期20卷 1582-1598页

作者： Yanxi li Jing xue Yuejia Ma Ke Ye xue Zhao Fangliang Ge Feifei Zheng Lulu liu xu Gao Dayong Wang Qing Xia Department of Biochemistry and Molecular Biology College of Basic Medical SciencesHarbin Medical UniversityHarbinHeilongjiang ProvinceChina College of Basic Medical Sciences Harbin Medical UniversityHarbinHeilongjiang ProvinceChina Basic Medical Institute Heilongjiang Academy of Medical SciencesHarbinHeilongjiang ProvinceChina Key Laboratory of Heilongjiang Province for Genetically Modified Animals Harbin Medical UniversityHarbinHeilongjiang ProvinceChina Translational Medicine Research and Cooperation Center of Northern China Heilongjiang Academy of Medical SciencesHarbinHeilongjiang ProvinceChina Dongzhimen Hospital Beijing University of Chinese MedicineBeijingChina

N6-methyladenosine(m^(6)A), the most prevalent and conserved RNA modification in eukaryotic cells, profoundly influences virtually all aspects of mRNA metabolism. mRNA plays crucial roles in neural stem cell genesis and neural regeneration, where it is highly concentrated and actively involved in these processes. Changes in m^(6)A modification levels and the expression levels of related enzymatic proteins can lead to neurological dysfunction and contribute to the development of neurological diseases. Furthermore, the proliferation and differentiation of neural stem cells, as well as nerve regeneration, are intimately linked to memory function and neurodegenerative diseases. This paper presents a comprehensive review of the roles of m^(6)A in neural stem cell proliferation, differentiation, and self-renewal, as well as its implications in memory and neurodegenerative diseases. m^(6)A has demonstrated divergent effects on the proliferation and differentiation of neural stem cells. These observed contradictions may arise from the time-specific nature of m^(6)A and its differential impact on neural stem cells across various stages of development. Similarly, the diverse effects of m^(6)A on distinct types of memory could be attributed to the involvement of specific brain regions in memory formation and recall. Inconsistencies in m^(6)A levels across different models of neurodegenerative disease, particularly Alzheimer's disease and Parkinson's disease, suggest that these disparities are linked to variations in the affected brain regions. Notably, the opposing changes in m^(6)A levels observed in Parkinson's disease models exposed to manganese compared to normal Parkinson's disease models further underscore the complexity of m^(6)A's role in neurodegenerative processes. The roles of m^(6)A in neural stem cell proliferation, differentiation, and self-renewal, and its implications in memory and neurodegenerative diseases, appear contradictory. These inconsistencies may be a

关键词： Alzheimer's disease cell self-renewal central nervous system memory microglia nerve regeneration neurodegenerative diseases neurogenesis RNA methylation