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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

Regulation and function of endoplasmic reticulum autophagy in neurodegenerative diseases

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Neural Regeneration Research 2025年第1期20卷 6-20页

作者： Xiu-Yun Zhao De-En xu Ming-Lei Wu Ji-Chuan Liu zi-Ling Shi Quan-Hong Ma Department of Neurology and Clinical Research Center of Neurological Disease the Second Affiliated Hospital of Soochow UniversitySuzhouJiangsu ProvinceChina Institute of Neuroscience&Jiangsu Key Laboratory of Translational Research and Therapy for Neuro-Psycho-Diseases Soochow UniversitySuzhouJiangsu ProvinceChina Department of Neurology Jiangnan University Medical CenterWuxiJiangsu ProvinceChina

The endoplasmic reticulum,a key cellular organelle,regulates a wide variety of cellular *** reticulum autophagy,one of the quality control systems of the endoplasmic reticulum,plays a pivotal role in maintaining endoplasmic reticulum homeostasis by controlling endoplasmic reticulum turnover,remodeling,and *** this review,we briefly describe the endoplasmic reticulum quality control system,and subsequently focus on the role of endoplasmic reticulum autophagy,emphasizing the spatial and temporal mechanisms underlying the regulation of endoplasmic reticulum autophagy according to cellular *** also summarize the evidence relating to how defective or abnormal endoplasmic reticulum autophagy contributes to the pathogenesis of neurodegenerative *** summary,this review highlights the mechanisms associated with the regulation of endoplasmic reticulum autophagy and how they influence the pathophysiology of degenerative nerve *** review would help researchers to understand the roles and regulatory mechanisms of endoplasmic reticulum-phagy in neurodegenerative disorders.

关键词： autophagy endoplasmic reticulum endoplasmic reticulum autophagy endoplasmic reticulum quality control system endoplasmic reticulum receptors endoplasmic reticulum-associated degradation neurodegeneration neurodegenerative disease selective autophagy unfolded protein response

Small extracellular vesicles derived from human induced pluripotent stem cell-differentiated neural progenitor cells mitigate retinal ganglion cell degeneration in a mouse model of optic nerve injury

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Neural Regeneration Research 2025年第2期20卷 587-597页

作者： tong Li Hui-Min Xing Hai-Dong Qian Qiao Gao Sheng-Lan xu Hua Ma Zai-Long Chi State Key Laboratory of Ophthalmology Optometry and Visual ScienceEye HospitalWenzhou Medical UniversityWenzhouZhejiang ProvinceChina National Clinical Research Center for Ocular Diseases Eye HospitalWenzhou Medical UniversityWenzhouZhejiang ProvinceChina

Several studies have found that transplantation of neural progenitor cells(NPCs)promotes the survival of injured ***,a poor integration rate and high risk of tumorigenicity after cell transplantation limits their clinical *** extracellular vesicles(sEVs)contain bioactive molecules for neuronal protection and *** studies have shown that stem/progenitor cell-derived sEVs can promote neuronal survival and recovery of neurological function in neurodegenerative eye diseases and other eye *** this study,we intravitreally transplanted sEVs derived from human induced pluripotent stem cells(hiPSCs)and hiPSCs-differentiated NPCs(hiPSC-NPC)in a mouse model of optic nerve *** results show that these intravitreally injected sEVs were ingested by retinal cells,especially those localized in the ganglion cell *** with hiPSC-NPC-derived sEVs mitigated optic nerve crush-induced retinal ganglion cell degeneration,and regulated the retinal microenvironment by inhibiting excessive activation of *** analysis further revealed that hiPSC-NPC derived sEVs transported neuroprotective and anti-inflammatory miRNA cargos to target cells,which had protective effects on RGCs after optic nerve *** findings suggest that sEVs derived from hiPSC-NPC are a promising cell-free therapeutic strategy for optic neuropathy.

关键词： exosome miRNA neural progenitor cell neurodegeneration neuroinflammation neuroprotection optic nerve crush optic neuropathy retinal ganglion cell small extracellular vesicles

Interfacial Zn2+-solvation regulator towards reversible and stable Zn anode

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Journal of Energy Chemistry 2025年第1期100卷 684-692页

作者： Miao Zhou Xiongbin Luo Hang Li Shan Guo Zhuang tong Xiaotao Zhou xu Li Zhaohui Hou Shuquan Liang Guozhao Fang College of Mechanical Engineering Key Laboratory of Hunan Province for Advanced Carbon-based Functional Materials Hunan Institute of Science and Technology School of Materials Science and Engineering Key Laboratory of Electronic Packaging and Advanced Functional Materials of Hunan Province Central South University College of Materials and Metallurgy Guizhou University National Energy Metal Resources and New Materials Key Laboratory Central South University

Aqueous zinc-ion batteries （AziBs） are fundamentally challenged by the instability of the electrode/electrolyte interface,predominantly due to irreversible zinc （Zn） deposition and hydrogen ***,the intricate mechanisms behind the electrochemical discrepancies induced by interfacial Zn2+-solvation and deposition behavior demand comprehensive *** molecules endowed with special functional groups （such as hydroxyl,carboxyl,etc.） have the potential to significantly optimize the solvation structure of Zn2+and regulate the interfacial electric double layer （EDL）.By increasing nucleation overpotential and decreasing interfacial free energy,these functional groups facilitate a lower critical nucleation radius,thereby forming an asymptotic nucleation model to promote uniform Zn ***,this study presents a pioneering approach by introducing trace amounts of n-butanol as solvation regulators to engineer the homogenized Zn （H-Zn） anode with a uniform and dense *** interfacial reaction and structure evolution are explored by in/ex-situ experimental techniques,indicating that the H-Zn anode exhibits dendrite-free growth,no by-products,and weak hydrogen evolution,in sharp contrast to the bare ***,the H-Zn anode achieves a remarkable Zn utilization rate of approximately 20% and simultaneously sustains a prolonged cycle life exceeding 500 ***,the H-Zn//NH4V4O10（NVO） full battery showcases exceptional cycle stability,retaining 95.04%capacity retention after 400 cycles at a large current density of 5 A *** study enlightens solvation-regulated additives to develop Zn anode with superior utilization efficiency and extended operational lifespan.

关键词： Solvation

Multivariate synergy for heightening ionic HOF robustness and proton conductivity

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Science China Chemistry 2025年

作者： Xiang-Tian Bai Li-Hui Cao xu-Yong Chen Jia-Yu Wang zi-Ye Zhou Shaanxi Key Laboratory of Chemical Additives for Industry College of Chemistry and Chemical EngineeringShaanxi University of Science and Technology

Multicomponent crystalline materials construct more complex and diversified structures with different combinations and modes,which expands the material structure space and application *** this work,we have successfully synthesized two twocomponent ionic hydrogen-bonded organic frameworks （iHOF-32 and iHOF-33） and a three-component iHOF （iHOF-34）.Guanidine hydrochloride which is rich in N and H and has a short chain length strengthens the hydrogen bonding network of iHOF,thereby aiding in the efficient migration of *** rigid architecture of 1,1'-diamino-4,4'-bipyridine diiodide furnishes additional scaffolding for the iHOFs and enhances its robustness under harsh ***-34 accomplishes the combination of the ultra-high proton conductivity of iHOF-32 and the robustness of iHOF-33 by the synergistic interaction among the three components of *** addition,iHOF-34 was fabricated as a composite membrane with a peak proton conductivity of 1.55×10-1S cm-1,which is 3.8 times higher than that of recast Nafion,and has extensive potential in fuel *** self-assembly strategy of multicomponent HOFs opens up new avenues for constructing diverse structures while promising new opportunities for applications in the fields of proton conduction and energy storage.

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Enantio-divergent C–H borylation with two different ligands from a single chiral source

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Science China Chemistry 2025年第1期68卷 226-232页

作者： Rongrong Du Senmiao xu State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical Physics Chinese Academy of Sciences College of Material Chemistry and Chemical Engineering Key Laboratory of Organosilicon Chemistry and Material TechnologyMinistry of Education Hangzhou Normal University University of Chinese Academy of Sciences

Reported here is an iridium-catalyzed enantio-divergent C（sp3）–H borylation of α-gem-dimethyl groups of trifluoromethyl ketone-derived hydrazones to construct a series of acyclic all-carbon quaternary stereocenters with a high level of chiral induction. Two different chiral bidentate boryl ligands from a common chiral source not only can switch the enantioselectivity but also are complementary in terms of the substrate scope.

关键词： asymmetric catalysis C–H borylation all-carbon quaternary stereocenters synthetic methods

Reverse modulation of defect density of Ce-MOF-808 by solventassisted ligand exchange for dicyclopentadiene hydrogenation

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Science China Chemistry 2025年

作者： Danfeng Zhao Fajie Hu Rushuo Li Xinmeng xu Zhaokun Wang Zuoshuai Xi Jun tong Xiubing Huang Ge Wang Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory of Function Materials for Molecule & Structure Construction School of Materials Science and Engineering University of Science and Technology Beijing

Defect engineering is a pivotal strategy for tailoring the electronic structure and physicochemical properties of catalysts, yet the straightforward manipulation of defect density in porous materials presents a current challenge. In this work, we achieved precise control over the coordination unsaturated site（CUS） content and pore architecture of Ce-MOF-808 by employing 2-fluorobenzoic acid（2-FBA） as a modifier. Leveraging the p Kadisparities among three ligands（1,3,5-tricarboxylic benzoic acid,formic acid, and 2-FBA）, we preserved the spn topology of Ce-MOF within an aqueous system, while realizing partial substitution of the auxiliary ligands and saturation of the CUS. The amount of 2-FBA was negatively correlated with the number of ligand defects, and the consequent decrease in Ce3+content and the increase in the number of ligand linkages also induced crystal structure transformation. The modulation of the defect structure was correlated with the catalytic performance of dicyclopentadiene（DCPD） hydrogenation reaction, in which Ce-MMF0.15, constructed by the modulation of 0.15 mol amount of 2-fluorobenzoic acid, exhibited an optimal ligand defect density and micro-mesoporous structure, enabling almost complete conversion of DCPD at 100 ℃ and 2 MPa. This article also elucidates the correlation between the regulation of defect density and the accessibility of frustrated Lewis pair（FLP） active sites, guiding the application of novel porous intrinsic FLP materials in hydrogenation catalysis.

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Aquaporin-4-IgG-seropositive neuromyelitis optica spectrum disorders:progress of experimental models based on disease pathogenesis

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Neural Regeneration Research 2025年第2期20卷 354-365页

作者： Li xu Huiming xu Changyong Tang Department of Neurology The Third Affiliated Hospital of Sun Yat-sen UniversityGuangzhouGuangdong ProvinceChina

Neuromyelitis optica spectrum disorders are neuroinflammatory demyelinating disorders that lead to permanent visual loss and motor *** date,no effective treatment exists as the exact causative mechanism remains ***,experimental models of neuromyelitis optica spectrum disorders are essential for exploring its pathogenesis and in screening for therapeutic *** most patients with neuromyelitis optica spectrum disorders are seropositive for IgG autoantibodies against aquaporin-4,which is highly expressed on the membrane of astrocyte endfeet,most current experimental models are based on aquaporin-4-IgG that initially targets *** experimental models have successfully simulated many pathological features of neuromyelitis optica spectrum disorders,such as aquaporin-4 loss,astrocytopathy,granulocyte and macrophage infiltration,complement activation,demyelination,and neuronal loss;however,they do not fully capture the pathological process of human neuromyelitis optica spectrum *** this review,we summarize the currently known pathogenic mechanisms and the development of associated experimental models in vitro,ex vivo,and in vivo for neuromyelitis optica spectrum disorders,suggest potential pathogenic mechanisms for further investigation,and provide guidance on experimental model *** addition,this review summarizes the latest information on pathologies and therapies for neuromyelitis optica spectrum disorders based on experimental models of aquaporin-4-IgG-seropositive neuromyelitis optica spectrum disorders,offering further therapeutic targets and a theoretical basis for clinical trials.

关键词： aquaporin-4 experimental model neuromyelitis optica spectrum disorder pathogenesis

Reducing the measurement errors in nonadiabatic holonomic quantum computers

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Science China(Physics,Mechanics & Astronomy) 2025年第1期Mechanics & Astronomy) .卷 64-70页

作者： Guo-Fu xu Department of Physics Shandong University

Nonadiabatic holonomic quantum computers serve as the physical platform for nonadiabatic holonomic quantum *** quantum computation has entered the noisy intermediate-scale era, building accurate intermediate-scale nonadiabatic holonomic quantum computers is clearly necessary. Given that measurements are the sole means of extracting information, they play an indispensable role in nonadiabatic holonomic quantum computers. Accordingly, developing methods to reduce measurement errors in nonadiabatic holonomic quantum computers is of great importance. However, while much attention has been given to the research on nonadiabatic holonomic gates, the research on reducing measurement errors in nonadiabatic holonomic quantum computers is severely lacking. In this study, we propose a measurement error reduction method tailored for intermediate-scale nonadiabatic holonomic quantum computers. The reason we say this is because our method can not only reduce the measurement errors in the computer but also be useful in mitigating errors originating from nonadiabatic holonomic gates. Given these features,our method significantly advances the construction of accurate intermediate-scale nonadiabatic holonomic quantum computers.

关键词： quantum holonomy quantum computation measurement errors