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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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Unveiling the promotion role of ZnO on Zn-Al spinel oxide for CO2 hydrogenation

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Journal of Energy Chemistry 2025年第1期100卷 18-25页

作者： Tongyao Wang Xinlong Yao Lixin Liang Hongyu Chen Pan Gao Guangjin Hou State Key Laboratory of Catalysis Dalian National Laboratory for Clean Energy Dalian Institute of Chemical Physics Chinese Academy of Sciences university of Chinese Academy of sciences

The Zn-Al spinel oxide stands out as one of the most active catalysts for high-temperature methanol synthesis from CO2hydrogenation. However, the structure–activity relationship of the reaction remains poorly understood due to challenges in atomic-level structural characterizations and analysis of reaction intermediates. In this study, we prepared two Zn-Al spinel oxide catalysts via coprecipitation（ZnAl-C）and hydrothermal（ZnAl-H） methods, and conducted a comparative investigation in the CO2hydrogenation reaction. Surprisingly, under similar conditions, ZnAl-C exhibited significantly higher selectivity towards methanol and DME compared to ZnAl-H. Comprehensive characterizations using X-ray diffraction（XRD）, Raman spectroscopy and electron paramagnetic resonance（EPR） unveiled that ZnAl-C catalyst had abundant ZnO species on its surface, and the interaction between the ZnO species and its ZnAl spinel oxide matrix led to the formation of oxygen vacancies, which are crucial for CO2adsorption and activation. Additionally, state-of-the-art solid-state nuclear magnetic resonance（NMR） techniques,including ex-situ and in-situ NMR analyses, confirmed that the surface ZnO facilitates the formation of unique highly reactive interfacial formate species, which was readily hydrogenated to methanol and DME. These insights elucidate the promotion effects of ZnO on the ZnAl spinel oxide in regulating active sites and reactive intermediates for CO2-to-methanol hydrogenation reaction, which is further evidenced by the significant enhancement in methanol and DME selectivity observed upon loading ZnO onto the ZnAl-H catalyst. These molecular-level mechanism understandings reinforce the idea of optimizing the ZnO-ZnAl interface through tailored synthesis methods to achieve activity-selectivity balance.

关键词： Reaction intermediates

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Bifunctional bridging capping layer enables 24.5% efficiency of perovskite solar cells with polymer-based hole transport materials

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Science China Chemistry 2025年第1期68卷 350-359页

作者： Can Zhu Yiyang Wang Lei Meng Beibei Qiu Jing Li Shucheng Qin Ke Hu Xin Jiang Wenbin Lai Minchao Liu Zhe Liu Chenxing Lu Jinyuan Zhang Yongfang Li Beijing National Laboratory for Molecular sciences CAS Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences School of Chemical Science University of Chinese Academy of Sciences Key Laboratory of Solid State Optoelectronic Devices of Zhejiang Province College of Physics and Electronic Information Engineering Zhejiang Normal University Key Laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and ChemistryChinese Academy of Sciences Laboratory of Advanced Optoelectronic Materials College of Chemistry Chemical Engineering and Materials ScienceSoochow University

Developing a bridge capping layer between perovskite and hole transport layer materials（HTMs） in the n-i-p perovskite solar cells（pero-SCs） is an effective approach to modify the morphology of HTMs and passivate the perovskite ***, we select the quinoxaline-based bifunctional passivation agent, quinoxalin-6-yl-methylamine hydrochloride（Qx MACl）,as the bridging layer, and a D-A copolymer PBQ12 containing the same quinoxaline unit as an HTM for the n-i-p pero-SCs. Due to the π-π stacking among the common quinoxaline units in the bridge layer and HTM, Qx MACl induces the π-π stacking of the PBQ12 film and improves the film morphology of HTMs with better conductivity. Additionally, Qx MACl can effectively passivate the perovskite surface, and PBQ12 possesses appropriate energy levels and high hole mobility. The pero-SCs based on FAPbI3with PBQ12/Qx MACl treatment showed a higher power conversion efficiency（PCE） of 24.05% and outstanding stability, maintaining 95.4% and 92.1% of its initial PCE after 750 h of storage and after over 800 h of thermal annealing at 85 °C, respectively. To further enhance the PCE of the PBQ12/Qx MACl-based devices, we developed a non-metal ion dopant for the PBQ12 HTM. Through trace doping of PBQ12 HTM by the non-metal ion dopant, the PCE of the PBQ12/Qx MACl-based devices reached 25.24%（the calibrated PCE of 24.55% by the National Institute of Metrology, China）.

关键词： D-A copolymer, hole transport materials, bifunctional bridge capping layer, passivation perovskite solar cells

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Engineering high-performance chemiluminescent probes via enzymatic pocket targeting: high-throughput screening for ultralong afterglow imaging of orthotopic hepatocellular carcinoma

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Science China Chemistry 2025年

作者： Shuai Huang Shuaige Bai Ting Luo Bin Feng Min Liu Fan Zheng Shuang Huang Yanpeng Fang Dan Ding Wenbin Zeng Xiangya School of Pharmaceutical sciences Central South University College of Life sciences Nankai University

Hepatocellular carcinoma （HCC） is a highly aggressive liver malignancy and the main form of liver cancer. Early diagnosis and treatment of HCC can effectively reduce mortality. Carboxylesterase （CE）-specific detection and imaging can be used for early diagnosis and image-guided surgical of HCC. However, traditional optical probes suffer from poor selectivity and low imaging signal-to-noise ratio. Here, we have constructed a series of chemiluminescent probes for carboxylesterase detection based on the strategy of enzymatic pocket-oriented steric tailoring techniques. The probes with different unique and excellent properties have been obtained through the structure-based steric hindrance adjustment on the recognition site. Here, CE-2 has been successfully used for high-throughput screening of rapid carboxylesterase inhibitors due to its extremely low detection limit (2.5×10-4U mL-1) and fast recognition ability. CE-3 has been successfully used for image-guided surgery of orthotopic hepatocellular carcinoma due to its ultra-long chemiluminescence imaging （over 12 h） of hepatocellular carcinoma. This study may promote advances in the rapid detection and screening of inhibitory drugs for CE and the field of surgical navigation in HCC.

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Tectonic modes of mantle convection and their implications for Earth's tectonic evolution based on three-dimensional numerical simulations

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Science China Earth sciences 2025年第1期68卷 270-296页

作者： Song XIANG Jinshui HUANG Bingcheng WU School of Earth and Space sciences University of Science and Technology of China CAS Center of Excellence in Comparative Planetary Studies

Five tectonic modes of mantle convection are obtained and analyzed with three-dimensional numerical models in a spherical shell domain. The five tectonic convective modes are non-plate mobile-lid, plate-like mobile-lid, episodic plate-like mobile-lid, episodic stagnant-lid, and stagnant-lid convective modes, respectively. The typical characteristics of these five tectonic modes and their numerical classification criteria based on plateness, mobility, and their standard deviations are presented and discussed. The results show that the yield stress of the lithosphere has profound effects on the tectonic convective *** the gradual increase of yield stress, the tectonic mode of mantle convection changes from one to another sequentially through the aforementioned five modes. Additionally, as the Rayleigh number increases, the range of yield stress for the platelike mobile-lid convective mode decreases, and the dimensionless transition stress between different tectonic modes ***, the dimensional transition stress between the non-plate mobile-lid convective mode and plate-like mobile-lid convective mode increases with the increase of Rayleigh number, but decreases between other tectonic modes. Furthermore, we find that the transition stress between different tectonic modes is inversely proportional to the internal heating rate, with the transition stress decreasing as the internal heating rate increases. The fitting analysis of the transition stress between tectonic modes shows that Earth's current plate tectonics correspond to a lithospheric yield stress of 150–250 MPa, which aligns with the strength of serpentinized mantle rock determined by experimental petrography. If the Archean mantle was 300°C warmer than it is today, then the Earth was in an episodic stagnant-lid convective mode. The tectonic evolution of the Earth's surface is closely related to the lithospheric strength and the process of thermal evolution. If the lithospheric strength w

关键词： Tectonic mode of mantle convection Plate-like mobile-lid convection Episodic plate-like mobile-lid convection Episodic stagnant-lid convection Plate tectonics and tectonic evolution of the Earth

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Dynamic performance enhancement in Ti/Au ohmic contacts on β-Ga2O3-on-Si C substrates: evidence from pulsed measurements

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Science China(Information sciences) 2025年第1期68卷 400-401页

作者： Chenyu LIU Yibo WANG Wenhui XU Shuqi HUANG Chunxiao YU Zeyu YANG Xiaole JIA Xiaoxi LI Bochang LI Zhengdong LUO Cizhe FANG Yan LIU Tiangui YOU Xin OU Genquan HAN School of Microelectronics Xidian University Suzhou Institute of Nano-Tech and Nano-Bionics Chinese Academy of Sciences Shanghai Institute of Microsystem and Information Technology Chinese Academy of Sciences Hangzhou Institute of Technology Xidian University

Titanium/Gold （Ti/Au） metals have been widely employed as ohmic metal contacts on n+Ga2O3,exhibiting the specific contact resistance （ρc） of 10-5-10-6Ω·cm2[1].But previous studies have revealed the presence of a defective Ga2O3layer and reactive Ti-Ga2O3layer at the annealed Ti/*** an interfacial layer can afect the performance of ohmic contact,which may become more pronounced in power devices subjected to electrical stress and high-frequency ***,there have been no reports on the impact of bias stress effects and dynamic degradation of Ti/Au ohmic contacts on n+Ga2O3.

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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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Solar cycles during the seventeenth century revealed by equatorial aurora records

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Earth and Planetary Physics 2025年第1期9卷 182-187页

作者： Yong Wei LiMei Yan Key Laboratory of Earth and Planetary Physics Institute of Geology and GeophysicsChinese Academy of SciencesBeijing 100029China College of Earth and Planetary sciences University of Chinese Academy of SciencesBeijing 100049China

Solar cycles are fundamental to astrophysics,space exploration,technological infrastructure,and Earth's climate.A better understanding of these cycles and their history can aid in risk mitigation on Earth,while also deepening our knowledge of stellar physics and solar system *** the solar cycles between 1600 and 1700-especially the post-1645 Maunder Minimum,characterized by significantly reduced solar activity-poses challenges to existing solar activity *** study utilizes a new red equatorial auroral catalog from ancient Korean texts to establish solar cycle patterns from 1623 to ***,a further reevaluation of the solar cycles between 1610 and 1755 identified a total of 13 cycles,diverging from the widely accepted record of 12 cycles during that *** research enhances our understanding of historical solar activity,and underscores the importance of integrating diverse historical sources into modern analyses.

关键词： solar cycle Maunder Minimum solar activity red equatorial aurora West Pacific geomagnetic anomaly

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Advances in genotypic antimicrobialresistance testing: a comprehensive review

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Science China Life sciences 2025年第1期68卷 130-143页

作者： Boheng Duan Xianjun Zeng Junping Peng Huan Kui College of Nanchang university Department of Imaging The Second Affiliated Hospital of Nanchang University NHC Key Laboratory of Systems Biology of Pathogens National Institute of Pathogen BiologyChinese Academy of Medical Sciences & Peking Union Medical College Key Laboratory of Respiratory Disease Pathogenomics Chinese Academy of Medical Sciences & Peking Union Medical College Key Laboratory of Pathogen Infection Prevention and Control (Ministry of Education) State Key Laboratory of Respiratory Health and MultimorbidityNational Institute of Pathogen BiologyChinese Academy of Medical Sciences & Peking Union Medical College

Antimicrobial resistance(AMR) represents a substantial threat to global public health, complicating the treatment of common infections and leading to prolonged illness and escalated healthcare expenses. To effectively combat AMR, timely and accurate detection is crucial for AMR surveillance and individual-based therapy. Phenotypic antibiotic resistance testing(AST) has long been considered the gold standard in clinical applications, serving as the foundation for clinical AMR diagnosis and optimized therapy. It has significantly contributed to ensuring patients′ health and the development of novel antimicrobials. Despite advancements in automated culture-based AST technologies,inherent limitations impede the widespread use of phenotypic AST in AMR surveillance. Genotypic AST technologies offer a promising alternative option, exhibiting advantages of rapidity, high sensitivity, and specificity. With the continuous advancement and expanding applications of genotypic AST technologies, such as microfluidics, mass spectrometry, and high-resolution melting curve analysis, new vigor has been injected into the development and clinical implementation of genotypic AST technologies. In this narrative review, we discuss the principles, applications, and advancements of emerging genotypic AST methods in clinical settings. The comprehensive review aims to highlight the significant scientific potential of emerging genotypic AST technologies in clinical AMR diagnosis, providing insights to enhance existing methods and explore novel approaches.

关键词： antimicrobial resistance (AMR) genotypic antibiotic resistance testing (AST) AST technologies review

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Single-cell omics: experimental workflow, data analyses and applications

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Science China Life sciences 2025年第1期68卷 5-102页

作者： Fengying Sun Haoyan Li Dongqing Sun Shaliu Fu Lei Gu Xin Shao Qinqin Wang Xin Dong Bin Duan Feiyang Xing Jun Wu Minmin Xiao Fangqing Zhao Jing-Dong J.Han Qi Liu Xiaohui Fan Chen Li Chenfei Wang Tieliu Shi Department of Clinical Laboratory the Affiliated Wuhu Hospital of East China Normal University (The Second People's Hospital of Wuhu City) Pharmaceutical Informatics Institute College of Pharmaceutical SciencesZhejiang University Key Laboratory of Spine and Spinal Cord Injury Repair and Regeneration (Tongji university) Ministry of EducationOrthopaedic DepartmentTongji HospitalBioinformatics DepartmentSchool of Life Sciences and TechnologyTongji University Frontier Science Center for Stem Cells School of Life Sciences and TechnologyTongji University Translational Medical Center for Stem Cell Therapy and Institute for Regenerative Medicine Shanghai East HospitalBioinformatics DepartmentSchool of Life Sciences and TechnologyTongji University Research Institute of Intelligent Computing Zhejiang Lab Shanghai Research Institute for Intelligent Autonomous Systems Center for Single-cell Omics School of Public HealthShanghai Jiao Tong University School of Medicine National Key Laboratory of Chinese Medicine Modernization Innovation Center of Yangtze River DeltaZhejiang University Center for Bioinformatics and Computational Biology Shanghai Key Laboratory of Regulatory Biologythe Institute of Biomedical Sciences and School of Life SciencesEast China Normal University Beijing Institutes of Life Science Chinese Academy of Sciences Peking-Tsinghua Center for Life sciences Academy for Advanced Interdisciplinary StudiesCenter for Quantitative Biology (CQB)Peking University Zhejiang Key Laboratory of Precision Diagnosis and Therapy for Major Gynecological Diseases Women's HospitalZhejiang University School of Medicine Key Laboratory of Advanced Theory and Application in Statistics and Data Science-MOE School of StatisticsEast China Normal University

Cells are the fundamental units of biological systems and exhibit unique development trajectories and molecular features. Our exploration of how the genomes orchestrate the formation and maintenance of each cell, and control the cellular phenotypes of various organismsis, is both captivating and intricate. Since the inception of the first single-cell RNA technology, technologies related to single-cell sequencing have experienced rapid advancements in recent years. These technologies have expanded horizontally to include single-cell genome, epigenome,proteome, and metabolome, while vertically, they have progressed to integrate multiple omics data and incorporate additional information such as spatial sc RNA-seq and CRISPR screening. Single-cell omics represent a groundbreaking advancement in the biomedical field,offering profound insights into the understanding of complex diseases, including cancers. Here, we comprehensively summarize recent advances in single-cell omics technologies, with a specific focus on the methodology section. This overview aims to guide researchers in selecting appropriate methods for single-cell sequencing and related data analysis.

关键词： single-cell sequencing genome epigenome proteomics metabolomics multimodal spatial transcriptomics CRISPR screening

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