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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

Impact of Startup Strategy and Buffer Tank Volume on the Compressor Inlet State for a 3-MW sCO2 Brayton Cycle

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Journal of Thermal Science 2025年第1期34卷 159-175页

作者： ZHAO Decai WANG Bo key laboratory of Advanced Energy and Power Institute of Engineering Thermophysics(IET)Chinese Academy of Sciences (CAS) University of chinese academy of sciences

The supercritical carbon dioxide（sCO2） Brayton cycle system has become an emerging and highly promising method of thermal power conversion due to its efficiency advantage,system compactness,and excellent adaptability of the heat *** the low carbon sCO2Brayton cycle testbed with cycle output power approaching 3 MW,a relatively detailed dynamic simulation model of the entire system is constructed to explore the dynamic response characteristics of the system with different startup strategies and different buffer tank volumes during the startup *** simulation results indicate that the smaller the volume of the buffer tank,the more rapid and obvious the parameter fluctuation in the buffer tank during the *** the allowable relative deviation limit of density is 5%,then the ratio of the buffer tank volume to the volume of the entire closed loop should not be lower than 36.80%.The strategy of simultaneous temperature and speed increase during turbine bypass start can effectively reduce the fluctuation of compressor inlet parameters and reach the steady-state more *** paper provides the recommended matching table for the opening of the turbine bypass valve（TBV） and the main regulating valve（MGV） to reduce the parameter fluctuation during the bypass *** effectiveness of the proposed turbine bypass and bypass switching startup strategy is verified by simulation,which may be used as a reference for test bench's future debugging and operation.

关键词： buffer tank dynamic characteristic dynamic model sCO2 Brayton cycle startup strategy

Crustal magma oxidation state and endowments in porphyry copper deposits

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Science China Earth sciences 2025年第1期68卷 226-236页

作者： Yumin AI Massimo CHIARADIA Chao WU Huayong CHEN key laboratory of Mineralogy and Metallogeny Guangzhou Institute of Geochemistry Chinese Academy of Sciences University of chinese academy of sciences Department of Earth sciences University of Geneva Guangdong Provincial key laboratory of Mineral Physics and Materials

Porphyry copper deposits（PCDs） supply the majority of the world's copper（Cu） as well as significant amounts of molybdenum（Mo） and gold（Au）. The formation of these deposits is controlled by a variety of geological factors, among which the magmatic oxidation is one of the focuses of current research. This study investigates the redox characteristics of arc magmas by analyzing the ratio of vanadium（V） to scandium（Sc） and its correlation with the oxygen fugacity （fO2） of magmas from arcs of various crustal thicknesses globally. We compiled an extensive dataset of published V/Sc values and studied the partition coefficients of Vand Sc between minerals and silicate melts across various magmatic environments. The results demonstrate that fractional crystallization of magnetite markedly reduces V/Sc values of the residual melt. Furthermore, magnesium number（Mg#） at the onset of magnetite fractionation is strongly positively correlated with fO2of the equilibrium magma. Based on this,the oxidation of arc magmas from different crustal thicknesses can be evaluated. The result suggests that magmas generated in crusts thicker than 20 km tend to be more oxidized with increasing crust thickness. This trend is attributed to enhanced intracrustal differentiation processes involving garnet and amphibole, particularly in mature island and continental arcs. In contrast,magmas in thinner arc crusts（<20 km）, which are significantly influenced by subducted slab materials, display higher oxidation states than most of their thicker crust counterparts. These findings suggest that both subduction dynamics and crustal thickness play a vital role in determining the oxidation state of arc magmas and, consequently, their capacity to generate PCDs. Highly oxidized, primitive arc magmas are less favorable for PCD formation due to that they tend to experience magnetite fractionation and thus sulfide saturation in the early stage of magma evolution, a process leading to copper depletion. On the contra

关键词： Magma evolution V/Sc systematics Magnetite Oxygen fugacity Porphyry copper deposits

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

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

Applications of in-situ solid-state nuclear magnetic resonance in methanol to olefins reaction

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Science China Chemistry 2025年第1期68卷 134-151页

作者： Jing Niu Shutao Xu Yingxu Wei Zhongmin Liu National Engineering Research Center of Lower-Carbon Catalysis Technology Dalian Institute of Chemical PhysicsChinese Academy of Sciences State key laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences University of chinese academy of sciences

The methanol-to-olefins（MTO） reaction offers an alternative pathway for the production of low-carbon olefins from non-oil feedstocks. Fundamental research has been impeded by a lack of comprehensive understanding of its underlying mechanism,despite the significant progress made in industry. In-situ solid-state nuclear magnetic resonance（ss NMR） spectroscopy has emerged as a pivotal tool, offering crucial insights into key species under real-time operando conditions. Furthermore, the host–guest interaction between zeolites or surface species residing on zeolites and the reactant/active intermediates is revealed by the combination of in-situ13C MAS NMR and 2D correlation spectroscopy. Moreover, recent technological advancements in hyperpolarization（HP） methods, including HP129Xe NMR and dynamic nuclear polarization（DNP）, have significantly improved the sensitivity of ss NMR, enabling detailed structural and kinetic analysis as well as the detection of trace species. In this feature article, we summarized recent advancements in（in-situ） ss NMR spectroscopy applied to MTO reaction processes,encompassing mechanistic investigations at various stages and the intricate host–guest interactions. These theoretical insights into the dynamic evolution of MTO reactions lay a solid foundation for the optimization of catalytic processes and the development of efficient catalysts, thereby advancing the techniques towards more sustainable and economical production route for olefins.

关键词： MTO zeolites in-situ ssNMR reactive intermediates reaction mechanism

Aerodynamic Optimization and Flow Mechanism for a Compressor Cascade at Low Reynolds Number

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Journal of Thermal Science 2025年第1期34卷 92-109页

作者： LI Lin ZHANG Jianshe CHEN Caiyan TAN Wei ZHANG Yanfeng key laboratory of Light-Duty Gas-Turbine Institute of Engineering ThermophysicsChinese Academy of Sciences University of chinese academy of sciences National key laboratory of Science and Technology on Advanced Light-duty Gas-turbine

Low-Reynolds-number effect is an important factor affecting the performance of compressors and other main components of high-altitude long-endurance unmanned aerial *** improve the flow condition and reduce flow loss under the condition of high altitude and low Reynolds number(Re),this paper proposes an optimization process based on a surrogate model,which combines the class-shape transformation method(CST),the Latin hypercube sampling(LHS) method,the light gradient-boosting machine algorithm(LightGBM),and a genetic algorithm(GA) to optimize a high-subsonic compressor *** surrogate model is verified to be accurate and can be used in the optimization *** accuracy of the GA is higher than the other algorithms under common test *** optimization results are verified by numerical simulation,and the flow differences before and after optimization are compared,especially the flow within the boundary *** changing the blade shape,the optimization process adjusts the loading distribution to delay the transition of the optimized blade on the suction surface,which changes the turbulent reattachment in the laminar separation bubble(LSB) into laminar ***,the mixing loss induced by the turbulent reattachment of the LSB and the wake loss of turbulent separation at the trailing edge are significantly reduced,and the performance of the compressor profile is finally *** addition,turbulent separation of the optimized profile is delayed reducing the range of the wake region on the suction *** this optimization process,the reduction of total pressure loss coefficient at Re of 2.5×10～5,3.5×10～5,and 4.5×10～5 are 16.32%,20.76%,and 22.16%,respectively.

关键词： Reynolds number

Reconstructing forest and grassland cover changes in China over the past millennium

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Science China Earth sciences 2025年第1期68卷 94-110页

作者： Fanneng HE Fan YANG Yafei WANG key laboratory of Land Surface Pattern and Simulation Institute of Geographic Sciences and Natural Resources Research Chinese Academy of Sciences key Research Institute of Yellow River Civilization and Sustainable Development Henan University University of chinese academy of sciences

Historical forest and grassland cover changes not only are critical indicators for quantifying ecological and environmental change processes but also serve as fundamental data for long-term climate change simulations and terrestrial ecosystem carbon emission assessments. However, because of limitations in historical data, quantitative estimations and spatially gridded reconstructions of these changes remain challenging, necessitating further methodological exploration. This study focused on China's present-day land area over the past millennium, objectively capturing the characteristics and drivers of forest and grassland cover changes. On this basis, using the forest transition theory and the space-for-time substitution method, we depicted the historical deforestation process as an inverted “S” curve and developed a model to reconstruct historical forest area changes based on the functional relationship between the forest area and population size dynamics. Subsequently, a gridded forest allocation model was established on the basis of deforestation tendencies. For the grassland cover, we implemented regionspecific methods, such as the cropland area deduction method and the habitat constraint method, to quantitatively reconstruct historical changes. Consequently, we obtained provincial forest and grassland area changes over the past millennium and mapped 10-km-resolution gridded data of forest and grassland cover. The results indicated the following.(1) The methods developed using population data as a proxy objectively reproduced the spatiotemporal evolution of forest and grassland cover in China over the past millennium. These feasible methods offer a novel pathway for the quantitative reconstruction of historical forest and grassland cover changes.(2) The data indicated that China's forest area generally decreased over the past millennium, characterized by a “decrease-then-increase” pattern. The forest area experienced three distinct phases: a slow decline(AD 1000

关键词： Land use and land cover change Forest Grassland Quantitative reconstruction Gridded reconstruction China historical period

Propagating subduction initiation of the Caroline Plate at the Mussau Trench

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Science China Earth sciences 2025年第1期68卷 253-269页

作者： Chun-Feng LI Yongkang DENG Tao WU Dongdong DONG Guoliang ZHANG Jiazheng ZHANG Yutao LIU Yaqing LI Fugui TANG Lulu ZHANG Department of Marine sciences Zhejiang University laboratory of Marine Mineral Resources Laoshan Laboratory key Lab of Marine Geology and Environment Institute of Oceanology Chinese Academy of Sciences key Lab of Ocean and Marginal Sea Geology South China Sea Institute of Oceanology Chinese Academy of Sciences Science & Technology on Integrated Information System Lab Institute of Software Chinese Academy of Sciences

New seismic imaging from the Mussau Trench confirms that, under horizontal compression on an oceanic plate boundary, it is within the young and weak oceanic plate that a trench will develop, and it is the young plate, not so long after its birth, that starts to subduct toward the old plate. The Mesozoic Pacific Plate cannot easily bend, under the joint horizontal compression and vertical gravity pull, even with a pre-existing weak zone in place and with a large age offset across the plate boundary. The bending of the Caroline Plate near the northern end of the Mussau Trench started only after a long-time span of trench migration, and/or after a prolonged transition from initial compression to trench development. Highly contrasting trench deformation and sedimentary accretion between two parallel seismic sections support an evident migration of underthrusting or significant longitudinal heterogeneity along the trench. The swift transition from underthrusting to non-thrusting can be explained by a counter-clockwise rotation of the Caroline Plate. That miniature accretionary wedges develop even before the subduction initiates imply strong compression and uplifting before the underthrusting can kick-start. Rotation of the Caroline Plate have been halted as the Mussau Trench is seismically rather quiet and the Lyra Trough to the east shows relaxational extension.

关键词： Mussau Trench Subduction initiation Seismic reflection Caroline Plate

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