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

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

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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

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Sky location of massive black hole binaries in the foreground of Galactic white dwarf binaries

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Science China(Physics,Mechanics & Astronomy) 2025年第1期Mechanics & Astronomy) .卷 97-108页

作者： Pan Guo Hong-Bo Jin Cong-Feng Qiao Yue-Liang Wu The International Centre for Theoretical Physics Asia-Pacific University of Chinese Academy of Sciences The School of Physical Sciences University of Chinese Academy of Sciences Institute for Frontiers in Astronomy and Astrophysics Beijing Normal University national Astronomical Observatories Chinese Academy of Sciences Institute of Theoretical Physics Chinese Academy of Sciences

For space-based gravitational wave （GW） detection,the main noise source for massive black hole binaries （MBHBs） is attributed to approximately 10～7double white dwarf binaries in the *** a GW source,the amplitude of the detector response,recorded by a space-based gravitational wave detector,exhibits a modulation effect with a year period when observing the source from various orbital *** the adverse conditions mentioned above,where there is a strong foreground noise and annual modulation in the signals,we employed the wavelet transform and the strong-amplitude relevant orbital position search methods,which allows the weak MBHB sources to achieve higher locating *** detail,for two MBHB sources of lower intensity,the precision of luminosity distance,represented by the ratio ?DL/DLat the 95%confidence level,is enhanced by factors of ～*** angular resolutions,denoted by??s,are enhanced by a factor of ～*** improvements increase the number of detectable GW sources,facilitate multi-messenger follow-up observations and provide constraints on the cosmological constant.

关键词： space-based gravitational wave detection gravitational waves massive black hole binaries

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Synergistic promotion strategy of “dual-site” and “dual-path” to enhance the C–C coupling between CO2 and HCHO driven by photoelectrocatalysis

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Journal of Energy Chemistry 2025年第1期100卷 39-49页

作者： Hongqiang Yang Jianfeng Zheng Guoyu Wang Yifei Gao Yatao Yang Jia Li Xiaojin Han Yan Cui Zhanggen Huang national Key Laboratory of High Efficiency and Low Carbon Utilization of Coal Institute of Coal Chemistry Chinese Academy of Science University of Chinese academy of Science Shenyang University of Chemical Technology

Photoelectrocatalytic coupling CO2and volatile organic compounds （VOCs） is a promising green strategy for the synergistic conversion of the two carbon-containing resources to *** catalytic efficiency is always at the mercy of chemical inertness of CO2and the competitive hydrogen evolution of ***,a modified g-C3N4/ZnAl-LDH Z-scheme heterojunction catalyst with dual reaction site was rationally designed and precisely *** Faraday efficiency of ethanol reached 68.67%with a corresponding formation rate of 227.3μmol *** revealed by in-situ characterizations and density functional theory calculations,CO2and HCHO were absorbed at Zn site and N site,***,*CO generated from CO2and HCHO was converted to*CH3O and*CHO on the dual-active-site *** detailed reaction mechanism experiments indicated that C–C coupling only occurred between*CO and*CH3O in electrocatalysis *** from the“*CO+*CH3O”path,another“*CO+*CHO”coupling path was also detected in photoelectrocatalytic *** selectivity of ethanol was significantly enhanced due to the synthesis of dual-site catalyst and the dual-path coupling path between CO2and HCHO simultaneously driven by light and electricity.

关键词： Ethanol

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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

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Optimizing Fine-Tuning in Quantized Language Models:An In-Depth Analysis of Key Variables

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Computers, Materials & Continua 2025年第1期82卷 307-325页

作者： Ao Shen Zhiquan Lai Dongsheng Li Xiaoyu Hu national Key Laboratory of Parallel and Distributed Computing National University of Defense TechnologyChangsha410073China Strategic Assessments and Consultation Institute Academy of Military ScienceBeijing100091China

Large-scale Language Models(LLMs)have achieved significant breakthroughs in Natural Language Processing(NLP),driven by the pre-training and fine-tuning *** this approach allows models to specialize in specific tasks with reduced training costs,the substantial memory requirements during fine-tuning present a barrier to broader ***-Efficient Fine-Tuning(PEFT)techniques,such as Low-Rank Adaptation(LoRA),and parameter quantization methods have emerged as solutions to address these challenges by optimizing memory usage and computational *** these,QLoRA,which combines PEFT and quantization,has demonstrated notable success in reducing memory footprints during fine-tuning,prompting the development of various QLoRA *** these advancements,the quantitative impact of key variables on the fine-tuning performance of quantized LLMs remains *** study presents a comprehensive analysis of these key variables,focusing on their influence across different layer types and depths within LLM *** investigation uncovers several critical findings:(1)Larger layers,such as MLP layers,can maintain performance despite reductions in adapter rank,while smaller layers,like self-attention layers,aremore sensitive to such changes;(2)The effectiveness of balancing factors depends more on specific values rather than layer type or depth;(3)In quantization-aware fine-tuning,larger layers can effectively utilize smaller adapters,whereas smaller layers struggle to do *** insights suggest that layer type is a more significant determinant of fine-tuning success than layer depth when optimizing quantized ***,for the same discount of trainable parameters,reducing the trainable parameters in a larger layer is more effective in preserving fine-tuning accuracy than in a smaller *** study provides valuable guidance for more efficient fine-tuning strategies and opens avenues for further research into optimizing LLM

关键词： Large-scale Language Model Parameter-Efficient Fine-Tuning parameter quantization key variable trainable parameters experimental analysis

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Unlocking the potential of spatial transcriptomics with custom microfluidic chips

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Science China Life Sciences 2025年

作者： Bingqi Wu Yuan Gao China national Center for Bioinformation Beijing Institute of Genomics Chinese Academy of Sciences University of Chinese academy of Sciences

Spatial transcriptomics technique detects RNA sequences (St?hl et al.,2016) and quantifies their expression in the positional context (Ke et al.,2013),which can provide important information such as cell heterogeneity,cell developmental trajectory,differential gene expression between tissue regions or *** date,it is becoming a powerful tool for exploring tumorigenesis (Ren et al.,2023),cerebral neurodevelopment (Shi et al.,2023),embryonic development(Arutyunyan et al.,2023),and other biological ***-dimensional(3D) spatial transcriptome typically requires stacking multiple tissue slices to obtain a 3D atlas (Schott et al.,2024);therefore it prefers a method that meets high throughput,large sample sizes,and affordable cost to cover large regions of the ***,the lack of a single method that meets all of these requirements limits large-scale application of 3D spatial transcriptomics.

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When AI meets sustainable 6G

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Science China(Information Sciences) 2025年第1期68卷 4-22页

作者： Xiaohu YOU Yongming HUANG Cheng ZHANG Jiaheng WANG Hao YIN Hequan WU national Mobile Communications Research Laboratory Southeast University Purple Mountain Laboratories Chinese academy of Military Science China Information Communication Technologies Group

Sixth-generation(6G) networks are anticipated to achieve transformative advancements, characterized by extreme connectivity, deep integration with artificial intelligence(AI) and sensing, and airground integration. The evolution of 6G exhibits two major trends: ubiquitous intelligence and sustainability. The former aims to embed state-of-the-art AI technology into the 6G network, from the physical layers to applications, while the latter emphasizes reducing energy consumption while enhancing network performance to address environmental concerns. Despite the amazing progress in recent years, AI advancements come with substantial increases in data and computational overhead, posing critical challenges for integrating AI into sustainable 6G networks. First, high energy consumption from large datasets and heavyweight AI models contradicts6G's green goals. Second, the precise collection of large datasets, message delivery latency, and inference delays in AI models pose challenges for real-time tasks in 6G. Third, the uninterpretability and unpredictability of AI models complicate meeting the stringent requirements for controllable transmission in dynamic wireless environments. Addressing these challenges and achieving sustainable 6G with ubiquitous intelligence calls for a revolutionary design of 6G architecture and AI frameworks. To this end, this paper introduces a novel and practical methodology for green, real-time, and controllable 6G native intelligence,starting with knowledge graph(KG) analysis to extract small but critical datasets, followed by the development of distributed lightweight AI models, and the use of digital twins(DTs) to create precise replicas of physical 6G networks. This leads to a pervasive multi-level(PML)-AI framework supported by a task-centric, three-layer 6G architecture. The AI framework operates through non-real-time and real-time cycles, leveraging three key technologies: wireless data KGs for efficient data management,lightweight AI mode

关键词： artificial intelligence sustainable 6G green real-time controllable

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Distribution and mapping of temperate savanna in the sandy lands of eastern China

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Science China Earth Sciences 2025年第1期68卷 128-141页

作者： Xiaoya LI Feng WANG Tao DUAN Kaijie YANG Bin YANG Chunmei WANG Xin TIAN Qi LU Institute of Ecological Conservation and Restoration Institute of Desertification Studies Chinese Academy of Forestry Institute of Desertification Institute of Desertification Studies Chinese Academy of Forestry Institute of Great Green Wall Satellite Application Centre for Ecology and Environment MEE Institute of Microelectronics Chinese Academy of Sciences Aerospace Information Research Institute Chinese Academy of Sciences Institute of Forest Resource Information Techniques Chinese Academy of Forestry

Savannas are distributed globally across various *** perform a significant socioeconomic role in regulating net primary productivity and the terrestrial carbon *** to the high spatial heterogeneity induced by the mixed distribution of trees and grasses,current global land-cover classification maps often classify savannas as forests or grasslands Temperate savannas in China cover a vast area,yet their spatial patterns and extent remain poorly *** study developed a novel remote sensing temperate savannas mapping method by integrating very high-resolution （VHR） unmanned aerial vehicle （UAV） and GF-6 satellite imagery based on the vegetation structure characteristics of temperate savannas using the FAO definition of *** and validation datasets were collected from VHR UAV imagery covering the main temperate savannah types with a ground area of 1818 *** fractional woody vegetation cover （FWVC） and fractional herbaceous vegetation cover （FHVC） in temperate savannas were estimated by integrating Classification and Regression Tree and Random Forest *** current distribution of temperate savannas in the Horqin and Otindag Sandy Lands of Eastern China was mapped to a unit area of 0.5 *** root-mean-square error （RMSE） values for the FWVC and FHVC models were 10.69% and 11.67%,and the R2values were 0.66 and 0.63,*** assessment indicated that the new temperate savanna map had high identification accuracy,with a Kappa coefficient of 0.70,overall accuracy of 0.88,and average accuracy of *** savannas in the sandy lands of eastern China were primarily distributed in the northern Horqin Sandy Land the central and eastern regions of the Otindag Sandy Land,and the transition zone from the southern slopes of the Greater Khingan Mountains to the plains,covering a total area of 3.27×10～6 *** main savannah types were elm,oak/maple,and shrub *** savannas were widely distributed in the Otindag Sandy

关键词： Temperate savanna UAV imagery GF-6 Fractional woody vegetation cover Fractional herbaceous vegetation cover Machine learning

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Anomalous quality factor evolution of induced transparency in a virtualized coupled-oscillator system

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Science China(Physics,Mechanics & Astronomy) 2025年第1期Mechanics & Astronomy) .卷 148-155页

作者： Yunhan Yang Han Jia Tuo Liu Yuzhen Yang Jun Yang Key Laboratory of Noise and Vibration Research Institute of Acoustics Chinese Academy of Sciences University of Chinese academy of Sciences State Key Laboratory of Acoustics Institute of Acoustics Chinese Academy of Sciences

The phenomenon of induced transparency, characterized by a high quality(Q) factor, holds significant importance in the fields of high-precision sensing, energy storage and wave manipulation. Conventional transparency systems are often constrained by the limited experimentally accessible parameter space and the lack of independent control over intrinsic parameters, thereby hindering advanced research on high-Q effects. Here we propose a virtualized coupled-oscillator system that enables reconfigurable induced transparency in the reflection spectrum. By virtually incorporating a pair of coupled oscillators into an individual acoustic meta-atom, we achieve the manipulation of induced transparency in a decoupled, wide-ranging, and elaborate manner. Exploiting the diverse evolutions across the intrinsic parameter space, we show experimentally a counter-intuitive increase in the Q-factor of the transparency window, which is attributed to the enhanced dissipation of the bright ***, a constant group delay at the center frequency is observed accompanying this evolution. Our work demonstrates an intriguing platform as well as a novel strategy to engineer high-Q induced transparency phenomenon, and paves the way towards applications in programmable acoustic sensors, filters and slow-wave devices.

关键词： induced transparency acoustic meta-atom high quality-factor scattering programmable intrinsic parameter

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