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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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Transforming waste particles into valuable adsorbents via amyloid-mediated molecular engineering

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Science China Chemistry 2025年第01期 317-328页

作者： Qingmin Yang Jian zhao Yujia Zhang Xingyu Zhou Hao Ren Bowen Hu Zhongli Lei Lixin Chen Peng Yang School of Material and Chemical Engineering Bengbu University Anhui Provincial Engineering Laboratory of Silicon-Based Materials School of Chemistry and Chemical Engineering Northwestern Polytechnical University Key Laboratory of Applied Surface and Colloid Chemistry Ministry of Education School of Chemistry and Chemical EngineeringShaanxi Normal University Xi'an Key Laboratory of Polymeric Soft Matter School of Chemistry and Chemical Engineering Shaanxi Normal University International Joint Research Center on Functional Fiber and Soft Smart Textile School of Chemistry and Chemical EngineeringShaanxi Normal University

The high-value utilization of industrial solid waste using a facile and eco-friendly process is of great interest and significance in reducing environmental pollution and developing a green circular economy. Herein, we propose an amyloid-mediated molecular engineering strategy to transform particulate waste into valuable adsorbents for metal ions. Our method has the advantage of aqueous solution fabrication under mild conditions without the use of high-temperature hydrothermal methods and toxic chemical reagents. Amyloid-mediated molecular engineering manipulates the phase transition of bovine serum albumin(BSA)on particulate waste surfaces, resulting in a remarkable ～3.1 times improvement in the adsorption capacity of fly ash, a typical industrial solid waste for gold ions after modification with the phase-transitioned BSA(PTB). The resultant adsorption ability was 69–1,980 times higher than those of conventional and emerging adsorbent materials such as ion exchange resins, activated carbon(AC), covalent organic frameworks(COFs), and metal-organic frameworks(MOFs). We further demonstrated the application of our PTB-modified materials in the recovery of precious metals from low-grade gold ore and electronic waste leachates. Consequently, this strategy could increase the value of waste materials nearly 27 times. In addition, this method is generally extendable to other conventional industrial adsorbents such as resin, clay, and Al2O3, and enhances their adsorption capabilities at least twofold. Overall, this work provides a simple and green approach for improving the adsorption performance of solid particles, and is expected to develop into a universal strategy for transforming waste particles into high-value-added products.

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Dietary carbohydrate intake and risk of type 2 diabetes:a 16-year prospective cohort study

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Science China Life Sciences 2025年

作者： Lu Gan Yi Yang Bin zhao Kai Yu Kehua Guo Fang Fang Zhiguang Zhou Demetrius Albanes Jiaqi Huang Key Laboratory of Diabetes Immunology Ministry of Education and Department of Metabolism and Endocrinology The Second Xiangya Hospital of Central South University CSU-Sinocare Research Center for Nutrition and Metabolic Health Xiangya School of Public Health Central South UniversityFurong Laboratory Division of Cancer Epidemiology and Genetics National Cancer Institute NIH Department of Health and Human Services School of Computer Science and Engineering Central South University Institute of Environmental Medicine Karolinska Institute National Clinical Research Center for Metabolic Diseases Key Laboratory of Diabetes Immunology Ministry of Education and Department of Metabolism and Endocrinology The Second Xiangya Hospital of Central South University

Despite considerable research underscoring the importance of carbohydrate intake in relation to the risk of type 2 diabetes(T2D), a comprehensive assessment of this relationship is currently lacking. We aimed to examine the associations of various types and food sources of dietary carbohydrate intake with the risk of T2D, to evaluate potential effect modification by other factors, including genetic susceptibility,and to explore the potential mediators for such associations. The present study included 161,872 participants of the UK Biobank who were free of prevalent cancer, cardiovascular disease, or diabetes, and had at least one validated 24-h dietary recall assessment. Multivariableadjusted age-stratified Cox proportional hazard regression models were applied to estimate hazard ratios(HRs) and 95% confidence intervals(CI) for the associations of various types and food sources of dietary carbohydrate intake with risk of T2D. During a median follow-up of13.6 years, 4,176 incident cases of T2D were identified. In the multivariable-adjusted models, a greater intake of fiber, carbohydrates from whole grains, and carbohydrates from non-starchy vegetables was significantly associated with a lower risk of T2D(highest vs. lowest quantile, HR [95% CI]=0.70 [0.62–0.79], 0.74 [0.67–0.82], and 0.83 [0.75–0.92], respectively, all P for trend <0.005). In contrast, a higher intake of starch and carbohydrate from starchy vegetables was associated with an increased risk of T2D(highest vs. lowest quantile, HR [95%CI]=1.31 [1.16–1.48] and 1.19 [1.09–1.31], respectively, both P for trend <0.005). Replacing one serving of refined grains or starchy vegetables with an equal amount of whole grains or non-starchy vegetables was associated with 4% to 10% lower risk of T2D(all P values <0.001).The observed associations were generally similar across population subgroups, including individuals with different genetic susceptibility to T2D. Mediation analyses of the inverse association between T

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Liquid refractive index measurement method based on orthogonal polarization laser self-mixing interference

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Optoelectronics Letters 2025年

作者： zhao Yan WANG Haipeng DU Shengzhi TONG Jigang KANG Jun School of Electrical Engineering and Automation， Tianjin University of Technology Tianjin Key Laboratory for Control Theory and Applications in Complicated Systems Department of Electrical Engineering， Tshwane University of Technology

In this paper， a novel method combining orthogonal polarization laser self-mixing interference is proposed. The method utilizes a rotating cuvette to measure the refractive index of liquids at different concentrations. The cuvette is filled with the liquid to be measured and rotated by a certain angle. The change in the number of interference fringes， caused by comparing an empty cuvette with a liquid-filled cuvette， is used to calculate the refractive index of the liquid. A four-fold logic subdivision algorithm is then used to improve measurement resolution. The experimental results show that for pure water and different NaCl and glucose solutions concentrations， the average relative errors are 0.47%， 0.59%， and 2.17%， respectively， with the maximum relative error within ±2.54%. The standard deviation of all solutions is less than 3.4%.

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Direct and rapid detection of serum amino acid and monoamine neurotransmitters to assist the diagnosis of panic disorder

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Science China Chemistry 2025年第01期 377-384页

作者： Shiwen Liu Xuerui Wan Meng zhao Jiaqi Wang Weilan Wu Linlin You Yonggui Yuan Qian Xu Rong Gao Key Laboratory of Environmental Medicine Engineering Ministry of Education School of Public Health Southeast University Key Laboratory of Modern Toxicology of Ministry of Education Department of Hygienic Analysis and Detection School of Public HealthNanjing Medical University Department of Psychosomatics and Psychiatry Zhongda Hospital School of Medicine Southeast University

The measurement of amino acid and monoamine neurotransmitters（NTs） in serum plays a central role in the identification and monitoring of clinical panic disorder（PD）. However, the strong polarity and chemical heterogeneity of NTs make direct extraction and rapid detection extremely challenging. Herein, we developed a strategy that integrated solid phase extraction based on magnetic Fe3O4coated with polydopamine（Fe3O4@PDA） and direct analysis of mass spectrometry in real time（DART-MS） for quantification of 10 NTs. We systematically investigated the optimal conditions of this strategy to achieve good accuracy and precision. Compared with existing magnetic solid phase extraction methods for NTs detection in biological samples, this strategy could adsorb more targets while having similar adsorption efficiencies, and the total process time was reduced by an average of 69.42%. We rapidly determined the metabolic abnormality of 6 types of NTs in the serum of PD patients and demonstrated their diagnostic accuracy. In addition, an outstanding feature of PD in which tryptophan was more metabolized by the KYN pathway and the 5-hydroxytryptamine pathway was inhibited could be elucidated by this strategy. Our results highlighted the potential ability of Fe3O4@PDA coupled with DART-MS to assist in the clinical diagnosis of PD.

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An efficient and balanced feature pyramid network: shared-FPN

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Optoelectronics Letters 2025年

作者： Tian Sulong Qin Longfei Pang Wenchao Gao Ying zhao Dexin School of Computer Science and Engineering， Tianjin University of Technology Tianjin Key Laboratory of Intelligence Computing and Novel Software Technology， Tianjin University of Technology

In the field of object detection， it is challenging to achieve a balance between neck complexity and accuracy. To address this issue， we propose an efficient and decoupled neck module called Shared-FPN(Shared Feature Pyramid Network). Our design aims to effectively address the trade-off between these two factors. Neck modules are crucial for effectively fusing multi-scale information in neural network models. However， traditional neck designs， with their single structure， have struggled to significantly improve detection performance. In recent years， the incorporation of neural architecture search techniques in neck design has led to an increase in model complexity. This trade-off between model complexity and detection performance highlights the need for more efficient neck design approaches. Not only does Shared-FPN not increase the number of model parameters and FLOPs， but it also can be easily ported to any of the detection models. It improves on PAFPN by using transposed convolution with a large convolution kernel as the upsampling module， designing spatial pyramidal pooling-fast downsampling(SPPFD) based on shared pooling， and designing shared convolution as the right part module. To evaluate the performance of Shared-FPN in object detection tasks， we conducted experiments on object detection datasets. The results show that Shared-FPN achieved excellent performance across all sizes. In particular， on the VOC 2012 dataset， which contains mostly large objects， Shared-FPN's mAP was improved by 11.2% compared to FPN with YOLOX-s as the detector. On the COCO dataset， which contains mostly small objects， Shared-FPN's mAP was improved by 7.8% compared to FPN and 7.1% compared to PAFPN with Faster RCNN as the detector. Shared-FPN can be easily inserted into any of the detectors for better performance in various scenarios， such as small， medium or large objects.

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Effects on antioxidant enzyme activities and osmolytes in Halocnemum strobilaceum under salt stress

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Research in Cold and Arid Regions 2016年第1期8卷 65-71页

作者： TianPeng Gao Rui Guo XiangWen Fang ZhiGang zhao GuoHua Chang yinquan Chen Qing Zhang Centre of Urban Ecology and Environmental Bioteehnology Lanzhou City UniversityLanzhouGansu 730070China State Key Laboratory of Grassland Agro-ecosystems Institute of Arid AgroecologySchool of Life SciencesLanzhou UniversityLanzhouGansu 730000China School of Chemistry and Environment Sciences Lanzhou City UniversityLanzhouGansu 730070China

The seedlings of Halocnermum strobilaceum were cultivated in 0.5% hoagland nutrient solution containing 0.0%, 0.9%, 2.7% and 5.4% of NaC1 as well as composite salt （Na^＋, Ca^2＋, K^＋, Si^4＋） for 20 days; all the contents are in weight ratio. Succulent level, inorganic ions （Na^＋, K^＋）, organics such as betaine, proline, malondialdehyde, and antioxidant enzyme activities including superoxide dismutase （SOD）, catalase （CAT）, peroxidase （POD）, betaine aldehyde dehydrogenase （BADH） were measured to reveal its salt tolerance mechanism. When the composite salt concentration reaches 5.4%, SOD activity level, and MDA content is five times the control group; when it reaches 2.7%, the succulent level of seedlings, and the content ofK＋ in roots is nearly two times the NaCl treatment; the dry weight is more than three times the control group; with the NaCl treatment, MDA is three times the contrast; when the salt concentration is 2.7%, POD reaches the maximum. Results indicate that Si^4＋, K^＋, and Ca^20 from composite salt in the roots of H. strobilaceum improved the water-holding capacity. The activities of antioxidant enzyme were raised by the accumulation ofproline and betaine, which increased the salt tolerance. The absorption of K^＋ promoted the high ratio of K^＋/Na^＋ and alleviated the damage of cell membranes of H. strobilaceum, which is associated with osmotic contents such as betaine and proline.

关键词： Halocnermum strobilaceum (Pall.) salt stress succulent antioxidant enzyme activities

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Molecule‑Level Multiscale Design of Nonflammable Gel Polymer Electrolyte to Build Stable SEI/CEI for Lithium Metal Battery

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Nano-Micro Letters 2025年第1期17卷 404-423页

作者： Qiqi Sun Zelong Gong Tao Zhang Jiafeng Li Xianli Zhu Ruixiao Zhu Lingxu Wang Leyuan Ma Xuehui Li Miaofa Yuan Zhiwei Zhang Luyuan Zhang zhao Qian Longwei Yin Rajeev Ahuja Chengxiang Wang Key Laboratory for Liquid‑Solid Structural Evolution and Processing of Materials(Ministry of Education) School of Materials Science and EngineeringShandong UniversityJinan 250061People’s Republic of China Condensed Matter Theory Department of Physics and AstronomyUppsala UniversityUppsala 75120Sweden

The risk of flammability is an unavoidable issue for gel polymer electrolytes(GPEs).Usually,flameretardant solvents are necessary to be used,but most of them would react with anode/cathode easily and cause serious interfacial instability,which is a big challenge for design and application of nonflammable ***,a nonflammable GPE(SGPE)is developed by in situ polymerizing trifluoroethyl methacrylate(TFMA)monomers with flame-retardant triethyl phosphate(TEP)solvents and LiTFSI–LiDFOB dual lithium *** is strongly anchored to PTFMA matrix via polarity interaction between-P=O and-CH_(2)CF_(3).It reduces free TEP molecules,which obviously mitigates interfacial reactions,and enhances flame-retardant performance of TEP *** TEP molecules are also inhibited in solvation of Li^(+),leading to anion-dominated solvation sheath,which creates inorganic-rich solid electrolyte interface/cathode electrolyte interface *** coordination structure changes Li^(+)transport from sluggish vehicular to fast structural transport,raising ionic conductivity to 1.03 mS cm^(-1) and transfer number to 0.41 at 30℃.The Li|SGPE|Li cell presents highly reversible Li stripping/plating performance for over 1000 h at 0.1 mA cm^(−2),and 4.2 V LiCoO_(2)|SGPE|Li battery delivers high average specific capacity>120 mAh g^(−1) over 200 *** study paves a new way to make nonflammable GPE that is compatible with Li metal anode.

关键词： Anchoring effect Nonflammable gel electrolyte In situ cross-linked Electrode-electrolyte interface Li metal battery

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Efficient and Stable Photoassisted Lithium‑Ion Battery Enabled by Photocathode with Synergistically Boosted Carriers Dynamics

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Nano-Micro Letters 2025年第3期17卷 440-454页

作者： Zelin Ma Shiyao Wang Zhuangzhuang Ma Juan Li Luomeng zhao Zhihuan Li Shiyuan Wang Yazhou Shuang Jiulong Wang Fang Wang Weiwei Xia Jie Jian Yibo He Junjie Wang Pengfei Guo Hongqiang Wang State Key Laboratory of Solidification Processing Center for Nano Energy MaterialsSchool of Materials Science and EngineeringNorthwestern Polytechnical University and Shaanxi Joint Laboratory of Graphene(NPU)Xi’an 710072People’s Republic of China State Key Laboratory of Solidification Processing School of Materials Science and Engineering DepartmentNorthwestern Polytechnical UniversityXi’an 710072People’s Republic of China State Key Laboratory of Solidification Processing Center of Advanced Lubrication and Seal MaterialsSchool of Materials Science and EngineeringNorthwestern Polytechnical UniversityXi’an 710072People’s Republic of China Research and Development Institute of Northwestern Polytechnical University in Shenzhen Shenzhen 518063People’s Republic of China Key Laboratory of Applied Surface and Colloid Chemistry Shaanxi Key Laboratory for Advanced Energy DevicesShaanxi Engineering Lab for Advanced Energy TechnologySchool of Materials Science and EngineeringNational Ministry of EducationShaanxi Normal UniversityXi’an 710119People’s Republic of China

Efficient and stable photocathodes with versatility are of significance in photoassisted lithium-ion batteries(PLIBs),while there is always a request on fast carrier transport in electrochemical active *** work proposes a general approach of creating bulk heterojunction to boost the carrier mobility of photocathodes by simply laser assisted embedding of plasmonic *** employed in PLIBs,it was found effective for synchronously enhanced photocharge separation and transport in light charging ***,experimental photon spectroscopy,finite difference time domain method simulation and theoretical analyses demonstrate that the improved carrier dynamics are driven by the plasmonic-induced hot electron injection from metal to TiO_(2),as well as the enhanced conductivity in TiO2 matrix due to the formation of oxygen vacancies after Schottky *** from these merits,several benchmark values in performance of TiO2-based photocathode applied in PLIBs are set,including the capacity of 276 mAh g^(−1)at 0.2 A g^(−1)under illumination,photoconversion efficiency of 1.276%at 3 A g^(−1),less capacity and Columbic efficiency loss even through 200 *** results exemplify the potential of the bulk heterojunction strategy in developing highly efficient and stable photoassisted energy storage systems.

关键词： Photoassisted lithium-ion batteries Bulk heterojunction Carrier dynamics TiO2 nanofiber Plasmonic metal nanocrystals

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Negative PO3-implanted bionic ion transport channels for promoting Li-S battery

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Science China Chemistry 2025年

作者： Wenhuan Huang Shun Wang Xuehan Hou Yanan Zhang Xingxing Zhang Yaoxiao zhao Xilang Jin Huabin Zhang Fei Wang Jian Zhang Key Laboratory of Chemical Additives for China National Light Industry College of Chemistry and Chemical EngineeringShaanxi University of Science and Technology School of Materials and Chemical Engineering Xi'an Technological University Chemistry Program Physical Science and Engineering Division King Abdullah University of Science and Technology State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences

Lithium-sulfur （Li-S） battery,as a promising next-generation high-energy-density battery,suffers from lithium polysulfides（LPSs） shuttle and Li dendrites *** crystalline framework-based membranes as separator can effectively absorb and restrain LPSs but without precise structural design principal exploration and mechanism ***,bio-inspired 1D oriented lithium-ion transport channels with molecular negatively charged PO3（-1） have been developed in hybrid tetrazole frameworks for promoting the transmission of Li+*** theoretical calculations and in situ spectroscopy demonstrated the higher binding energy and inhibited diffusion of LPSs in *** assembled PP@PO3Janus separator in Li-S coin cell delivered a high initial capacity of 1410.9 mAh g-1at 0.1 C and a low attenuation rate of 0.038%per cycle over 500 cycles at 5 ***,the high capacities of 862,542 and 409 mAh g-1based on high-sulfur-loading cathodes of 2.6,3.8 and 5.0 mg cm-2at0.5 C were achieved,***,the punch battery of PO3@PP separator with S-cathode of 1.2 mg cm-2has been developed for demonstrating its potentials commercial application,which displays impressive capacity of 873.4 mAh g-1with the retention of～78.9%over 50 cycles.

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