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Rare Metals 2024年第6期43卷 2536-2545页

作者： Lin-Tao dou Bei Li Hao-Long Nie Dong-Dong Xiao Chao-Qun Shang Xiao-Min Wang Zhan-Hui Zhang Katerina e.Aifantis Pu Hu School of Materials Science and engineering Wuhan Institute of TechnologyWuhan 430205China Huairou Division Institute of PhysicsChinese Academy of SciencesBeijing 101400China Department of Mechanical and Aerospace engineering University of FloridaGainesvilleFL 32603USA

LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)is the most promising cathode for high-energy Li-ion batteries,despite its poor cycling stability that originates from the reactions that occur with the ***,to solve this interfacial issue,a facile electrolytic electrochemical polymerization process was introduced in this paper,and a uniform conductive electrolyte interfa.e(polyaniline)was successfully constructed on the surfa.e of the NCM811 porous electrode(PANI-NCM),which facilitated the charge transfer during charge/*** side reactions at the interfa.e between the cathode and the electrolyte are suppressed,and thereby,the cycling performance and rate capability are considerably ***-NCM delivers an initial capacity of 157.2 mAh·g^(-1)as well as excellent cyclability(capacity retention of 88%after 500 cycles at 2C),whereas the capacity of the bare NCM811 has dropped to 31.3 mAh·g^(-1).In addition,polypyrrole and polythiophene also can be formed through electrolytic electrochemical polymerization process,which provides a practicable tactic to modify the interfacial stability of cathodes for high-energy Li-ion batteries.

关键词： Lithium-ion battery Ni-rich cathode In-situ polymerization Conductive polymer electrochemical performance

Co-aromatization of methane and hexane over Pt encapsulated in ZSM-5 zeolite and the electronic effect of K promoters

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Science China Chemistry 2024年第3期67卷 1017-1027页

作者： Bei Liu fan Wang Xiaomeng dou Pengfei Li Hongwei Xiang Yong Yang Peng He State Key Laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001China Department of Chemistry Tsinghua UniversityBeijing 100084China National energy R&D Center for Coal to Liquid Fuels Synfuels China Technology Co.Ltd.Beijing 101407China University of Chinese Academy of Sciences Beijing 101408China Leibniz-Institut für Katalyse e.V.an der Universitat Rostock Rostock 18059Germany

The co-aromatization of methane with higher hydrocarbons represents a promising route to valorize methane, an abundant but underexploited carbon resource. In this study, we elucidate a novel approach to enhance the catalytic co-aromatization of hexane and methane by confining Pt within zeolite catalysts and modulating its electron density. Our findings show that encapsulating Pt within MFI structure is pivotal for activating the feedstock and fostering the formation of aromatic products. Interaction between K atoms and the silanol nest forms siloxy groups which are critical for the stabilization of Pt species. Tuning the K content in PtSn@MFI catalysts adeptly alters the electronic configuration of Pt clusters. This modification is corroborated by infrared and X-ray photoelectron spectroscopy analysis, and density functional theory calculations. Remarkably, the catalyst with 0.8 wt% K exhibits an optimal Pt electron density, driving its superior efficacy in the co-aromatization reaction, converting 0.78 mol of methane for each mole of hexane processed. By employing ~(13)C isotopic labeling and solid-state NMR studies, we demonstrate the participation of methane in the adsorbed species inside the zeolite channel and its incorporation to the benzyl site of the substitute group and phenyl rings in aromatic compounds, underscoring the importance of Pt encapsulation.

关键词： Pt encapsulation MFI zeolite methane activation co-aromatization ^(13)C solid-state NMR

A systematic understanding of microbial reductive dechlorination towards an improved “one health” soil bioremediation: A review and perspective

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Science China Technological Sciences 2024年第10期67卷 3009-3031页

作者： He Yan LI ShuYao YUAN Jing CHeNG Jie dou JiBo YANG XueLing XU JianMing Zhejiang Provincial Key Laboratory of Agricultural Resources and environment Institute of Soil and Water Resources and Environmental ScienceCollege of Environmental and Resource SciencesZhejiang University Key Laboratory of environment Remediation and ecological Health Ministry of Education Microbiome Network and Department of Agricultural Biology Colorado State University Departments of Chemistry and Chemical & Biomolecular engineering Institute for Functional Intelligent Materials (I-FIM)National University of Singapore

Chlorinated organic pollutants(COPs), both emerging and traditional, are typical persistent pollutants that harm soil health worldwide. Dechlorinators mediated reductive dechlorination is the optimal way to completely remove COPs from anaerobic soil through a redox reaction driven by electron transfer during microbial anaerobic respiration. Generally, the dechlorinated depletion of COPs in situ often interacts with multiple element biogeochemical activities, e.g., methanogenesis, sulfa.e reduction, iron reduction, and denitrification. elucidating the relevance of biogeochemical cycles between COPs and multiple elements and the coupled mechanisms involved, thus, helps to develop effective pollution control strategies with the balance between pollution degradation and element cycles in heterogeneous soil, ultimately contributing to “one health” goal. In this review, we summarized the microbial-chemical coupling redox processes and the driving factors, elucidated the interspecies metabolites exchange and electron transfer mechanisms within COP-dechlorinating communities, and further proposed a detailed design, construction, and analysis framework of engineering COP-dechlorinating microbiomes via “top-down” selfassembly and “bottom-up” synthesis to pave the way from laboratory to practical field application. especially, we delve into the major challenges and perspectives surrounding the design of state-of-the-art synthetic microbial communities. Our goal is to improve the understanding of the microbial-mediated coupling between reductive dechlorination and element biogeochemical cycling, with a particular focus on the implications for health-integrated soil bioremediation under the “one health” concept.

关键词： reductive dechlorination biogeochemical redox processes interspecies interaction synthetic microbiomes, anaerobic soils

Comprehensive analysis and mitigation strategies for safety issues of sodium-ion batteries

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Rare Metals 2024年第4期43卷 1343-1349页

作者： Tao Wei Xiao-Ling Xian Shi-Xue dou Wei Chen Shu-Lei Chou Institute for Carbon Neutralization College of Chemistry and Materials EngineeringWenzhou UniversityWenzhou325035China Wenzhou Key Laboratory of Sodium-Ion Batteries Wenzhou University Technology Innovation Institute for Carbon NeutralizationWenzhou325035China Zhejiang Key Laboratory of Carbon Materials College of Chemistry and Materials EngineeringWenzhou UniversityWenzhou325035China Institute for Superconducting and electronic Materials Australian Institute for Innovative MaterialsUniversity of WollongongInnovation CampusWollongongNSW2522Australia

Sodium-ion batteries show great potential as an alternative energy storage system,but safety concerns remain a major hurdle to their mass *** paper analyzes the key factors and mechanisms leading to safety issues,including thermal runaway,sodium dendrite,internal short circuits,and gas *** promising solutions are proposed,such as high-safety electrode materials in the cathode and anode,high-safety electrolytes,and external battery management *** in also we emphasize the importance of selecting appropriate analysis methods and developing reliable failure models while suggesting advanced machine learning tools for *** a comprehensive approach,this study offers valuable recommendations to optimize materials and solutions for improving the safety of sodium-ion batteries.

关键词： Sodium-ion batteries Safety issues Thermal runaway Sodium dendrites

Degradation properties of fulvic acid and its microbially driven mechanism from a partial nitritation bioreactor through multi-spectral and bioinformatic analysis

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Journal of environmental Sciences 2024年第1期135卷 318-331页

作者： Quanhao dou Li Zhang Tingjun Dong Zixuan Song Xuepeng fan Yongzhen Peng Xiayan Wang Jiachun Yang National engineering Laboratory for Advanced Municipal Wastewater Treatment and Reuse Technology Key Laboratory of Beijing for Water Quality Science and Water Environment Recovery EngineeringBeijing University of TechnologyBeijing 100124China Department of Chemistry and Biology Center of Excellence for Environmental Safety and Biological EffectsBeijing Key Laboratory for Green Catalysis and SeparationBeijing University of TechnologyBeijing 100124China environmental Protection Development Group Co. Ltd.Shandong 250101China

This study employed multispectral techniques to evaluate fulvic acid(fa)compositional characteristic and elucidate its biodegradation mechanisms during partial nitritation(PN)*** showed that fa removal efficiency(FRe)decreased from 90.22 to 23.11%when fa concentrations in the reactor were increased from 0 to 162.30 mg/L,and that molecular size,degree of aromatization and humification of the effluent fa macromolecules all increased after *** population analysis indicated that the proliferation of the Comamonas,OLB12 and Thauera exhibit high fa utilization capacity in lower concentrations(e degradation and removal of macromolecular *** addition,the sustained increase in external fa may decrease the abundance of above functional microorganisms,resulting in a rapid drop in ***,from the genetic perspective,the elevated fa levels restricted carbohydrate(ko00620,ko00010 and ko00020)and nitrogen(HAO,AMO,NIR and NOR)metabolism-related pathways,thereby impeding fa removal and total nitrogen loss associated with N_(2)O emissions.

关键词： Partial nitritation Fulvic acid 3DeeM-PARAfaC UV/Vis Microbially driven mechanism

Novel C_(sf)/SiBCN composites prepared by densifying C_(sf)/MA-SiBCN with the PIP process:Oxidation behavior and damage mechanism

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Journal of Advanced Ceramics 2024年第5期13卷 666-678页

作者： Wenhao dou Daxin Li Bingzhu Wang Zhihua Yang Jun Chen Dechang Jia Ralf Riedel Yu Zhou Institute for Advanced Ceramics School of Materials Science and EngineeringHarbin Institute of TechnologyHarbin 150001China Key Laboratory of Advanced Structural-Functional Integration Materials and Green Manufacturing Technology Harbin Institute of TechnologyHarbin 150001China Chongqing Research Institute of HIT Chongqing 401135China Beijing Institute of Control engineering Beijing 100094China Institut für Materialwissenschaft Technische Universität DarmstadtDarmstadt D-64287Germany School of Materials Science and engineering Harbin Institute of Technology(Shenzhen)Shenzhen 518055China

To improve the oxidation resistance of short carbon fiber(C_(sf))-reinforced mechanically alloyed SiBCN(MA-SiBCN)(C_(sf)/MA-SiBCN)composites,dense amorphous C_(sf)/SiBCN composites containing both MA-SiBCN and polymer-derived ceramics SiBCN(PDCs-SiBCN)were prepared by repeated polymer infiltration and pyrolysis(PIP)of layered C_(sf)/MA-SiBCN composites at 1100℃,and the oxidation behavior and damage mechanism of the as-prepared C_(sf)/SiBCN at 1300–1600℃ were compared and discussed with those of C_(sf)/*** C_(sf)/MA-SiBCN composites resist oxidation attack up to 1400℃ but fail at 1500℃ due to the collapse of the porous framework,while the PIP-densified C_(sf)/SiBCN composites are resistant to static air up to 1600℃.During oxidation,oxygen diffuses through preexisting pores and the pores left by oxidation of carbon fibers and pyrolytic carbon(PyC)to the interior of the *** to the oxidative coupling effect of the MA-SiBCN and PDCs-SiBCN matrices,a relatively continuous and dense oxide layer is formed on the sample surfa.e,and the interfacial region between the oxide layer and the matrix of the as-prepared composite contains an amorphous glassy structure mainly consisting of Si and O and an incompletely oxidized but partially crystallized matrix,which is primarily responsible for improving the oxidation resistance.

关键词： mechanically alloyed SiBCN(MA-SiBCN) polymer-derived ceramics SiBCN(PDCs-SiBCN) short carbon fiber-reinforced SiBCN(C_(sf)/SiBCN)composites polymer infiltration and pyrolysis(PIP) oxidation damage mechanism

Robust Cross-Linked Na_(3)V_(2)(PO_(4))_(2)F_(3) Full Sodium-Ion Batteries

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energy & environmental Materials 2024年第1期7卷 9-20页

作者： Jinqiang Gao Ye Tian Lianshan Ni Baowei Wang Kangyu Zou Yingchang Yang Ying Wang Craig e.Banks dou Zhang Kechao Zhou Huan Liu Wentao Deng Guoqiang Zou Hongshuai Hou Xiaobo Ji College of Chemistry and Chemical engineering Central South UniversityChangsha 410083China College of Material and Chemical engineering Tongren UniversityTongren 554300China Department of Chemistry The Chinese University of Hong KongShatinN.T.Hong Kong S.A.R.China faculty of Science and engineering Manchester Metropolitan UniversityManchester UK State Key Laboratory of Powder Metallurgy Central South UniversityChangsha 410083China School of Materials Science and engineering Hunan Provincial Key Lab of Advanced Materials for New Energy Storage and ConversionHunan University of Science and TechnologyXiangtan 411201China School of Materials and engineering Zhengzhou UniversityZhengzhou 450001China

Sodium-ion batteries(SIBs)have rapidly risen to the forefront of energy storage systems as a promising supplementary for Lithium-ion batteries(LIBs).Na_(3)V_(2)(PO_(4))_(2)F_(3)(NVPF)as a common cathode of SIBs,features the merits of high operating voltage,small volume change and favorable specific energy ***,it suffers from poor cycling stability and rate performance induced by its low intrinsic ***,we propose an ingenious strategy targeting superior SIBs through cross-linked NVPF with multi-dimensional nanocarbon frameworks composed of amorphous carbon and carbon nanotubes(NVPF@C@CNTs).This rational design ensures favorable particle size for shortened sodium ion transmission pathway as well as improved electronic transfer network,thus leading to enhanced charge transfer kinetics and superior cycling *** from this unique structure,significantly improved electrochemical properties are obtained,including high specific capacity(126.9 mAh g^(-1)at 1 C,1 C=128 mA g^(-1))and remarkably improved long-term cycling stability with 93.9%capacity retention after 1000 cycles at 20 *** energy density of 286.8 Wh kg^(-1)can be reached for full cells with hard carbon as anode(NVPF@C@CNTs//HC).Additionally,the electrochemical performance of the full cell at high temperature is also investigated(95.3 mAh g^(-1)after 100 cycles at 1 C at 50℃).Such nanoscale dual-carbon networks engineering and thorough discussion of ion diffusion kinetics might make contributions to accelerating the process of phosphate cathodes in SIBs for large-scale energy storages.

关键词： dual-nanocarbon networks full sodium-ion battery ion transfer kinetics Na_(3)V_(2)(PO_(4))_(2)F_(3) NASICON structure

Inetetamab combined with pyrotinib and chemotherapy in the treatment of breast cancer brain metastasis: A case report

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World Journal of Clinical Cases 2024年第3期12卷 575-581页

作者： Qing-Qing dou Ting-Ting Sun Guo-Qiang Wang Wei-Bing Tong Graduate Student Institute Inner Mongolia Medical UniversityHohhot 010000Inner Mongolia Autonomous RegionChina Central Breast Area B Beijing University Cancer Hospital Inner Mongolia HospitalHohhot 010000Inner Mongolia Autonomous RegionChina

BACKGROUND Breast cancer brain metastasis(BCBM)is an advanced breast disease that is difficult to treat and is associated with a high risk of *** prognosis is usually poor,with reduced quality of *** this context,we report the case of a patient with HeR-2-positive BCBM treated with a macromolecular mAb(ine-tetamab)combined with a small molecule tyrosine kinase inhibitor(TKI).CASe SUMMARY The patient was a 58-year-old woman with a 12-year history of type 2 *** was compliant with regular insulin treatment and had good blood glucose *** patient was diagnosed with invasive carcinoma of the right breast(T3N1M0 stage IIIa,HeR2-positive type)through aspiration biopsy of the ipsilateral breast due to the discovery of a breast tumor in February *** showed eR(-),PR(-),HeR-2(3+),and Ki-67(55-60%+).Preoperative neoadjuvant chemotherapy,i.e.,the AC-TH regimen(epirubicin,cyclophosphamide,docetaxel-paclitaxel,and trastuzumab),was administered for 8 *** underwent modified radical mastectomy of the right breast in November 2019 and received tocilizumab targeted therapy for 1 *** metastasis was found 9 mo after *** underwent brain metastasectomy in August *** showed eR(-)and PR.(-),HeR-2(3+),and Ki-67(10-20%+).In November 2020,the patient experienced headache *** an examination,tumor recurrence in the original surgical region of the brain was observed,and the patient was treated with inetetamab,pyrotinib,and ***-brain radiotherapy was *** patient and her family refused radiotherapy for personal *** September 2021,a routine examination revealed that the brain tumor was considerably *** original systemic treatment was continued and combined with intensity-modulated radiation therapy for brain metastases,followed by regular hospitalization and routine *** patient’s condition is generally stable,and she has a relatively high qua

关键词： Breast cancer brain metastasis Resistance to trastuzumab Macromolecule inetetamab Small molecule tyrosine kinase inhibitor Radiation therapy HeR2-positive Case report

A Simple yet effective Framework for Active Learning to Rank

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Machine Intelligence Research 2024年第1期21卷 169-183页

作者： Qingzhong Wang Haifang Li Haoyi Xiong Wen Wang Jiang Bian Yu Lu Shuaiqiang Wang Zhicong Cheng Dejing dou Dawei Yin Baidu Incorporated Beijing 100085China

While China has become the largest online market in the world with approximately 1 billion internet users,Baidu runs the world's largest Chinese search engine serving more than hundreds of millions of daily active users and responding to billions of queries per *** handle the diverse query requests from users at the web-scale,Baidu has made tremendous efforts in understanding users'queries,retrieving relevant content from a pool of trillions of webpages,and ranking the most relevant webpages on the top of the *** the components used in Baidu search,learning to rank(LTR)plays a critical role and we need to timely label an extremely large number of queries together with relevant webpages to train and update the online LTR *** reduce the costs and time con-sumption of query/webpage labelling,we study the problem of active learning to rank(active LTR)that selects unlabeled queries for an-notation and training in this ***,we first investigate the criterion-Ranking entropy(Re)characterizing the entropy of relevant webpages under a query produced by a sequence of online LTR models updated by different checkpoints,using a query-by-com-mittee(QBC)***,we explore a new criterion namely prediction variances(PV)that measures the variance of prediction res-ults for all relevant webpages under a *** empirical studies find that Re may favor low-frequency queries from the pool for la-belling while PV prioritizes high-frequency queries ***,we combine these two complementary criteria as the sample selection strategies for active *** experiments with comparisons to baseline algorithms show that the proposed approach could train LTR models to achieve higher discounted cumulative gain(i.e.,the relative improvement DCG4=1.38%)with the same budgeted labellingefforts.

关键词： Search information retrieval learning to rank active learning query by committee

High-rate electrochemical H_(2)O_(2) production over multimetallic atom catalysts under acidic–neutral conditions

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Carbon energy 2024年第1期6卷 44-62页

作者： Yueyu Tong Jiaxin Liu Bing-Jian Su Jenh-Yih Juang Feng Hou Lichang Yin Shi Xue dou Ji Liang Key Laboratory for Advanced Ceramics and Machining Technology of Ministry of education School of Materials Science and EngineeringTianjin UniversityTianjinChina Institute for Superconducting and electronic Materials University of WollongongInnovation CampusNorth WollongongNew South WalesAustralia Department of electrophysics National Chiao Tung UniversityHsinchuTaiwanChina Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of SciencesShenyangLiaoningChina Institute of energy Materials Science University of Shanghai for Science and TechnologyShanghaiChina

Hydrogen peroxide(H_(2)O_(2))production by the electrochemical 2-electron oxygen reduction reaction(2e−ORR)is a promising alternative to the energy-intensive anthraquinone process,and single-atom electrocatalysts show the unique capability of high selectivity toward 2e−ORR against the 4e−*** extremely low surfa.e density of the single-atom sites and the inflexibility in manipulating their geometric/electronic configurations,however,compromise the H_(2)O_(2) yield and impede further performance ***,we construct a family of multiatom catalysts(MACs),on which two or three single atoms are closely coordinated to form high-density active sites that are versatile in their atomic configurations for optimal adsorption of essential*OOH *** them,the Cox–Ni MAC presents excellent electrocatalytic performance for 2e−ORR,in terms of its exceptionally high H_(2)O_(2) yield in acidic electrolytes(28.96 mol L^(−1) gcat.^(−1) h^(−1))and high selectivity under acidic to neutral conditions in a wide potential region(>80%,0–0.7 V).Operando X-ray absorption and density functional theory analyses jointly unveil its unique trimetallic Co2NiN8 configuration,which efficiently induces an appropriate Ni–d orbital filling and modulates the*OOH adsorption,together boosting the electrocatalytic 2e−ORR *** work thus provides a new MAC strategy for tuning the geometric/electronic structure of active sites for 2e−ORR and other potential electrochemical processes.

关键词： hydrogen peroxide production multiatom catalysts operando X-ray adsorption spectrum reaction mechanism tendency structure-property relation