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Free radicals trigger the closure of open pores in lignin-derived hard carbons toward improved sodium-storage capacity

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Journal of Energy Chemistry 2024年第7期94卷 551-559页

作者： Wen-Jun Ji Zong-Lin Yi Ming-Xin Song Xiao-Qian Guo Yi-Lin Wang Yi-Xuan Mao fang-Yuan Su Jing-Peng Chen xian-xian Wei Li-Jing Xie Cheng-Meng Chen CAS Key Laboratory of Carbon Materials Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001ShanxiChina University of Chinese Academy of Sciences Beijing 100049China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China School of Environment and Safety Taiyuan University of Science and TechnologyTaiyuan 030001ShanxiChina

The chemical activation of various precursors is effective for creating additional closed pores in hard carbons for sodium ***,the formation mechanism of closed pores under the influence of pore-forming agents is not well ***,an effective chemical activation followed by a high-temperature self-healing strategy is employed to generate interconnected closed pores in lignin-derived hard carbon(HCs).By systematic experimental design combined with electron paramagnetic res-onance spectroscopy,it can be found that the content of free radicals in the carbon matrix influences the closure of open pores at high *** high activation temperature(>700 C)leads to a low free radical concentration,making it difficult to achieve self-healing of open pores at high *** activation at 700°C,a balance between pore making and self-healing is achieved in the final hard carbon.A large number of free radicals triggers rapid growth and aggregation of carbon microcrys-tals,blocking pre-formed open micropores and creating additional interconnected closed pores in as-obtained hard *** a result,the optimized carbon anode(LK-700-1300)delivers a high reversible capacity of 330.8 mA h g^(-1) at 0.03 A g^(-1),which is an increase of 86 mA h g^(-1) compared to the pristine lignin-derived carbon anode(L-700-1300),and exhibits a good rate performance(202.1 mA h g^(-1) at 1 A g^(-1)).This work provides a universal and effective guidance for tuning closed pores of hard carbons from otherprecursors.

关键词： Hard carbon Chemical activation Free radical Self-healing Closed pores Sodium ion batteries

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Strong electron correlation-induced Mott-insulating electrides of Ae_(5)X_(3)(Ae=Ca,Sr,and Ba;X=As and Sb)

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Matter and Radiation at Extremes 2024年第3期9卷 74-82页

作者： Ya Xu Lu Zheng Yunkun zhang Zhuangfei zhang QianQian Wang Yuewen zhang Liangchao Chen Chao fang Biao Wan Huiyang Gou Key Laboratory of Material Physics of Ministry of Education School of Physics and Laboratory of Zhongyuan LightZhengzhou UniversityZhengzhou 450052China School of Mechanical and Equipment Engineering Hebei University of EngineeringHandan 056038China Center for High Pressure Science and Technology Advanced Research Beijing 100094China

The presence of interstitial electrons in electrides endows them with interesting attributes,such as low work function,high carrier concentration,and unique magnetic *** knowledge and understanding of electrides are thus of both scientific and technological ***,we employ first-principles calculations to investigate Mott-insulating Ae_(5)X_(3)(Ae=Ca,Sr,and Ba;X=As and Sb)electrides with Mn_(5)Si_(3)-type structure,in which half-filled interstitial electrons serve as ions and are *** Mott-insulating property is induced by strong electron correlation between the nearest interstitial electrons,resulting in spin splitting and a separation between occupied and unoccupied *** half-filled antiferromagnetic configuration and localization of the interstitial electrons are critical for the Mott-insulating properties of these *** with that in intermetallic electrides,the orbital hybridization between the half-filled interstitial electrons and the surrounding atoms is weak,leading to highly localized magnetic centers and pronounced correlation ***,the Mott-insulating electrides Ae_(5)X_(3)have very large indirect bandgaps(0.30 eV).In addition,high pressure is found to strengthen the strong correlation effects and enlarge the *** present results provide a deeper understanding of the formation mechanism of Mott-insulating electrides and provide guidance for the search for new strongly correlated electrides.

关键词： intermetallic filled occupied

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AdaPIP: Adaptive picture-in-picture guidance for 360 ◦ film watching

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Computational Visual Media 2024年第3期10卷 487-503页

作者： Yi-Xiao Li Guan Luo Yi-Ke Xu Yu He fang-Lue zhang Song-Hai zhang Department of Computer Science and Technology Tsinghua UniversityBeijingChinaand Beijing National Research Center for Information Science and Technology(BNRist)Tsinghua UniversityBeijingChina Key Laboratory of Space Utilization Technology and Engineering Center for Space UtilizationChinese Academy of SciencesBeijingChina Victoria University of Wellington WellingtonNew Zealand

360◦videos enable viewers to watch freely from different directions but inevitably prevent them from perceiving all the helpful *** mitigate this problem,picture-in-picture(PIP)guidance was proposed using preview windows to show regions of interest(ROIs)outside the current view *** identify several drawbacks of this representation and propose a new method for 360◦ﬁlm watching called *** enhances traditional PIP by adaptively arranging preview windows with changeable view ranges and *** addition,AdaPIP incorporates the advantage of arrow-based guidance by presenting circular windows with arrows attached to them to help users locate the corresponding ROIs more *** also adapted AdaPIP and Outside-In to HMD-based immersive virtual reality environments to demonstrate the usability of PIP-guided approaches beyond 2D *** user experiments on 2D screens,as well as in VR environments,indicate that AdaPIP is superior to alternative methods in terms of visual experiences while maintaining a comparable degree of immersion.

关键词： 360◦videos picture-in-picture(PIP) virtual reality(VR) visual guidance

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Experimental Study on Mixed-Mode(Ⅰ–Ⅱ)Fracture Toughness of Freshwater Ice

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Acta Mechanica Solida Sinica 2024年第2期37卷 252-264页

作者： Yaozhong Xu Mao Zhou xian Yi Wen Hua Jiuzhou Huang Wenyu zhang Shiming Dong Key Laboratory of Deep Underground Science and Engineering Ministry of EducationCollege of Architecture and EnvironmentSichuan UniversityChengdu610065China Failure Mechanics and Engineering Disaster Prevention Key Laboratory of Sichuan Province Sichuan UniversityChengdu610065China China Aerodynamics Research and Development Center/Low Speed Aerodynamics Research Institute Mianyang621000China College of Mechanical and Electrical Engineering Xichang UniversityXichang615000China

In recent years,the issue of aircraft icing has gained widespread *** breaking and detachment of dynamic ice can pose a threat to flight ***,the shedding and fracture mechanisms of dynamic ice are unclear and cannot meet the engineering needs of ice-shedding hazard ***,studying the fracture toughness of ice bodies has extremely important practical *** address this issue,this article uses a centrally cracked Brazilian disk(CCBD)specimen to measure the pure modeⅠtoughness and pure modeⅡfracture toughness of freshwater ice at different loading *** mixed-mode(Ⅰ–Ⅱ)fracture characteristics of ice are discussed,and the experimental results are compared and analyzed with the theoretical values of the generalized maximum tangential stress(GMTS)criterion considering the influence of *** results indicated that as the loading rate increases,the pure modeⅠtoughness and pure modeⅡfracture toughness of freshwater ice decrease,and the fracture toughness of freshwater ice is more sensitive to the loading rate.Ⅰn terms of fracture criteria,the theoretical value of the ratio of pure modeⅡfracture toughness to pure modeⅠfracture toughness based on the GMTS criterion is in good agreement with the experimental value,while the theoretical value based on the maximum tangential stress(MTS)criterion deviates significantly from the experimental value,indicating that the GMTS criterion considering the influence of T-stress can better predict the experimental results.

关键词： Freshwater ice Fracture criteria Centrally cracked Brazilian disk(CCBD) Mixed-mode(Ⅰ-Ⅱ) Loading rate

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Syntheses and properties of associative acrylamide copolymers containing short hydrophobic chains used in a friction reducer for slick-water fracturing

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Petroleum Science 2024年第3期21卷 1889-1901页

作者： Ya-Xing Dai xian-Li zhang Si-Yuan Liu Feng-Run-Ze zhang Yi-Xi zhang Yu-Tong Sang Jing-Xi Zheng Zhao-Sheng Liu Peng zhang College of Chemistry and Chemical Engineering Chongqing University of Science and TechnologyChongqing401331China College of Ecology and Environment Chongqing Resources and Environmental Protection of UniversityChongqing401331China China China Property Project Department of Dezhou Mining Property Service CenterShengli Oilfield Company of SinopecDezhou253000ShandongChina

Two allyldimethylalkyl quaternary ammonium salt(AQAS)monomers,N,N-dimethylallylphenylpropylammonium bromide(AQAS1)and N,N-dimethylallylnonylammonium bromide(AQAS2),were synthesized and used to prepare modified polyacrylamide *** new drag reducers were synthesized from acrylamide(AM),sodium acrylate(Na AA)and a cationic modified monomer(AQAS1 or AQAS2)via aqueous solution polymerization,and the copolymers were named P(AM/Na AA/AQAS1)and P(AM/Na AA/AQAS2),*** structures of the drag reduction agents were confirmed by IR and1H NMR *** molecular weight(Mw)of P(AM/Na AA/AQAS1)was 1.79×10^(6)g/*** the copolymer concentration was 1000 mg/L and the flow rate was 45 L/min,in fresh water the highest drag reduction rate was 75.8%,in 10,000 mg/L Na Cl solution the drag reduction rate decreased to 72.9%.The molecular weight of P(AM/Na AA/AQAS2)was 3.17×10^(6)g/*** the copolymer concentration was500 mg/L and the flow rate was 45 L/min,the drag reduction rate reached 75.2%,and in 10,000 mg/L Na Cl solution the drag reduction rate was 73.3%,decreased by approximately 1.9%.The drag reduction rate for partially hydrolyzed polyacrylamide(HPAM)was also investigated,and the results showed that the drag reduction rates for 500 and 1000 mg/L HPAM solutions were merely 43.2%and 49.0%in brine,*** with HPAM,both of the above copolymers presented better drag reduction capacities.

关键词： Shale gas Slick water Drag reducer Modified monomer Copolymerization

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A comparison of statistical learning of naturalistic textures between DCNNs and the human visual hierarchy

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Science China Technological Sciences 2024年第8期67卷 2310-2318页

作者： LU XinCheng YUAN ZiQi zhang YiChi AI HaiLin CHENG SiYuan GE YiRan fang fang CHEN NiHong Department of Psychological and Cognitive Sciences Tsinghua University Department of Computer Science and Technology Tsinghua University School of Psychological and Cognitive Sciences and Beijing Key Laboratory of Behavior and Mental Health Peking University Key Laboratory of Machine Perception (Ministry of Education) Peking University Peking-Tsinghua Center for Life Sciences Peking University IDG/McGovern Institute for Brain Research Peking University State Key Laboratory of Brain and Cognitive Science Institute of Psychology Chinese Academy of Sciences IDG/McGovern Institute for Brain Research Tsinghua University

The visual system continuously adapts to the statistical properties of the environment. Existing evidence shows a close resemblance between deep convolutional neural networks(CNNs) and primate visual stream in neural selectivity to naturalistic textures above the primary visual processing stage. This study delves into the mechanisms of perceptual learning in CNNs,focusing on how they assimilate the high-order statistics of natural textures. Our results show that a CNN model achieves a similar performance improvement as humans, as manifested in the learning pattern across different types of high-order image statistics. While L2 was the first stage exhibiting texture selectivity, we found that stages beyond L2 were critically involved in learning. The significant contribution of L4 to learning was manifested both in the modulations of texture-selective responses and in the consequences of training with frozen connection weights. Our findings highlight learning-dependent plasticity in the mid-to-high-level areas of the visual hierarchy. This research introduces an AI-inspired approach for studying learning-induced cortical plasticity, utilizing DCNNs as an experimental framework to formulate testable predictions for empirical brain studies.

关键词： CNN perceptual learning naturalistic texture psychophysics

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Training Generative Adversarial Networks with Adaptive Composite Gradient

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Data Intelligence 2024年第1期6卷 120-157页

作者： Huiqing Qi fang Li Shengli Tan xiangyun zhang School of Mathematical Sciences East China Normal UniversityShanghai 200241China

The wide applications of Generative adversarial networks benefit from the successful training methods,guaranteeing that an object function converges to the local ***,designing an efficient and competitive training method is still a challenging task due to the cyclic behaviors of some gradient-based ways and the expensive computational cost of acquiring the Hessian *** address this problem,we proposed the Adaptive Composite Gradients(ACG)method,linearly convergent in bilinear games under suitable *** analysis and toy-function experiments both suggest that our approach alleviates the cyclic behaviors and converges faster than recently proposed SOTA *** convergence speed of the ACG is improved by 33%than other *** ACG method is a novel Semi-Gradient-Free algorithm that can reduce the computational cost of gradient and Hessian by utilizing the predictive information in future *** mixture of Gaussians experiments and real-world digital image generative experiments show that our ACG method outperforms several existing technologies,illustrating the superiority and efficacy of our method.

关键词： Generative adversarial networks adaptive composite gradient semi-gradient free game theory bilinear game

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Synergy enhancement of Co single atoms and asymmetric subnanoclusters for Fenton-like activation

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Nano Research 2024年第9期17卷 7935-7944页

作者： Ming Ma Zhiyi Sun Ziwei Deng xiang Li fang zhang Wenxing Chen School of Materials Key Laboratory of Cluster Science Ministry of EducationBeijing Key Laboratory of Photoelectronic/Electrophotonic Conversion MaterialsAdvanced Technologies Research Institute(Jinan)Advanced Research Institute of Multidisciplinary ScienceSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081China Energy and Catalysis Center School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China Analysis and Testing Center Beijing Institute of TechnologyBeijing Institute of TechnologyBeijing 100081China

As a new water treatment technology,Fenton-like reaction has great *** this study,we successfully prepared an excellent Fenton-like catalyst,which is composed of cobalt monoatoms and asymmetric subnanoclusters(labeled CoSA/Clu-C_(2)N),and exhibits excellent peroxymonosulfate(PMS)activation *** directly comparing the catalytic properties of CoSA-C_(2)N and CoSA/Clu-C_(2)N,the synergistic effects of coasymmetric Co subclusters and Co atoms on the activation of PMS and degradation of organic micropollutants were *** results showed that CoSA/Clu-C_(2)N had higher degradation rates of carbamazepine(CBZ),antipyrine(AT)and chlorobenzoic acid(CA)when combined with active oxidant *** cyclic frequency of CBZ was 5.4 min^(-1),which was twice as high as the catalytic constant of CoSA-C_(2)N(2.4 min^(-1)).The results show that CoSA/Clu-C_(2)N cobalt subnanoclusters and cobalt single atom can synergistically improve the catalytic performance of activated PMS oxidation of micropollutants in *** addition,electron paramagnetic resonance(EPR)technology has proved that the introduction of Co subnano clusters in CoSA/Clu-C_(2)N is conducive to the production of singlet oxygen(1O2),thereby improving the efficiency of pollutant *** work lays a solid foundation for the future design of advanced multifunctional catalysts by carefully regulating and combining monmetallic atoms and metal subnanoclusters.

关键词： carbamazepine Fenton-like reaction Co single atoms asymmetrical sub-nanoclusters peroxymonosulfate synergy enhancement

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Highly Hydrolysis-Resistant Polyimide Fibers Prepared by Thermal Crosslinking with Inherent Carboxyl Groups

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Chinese Journal of Polymer Science 2024年第2期42卷 247-255,I0010页

作者： Can-Can zhang Jun-Long Yang Ya-Jiang Huang Guang-xian Li College of Polymer Science and Engineering State Key Laboratory of Polymer Materials Engineering of ChinaSichuan UniversityChengdu610065China

Easy hydrolysis in alkaline environments limits the use of polyimide fibers in environmental protection. The hydrolysis resistance levels of polyimide fibers can be improved by crosslinking of the macromolecular chains. In this work, crosslinked polyimide fibers(CPI fibers) were produced by intrinsic carboxyl decarboxylation for the first time. The thermal stability of the polyimide fibers containing the intrinsic carboxyl groups(PIC fibers) was studied, and the temperature of the decarboxylation-crosslinking reaction was determined to be 450 ℃. The PIC fibers were hotdrawn to initiate thermal crosslinking of the carboxyl groups and molecular chain orientation at high temperature. The CPI fibers had high tensile strengths(0.72-1.46 GPa) and compressive strengths(401-604 MPa). The oriented macromolecules and chemically crosslinked structure improved the tightness of the molecular chains and endowed the CPI fibers with excellent hydrolytic resistance. The CPI-50 fiber did not dissolve in a 0.5 wt% NaOH solution during heating at 90 ℃ for 10 h, and the tensile strength retention reached 87% when treated in 0.5 wt% NaOH solutions at 90 ℃ for 1 h, providing a guarantee for its application in alkaline corrosive environments.

关键词： Polyimide Carboxyl group Crosslinking Hydrolysis-resistance

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Highly efficient catalyst for 1,1,2-trichloroethane dehydrochlorination via BN_(3) frustrated Lewis acid-base pairs

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Nano Research 2024年第6期17卷 4773-4781页

作者： Yuxue Yue fangmin Zuo Bolin Wang Xiaoling xian Jun Tang Haifeng zhang Zilong zhang Qingping Ke Wei Chen School of Chemical Engineering Northeast Electric Power UniversityJilin 132012China Industrial Catalysis Institute of Zhejiang University of Technology Hangzhou 310014China Key Laboratory of Carbon Materials of Zhejiang Province College of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325035China College of Chemistry and Chemical Engineering Anhui University of TechnologyMaanshan 243002China

In this study,a novel non-metallic carbon-based catalyst co-doped with boron and nitrogen(B,N)was successfully *** precisely controlling the carbonization temperature of a binary mixed ionic liquid,we selectively modified the doping site structure,ultimately constructing a B,N co-doped frustrated Lewis acid-base pair *** catalyst exhibited remarkable catalytic activity,selectivity,and stability in the dehydrochlorination reaction of 1,1,2-trichloroethane(TCE).Detailed characterization and theoretical calculations revealed that the primary active center of this catalyst was the BN_(3)*** to conventional graphitic N structures,the BN_(3)structure had a higher p-band center,ensuring superior adsorption and activation capabilities for TCE during the *** the BN_(3)site,three negatively charged nitrogen atoms acted as Lewis bases,while positively charged boron atoms acted as Lewis *** synergistic interaction facilitated the specific dissociation of chlorine and hydrogen atoms from TCE,significantly enhancing the 1,1-dichloroethene *** this research,we not only explored the active site structure and catalytic mechanism of B,N co-doped catalysts in depth but also provided an efficient,selective,and stable catalyst for the dehydrochlorination of TCE,contributing significantly to the development of non-metallic catalysts.

关键词： B N co-doped sites dehydrochlorination frustrated Lewis acid-base pairs catalytic mechanism

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