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Theoretical probe into universal tetrad effect for complexation discrepancy between lanthanide elements and organophosphoric extractant diethyl phosphoric acid

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Journal of Rare Earths 2024年第6期42卷 1142-1148,I0006页

作者： haifeng zheng Yanling Li Xuyi Zhang Jinglu Han Songsong Li Guolong Wu Qingshi Liu Xiaojuan Liu Wuping Liao State Key Laboratory of Rare Earth Resources Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun130022China University of Science and Technology of China Hefei230026China School of Chemistry and Chemical Engineering Nanchang UniversityNanchang330031China Ganjiang Innovation Academy Chinese Academy of SciencesGanzhou341000China

The deep understanding of 4f-correlated electron motion behavior is experimentally limited due to similar physicochemical properties of rare earth elements(REEs).While the solvent extraction behavior originating from the continuous occupation of 4f electrons along the lanthanide family provides a particular platform to probe the 4f electrons motion behavior and its correlations to their versatile functions.Herein,the complexation between REEs and the prototypical extractant of diethyl phosphoric acid(DEP)was substantially studied based on quantum mechanical calculation.The results firstly show that the average bond lengths between Ln and six coordinated oxygen atoms are consistent with lanthanide contraction phenomenon,and gadolinium break effect is also obviously observed.Secondly,the"tetrad effect"is figured out based on the subtle discrepancy of 4f electrons occupation,namely La-Nd,Sm-Eu,Gd-Dy and Ho-Lu.Specifically,the main composition is 4f5d6p for La-Nd,while the discrepancy is due to the increasing electrons in the 5d shell,while it is 4f5d for Pm-Eu.For Gd-Dy,their 4f orbitals accept little electrons and the donating electrons flow into 6s5d subshells due to the half-filled stability and the enhancement of shielding effect.The electrons donate into 5d6p subshells due to multiply electrons occupation of 4f orbitals for Ho-Lu.These detailed analyses obviously clarify the"tetrad effect"along the lanthanide family due to the different variation of 4f orbital occupation.It is expected that these microscopic understandings provide important guidance for the separation of REEs and the design of new extractants.

关键词： Theoretical calculation Rare earths 4f electron Tetrad effect Gadolinium break

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Asymmetric Hydrogenation of Phenanthridines with Chiral Boranes

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Chinese Journal of Chemistry 2024年第6期42卷 631-635页

作者： Guangyu Cui Xiangqing Feng haifeng Du Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Molecular Recognition and FunctionInstitute of ChemistryChinese Academy of SciencesBeijing100190 China University of Chinese Academy of Sciences Beijing100049 China

The asymmetric hydrogenation of N-heteroarenes provides an efficient method for the synthesis of optically active cyclic secondary amines.In this paper,we described an asymmetric hydrogenation of phenanthridines using a chiral mono-alkene-derived borane.A variety of dihydrophenanthridines were furnished in high yields with up to 93%ee.The current catalytic system was very sensitive for the steric hindrance of phenanthridines.Bulky substituents at one phenyl group of phenanthridines were required to obtain the high enantioselectivity.But large substituents on the carbon of the C=N bonds would diminish the reactivity sharply.

关键词： Asymmetric catalysis Hydrogenation Nitrogen heterocycles Phenanthridines Frustrated Lewis pairs Chiral boranes

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Thermal safety boundary of lithium-ion battery at different state of charge

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Journal of Energy Chemistry 2024年第4期91卷 59-72页

作者： Hang Wu Siqi Chen Yan Hong Chengshan Xu Yuejiu zheng Changyong Jin Kaixin Chen Yafei He Xuning Feng Xuezhe Wei haifeng Dai Clean Energy Automotive Engineering Center Tongji UniversityShanghai 201804China College of Mechanical Engineering University of Shanghai for Science and TechnologyShanghai 200093China State Key Laboratory of Automotive Safety and Energy Tsinghua UniversityBeijing 100084China

Thermal runaway(TR)is a critical issue hindering the large-scale application of lithium-ion batteries(LIBs).Understanding the thermal safety behavior of LIBs at the cell and module level under different state of charges(SOCs)has significant implications for reinforcing the thermal safety design of the lithium-ion battery module.This study first investigates the thermal safety boundary(TSB)correspondence at the cells and modules level under the guidance of a newly proposed concept,safe electric quantity boundary(SEQB).A reasonable thermal runaway propagation(TRP)judgment indicator,peak heat transfer power(PHTP),is proposed to predict whether TRP occurs.Moreover,a validated 3D model is used to quantitatively clarify the TSB at different SOCs from the perspective of PHTP,TR trigger temperature,SOC,and the full cycle life.Besides,three different TRP transfer modes are discovered.The interconversion relationship of three different TRP modes is investigated from the perspective of PHTP.This paper explores the TSB of LIBs under different SOCs at both cell and module levels for the first time,which has great significance in guiding the thermal safety design of battery systems.

关键词： Lithium-ion battery Battery safety Thermal runaway State of charge Numerical analysis

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An Empirical Study on Google Research Football Multi-agent Scenarios

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Machine Intelligence Research 2024年第3期21卷 549-570页

作者： Yan Song He Jiang zheng Tian haifeng Zhang Yingping Zhang Jiangcheng Zhu Zonghong Dai Weinan Zhang Jun Wang Institute of Automation Chinese Academy of SciencesBeijing100190China Digital Brain Lab Shanghai200001China ShanghaiTech University Shanghai200001China Huawei Cloud Guiyang550003China Shanghai Jiao Tong University Shanghai200001China University College London LondonWC1E 6PTUK

Few multi-agent reinforcement learning (MARL) researches on Google research football (GRF) focus on the 11-vs-11 multi-agent full-game scenario and to the best of our knowledge, no open benchmark on this scenario has been released to the public. In this work, we fill the gap by providing a population-based MARL training pipeline and hyperparameter settings on multi-agent football scenario that outperforms the bot with difficulty 1.0 from scratch within 2 million steps. Our experiments serve as a reference for the expected performance of independent proximal policy optimization (IPPO), a state-of-the-art multi-agent reinforcement learning algorithm where each agent tries to maximize its own policy independently across various training configurations. Meanwhile, we release our training framework Light-MALib which extends the MALib codebase by distributed and asynchronous implementation with additional analytical tools for football games. Finally, we provide guidance for building strong football AI with population-based training and release diverse pretrained policies for benchmarking. The goal is to provide the community with a head start for whoever experiment their works on GRF and a simple-to-use population-based training framework for further improving their agents through self-play. The implementation is available at https://***/Shanghai-Digital-Brain-Laboratory/DB-Football.

关键词： Multi-agent reinforcement learning(RL) distributed RL system population-based training reward shaping game theory.

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Dynamic tracking of exsolved PdPt alloy/perovskite catalyst for efficient lean methane oxidation

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Chinese Chemical Letters 2024年第4期35卷 170-175页

作者： Yanling Yang Zhenfa Ding Huimin Wang Jianhui Li Yanping zheng Hongquan Guo Li Zhang Bing Yang Qingqing Gu haifeng Xiong Yifei Sun College of Energy Xiamen UniversityXiamen 361005China School of Environment and Civil Engineering Dongguan University of TechnologyDongguan 523808China Department of Chemistry College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) Xiamen 361102China

Supported Pd based catalysts are considered as the efficient candidates for low-carbon alkane oxidation for their outstanding capability to break C-H bond. Whereas, the irreversible deactivation of Pd based catalysts was still frequently observed. Herein, we reinforced the extruded Pd nanoparticles with quantitive Pt to assemble the evenly distributed Pd Pt nanoalloy onto ferrite perovskite(Pd Pt-LCF) matrix with strengthened robustness of metal/oxide support interface. We further co-achieved the enhanced performance, anti-overoxidation as well as resistance of vapor-poisoning in durability measurement. The operando X-ray photoelectron spectroscopy(O-XPS) combined with various morphology characterizations confirms that the accumulation of surface deep-oxidation species of Pd^(4+) is the culprit for fast activity loss in exsolved Pd system, especially at high temperature of 400 ℃. Conversely, it could be completely suppressed by in-situ alloying Pd with equal amount of Pt, which helps maintain the metastable Pd^(2+)/Pd shell and metallic solid-solution core structure. The density function theory(DFT) calculations further buttress that the dissociation of C–H was facilitated on alloy/perovskite interface which is, on the contrary, resistant toward O–H bond cleavage, as compared to Pd/perovskite. Our work suggests that the modification of exsolved metal/oxide catalytic interface could further enrich the toolkit of heterogeneous catalyst design.

关键词： Exsolution PdPt alloy Operando characterization Methane conversion Deep-oxidation

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Dual metal ions/BNQDs boost PMS activation over copper tungstate photocatalyst for antibiotic removal:Intermediate,toxicity assessment and mechanism

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Journal of Materials Science & Technology 2024年第3期170卷 11-24页

作者： Ruyao Chen Haiyue Zhang Yuming Dong haifeng Shi School of Science Jiangnan UniversityWuxi214122China The Key Laboratory of Synthetic and Biological Colloids Ministry of EducationJiangnan UniversityWuxi214122China National Laboratory of Solid State Microstructures Nanjing UniversityNanjing210093China

In the metal-based peroxymonosulfate(PMS)activation process,the sluggish surface redox cycle of metal ions generally hampered the efficiency of PMS activation for pollutant removal.Herein,Codoped CuWO 4/BN quantum dots(CW/Co/BNQDs)photocatalysts were developed to realize Cu^(2+)/Cu+and Co^(2+)/Co^(3+)dual ions redox cycles for PMS activation,which would facilitate the tetracycline(TC)removal.CW/4Co/2BNQDs could degrade 94.8%TC within 30 min in PMS/Vis system,and the apparent rate constant of CW/4Co/2BNQDs was 2.7 times and 1.2 times higher than those of CW and CW/4Co,respectively.The improved TC degradation performance could be attributed to the synergetic effect between BNQDs and dual redox cycles.X-ray photoelectron spectroscopy(XPS)spectra of samples before and after the reaction demonstrated that BNQDs were beneficial for accelerating the Cu^(2+)/Cu+and Co^(2+)/Co^(3+)redox cycles in CW/4Co/2BNQDs,further boosting the activation of PMS in TC degradation.Experiments of different radical scavengers revealed that the SO_(4)^(·−)/·OH/h+/^(1)O_(2)reactive species participated in the PMS activation for the TC degradation process.The possible TC degradation pathway and intermediate toxicity were detailed investigated.In addition,CW/4Co/2BNQDs exhibited outstanding photocatalytic activity over five consecutive cycles,which illustrated that it was supposed to be a reliable PMS activator over antibiotic elimination for practical application.And this work shed new light on constructing dual redox cycles for efficient PMS activation.

关键词： Dual redox cycles Photocatalysis Peroxymonosulfate BN quantum dots Toxicity assessment

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An Environment‑Tolerant Ion‑Conducting Double‑Network Composite Hydrogel for High‑Performance Flexible Electronic Devices

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Nano-Micro Letters 2024年第5期16卷 352-369页

作者： Wenchao Zhao haifeng Zhou Wenkang Li Manlin Chen Min Zhou Long Zhao State Key Laboratory of Advanced Electromagnetic Technology School of Electrical and Electronic EngineeringHuazhong University of Science and TechnologyWuhan 430074People’s Republic of China School of Chemistry and Chemical Engineering Huazhong University of Science and TechnologyWuhan 430074People’s Republic of China

High-performance ion-conducting hydrogels(ICHs)are vital for developing flexible electronic devices.However,the robustness and ion-conducting behavior of ICHs deteriorate at extreme tempera-tures,hampering their use in soft electronics.To resolve these issues,a method involving freeze–thawing and ionizing radiation technology is reported herein for synthesizing a novel double-network(DN)ICH based on a poly(ionic liquid)/MXene/poly(vinyl alcohol)(PMP DN ICH)system.The well-designed ICH exhibits outstanding ionic conductivity(63.89 mS cm^(-1) at 25℃),excellent temperature resistance(-60–80℃),prolonged stability(30 d at ambient temperature),high oxidation resist-ance,remarkable antibacterial activity,decent mechanical performance,and adhesion.Additionally,the ICH performs effectively in a flexible wireless strain sensor,thermal sensor,all-solid-state supercapacitor,and single-electrode triboelectric nanogenerator,thereby highlighting its viability in constructing soft electronic devices.The highly integrated gel structure endows these flexible electronic devices with stable,reliable signal output performance.In particular,the all-solid-state supercapacitor containing the PMP DN ICH electrolyte exhibits a high areal specific capacitance of 253.38 mF cm^(-2)(current density,1 mA cm^(-2))and excellent environmental adaptability.This study paves the way for the design and fabrication of high-performance mul-tifunctional/flexible ICHs for wearable sensing,energy-storage,and energy-harvesting applications.

关键词： Ionic liquids Double-network hydrogels Temperature tolerance Multifunctionality Flexible electronic devices

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Reducing idleness in financial cloud services via multi-objective evolutionary reinforcement learning based load balancer

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Science China(Information Sciences) 2024年第2期67卷 20-40页

作者： Peng YANG Laoming ZHANG haifeng LIU Guiying LI Department of Statistics and Data Science Southern University of Science and Technology Guangdong Provincial Key Laboratory of Brain-Inspired Intelligent Computation Department of Computer Science and EngineeringSouthern University of Science and Technology Academy for Advanced Interdisciplinary Studies Southern University of Science and Technology Guangdong OPPO Mobile Telecommunications Corp. Ltd Research Institute of Trustworthy Autonomous Systems Southern University of Science and Technology

In recent years, various companies have started to shift their data services from traditional data centers to the cloud. One of the major motivations is to save on operational costs with the aid of cloud elasticity. This paper discusses an emerging need from financial services to reduce the incidence of idle servers retaining very few user connections, without disconnecting them from the server side. This paper considers this need as a bi-objective online load balancing problem. A neural network based scalable policy is designed to route user requests to varied numbers of servers for the required elasticity. An evolutionary multi-objective training framework is proposed to optimize the weights of the policy. Not only is the new objective of idleness reduced by over 130% more than traditional industrial solutions, but the original load balancing objective itself is also slightly improved. Extensive simulations with both synthetic and real-world data help reveal the detailed applicability of the proposed method to the emergent problem of reducing idleness in financial services.

关键词： evolutionary reinforcement learning evolutionary multi-objective optimization load balance cloud computing

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Asymmetric Partial Hydrosilylation of 2,2-Difluoro-1,3-diketones with Chiral Frustrated Lewis Pairs

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Chinese Journal of Chemistry 2024年第8期42卷 853-857页

作者： Ting Liu Xiangqing Feng haifeng Du Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Molecular Recognition and FunctionInstitute of ChemistryChinese Academy of SciencesBeijing100190 China University of Chinese Academy of Sciences Beijing100049 China

Comprehensive Summary,The asymmetric partial reduction of 1,3-diketones stands as a straightforward pathway to access optically active β-hydroxyketones. In this paper, an asymmetric Piers-type hydrosilylation of 2,2-difluoro-1,3-diketones was successfully realized by using a frustrated Lewis pair of chiral borane and tricyclohexylphosphine as a catalyst, delivering a variety of α,α-difluoro-β-hydroxyketones in high yields with up to 99% ee. Significantly, no over-reduced diol products were observed even with an excess amount of silanes. The product can be conveniently converted to α,α-difluoro-β-hydroxyester or 1,3-anti-diol via an oxidation with m-CPBA or a reduction with DIBAL-H without obvious loss of ee.

关键词： Asymmetric catalysis Hydrosilylation Ketones Frustrated Lewis pairs Chiral boranes

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Cooperative Caching for Scalable Video Coding Using Value-Decomposed Dimensional Networks

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China Communications 2022年第9期19卷 146-161页

作者： Youjia Chen Yuekai Cai haifeng zheng Jinsong Hu Jun Li Fujian Key Lab for Intelligent Processing and Wireless Transmission of Media Information College of Physics and Information EngineeringFuzhou UniversityFuzhou 350000China School of Electronic and Optical Engineering Nanjing University of Science and TechnologyNanjing 210000China

Scalable video coding(SVC)has been widely used in video-on-demand(VOD)service,to efficiently satisfy users’different video quality requirements and dynamically adjust video stream to timevariant wireless channels.Under the 5G network structure,we consider a cooperative caching scheme inside each cluster with SVC to economically utilize the limited caching storage.A novel multi-agent deep reinforcement learning(MADRL)framework is proposed to jointly optimize the video access delay and users’satisfaction,where an aggregation node is introduced helping individual agents to achieve global observations and overall system rewards.Moreover,to cope with the large action space caused by the large number of videos and users,a dimension decomposition method is embedded into the neural network in each agent,which greatly reduce the computational complexity and memory cost of the reinforcement learning.Experimental results show that:1)the proposed value-decomposed dimensional network(VDDN)algorithm achieves an obvious performance gain versus the traditional MADRL;2)the proposed VDDN algorithm can handle an extremely large action space and quickly converge with a low computational complexity.

关键词： cooperative caching multi-agent deep reinforcement learning scalable video coding value-decomposition network

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