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Unraveling high efficiency multi-step sodium storage and bidirectional redox kinetics synergy mechanism of cobalt-doping vanadium disulfide anode

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Journal of Energy Chemistry 2024年第7期94卷 148-157页

作者： Enzhi Li Mingshan Wang yuanlong Feng Lin Yang Qian Li Zhenliang Yang Junchen Chen Bo yu Bingshu Guo Zhiyuan Ma yun Huang Jiangtao Liu Xing Li School of New Energy and Materials Southwest Petroleum UniversityChengdu 610500SichuanChina Institute of Materials China Academy of Engineering PhysicsMianyang 621908SichuanChina State Key Laboratory of Advanced Chemical Power Sources Guizhou Meiling Power Sources Co.Ltd.Zunyi 563003GuizhouChina school of Chemistry and Chemical Engineering Harbin Institute of TechnologyHarbin 150001HeilongjiangChina

Sodium-based storage devices based on conversion-type metal sulfide anodes have attracted great atten-tion due to their multivalent ion redox reaction ability.However,they also suffer from sodium polysul-fides(NaPSs)shuttling problems during the sluggish Na^(+)redox process,leading to"voltage failure"and rapid capacity decay.Herein,a metal cobalt-doping vanadium disulfide(Co-vS_(2))is proposed to simulta-neously accelerate the electrochemical reaction of vS_(2) and enhance the bidirectional redox of soluble NaPSs.It is found that the strong adsorption of NaPSs by V-Co alloy nanoparticles formed in situ during the conversion reaction of Co-VS_(2) can effectively inhibit the dissolution and shuttle of NaPSs,and ther-modynamically reduce the formation energy barrier of the reaction path to effectively drive the complete conversion reaction,while the metal transition of Co elements enhances reconversion kinetics to achieve high reversibility.Moreover,Co-VS_(2) also produce abundant sulfur vacancies and unsaturated sulfur edge defects,significantly improve ionic/electron diffusion kinetics.Therefore,the Co-VS_(2) anode exhibits ultrahigh rate capability(562 mA h g^(-1) at 5 A g^(-1)),high initial coulombic efficiency(~90%)and 12,000 ultralong cycle life with capacity retention of 90%in sodium-ion batteries(SIBs),as well as impressive energy/power density(118 Wh kg^(-1)/31,250 W kg^(-1))and over 10.000 stable cycles in sodium-ion hybrid capacitors(SIHCs).Moreover,the pouch cell-type SIHC displays a high-energy density of 102 Wh kg^(-1) and exceed 600 stable cycles.This work deepens the understanding of the electrochem-ical reaction mechanism of conversion-type metal sulfide anodes and provides a valuable solution to the shuttlingofNaPSs inSIBsandSIHCs.

关键词： Sodium-ionbatteries Sodium-ion hybrid capacitors Pouch cells Vanadium disulfide Shuttle effect

Skill Learning for Human-Robot Interaction Using Wearable Device

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Tsinghua Science and Technology 2019年第6期24卷 654-662页

作者： Bin Fang Xiang Wei Fuchun Sun Haiming Huang yuanlong yu Huaping Liu Department of Computer Science and Technology Tsinghua UniversityBeijing 100084China Fuzhou University Fuzhou 350108 China College of Information Engineering Shenzhen UniversityShenzhen 518060China

With the accelerated aging of the global population and escalating labor costs, more service robots are needed to help people perform complex tasks. As such, human-robot interaction is a particularly important research topic. To effectively transfer human behavior skills to a robot, in this study, we conveyed skill-learning functions via our proposed wearable device. The robotic teleoperation system utilizes interactive demonstration via the wearable device by directly controlling the speed of the motors. We present a rotation-invariant dynamicalmovement-primitive method for learning interaction skills. We also conducted robotic teleoperation demonstrations and designed imitation learning experiments. The experimental human-robot interaction results confirm the effectiveness of the proposed method.

关键词： skill learning interaction teleoperation dynamical movement primitive

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量子系统辨识与参数估计

中国科学：数学 2024年第5期54卷 785-822页

作者：王元龙肖水鑫余其董道毅中国科学院数学与系统科学研究院北京100190 School of Engineering Australian National UniversityCanberraACT 2601Australia Centre for Quantum Dynamics Griffith UniversityBrisbaneQLD 411lAustralia

量子信息的飞速发展对人们调控量子系统的能力提出了更高的要求,而对量子系统进行辨识与参数估计是进行量子控制的基本且重要的环节.本文综述量子系统辨识和参数估计这一方向,侧重于量子度量学、量子层析、量子滤波和量子噪声谱学4个分... 详细信息

量子信息的飞速发展对人们调控量子系统的能力提出了更高的要求,而对量子系统进行辨识与参数估计是进行量子控制的基本且重要的环节.本文综述量子系统辨识和参数估计这一方向,侧重于量子度量学、量子层析、量子滤波和量子噪声谱学4个分支,介绍其问题建模、分析工具、求解方法及不同的应用等.

关键词：量子系统量子度量学量子层析量子滤波量子噪声谱学

New Record Ocean Temperatures and Related Climate Indicators in 2023

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Advances in Atmospheric Sciences 2024年第6期41卷 1068-1082页

作者： Lijing CHENG John ABRAHAM Kevin E.TRENBERTH Tim BOYER Michael EMANN Jiang ZHU Fan WANG Fujiang yu Ricardo LOCARNINI John FASULLO Fei ZHENG yuanlong LI Bin ZHANG Liying WAN Xingrong CHEN Dakui WANG Licheng FENG Xiangzhou SONG yulong LIU Franco RESEGHETTI Simona SIMONCELLI Viktor GOURETSKI Gengxin CHEN Alexey MISHONOV Jim REAGAN Karina VON SCHUCKMANN yuying PAN Zhetao TAN yujing ZHU Wangxu WEI Guancheng LI Qiuping REN Lijuan CAO Yayang LU International Center for Climate and Environment Sciences Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China University of St.Thomas School of EngineeringMinnesota 55105USA NSF National Center for Atmospheric Research BoulderColorado 80307USA University of Auckland Auckland 1010New Zealand National Oceanic and Atmospheric Administration National Centers for Environmental InformationSilver SpringMaryland 20910USA Department of Earth and Environmental Science University of PennsylvaniaPhiladelphiaPennsylvania 19104USA Institute of Oceanology Chinese Academy of SciencesQingdao 266071China National Marine Environmental Forecasting Center Ministry of Natural Resources of ChinaBeijing 100081China Oceanographic Data Center Chinese Academy of SciencesQingdao 266071China College of Oceanography Hohai UniversityNanjing 210098China National Marine Data and Information Service Tianjin 300171China Italian National Agency for New Technologies Energy and Sustainable Economic DevelopmentS.Teresa Research CenterLerici 19032Italy Istituto Nazionale di Geofisica e Vulcanologia Sede di BolognaBologna 40128Italy South China Sea Institute of Oceanology Chinese Academy of SciencesGuangzhou 510301China ESSIC/CISESS-MD University of MarylandCollege ParkMD20740USA Mercator Ocean International Toulouse 31400France Eco-Environmental Monitoring and Research Center Pearl River Valley and South China Sea Ecology and Environment AdministrationMinistry of Ecology and EnvironmentPRCGuangzhou 510611China National Meteorological Information Center China Meteorological AdministrationBeijing 100081China International Research Center of Big Data for Sustainable Development Goals Beijing 100094China

The global physical and biogeochemical environment has been substantially altered in response to increased atmospheric greenhouse gases from human activities.In 2023,the sea surface temperature(SST)and upper 2000 m ocean heat content(OHC)reached record highs.The 0–2000 m OHC in 2023 exceeded that of 2022 by 15±10 ZJ(1 Zetta Joules=1021 Joules)(updated IAP/CAS data);9±5 ZJ(NCEI/NOAA data).The Tropical Atlantic Ocean,the Mediterranean Sea,and southern oceans recorded their highest OHC observed since the 1950s.Associated with the onset of a strong El Niño,the global SST reached its record high in 2023 with an annual mean of~0.23℃ higher than 2022 and an astounding>0.3℃ above 2022 values for the second half of 2023.The density stratification and spatial temperature inhomogeneity indexes reached their highest values in 2023.

关键词： ocean heat content salinity stratification global warming climate

Lateral-profile planning:Three-dimensional-profile-based optimal trajectory generation

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Science China(Technological Sciences) 2022年第12期65卷 3057-3068页

作者： ZHANG yuanlong XIE yu BAO WeiMin College of Intelligence Science and Technology National University of Defense TechnologyChangsha 410073China Science and Technology Committee of China Aerospace Science and Technology Corporation Beijing 100048China

The conventional re-entry guidance method considerably limits the maneuverability of hypersonic glide vehicles under pre-given angle-of-attack profiles.To address this issue,based on a previous three-dimensional(3D)profile guidance method,we propose a lateral-profile-first 3D profile optimization design strategy to solve the trajectory generation problem under complex conditions involving multiple constraints.Unlike the traditional method,which prioritizes the design of the longitudinal drag acceleration profiles,our method first converted the re-entry flight constraints into a lateral flight corridor,generated the initial lateral profile via parameterization,and solved the 3D profile using the coupling relationship between the longitudinal and lateral motions.The design of the 3D profile requires simultaneous consideration of waypoints,no-fly zones,and altitude profiles;hence,a new 3D profile optimization design model was constructed,and a customized sequential quadratic programming algorithm was employed to solve it.The advantages of the proposed method were demonstrated based on landing footprint results obtained using the lateral profile-first strategy.Finally,simulation results based on the common aero vehicle-high-performance model verified the feasibility and effectiveness of the strategy.

关键词： hypersonic glide vehicle three-dimensional profile lateral profile-first planning optimal trajectory footprint

准噶尔盆地玛湖凹陷含油储集岩连续抽提组分地球化学特征与油源对比

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地球化学 2024年第3期53卷 351-369页

作者：张仲达谷元龙靳军李二庭于双潘长春中国科学院广州地球化学研究所有机地球化学国家重点实验室广东广州510640 中国科学院大学北京100049 中国科学院深地科学卓越创新中心广东广州510640 中国石油新疆油田公司实验检测研究院新疆克拉玛依834000

近十年来,在玛湖凹陷发现了大面积连片分布的砾岩大油区,但凹陷区及其西部边缘克–百断裂带油气富集区的油源仍不清晰,分析原油的来源和充注过程对于推动该地区勘探具有重要的实际意义。通过对玛湖凹陷南斜坡和西斜坡21个含油储集岩样... 详细信息

近十年来,在玛湖凹陷发现了大面积连片分布的砾岩大油区,但凹陷区及其西部边缘克–百断裂带油气富集区的油源仍不清晰,分析原油的来源和充注过程对于推动该地区勘探具有重要的实际意义。通过对玛湖凹陷南斜坡和西斜坡21个含油储集岩样品进行连续抽提,获得了自由态组分a1和a2、束缚态组分b和包裹体组分c。对这些组分与同井位的13个原油样品进行GC、GC-MS以及GC-IRMS分析,依据正构烷烃单体C同位素组成特征,将含油储集岩连续抽提组分和原油样品分为Ⅰ、Ⅱ和Ⅲ类油组分。Ⅰ类油组分来源于下二叠统风城组(P_(1)f)烃源岩,Ⅱ类油组分来源于中二叠统下乌尔禾组(P_(2)w)烃源岩,Ⅲ类油组分来源于两套烃源岩的混合原油。含油储集岩连续抽提组分和原油样品成熟度变化大,从生油窗早期至晚期,成熟度严重影响了油源分子指标的应用效果。本文提出,应用成熟度分子指标与油源分子指标绘制交会图,可以对成熟度相近的连续抽提组分和原油样品进行油源对比。例如,应用C_(30)藿烷/n-C_(21)与Pr、Ph、伽马蜡烷、Ts、C_(29)Ts、C_(30)重排藿烷和C_(20)、C_(21)和C_(23)三环萜烷与n-C_(21)的比值绘制交会图,可以将Ⅰ、Ⅱ和Ⅲ类油组分有效区分开来,为玛湖凹陷油源对比研究提供了一个新方法。

关键词：玛湖凹陷砾岩大油区连续抽提单体烃C同位素分子地球化学

SnCl_(2)促进的Pt1/PS-PPh_(2)催化剂高选择性催化高碳烯烃氢甲酰化反应

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Chinese Journal of Catalysis 2024年第5期60卷 316-326页

作者：虞周楠张磊磊谈源龙井日峥曹宏晨楼才溢格日乐王军虎王爱琴张涛中国科学院大连化学物理研究所中国科学院应用催化科学技术重点实验室辽宁大连116023 中国科学院大学北京100049 中国科学院大连化学物理研究所低碳催化技术国家工程研究中心辽宁大连116023 中国科学院大连化学物理研究所穆斯堡尔谱数据中心辽宁大连116023

氢甲酰化作为工业上制备醛、醇等含氧化合物的重要反应,广泛应用于制备洗涤剂、增塑剂、表面活性剂和香料等.目前,氢甲酰化反应主要使用HCo(CO)4,HCo(CO)3(PR3)和HRh(CO)(PPh3)2等配合物作为催化剂.尽管Co基催化剂可以将高碳烯烃、内烯... 详细信息

氢甲酰化作为工业上制备醛、醇等含氧化合物的重要反应,广泛应用于制备洗涤剂、增塑剂、表面活性剂和香料等.目前,氢甲酰化反应主要使用HCo(CO)4,HCo(CO)3(PR3)和HRh(CO)(PPh3)2等配合物作为催化剂.尽管Co基催化剂可以将高碳烯烃、内烯烃以及支链烯烃高选择性地转化为直链醛,但其反应条件(5-30 MPa,140-200℃)较苛刻,且容易发生烯烃加氢等副反应.相比之下,Rh催化剂的活性比Co基催化剂高1-2个数量级,且反应条件较为温和.但Rh储量稀少,价格昂贵,而且对于高碳烯烃氢甲酰化反应,Rh催化剂难以分离和循环使用.因此,研究者开展了其他金属催化剂的研究,其中Pt-Sn催化剂因其出色的区域选择性而备受关注.但目前Pt-Sn催化剂多局限于均相催化体系,而且Sn助剂的作用尚不明确.本文采用商业化三苯基膦嫁接的聚苯乙烯小球为载体,通过浸渍法制备了SnCl_(2)-Pt1/PS-PPh_(2)单原子催化剂,考察了其在长链-烯烃氢甲酰化反应中的催化性能,并研究了Sn的促进作用.首先,以1-己烯氢甲酰化为探针反应,对催化剂的组成以及反应条件进行了优化.当Pt/P/Sn=1/2/5时,催化剂表现出最高的催化活性,在90-120℃和4-6 MPa合成气条件下,催化剂转化频率(TOF)为40 h^(-1),产物醛的正异比>42.随后,考察了催化剂的底物适用性.结果表明,C6-C12的高碳烯烃均可被高选择性地转化为相应的醛(正异比>20).然而,在循环使用实验中,由于SnCl_(2)不能稳定锚定在载体上,第二次循环时催化活性降低.但通过补加SnCl_(2),催化活性可以完全恢复.高压热过滤实验及元素检测结果表明,反应过程中Pt没有流失.X射线吸收光谱(XAFS)表征结果表明,反应后Pt仍以单原子形式存在,说明Pt1/PS-PPh_(2)具有良好的稳定性.通过准原位X-射线吸收谱、Mössbauer谱和红外光谱表征对反应过程中Pt和Sn的电子性质和配位结构进行了研究.结果表明,SnCl_(2)在反应过程中逐渐转化为Sn(dioxane)Cl3-物种(1,4-二氧六环为反应溶剂),并与Pt原子形成Pt-Sn键.当反应体系中没有Sn时,Pt(II)会被合成气过度还原并发生团聚.当没有膦配体时,Pt原子也会发生聚集,而且SnCl_(2)会在Pt(II)的催化作用下发生水解生成SnO.因此Sn(dioxane)Cl3-与膦配体共同抑制了Pt(I)在反应过程中的还原与聚集.最后,通过XAFS表征深入研究了反应机理.分析结果表明,CO在催化剂上具有较强的吸附作用,而H_(2)则可能以异裂的方式在催化剂上被活化.据此提出可能的反应机理:首先,H_(2)在催化剂上活化先形成Pt-H物种;随后,烯烃插入Pt-H,形成Pt-烷基物种;接着,CO迁移并插入,生成Pt-酰基物种;最后,经过还原消除步骤,得到最终的产物醛.综上,本文制备了一种对高碳烯烃氢甲酰化反应具有良好催化性能的SnCl_(2)-Pt1/PS-PPh_(2)单原子催化剂,为低成本非Rh基催化剂的开发提供借鉴.同时,揭示了催化体系中Sn的促进作用,为通过Lewis酸来调控催化剂的性能提供了参考.

关键词：氢甲酰化反应铂-锡催化剂高碳烯烃区域选择性单原子催化剂

3D Printing of NiCoP/Ti3C2 MXene Architectures for Energy Storage Devices with High Areal and Volumetric Energy Density

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Nano-Micro Letters 2020年第10期12卷 300-312页

作者： Lianghao yu Weiping Li Chaohui Wei Qifeng Yang yuanlong Shao Jingyu Sun College of Energy Soochow Institute for Energy and Materials InnovationS(SIEMIS)Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu ProvinceSoochow University215006 SuzhouJiangsuPeople’s Republic of China

Designing high-performance electrodes via 3D printing for advanced energy storage is appealing but remains challenging.In normal cases,light-weight carbonaceous materials harnessing excellent electrical conductivity have served as electrode candidates.However,they struggle with undermined areal and volumetric energy density of supercapacitor devices,thereby greatly impeding the practical applications.Herein,we demonstrate the in situ coupling of NiCoP bimetallic phosphide and Ti3C2 MXene to build up heavy NCPM electrodes affording tunable mass loading throughout 3D printing technology.The resolution of prints reaches 50μm and the thickness of device electrodes is ca.4 mm.Thus-printed electrode possessing robust open framework synergizes favorable capacitance of NiCoP and excellent conductivity of MXene,readily achieving a high areal and volumetric capacitance of 20 F cm^-2 and 137 F cm^-3 even at a high mass loading of^46.3 mg cm^-2.Accordingly,an asymmetric supercapacitor full cell assembled with 3D-printed NCPM as a positive electrode and 3D-printed activated carbon as a negative electrode harvests remarkable areal and volumetric energy density of 0.89 mWh cm^-2 and 2.2 mWh cm^-3,outperforming the most of state-of-the-art carbon-based supercapacitors.The present work is anticipated to offer a viable solution toward the customized construction of multifunctional architectures via 3D printing for high-energy-density energy storage systems.

关键词： 3D printing NiCoP/MXene Asymmetric supercapacitor Energy density Tailorable loading

Subtropical sea surface salinity maxima in the South Indian Ocean

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Journal of Oceanology and Limnology 2020年第1期38卷 16-29页

作者： WANG yu LI yuanlong WEI Chuanjie North China Sea Off shore Engineering Survey Institute North China Sea Branch of Ministry of Natural ResourcesQingdao 266061China Key Laboratory of Ocean Circulation and Waves Institute of OceanologyChinese Academy of SciencesQingdao 266071China Center for Ocean Mega-Science Chinese Academy of SciencesQingdao 266071China Engineering and Technology Department Institute of OceanologyChinese Academy of SciencesQingdao 266071China University of Chinese Academy of Sciences Beijing 100049China

Subtropical sea surface salinity(SSS)maximum is formed in the subtropical South Indian Ocean(SIO)by excessive evaporation over precipitation and serves as the primary salt source of the SIO.Spaceborne SSS measurements by Aquarius satellite during September 2011-May 2015 detect three disconnected SSS maximum regions(>35.6)in the eastern(105°E-115°E,38°S-28°S),central(60°E-100°E,35°S-25°S),and western(25°E-40°E,38°S-20°S)parts of the subtropical SIO,respectively.Such structure is however not seen in gridded Argo data.Analysis of Argo profile data confirms the existence of the eastern maximum patch and also reveals SSS overestimations of Aquarius near the western and eastern boundaries.Although subjected to large uncertainties,a mixed-layer budget analysis is employed to explain the seasonal cycle of SSS.The eastern and central regions reach the highest salinity in February-March and lowest salinity in August-September,which can be well explained by surface freshwater forcing(SFF)term.SFF is however not controlled by evaporation(E)or precipitation(P).Instead,the large seasonal undulations of mixed layer depth(MLD)is the key factor.The shallow(deep)MLD in austral summer(winter)amplifies(attenuates)the forcing effect of local positive E-P and causes SSS rising(decreasing).Ocean dynamics also play a role.Particularly,activity of mesoscale eddies is a critical factor regulating SSS variability in the eastern and western regions.

关键词： sea surface salinity(SSS) subtropical salinity maximum Aquarius Argo float freshwater flux