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Enabling an Inorganic-Rich Interface via Cationic Surfactant for High-Performance Lithium Metal Batteries

Nano-Micro Letters 2024年第8期16卷 1-17页

作者： Zejun Sun jinlin yang Hongfei Xu Chonglai Jiang Yuxiang Niu Xu Lian Yuan Liu Ruiqi Su Dayu Liu Yu Long Meng Wang Jingyu Mao Haotian yang Baihua Cui Yukun Xiao Ganwen Chen Qi Zhang Zhenxiang Xing Jisheng Pan Gang Wu Wei Chen Department of Chemistry National University of Singapore3 Science Drive 3Singapore 117543Singapore Agency for Science Technology and Research(A*STAR)Institute of High-Performance Computing1 Fusionopolis Way#16‑16 ConnexisSingapore 138632Singapore Department of Physics National University of Singapore2 Science Drive 3Singapore 117542Singapore Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityBinhai New CityFuzhou 350207People’s Republic of China Agency for Science Technologyand Research(A*STAR)Institute of Materials Research and EngineeringInnovis2 Fusionopolis Way#08‑03Singapore 138634Singapore

An anion-rich electric double layer(EDL)region is favorable for fabricating an inorganic-rich solid-electrolyte interphase(SEI)towards stable lithium metal anode in ester electrolyte.Herein,cetyltrimethylammonium bromide(CTAB),a cationic surfactant,is adopted to draw more anions into EDL by ionic interactions that shield the repelling force on anions during lithium plating.In situ electrochemical surface-enhanced Raman spectroscopy results combined with molecular dynamics simulations validate the enrichment of NO_(3)^(−)/FSI−anions in the EDL region due to the positively charged CTA^(+).In-depth analysis of SEI structure by X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry results confirmed the formation of the inorganic-rich SEI,which helps improve the kinetics of Li^(+)transfer,lower the charge transfer activation energy,and homogenize Li deposition.As a result,the Li||Li symmetric cell in the designed electrolyte displays a prolongated cycling time from 500 to 1300 h compared to that in the blank electrolyte at 0.5 mA cm^(-2) with a capacity of 1 mAh cm^(-2).Moreover,Li||LiFePO_(4) and Li||LiCoO_(2) with a high cathode mass loading of>10 mg cm^(-2) can be stably cycled over 180 cycles.

关键词： Cationic surfactant Lithium nitrate additive Solid-electrolyte interphase Electric double layer Lithium metal batteries

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Probing fluorination promoted sodiophilic sites with model systems of F_(16)CuPc and CuPc

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Frontiers of Optoelectronics 2022年第2期15卷 53-64页

作者： Yuan Liu Xu Lian Zhangdi Xie jinlin yang Yishui Ding Wei Chen Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityBinhai New CityFuzhou 350207China Department of Chemistry National University of Singapore3 Science Drive 3Singapore117543Singapore Centre for Advanced 2D Materials National University of Singapore6 Science Drive 2Singapore117546Singapore Department of Physics National University of Singapore2 Science Drive 3Singapore117542Singapore

Sodium metal batteries(SMBs)are receiving broad attention due to the high specific capacity of sodium metal anodes and the material abundance on earth.However,the growth of dendrites results in poor battery performance and severe safety problems,inhibiting the commercial application of SMBs.To stabilize sodium metal anodes,various methods have been developed to optimize the solid electrolyte interphase(SEI)layer and adjust the electroplating/stripping behavior of sodium.Among the methods,developing anode host materials and adding electrolyte additives to build a protective layer are promising and convenient.However,the understanding of the interaction process between sodium metal and those organic materials is still limited,but is essential for the rational design of advanced anode hosts and electrolyte additives.In this study,we use copper(II)hexadecafluorophthalocyanine(F_(16)CuPc),and copper(II)phthalocyanine(CuPc),as model systems to unravel the sodium interaction with polar functional groups by in-situ photoelectron spectroscopy and density functional theory(DFT)calculations.It is found that sodium atoms prefer to interact with the inner pyrrolic nitrogen sites of CuPc,while they prefer to interact with the outer aza bridge nitrogen atoms,owing to Na-F interaction at the Na/F_(16)CuPc interface.Besides,for the both organic molecules,the central Cu(II)ions are reduced to Cu(I)ions by charge transfer from deposited sodium.The fluorine-containing groups are proven to promote the interaction process of sodium in organic materials,which sheds light on the design of functional interfaces in host materials and anode protective layers for sodium metal anodes.

关键词： Fluorination Phthalocyanines Sodium metal anode Sodiophilic sites In-situ X-ray photoelectron spectroscopy(XPS)

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Engineering Cu_(1.96)S/Co_(9)S_(8) with sulfur vacancy and heterostructure as an efficient bifunctional electrocatalyst for water splitting

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Journal of Materials Science & Technology 2023年第23期154卷 1-8页

作者： Yuanhua Xiao Ya Shen Dangcheng Su Shiwei Zhang jinlin yang Dafeng Yan Shaoming Fang Xuezhao Wang Key Laboratory of Surface & Interface Science and Technology/College of Material and Chemical Engineering Zhengzhou University of Light Industry Zhengzhou 450002 China Department of Chemistry National University of Singapore 3 Science Drive 3 Singapore 117543 Singapore College of Chemistry and Chemical Engineering Hubei University Wuhan 430062 China College of Chemical and Food Zhengzhou University of Technology Zhengzhou 450044 China

Defect and interface engineering have been recognized as efficient strategies for developing high-performance electrocatalysts.However,it is still challenging to couple defect and interface engineering in transition metal sulfides and understand their dynamic evolution process during electrocatalysis.Herein,we developed one-step pyrolysis of bimetallic sulfide to construct S vacancy-rich Cu_(1.96)S/Co_(9)S_(8) heterostructure by controlling the critical decomposition temperature.The as-synthesized Cu_(1.96)S/Co_(9)S_(8) exhibits excellent bifunctional electrocatalytic performance,with a low overpotential of 99 and 200 mV at 10 mA cm−2 towards hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)in 1.0 mol/L KOH electrolyte,respectively.A symmetric two-electrode cell with Cu_(1.96)S/Co_(9)S_(8) delivered a current density of 10 mA cm^(−2) at a low voltage of 1.43 V and showed long-term stability for 200 h.A series of in/ex-situ techniques revealed that the electrochemical reconfiguration only appeared in the OER process,resulting in the CoOOH/CuO and SO42−species promoting OER performance.Meanwhile,the S vacancy and heterostructure interface in Cu_(1.96)S/Co_(9)S_(8) were proved to optimize the electronic structure and the adsorption of intermediates for HER by density function theory(DFT)simulations.This work provides a promising strategy to construct metal sulfides with rich defects and heterogeneous interfaces and understand their dynamic evolution process for electrochemical storage and conversion devices.

关键词： Cu_(1.96)S/Co_(9)S_(8) S vacancy Heterostructure Overall water-splitting

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自由与责任:康德与阿伦特论根本恶

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上饶师范学院学报 2024年第1期44卷 60-68页

作者：杨金霖湖南师范大学中华伦理文明研究中心湖南长沙410081

康德和阿伦特都对恶的问题进行了深入思考,但对于二者根本恶概念之间的关系,学界尚未有详细的讨论.采用准先验分析进路,可以发现恶的形成既受到先天因素的影响,也与社会环境因素紧密相关.这一路径为深化对康德和阿伦特根本恶理论共通性... 详细信息

康德和阿伦特都对恶的问题进行了深入思考,但对于二者根本恶概念之间的关系,学界尚未有详细的讨论.采用准先验分析进路,可以发现恶的形成既受到先天因素的影响,也与社会环境因素紧密相关.这一路径为深化对康德和阿伦特根本恶理论共通性的理解提供了一个有效的分析视角.基于此,对根本恶的分析应从经验性恶行出发,进而追溯到其更深层次的主观根据——人的自由本性.阿伦特和康德的自由概念在结构上具有相似性,二者在对根本恶的讨论中都十分关注人类的自由本性与道德责任.阿伦特对康德根本恶理论继承与发展,为深刻理解恶的问题提供了新的视角和更广阔的理论维度.

关键词：根本恶恶的平庸性康德阿伦特自由准先验路径

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From Micropores to Ultra-micropores inside Hard Carbon: Toward Enhanced Capacity in Room-/ Low-Temperature Sodium-Ion Storage

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Nano-Micro Letters 2021年第6期13卷 297-310页

作者： jinlin yang Xiaowei Wang Wenrui Dai Xu Lian Xinhang Cui Weichao Zhang Kexin Zhang Ming Lin Ruqiang Zou Kian Ping Loh Quan-Hong yang Wei Chen Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityBinhai New CityFuzhou 350207People’s Republic of China Department of Chemistry National University of Singapore3 Science Drive 3Singapore 117543Singapore National University of Singapore(Suzhou)Research Institute 377 Lin Quan StreetSuzhou Industrial ParkSuzhou 215123JiangsuChina Department of Physics National University of Singapore2 Science Drive 3Singapore 117542Singapore Nanoyang Group State Key Laboratory of Chemical EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300350People’s Republic of China Beijing Key Laboratory for Theory and Technology of Advanced Battery Materials Department of Materials Science and EngineeringCollege of EngineeringPeking UniversityBeijing 100871People’s Republic of China Institute of Materials Research and Engineering(IMRE) Agency of ScienceTechnologyand Research(A*STAR)3 Research LinkSingapore 117602Singapore

Pore structure of hard carbon has a fundamental influence on the electrochemical properties in sodium-ion batteries(SIBs).Ultra-micropores(1 nm)inside carbon into ultra-micropores(<0.5 nm).Consequently,the designed carbon anode displays an enhanced capacity of 346 mAh g^(−1) at 30 mA g^(−1) with a high ICE value of~80.6%and most of the capacity(~90%)is below 1 V.Moreover,the high-loading electrode(~19 mg cm^(−2))exhibits a good temperature endurance with a high areal capacity of 6.14 mAh cm^(−2) at 25℃ and 5.32 mAh cm^(−2) at −20℃.Based on the in situ X-ray diffraction and ex situ solid-state nuclear magnetic resonance results,the designed ultra-micropores provide the extra Na+storage sites,which mainly contributes to the enhanced capacity.This proposed strategy shows a good potential for the development of high-performance SIBs.

关键词： Carbon anode Ultra-micropores Extra sodium-ion storage sites Low-voltage capacity High areal capacity

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One-step synthesis of hierarchically porous hybrid TiO2 hollow spheres with high photocatalytic activity

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Frontiers of Materials Science 2016年第1期10卷 15-22页

作者： Ruiping LIU Feng REN jinlin yang Weiming SU Zhiming SUN Lei ZHANG Chang-an WANG Department of Materials Science and Engineering China University of Mining & Technology (Beijing) Beijing 100083 China School of Chemical & Environmental Engineering China University of Mining & Technology (Beijing) Beijing 100083 China Department of Mechanical Engineering PO Box 755905 University of Alaska Fairbanks Fairbanks AK 99775 USA School of Materials Science and Engineering State Key Laboratory of New Ceramics and Fine Processing Tsinghua University Beijing 100084 China

Hierarchically porous hybrid TiO2 hollow spheres were solvothermally synthesized successfully by using tetrabutyl titanate as titanium precursor and hydrated metal sulfates as soft templates. The as-prepared TiO2 spheres with hierarchically pore structures and high specific surface area and pore volume consisted of highly crystallized anatase TiO2 nanocrystals hybridized with a small amount of metal oxide from the hydrated sulfate. The proposed hydrated-sulfate assisted solvothermal （HAS） synthesis strategy was demonstrated to be widely applicable to various systems. Evaluation of the hybrid TiO2 hollow spheres for the photo-decomposition of methyl orange （MO） under visible-light irradiation revealed that they exhibited excellent photocatalytic activity and durability.

关键词： titania hybrid composite hollow spheres photocatalytic property

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追加外科手术治疗对高风险T1期结直肠癌内镜切除患者的预后影响

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四川大学学报（医学版） 2024年第2期55卷 411-417页

作者：罗鑫悦陈宇翔杨锦林邓凯吴俊超甘涛四川大学华西医院消化内科成都610041

目的分析内镜下切除后追加外科手术对于高风险T1期结直肠癌患者生存预后的影响。方法回顾性收集高风险T1期结直肠癌患者,根据内镜下切除后是否追加外科手术分为追加外科手术(endoscopic resection+surgical resection, ER+SR)组和内... 详细信息

目的分析内镜下切除后追加外科手术对于高风险T1期结直肠癌患者生存预后的影响。方法回顾性收集高风险T1期结直肠癌患者,根据内镜下切除后是否追加外科手术分为追加外科手术(endoscopic resection+surgical resection, ER+SR)组和内镜切除(endoscopic resection, ER)组,收集患者基线信息及病变部位、大小、术后病理等资料,并通过病历系统及随访等获得患者生存相关信息,主要结局指标为总生存率以及结直肠癌特异性生存率。采用单因素Cox回归分析分析筛选生存相关风险因素,计算风险比(HR),并通过多因素Cox回归分析独立影响因素。结果共收集109例高风险T1期结直肠癌患者,其中ER组52例,ER+SR组57例,ER组的患者平均年龄高于ER+SR组(65.21岁vs. 60.54岁,P=0.035),ER组内镜下病变长径中位数略小于ER+SR组(2.00 cm vs. 2.50 cm,P=0.026)。ER+SR组中位随访时间为30.00个月,最长随访119.00个月,共有4名患者死亡,1名为结直肠癌相关死亡;而ER组中位随访时间为28.50个月,最长随访78.00个月,共有4名患者死亡,1名死于结直肠癌。5年累积生存率比较中,ER+SR组及ER组总生存率分别为94.44%和81.65%,而5年累积肿瘤特异性生存率分别为97.18%和98.06%。Kaplan-Meier分析显示ER+SR组及ER组患者累积总生存率、累积肿瘤特异性生存率差异无统计学意义。Cox单因素回归分析显示年龄及复查次数为总生存率相关危险因素(HR=1.16及0.27,P=0.005及0.025),进一步多因素Cox回归分析显示年龄为总生存率相关独立危险因素(HR=1.10,P=0.045)。结论对于内镜切除术后存在高风险因素的T1期结直肠癌患者,也不可忽视患者年龄、自身意愿等因素,在实际临床实践过程中更加慎重地选择追加外科手术。

关键词： T1期结直肠癌高风险内镜切除外科手术生存预后

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基于累加式实时串并联变换算法的机械故障声学监测方法

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机电工程 2024年第2期41卷 364-370页

作者：祝洲杰杨金林毛鹏峰浙江机电职业技术学院智能制造学院浙江杭州310053 浙江理工大学机械工程学院浙江杭州310018 中杭监测技术研究院有限公司浙江杭州310022

针对基于物联网(IoT)的冲压机床故障监测问题,为了降低冲压机床故障监测的计算复杂度,并提高其低频识别的精度,提出了一种无需机器学习技术的实时性机械故障声学监测方法,即基于累加式实时串并联变换算法的机械故障声学监测方法。首先,... 详细信息

针对基于物联网(IoT)的冲压机床故障监测问题,为了降低冲压机床故障监测的计算复杂度,并提高其低频识别的精度,提出了一种无需机器学习技术的实时性机械故障声学监测方法,即基于累加式实时串并联变换算法的机械故障声学监测方法。首先,研究了物联网场景中冲压机床声学低频分析的必要性,并给出了声学信号的表达式;然后,针对频率轴上多个周期信号重叠导致参数估计较为困难的问题,提出了一种累加式实时串并联变换算法,将输入的采样序列馈入多个具有不同输出端口的串并转换器,从累加的波形中检测出最大绝对值,并进行了比较;最后,通过样本时隙划分,将累加式实时串并联变换算法应用于机械故障监测;通过仿真和冲压机床实机测试,对累加式实时串并联变换算法和实时性机械故障声学监测方法的有效性进行了验证。研究结果表明:在无需大量信号样本的情况下,使用累加式实时串并联变换算法有利于提高低频带的识别精度;在直方图相关性方面,累加式实时串并联变换算法和Morlet小波变换具有相同的性能,且均明显优于短时傅立叶变换;同时,尽管累加式实时串并联变换算法需要的加法总数比Morlet小波变换多2.5倍,但是乘法总数减少了20447%,大幅减少了计算的复杂度。

关键词：机械故障监测冲压机床累加式实时串并联变换算法串并转换器低频识别精度计算复杂度

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Carbon-based flexible self-supporting cathode for lithium-sulfur batteries:Progress and perspective

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Carbon Energy 2021年第2期3卷 271-302页

作者： Qinghuiqiang Xiao jinlin yang Xiaodong Wang Yirui Deng Peng Han Ning Yuan Lei Zhang Ming Feng Chang‐an Wang Ruiping Liu Department of Materials Science and Engineering China University of Mining and Technology(Beijing)BeijingChina School of Materials Science and Engineering Tsinghua UniversityBeijingChina Department of Mechanical Engineering University of Alaska FairbanksFairbanksAlaskaUSA Department of Applied Physics Key Laboratory of Functional Materials Physics and Chemistry of the Ministry of EducationJilin Normal UniversityChangchunChina

The flexible self-supporting electrode can maintain good mechanical and electrical properties while retaining high specific capacity,which meets the requirements of flexible batteries.Lithium-sulfur batteries(LSBs),as a new generation of energy storage system,hold much higher theoretical energy density than traditional batteries,and they have attracted extensive attention from both the academic and industrial communities.Selection of a proper substrate material is important for the flexible self-supporting electrode.Carbon materials,with the advantages of light weight,high conductivity,strong structural plasticity,and low cost,provide the electrode with a large loading space for the active material and a conductive network.This makes the carbon materials meet the mechanical and electrochemical requirements of flexible electrodes.In this paper,the commonly used fabrication methods and recent research progresses of the flexible self-supporting cathode with a carbon material as the substrate are introduced.Various sulfur loading methods are summarized,which provides useful information for the structural design of the cathode.As the first review article of the carbon-based flexible self-supporting LSB cathodes,it provides valuable guidance for the researchers working in the field of LSB.

关键词： carbon flexible lithium sulfur batteries self-supporting

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An in-situ spectroscopy investigation of alkali metal interaction mechanism with the imide functional group

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Nano Research 2020年第12期13卷 3224-3229页

作者： Xu Lian Zhirui Ma Zhonghan Zhang jinlin yang Shuo Sun Chengding Gu Yuan Liu Honghe Ding Jun Hu Xu Cao Junfa Zhu Shuzhou Li Wei Chen Department of Chemistry National University of SingaporeSingapore117543Singapore Centre for Advanced 2D Materials National University of SingaporeSingapore117546Singapore School of Materials Science and Engineering Nanyang Technological UniversitySingapore639798Singapore National University of Singapore(Suzhou)Research Institute Suzhou215123China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityFuzhou350207China National Synchrotron Radiation Laboratory Department of Chemical PhysicsUniversity of Science and Technology of ChinaHefei230029China Department of Physics National University of SingaporeSingapore117542Singapore

Organic anode materials have attracted considerable interest owing to their high tunability by adopting various active functional groups.However,the interaction mechanisms between the alkali metals and the active functional groups in host materials have been rarely studied systematically.Here,a widely used organic semiconductor of perylene-3,4,9,10-tetracarboxylic diimide(PTCDI)was selected as a model system to investigate how alkali metals interact with imide functional groups and induce changes in chemical and electronic structures of PTCDI.The interaction at the alkali/PTCDI interface was probed by in-situ X-ray photoelectron spectroscopy(XPS),ultraviolet photoelectron spectroscopy(UPS),synchrotron-based near edge X-ray absorption fine structure(NEXAFS),and corroborated by density functional theory(DFT)calculations.Our results indicate that the alkali metal replaces the hydrogen atoms in the imide group and interact with the imide nitrogen of PTCDI.Electron transfer induced gap states and downward band-bending like effects are identified on the alkali-deposited PTCDI surface.It was found that Na shows a stronger electron transfer effect than Li.Such a model study of alkali insertion/intercalation in PTCDI gives insights for the exploration of the potential host materials for alkali storage applications.

关键词： perylene-3,4,9,10-tetracarboxylic diimide(PTCDI) lithium storage organic anode imide electron transfer

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