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Optimizing high-coordination shell of Co-based single-atom catalysts for efficient ORR and zinc-air batteries

Journal of Energy Chemistry 2024年第8期95卷 306-314页

作者： Yugang Qi Qing Liang Kexin Song Xinyan Zhou Meiqi liu Wenwen Li Fuxi liu Zhou Jiang Xu Zou zhongjun Chen Wei Zhang Weitao Zheng Key Laboratory of Automobile Materials MOE School of Materials Science & Engineering Electron Microscopy Center and International Center of Future Science Jilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy Materials Jilin University Institute of High Energy Physics Chinese Academy of Sciences

Atom-level modulation of the coordination environment for single-atom catalysts(SACs) is considered as an effective strategy for elevating the catalytic performance. For the MNxsite, breaking the symmetrical geometry and charge distribution by introducing relatively weak electronegative atoms into the first/second shell is an efficient way, but it remains challenging for elucidating the underlying mechanism of interaction. Herein, a practical strategy was reported to rationally design single cobalt atoms coordinated with both phosphorus and nitrogen atoms in a hierarchically porous carbon derived from metal-organic frameworks. X-ray absorption spectrum reveals that atomically dispersed Co sites are coordinated with four N atoms in the first shell and varying numbers of P atoms in the second shell(denoted as Co-N/P-C).The prepared catalyst exhibits excellent oxygen reduction reaction(ORR) activity as well as zinc-air battery performance. The introduction of P atoms in the Co-SACs weakens the interaction between Co and N,significantly promoting the adsorption process of *OOH, resulting in the acceleration of reaction kinetics and reduction of thermodynamic barrier, responsible for the increased intrinsic activity. Our discovery provides insights into an ultimate design of single-atom catalysts with adjustable electrocatalytic activities for efficient electrochemical energy conversion.

关键词： Electrocatalytic Oxygen reduction reaction Shell coordination optimization Single atom catalyst

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Manipulating Na occupation and constructing protective film of P2-Na_(0.67)Ni_(0.33)Mn_(0.67)O_(2) as long-term cycle stability cathode for sodium-ion batteries

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Journal of Energy Chemistry 2024年第1期88卷 603-611,I0013页

作者： Yiran Sun Pengfei Zhou Siyu liu zhongjun Zhao Yihao Pan Xiangyan Shen Xiaozhong Wu Jinping Zhao Junying Weng Jin Zhou School of Chemistry and Chemical Engineering Shandong University of TechnologyZibo 0255000ShandongChina School of Materials Science and Engineering Shandong University of TechnologyZibo 255049ShandongChina

P2-Na_(0.67)Ni_(0.33)Mn_(0.67)O_(2)(NNMO)is promising cathode material for sodium-ion batteries(SIBs)due to its high specific capacity and fast Na+diffusion rate.Nonetheless,the irreversible P2-O_(2)phase transformation,Na+/vacancy ordering,and transition metal(TM)dissolution seriously damage its cycling stability and restrict its commercialization process.Herein,Na occupation manipulation and interface stabilization are proposed to strengthen the phase structure of NNMO by synergistic Zn/Ti co-doping and introducing lithium difluorophosp(LiPO_(2)F_(2))film-forming electrolyte additive.The Zn/Ti co-doping regulates the occupancy ratio of Nae/Nafat Na sites and disorganizes the Na+/vacancy ordering,resulting in a faster Na+diffusion kinetics and reversible P2-Z phase transition for P2-Na_(0.67)Ni_(0.28)Zn_(0.05)Mn_(0.62)Ti_(0.05)O_(2)(NNZMTO).Meanwhile,the LiPO_(2)F_(2)additive can form homogeneous and ultrathin cathode-electrolyte interphase(CEI)on NNZMTO surface,which can stabilize the NNZMTO-electrolyte interface to prevent TM dissolution,surface structure transformation,and micro-crack generation.Combination studies of in situ and ex situ characterizations and theoretical calculations were used to elucidate the storage mechanism of NNZMTO with Li PO_(2)F_(2)additive.As a result,the NNZMTO displays outstanding capacity retention of 94.44%after 500 cycles at 1C with 0.3 wt%Li PO_(2)F_(2),excellent rate performance of 92.5 mA h g^(-1)at 8C with 0.1 wt%Li PO_(2)F_(2),and remarkable full cell capability.This work highlights the important role of manipulating Na occupation and constructing protective film in the design of layered materials,which provides a promising direction for developing high-performance cathodes for SIBs.

关键词： Layered cathode Zn/Ti co-doping Na occupation Electrolyte additive Sodium-ion batteries

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N-Glycosylated type Ⅱ collagen peptides as therapeutic saccharide vaccines for rheumatoid arthritis

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Chinese Chemical Letters 2024年第5期35卷 197-200页

作者： Dake liu Shuyan liu Fanlei Hu Zhongtang Li zhongjun Li State Key Laboratory of Natural and Biomimetic Drugs School of Pharmaceutical SciencesPeking UniversityBeijing 100191China Department of Rheumatology and Immunology Peking University People’s HospitalBeijing 100044China

The interaction among type Ⅱ collagen(CⅡ),human DR4 major histocompatibility complex type Ⅱ molecule(MHC Ⅱ)and T-cell receptor(TCR)is associated with the development of rheumatoid arthritis(RA).The activation of T cells can be reduced through exposure to modified CⅡ(263-272)glycopeptide fragment via competitive inhibition with self-antigen.In this work,30 peptides based on the sequence of CⅡ(263-272)were prepared and evaluated for their binding to DR4 protein by surface plasmon resonance(SPR)assay.The effect on the secretion of pro-inflammatory factors by the spleen cells in collagen induced rheumatoid arthritis(CIA)mouse was also investigated.Two N-glycosylated CⅡ peptides were identified to have strong binding to the human recombinant DR4 protein and weak proinflammatory effect.These glycopeptides could be developed as therapeutic saccharide vaccines for the treatment of rheumatoid arthritis(RA).

关键词： Rheumatoid arthritis TypeⅡcollegan Glycosylation N-Glycosylated altered peptides Saccharide vaccines

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High efficacy of tetra-PEG hydrogel sealants for sutureless dural closure

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Bioactive Materials 2022年第2期7卷 12-19页

作者： Tengjiao Zhu Hufei Wang Zehao Jing Daoyang Fan zhongjun liu Xing Wang Yun Tian Department of Orthopaedics Peking University Third HospitalBeijing100191China Beijing Key Laboratory of Spinal Disease Research Beijing100191China Engineering Research Center of Bone and Joint Precision Medicine Ministry of EducationBeijing100191China Beijing National Laboratory for Molecular Sciences Institute of ChemistryChinese Academy of SciencesBeijing100190China University of Chinese Academy of Sciences Beijing 100049China

Advances in meticulous dural closure technique remain a great challenge for watertight dural closure in the aged society,because the cerebrospinal fluid(CSF)leakage after spinal surgery is often accompanied with the disgusting wound infection,meningitis and pseudomeningocele.Here,a tetra-poly(ethylene glycol)(PEG)-based hydrogel sealant is developed with collective advantages of facile operation,high safety,quick set time,easy injectability,favorable mechanical strength and powerful tissue adhesion for effective sutureless dural closure during the surgery procedure.Impressively,this tetra-PEG sealant can instantaneously adhere to the irregular tissue surfaces even in a liquid environment,and effectively prevent or block off the intraoperative CSF leakage for sutureless dural closure and dura regeneration.Together,this sutureless tetra-PEG adhesive can be utilized as a very promising alternative for high-efficient watertight dural closure of the clinical patients who incidentally or deliberately undergo the durotomy during the spinal surgery.

关键词： CSF leakage Dural repair Watertight closure Sutureless Tetra-PEG hydrogel

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径-轴向磁轴承冷却设计及温度场分析

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中国电机工程学报 2024年第12期44卷 4945-4955,I0029页

作者：刘斌余中军付佳舰船综合电力技术国防科技重点试验室(海军工程大学) 湖北省武汉市430033

由于磁轴承与转子无直接物理接触、支承特性可控,在小功率等级电机环境下其损耗较低,可采用自然冷却。而对于大功率等级电机,磁轴承损耗增大,必须考虑冷却设计以降低其温升。该文以某型兆瓦级高速永磁发电机磁轴承为研究对象,在考虑径-... 详细信息

由于磁轴承与转子无直接物理接触、支承特性可控,在小功率等级电机环境下其损耗较低,可采用自然冷却。而对于大功率等级电机,磁轴承损耗增大,必须考虑冷却设计以降低其温升。该文以某型兆瓦级高速永磁发电机磁轴承为研究对象,在考虑径-轴向磁轴承集成状态及发电机实际内部环境条件下,基于径-轴向磁轴承三维流场、温度场分析,首先研究了自然冷却条件下磁轴承温度场特征,结果表明磁轴承温度过高,径向磁轴承定转子会产生较大热变形,增大磁轴承安全运行风险。为了解决该问题,该文结合电机空冷结构和磁轴承结构特征,提出一种集成化主动冷却结构,并仿真分析了冷却效果,结果表明进行主动冷却后径-轴向磁轴承温度明显下降,径向磁轴承定转子气隙变化量大幅减小。最后,进行样机温升试验,试验结果与仿真结果一致。

关键词：磁轴承集成状态三维温度场分析冷却设计

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Tuning the Surface Field by Embedding Cations into Metals to Direct the Reaction Pathway of CO_(2) Electroreduction

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CCS Chemistry 2024年第3期6卷 631-640页

作者： Pei Zhang Meng Zhou Shiqiang liu Xueqing Xing Jiahao Yang Peng Chen Yaoyu Yin Yingying Cheng Xing Tong Jun Ma Qinggong Zhu Xiaofu Sun zhongjun Chen Xinchen Kang Buxing Han Beijing National Laboratory for Molecular Sciences CAS Laboratory of Colloid and Interface and ThermodynamicsCAS Research/Education Center for Excellence in Molecular SciencesCenter for Carbon Neutral ChemistryInstitute of ChemistryChinese Academy of SciencesBeijing 100190 Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049 Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai 200062 School of Chemistry University of Chinese Academy of SciencesBeijing 100049

The creation of universal strategies to affect the reaction route of the electroreduction of CO_(2) is critical.Here,we report the first work to introduce cations into diverse metals such as Cu,Bi,In,and Sn via the electroreduction of related metallic oxides in quaternary ammonium surfactant solutions.Compared to their physical adsorption,cations embedded into the electrodes have a more pronounced impact on the electrical field,which effectively influences the adsorption state of intermediates.With the increase of surface field,the hydrogen evolution reaction and*COOH route are significantly reduced,favouring the*OCHO pathway instead.As a result,hydrogen,CO,and C_(2+)products almost completely vanish at−0.5 V versus RHE in 0.1 M Na_(2)SO_(4)in an H-type cell after enough cations are embedded into the Cu electrode,and the faradaic efficiency of formate rises from 18.0%to 99.5%simultaneously.

关键词： CO_(2)electroreduction tuneable products electrical field reaction pathway cations embedding

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Surface treatment of 3D printed porous Ti6Al4V implants by ultraviolet photofunctionalization for improved osseointegration

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Bioactive Materials 2022年第1期7卷 26-38页

作者： Chuan Yin Teng Zhang Qingguang Wei Hong Cai Yan Cheng Yun Tian Huijie Leng Caimei Wang Shiqing Feng zhongjun liu Department of Orthopedics Peking University Third HospitalBeijing100191People’s Republic of China Department of Orthopedics Qilu Hospital of Shandong UniversityJinan250012People’s Republic of China Center for Biomedical Materials and Tissue Engineering Academy for Advanced Interdisciplinary StudiesPeking UniversityBeijing100871People’s Republic of China Beijing AKEC Medical Company Ltd. Beijing102200People’s Republic of China

Three-dimensional(3D)-printed porous Ti6Al4V implants play an important role in the reconstruction of bone defects.However,its osseointegration capacity needs to be further improved,and related methods are inadequate,especially lacking customized surface treatment technology.Consequently,we aimed to design an omnidirectional radiator based on ultraviolet(UV)photofunctionalization for the surface treatment of 3D-printed porous Ti6Al4V implants,and studied its osseointegration promotion effects in vitro and in vivo,while elucidating related mechanisms.Following UV treatment,the porous Ti6Al4V scaffolds exhibited significantly improved hydrophilicity,cytocompatibility,and alkaline phosphatase activity,while preserving their original mechanical properties.The increased osteointegration strength was further proven using a rabbit condyle defect model in vivo,in which UV treatment exhibited a high efficiency in the osteointegration enhancement of porous Ti6Al4V scaffolds by increasing bone ingrowth(BI),the bone-implant contact ratio(BICR),and the mineralized/osteoid bone ratio.The advantages of UV treatment for 3D-printed porous Ti6Al4V implants using the omnidirectional radiator in the study were as follows:1)it can significantly improve the osseointegration capacity of porous titanium implants despite the blocking out of UV rays by the porous structure;2)it can evenly treat the surface of porous implants while preserving their original topography or other morphological features;and 3)it is an easy-to-operate low-cost process,making it worthy of wide clinical application.

关键词： Three-dimensional-printed porous implants UV photofunctionalization Omnidirectional UV radiator Osseointegration

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播种机星齿球面盘式覆土装置设计与试验

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农业机械学报 2024年第4期55卷 23-31,73页

作者：卢琦刘立晶刘忠军靳文停中国农业机械化科学研究院集团有限公司北京100083 农业装备技术全国重点实验室北京100083

针对V型挤压式覆土装置在黏土条件下作业不可靠,种沟闭合不严实,易造成种子“架空”和“晾种”的生产实际问题,设计一种星齿球面盘式覆土装置,提高播种机覆土质量。分析了星齿球面盘式覆土装置的作业原理,通过对覆土作业过程中土壤颗粒... 详细信息

针对V型挤压式覆土装置在黏土条件下作业不可靠,种沟闭合不严实,易造成种子“架空”和“晾种”的生产实际问题,设计一种星齿球面盘式覆土装置,提高播种机覆土质量。分析了星齿球面盘式覆土装置的作业原理,通过对覆土作业过程中土壤颗粒的运动学分析,确定了影响覆土作业质量的主要结构参数,并对星齿球面覆土盘主要结构参数和安装参数进行了设计。借助EDEM离散元仿真技术,建立了土壤与覆土装置的互作模型,以星齿球面覆土盘安装倾角、安装间距、入土深度为试验因素,以覆土量与覆土量变异系数为评价指标,分别进行了单因素与Box-Behnken试验,确定了星齿球面覆土盘的最优结构参数组合为安装倾角25.03°、安装间距196.66 mm、入土深度77.65 mm。取安装倾角25°、安装间距197 mm、入土深度77 mm进行了田间验证试验,试验结果表明:最优参数组合下,覆土量平均值为241.46 g,与仿真结果基本一致,相对误差为5.12%,覆土量变异系数为3.71%,覆土均匀,作业质量好,覆土作业后种子播深满足农艺要求,星齿球面盘式覆土装置能有效改善播种机的覆土性能。

关键词：播种机覆土装置星齿球面盘 EDEM仿真

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碳纳米管内水吸附行为及等量吸附热的巨正则Monte Carlo模拟

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计算物理 2024年第2期41卷 203-213页

作者：刘晨刘忠军赵明慧敖庆波西安石油大学材料科学与工程学院陕西西安710065 西北有色金属研究院金属多孔材料国家重点实验室陕西西安710016

采用巨正则蒙特卡罗方法对单壁碳纳米管-水吸附体系进行计算模拟,通过对吸附和脱附等温线、局部密度分布、等量吸附热等进行表征,系统研究298 K时孔长、孔径以及表面强度对孔隙内水吸附行为的影响。结果表明:孔径效应对孔内水吸附行为... 详细信息

采用巨正则蒙特卡罗方法对单壁碳纳米管-水吸附体系进行计算模拟,通过对吸附和脱附等温线、局部密度分布、等量吸附热等进行表征,系统研究298 K时孔长、孔径以及表面强度对孔隙内水吸附行为的影响。结果表明:孔径效应对孔内水吸附行为影响显著,随着孔径逐渐增大,水分子先后以单链水、双链空心水环、水团簇的排列状态在孔内完成吸附。孔长在4~8 nm范围内时,随着孔长变大,发生吸附的初始压力越来越小,但当孔长增加到10 nm时,其对初始吸附压力的影响不再明显。最后,随着表面强度增大,发生水吸附的初始压力越来越小;同时,较小表面强度水分子的毛细蒸发相变过程瞬间完成,而当表面强度提高到40 K时,毛细蒸发相变过程则呈现出连续、逐渐完成的特点。

关键词：碳纳米管吸附作用蒙特卡罗模拟等量吸附热相变

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过滤用金属多孔材料力学性能研究进展

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粉末冶金技术 2024年第1期42卷 59-67页

作者：梁凯刘忠军姬帅高博阳西安石油大学材料科学与工程学院西安710065

金属多孔材料作为功能与结构兼具的一类新型材料,已被广泛应用于吸声、吸能、流体分布、换热、催化、过滤分离等领域,其中在过滤分离领域应用最为广泛。金属多孔材料在石油石化、精细化工、煤化工等领域可以实现不同流体的液–固、气–... 详细信息

金属多孔材料作为功能与结构兼具的一类新型材料,已被广泛应用于吸声、吸能、流体分布、换热、催化、过滤分离等领域,其中在过滤分离领域应用最为广泛。金属多孔材料在石油石化、精细化工、煤化工等领域可以实现不同流体的液–固、气–固过滤分离,不同领域对所用金属多孔材料的材质及力学性能要求也不尽相同。过滤用金属多孔材料的制备工艺已相对成熟,但对其耐蚀性能及力学性能的表征研究较少,金属过滤元件的力学性能及耐腐蚀性能将直接关系到该类材料的使用效果和寿命。本文总结了近几年过滤用金属多孔材料力学性能及耐腐蚀行为的研究进展,探讨了该类材料在腐蚀与力学行为中存在的问题,最后展望了过滤用金属多孔材料的发展方向。

关键词：金属多孔材料过滤分离力学性能腐蚀行为

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