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Metal-organic frameworks for electrochemical energy conversion:status and challenges

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Science China Chemistry 2020年第1期63卷 7-10页

作者： Kexin Zhang zibin liang Ruqiang Zou Beijing Key Laboratory for Theory and Technology of Advanced Battery Materials Department of Materials Science and Engineering College of Engineering Peking University

The quickly expanded energy consumption based on traditional fossil fuels has resulted in energy crises and severe environmental problems.Developing sustainable energy conversion technology is an important issue confronting the global energy security and consumption.Electrochemical energy storage and conversion is one of the most perspective renewable ways to produce carbon-free fuels via water splitting,and convert chemicals into electricity by fuel cells and metal-air batteries.A recent class of porous materials,metal-organic frameworks(MOFs),has been extensively explored as electrocatalysts or precursors to derive efficient composites in virtue of their large surface area,high porosity,tunable structures,and uniform dispersion of components[1].Because most MOFs are formed by inexpensive transition metals and commercial organic ligands.

关键词： composites energy porosity

Metal-organic framework based nanomaterials for electrocatalytic oxygen redox reaction

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Science China Chemistry 2019年第4期62卷 417-429页

作者： Kexin Zhang Wenhan Guo zibin liang Ruqiang Zou Beijing Key Laboratory for Theory and Technology of Advanced Battery Materials Department of Materials Science and EngineeringCollege of Engineering Peking University

Due to the severe environmental issues, many advanced technologies, typically fuel cells and metal-air batteries have aroused widespread concerns and been intensively studied in recent years. However, oxygen redox reactions including oxygen evolution reaction(OER) and oxygen reduction reaction(ORR) as the core reactions suffer from sluggish kinetics of the multiple electron transfer process. Currently, Pt, RuO_2, and IrO_2 are considered to be the benchmark catalysts for ORR and OER, but their high price, scarcity and instability hinder them from large-scale application. To overcome these limits, exploring alternative electrocatalysts with low cost, high activity, long-term stability, and earth-abundance is of extreme urgency. Metal-organic frameworks(MOFs) are a family of inorganic-organic hybrid materials with high surface areas and tunable structures, making them proper as catalyst candidates. Herein, the recent progress of MOFs and MOF-derived materials for ORR and OER is systematically reviewed, and the relationship between compositions and electrochemical performance is discussed. It is expected that this review can be helpful for the future development of related MOF-based materials with excellent electrochemical performance.

关键词： metal-organic frameworks oxygen evolution reaction oxygen reduction reaction earth-abundant materials electrocatalysis nanomaterials

Targeting β-secretase with RNAi in neural stem cells for Alzheimer's disease therapy

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Neural Regeneration Research 2013年第33期8卷 3095-3106页

作者： Zhonghua Liu Shengliang Li zibin liang Yan Zhao Yulin Zhang Yaqi Yang Minjuan Wang Feng Li Department of Neurobiology and Anatomy Zhongshan School of MedicineSun Yat-sen University

There are several major pathological changes in Alzheimer＇s disease, including apoptosis of cho- linergic neurons, overactivity or overexpression of 13-site amyloid precursor protein cleaving enzyme 1 （BACE1） and inflammation. In this study, we synthesized a 19-nt oligonucleotide targeting BACE1, the key enzyme in amyloid beta protein （AI3） production, and introduced it into the pSilenCircle vector to construct a short hairpin （shRNA） expression plasmid against the BACE1 gene. We transfected this vector into C17.2 neural stem cells and primary neural stem cells, resulting in downregulation of the BACE1 gene, which in turn induced a considerable reduction in reducing AI3 protein production. We anticipate that this technique combining cell transplantation and gene ther- apy will open up novel therapeutic avenues for Alzheimer＇s disease, particularly because it can be used to simultaneously target several pathogenetic changes in the disease.

关键词： neural regeneration neurodegenerative disease secretase neural stem cells Alzheimer＇sdisease C17.2 neural stem cells primary neural stem cells shRNA plasmid genetic modification grants-supported paper neuroregeneration

A new dual-ion battery based on amorphous carbon

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Science Bulletin 2019年第21期64卷 1634-1642页

作者： Wei(Alex)Wang Hanxin Huang Bin Wang Chang Qian Peihao Li Jinhui Zhou zibin liang Chao Yang Shaojun Guo Department of Materials Science and Engineering College of EngineeringPeking UniversityBeijing 100871China BIC-ESAT College of EngineeringPeking UniversityBeijing 100871China Beijing Key Laboratory for Magnetoeletric Materials and Devices(BKL-MEMD) Peking UniversityBeijing 100871China Department of Energy and Resources Engineering College of EngineeringPeking UniversityBeijing 100871China

The Na-based dual-ion batteries(NDIBs),combining the advantages of Na-ion batteries and dual-ion batteries,are attracting more attention due to their merits of abundant source,low cost and high energy density.However,the main challenges faced by NDIBs are their low capacity and poor cycling.Herein,we report a new ion storage mechanism for high-performance NDIBs using amorphous carbon(AOMC)as cathode.Unlike the graphite carbon that can only accommodate the PF6-anion(typical DIB system),the AOMC herein can both accommodate Na+cation and PF6-anion due to its amorphous feature,which is conceptually new dual-ion system for achieving much higher capacity.Ex-situ X-ray photoelectron spectroscopy,X-ray diffraction and Raman studies reveal that the disordered carbon in the AOMC can be transformed to the partial graphitic stacking in short range,improving both capacity and cycling stability of NDIBs.As a consequence,the AOMC delivers a highly reversible storage capacity of 136 mAhg-1 for 800 cycles at a very high current density of 2.0 Ag-1,much higher than all the reported NDIBs.Such concept can be generalized to develop high-performance dual-ion full cell using sodium ion preintercalated materials as anode and AOMC as cathode.

关键词： Na-based dual-ion batteries Amorphous carbon Storage mechanism Larger interlayer spacing

Metal-organic framework-derived Fe/Cu-substituted Co nanoparticles embedded in CNTs-grafted carbon polyhedron for Zn-air batteries

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Carbon Energy 2020年第2期2卷 283-293页

作者： Kexin Zhang Yelong Zhang Qinghua Zhang zibin liang Lin Gu Wenhan Guo Bingjun Zhu Shaojun Guo Ruqiang Zou Beijing Key Laboratory for Theory and Technology of Advanced Battery Materials Department of Materials Science and EngineeringCollege of EngineeringPeking UniversityBeijingChina Department of Applied Physics and Materials Wuyi UniversityJiangmenGuangdong ProvinceChina Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of SciencesBeijingChina Institute of Clean Energy Peking UniversityBeijingChina

Metal-organic frameworks(MOFs)and MOF-derived materials have attracted great attention as alternatives to noble-metal based electrocatalysts owing to their intriguing structure properties,especially for high efficiency and stable oxygen reduction reaction(ORR).Herein,we employed a one-pot reaction to make a multimetal(Fe,Co,Cu,and Zn)mixed zeolitic imidazolate framework(MM-ZIF)via adopting a simple in situ redox reaction.Further pyrolysis of the target MM-ZIF,a highly porous carbon polyhedron(FC-C@NC)grafted with abundant carbon nanotubes was obtained,in which ultrasmall Co nanoparticles with partial lattice sites substituted by Fe and Cu were embedded.The obtained FC-C@NC possessed large surface area,highly porous structure,widely-spread metal active sites,and conductive carbon frameworks,contributing to outstanding ORR activity and long-term stability.It displayed superior tolerance to methanol crossover and exceeded the commercial Pt/C catalyst and most previously reported non-noble-metal catalysts.Impressively,the as-produced FC-C@NC-based zinc-air battery afforded an open-circuit potential of 1.466 V,a large specific capacity of 659.5 mAh/g,and a high gravimetric energy density of 784.3 Wh/kgZn,significantly outperforming the Pt/C-based cathode.

关键词： electrocatalysis lattice sites substitution metal-organic frameworks oxygen reduction reaction zinc-air battery

Atomic Fe-N4 sites on electrospun hierarchical porous carbon nanofibers as an efficient electrocatalyst for oxygen reduction reaction

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Chinese Chemical Letters 2020年第6期31卷 1588-1592页

作者： Ruiqin Zhong Chenxu Zhi Yingxiao Wu zibin liang Hassina Tabassum Hao Zhang Tianjie Qiu Song Gao Jinming Shi Ruqiang Zou State Key Laboratory of Heavy Oil Processing China University of PetroleumBeijing 102249China Beijing Key Laboratory for Theory and Technology of Advanced Battery Materials Department of Materials Science and EngineeringCollege of EngineeringPeking UniversityBeijing J00871China

Porous carbon materials doped with atomically dispersed metal sites(ADMSs)are promising electrocatalysts for oxygen reduction reaction(ORR)electrocatalysis.In this work,we fabricated hierarchical porous nitrogen-doped carbon nanofibers with atomically dispersed Fe-N4 sites by carbonization of electrospinning iron-based metal-organic frameworks(MOFs)/polyacrylonitrile nanofibers for ORR electrocatalysis.Remarkably,the re sultant carbon nanofibers with atomically dispersed FeN4 sites exhibit extraordinary electrochemical performance with an onset potential of 0.994 V and a halfwave potential of 0.876 V in alkaline electrolyte,comparable to the benchmark commercial Pt/C catalyst.The high catalytic performance is originated from the unique hierarchically porous 1 D carbon structure and abundant highly active atomically dispersed Fe-N4 sites.

关键词： Atomically dispersed metal sites Metal-organic frameworks Electrospinning Oxygen reduction reaction Electrocatalysis

Highly efficient K-Fe/C catalysts derived from metal-organic frameworks towards ammonia synthesis

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Nano Research 2019年第9期12卷 2341-2347页

作者： Pengqi Yan Wenhan Guo zibin liang Wei Meng Zhen Yin Siwei Li Mengzhu Li Mengtao Zhang Jie Yan Dequan Xiao Ruqiang Zou Ding Ma Beijing National Laboratory for Molecular Sciences College of Chemistry and Molecular Engine ering and College of Engineeringand BIC-ESATPeking UniversityBeijing 100871China Beijing Key Laboratory for Theory and Technology of Advanced Battery Materials Department of Materials Science and EngineeringCollege of EngineeringPeking UniversityBeijing 10087China State Key Laboratory of Separation Membranes and Membrane Processes School of Chemistry and Chemical EngineeringTianjin Polytechnic UniversityTianjin 300387China Department of Chemistry and Chemical Engineering University of New HavenWest HavenCT 06516USA

Fe-based catalysts have been discovered as the best elementary metal-based heterogeneous catalysts for the ammonia synthesis in industrial application during the last century.Herein,a novel and scalable strategy is developed to prepare the K-promoted Fe/C catalyst with extremely high Fe loading (> 50 wt.%) through pyrolysis of the Fe-based metal-organic framework (MOF) xerogel.The obtained K-Fe/C catalysts exhibited superior activity and stability towards ammonia synthesis.The weight-specific reaction rate of Fe/C with K2O as promoter can achieve 12.4 mmol·g-1·h-1 at 350 ℃ and 30.4 mmol·g-1·h-1 at 400 ℃,approximately four and two times higher than that of the commercial fused-iron catalyst (3.4 mmol·g-1·h-1 at 350 ℃ and 16.7 mmol·g-1·h-1 at 400 ℃) under the same condition,respectively.The excellent performance of K-Fe/C can be ascribed to the inherited structure derived from the metal-organic frame precursors and the promotion of potassium,which can modify the binding energy of reactant molecules on the Fe surface,transfer electrons to iron for effective activation of nitrogen,prevent agglomeration of Fe nanoparticle (NPs) and restrain side reaction of carbon matrix to methane.

关键词： metal-orga nic frameworks pyrolysis ammonia syn thesis ir on nano particles K promotion

Probabilistic-Ellipsoid Hybrid Reliability Multi-Material Topology Optimization Method Based on Stress Constraint

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Computer Modeling in Engineering & Sciences 2024年第7期140卷 757-792页

作者： zibin Mao Qinghai Zhao liang Zhang College of Mechanical and Electrical Engineering Qingdao UniversityQingdao266071China National Engineering Research Center for Intelligent Electrical Vehicle Power System Qingdao UniversityQingdao266071China

This paper proposes a multi-material topology optimization method based on the hybrid reliability of the probability-ellipsoid model with stress constraint for the stochastic uncertainty and epistemic uncertainty of mechanical loads in optimization design.The probabilistic model is combined with the ellipsoidal model to describe the uncertainty of mechanical loads.The topology optimization formula is combined with the ordered solid isotropic material with penalization(ordered-SIMP)multi-material interpolation model.The stresses of all elements are integrated into a global stress measurement that approximates the maximum stress using the normalized p-norm function.Furthermore,the sequential optimization and reliability assessment(SORA)is applied to transform the original uncertainty optimization problem into an equivalent deterministic topology optimization(DTO)problem.Stochastic response surface and sparse grid technique are combined with SORA to get accurate information on the most probable failure point(MPP).In each cycle,the equivalent topology optimization formula is updated according to the MPP information obtained in the previous cycle.The adjoint variable method is used for deriving the sensitivity of the stress constraint and the moving asymptote method(MMA)is used to update design variables.Finally,the validity and feasibility of the method are verified by the numerical example of L-shape beam design,T-shape structure design,steering knuckle,and 3D T-shaped beam.

关键词： Stress constraint probabilistic-ellipsoid hybrid topology optimization reliability analysis multi-material design

AstroPose: Astronaut pose estimation using a monocular camera during extravehicular activities

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Science China Technological Sciences 2024年第6期67卷 1933-1945页

作者： LIU zibin LI You WANG ChunHui LIU liang GUAN BangLei SHANG Yang YU QiFeng College of Aerospace Science and Engineering National University of Defense Technology Key Laboratory of Human Factors Engineering China Astronaut Research and Training Center

With the completion of the Chinese space station, an increasing number of extravehicular activities will be executed by astronauts,which is regarded as one of the most dangerous activities in human space exploration. To guarantee the safety of astronauts and the successful accomplishment of missions, it is vital to determine the pose of astronauts during extravehicular activities. This article presents a monocular vision-based pose estimation method of astronauts during extravehicular activities, making full use of the available observation resources. First, the camera is calibrated using objects of known structures, such as the spacesuit backpack or the circular handrail outside the space station. Subsequently, the pose estimation is performed utilizing the feature points on the spacesuit. The proposed methods are validated both on synthetic and semi-physical simulation experiments, demonstrating the high precision of the camera calibration and pose estimation. To further evaluate the performance of the methods in real-world scenarios, we utilize image sequences of Shenzhou-13 astronauts during extravehicular activities. The experiments validate that camera calibration and pose estimation can be accomplished solely with the existing observation resources, without requiring additional complicated equipment. The motion parameters of astronauts lay the technological foundation for subsequent applications such as mechanical analysis, task planning, and ground training of astronauts.

关键词： monocular camera astronaut pose estimation camera calibration