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Identification of Dynamic Active Sites Among Cu Species Derived from MOFs@CuPc for Electrocatalytic Nitrate Reduction Reaction to Ammonia

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Nano-Micro Letters 2023年第8期15卷 20-34页

作者： Xue‑Yang Ji Ke Sun Zhi‑Kun Liu Xinghui Liu Weikang Dong Xintao Zuo ruiwen shao Jun Tao Key Laboratory of Cluster Science of Ministry of Education School of Chemistry and Chemical EngineeringLiangxiang CampusBeijing Institute of TechnologyBeijing 102488People’s Republic of China Department of Chemistry Sungkyunkwan University(SKKU)Suwon 16419Republic of Korea Department of Materials Physics Saveetha School of EngineeringSaveetha Institute of Medical and Technical Sciences(SIMTS)ThandalamChennaiTamilnadu 602105India Beijing Advanced Innovation Center for Intelligent Robots and Systems and Institute of Engineering Medicine Beijing Institute of TechnologyBeijing 100081People’s Republic of China Key Laboratory of Bio‑inspired Smart Interfacial Science and Technology of Ministry of Education School of ChemistryBeihang UniversityBeijing 100191People’s Republic of China

Direct electrochemical nitrate reduction reaction(NITRR)is a promising strategy to alleviate the unbalanced nitrogen cycle while achieving the electrosynthesis of ammonia.However,the restructuration of the high-activity Cu-based electrocatalysts in the NITRR process has hindered the identification of dynamical active sites and in-depth investigation of the catalytic mechanism.Herein,Cu species(single-atom,clusters,and nanoparticles)with tunable loading supported on N-doped TiO_(2)/C are successfully manufactured with MOFs@CuPc precursors via the pre-anchor and post-pyrolysis strategy.Restructuration behavior among Cu species is co-dependent on the Cu loading and reaction potential,as evidenced by the advanced operando X-ray absorption spectroscopy,and there exists an incompletely reversible transformation of the restructured structure to the initial state.Notably,restructured CuN_(4)&Cu_(4) deliver the high NH_(3) yield of 88.2 mmol h^(−1)g_(cata)^(−1) and FE(~94.3%)at−0.75 V,resulting from the optimal adsorption of NO_(3)^(−) as well as the rapid conversion of^(*)NH_(2)OH to^(*)NH_(2) intermediates originated from the modulation of charge distribution and d-band center for Cu site.This work not only uncovers CuN_(4)&Cu_(4) have the promising NITRR but also identifies the dynamic Cu species active sites that play a critical role in the efficient electrocatalytic reduction in nitrate to ammonia.

关键词： Metal-organic frameworks Copper phthalocyanine Electrocatalytic nitrate reduction reaction

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Orderly defective superstructure for enhanced pseudocapacitive storage in titanium niobium oxide

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Nano Research 2022年第2期15卷 1570-1578页

作者： Le Yang Jinfeng Zeng Lei Zhou ruiwen shao Wellars Utetiwabo Muhammad Khurram Tufail Saisai Wang Wen Yang Jiatao Zhang Key Laboratory of Cluster Science of Ministry of Education Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion MaterialsSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081China Beijing Advanced Innovation Center for Intelligent Robots and Systems and Institute of convergence in medicine and engineering Beijing institute of technologyBeijing 100081China Key Laboratory of Active Components of Xinjiang Natural Medicine and Drug Release Technology School of PharmacyXinjiang Medical UniversityUrumqi 830011China

Artificial defect engineering in transition metal oxides is of important terms for numerous applications.In the present work,we proposed an in-situ gas reduction strategy to introduce ordered defects into titanium niobium oxide embedding on vapor grew carbon fibers(Ti_(2)Nb_(10)O_(29-x)@VGCFs).High-resolution transmission electron microscopy(HRTEM)and fast Fourier transform(FFT)simulation indicate that the ordered oxygen defects locate at interval layers,which leads to a new superstructure in Ti_(2)Nb_(10)O_(29).The ordered defects could provide extra active sites for lithium-ion storage and modulate ionic migration,resulting an enhanced pseudocapacitive performance.In addition,the excellent structural stability of the superstructure was proved by in-situ HRTEM under a harsh electrochemical process.Our work provides a directly observation of orderly defective superstructure in transition metal oxide,and its functionality on electrochemistry was revealed.

关键词： Ti_(2)Nb_(10)O_(29) in-situ gas reduction ordered defect lithium-ion hybrid capacitor pseudocapacitance

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A Planar 4-Bit Reconfigurable Antenna Array Based on the Design Philosophy of Information Metasurfaces

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Engineering 2022年第10期17卷 64-74页

作者： Zheng Xing Wang Hanqing Yang ruiwen shao Jun Wei Wu Guobiao Liu Feng Zhai Qiang Cheng Tie Jun Cui State Key Laboratory of Millimeter Waves School of Information Science and EngineeringSoutheast UniversityNanjing 210096China The Institute of Electromagnetic Space Southeast UniversityNanjing 210096China

Inspired by the design philosophy of information metasurfaces based on the digital coding concept,a planar 4-bit reconfigurable antenna array with low profile of 0.15λ0(whereλ0is the free-space wavelength)is presented.The array is based on a digital coding radiation element consisting of a 1-bit magnetoelectric(ME)dipole and a miniaturized reflection-type phase shifter(RTPS).The proposed 1-bit ME dipole can provide two digital states of"0"and"1"(with 0°and 180°phase responses)over a wide frequency band by individually exciting its two symmetrical feeding ports.The designed RTPS is able to realize a relative phase shift of 173°.By digitally quantizing its phase in the range of 157.5°,additional eight digital states at intervals of 22.5°are obtained.To achieve low sidelobe levels,a 1:16 power divider based on the Taylor line source method is employed to feed the array,A prototype of the proposed 4-bit antenna array has been fabricated and tested,and the experimental results are in good agreement with the simulations.Scanning beams within a±45°range were measured with a maximum realized gain of 13.4 dBi at12 GHz.The sidelobe and cross-polarization levels are below-14.3 and-23.0 dB,respectively.Furthermore,the beam pointing error is within 0.8°,and the 3 dB gain bandwidth of the broadside beam is 25%.Due to its outstanding performance,the array holds potential for significant applications in radar and wireless communication systems.

关键词： 4-bit reconfigurable antenna array Information metasurface Digital coding method Low sidelobe Low profile

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Vapor phase epitaxy of PbS single-crystal films on water-soluble substrates and application to photodetectors

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Nano Research 2022年第6期15卷 5402-5409页

作者： Yifan Wang Jing Xia Xuanze Li Fan Ru Xue Chen Ze Hua ruiwen shao Xuecong Wang Wenjun Zhang Chun-Sing Lee Xiangmin Meng Key Laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190China Institute of Process Engineering Chinese Academy of SciencesBeijing 100190China Centre of Material Science and Optoelectronic Engineering University of Chinese Academy of SciencesBeijing 10049China Engineering Research Center for Semiconductor Integrated Technology Institute of SemiconductorsChinese Academy of SciencesBeijing 100083China Analysis&Testing Center Beijing Institute of TechnologyBeijing 102488China Beijing Advanced Innovation Center for Intelligent Robots and Systems and Institute of Convergence in Medicine and Engineering Beijing Institute of TechnologyBeijing 100081China Center of Super-Diamond and Advanced Films(COSADF)and Department of Materials Science and Engineering City University of Hong KongHong KongChina Center of Super-Diamond and Advanced Films(COSDAF)and Department of Chemistry City University of Hong KongHong KongChina

Lead sulfide(PbS),a typical functional semiconductor material,has attracted serious attention due to its great potential in optoelectronics applications.However,controllable growth of PbS single-crystal film still remains a great challenge.Here,we report heteroepitaxial growth of large-scale highly crystalline PbS films on alkali salt(NaCl and KCl)substrates via chemical vapor deposition(CVD).Structural characterizations demonstrate that the as-grown PbS films exhibit an atomically sharp interface with the underlying substrates.The epitaxial relationships between the epilayers and substrates were determined to be PbS(100)//NaCl(100)or KCl(100),PbS[010]//NaCl[010]or KCl[010].Owing to the high solubility of alkali salt,the epitaxial PbS films can be rapidly released from the underlying substrates and transferred to other substrates of interest while maintaining good integrity and crystallinity,the process of which is particularly attractive in the fields of electronics and optoelectronics.Furthermore,photodetectors based on the transferred PbS films were fabricated,exhibiting a high photoresponsivity of 7.5 A/W,a detectivity of 1.44×10^(12)Jones,and a rapid response time of approximately 0.25 s.This work sheds light on the batch production,green transfer,and optoelectronic application of PbS films.

关键词： heteroepitaxial growth lead sulfide(PbS) single-crystal film photodetector transferable

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In situ TEM revealing the effects of dislocations on lithium-ion migration in transition metal dichalcogenides

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Journal of Energy Chemistry 2021年第7期30卷 280-284页

作者： ruiwen shao Chengkai Yang Chen Yang Shulin Chen Weikang Dong Bairong Li Xiumei Ma Jing Lu Lixin Dong Peng Gao Dapeng Yu Beijing Advanced Innovation Center for Intelligent Robots and Systems and Institute of Convergence in Medicine and Engineering Beijing Institute of TechnologyBeijing 100081China Electron Microscopy Laboratory School of PhysicsPeking UniversityBeijing 100871China College of Materials Science and Engineering Fuzhou UniversityFuzhou 350108FujianChina State Key Laboratory for Artiﬁcial Microstructure&Mesoscopic Physics School of PhysicsPeking UniversityBeijing 100871China Analysis and Testing Center Beijing Institute of TechnologyBeijing 100081China Collaborative Innovation Center of Quantum Matter Beijing 100871China Department of Biomedical Engineering City University of Hong KongHong KongChina International Center for Quantum Materials School of PhysicsPeking UniversityBeijing 100871China Department of Physics South University of Science and Technology of ChinaShenzhen 518055GuangdongChina

The two-dimensional (2D) structure of layered transition metal dichalcogenides (TMDs) provides unusual physical properties [1,2]and chemical reactivity [3,4], which can be influenced by defects such as dislocations [5,6]. For example, dislocations can act as nucleation sites for the onset of deformation when subjected to stress [7].

关键词： Batteries Defect Structure–property relationships Electrodes Transition metal dichalcogenides

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Non-Hermitian Skin Effect in a Non-Hermitian Electrical Circuit

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Research 2021年第1期2021卷 277-285页

作者： Shuo Liu ruiwen shao shaojie Ma Lei Zhang Oubo You Haotian Wu Yuan Jiang Xiang Tie Jun Cui Shuang Zhang School of Physics and Astronomy University of BirminghamBirmingham B152TTUK State Key Laboratory of Millimeter Waves Southeast UniversityNanjing 210096China School of Physics and Electronics Hunan UniversityChangsha 410082China

The conventional bulk-boundary correspondence directly connects the number of topological edge states in a finite system with the topological invariant in the bulk band structure with periodic boundary condition(PBC).However,recent studies show that this principle fails in certain non-Hermitian systems with broken reciprocity,which stems from the non-Hermitian skin effect(NHSE)in the finite system where most of the eigenstates decay exponentially from the system boundary.In this work,we experimentally demonstrate a 1D non-Hermitian topological circuit with broken reciprocity by utilizing the unidirectional coupling feature of the voltage follower module.The topological edge state is observed at the boundary of an open circuit through an impedance spectra measurement between adjacent circuit nodes.We confirm the inapplicability of the conventional bulk-boundary correspondence by comparing the circuit Laplacian between the periodic boundary condition(PBC)and open boundary condition(OBC).Instead,a recently proposed non-Bloch bulk-boundary condition based on a non-Bloch winding number faithfully predicts the number of topological edge states.

关键词： topological boundary system

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In situ atomic-scale observation of size-dependent (de) potassiation and reversible phase transformation in tetragonal FeSe anodes

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InfoMat 2023年第1期5卷 161-171页

作者： Ran Cai Lixia Bao Wenqi Zhang Weiwei Xia Chunhao Sun Weikang Dong Xiaoxue Chang Ze Hua ruiwen shao Toshio Fukuda Zhefei Sun Haodong Liu Qiaobao Zhang Feng Xu Lixin Dong Beijing Advanced Innovation Center for Intelligent Robots and Systems School of Medical TechnologyBeijing Institute of TechnologyBeijingPeople's Republic of China Analysis&Testing Center Beijing Institute of TechnologyBeijingPeople's Republic of China Department of Biomedical Engineering City University of Hong KongHong KongPeople's Republic of China Shaanxi Materials Analysis and Research Center School of Materials Science and EngineeringNorthwestern Polytechnical UniversityXi'anPeople's Republic of China School of Environmental and Safety Engineering North University of ChinaTaiyuanPeople's Republic of China Department of Materials Science and Engineering College of MaterialsXiamen UniversityXiamenFujianPeople's Republic of China Department of Nanoengineering University of California San DiegoLa JollaCaliforniaUSA SEU-FEI Nano-Pico Center Key Laboratory of MEMS of Ministry of EducationSoutheast UniversityNanjingPeople's Republic of China

Potassium-ion batteries(PIBs)are considered promising alternatives to lithium-ion batteries owing to cost-effective potassium resources and a suitable redox potential of-2.93 V(vs.-3.04 V for Li+/Li).However,the exploration of appro-priate electrode materials with the correct size for reversibly accommodating large K+ions presents a significant challenge.In addition,the reaction mecha-nisms and origins of enhanced performance remain elusive.Here,tetragonal FeSe nanoflakes of different sizes are designed to serve as an anode for PIBs,and their live and atomic-scale potassiation/depotassiation mechanisms are revealed for the first time through in situ high-resolution transmission electron micros-copy.We found that FeSe undergoes two distinct structural evolutions,sequen-tially characterized by intercalation and conversion reactions,and the initial intercalation behavior is size-dependent.Apparent expansion induced by the intercalation of K+ions is observed in small-sized FeSe nanoflakes,whereas unexpected cracks are formed along the direction of ionic diffusion in large-sized nanoflakes.The significant stress generation and crack extension originating from the combined effect of mechanical and electrochemical interactions are elucidated by geometric phase analysis and finite-element analysis.Despite the different intercalation behaviors,the formed products of Fe and K_(2)Se after full potassiation can be converted back into the original FeSe phase upon depotassiation.In particular,small-sized nanoflakes exhibit better cycling perfor-mance with well-maintained structural integrity.This article presents the first successful demonstration of atomic-scale visualization that can reveal size-dependent potassiation dynamics.Moreover,it provides valuable guidelines for optimizing the dimensions of electrode materials for advanced PIBs.

关键词： elucidated by geometric phase analysis and finite-element analysis. Despite the different intercalation behaviors the formed products of Fe and K 2 Se after full potassiation can be converted back into the original FeSe phase upon depotassiation. In particular small-sized nanoflakes exhibit better cycling perfor- mance with well-maintained structural integrity. This article presents the first successful demonstration of atomic-scale visualization that can reveal size- dependent potassiation dynamics. Moreover it provides valuable guidelines for optimizing the dimensions of electrode materials for advanced PIBs. KEYWOR DS in situ transmission electron microscopy potassium-ion batteries potassium-ion storage mechanism size-dependent effects tetragonal FeSe

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Sb_(2)Se_(3)单晶中的各向异性锂离子迁移和电化学-力学耦合

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Science China Materials 2022年第10期65卷 2657-2664页

作者：孙春浩董伟康杨乐左鑫涛暴丽霞华泽常晓雪蔡然陈浩森韩晓东何洋刘天生邵瑞文董立新 School of Environmental and Safety Engineering North University of ChinaTaiyuan 030051China Beijing Advanced Innovation Center for Intelligent Robots and Systems School of Medical TechnologyBeijing Institute of TechnologyBeijing 100081China Beijing Key Laboratory of Lightweight Multi-Functional Composite Materials and Structures Institute of Advanced Structure TechnologyBeijing Institute of TechnologyBeijing 100081China Analysis&Testing Center Beijing Institute of TechnologyBeijing 100081China Beijing Key Laboratory of Microstructure and Property of Advanced Materials Beijing University of TechnologyBeijing 100124China Beijing Advanced Innovation Center for Materials Genome Engineering School of Materials Science and EngineeringUniversity of Science and Technology BeijingBeijing 100083China Department of Biomedical Engineering City University of Hong KongHong KongChina

高能量密度的锂离子电池先进电极材料的开发,依赖于对材料在电池循环中的运行和失效机制的理解.本文使用原位高分辨TEM技术跟踪了Sb_(2)Se_(3)单晶锂化/脱锂过程中的相变,并揭示了反应界面处的电化学-力学耦合.这种电化学-力学耦合效应... 详细信息

高能量密度的锂离子电池先进电极材料的开发,依赖于对材料在电池循环中的运行和失效机制的理解.本文使用原位高分辨TEM技术跟踪了Sb_(2)Se_(3)单晶锂化/脱锂过程中的相变,并揭示了反应界面处的电化学-力学耦合.这种电化学-力学耦合效应对锂化动力学具有复杂的相互作用,并在反应前端引起各种类型的缺陷,包括位错对、反相边界和裂纹.另一方面,形成的裂缝和相关缺陷为锂离子的快速扩散开辟了道路,并在扭曲的反应前沿引发高度各向异性的锂化,从而在无定形Li_(x)Sb_(2)Se_(3)中形成可能“失效”的Sb_(2)Se_(3)畴.我们对Sb_(2)Se_(3)电化学过程机理的详细研究有助于更合理地设计和制备高容量电极材料.

关键词：锂离子电池电极材料锂化电化学过程各向异性高能量密度失效机制反应界面

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Ag掺杂对Ge2 Sb2 Te5结晶行为的影响

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电子显微学报 2014年第1期33卷 1-6页

作者：张滔郑坤张斌邵瑞文韩晓东张泽北京工业大学固体微结构与性能研究所北京100124 浙江大学电镜中心材料科学与工程学系浙江杭州310027

通过磁控溅射仪制备了Ge2Sb2Te5(GST)和Ag10.6(GST)89.4薄膜,利用X射线衍射(XRD)、电阻-温度(RT)测试、透射电子显微学以及径向分布函数(RDF)等方法对比研究了GST和Ag10.6(GST)89.4的结晶过程和微观结构及其演化的差异。发现掺Ag的薄膜... 详细信息

通过磁控溅射仪制备了Ge2Sb2Te5(GST)和Ag10.6(GST)89.4薄膜,利用X射线衍射(XRD)、电阻-温度(RT)测试、透射电子显微学以及径向分布函数(RDF)等方法对比研究了GST和Ag10.6(GST)89.4的结晶过程和微观结构及其演化的差异。发现掺Ag的薄膜非晶态、晶态电阻均比GST更高,而且结晶过程只有非晶相到面心立方相(fcc)的转变,没有出现GST的非晶到fcc再到六方相(hcp)的过程,XRD分析进一步证实了这一结果。同时,透射电镜原位加热实验证实了在300℃时,Ag10.6(GST)89.4仍然保持着fcc结构,而GST中已经出现了hcp相。通过统计230℃下时效处理的晶态薄膜的晶粒尺寸,发现Ag10.6(GST)89.4的平均晶粒尺寸小于Ge2Sb2Te5薄膜的,这可能是造成其晶态电阻高于GST的主要原因。

关键词： Ag掺杂相变材料磁控溅射透射电镜

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透射电镜电学测试样品杆与扫描电镜联合系统的搭建

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电子显微学报 2016年第4期35卷 287-292页

作者：矫丽丽郑坤王晋高攀邵瑞文张跃飞韩晓东张泽北京工业大学固体微结构与性能研究所北京100124 浙江大学电子显微镜中心材料科学与工程学院浙江杭州310027

透射电子显微镜电学测试样品杆是用于透射电子显微镜中测试样品外场加载下电学性能的专用仪器。本文介绍通过对法兰及其它对接接口的系列设计,使该系统可应用于扫描电子显微镜中。该系列设计改造,能够大大拓展该电学测试系统的应用范围... 详细信息

透射电子显微镜电学测试样品杆是用于透射电子显微镜中测试样品外场加载下电学性能的专用仪器。本文介绍通过对法兰及其它对接接口的系列设计,使该系统可应用于扫描电子显微镜中。该系列设计改造,能够大大拓展该电学测试系统的应用范围。以单根Si纳米线为例,在扫描电子显微镜中利用该电学测试系统实现Si纳米线弯曲变形下电输运性能的研究。

关键词：扫描电镜透射电镜电学性能

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