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Nurturing the marriages of single atoms with atomic clusters and nanoparticles for better heterogeneous electrocatalysis

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Interdisciplinary materials 2022年第1期1卷 51-87页

作者： Lei Zhang Jiawei Zhu Xin Li Shichun Mu Francis Verpoort Junmin Xue Zongkui Kou John Wang Department of Materials Science and Engineering National University of SingaporeSingaporeSingapore State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhanChina School of Physical&Mathematical Sciences Nanyang Technological UniversitySingaporeSingapore

Single-atom catalysts,featuring some of the most unique activities,selectivity,and high metal utilization,have been extensively studied over the past *** their high activity,selectivity,especially towards small molecules or key intermediate conversions,they can be synergized together with other active species(typically other single atoms,atomic clusters,or nanoparticles)in either tandem or parallel or both,leading to much better performance in complex catalytic *** there have been reports on effectively combining the multiple components into one single catalytic entity,the combination and synergy between single atoms and other active species have not been reviewed and examined in a systematic ***,in this overview,the key synergistic interactions,binary complementary effects,and the bifunctional functions of single atoms with other active species are defined and discussed in *** integration functions of their marriages are in-vestigated with particular emphasis on the homogeneous and heterogeneous combinations,spatial distribution,synthetic strategies,and the thus-derived outstanding catalytic performance,together with new light shined on the catalytic mechanisms by zooming in several case *** dynamic nature of each of the active species and in particular their interactions in such new catalytic entities in the heterogeneous electrocatalytic processes are visited,on the basis of the in situ/operando ***,we feature the current chal-lenges and future perspectives of these integrated catalytic entities that can offer guidance for advanced catalyst design by the rational combination and synergy of binary or multiple active species.

关键词： atomic clusters binary/multiple synergy heterogeneous catalysis nanoparticles single atoms

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Tunable Atomic-Scale Steps and Cavities Break Both Stability and Activity Limits of CoO_(x) Nanosheets to Catalyze Oxygen Evolution

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Renewables 2023年第4期1卷 465-473页

作者： Min Yu Xueqin Mu Weitao Meng Ziyue Chen Yu Tong Yu Ge Shiyuan Pang Shengjie Li Suli Liu Shichun Mu Key Laboratory of Advanced Functional Materials of Nanjing Nanjing Xiaozhuang UniversityNanjing 211171 State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070

A highly active interface can enhance the catalytic efficiency of catalysts toward the oxygen evolution reaction(OER).However,accurately tuning their atomic interface configurations of defects with sufficient activity and stability remains a grand ***,we report on breaking the activity and stability limits of CoO_(x) nanosheets in the OER process by constructing copious high-energy atomic steps and cavities,in which S or Ce atoms simultaneously replace O or Co atoms from CoO_(x),thus achieving high-energy atomic interface Ce,O-Co_(3)S_(4) *** combining in situ characterization and density functional theory calculations,it is shown that the unique orbital coupling between Ce-4f,O(S)-2p,and Co-3d causes it to be closer to the Fermi level,leading to faster charge transfer *** importantly,the novel structure breaks the stability limit of cobalt sulfide with planar defects,which gives high catalytic activity and stability in 0.1 M KOH solutions,better than commercial RuO_(2) and IrO_(2) noble metal *** expected,Ce,O-Co_(3)S_(4) possesses much better turnover frequency activity(0.064 s^(-1))at an overpotential of 300 mV,which is ~7 times larger than that of Ce-CoO_(x)(0.009 s^(-1)).Our work presents a new perspective of designing catalysts with atomically dispersed orbital electronic coupling defects toward efficient OER electrocatalysis.

关键词： atomic replacement amorphous structures interface active centers atomic defect oxygen evolution reaction

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具有分级界面的纳米纤维增强聚合物复合材料:用于高温介电储能应用

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Science China materials 2023年第7期66卷 2652-2661页

作者：智佳鹏王建沈忠慧李宝文张鑫南策文 State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Center of Smart Materials and Devices&International School of Materials Science and EngineeringWuhan University of TechnologyWuhan 430070China School of Materials Science and Engineering State Key Lab of New Ceramics and Fine ProcessingTsinghua UniversityBeijing 100084China

陶瓷纳米填料增强的柔性聚合物基复合材料在先进电子电气系统中显示出巨大的储能应用潜力.但如何在高于150℃的条件下提高其能量密度和效率仍然是一个挑战.本文中我们采用氮化硼-钛酸钡(BNBaTiO_(3))非均质纳米纤维作为填料,耐高温的聚... 详细信息

陶瓷纳米填料增强的柔性聚合物基复合材料在先进电子电气系统中显示出巨大的储能应用潜力.但如何在高于150℃的条件下提高其能量密度和效率仍然是一个挑战.本文中我们采用氮化硼-钛酸钡(BNBaTiO_(3))非均质纳米纤维作为填料,耐高温的聚醚酰亚胺(PEI)为基体,使复合材料的介电常数和击穿强度同时提高.分级结构的BN/BaTiO_(3)/PEI界面提升了材料的陷阱密度和能级,可进一步抑制传导损耗.在此基础上,复合材料在150℃,能量效率高于90%时展现出5.23J cm^(-3)的超高能量密度,这是迄今为止纳米纤维增强聚合物复合材料中最高的能量密度.研究表明,分级界面是提高材料高温储能的有效策略,对介电材料在高温下的应用具有重要意义.

关键词： high temperature energy storage dielectrics polymer nanocomposite film capacitor

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Confined nanospace for enhanced photocatalysis

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国家科学评论（英文版） 2021年第3期8卷 3-4页

作者： Bao-Lian Su State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyChina Laboratory of Inorganic Materials Chemistry(CMI) University of NamurBelgium

The world today is very different from how it *** consumption rate of fos-sil fuels compared with the available re-sources and the calamity of global warm-ing frighten *** entire planet is at risk,but these are our *** is the cause and so mankind should find sustainable and green energy solutions to satisfy the needs of society.

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Boosting molecular diffusion following the generalized Murray's Law by constructing hierarchical zeolites for maximized catalytic activity

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国家科学评论（英文版） 2022年第12期9卷 143-156页

作者： Ming-Hui Sun Shu-Shu Gao Zhi-Yi Hu Tarek Barakat Zhan Liu Shen Yu Jia-Min Lyu Yu Li Shu-Tao Xu Li-Hua Chen Bao-Lian Su State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Laboratory of Inorganic Materials Chemistry(CMI) University of NamurNamur B-5000Belgium Division of Analysis Sinopec Beijing Research Institute of Chemical IndustryBeijing 100013China National Engineering Laboratory for Methanol to Olefins Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Nanostructure Research Centre Wuhan University of TechnologyWuhan 430070China Laboratory of Inorganic Materials Chemistry(CMI) University of NamurNamur B-5000Belgium State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China National Engineering Laboratory for Methanol to Olefins Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China

Diffusion is an extremely critical step in zeolite catalysis that determines the catalytic performance,in particular for the conversion of bulky *** interconnected mesopores and macropores into a single microporous zeolite with the rationalized pore size at each level is an effective strategy to suppress the diffusion limitations,but remains highly challenging due to the lack of rational design ***,we demonstrate the first example of boosting molecular diffusion by constructing hierarchical Murray zeolites with a highly ordered and fully interconnected macro-meso-microporous structure on the basis of the generalized Murray's *** a hierarchical Murray zeolite with a refined quantitative relationship between the pore size at each length scale exhibited 9 and 5 times higher effective diffusion rates,leading to 2.5 and 1.5 times higher catalytic performance in the bulky 1,3,5-triisopropylbenzene cracking reaction than those of microporous ZSM-5 and ZSM-5 nanocrystals,*** concept of hierarchical Murray zeolites with optimized structural features and their design principles could be applied to other catalytic reactions for maximized performance.

关键词： catalytic cracking generalized Murray's Law hierarchical Murray structure ordered porous hierarchy zeolites

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Metal-organic frameworks enable broad strategies for lithium-sulfur batteries

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National Science Review 2021年第12期8卷 104-121页

作者： Cheng Zhou Zhaohuai Li Xu Xu Liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology International Schoo of Materials Science and Engineering Wuhan University of Technology Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory

The lithium-sulfur(Li-S) battery is considered to be a potential next-generation power battery system,however, it is urgent that suitable materials are found in order to solve a series of challenges, such as the shuttle effect and lithium dendrite growth. As a multifunctional porous material, metal-organic frameworks(MOFs) can be used in different parts of Li-S batteries. In recent years, the application of MOFs in Li-S batteries has been developed rapidly. This review summarizes the milestone works and recent advances of MOFs in various aspects of Li-S batteries, including cathode, separator and electrolyte. The factors affecting the performance of MOFs and the working mechanisms of MOFs in these different parts are also discussed in detail. Finally, the opportunities and challenges for the application of MOFs in Li-S batteries are proposed. We also put forward feasible solutions to related problems. This review will provide better guidance for the rational design of novel MOF-based materials for Li-S batteries.

关键词： metal-organic frameworks lithium-sulfur batteries cathode separator electrolyte

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Wet-milling synthesis of immobilized Pt/Ir nanoclusters as promising heterogeneous catalysts

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Nano Research 2022年第4期15卷 3065-3072页

作者： Peng Du Kai Huang Xiaoyuan Fan Jingteng Ma Naveed Hussain Ruyue Wang Bohan Deng Binghui Ge Haolin Tang Ru Zhang Ming Lei Hui Wu State Key Laboratory of Information Photonics and Optical Communications&School of Science Beijing University of Posts and TelecommunicationsBeijing 100876China State Key Laboratory of New Ceramics and Fine Processing School of Materials Science and EngineeringTsinghua UniversityBeijing 100084China Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 610054China Institutes of Physical Science and Information Technology Anhui UniversityHefei 230601China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China

Being a typical state of the art heterogeneous catalyst,supported noble metal catalyst often demonstrates enhanced catalytic ***,a facile synthetic method for realizing large-scale and low-cost supported noble metal catalyst is strictly *** this end,by making use of the strong metal-support interaction(SMSI)and mechanochemical reaction,we introduce an efficient synthetic route to obtain ultrafine Pt and Ir nanoclusters immobilized on diverse substrates by wet chemical *** further demonstrate the scaling-up effect of our approach by large-scale ball-milling production of Pt nanoclusters immobilized on TiO_(2)*** synthesized Pt/Ir@Co_(3)O_(4)catalysts exhibit superior oxygen evolution reaction(OER)performance with only 230 and 290 mV overpotential to achieve current density of 10 and 100 mA·cm^(-2),beating the catalytic performance of Co_(3)O_(4)supported Pt or Ir clusters and commercial Ir/*** is envisioned that the present work strategically directs facile ways for fabricating supported noble metal heterogeneous catalysts.

关键词： heterogeneous catalysts metal clusters wet milling large-scale production strong metal–support interaction

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Rechargeable metal(Li, Na, Mg, Al)-sulfur batteries: materials and advances

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Journal of Energy Chemistry 2021年第10期30卷 104-134,I0004页

作者： Xue Liu Yan Li Xu Xu Liang Zhou Liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing International School of Materials Science and EngineeringWuhan University of TechnologyWuhan 430070HubeiChina Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Xianhu Hydrogen ValleyFoshan 528200GuangdongChina

Energy and environmental issues are becoming more and more severe and renewable energy storage technologies are vital to solve the *** metal(Li,Na,Mg,Al)-sulfur batteries with low-cost and earth-abundant elemental sulfur as the cathode are attracting more and more interest for electrical energy storage in recent ***-sulfur(Li-S),room-temperature sodium-sulfur(RT Na-S),magnesium-sulfur(Mg-S)and aluminum-sulfur(Al-S)batteries are the most prominent candidates among *** obvious obstacles are hampering the developments of metal-sulfur ***-S and Na-S batteries are encumbered mainly by anode dendrite issues,polysulfides shuttle and low conductivity of ***-S and Al-S batteries are short of suitable *** this review,relationships between various employed nanostructured materials and electrochemical performances of metal-sulfur batteries have been ***,the selections of suitable electrolytes,anode protection,separator modifications and prototype innovations are all crucial to the developments of metal-sulfur batteries and are discussed at the same ***,we give a review on the advances of Li-S,RT Na-S,Mg-S and Al-S batteries from the point of view of materials,and then focus on perspectives of their future developments.

关键词： Lithium sulfur batteries Sodium sulfur batteries Magnesium sulfur batteries Aluminum sulfur batteries Energy materials

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Deep learning-enhanced NIR-II fluorescence volumetric microscopy for dynamic 3D vascular imaging

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Journal of Innovative Optical Health Sciences 2025年第3期18卷 154-164页

作者： Shiyi Peng Yuhuang Zhang Xuanjie Mou Tianxiang Wu Mingxi Zhang Jun Qian State Key Laboratory of Extreme Photonics and Instrumentation International Research Center for Advanced PhotonicsCentre for Optical and Electromagnetic ResearchCollege of Optical Science and EngineeringZhejiang UniversityHangzhou 310058P.R.China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070P.R.China

Three-dimensional (3D) visualization of dynamic biological processes in deep tissue remains challenging due to the trade-off between temporal resolution and imaging depth. Here, we present a novel near-infrared-II (NIR-II, 900–1880nm) fluorescence volumetric microscopic imaging method that combines an electrically tunable lens (ETL) with deep learning approaches for rapid 3D imaging. The technology achieves volumetric imaging at 4.2 frames per second (fps) across a 200 μm depth range in live mouse brain vasculature. Two specialized neural networks are utilized: a scale-recurrent network (SRN) for image enhancement and a cerebral vessel interpolation (CVI) network that enables 16-fold axial upsampling. The SRN, trained on two-photon fluorescence microscopic data, improves both lateral and axial resolution of NIR-II fluorescence wide-field microscopic images. The CVI network, adapted from video interpolation techniques, generates intermediate frames between acquired axial planes, resulting in smooth and continuous 3D vessel reconstructions. Using this integrated system, we visualize and quantify blood flow dynamics in individual vessels and are capable of measuring blood velocity at different depths. This approach maintains high lateral resolution while achieving rapid volumetric imaging, and is particularly suitable for studying dynamic vascular processes in deep tissue. Our method demonstrates the potential of combining optical engineering with artificial intelligence to advance biological imaging capabilities.

关键词： NIR-II fluorescence bioimaging volumetric microscopy deep learning reconstruction dynamic vascular imaging

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Interdisciplinary exploration between magnetism and thermoelectricity

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Science Bulletin 2022年第9期67卷 891-894,M0003页

作者： Cuncheng Li Wenyu Zhao Qingjie Zhang State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China

Thermoelectrics have important applications in power generation and refrigeration through the direct energy conversion between heat and *** performance of thermoelectric(TE)materials can be qualified by dimensionless figure of merit ZT=σa2/κ,whereσ,a andκare the electrical conductivity,Seebeck coefficient and thermal conductivity,respectively.

关键词： conductivity Seebeck electrical

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