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Rare Earth Single-Atom Catalysis for High-Performance Li−S Full Battery with Ultrahigh Capacity

Angewandte Chemie 2024年第31期136卷

作者： Rong Zhou Yongqiang Ren Weixin Li Meng Guo Yinan Wang Haixin Chang Xin Zhao Wei Hu Guowei Zhou Shaonan Gu Key Laboratory of Fine Chemicals in Universities of Shandong Jinan Engineering Laboratory for Multi-scale Functional Materials School of Chemistry and Chemical Engineering Qilu University of Technology (Shandong Academy of Sciences) Jinan 250353 China State Key Laboratory of Material Processing and Die & Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan 430074 China State Key Laboratory of Biobased Material and Green Parking Qilu University of Technology (Shandong Academy of Sciences) Jinan 250353 China

Lithium-sulfur (Li−S) batteries have many advantages but still face problems such as retarded polysulfides redox kinetics and Li dendrite growth. Most reported single atom catalysts (SACs) for Li−S batteries are based on d -band transition metals whose d orbital constitutes active valence band, which is inclined to occur catalyst passivation. SACs based on 4 f inner valence orbital of rare earth metals are challenging for their great difficulty to be activated. In this work, we design and synthesize the first rare earth metal Sm SACs which has electron-rich 4 f inner orbital to promote catalytic conversion of polysulfides and uniform deposition of Li. Sm SACs enhance the catalysis by the activated 4 f orbital through an f-d-p orbital hybridization. Using Sm-N 3 C 3 modified separators, the half cells deliver a high capacity over 600 mAh g −1 and a retention rate of 84.3 % after 2000 cycles. The fabricated Sm-N 3 C 3 -Li|Sm-N 3 C 3 @PP|S/CNTs full batteries can provide an ultra-stable cycling performance of a retention rate of 80.6 % at 0.2 C after 100 cycles, one of the best full Li−S batteries. This work provides a new perspective for the development of rare earth metal single atom catalysis in electrochemical reactions of Li−S batteries and other electrochemical systems for next-generation energy storage.

关键词： rare earth element single atom catalyst polysulfides catalysis Li−S full batteries

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Chemical-Reductant-Free Electrochemical Deuteration Reaction using Deuterium Oxide

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Angewandte Chemie 2020年第33期132卷 14066-14071页

作者： Liu X. Liu R. Qiu J. Cheng X. Li G. Institute of Chemistry and Biomedical Sciences Jiangsu Key Laboratory of Advanced Organic Materials School of Chemistry and Chemical Engineering National Demonstration Center for Experimental Chemistry Education Nanjing University Nanjing 210023 China State Key Laboratory Breeding Base of Green Chemistry-Synthesis Technology Zhejiang University of Technology Hangzhou 310032 China Department of Chemistry and Biochemistry Texas Tech University Lubbock TX United States

We report a method for the electrochemical deuteration of α,β-unsaturated carbonyl compounds under catalyst- and external-reductant-free conditions, with deuteration rates as high as 99 % and yields up to 91 % in 2 h. The use of graphite felt for both the cathode and the anode was key to ensuring chemoselectivity and high deuterium incorporation under neutral conditions without the need for an external reductant. This method has a number of advantages over previously reported deuteration reactions that use stoichiometric metallic reductants. Mechanistic experiments showed that O2 evolution at the anode not only eliminates the need for an external reductant but also regulates the pH of the reaction mixture, keeping it approximately neutral. © 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

关键词： D2O deuteration electrochemistry graphite felt oxygen evolution

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Microstructure evolution and mechanical properties of Cu-0.36Be-0.46Co alloy fabricated by heating-cooling combined mold horizontal continuous casting during cold rolling

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Transactions of Nonferrous Metals Society of China 2020年第4期30卷 958-971页

作者： Yan-bin JIANG Tong-tong ZHANG Yu LEI Xin-hua LIU Yang CAO Jian-xin XIE Bing ZHAO Yong-hua LI Chuan-rong JIAO School of Materials Science and Engineering Central South UniversityChangsha 410083China Key Laboratory for Advanced Materials Processing(MOE) University of Science and Technology BeijingBeijing 100083China East Nonferrous Metal Corporation Ningxia Shizuishan 753000China Centra Research Institute of BYD Company Shenzhen 518118China

Cu-0.36 wt.%Be-0.46 wt.%Co alloy plate with 300 mm in width and 10 mm in thickness prepared by heating-cooling combined mold(HCCM) horizontal continuous casting was cold rolled. Microstructure evolution and mechanical properties of the alloy as well as its deformation mechanism were investigated. The results showed that the as-cast alloy plate had columnar grains along the length direction, good surface quality and elongation of 35%, which was directly large-reduction cold rolled without surface treatment, and the accumulative cold rolling reduction reached 98%. When the reduction was small(20%), numerous dislocations and dislocation cells formed, and the deformation mechanism was dislocation slip. When the reduction was 40%, deformation twins appeared, and interactions between twins and dislocation cells induced strip-like dislocation cells. When the reduction exceeded 60%, shear bands formed and apparent crystal rotation in the micro-region happened. Further increasing the reduction, the amount of the shear bands rose and they interacted with each other, which refined the grains apparently. The tensile strength and hardness increased from 353 MPa and HV 119 of the as-cast alloy to 625 MPa and HV 208 with 95% reduction, respectively, and the elongation reduced from 35% to 7.6%. A process of HCCM horizontal continuous casting-cold rolling can work as a novel compact method to fabricate Cu-Be alloy sheet.

关键词： HCCM horizontal continuous casting copper-beryllium alloy rolling microstructure mechanical properties

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Fractional Modeling and Dynamic Analysis of Two Kinds of Viscoelastic Thin Plates with Gaussian White Noise

SSRN

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SSRN 2023年

作者： Deng, Jinna Liu, Qiumei Yang, Aimin Chen, Yiming College of Science North China University of Science and Technology Tangshan063210 China Hebei Key Laboratory of Data Science and Application North China University of Science and Technology Tangshan063210 China The Key Laboratory of Engineering Computing in Tangshan City North China University of Science and Technology Tangshan063210 China Tangshan Intelligent Industry and Image Processing Technology Innovation Center North China University of Science and Technology Tangshan063210 China Hebei Engineering Research Center for the Intelligentization of Iron Ore Optimization and Ironmaking Raw Materials Preparation Processes North China University of Science and Technology Tangshan063210 China School of Science Yanshan University Qinhuangdao066004 China LE STUDIUM Loire Valley Institute for Advanced Studies Orléans & Tours Orléans45000 France

According to fractional order model, the governing equation of viscoelastic plate is established. Using the properties of the shifted Bernstein polynomials, the fractional order equation of viscoelastic plate is resolved, the conversion of fractional differential equations to algebraic equations, and operator matrices represented by Kronecker products are solved in the domain. The convergence study validates the algorithm's efficacy and precision in solving differential equations. The displacement of viscoelastic metal thin plate under different external loads (uniform distribution and linear distribution), the effect of white Gaussian noise on the thin metal plate displacement, the effect of different boundary conditions on thin metal plate displacement under harmonic load are studied, the displacements of metal and polymer plates under different loads are contrasted and stress and strain relationship of two kinds of plates are discussed. Based on the outcomes, it can be concluded that the shift Bernstein polynomial approach is useful for numerically simulating viscoelastic plates. © 2023, The Authors. All rights reserved.

关键词： Gaussian noise (electronic)

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Fabrication of silicon nitride Nanowires@Carboxylated carbon nanotubes scaffolds inducing hydroxyapatite plane connection growth for bone defect repair

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Applied Surface Science 2025年 708卷

作者： Lina Sun Leilei Zhang Han Yu Tongtong Cui Yeye Liu Shanshan Ma Hejun Li State Key Laboratory of Solidification Processing Shaanxi Key Laboratory of Fiber Reinforced Light Composite Materials Northwestern Polytechnical University Xi’an 710072 China State Key Laboratory of Metal Matrix Composites School of Materials Science and Engineering Shanghai Jiao Tong University Shanghai 200240 China Institute for Technical Chemistry and Polymer Chemistry (ITCP) Karlsruhe Institute of Technology (KIT) Engesserstraße 18 76131 Karlsruhe Germany

Hydroxyapatite (HA) is an essential inorganic component of bone tissue. However, the low strength and poor stability of HA limit the application in implantable materials. Herein, we report a strategy to fabricate SW@CNT by grafting carbon nanotubes (CNT) on the surface of silicon nitride nanowires (SW). Subsequently, carboxylic groups were introduced to the surface of SW@CNT to form hydrophilic SW@CCNT. Then, the honeycomb-like HA grows in the SW@CCNT network structure in a plane connection pattern to fabricate SW@CCNT/HA, which is similar to the natural bone structure. Specifically, the SW@CCNT network was embedded in SW@CCNT/HA, which enhances the cohesion of SW@CCNT/HA. Meanwhile, the hydrophilic SW@CCNT promotes the HA growth in a plane connection pattern, which effectively enhances the interfacial bonding strength of HA. Compared to SW@CNT/HA, the tensile strength, elastic modulus and elongation of SW@CCNT/HA were increased by 237.75 %, 245.17 %, and 158.65 %, respectively. Moreover, SW@CCNT/HA exhibited 8.26 % higher bone volume fraction and 65.43 % higher bone mineral density than SW@CNT/HA at 12 weeks, indicating significantly enhanced bone regeneration and mineralization capacity. Summarily, the network scaffolds with mechanical strength and bone regeneration properties provided a promising strategy for enhancing HA applied to bone defect repair.

关键词： Tensile strength

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Catalase-powered hollow rod-shaped mesoporous silica nanomotor with targeted effect for smart drug delivery

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materials Today Communications 2025年 46卷

作者： Li, Jiayi Qiu, Yinwei Ke, Ming Wang, Zixiang Qin, Yuchang Luo, Yujie Yu, Feng Li, Yongsheng Yang, Shengchao School of Chemistry and Chemical Engineering Shihezi University Shihezi832003 China State Key Laboratory Incubation Base for Green Processing of Chemical Engineering Shihezi University Shihezi832003 China Lab of Low-Dimensional Materials Chemistry Key Laboratory for Ultrafine Materials of Ministry of Education School of Materials Science and Engineering East China University of Science and Technology Shanghai200237 China

To overcome the problems of low drug loading, poor targeting ability, and low uptake by tumor cells of mesoporous silica nanoparticles (MSN), in this study, hollow rod-shaped mesoporous silica nanoparticles (HRMSN) were successfully synthesized by template method. Through surface modification and linker conjugation, we developed a dual-responsive (pH/H2O2) and folic acid (FA)-targeted nanomotor drug delivery system designated as HRMSN-Catalase-FA. The drug delivery system could autonomously move and exhibit a higher drug loading rate (31.92 %) and easier cellular uptake of doxorubicin (DOX) and can significantly reduce toxic side effects on normal cells. In addition, the lC50 of the drug delivery system against cancer cells decreased from 10.86 µg/mL to 6.08 µg/mL, indicating that the introduction of FA and the presence of H2O2 significantly enhanced the cytotoxicity of the nanosystem on cancer cells. The drug delivery system has potential application prospects in the field of anti-tumor drug delivery, and provides an important reference value for the design of active targeted nanomedicine carriers. © 2025 Elsevier Ltd

关键词： Controlled drug delivery

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Strong and Tough MXene Bridging-induced Conductive Nacre

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Angewandte Chemie 2024年第30期136卷

作者： Jia Yan Dr. Tianzhu Zhou Xinyu Yang Zejun Zhang Lei Li Prof. Zhaoyong Zou Prof. Zhengyi Fu Prof. Qunfeng Cheng School of Chemistry Key Laboratory of Bio-inspired Smart Interfacial Science and Technology of Ministry of Education Beihang University Beijing 100191 P. R. China School of Chemistry and Materials Science University of Science and Technology of China Hefei 230026 P. R. China Suzhou Institute for Advanced Research University of Science and Technology of China Suzhou 215123 P. R. China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 P. R. China Institute of Energy Materials Science (IEMS) University of Shanghai for Science and Technology Shanghai 200093 P. R. China

Nacre is a classic model, providing an inspiration for fabricating high-performance bulk nanocomposites with the two-dimensional platelets. However, the “brick” of nacre, aragonite platelet, is an ideal building block for making high-performance bulk nanocomposites. Herein, we demonstrated a strong and tough conductive nacre through reassembling aragonite platelets with bridged by MXene nanosheets and hydrogen bonding, not only providing high mechanical properties but also excellent electrical conductivity. The flexural strength and fracture toughness of the obtained conductive nacre reach ~282 MPa and ~6.3 MPa m 1/2 , which is 1.6 and 1.6 times higher than that of natural nacre, respectively. These properties are attributed to densification and high orientation degree of the conductive nacre, which is effectively induced by the combined interactions of hydrogen bonding and MXene nanosheets bridging. The crack propagations in conductive nacre are effectively inhibited through crack deflection with hydrogen bonding, and MXene nanosheets bridging between aragonite platelets. In addition, our conductive nacre also provides a self-monitoring function for structural damage and offers exceptional electromagnetic interference shielding performance. Our strategy of reassembling the aragonite platelets exfoliated from waste nacre into high-performance artificial nacre, provides an avenue for fabricating high-performance bulk nanocomposites through the sustainable reutilization of shell resources.

关键词： aragonite platelet MXene mechanical properties electrical conductivity

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Edge supercurrent in Josephson junctions based on topological materials

arXiv

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arXiv 2024年

作者： Qi, Junjie Chen, Chui-Zhen Song, Juntao Liu, Jie He, Ke Sun, Qing-Feng Xie, X.C. Beijing Academy of Quantum Information Sciences Beijing100193 China School of Physical Science and Technology Soochow University Suzhou215006 China Institute for Advanced Study Soochow University Suzhou215006 China College of Physics Hebei Advanced Thin Films Laboratory Hebei Normal University Hebei Shijiazhuang050024 China School of Physics Xi’an Jiaotong University Ministry of Education Key Laboratory for Non-Equilibrium Synthesis and Modulation of Condensed Matter Xi’an710049 China State Key Laboratory of Low Dimensional Quantum Physics Department of Physics Tsinghua University Beijing100084 China Frontier Science Center for Quantum Information Beijing100084 China Hefei National Laboratory Hefei230088 China International Center for Quantum Materials School of Physics Peking University Beijing100871 China Interdisciplinary Center for Theoretical Physcics and Information Sciences Fudan University Shanghai200433 China

The interplay between novel topological states and superconductivity has garnered substantial interest due to its potential for topological quantum computing. The Josephson effect serves as a useful probe for edge superconductivity in these hybrid topological materials. In Josephson junctions based on topological materials, supercurrents exhibit unique quantum interference patterns, including the conventional Fraunhofer oscillations, the Φ0-periodic oscillation, and the 2Φ0-periodic oscillation in response to the external magnetic field (Φ0 = h/2e is the flux quantum, h the Planck constant, and e the electron charge). These interference patterns stem from varied Andreev reflection mechanisms and the associated current density profiles. This review seeks to comprehensively examine the theoretical and experimental advancements in understanding the quantum interference patterns of edge supercurrents in Josephson junctions based on quantum spin Hall, quantum Hall, and quantum anomalous Hall systems. Copyright © 2024, The Authors. All rights reserved.

关键词： Quantum computers

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Mn species-induced high-efficiency nickel hydroxide electrocatalyst for co-production of 2,5-furandicarboxylic acid and hydrogen

Sustainable Chemistry for Energy Materials

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Sustainable Chemistry for Energy materials 2025年

作者： Junting Dong Le Zhang Xuedan Song Lin Chen Jiarui Zhao Jiawei Mu Chang Yu Jieshan Qiu State Key Laboratory of Fine Chemicals Frontier Science Center for Smart Materials School of Chemical Engineering Dalian University of Technology Dalian 116024 Liaoning China Sinopec Research Instutute of Petroleum Processing(RIPP) Beijing 100083 China College of Chemical Engineering State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology Beijing 100029 China

Hybrid water electrolysis is a potential system for simultaneously efficiently producing hydrogen and value-added chemicals. Owing to the superior electrochemical oxidation capabilities, Ni-based electrocatalysts have emerged as the dominant electrocatalyst for the anode in hybrid water electrolysis systems. However, the slow catalytic conversion of Ni-based electrocatalysts limits their further development for oxidation reactions. Herein, we prepared an efficient anodic Ni-based electrocatalyst under Mn species-induced effects for the 5-hydroxymethylfurfural oxidation reaction, achieving co-production of 2,5-furandicarboxylic acid and hydrogen. Such an anodic electrocatalyst has a capability of promoting the Ni species oxidation to high valence active species NiOOH, leading to the rapid conversion of 5-hydroxymethylfurfural to the 2,5-furandicarboxylic acid products efficiently. Furthermore, the catalyst was used as an anodic catalyst for a membrane electrode assembly electrolyzer with about 20% lower energy consumption for hydrogen production, enabling the preparation of 4.65 g of 2,5-furandicarboxylic acid products. Such a catalyst design concept will facilitate the rational design of Ni-based catalysts based on the electrochemical reaction mechanism, which promotes the development of green hydrogen production and the hybrid water electrolysis system.

关键词： Ni-based electrocatalyst 5-Hydroxymethylfurfural Selective oxidation Reaction mechanism Hydrogen

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Effect of Ca addition on solidification microstructure of hypoeutectic Al-Si casting alloys

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China Foundry 2019年第3期16卷 153-160页

作者： Xiang-yi Jiao Chao-feng Liu Jun Wang Zhi-peng Guo Jun-you Wang Zhuo-ming Wang Jun-ming Gao Shou-mei Xiong School of Materials Science and Engineering Tsinghua University Beijing 100084 China Key Laboratory for Advanced Materials Processing Technology Tsinghua University Beijing 100084 China Hong Bang Die Casting (Nantong) Co. Ltd. Nantong China

The effect of Ca addition on the solidification microstructure of hypoeutectic Al-Si casting alloys was investigated using scanning electron microscopy (SEM) and differential scanning calorimetry (DSC) methods with particular attention focused on the change of morphologies of primary α-Al and eutectic silicon. Meanwhile,solute distribution in solid-liquid was simulated according to Scheil-Gulliver law. Results showed that primary α-Al and eutectic silicon were refined as Ca content increased because of the variation of the solute concentration in liquid. The addition of Ca increased the nucleation sites like Al3Ti or Al2Cu to promote the nucleation of primary α-Al. Affected by modification effect of Ca, the shape of eutectic silicon changed from flake to fibrous structure. In addition, coarse plate Ca-rich phases could be found along the grain boundary with high Ca content.

关键词： Ca addition primary α-Al eutectic silicon refinement

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