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SSRN 2023年

作者： Liu, Qiuyu Tang, Qinchao Huang, Zhifeng Li, Zhiwei Wang, Xuye Wen, Pin Bai, Yi Chen, Fei Hubei Longzhong Laboratory Wuhan University of Technology Xiangyang Demonstration Zone Xiangyang441000 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan430070 China International School of Materials Science and Engineering Wuhan University of Technology Wuhan430070 China State Key Laboratory of Oral & Maxillofacial Reconstruction and Regeneration Key Laboratory of Oral Biomedicine Ministry of Education Hubei Key Laboratory of Stomatology School & Hospital of Stomatology Wuhan430079 China Hubei Key Laboratory of Theory and Application of Advanced Materials Mechanics School of Science Wuhan University of Technology Wuhan430070 China

Hydroxyapatite (HA) is widely used in scaffolds due to its high similarity in the composition to natural bone. However, the weak and fragile characteristics of synthetic HA limit its application. The strength of HA can be increased by the incorporation of alumina (Al2O3) to obtain composites with extraordinary compressive strength and biocompatibility. HA-Al2O3 composites with different ratios were prepared by Vat photopolymerization 3D printing, and their shrinkage, porosity, phase composition and biocompatibility were systematically investigated. In addition, the Diamond structure of the scaffold was chosen to achieve the trade-off relationship between compressive strength and porosity. The results suggest that the HA-Al2O3 composite with 20 vol% HA possesses the maximum compressive strength and 60 vol% HA has optimal biocompatibility. A compositional gradient scaffold from 60 vol% HA and 20 vol% HA was proposed to satisfy different needs of the different parts in scaffold for biocompatibility and compressive strength. The HA-Al2O3 gradient scaffold achieves a preferable compressive strength of 13.7 MPa while possessing gradient biocompatibility. © 2023, The Authors. All rights reserved.

关键词： Hydroxyapatite

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synthesis of amorphous Pd-based nanocatalysts for efficient alcoholysis of styrene oxide and electrochemical hydrogen evolution

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Nano Research 2023年第4期16卷 4650-4655页

作者： Yiyao Ge Jingjie Ge Biao Huang Xixi Wang Guigao Liu Xiang-Huan Shan Lu Ma Bo Chen Guanghua Liu Songmo Du An Zhang Hongfei Cheng Qingbo Wa Shiyao Lu Lujiang Li Qinbai Yun Kuo Yuan Qinxin Luo Zhichuan J.Xu Yonghua Du Hua Zhang Department of Chemistry City University of Hong KongHong KongChina Hong Kong Branch of National Precious Metals Material Engineering Research Center(NPMM) City University of Hong KongHong KongChina Shenzhen Research Institute City University of Hong KongShenzhen 518057China Department of Chemical and Biological Engineering HKUST Jockey Club Institute for Advanced Study&Energy InstituteThe Hong Kong University of Science and TechnologyHong KongChina School of Materials Science and Engineering Nanyang Technological UniversitySingapore 639798Singapore Department of Chemistry University of Science and Technology of ChinaHefei 230026China National Synchrotron Light Source II Brookhaven National LaboratoryUptonNew York 11973USA State Key Laboratory of New Ceramics&Fine Processing School of Materials Science and EngineeringTsinghua UniversityBeijing 100084China

Amorphous nanomaterials with long-range disordered structures could possess distinct properties and promising applications,especially in catalysis,as compared with their conventional crystalline *** is imperative to achieve the controlled preparation of amorphous noble metal-based nanomaterials for the exploration of their phase-dependent ***,we report a facile wet-chemical reduction strategy to synthesize various amorphous multimetallic Pd-based nanomaterials,including PdRu,PdRh,and *** phase-dependent catalytic performances of distinct Pd-based nanomaterials towards diverse catalytic applications have been ***,the usage of PdRu nanocatalysts with amorphous and crystalline face-centered cubic(fcc)phases can efficiently switch the ring-opening route of styrene oxide to obtain different products with high selectivity through alcoholysis reaction and hydrogenation reaction,***,when used as an electrocatalyst for hydrogen evolution reaction(HER),the synthesized amorphous PdRh nanocatalyst exhibits low overpotential and high turnover frequency values,outperforming its crystalline fcc counterpart and most of the reported Pd-based HER electrocatalysts.

关键词： amorphous nanomaterials Pd-based nanocatalysts phase engineering of nanomaterials ring-opening reaction of styrene oxide electrocatalytic hydrogen evolution

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Hierarchical ZrO2@N-doped carbon nano-networks anchored ultrafine Pd nanoparticles for highly efficient catalytic hydrogenation

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Science China Chemistry 2022年第8期65卷 1661-1669页

作者： Pu, Chun Li, Rui-Dong Chang, Gang-Gang Chen, Min-Jie Yao, Yao Li, Jun-Sheng Zhao, Bo Wu, Lu Zhang, Yue-Xing Yang, Xiao-Yu School of Chemistry Chemical Engineering and Life Science & State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan China School of Power Engineering Naval University of Engineering Wuhan China Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials Key Laboratory for the Synthesis and Application of Organic Functional Molecules of Ministry of Education College of Chemistry and Chemical Engineering Hubei University Wuhan China

Carbon supported metal catalysts have received considerable interest due to their widespread applications in heterogeneous catalysis. However, the controllable synthesis of carbon support with defined morphology and composition still represents great challenging. Herein, we reported the synthesis of a well-defined hierarchically nanosized H-ZrO2/NC (nitrogen-doped carbon) network via an inheritable carbonization strategy. When immobilizing the palladium clusters into the support, the N-doped sites and oxygen vacancy of the carbon composite can effectively stabilize and activate Pd through strong metal-support interaction which was also confirmed by density functional theory (DFT) calculations. Moreover, the hierarchically nanosized network can contribute to the exposure of active sites and facilitate the mass transfer during the catalytic process. As a result, benefiting from the hierarchical structure, composition and hydrolytic nature, Pd@H-ZrO2/NC exhibited excellent catalytic activity and stability towards the hydrogenation of furfural in mild reaction conditions, as well as good universality toward the hydrogenation of a series of unsaturated hydrocarbons.

关键词： hierarchical carbon nanosized networks composites metal-support interaction catalytic hydrogenation

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The Ordered Lattice Host Framework Induced Guest Li+ Disordering in High Performance Cobalt-Free Ni-Rich Cathode materials

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SSRN 2024年

作者： Xu, Jia Zhang, Xiaoyu Sun, Shixiong Fu, Rong Cheng, Fangyuan Wei, Peng Li, Qing Fang, Chun Lin, He Han, Jiantao State Key Laboratory of Material Processing and Die & Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology Hubei Wuhan430074 China School of Materials Science and Engineering State Key Laboratory of Advanced Special Steel Shanghai University Shanghai200444 China School of Mathematical and Physical Sciences University of Technology SydneyNSW2007 Australia Shanghai Synchrotron Radiation Facility Zhangjiang Lab Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai201204 China

Recently, due to high price, resource shortage and unstable supply of cobalt, the development of low-cost cobalt-free Ni-rich cathodes has attracted extensive attention with the ever-increasing lithium-ion batteries (LIBs) industry. Selecting cost-effective elements to replace cobalt in Ni-rich cathodes is urgent. However, the principle of structural design of Ni-rich cathode remains unclear, hampering the selection of alternative elements. Herein, the cobalt-free cathodes of LiNi0.95Mg0.05O2 (NiMg) and LiNi0.95Mn0.05O2 (NiMn) are designed as alternatives to LiNi0.96Co0.04O2 (NiCo). NiMg has comparable cycle stability with NiCo, while NiMn has inferior cycle performance. Reverse Monte Carlo modelling was used to generate structural model and uncover local structure by fitting pair distribution function. It reveals Mn causes more severe Jahn-Teller distortions and disordered lattice host framework (Ni0.95M0.05O2, M = Co/Mn/Mg) than Co and Mg due to the strong size effect and coulomb interactions of Mn in Ni0.95Mn0.05O2 layer. The outstanding cycle stability of NiMg and NiCo originates from the ordered lattice host frameworks, which relieve stress and inhibit particle breakage during cycle. Meanwhile, the ordered lattice host framework induced guest Li+ disordering reduces Li+ diffusion energy barrier, improving the rate capability. This study provides a new perspective for the structural design of cobalt-free Ni-rich cathodes. © 2024, The Authors. All rights reserved.

关键词： Cathodes

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Cathodic Zn underpotential deposition:an evitable degradation mechanism in aqueous zinc-ion batteries

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Science Bulletin 2022年第18期67卷 1882-1889,M0004页

作者： Shaohua Zhu Yuhang Dai Jinghao Li Chumei Ye Wanhai Zhou Ruohan Yu Xiaobin Liao Jiantao Li Wei Zhang Wei Zong Ruwei Chen Guanjie He Dongliang Chao Qinyou An State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Laboratory of Advanced Materials Shanghai Key Laboratory of Molecular Catalysis and Innovative Materialsand School of Chemistry and MaterialsFudan UniversityShanghai 200433China Christopher Ingold Laboratory Department of ChemistryUniversity College LondonLondon WC1H 0AJUK Electrochemical Innovation Laboratory Department of Chemical EngineeringUniversity College LondonLondon WC1E 7JEUK State Key Laboratory of Silicate Materials for Architectures Wuhan University of TechnologyWuhan 430070China Department of Materials Science and Metallurgy University of CambridgeCambridge CB30FSUK

Aqueous zinc-ion batteries(AZIBs)are promising for large-scale energy storage,but their development is plagued by inadequate cycle ***,for the first time,we reveal an unusual phenomenon of cathodic underpotential deposition(UPD)of Zn,which is highly irreversible and considered the origin of the inferior cycling stability of *** experimental and theoretical simulation approaches,we propose that the UPD process agrees with a two-dimensional nucleation and growth model,following a thermodynamically feasible ***,the universality of Zn UPD is identified in systems,including VO_(2)//Zn,TiO_(2)//Zn,and SnO_(2)//*** practice,we propose and successfully implement removing cathodic Zn UPD and substantially mitigate the degradation of the battery by controlling the end-ofdischarge *** work provides new insights into AZIBs degradation and brings the cathodic UPD behavior of rechargeable batteries into the limelight.

关键词： Underpotential deposition Zn metal deposition Zinc-ion battery Aqueous battery Degradation mechanism

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Facile synthesis of Tunable Ultra-Thin Anodes for Long-Lasting and High-Energy-Density Lithium Metal Batteries

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SSRN 2024年

作者： Tian, Du Chen, Weimin Shen, Yue Cao, Wenzhu Miao, Wenwen Lai, Zhenghan Chen, Hong Yang, Shanshan Wang, Liang Yu, Faquan Key Laboratory for Green Chemical Process Ministry of Education Hubei Key Laboratory for Novel Reactor and Green Chemistry Technology Hubei Three Gorges Laboratory Hubei Engineering Research Center for Advanced Fine Chemicals School of Chemical Engineering and Pharmacy Wuhan Institute of Technology Wuhan430205 China State Key Laboratory of Material Processing and Die and Mold Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan430074 China Chongqing Institute of Green and Intelligent Technology Chinese Academy of Sciences Chongqing400714 China

Thin lithium metal anodes (LMAs) play a crucial role in realizing lithium metal batteries (LMBs) with high-energy-density. However, the commercial production of thin lithium anode continues to face challenges in manufacturing complexities, inadequate reversible capacity and unstable cyclability. Herein, we show a facile and effective strategy to produce ultra-thin LMAs with tunable thickness (10~50 μm), in which the Li-Ag alloy is in-situ formed and uniformly loaded on the cellulose-derived carbon supported reduced graphene oxide (CC-rGO). Density functional theory (DFT) calculations reveal that the Li-Ag alloy has strong adsorption energy and minimal energy barrier for Li diffusion, which can effectively meliorate Li transfer and homogeneous deposition. Due to the advantages of the synergistic effect of Li-Ag alloy modification, the elaborate-designed ultra-thin and 3D structure, the CC-rGO/LixAgy/Li anode facilitates the acceleration of Li-ion transport kinetics, reduce the nucleation barrier and offer adequate active sites, thereby improving the electrochemical characteristics. The CC-rGO/LixAgy/Li symmetric cell exhibits stably Li plating/stripping for 5000 h at 1 mA cm−2. When matched with LiFePO4 cathode, the full cell delivers remarkable cycling reversibility for 900 cycles at 3 C and the negative/positive capacity (N/P) ratio can be down to 1.18. More impressively, the pouch cell reveals an excellent flexibility with maintaining more than 80% capacity over 80 cycles at 0.3 C in folded states. This study provides a promising avenue to developing viable high-energy-density LMBs. © 2024, The Authors. All rights reserved.

关键词： Lithium alloys

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S‐Scheme 2D/2D Bi_(2)MoO_(6)/BiOI van der Waals heterojunction for CO_(2) photoreduction

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Chinese Journal of Catalysis 2022年第7期43卷 1657-1666页

作者： Zhongliao Wang Bei Cheng Liuyang Zhang Jiaguo Yu Youji Li S.Wageh Ahmed A.Al‐Ghamdi State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070HubeiChina Laboratory of Solar Fuel Faculty of Materials Science and ChemistryChina University of GeosciencesWuhan 430074HubeiChina College of chemistry and chemical engineering Jishou UniversityJishou 416000HunanChina Department of Physics Faculty of ScienceKing Abdulaziz UniversityJeddah 21589Saudi Arabia

Reducing CO_(2) to hydrocarbon fuels by solar irradiation provides a feasible channel for mitigating excessive CO_(2) emissions and addressing resource ***,severe charge recombi‐nation and the high energy barrier for CO_(2) photoreduction on the surface of photocatalysts com‐promise the catalytic ***,a 2D/2D Bi_(2)MoO_(6)/BiOI composite was fabricated to achieve improved CO_(2) photoreduction *** transfer in the composite was facilitated by the van der Waals heterojunction with a large‐area *** function calculation demon‐strated that S‐scheme charge transfer is operative in the composite,and effective charge separation and strong redox capability were revealed by time‐resolved photoluminescence and electron para‐magnetic resonance ***,the intermediates of CO_(2) photoreduction were identi‐fied based on the in situ diffuse reflectance infrared Fourier‐transform *** functional theory calculations showed that CO_(2) hydrogenation is the rate‐determining step for yielding CH_(4) and *** Bi_(2)MoO_(6) into the composite further decreased the energy barrier for CO_(2) photoreduction on BiOI by 0.35 *** study verifies the synergistic effect of the S‐scheme heterojunction and van der Waals heterojunction in the 2D/2D composite.

关键词： 2D/2D S‐scheme heterojunction van der Waals heterojunction CO_(2)photoreduction

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Off-centering effect and crystal symmetry modification lead to high thermoelectric performance in diamondoid Cu_(2)SnSe_(3)

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National Science Open 2025年第3期4卷 35-52页

作者： Pengpeng Chen Shulin Bai Yi Wen Yichen Li Zihao Zhao Dezheng Gao Houdong Huang Yixuan Hu Tian Gao Lei Wang Shaoping Zhan Xiang Gao Xianli Su Hongyao Xie Li-Dong Zhao School of Materials Science and Engineering Beihang UniversityBeijing 100191China Center for Bioinspired Science and Technology Hangzhou International Innovation InstituteBeihang UniversityHangzhou 311115China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Center for High Pressure Science and Technology Advanced Research(HPSTAR) Beijing 100094China

Recently,dimensionless figure of merit(ZT)beyond 1.0 has been demonstrated in diamondoid Cu_(2)SnSe_(3),positioning it as a low-cost and ecofriendly thermoelectric alternative,and sparking intense interest in further optimizing its thermoelectric ***,its intrinsic monoclinic structure and the compact packing of tetrahedral coordination lead to a light valence band and high thermal conductivity,which impede further performance improvement in Cu_(2)SnSe_(3).Thus,developing effective approaches to altering the local structure of Cu_(2)SnSe_(3)is important for further optimizing its thermoelectric ***,we identified and thoroughly investigated the atomic off-centering behavior in Cu_(2)SnSe_(3),and demonstrated the electronic and phonon transport properties of Cu_(2)SnSe_(3)can be significantly enhanced by carefully modifying its monoclinic lattice into a distorted zinc-blende cubic structure via introducing Cd and off-centering Ag *** structure transition leads to band convergence and a reduction in the deformation potential of the material,resulting in a 7-fold enhancement in the density-of-state effective mass and an 85%increase in carrier ***,the off-centering effect results in strong acoustic-optical phonon scattering and an ultra-low lattice thermal conductivity of 0.3 W m^(-1)K^(-1).Consequently,a maximum ZT of 1.3 was obtained at 800 K for the Cu_(1.85)Ag_(0.15)Sn_(0.9)Cd_(0.1)Se_(3).

关键词： thermoelectric crystal structure transition off-centering behavior local symmetry breaking

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Optimizing Light and Heavy Aromatic Ratios in Fluid Catalytic Cracking Slurry Oil for Mesophase Pitch with Wide-Area Optically Anisotropic Texture

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SSRN 2024年

作者： Liao, Gen Shi, Kui Ye, Chong Fan, Zhen Li, Tongqi Zhu, Shipeng He, Xubin Huang, Dong Han, Fei Liu, Hongbo Liu, Jinshui College of Materials Science and Engineering Hunan Province Key Laboratory for Advanced Carbon Materials and Applied Technology Hunan University Changsha410082 China Hunan Province Engineering Research Center for High Performance Pitch-based Carbon Materials Hunan Toyi Carbon Material Technology Co. Ltd. Changsha410000 China State Key Laboratory of Advanced Design and Manufacturing for vehicle Hunan University Changsha410082 China Key Laboratory of Advanced Functional Composite Materials Aerospace Research Institute of Materials and Processing Technology Beijing100076 China China Academy of Launch Vehicle Technology China

Aromatics are the preponderant component of fluid catalytic cracking (FCC) slurry oil, with notable differences in molecular structure between the light and heavy aromatics. The effect of these differences on the formation and optically anisotropic texture of mesophase remains elusive, impeding the preparation of high-quality mesophase pitch. This paper aims to regulate the ratio of light to heavy aromatics in the FCC slurry oil for optimizing the optically anisotropic texture of mesophase pitch. The results show that the heavy aromatics possess higher aromaticity, longer alkane side chains, larger molecular size and more reactive structures (methylene bridges, n-alkane structures) compared with the light aromatics. As an "accelerator", heavy aromatics can form mesophase quickly. Light aromatics not only served as a "diluent," but also assumed the function of a "lubricant", which facilitated the orderly arrangement of aromatic molecular lamellar. The system exhibits moderate reactivity that inhibits excessive condensation and modifies the structural orientation of pyrolysis products with the 2/5 ratio of light to heavy aromatics. Under these conditions, a high-quality mesophase pitch (d002=3.485 Å, Lc=19.832 Å) with wide-area optically anisotropic texture, suitable softening point (262°C) and short polymerization time (t=5.5 h) was obtained. This work provides theoretical support for the preparation of high-quality mesophase pitch by regulating the components of slurry oil. © 2024, The Authors. All rights reserved.

关键词： Aromatization

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Nanomultilayer Gradation Strategy to Improve Mechanical Properties of Tisin/Alcrn Hard Coatings

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SSRN 2024年

作者： Li, Qizhong Liu, Fazhen Yang, Mai Gao, Tenghua Ji, Baifeng Zhang, Song Tu, Rong Zhang, Lianmeng Chaozhou Branch of Chemistry and Chemical Engineering Guangdong Laboratory Chaozhou521000 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 122 Luoshi Road Wuhan430070 China Wuhan University of Technology Advanced Engineering Technology Research Institute of Zhongshan City Xiangxing Road 6 Guangdong Zhongshan528400 China Hubei Technology Innovation Center for Advanced Composites Wuhan University of Technology 122 Luoshi Road Wuhan430070 China School of Civil Engineering and Architecture Wuhan University of Technology 122 Luoshi Road Wuhan430070 China Hubei Key Laboratory of Advanced Technology for Automotive Components Wuhan University of Technology Wuhan430070 China

The structures design and optimization of multilayer coatings, which are utilized to surmount the trade-off between hardness and toughness, has been a current hot topic in the field of hard ceramic coatings. Herein, multi-layered TiSiN/AlCrN coatings with a constant and gradient sublayer thickness (Λ, modulation periods) ranging from 20 to 3.8 nm were prepared by the Cathodic Arc Ion plating. The microstructure, mechanical properties, residual stress and fracture toughness of four gradient structures were investigated systematically. All coatings exhibit a typical FCC crystal structure. In the coating with a monotonous decrease of modulation period (G2 gradient structure), the interface between the TiSiN layer and the AlCrN layer transformed from a partially semi-coherent interface at the bottom layers of Λ = 20 nm, to a fully coherent interface at the top layers of Λ = 3.8 nm, showing the higher mechanical properties than those of G2 (reverse structure of G1). The coating with dual-gradient V2 structure (G1+G2) demonstrated the highest hardness (37.6 ± 1.0 GPa), H/E and H3/E2 ratios (0.095 and 0.34 GPa), and bonding strength (75.3 N), as well as lowest friction coefficient (0.34) and wear rate (6.7×10-6 mm3/Nm). The remarkable resistance to damage and toughness displayed by the V2 structure could be ascribed to its intrinsic capacity for effectively alleviating stress concentration and accommodating incompatibilities during the plastic deformation process. This work offers insights into employing gradient architecture design to enhance the strength and toughness of coatings. © 2024, The Authors. All rights reserved.

关键词： Silicon compounds

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