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Catalysis Today 2022年 405-406卷 82-91页

作者： Jia-Min Lyu Shen Yu Zhao Peng Jian Zhou Zhan Liu Xiao-Yun Li Yu-Li Li-Hua Chen Bao-Lian Su State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 Hubei China State Key Laboratory of Green Chemical Engineering and Industrial Catalysis Shanghai Research Institute of Petrochemical Technology SINOPEC Shanghai 201208 China State Key Laboratory of Silicate Materials for Architecture Wuhan University of Technology Wuhan 430070 Hubei China Laboratory of Inorganic Materials Chemistry (CMI) University of Namur Namur B-5000 Namur Belgium

Bifunctional catalysts are widely applied for many important reactions as the synergetic effect of two types of active sites remarkably improves catalysis performance. However, their bifunctionality has not been fully exploited since the proximity of bifunctional catalysts is hard to control. Herein, we demonstrate a bifunctional [email protected] 2 O 3 catalyst with a core-shell structure and a nano-scale proximity by in-situ growth of γ-Al 2 O 3 nanosheets on the surface of ZSM-5 crystals for methanol conversion. The nano-scale proximity endows the catalyst with higher reaction activity and C 2 –C 3 olefins yield (53 %) in comparison to the catalysts with micro-scale proximity (20 %) and millimeter-scale proximity (27 %), which can be attributed to the fluent transport of the reaction intermediates between two types of active sites. This strategy for constructing bifunctional catalysts with nano-scale proximity is conducive to understanding the relationship between proximity and catalytic performance in methanol conversion.

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Enhancing the Humidity Resistance of Perovskite Photovoltaics: Comprehensive PbI2 Management Utilizing Long-Chain Ionic Liquid

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SSRN 2024年

作者： Sun, Yonggui Wang, Fei Lu, Lu Wang, Taomiao Yang, Guo Liang, Xiao Zhou, Xianfang Sun, Xiaokang Li, Qiannan Li, Yongjun Zhang, Fan Duan, Dawei Zhu, Jiajie Zhu, Quanyao Hu, Ruiyuan Yuan, Mingjian Hu, Hanlin Hoffmann Institute of Advanced Materials Shenzhen Polytechnic University 7098 Liuxian Boulevard Shenzhen518055 China Nanjing University of Posts and Telecommunications Nanjing210023 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of Materials Science and Engineering Wuhan University of Technology Wuhan China Shenzhen University China College of Chemistry Nankai University Tianjin China

Effectively managing residual PbI2 in two-step perovskite fabrication, while simultaneously enhancing the device performance, especially its humidity stability, poses a significant challenge. Herein, we introduced a novel ionic liquid (IL) molecule, long-chain alkane-based 1-octyl-3-methylimidazolium chloride (OMIMCl), with excellent hydrophobicity to regulate the perovskite conversion process, aiming to enhance the performance of resulting perovskite solar cells. The introduction of OMIMCl contributes to the formation of a uniform porous PbI2 film, facilitating comprehensive penetration of the second-step organic salt to fully convert PbI2 into perovskite material. Interestingly, nearly no residual PbI2 clusters are observed at both the top and bottom surfaces of OMIMCl-modified perovskite films. Meanwhile, depth-resolved grazing incidence wide-angle x-ray scattering (GIWAXS) measurements have quantitatively demonstrated the reduction of PbI2 in OMIMCl-modified perovskite thin films. Notably, the incorporation of OMIMCl retards the growth rate of perovskite crystals efficiently, thereby assisting in generating high-quality of perovskite films with larger grain size. Moreover, density functional theory (DFT) calculations of binding energy numerically demonstrate the hydrophobic property of IL OMIMCl, which plays a crucial role in improving the humidity stability of PSCs, as evidenced by direct water-dipping test. Consequently, we achieved a champion power conversion efficiency (PCE) of 24.72% and significantly improved long-term stability. © 2024, The Authors. All rights reserved.

关键词： Lead compounds

Functionally Graded Triply Periodic Minimal Surface Scaffold of Ha-Al2o3 Via Vat Photopolymerization 3d Printing

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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

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

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

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

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

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

Enhanced the Impact Resistance by Gradient Face-Sheet Design of a Sandwich Structure

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SSRN 2023年

作者： Wei, Jing Luo, Guoqiang Liu, Ao Wei, Qinqin Xia, Zhilin Zhang, Ruizhi Shen, Qiang State Key Lab of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan430070 China School of Materials Science and Engineering Wuhan University of Technology Wuhan430070 China National Key Laboratory of Shock Wave and Detonation Physics Institute of Fluid Physics China Academy of Engineering Physics Mianyang621900 China

Sandwich structure has been designed to reduce the impact damage of the stress waves. However, the existing work focuses on the optimization of sandwich cores while the important face-sheet structure is seldom improved. Here, we used the impedance matching theory to design a negative gradient face-sheet sandwich structure with excellent stress wave attenuation performance. Owing to stress wave attenuation form a high impedance to a low one, the negative gradient face-sheet sandwich structure shows a low peak stress of 5.51 MPa, and the average transmission peak stress is 2.69 MPa. The gradient face-sheet structure changes the compressive deformation behavior;thus, the energy absorption performance of the negative gradient face-sheet sandwich structure increases to be 1311.8 KJ/m3 and the specific energy absorption reaches 1072 J/kg. Finite-element methods further demonstrate the overall sandwich structures can be enhanced through alleviating the failure of sandwich core by a gradient face-sheet structure. This work provides a paradigm for the design of sandwich structures with high energy absorption performance. © 2023, The Authors. All rights reserved.

关键词： Energy absorption

Vacancy-Based Defect Regulation for High Thermoelectric Performance in Ge9Sb2Te12-x Compounds

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ACS APPLIED MATERIALS & INTERFACES 2020年第17期12卷 19664-19673页

作者： Chen, Shuo Bai, Hui Li, Junjie Pan, Wenfeng Jiang, Xianyan Li, Zhi Chen, Zhiquan Yan, Yonggao Su, Xianli Wu, Jinsong Uher, Ctirad Tang, Xinfeng State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China Hubei Nuclear Solid Physics Key Laboratory Department of Physics Wuhan University Wuhan 430072 China Department of Physics University of Michigan Ann Arbor Michigan 48109 United States

Defect engineering is the core strategy for improving thermoelectric properties. Herein, cation doping along with modulation of cation vacancy has been developed in GeTe-based materials as an effective method to induce vacancy-based defects to boost their thermoelectric performance. A series of ternary compounds of Ge9Sb2Te12-x (x = 0, 0.03, 0.06, 0.09, 0.12, 0.15) was prepared by vacuum-melting and annealing combined with the spark plasma sintering (SPS) process. The role of Sb doping and cation vacancy on thermoelectric properties was systematically investigated. It is found that alloying Sb2Te3 into GeTe increases the concentration of cation vacancies, which is corroborated by both positron annihilation measurements and theoretical calculations. The vacancies, stacking faults, and planar defect interactions determine the thermoelectric transport properties. Adjusting the deficiency of Te effectively tunes the concentration of cation vacancies and dopant defects in the structure. In turn, this tunes the carrier concentration close to its optimum. A high power factor of 32.6 mu W cm(-1) K-2 is realized for Ge9Sb2Te11.91 at 725 K. Moreover, large strains induced by the defect structures, including Sb dopant, vacancy, staking faults, as well as planar defects intensify phonon scattering, leading to a significant decrease in the thermal conductivity from 7.6 W m(-1) K-1 for pristine GeTe to Ge9Sb2Te11.85 at room temperature. All of the above contribute to a high ZT value of 2.1 achieved for the Ge9Sb2Te11.91 sample at 775 K.

关键词： GeTe-based compounds alloying with Sb2Te3 deficiency of Te stacking fault vacancy plane thermoelectric