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SSRN 2023年

作者： Wang, Chenguang Dai, Jianan Zhao, Meng Qi, Shuo Liu, Jing Jia, Tao Liu, Fangmeng Sun, Peng Li, Bo Zhou, Ji Lu, Geyu State Key Laboratory of Integrated Optoelectronics Key Laboratory of Advanced Gas Sensors of Jilin Province College of Electronic Science & Engineering Jilin University Changchun130012 China Key Laboratory of Forest Plant Ecology Ministry of Education Engineering Research Center of Forest Bio-Preparation College of Chemistry Chemical Engineering and Resource Utilization Northeast Forestry University Harbin150040 China Hebei Key Laboratory of Hazardous Chemicals Safety and Control Technology School of Chemical Safety North China Institute of Science and Technology Langfang065201 China State Kay Lab of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua University Beijing100084 China International Center of Future Science Jilin University Changchun130012 China

Organic photothermal materials, particular the donor-acceptor (D-A) type ones, have attracted increased attention because they could efficiently transform solar energy to heat in an environmentally friendly manner. So far, there are many strategies to improve the fluorescence of D-A type molecules, while how to quench the fluorescence via non-radiative decay process and thus maximize the solar-thermal conversion efficiency is rarely investigated. Herein, a new design strategy is proposed to overcome this bottleneck, that is, formatting a unique twisted intramolecular charge-transfer (TICT) excitation state for the D-A type molecule. To demonstrate this new design strategy, three D-A molecules TPA-BTO, TPA-BTO-Py+ and GTPA-BTO-Py+ are synthesized with the consideration of employing stronger donor/acceptor moieties. The photophysical measurements and theoretical calculations reveal that these molecules display strong tendency to form TICT state, and the stronger donor/acceptor would significantly promote the TICT-based non-radiative decay process. Consequently, the target molecule GTPA-BTO-Py+ is totally non-fluorescent and could efficiently transform the absorbed solar energy to heat. Further combined with the wide absorption up to 1300 nm, GTPA-BTO-Py+ solid displays a high solar-thermal conversion efficiency of 20.5%. Finally, the utility of GTPA-BTO-Py+ as highly efficient photothermal material in solar energy is highlighted by water evaporation and thermoelectric generation. © 2023, The Authors. All rights reserved.

关键词： Molecules

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Modulating electron density to boost photoluminescence of Eu 3+ -doped Gd 3 Ga 5 O 12 garnet by Al 3+ ion incorporation

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Journal of Rare Earths 2025年

作者： Zhengjie Tian Haiyan Wang Xiyong Chen Mingjian Yuan Bingsuo Zou Ruosheng Zeng School of Physical Science and Technology State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured Materials Guangxi University Nanning 530004 China State Key Laboratory of Advanced Chemical Power Sources Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Frontiers Science Center for New Organic Matter College of Chemistry Nankai University Tianjin 300071 China

Rare earth-doped garnet materials are highly promising for applications in solid-state lighting, display, and radiation detection due to their tunable optical properties and excellent thermal stability. However, the radius mismatch between rare earth ion and host cation can lead to lattice distortion and defect formation, resulting in low photoluminescence quantum yield (PLQY), which severely limits their practical applications. In this study, a co-doping strategy was employed by introducing smaller Al 3+ into the Gd 3 Ga 5 O 12 :Eu 3+ garnet, successfully mitigating the lattice mismatch. It is found that the incorporation of Al 3+ significantly enhances the photoluminescence efficiency, and the PLQY increases from 5.6% to 21.5%. Density functional theory calculations confirm that Al 3+ does not directly participate in the luminescence process but rather enhances the electron transition probability by modulating charge density, thereby achieving luminescence enhancement. Notably, with Al 3+ doping, the light-emitting diodes exhibit both high color purity and a 75% improvement in photoelectric conversion efficiency (from 4.23% to 7.41%). This work not only provides new insights into luminescence regulation in rare earth-doped garnets, also expands the potential for multifunctional applications of garnet materials.

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MIL-53(Al)derived single-atom Rh catalyst for the selective hydrogenation of m-chloronitrobenzene into m-chloroaniline

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Chinese Journal of Catalysis 2021年第5期42卷 824-834页

作者： Weiyin Wang Lu Lin Haifeng Qi Wenxiu Cao Zhi Li Shaohua Chen Xiaoxuan Zou Tiehong Chen Nanfang Tang Weiyu Song Aiqin Wang Wenhao Luo College of Chemistry Xiangtan UniversityXiangtan 411105HunanChina CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China College of Chemistry and Chemical Engineering Jishou UniversityJishou 416000HunanChina State Key Laboratory of Heavy Oil Processing China University of PetroleumBeijing 102249China Institute of New Catalytic Materials Science School of Materials Science and EngineeringKey Laboratory of Advanced Energy Materials Chemistry(MOE)Nankai UniversityTianjin 300350China State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina

The catalytic hydrogenation of halonitroarenes to haloanilines is a green and sustainable process for the production of key nitrogen-containing intermediates in fine chemical *** hydrogenation poses a significant challenge,which requires the rational design of the catalysts with proper hydrogenation ability for nitro group and simultaneously preventing dehalogenation of halogen ***,a highly effective Rh@Al_(2)O_(3)@C single-atom catalyst(SAC)was developed for the hydrogenation of m-chloronitrobenzene(m-CNB)to m-chloroaniline(m-CAN),through an in-situ grafting of metal during the assembly of MIL-53(Al),followed by confined *** characterizations reveal an exquisite structure of the Rh@Al_(2)O_(3)@C,containing atomically dispersed Rh sites onto Al_(2)O_(3) confined by the amorphous *** five-coordinated aluminum(Al^(Ⅴ))species are essential for achieving the atomic dispersion of Rh atoms,providing the unsaturated coordinative sites for *** to the benchmark Rh/γ-Al_(2)O_(3) and Rh/C nanocatalysts,the Rh@Al_(2)O_(3)@C SAC affords an excellent turnover frequency of 2317 molm-CNB·molRh^(–1)·h^(–1),the highest value to date in heterogeneous catalyst systems for the hydrogenation of m-CNB at 313 K and 20 bar H2,together with a sustained selectivity to m-CAN(~98%)during five consecutive *** superior catalytic performance of the Rh@Al_(2)O_(3)@C is attributed to a proper modulation of electronic structure of hydrogenation metal by forming SAC,together with an enhanced accessibility of acid function sites.

关键词： Single-atom catalyst Rhodium Metal-organic framework Hydrogenation Chemoselectivity

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Design and intelligent colour regulation of luminescent silk chemically bonded with Eu(III) and Eu(III)/Tb(III)

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COLORATION technology 2018年第5期134卷 373-380页

作者： Xiao, Xingfang Ren, Lipei Zhang, Yawei Zhang, Qian Zhao, Sanping Liu, Ruina Xu, Weilin College of Material Science and Engineering Wuhan Institute of Technology Wuhan China State Key Laboratory of New Textile Materials and Advanced Processing Technologies Wuhan Textile University Wuhan China State Key Laboratory of New Textile Materials and Advanced Processing Technologies Wuhan Textile University Wuhan China State Key Laboratory of New Textile Materials and Advanced Processing Technologies Wuhan Textile University Wuhan China State Key Laboratory of New Textile Materials and Advanced Processing Technologies Wuhan Textile University Wuhan China Key Laboratory for the Green Preparation and Application of Functional Materials Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials Ministry of Education Hubei Key Laboratory of Polymer Materials School of Materials Science and Engineering Hubei University Wuhan China State Key Laboratory of New Textile Materials and Advanced Processing Technologies Wuhan Textile University Wuhan China State Key Laboratory of New Textile Materials and Advanced Processing Technologies Wuhan Textile University Wuhan China State Key Laboratory of New Textile Materials and Advanced Processing Technologies Wuhan Textile University Wuhan China

Design and successful synthesis of a series of novel luminescent silk chemically modified with europium(III) [Eu(III)] and europium(III)/terbium(III) [Eu(III)/Tb(III)] is reported. The modified silk specimens were characterised by infrared spectroscopy, fluorescence spectroscopy, scanning electron microscopy, and evaluated for their colour fastness. The rare earth ions were linked to the silk fibre via chemical bonds with the aid of tetracarboxylic acids used as the bridging ligands. Therefore, the modified silk had excellent luminescent stability and colour fastness to water and sunlight. Based on the blue fluorescence of silk along with the red and green luminescence of Eu(III) and Tb(III), respectively, under ultraviolet irradiation intelligent colour regulation was easily achieved by adjusting either the amount of Eu(III) or the ratio of Eu(III)/Tb(III). The Commission International de l'Eclairage chromaticity co-ordinates calculated from the emission spectra also confirm the colour changes. Benefiting from the tunable colour and high stability, the modified silk could be an excellent candidate for applications in anti-counterfeiting and flexible tunable light- emitting materials.

关键词： silks Silk rare earth ion carburizing Color emission spectrum Remainder of a Series textiles-Color fastness Sunlight chemical bond resin bonding Telescoping a series

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Electronic Metal-Support Interaction Induces Hydrogen Spillover and Platinum Utilization in Hydrogen Evolution Reaction

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Angewandte Chemie 2024年第1期137卷

作者： Yumei Feng Yuhua Xie Yingjie Yu Dr. Yazhou Chen Prof. Dr. Qingting Liu Prof. Dr. Haifeng Bao Dr. Fang Luo Shuyuan Pan Prof. Dr. Zehui Yang State Key Laboratory of New Textile Materials & Advanced Processing Technology College of Materials Science and Engineering Wuhan Textile University Wuhan 430200 China Faculty of Materials Science and Chemistry China University of Geosciences Wuhan 388 Lumo RD Wuhan 430074 China Y. Feng Y. Xie and Y. Yu equally contributed to this work. Hubei Provincial Key Laboratory of Green Materials for Light Industry Hubei University of Technology Wuhan 430068 China

The substantial promotion of hydrogen evolution reaction (HER) catalytic performance relies on the breakup of the Sabatier principle, which can be achieved by the alternation of the support and electronic metal support interaction (EMSI) is noticed. Due to the utilization of tungsten disulfides as support for platinum (Pt@WS 2 ), surprisingly, Pt@WS 2 demands only 31 mV overpotential to attain 10 mA cm −2 in acidic HER test, corresponding to a 2.5-fold higher mass activity than benchmarked Pt/C. The pH dependent electrochemical measurements associated with H 2 -TPD and in situ Raman spectroscopy indicate a hydrogen spillover involved HER mechanism is confirmed. The WS 2 support triggers a higher hydrogen binding strength for Pt leading to the increment in hydrogen concentration at Pt sites proved by upshifted d band center as well as lower Gibbs free energy of hydrogen, favourable for hydrogen spillover. Besides, the WS 2 shows a comparably lower effect on Gibbs free energy for different Pt layers (−0.50 eV layer −1 ) than carbon black (−0.88 eV layer −1 ) contributing to a better Pt utilization. Also, the theoretical calculation suggests the hydrogen spillover occurs on the 3 rd Pt layer in Pt@WS 2 ; moreover, the energy barrier is lowered with increment in hydrogen coverage on Pt. Therefore, the boosted HER activity attributes to the EMSI effect caused hydrogen spillover and enhancement in Pt utilization efficiency.

关键词： Hydrogen evolution reaction Electronic metal-support interaction Hydrogen spillover Tungsten sulfides in situ Raman spectroscopy

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Multi-crosslinked network magnesium phosphate bone cement with high flexural properties

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Ceramics International 2025年

作者： Zijie Gao Jiawei Liu Mingjiang Zhang Pengfei Chen Takashi Goto Rong Tu Honglian Dai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China National energy key laboratory for new hydrogen-ammonia energy technologies Foshan Xianhu Laboratory Foshan 528200 China New Industry Creation Hatchery Center Tohoku University Sendai 980-8579 Japan

Magnesium phosphate cement (MPC) is a bone repair material with good early strength, but its low flexural strength limits its application in bone defect regions subjected to multi-directional loads and repeated stresses. Traditional strategies for reinforcing inorganic bone cement, such as lamination, provide excellent mechanical strength but result in the deterioration of other properties. For instance, the reduction in injectability makes it difficult for the bone cement to fill irregular bone defect sites. Therefore, developing a bone cement with high strength, good operability, and biological activity remains a significant challenge. This study aimed to construct a triple-cured gel-based bone cement by incorporating polyurethane-sodium alginate (EPU-SA) emulsion into magnesium phosphate bone cement (TMPC), forming a structurally more continuous and stable interpenetrating triple network composite system (ES-T) during the hydration process. The in-situ reinforcement of TMPC was achieved through the dual effects of physical and chemical interactions. The results showed that the flexural strength of ES-T under humid conditions was 214% higher than that of TMPC, reaching 50.5 MPa. Interface analysis between organic and inorganic components confirmed the bonding mechanism between the emulsion and bone cement and clarified the reinforcement mechanism. In addition, ES-T demonstrated promotive effects on cellular osteogenic differentiation and generation of new bone tissue by in vitro and in vivo experiments.

关键词： Bone cement

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Effect of Binder Concentration on Piezoelectric Properties of Lead Zirconate Titanate Ceramics Based on Material Extrusion Additive Manufacturing

SSRN

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SSRN 2022年

作者： Liu, Kai Xia, Yuhang Zhang, Qingqing Du, Yanying Shi, Yusheng Joshi, Sanjay Yan, Chunze Wu, Yanjiao Huang, Shangyu Sun, Huajun State Key Laboratory of Silicate Materials for Architectures Wuhan University of Technology Hubei Wuhan430070 China School of Materials Science and Engineering Wuhan University of Technology Hubei Wuhan430070 China School of Logistics Engineering Wuhan University of Technology Hubei Wuhan430070 China Advanced Ceramics Institute of Zibo New & High-Tech Industrial Development Zone Zibo255000 China State Key Laboratory of Materials Processing and Die & Mould Technology Huazhong University of Science and Technology Hubei Wuhan430074 China Penn State University University ParkPA16802 United States Ningbo volken Technology Co. Ltd Zhengjiang Ningbo315000 China

In order to further improve the piezoelectric properties of PZT ceramics formed by material extrusion (MEX) additive manufacturing process, this article systematically studied the influence of binder concentration on the rheology of MEX ceramic slurry. By comparing the rheological properties of the slurry, PZT slurry with high solid content and suitable for printing was obtained. The closed porosity of the green body after debinding was evaluated by comparing the breaking strength of the green body. Sintered samples were obtained after a lead-rich atmosphere sintering process. It was noted that the binder concentration affects the piezoelectric properties of the ceramic by affecting the porosity of the green body and the grain size of the sintered ceramics. The PZT ceramics fabricated with a binder concentration of 10wt.% shows the largest relative density (96.9%), the smallest closed porosity (2.51%), and the largest piezoelectric constant (342.6pC/N). This research has laid the foundation for the preparation of high-performance piezoelectric ceramics by MEX. © 2022, The Authors. All rights reserved.

关键词： Extrusion

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Modulation of magnetic and electrical properties of bilayer graphene quantum dots using rotational stacking faults

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Chinese Physics B 2019年第7期28卷 504-510页

作者： Hong-Ping Yang Wen-Juan Yuan Jun Luo Jing Zhu National Center for Electron Microscopy in Beijing School of Materials Science and Engineering the State Key Laboratory of New Ceramics and Fine Processing Key Laboratory of Advanced Materials(MOE) Tsinghua University Beijing 100084 China Center for Electron Microscopy Institute for New Energy Materials & Low-Carbon Technologies School of Materials Science and Engineering Tianjin University of Technology Tianjin 300384 China

Bilayer graphene quantum dots with rotational stacking faults(RSFs) having different rotational angles were *** the first-principles calculation, we determined that these stacking faults could quantitatively modulate the magnetism and the distribution of spin and energy levels in the electronic structures of the *** addition, by examining the spatial distribution of unpaired spins and Bader charge analysis, we found that the main source of magnetic moment originated from the edge atoms of the quantum *** research results can potentially provide a new path for producing all-carbon nanodevices with different electrical and magnetic properties.

关键词： bilayer graphene quantum dots rotational stacking faults first-principles calculation

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Nanofibril Organization in Silk Fiber as Inspiration for Ductile and Damage-Tolerant Fiber Design

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advanced Fiber materials 2019年第3期1卷 231-240页

作者： Shihui Lin Chao Ye Wenwen Zhang Anchang Xu Shixian Chen Jing Ren Shengjie Ling School of Physical Science and Technology ShanghaiTech University393 Middle Huaxia RoadShanghai 201210China Jiangsu Co‑Innovation Center of Efficient Processing and Utilization of Forest Resources Jiangsu Key Lab of Biomass‑Based Green Fuel and ChemicalsCollege of Chemical EngineeringNanjing Forestry UniversityNanjing 210037China State Key Laboratory of New Textile Materials and Advanced Processing Technology School of Textile Science and EngineeringWuhan Textile UniversityWuhan 430200China

Ductile and damage-tolerant fibers(DDTFs)are desired in aerospace engineering,mechanical engineering,and biomedical engineering because of their ability to prevent the catastrophic sudden structural/mechanical ***,in practice,design and fabrication of DDTFs remain a major challenge due to finite fiber size and limited processing *** this regard,animal silks can provide *** are hierarchically structured protein fibers with an elegant trade-off of mechanical strength,extensibility and damage tolerance,making them one of the toughest materials *** this article,we confirmed that nanofibril organization could improve the ductility and damage-tolerance of silk fibers through restricted fibril shearing,controlled slippage and *** by these strategies,we further established a rational strategy to produce polyamide DDTFs by combining electrospinning and yarn-spinning *** resultant polymeric DDTFs show a silk-like fracture resistance behavior,indicating potential applications in smart textile,biomedicine,and mechanical engineering.

关键词： Fiber Silk Mechanical property Damage tolerance Bioinspired materials

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Microporous Hard Carbon Support Provokes Exceptional Performance of Single Atom Electrocatalysts for advanced Air Cathodes

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Angewandte Chemie 2025年

作者： Haijing Liu Ping Li Kaicai Fan Fenghong Lu Qi Sun Qi Zhang Bin Li Yajie Shu Lingbo Zong Lei Wang State Key Laboratory of Eco-chemical Engineering College of Chemistry and Molecular Engineering Qingdao University of Science and Technology Qingdao 266042 China State Key Laboratory of Eco-chemical Engineering College of Environment and Safety Engineering Qingdao University of Science and Technology Qingdao 266042 China State Key Laboratory of Eco-chemical Engineering College of Materials Science and Engineering Qingdao University of Science and Technology Qingdao 266042 China National Local Joint Laboratory for Advanced Textile Processing and Clean Production Wuhan Textile University Wuhan 430200 China

Single atom catalysts embracing metal-nitrogen (MN x ) moieties show promising performance for oxygen reduction reaction (ORR). The modification on spatially confined microenvironments, which won copious attention with respect to achieving efficient catalysts, are auspicious but yet to be inspected for MN x moieties from modulating the energetics and kinetics of ORR. Here, Fe single atoms (SAs) are immobilized in microporous hard carbon (Fe-SAs/MPC), in which the microporous structure with crumpled graphene sheets serves confined microenvironment for catalysis. Fe-SAs/MPC holds a remarkable half-wave potential of 0.927 V and excellent stability for ORR. Theoretical studies unveil that hydrogen bonding between the intermediate of O* and micropore interior surfaces substantially promote its protonation and accelerate the overall ORR kinetics. Both the aqueous and quasi-solid-state zinc-air batteries driven by Fe-SAs/MPC air cathode show excellent stability with small charging/discharging voltage gaps. Importantly, when used as the air cathode for industrial chlor-alkali process, the applied voltage of Fe-SAs/MPC-based flow cell to reach 300 mA cm −2 is 1.57 V, which is 210 mV smaller than Pt/C-based one. These findings provide in-depth insights into the confined microenvironment of MN x moieties for boosted electrochemical performance, and pave the pathways for future catalyst development satisfying the requirement of industrial applications.

关键词： Chlor-alkali process Microporous hard carbon Oxygen reduction reaction Single atom Zn-air battery

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