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PTCDA/CuS cathode enabling stable sulfide-based all-solid-state batteries

Journal of Materiomics 2025年

作者： Zhixing Wan Shuo Wang Yahao Mu Ruihua Zhou Hang Liu Tingwu Jin Di Wu Jianlong Xia Ce-Wen Nan Center of Smart Materials and Devices State Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of Material Science and Engineering Wuhan University of Technology Wuhan 430070 China School of Chemistry Chemical Engineering and Life Science Wuhan University of Technology Wuhan 430070 China State Key Laboratory of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua University Beijing 100084 China

Organic cathode materials have garnered significant attention for their potential application in lithium-ion batteries due to their lightweight nature, tunable structures, high energy density, and environmental friendliness. However, the dissolution of organic cathodes in liquid electrolytes often leads to poor cycling stability, which limits their practical application. In this study, a composite cathode was prepared by ball milling the PTCDA/CuS (perylene-3,4,9,10-tetracarboxylic dianhydride, PTCDA) with a sulfide-based electrolyte and carbon nanotubes. By optimizing the component ratios, the assembled all-solid-state batteries (ASSBs) show a high discharge capacity of 210 mA⸱h/g after 200 cycles without any capacity degradation at a current density of 33.0 mA/g. Through comprehensive characterization techniques including X-ray diffraction (XRD), Raman spectroscopy, Fourier-transform infrared spectroscopy (FTIR), and X-ray photoelectron spectroscopy (XPS), the coordination of Cu 2+ and the formation of sulfur-linked polymers during the charge-discharge processes are elucidated, and the reversibility of the electrochemical reactions has been confirmed. This work highlights the excellent compatibility between organic cathodes and sulfide-based electrolytes, providing a new way for the development of high-performance ASSBs with high energy density and extended lifespan.

关键词： PTCDA/CuS lithium argyrodite organic cathode all-solid-state battery

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Fe-N-C Single-Atom Nanozyme for Ultrasensitive, On-Site and Multiplex Detection of Mycotoxins Using Lateral Flow Immunoassay

SSRN

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SSRN 2022年

作者： Cai, Xinfa Ma, Fei Jiang, Jun Yang, Xianglong Zhang, Zhaowei Jian, Zelang Liang, Meijuan Li, Peiwu Yu, Li Oil Crops Research Institute Chinese Academy of Agricultural Sciences Wuhan430062 China Key Laboratory of Biology and Genetic Improvement of Oil Crops Ministry of Agriculture and Rural Affairs Wuhan430062 China Key Laboratory of Detection for Mycotoxins Ministry of Agriculture and Rural Affairs Wuhan430062 China Ministry of Agriculture and Rural Affairs Wuhan430062 China Quality Inspection and Test Center for Oilseeds Products Ministry of Agriculture and Rural Affairs Wuhan430062 China Wuhan University of Technology State Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of Material Science and Engineering Wuhan430070 China

Sensitive, on-site and multiple detection of mycotoxins is a vital early-warning tool to minimize food losses and protect human health and the environment. Although paper-based lateral flow immunoassay (LFIA) have been extensively applied in mycotoxins monitoring, low-cost, portable, ultrasensitive and quantitative detection is still a formidable challenge. Herein, a series of Fe-N-C single-atom nanozymes (SAzymes) were synthesized and systematic characterized. The optimal Fe-N-C SAzyme with highly efficient catalytic performance was successfully used as both label and catalyst in lateral flow immunoassays for mycotoxin detection. By taking advantage of the catalytic amplified system, the qualitative and quantitative detection can be easily and flexibly done via observing the test lines by naked eyes or a smartphone, with the LODs of 2.8 and 13.9 pg mL -1 for AFB 1 and FB 1 , which were respectively over 700- and 71000-fold lower than the maximum limit set by the European Union. Besides, underlying catalytic mechanisms and the active sites of the Fe-N-C SAzyme are also investigated by DFT simulation. This work not only provided a promising detection strategy for the application of advanced SAzymes but also offers experimental and theoretical guidelines to understand the active centers of Fe-N-C SAzymes and the catalytic process. © 2022, The Authors. All rights reserved.

关键词： Mycotoxins

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First-principles study of the Pr-doped bilayer nickelate La3Ni2O7

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Physical Review B 2025年第19期111卷 195118-195118页

作者： Zihao Huo Peng Zhang Haoliang Shi Xiaochun Yan Defang Duan Tian Cui Key Laboratory of Material Simulation Methods and Software of Ministry of Education State Key Laboratory of Superhard Materials College of Physics Jilin University Changchun 130012 China MOE Key Laboratory for Non-equilibrium Synthesis and Modulation of Condensed Matter Shaanxi Province Key Laboratory of Advanced Functional Materials and Mesoscopic Physics School of Physics Xi'an Jiaotong University Xi'an 710049 China Institute of High Pressure Physics School of Physical Science and Technology Ningbo University Ningbo 315211 China

Recently, the Pr-doped Ruddlesden-Popper (RP) phase of bilayer nickelate La3Ni2O7 has been reported to exhibit a superconducting transition temperature (Tc) of 82.5 K and a superconducting volume fraction of about 57% at high pressure. However, the effect of Pr doping on La3Ni2O7 remains unclear. Here, we studied the crystal structures and electronic properties of Pr-doped La3Ni2O7 at 0 and 15 GPa based on the first-principles calculations to explore the doping effect of Pr. Our findings indicate that the praseodymium atoms prefer to occupy the outer La-O layers site. We then investigated the evolution of crystal structures in both the ambient pressure phase and the high-pressure phase of La3Ni2O7 as a function of doping concentration, revealing inconsistent trends in their evolution with increasing doping levels. Finally, by fitting the bilayer two-orbital model, we propose that doping Pr may reduce the required pressure for the superconductivity of La3Ni2O7. These results not only can help the further experimental search of RP phase nickelate at lower pressure, but also provide a helpful guide for understanding the effect of chemical pressure in an isovalent-doped RP phase nickelate superconductor.

关键词： Crystal atomic structure

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Alloying effect enhanced bimetallic Ni-Fe/TiO 2 catalysts for selective hydrogenation of 1,3-butadiene in the presence of an excess of propylene

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Molecular Catalysis 2023年 550卷

作者： Wei-Hao Wang Bo Jiang Zhao Wang Ya Chen Yao Li Ting-Ting Luo Feng Cheng Bao-Lian Su The State Key Laboratory of Advanced Technology for Material Synthesis and processing Wuhan University of Technology Wuhan 430070 China Center for Materials Research and Analysis Wuhan University of Technology Wuhan 430070 China Laboratory of Inorganic Materials Chemistry (CMI) University of Namur 61 Rue de Bruxelles B-5000 Namur Belgium

Nickel is a promising Pd alternative candidate for selective alkynes/alkadienes hydrogenation owing to its high catalytic activity and cheap price, however, with fatal restrictions of low alkenes selectivity and inferior stability caused by its strong olefin adsorption and the cleavage of carbon-carbon bond. Herein, controlled amounts of iron were introduced into nickel as catalytic assistant by deposition-precipitation with urea on TiO 2 support. Using 1,3-butadiene in an excess of propylene to simulate the industrial process, the additional Fe shows a significant enhancement to the catalytic performance of Ni, i.e., Ni-Fe/TiO 2 with Ni/Fe atomic ratio 1:0.33 shows >94% of 1,3-butadiene conversion and >95% of alkenes selectivity after above 200 h of time on stream, superior to that of commercial Pd/Al 2 O 3 catalyst. Further in-situ analysis reveals that the alloying effect from the formation of Ni-rich Ni-Fe intermetallic compound (e.g., Ni 3 Fe alloy) enlarges the distance between two Ni active sites and enriches the electronic density of Ni sites, resulting in a weak adsorption of butenes products for offering such excellent catalytic performance. To the best of our knowledge, this is the first in-depth exploration on supported Ni-Fe bimetallic catalyst for selective hydrogenation of light alkynes/alkadienes. It shows a high potential for replacing the commercial Pd-based catalysts.

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Bronze TiO2 as a cathode host for lithium-sulfur batteries

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能源化学 2020年第9期48卷 259-266页

作者： Wenjing Dong Di Wang Xiaoyun Li Yuan Yao Xu Zhao Zhao Wang Hong-En Wang Yu Li Lihua Chen Dong Qian 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 Silicate Material for Architectures Wuhan University of Technology Wuhan 430070 Hubei China Beijing National Laboratory of Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing 100190 China Institute of Chemical Materials Chinese Academy of Engineering Physics Mianyang 621900 Sichuan China College of Chemistry and Chemical Engineering Central South University Changsha 410083 Hunan China Laboratory of Inorganic Materials Chemistry (CMI) University of Namur B-5000 Namur Belgium

Lithium-sulfur batteries (LSBs) are very promising for large-scale electrochemical energy ***,dissolution and shuttling of lithium polysulfides (LiPSs) intermediates have severely affected their overall electrochemical properties and limited their practical *** polar cathode hosts that can effectively bind LiPSs and simultaneously promote their redox conversion is crucial for realizing high-performance ***,we report bronze TiO2 (TiO2-B) nanosheets (-5 nm in thickness) chemically bonded with carbon as a novel multifunctional cathode host for advanced *** lobservation and first-principles density functional theory (DFT) calculations reveal that the TiO2-B with exposed (100) plane and Ti3+ ions exhibited high chemical affinity toward polysulfides and effectively confined them at ***,Ti3+ ions and interface coupling with carbon promoted electronic conductivity of the composite cathode,leading to enhanced redox conversion kinetics of LiPSs during charge/***,the as-assembled TiO2-B/S cathode manifested high capacity (1165 mAh/g at 0.2 C),excellent rate capability (244 mAh/g at 5 C) and outstanding cyclability (572 mAh/g over 500 cycles at 0.2 C).This work sheds insights on rational design and fabrication of novel functional electrode materials for beyond Li-ion batteries.

关键词： Titanium dioxide Cathode Polysulfides Shuttle effect Lithium-sulfur batteries Electrochemistry Density functional theory

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Preface to the Special Issue on Photocatalytic H2 Production and CO2 Reduction

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Chinese Journal of Catalysis 2020年第1期41卷 1-1页

作者： Jiaguo Yu Jian Ru Gong Quanjun Xiang State Key Laboratory of Advanced Technology for Material Synthesis and Processing Wuhan University of Technology National Center for Nanoscience and Technology State Key Laboratory of Electronic Thin Film and Integrated Devices University of Electronic Science and Technology of China

Jointly hosted by Wuhan University of technology,Changsha University and Kent state University,the 3rd International Workshop on Graphene and C3N4-based Photocatalysts(IWGCP3)was held at Wuhan University of technology,Wuhan,China on March 23-26,*** workshop was sponsored by National Natural Science Foundation of China(NSFC),Wuhan University of technology,Changsha University,Beijing Perfectlight and *** 300 colleagues from all over the world participated in this workshop,which featured 8 plenary lectures,12 keynote lectures,22 invited lectures,13 oral lectures and 157 *** ten posters enjoyed recognition by the scientific committee during the workshop.

关键词： Wuhan Perfect workshop

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Enhanced stability of highly-dispersed copper catalyst supported by hierarchically porous carbon for long term selective hydrogenation

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催化学报 2020年第7期41卷 1081-1090页

作者： Hu Nian Li Xiaoyun Liu Siming Wang Zhao He Xiaoke Hou Yuexin Wang Yuxiang Deng Zhao Chen Lihua Su Baolian Laboratory of Living Materials Wuhan University of Technology the State Key Laboratory of Advanced Technology for Material Synthesis and Processing Hubei Wuhan 430070 Wuhan University of Technology State Key Laboratory of Silicate Materials for Architectures Hubei Wuhan 430070 Laboratory of Inorganic Materials Chemistry (CMI) University of Namur Belgium Namur B-5000 Clare Hall University of Cambridge Cambridge CB3 9AL

Copper based catalysts have high potential for the substituent of noble-metal based catalysts as their high selectivity and moderate activity for selective hydrogenation reaction; however, achieving further high catalytic stability is very difficult. In this work, the carbonization process of Cu-based organic frameworks was explored for the synthesis of highly-dispersed Cu supported by hierarchically porous carbon with high catalytic performance for selective hydrogenation of 1,3-butadiene. The porous hierarchy of carbon support and the dispersion of copper nanoparticles can be precisely tuned by controlling the carbonization process. The resultant catalyst carbonized at 600 °C exhibits a rather low reaction temperature at 75 °C for 100% butadiene conversion with 100% selectivity to butenes, due to its reasonable porous hierarchy and highly-dispersed copper sites. More importantly, unprecedentedly stability of the corresponding Cu catalyst was firstly observed for selective 1,3-butadiene hydrogenation, with both 100% butadiene conversion and 100% butenes selectivity over 120 h of reaction at 75 °C. This study verifies that a simply control the carbonization process of metal organic frameworks can be an effective way to obtain Cu-based catalysts with superior catalytic performance for selective hydrogenation reaction.

关键词： Hierarchically porous structure Catalyst Cu/C Selective hydrogenation Metal organic frameworks

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Hydrogen/Electron Amphiphilic Bi-Functional Water Molecular Inactivator-Assisted Interface Stabilization in Highly Reversible Zn Metal Batteries

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Angewandte Chemie 2024年第7期137卷

作者： Wenwei Zhang Dr. Shaohua Zhu Tong Yang Lu Wu Jinghao Li Jiang Liang Dr. Yu Liu Lianmeng Cui Chen Tang Xinran Chen Huiqing Zhou Fan Qiao Min Zhou Prof. Ping Luo Fengtong Chi Dr. Xiaobin Liao Prof. Lei Zhang Prof. Qinyou An State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China The State Key Laboratory of Refractories and Metallurgy and Institute of Advanced Materials and Nanotechnology Wuhan University of Science and Technology Wuhan 430081 China School of Chemistry and Chemical Engineering Shanghai Jiao Tong University 800 Dongchuan Road Shanghai 200240 China School of Materials and Chemical Engineering Hubei University of Technology Wuhan 430068 China Hubei Longzhong Laboratory Wuhan University of Technology (Xiangyang Demonstration Zone) Xiangyang Hubei 441000 China Zhongyu Feima New Material Technology Innovation Center (Zhengzhou) Co. Ltd. High Technology Industrial Development Zone Zhengzhou 450001 China

Continuous hydrogen-bond-network in aqueous electrolytes can lead to uncontrollable hydrogen transfer, and combining the interfacial parasitic electron consumption cause the side reaction in aqueous zinc metal batteries (AZMBs). Herein, hydrogen/electron amphiphilic bi-functional 1,5-Pentanediol (PD) molecule was introduced to stabilize the electrode/electrolyte interface. Stronger proton affinity of -OH in PD can break bulk-H 2 O hydrogen-bond-network to inhibit the activity of water, and electron affinity can enhance electron acceptation capability, which ensures that PD is preferentially bound to electrode material over H 2 O. Besides, the participation of PD in the Zn 2+ solvation structure reduces water content at the solid–liquid interface and promotes uniform deposition process by optimizing Zn 2+ de-solvation energy. Accordingly, dense and vertical zinc texture based on intrinsic steric hindrance effect of PD and formed SEI protective layer to induce stable Zinc anode-electrolyte interface. Moreover, an organic–inorganic shielding water layer was formed at the cathode side to suppress vanadium dissolution in vanadium Oxide. Consequently, Zn//Zn symmetric cell could cycle for more than 5600 hours at 1 mAh cm −2 @1 mA cm −2 (more than 250 hours at 50 °C). Besides, the VO 2 and I 2 cathode all achieved stable cycling performance and former pouch cell could reach average capacity of 0.13 Ah.

关键词： Electrode/electrolyte interface Active-water SEI Electron and proton affinity Cathode dissolution

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Solvent-free synthesis of Co single atom and nanocluster decorated N-doped carbon for efficient oxygen reduction

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Chinese Chemical Letters 2024年

作者： Xinyuan Li Zhuozhu Li Wenzhong Huang Jiantao Li Wei Zhang Shihao Feng Hao Fan Zhuo Chen Sungsik Lee Congcong Cai Liang Zhou Hubei Longzhong Laboratory Wuhan University of Technology (Xiangyang Demonstration Zone) Xiangyang 441000 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China Chemical Sciences and Engineering Division Argonne National Laboratory Lemont IL 60439 United States X-ray Science Division Argonne National Laboratory Lemont IL 60439 United States Zhongyu Feima New Material Technology Innovation Center (Zhengzhou) Co. Ltd. High Technology Industrial Development Zone Zhengzhou 450001 China

The advancement of efficient, cheap, and durable catalysts for oxygen reduction reaction (ORR) to substitute Pt/C in metal-air batteries is of paramount importance. However, traditional solvent-based methods fall short in terms of environmental benign and scalability. Herein, a solvent-free organic-inorganic self-assembly approach is explored to construct cobalt single atom and cobalt nanocluster decorated nitrogen-doped porous carbon spheres (Co-SA/NC@NCS). The solvent-free synthesis demonstrates an impressively high yield (282 g/L) and the resultant Co-SA/NC@NCS possesses a high N content (6.9 wt%). Density functional theory calculations disclose that the Co-SAs and Co-NCs are able to optimize the surface oxygen adsorption capability and enhance the conductivity of the NCS, thereby facilitating the ORR performance. The solvent-free synthesis is also feasible for the synthesis of other non-noble metal element (Fe, Ni, and Zn) decorated nitrogen-doped porous carbon spheres.

关键词： Organic-inorganic self-assembly Nitrogen-doped carbon Oxygen reduction reaction Single atom catalyst Zn-air battery

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Effect of Constituent Core-sizes on Microstructure and Dielectric Properties of BaTiO_3@(0.6BaTiO_3-0.4BiAlO_3) Core-Shell material

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Journal of Wuhan University of technology(materials Science) 2018年第3期33卷 589-597页

作者： APPIAH Millicent 郝华 CHEN Wenjin CHEN Cheng YAO Zhonghua CAO Minghe LIU Hanxing State Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of Material Science and EngineeringWuhan University of Technology International School of Materials Science and Engineering Wuhan University of Technology

The fundamental characteristics of varied initial core-sizes of Ba Ti O3（BT） and its influential role on the morphology and dielectric properties of Ba Ti O3@0.6 Ba Ti O3-0.4 Bi Al O3（BT@0.6 BT-0.4 BA） ceramic samples were studied. Alkoxide sol-precipitation method was adopted as revised chemical route to synthesize the constituent ＂core＂ BT powders in a dispersed phase, whereas the distinctive initial nano-sized particles were affected by the pre-calcination temperatures（600-900 ℃）.The microstructure of the uncoated BT ceramics revealed an exaggerated grain growth with an optimized dielectric constant（ε（max）〉9 000） whilst the coated ceramics behaved otherwise（grain growth inhibited） when sintered at an elevated temperature. Regardless of the previously studied solubility limit（about 0.1%） of BT-BA samples, BT@0.6 BT-0.4 BA maintained a maximum dielectric constant（ε（max）） ranging from 1 592 to 1 708 and tan δ less than 2% under a unit mole ratio at room temperature. In view of all these analyses, the initial nanometer sizes of the as-prepared BT-core powders combined with the increase effect of cation substitutions of Bi^（3＋） and Al^（3＋） in the shell content, induced the diffuse transition phase of BT@0.6 BT-0.4 BA composition.

关键词： MLCCs core-shell Alkoxide sol-precipitation relaxor grain boundary segregation

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