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Chinese Chemical Letters 2024年第5期35卷 45-56页

作者： Feifei Wang Hang Yao Xinyue Wu Yijian Tang Yang Bai Hui Chong huan pang School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225002China School of Pharmacy Changzhou UniversityChangzhou 213164China State Key Laboratory of Coordination Chemistry Nanjing UniversityNanjing 210023China

Metal-organic framework(MOF)is a periodic sexual network structure with large surface area and high porosity,which is assembled by inorganic nodes and organic ligands through coordinate covalent bond.MOFs have the advantages of controllable pore size and shape,large specific surface area,easy modification and more active sites.In addition,MOF based nanoenzymes display excellent enzyme catalytic activity due to their special structure and multiple exposed metal active sites,controlling the production of reactive oxygen species(ROS)in cells or the body,and thus regulating the polarization of macrophage.This article reviews the mechanism of MOF material regulating macrophage polarization and the function of macrophages with different phenotypes.By utilizing the excellent properties of MOFs and the advantages of combining them with bioactive materials,we have discovered their excellent applications in the treatment of inflammatory diseases.Finally,we discussed the current challenges and prospects faced by MOF based composite materials.We expect that the research in this developing field will play a more important role in combating inflammatory diseases in the field of nanomedicine.

关键词： Metal-organic framework Inflammation Macrophage polarization Reactive oxygen species Nanozyme activity

Durable hierarchical phosphorus‐doped biphase MoS_(2)electrocatalysts with enhanced H^(*)adsorption

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Carbon Energy 2024年第4期6卷 104-114页

作者： Yongteng Qian Jianmin Yu Zhiyi Lyu Qianwen Zhang Tae Hyeong Lee huan pang Dae Joon Kang College of Pharmacy Jinhua PolytechnicJinhuaZhejiangChina Department of Physics Sungkyunkwan UniversitySuwonGyeonggi‐doRepublic of Korea International Collaborative Laboratory of 2D Materials for Optoelectronic Science and Technology of Ministry of Education Institute of Microscale OptoelectronicsShenzhen UniversityShenzhenGuangdongChina School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhouJiangsuChina

Phase engineering is an efficient strategy for enhancing the kinetics of electrocatalytic reactions.Herein,phase engineering was employed to prepare high‐performance phosphorous‐doped biphase(1T/2H)MoS_(2)(P‐BMS)nanoflakes for hydrogen evolution reaction(HER).The doping of MoS_(2)with P atoms modifies its electronic structure and optimizes its electrocatalytic reaction kinetics,which significantly enhances its electrical conductivity and structural stability,which are verified by various characterization tools,including X‐ray photoelectron spectroscopy,high‐resolution transmission electron microscopy,X‐ray absorption near‐edge spectroscopy,and extended X‐ray absorption fine structure.Moreover,the hierarchically formed flakes of P‐BMS provide numerous catalytic surface‐active sites,which remarkably enhance its HER activity.The optimized P‐BMS electrocatalysts exhibit low overpotentials(60 and 72 mV at 10 mA cm^(−2))in H_(2)SO_(4)(0.5 M)and KOH(1.0 M),respectively.The mechanism of improving the HER activity of the material was systematically studied using density functional theory calculations and various electrochemical characterization techniques.This study has shown that phase engineering is a promising strategy for enhancing the H*adsorption of metal sulfides.

关键词： 1T/2H MoS_(2) density functional theory electrocatalysts phase engineering phosphorous doping

Core-shell heterostructure by coupling layered ReS_(2) with Co_(9)S_(8) nanocubes for boosted oxygen evolution reaction

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Chinese Chemical Letters 2024年第3期35卷 518-522页

作者： Xu Yu Zhiqiang Pan Chengang Pei Longjie Lin Yanhui Lu Ho Seok Park huan pang School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225009China School of Chemical Engineering Sungkyunkwan University2066Seobu-roJangan-guSuwon-siGyeonggi-do 440-746Republic of Korea

The controllable morphology and composition of catalysts are crucial to improving the electrocatalytic activity of oxygen evolution reaction(OER).Herein,we construct a bimetallic heterostructure by sulfidation and hydrothermal methods,and the layered ReS_(2)is vertically aligned on Prussian blue-derived hollow Co_(9)S_(8)nanocubes(Co_(9)S_(8)@ReS_(2)).The core-shell structure of Co_(9)S_(8)@ReS_(2)can effectively prevent the restacking of layered ReS_(2),expose the abundant surface area and improve the utilization of electrocatalytic sites,resulting in fast electrolyte diffusion and charge transfer during OER.Due to the synergistic effect of the core-shell morphology and the formed bimetallic heterostructure,Co_(9)S_(8)@ReS_(2)exhibits excellent catalytic OER performance.At 10 mA/cm^(2),only 288 mV of overpotential is required with the Tafel slope of 73.3 mV/dec for Co_(9)S_(8)@ReS_(2),which are both lower than that of Co_(9)S_(8)and ReS_(2).Meanwhile,Co_(9)S_(8)@ReS_(2)exhibits high catalytic stability and low charge transfer resistance and the boosted active sites are confirmed by density functional theory.This work provides a rational design of the OER catalysts by constructing the bimetallic heterostructure.

关键词： Oxygen evolution reaction Rhenium disulfide Metal-organic framework Heterostructure Core-shell

Ultrathin curved PdNiRu nanosheets as bifunctional catalysts for oxygen reduction and ethylene glycol oxidation

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Nano Research 2024年第5期17卷 3777-3784页

作者： Xianzeng Li Tingyu Lu huan pang Mingyi Zhang Dongdong Xu Lin Xu Min Han Jun Yang Jiangsu Key Laboratory of New Power Batteries Jiangsu Collaborative Innovation Center of Biomedical Functional MaterialsSchool of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023China Fujian Cross Strait Institute of Flexible Electronics(Future Technology) Fujian Normal UniversityFuzhou 350117China State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China State Key Laboratory of Coordination Chemistry Nanjing UniversityNanjing 210023China School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225009China Key Laboratory for Photonic and Electronic Bandgap Materials Ministry of EducationSchool of Physics and Electronic EngineeringHarbin Normal UniversityHarbin 150025China

Pd-based metallic nanosheets with advanced physicochemical properties have been widely prepared and employed in various electrocatalytic reactions.However,few concerns were focused on their multiple performances in different electrocatalysis.Here,highly curved and ultrathin PdNiRu nanosheets(NSs)are developed by facile wet-chemistry strategy and exhibit excellent electrocatalytic performance toward both oxygen reduction reaction(ORR)and ethylene glycol oxidation reaction(EGOR).Owing to the synergistically structural(e.g.,ultrathin,curved,defects/steps-rich)and compositional(ternary alloy)advantages,PdNiRu NSs exhibited enhanced ORR and EGOR specific/mass activities and better stability/durability than control electrocatalysts.The specific activity(5.52 mA·cm^(−2))and mass activity(1.13 A·mg_(Pd)^(−1))of the PdNiRu NSs in ORR are 4.8 and 3.4 times as the ones of commercial Pt/C,respectively.The mass activity of PdNiRu NSs(3.86 A·mg_(Pd)^(−1))in EGOR is 2.6 times as commercial Pd/C(1.51 A·mg_(Pd)^(−1)).This study is helpful for the development of desired electrocatalysts with multi-functional application in practical fuel cells.

关键词： ultrathin nanosheets noble metal electrocatalysts bifunctional

Manipulating d-d orbital hybridization induced by Mo-doped Co_(9)S_(8) nanorod arrays for high-efficiency water electrolysis

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Journal of Energy Chemistry 2024年第6期93卷 592-600,I0015页

作者： Xue Zhou Jing Li Guangyao Zhou Weiran huang Yucan Zhang Jun Yang huan pang Mingyi Zhang Dongmei Sun Yawen Tang Lin Xu Jiangsu Key Laboratory of New Power Batteries Jiangsu Collaborative Innovation Centre of Biomedical Functional MaterialsSchool of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023JiangsuChina 'College of Science Jinling Institute of TechnologyNanjing 211169JiangsuChina State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Nanjing IPE Institute of Green Manufacturing Industry Nanjing 211100JiangsuChina School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225009JiangsuChina Key Laboratory for Photonic and Electronic Bandgap Materials Ministry of EducationSchool of Physics and Electronic EngineeringHarbin Normal UniversityHarbin 150025HeilongjiangChina

Precisely refining the electronic structure of electrocatalysts represents a powerful approach to further optimize the electrocatalytic performance.Herein,we demonstrate an ingenious d-d orbital hybridization concept to construct Mo-doped Co_(9)S_(8) nanorod arrays aligned on carbon cloth(CC)substrate(abbreviated as Mo-Co_(9)S_(8)@CC hereafter)as a high-efficiency bifunctional electrocatalyst toward water electrolysis.It has experimentally and theoretically validated that the 4d-3d orbital coupling between Mo dopant and Co site can effectively optimize the H_(2)O activation energy and lower H^(*)adsorption energy barrier,thereby leading to enhanced hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)activities.Thanks to the unique electronic and geometrical advantages,the optimized Mo-Co_(9)S_(8)@CC with appropriate Mo content exhibits outstanding bifunctional performance in alkaline solution,with the overpotentials of 75 and 234 mV for the delivery of a current density of 10 mA cm^(-2),small Tafel slopes of 53.8 and 39.9 mV dec~(-1)and long-term stabilities for at least 32 and 30 h for HER and OER,respectively.More impressively,a water splitting electrolylzer assembled by the self-supported Mo-Co_(9)S_(8)@CC electrode requires a low cell voltage of 1.53 V at 10 mA cm^(-2)and shows excellent stability and splendid reversibility,demonstrating a huge potential for affordable and scalable electrochemical H_(2) production.The innovational orbital hybridization strategy for electronic regulation herein provides an inspirable avenue for developing progressive electrocatalysts toward new energy systems.

关键词： d-d orbital hybridization Transition metal sulfides Nanorods arrays Water electrolysis

Imide-based covalent organic framework with excellent cyclability as an anode material for lithium-ion battery

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Chinese Chemical Letters 2024年第6期35卷 206-210页

作者： Yue Qian Zhoujia Liu Haixin Song Ruize Yin Hanni Yang Siyang Li Weiwei Xiong Saisai Yuan Junhao Zhang huan pang School of Environmental&Chemical Engineering Jiangsu University of Science and TechnologyZhenjiang 212003China School of Chemistry&Chemical Engineering Yangzhou UniversityYangzhou 225009China Shandong Key Laboratory of Biochemical Analysis College of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China

Covalent organic frameworks(COFs)exhibiting reversible redox behaviors have been identified as promising candidates for constructing electrode materials in lithium-ion batteries(LIBs).However,their extensive application has been limited due to finite redox sites and poor structural stability.In this study,we design and synthesize a novel polyimide covalent organic framework(PI-COF)using the traditional solvothermal method and successfully apply it as an anode material for LIBs.The large conjugated structure of PI-COF accelerates charge transfer,while its large surface area provides more active sites,making PI-COF an attractive anode material for LIBs.Furthermore,the PI-COF anode material demonstrates high reversible specific capacity and excellent long-term cycling stability due to its COF characteristics.Specifically,the PI-COF electrodes deliver a specific capacity of 800 m Ah/g at a current density of 200 m A/g after 200 cycles,while a specific capacity of 450 m Ah/g at a current density of 1000 m A/g is sustained after 800 cycles.The outstanding lithium storage capacity,particularly the satisfactory long-term cycling stability,establishes PI-COF as a promising material for LIBs.

关键词： Ethylenediaminetetraacetic dianhydride Covalent organic frameworks Polyimide Lithium-ion battery Anode material

MnO-pillared graphene blocks enabling the ultrastable and ultrafast aqueous zinc ion batteries

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Science China Chemistry 2024年

作者： Zheng Liu Zhipeng Qiu Zhiyuan Li Tong Wei Zhuangjun Fan huan pang School of Chemistry and Chemical Engineering Yangzhou University School of Materials Science and Engineering China University of PetroleumQingdao

Due to the low cost, high theoretical capacity, and environmental friendliness, manganese-based cathodes are regarded as promising alternatives for aqueous zinc ion batteries（AZIBs）. However, the practicality of the zinc-manganese system is faced with great challenges, such as the inevitable structural collapse of the cathode and controversial energy storage mechanisms.Herein, we propose a novel concept of spatial deposition mechanism through the addition of MnSO4additives in the MnOpillared graphene blocks（G-MnO）. The covalent interface between MnO nanoparticles and multilayered graphene nanosheets can construct an in-built micro-electric field, which is beneficial for consecutive electron transfer（in both horizontal and vertical directions）. On this basis, the surficial activity of MnO confined in the interlayered nano-space is greatly enhanced and provides enough spatial deposition and subsequent reaction site for MnSO4additives, thus firstly extending the surficial controlled process to stereoscopic space, effectively improving the electrochemical performance of AZIBs. Therefore, the assembled Zn//G-MnO battery exhibits an excellent rate capability of 281.5 mAh g-1at 0.1 A g-1and 106 m Ah g-1at 20 A g-1, and impressive cycling stability(93 m Ah g-1remaining after 5,000 cycles). This finding may provide a new opportunity for the rational design of surficial controlled energy storage and conversion devices.

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Electrochemical reconstruction: a new perspective on Sn metal-organic complex microbelts as robust anode for lithium storage

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Rare Metals 2024年第1期43卷 76-86页

作者： Jin-Ke Shen Nai-Teng Wu Li-Yuan Wang Gang Jiang Dong-Lei Guo Jin Li Gui-Long Liu Hong-Yu Mi huan pang Xian-Ming Liu Key Laboratory of Function-oriented Porous Materials of Henan Province College of Chemistry and Chemical EngineeringLuoyang Normal UniversityLuoyang 471934China State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources School of Chemical Engineering and TechnologyXinjiang UniversityUrumqi 830046China School of Chemistry and Chemical Engineering Institute for Innovative Materials and EnergyYangzhou UniversityYangzhou 225009JiangsuChina

Tin-based materials with high theoretical capacity and suitable working voltage are ideal anode materials for lithium-ion batteries(LIBs). However, to overcome their shortcomings(volume expansion and inferior stability), the preparation processes are usually complicated and expensive. Herein, a tin-based metal-organic complex(tin 1,2-benzenedicarboxylic acid, Sn-BDC)with one-dimensional microbelt morphology is synthesized by a facile, rapid and low-cost co-precipitation method, and served as anode material for LIBs without any post-treatment. Sn-BDC exhibits a high reversible capacity with609/440 m Ah·g^(-1) at 50/2000 m A·g^(-1), and robust cycling stability of 856 m Ah·g^(-1) after 200 cycles at 200 m A·g^(-1),which are obviously superior to that of the Sn Ox/C counterparts. Moreover, an electrochemical reconstruction perspective on the lithium storage mechanism of Sn-BDC is proposed by systematic ex-situ characterizations. The reconstructed SnO_(2) replaces Sn-BDC and becomes the active material in the subsequent cycles. As the by-product of the lithiation reaction, the formed Li-based metal-organic complex(Li-BDC, wrapped around the reconstructed SnO_(2)) plays an important role in alleviating volume expansion and accelerating the charge transfer kinetics.This work is beneficial to design and construct the new electrode materials based on the electrochemical reconstruction for advanced LIBs.

关键词： Electrochemical reconstruction Metal-organic complex Anode Lithium storage mechanism Lithium-ion batteries

An aqueous rechargeable Fe//LiMn_(2)O_()hybrid battery with superior electrochemical performance beyond mainstream Fe-based batteries

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Nano Research 2024年第6期17卷 5168-5178页

作者： Yu Liu Dehui Xie Yuxin Shi Rongguan Lv Yingna Chang Yuzhen Sun Zhiyuan Zhao Jindi Wang Kefan Song Huayu Wu Tuan K.A.Hoang Rong Xing huan pang Institute of New Energy on Chemical Storage and Power Sources School of Chemical and Environmental EngineeringYancheng Teachers UniversityYancheng 224000China School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225009China Department of Chemical Engineering University of Waterloo200 University Avenue WestWaterlooOntario N2L 3G1Canada

Aqueous rechargeable batteries(ARBs)are generally safer than non-aqueous analogues,they are also less-expensive,and more friendly to the environment.However,the inherent disadvantage of the narrow electrochemical window of H2O seriously restricts the energy density and output voltage of ARBs,especially aqueous rechargeable Fe-based batteries.Herein,we introduce a new battery system:the anode contains C@Fe/Fe_(2)O_(3)composite,which is interfaced with an alkaline electrolyte;the cathode contains LiMn_(2)O_()in contact with a neutral electrolyte.A Li^(+)-conducting membrane is carefully selected to decouple the electrode-electrolyte,which effectively widens the electrochemical window to above 2.65 V,thereby enables an aqueous rechargeable iron battery.Its average output voltage is 1.83 V and its energy density is 235.3 Wh/kg at 549 W/kg.In this work,we propose the energy storage mechanism with the aid of density functional theory(DFT).The calculated reduction potential of the anode agrees with the experimental value.Furthermore,this battery system demonstrates long cycle lifespan of approximately 2500 cycles at 2 A/g,corresponding to a capacity retention of 82.1%.These results are very far superior than those of mainstream aqueous rechargeable Fe-based batteries,which guarantee future investigation for storing electricity energy.

关键词： aqueous battery high voltage high energy iron oxide theoretical calculation

Dual-ligand and hard-soft-acid-base strategies to optimize metal-organic framework nanocrystals for stable electrochemical cycling performance

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National Science Review 2022年第7期9卷 88-96页

作者： Shasha Zheng Yan Sun Huaiguo Xue Pierre Braunstein Wei huang huan pang School of Chemistry and Chemical Engineering Yangzhou University Institut de Chimie UMR 7177 Universite′ de StrasbourgCNRS State Key Laboratory of Organic Electronics and Information Displays and Institute of Advanced Materials (IAM)Nanjing University of Posts and Telecommunications Frontiers Science Center for Flexible Electronics (FSCFE) MIIT Key Laboratory of Flexible Electronics (KLo FE)Northwestern Polytechnical University

Most metal-organic frameworks(MOFs) hardly maintain their physical and chemical properties after exposure to acidic,neutral,or alkaline aqueous solutions,resulting in insufficient stability,therefore limiting their applications.Thus,the design and synthesis of stable size/morphology-controlled MOF nanocrystals is critical but challenging.In this study,dual-ligand and hard-soft-acid-base strategies were used to fabricate a variety of 3D pillared-layer [Ni(thiophene-2,5-dicarboxylate)(4,4’-bipyridine)]nMOF nanocrystals(1D nanofibers,2D nanosheets and 3D aggregates) with controllable morphology by varying the concentration of 4,4’-bipyridine and thus controlling the crystal growth direction.Owing to the shorter ion diffusion length,enhanced ele ctron/ion transfer and strong interactions between thiophene-2,5-dicarboxylate and4,4’-bipyridine,the 2D nanosheets showed much larger specific capacitance than 1D nanofibers and 3D aggregates.A single device with an output voltage as high as 3.0 V and exceptional cycling performance(95% of retention after 5000 cycles at 3 mA cm-2) was realized by configuring two aqueous asymmetric super capacitive devices in series.The excellent cycling property and charge-discharge mechanism are consistent with the hard-soft-acid-base theory.

关键词： metal-organic framework dual ligand hard-soft-acid-base electrochemical energy storage supercapacitor