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Self-supported NiFe-LDH nanosheets on NiMo-based nanorods as high-performance bifunctional electrocatalysts for overall water splitting at industrial-level current densities

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Nano Research 2024年第5期17卷 3769-3776页

作者： Yan Zhang Biao Feng MingLei Yan Zhen Shen Yiqun Chen Jingyi Tian Fengfei Xu Guanghai Chen Xizhang Wang Lijun Yang Qiang Wu Zheng Hu key laboratory of mesoscopic chemistry of Ministry of Education(moe)and jiangsu provincial Lab for nanotechnology School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China College of Water Conservancy and Hydropower Engineering Sichuan Agricultural UniversityYa’an 625014China

Efficient,durable and economic electrocatalysts are crucial for commercializing water electrolysis technology.Herein,we report an advanced bifunctional electrocatalyst for alkaline water splitting by growing NiFe-layered double hydroxide(NiFe-LDH)nanosheet arrays on the conductive NiMo-based nanorods deposited on Ni foam to form a three-dimensional(3D)architecture,which exhibits exceptional performances for both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).In overall water splitting,only the low operation voltages of 1.45/1.61 V are required to reach the current density of 10/500 mA·cm^(-2),and the continuous water splitting at an industrial-level current density of 500 mA·cm^(-2) shows a negligible degradation(1.8%)of the cell voltage over 1000 h.The outstanding performance is ascribed to the synergism of the HER-active NiMo-based nanorods and the OER-active NiFe-LDH nanosheet arrays of the hybridized 3D architecture.Specifically,the dense NiFe-LDH nanosheet arrays enhance the local pH on cathode by retarding OH-diffusion and enlarge the electrochemically active surface area on anode,while the conductive NiMo-based nanorods on Ni foam much decrease the charge-transfer resistances of both electrodes.This study provides an efficient strategy to explore advanced bifunctional electrocatalysts for overall water splitting by rationally hybridizing HER-and OER-active components.

关键词： alkaline water splitting bifunctional electrocatalysts layered double hydroxides high durability industrial current densities

Defect-induced deposition of manganese oxides on hierarchical carbon nanocages for high-performance lithium-oxygen batteries

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Nano Research 2022年第5期15卷 4132-4136页

作者： Baoxing Wang Chenxia Liu Lijun Yang Qiang Wu Xizhang Wang Zheng Hu key laboratory of mesoscopic chemistry of moe and jiangsu provincial laboratory for nanotechnology School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

The cathode of lithium-oxygen(Li-O_(2))batteries should have large space for high Li_(2)O_(2) uptake and superior electrocatalytic activity to oxygen evolution/reduction for long lifespan.Herein,a high-performance MnO_(x)/hCNC cathode was constructed by the defect-induced deposition of manganese oxide(MnOx)nanoparticles on hierarchical carbon nanocages(hCNC).The corresponding Li-O2 battery(MnOx/hCNC@Li-O_(2))exhibited excellent electrocatalytic activity with the low overpotential of 0.73-0.99 V in the current density range of 0.1-1.0 A·g^(-1).The full discharge capacity and cycling life of MnO_(x)/hCNC@Li-O_(2) were increased by~86.7%and~91%,respectively,compared with the hCNC@Li-O_(2) counterpart.The superior performance of MnO_(x)/hCNC cathode was ascribed to(i)the highly dispersed MnO_(x) nanoparticles for boosting the reversibility of oxygen evolution/reduction reactions,(ii)the interconnecting pore structure for increasing Li_(2)O_(2) accommodation and facilitating charge/mass transfer,and(iii)the concealed surface defects of hCNC for suppressing side reactions.This study demonstrated an effective strategy to improve the performance of Li-O_(2) batteries by constructing cathodes with highly dispersed catalytic sites and hierarchical porous structure.

关键词： Li-O_(2) batteries hierarchical carbon nanocages manganese oxide electrocatalysis defect-induced deposition

Boosting faradaic efficiency of CO_(2)electroreduction to CO for Fe-NC single-site catalysts by stabilizing Fe^(3+)sites via F-doping

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Nano Research 2022年第9期15卷 7896-7902页

作者： Yiqun Chen Guochang Li Yu Zeng Lijie Yan Xizhang Wang Lijun Yang Qiang Wu Zheng Hu key laboratory of mesoscopic chemistry of moe and jiangsu provincial Lab for nanotechnology School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

The atomically dispersed Fe^(3+)sites of Fe-N-C single-site catalysts(SSCs)are demonstrated as the active sites for CO_(2)electroreduction(CO_(2)RR)to CO but suffer from the reduction to Fe^(2+)at~−0.5 V,accompanied by the drop of CO faradaic efficiency(FECO)and deterioration of partial current(JCO).Herein,we report the construction of F-doped Fe-N-C SSCs and the electron-withdrawing character of fluorine could stabilize Fe3+sites,which promotes the FECO from the volcano-like highest value(88.2%@−0.40 V)to the high plateau(>88.5%@−0.40-−0.60 V),with a much-increased JCO(from 3.24 to 11.23 mA·cm^(−2)).The enhancement is ascribed to the thermodynamically facilitated CO_(2)RR and suppressed competing hydrogen evolution reaction,as well as the kinetically increased electroactive surface area and improved charge transfer,due to the stabilized Fe^(3+)sites and enriched defects by fluorine doping.This finding provides an efficient strategy to enhance the CO_(2)RR performance of Fe-N-C SSCs by stabilizing Fe^(3+).

关键词： carbon dioxide electroreduction iron-nitrogen-carbon single-site catalysts fluorine-doping active site regulation

Advanced non-precious electrocatalyst of the mixed valence CoO_x nanocrystals supported on N-doped carbon nanocages for oxygen reduction

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Science China chemistry 2015年第1期58卷 180-186页

作者： Sheng Chen Liwei Wang Qiang Wu Xiang Li Yu Zhao Hongwei Lai Lijun Yang Tao Sun Yi Li Xizhang Wang Zheng Hu key laboratory of mesoscopic chemistry of Ministry of Education jiangsu provincial Lab for nanotechnology School of chemistry and Chemical Engineering Nanjing University

Taking advantage of the nitrogen(N)-participation and large surface area of N-doped carbon nanocages(NCNCs),the Co Ox nanocrystals are conveniently immobilized onto the NCNCs with high dispersion.The Co Ox/NCNCs hybrid exists in the mixed valence with predominant Co O over Co3O4 and demonstrates superb oxygen reduction reaction activity and stability remaining^94%current density even after operation over 100 h.These results suggest a promising strategy to develop advanced electrocatalysts with the novel NCNCs or even beyond.

关键词：氧还原反应纳米晶体混合价纳米笼 N掺杂金属电极碳四氧化三钴

DOXORUBICIN-LOADED BORON-RICH POLYMER NANOPARTICLES FOR ORTHOTOPICALLY IMPLANTED LIVER TUMOR TREATMENT

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Chinese Journal of Polymer Science 2013年第5期31卷 778-786页

作者： Lu-zhong Zhang Ya-jun Zhang 武伟蒋锡群 laboratory of mesoscopic chemistry and Department of Polymer Science & Engineering College of Chemistry & Chemical Engineering jiangsu provincial laboratory for nanotechnology Nanjing University jiangsu key laboratory of Neuroregeneration Nantong University

The in vivo behaviors of doxorubicin （DOX）-loaded dextran-poly（3-acrylamidophenylboronic acid）（Dextran- PAPBA） nanoparticles （NPs） were studied. The DOX-loaded NPs had a narrowly distributed diameter of ca. 74 nm and mainly accumulated in liver of tumor-bearing mice after intravenous injection as demonstrated by in vivo real-time near infrared fluorescent imaging. The DOX contents in various tissues were quantified and consisted well with the results of fluorescent imaging. The biodistribution pattern of DOX-loaded NPs encourages us to investigate their liver tumor treatment by using an orthotopically implanted liver tumor model, revealing that the DOX-loaded NPs formulation had better antitumor effect than free DOX.

关键词： Dextran-PAPBA nanoparticles DOX Drug delivery Antitumor.

Flexible capacitive pressure sensor based on interdigital electrodes with porous microneedle arrays for physiological signal monitoring

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nanotechnology and Precision Engineering 2024年第1期7卷 18-31页

作者： Jiahui Xu Minghao Wang Minyi Jin Siyan Shang Chuner Ni Yili Hu Xun Sun Jun Xu Bowen Ji Le Li Yuhua Cheng Gaofeng Wang School of Electronics&Information MOE Engineering Research Center of Smart Microsensors and MicrosystemsHangzhou Dianzi UniversityHangzhou 310018China Wenzhou Institute of Hangzhou Dianzi University Wenzhou 310018China key laboratory of Intelligent Operation and Maintenance Technology&Equipment for Urban Rail Transit of Zhejiang Province College of EngineeringInstitute of Precision Machinery and Smart StructureZhejiang Normal UniversityJinhua 321004China Institute of Guizhou Aerospace Measuring and Testing Technology Guiyang 550009China Unmanned System Research Institute Northwestern Polytechnical UniversityXi’an 710072China Research&Development Institute of Northwestern Polytechnical University in Shenzhen Shenzhen 518057China

Flexible pressure sensors have many potential applications in the monitoring of physiological signals because of their good biocompatibil-ity and wearability.However,their relatively low sensitivity,linearity,and stability have hindered their large-scale commercial application.Herein,aﬂexible capacitive pressure sensor based on an interdigital electrode structure with two porous microneedle arrays(MNAs)is pro-posed.The porous substrate that constitutes the MNA is a mixed product of polydimethylsiloxane and NaHCO3.Due to its porous and interdigital structure,the maximum sensitivity(0.07 kPa-1)of a porous MNA-based pressure sensor was found to be seven times higher than that of an imporous MNA pressure sensor,and it was much greater than that of aﬂat pressure sensor without a porous MNA structure.Finite-element analysis showed that the interdigital MNA structure can greatly increase the strain and improve the sensitivity of the sen-sor.In addition,the porous MNA-based pressure sensor was found to have good stability over 1500 loading cycles as a result of its bilayer parylene-enhanced conductive electrode structure.Most importantly,it was found that the sensor could accurately monitor the motion of aﬁnger,wrist joint,arm,face,abdomen,eye,and Adam’s apple.Furthermore,preliminary semantic recognition was achieved by monitoring the movement of the Adam’s apple.Finally,multiple pressure sensors were integrated into a 33 array to detect a spatial pressure distribu-×tion.Compared to the sensors reported in previous works,the interdigital electrode structure presented in this work improves sensitivity and stability by modifying the electrode layer rather than the dielectric layer.

关键词： Capacitive pressure sensor Microneedle array Porous PDMS Interdigital electrode

Micro–meso-macroporous FeCo-N-C derived from hierarchical bimetallic FeCo-ZIFs as cathode catalysts for enhanced Li-O2 batteries performance

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Journal of Energy chemistry 2019年第8期28卷 212-219,I0008页

作者： Fufang Chao Baoxing Wang Jiaojiao Ren Yingwei Lu Wenrui Zhang Xizhang Wang Lin Cheng Yongbing Lou Jinxi Chen School of chemistry and Chemical Engineering Jiangsu Engineering Laboratory of Smart Carbon-Rich Materials and Device Southeast UniversityNanjing 211189 Jiangsu China key laboratory of mesoscopic chemistry of moe Jiangsu Provincial Lab for Nanotechnology School of Chemistry and Chemical Engineering Nanjing UniversityNanjing 210093 Jiangsu China

Developing bifunctional catalysts that increase both the OER and ORR kinetics and transport reactants with high efficiency is desirable. Herein, micro–meso-macroporous FeCo-N-C-X(denoted as "MFeCo-N-C-X", X represents Fe/Co molar ratio in bimetallic zeolite imidazole frameworks FeCo-ZIFs) catalysts derived from hierarchical M-FeCo-ZIFs-X was prepared. The micropores in M-FeCo-N-C-X have strong capability in O2 capture as well as dictate the nucleation and early-stage deposition of Li2O2,the mesopores provided a channel for the electrolyte wetting, and the macroporous structure promoted more available active sites when used as cathode for Li-O2 batteries. More importantly, M-Fe CoN-C-0.2 based cathode showed a high initial capacity(18,750 mAh g-1@0.1 A g-1), good rate capability(7900 m Ah g-1@0.5 A g-1), and cycle stability up to 192 cycles. Interestingly, the FeCo-N-C-0.2 without macropores suffered relatively poorer stability with only 75 cycles, although its discharge capacity was still as high as 17,200 mA h g-1(@0.1 A g-1). The excellent performance attributed to the synergistic contribution of homogeneous Fe, Co nanoparticles and N co-doping carbon frameworks with special micro–meso-macroporous structure. The results showed that hierarchical FeCo-N-C architectures are promising cathode catalysts for Li-O2 batteries.

关键词： Micro–meso-macroporous FeCo-N-C Li-O2 battery Cathode catalyst Oxygen evolution/reduction reaction

Single molecular insight into steric effect on C-terminal amino acids with various hydrogen bonding sites

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Chinese Chemical Letters 2022年第10期33卷 4649-4654页

作者： Yunzhi Xie Chunhua Liu Linxiu Cheng Yulan Fan Huifang Li Wei Liu Lei Zhu Xun Li Ke Deng Qingdao Zeng Shoufa Han State key laboratory for Physical chemistry of Solid Surfaces Department of Chemical BiologyCollege of Chemistry and Chemical EngineeringThe Key Laboratory for Chemical Biology of Fujian ProvinceThe MOE Key Laboratory of Spectrochemical Analysis&Instrumentationand Innovation Center for Cell Signaling NetworkXiamen UniversityXiamen 361005China Jiangxi provincial key laboratory of Low-Carbon Solid Waste Recycling School of Geography and Environmental EngineeringGannan Normal UniversityGanzhou 341000China Jiangxi key laboratory of Organo-Pharmaceutical chemistry Chemistry and Chemical Engineering CollegeGannan Normal UniversityGanzhou 341000China CAS key laboratory of Standardization and Measurement for nanotechnology CAS Center for Excellence in NanoscienceNational Center for Nanoscience and Technology(NCNST)Beijing 100190China

Amino acids are basic units to construct a protein with the assistance of various interactions.During this building process,steric hindrance derived from amino acid side groups or side chains is a factor that could not be ignored.In this contribution,adsorption behaviors of C-terminal amino acid derivatives with amino acid residues fused in 3,4,9,10-perylenetetracarboxylic dianhydride were investigated by scanning tunneling microscopy(STM)and density functional theory(DFT)calculations at various liquid/solid interfaces.STM results at 1-phenyloctane/HOPG interface show that N,N'-3,4,9,10-perylenedicarboximide(GP)and N,N'-methyl-3,4,9,10-perylenedicarboximide(AP)formed linear and herringbone structures,respectively.The driving force could be attributed to different H-bonding sites induced by steric hindrance at side groups.N,N'-Benzyl-3,4,9,10-perylenedicarboximide(PP)generates both linear and herringbone structures because steric hindrance changes the H-bonding sites between PP molecules,whereas N,N'-isopropyl-3,4,9,10-perylenedicarboximide(LP)failed to be imaged because of strong steric hindrance coming from larger side group.To further investigate the impact of steric hindrance,we utilized octanoic acid(OA)as solvent to capture the adsorption details of LP and PP.We found that OA molecules drag PP and LP molecules in a different direction to generate linear structure,impeding the molecular rotation.The structure–solvent relationship shows that the steric hindrance is brought by the large side group,which makes it easier to recognize OA molecules at the interface.These results demonstrate that steric effect plays a significant role in altering interaction sites of the compounds during the adsorption process at the liquid/solid interface.

关键词： C-terminal amino acids Steric effect Bonding site Scanning tunneling microscopy DFT calculations

Nonmacrocyclic Iron(II)Soluble Redox Mediators Leading to High-Rate Li-O_(2)Battery

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CCS chemistry 2021年第5期3卷 1350-1358页

作者： Baoxing Wang Xiao Wang Xueyi Cheng Jing Zhang Minglei Yan Guochang Li Lijun Yang Qiang Wu Xizhang Wang Zheng Hu key laboratory of mesoscopic chemistry of moe Jiangsu Provincial Laboratory for Nano technologySchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023

The lithium-oxygen(Li-O_(2))battery is highly promising but suffers from poor cycling life,especially at high rates;hence,the need for high-efficient accelerating agents is crucial.Recently macrocyclic Fe-based redox mediators,such as iron(II)phthalocyanine(FePc)and heme,have been developed and anticipated to be ideal due to their bifunctional charge and superoxide shuttling capabilities.However,they still operate far below expectations,which could result from the low concentrations in electrolyte due to the strongπ-πinteraction at carbon cathode.Herein,the authors report a new type of nonmacrocyclic Fe-based redox mediators,iron(II)acetylacetonate[Fe(acac)2]and iron(II)glycinate[Fe(gly)2],which have weakπ-πinteraction with the carbon cathode,thus,remain at high concentrations in the electrolyte.The Fe(gly)2@Li-O_(2)battery reaches a long life of 321 cycles at 0.5 A g^(−1),which is much superior to the counterpart with the typical macrocyclic FePc,and particularly exhibits a long life of 167 cycles at 2.0 A g^(−1)and 136 cycles at ultrahigh 5.0 A g^(−1).This study demonstrates an efficient strategy to achieve a high-rate performance of Li-O_(2)batteries by developing nonmacrocyclic Fe-based redox mediators with high-efficient electron and superoxide shuttling.

关键词： lithium-oxygen battery redox mediator nonmacrocyclic iron(II)mediator superoxide shuttling high-rate performance