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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

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

钴基纳米晶-氮掺杂碳纳米笼复合材料的构建与电化学储能性能研究（英文）

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Science China Materials 2019年第10期62卷 1393-1402页

作者：麻青明姚月坚闫明磊赵杰葛承宣吴强杨立军王喜章胡征 key laboratory of mesoscopic chemistry of moe and jiangsu provincial Lab for nanotechnology School of Chemistry and Chemical EngineeringNanjing University

Co(OH)2、CoO和Co3O4等钴基化合物因具有高理论容量和赝电容性质而备受关注.但受限于活性表面积小、电荷传输缓慢等原因,钴基纳米材料的实际储能性能却有限.本文以我们前期开发的具有大比表面积、高导电性和微孔-介孔-大孔共存的分级结... 详细信息

Co(OH)2、CoO和Co3O4等钴基化合物因具有高理论容量和赝电容性质而备受关注.但受限于活性表面积小、电荷传输缓慢等原因,钴基纳米材料的实际储能性能却有限.本文以我们前期开发的具有大比表面积、高导电性和微孔-介孔-大孔共存的分级结构氮掺杂碳纳米笼(hNCNCs)为载体,成功构建了晶粒尺寸小、电荷转移快的系列钴基纳米晶-hNCNCs复合材料,有效地提高了活性材料的利用率.其中,Co(OH)2/hNCNCs在2 Ag ^-1下表现出1170 F g^-1的高比容量,基于活性物种Co(OH)2的比电容高达2214 Fg^-1,接近其理论值(2595 Fg^-1).研究发现,具有不同组成的Co(OH)2、CoO和Co3O4纳米晶通过相同的可逆氧化还原反应存储/释放电能.这种新的储能机理表明将碳基载体上的活性物种Co(OH)2转化为CoO或Co3O4的操作是非必要的,甚至可能损害其储能性能.本研究可为开发过渡金属化合物基高能量密度电极材料提供借鉴.

关键词： Co(OH)2 过渡金属化合物 Co3O4 氧化还原反应活性材料高能量密度活性物种理论容量

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

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.

In situ construction of porous hierarchical(Ni3-xFex)FeN/Ni heterojunctions toward efficient electrocatalytic oxygen evolution

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Nano Research 2020年第2期13卷 328-334页

作者： Minglei Yan Kun Mao Peixin Cui Chi Chen Jie Zhao Xizhang Wang Lijun Yang Hui Yang Qiang Wu Zheng Hu key laboratory of mesoscopic chemistry of moe and jiangsu provincial laboratory of nanotechnology School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China key laboratory of Soil Environment and Pollution Remediation Institute of Soil ScienceChinese Academy of SciencesNanjing 210008China Shanghai Advanced Research Institute Chinese Academy of SciencesShanghai 201210China

As a choke point in water electrolysis,the oxygen evolution reaction(OER)suffers from the severe electrode polarization and large overpotential.Herein,the porous hierarchical hetero-(Nis Fe)FeN/Ni catalysts are in situ constructed for the eficient electrocatalytic OER.X-ray absorption fine structure characterizations reveal the strong Ni-Fe bimetallic interaction in(Niz Fex)FeN/Ni.Theoretical study indicates the heterojunction and bimetallic interaction decrease the free-energy change for the rate-limiting step of the OER and the overpotential thereof.In addition,the high conductivity and porous hierarchical morphology favor the electron transfer,electrolyte access and O2 release.Consequently,the optimized catalyst achieves a low overpotential of 223 mV at 10 mA.cm^-2,a small Tafel slope of 68 mV:dec^-1,and a high stability.The excellent performance of the optimized catalyst is also demonstrated by the overall water electrolysis with a low working voltage and high Faradaic efficiency.Moreover,the correlation between the structure and performance is well established by the experimental characterizations and theoretical calculations,which confirms the origin of the OER activity from the surface metal oxyhydroxide in situ generated upon applying the current.This study suggests a promising approach to the advanced OER electrocatalysts for practical applications by constructing the porous hierarchical metal-compound/metal heterojunctions.

关键词： oxygen evolution reaction electrocatalysts ternary Ni-Fe nitrides heterojunctions /n s/fty construction

Alloyed Pt-Sn nanoparticles on hierarchical nitrogen-doped carbon nanocages for advanced glycerol electrooxidation

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Nano Research 2024年第5期17卷 4055-4061页

作者： Jietao Jiang Liqi Zhou Fengfei Xu Guanghai Chen Xiaoyu Liu Zhen Shen Lijun Yang Qiang Wu Xizhang Wang Zheng Hu key laboratory of mesoscopic chemistry of moe Jiangsu Provincial Laboratory for NanotechnologySchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China National laboratory of Solid State Microstructures Jiangsu Key Laboratory of Artificial Functional MaterialsCollege of Engineering and Applied Sciences and Collaborative Innovation Center of Advanced MicrostructuresNanjing UniversityNanjing 210093China

Glycerol is an alternative sustainable fuel for fuel cells,and efficient electrocatalyst is crucial for glycerol oxidation reaction(GOR).The promising Pt catalysts are subject to the inadequate capability of C-C bond cleavage and the susceptibility to poisoning.Herein,Pt-Sn alloyed nanoparticles are immobilized on hierarchical nitrogen-doped carbon nanocages(hNCNCs)by convenient ethylene glycol reduction and subsequent thermal reduction.The optimal Pt_(3)Sn/hNCNC catalyst exhibits excellent GOR performance with a high mass activity(5.9 A·mg_(Pt)^(-1)),which is 2.7 and 5.4 times higher than that of Pt/hNCNC and commercial Pt/C,respectively.Such an enhancement can be mainly ascribed to the increased anti-poisoning and C-C bond cleavage capability due to the Pt_(3)Sn alloying effect and Sn-enriched surface,the high dispersion of Pt_(3)Sn active species due to N-participation,as well as the high accessibility of Pt_(3)Sn active species due to the three-dimensional(3D)hierarchical architecture of hNCNC.This study provides an effective GOR electrocatalyst and convenient approach for catalyst preparation.

关键词： Pt_(3)Sn alloy hierarchical nitrogen-doped carbon nanocages glycerol electrooxidation anti-poisoning C-C bond cleavage

Hierarchical sulfur and nitrogen co-doped carbon nanocages as efficient bifunctional oxygen electrocatalysts for rechargeable Zn-air battery

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Journal of Energy chemistry 2019年第7期28卷 64-71页

作者： Hao Fan Yu Wang Fujie Gao Longqi Yang Meng Liu Xiao Du Peng Wang Lijun Yang Qiang Wu Xizhang Wang Zheng Hu key laboratory of mesoscopic chemistry of moe and Collaborative Innovation Center of chemistry for Life Sciences Jiangsu Provincial Laboratory for NanotechnologySchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023.JiangsuChina National laboratory of Solid State Microstructures Nanjing UniversityNanjing 210023JiangsuChina College of Engineering and Applied Sciences and Collaborative Innovation Center of Advanced Microstructures Nanjing UniversityNanjing 210023JiangsuChina

Exploring inexpensive and efficient bifunctional electrocatalysts for oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) is critical for rechargeable metal-air batteries. Herein, we report a new 3D hierarchical sulfur and nitrogen co-doped carbon nanocages(hSNCNC) as a promising bifunctional oxygen electrocatalyst by an in-situ MgO template method with pyridine and thiophene as the mixed precursor. The as-prepared h SNCNC exhibits a positive half-wave potential of 0.792 V(vs. reversible hydrogen electrode, RHE) for ORR, and a low operating potential of 1.640 V at a 10 mA cm-2 current density for OER. The reversible oxygen electrode index is 0.847 V, far superior to commercial Pt/C and IrO2,which reaches the top level of the reported bifunctional catalysts. Consequently, the hSNCNC as air cathodes in an assembled Zn-air battery features low charge/discharge overpotential and long lifetime. The remarkable properties arises from the introduced multiple heteroatom dopants and stable 3D hierarchical structure with multi-scale pores, which provides the abundant uniform high-active S and N species and efficient charge transfer as well as mass transportation. These results demonstrate the potential strategy in developing suitable carbon-based bi-/multi-functional catalysts to enable the next generation of the rechargeable metal-air batteries.

关键词： 3D hierarchical Carbon nanocages S,N co-doping Bifunctional electrocatalysis Zn-air battery

Boosting oxygen reduction activity of spinel CoFe2O4 by strong interaction with hierarchical nitrogen-doped carbon nanocages

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Science Bulletin 2017年第20期62卷 1365-1372页

作者： Hao Fan Lijun Yang Yu Wang Xiali Zhang Qingsong Wu Renchao Che Meng Liu Qiang Wu Xizhang Wang Zheng Hu key laboratory of mesoscopic chemistry of Ministry of Education and jiangsu provincial Lab for nanotechnology School of Chemistry and Chemical Engineering Nanjing University Nanjing 210023 China Department of Materials Science and Advanced Materials laboratory Fudan University Shanghai 200438 China

The unique hierarchical nitrogen-doped carbon nanocages(h NCNC) are used as a new support to homogeneously immobilize spinel Co Fe_2O_4 nanoparticles by a facile solvothermal method. The so-constructed hierarchical Co Fe_2O_4/h NCNC catalyst exhibits a high oxygen reduction activity with an onset potential of0.966 V and half-wave potential of 0.819 V versus reversible hydrogen electrode, far superior to the corresponding 0.846 and 0.742 V for its counterpart of Co Fe_2O_4/h CNC with undoped hierarchical carbon nanocages(h CNC) as the support, which locates at the top level for spinel-based catalysts to date.Consequently, the Co Fe_2O_4/h NCNC displays the superior performance to the Co Fe_2O_4/h CNC, when used as the cathode catalysts in the home-made Al-air batteries. X-ray photoelectron spectroscopy characterizations reveal the more charge transfer from Co Fe_2O_4 to h NCNC than to h CNC, indicating the stronger interaction between Co Fe_2O_4 and h NCNC due to the nitrogen participation. The enhanced interaction and hierarchical morphology favor the high dispersion and modification of electronic states for the active species as well as the mass transport during the oxygen reduction process, which plays a significant role in boosting the electrocatalytic performances. In addition, we noticed the high sensitivity of O 1 s spectrum to the particle size and chemical environment for spinel oxides, which is used as an indicator to understand the evolution of ORR activities for all the Co Fe_2O_4-related contrast catalysts. Accordingly,the well-defined structure-performance relationship is demonstrated by the combination of experimental characterizations with theoretical calculations. This study provides a promising strategy to develop efficient, inexpensive and durable oxygen reduction electrocatalysts by tuning the interaction between spinel metal oxides and the carbon-based supports.

关键词： Oxygen reduction electrocatalyst Spinel cobalt ferrite oxide Hierarchical nitrogen-doped carbon nanocages Strong interaction Structure-performance relationship Al-air battery