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fullerene-derived boron-doped defective nanocarbon for highly selective H_(2)O_(2) electrosynthesis

Nano Research 2024年第3期17卷 1217-1224页

作者： Wangqiang Shen Chang Zhang Muneerah Alomar Zhiling Du Zepeng Yang Junjie Wang Guangqing Xu Jian Zhang Jun Lv Xing Lu School of Materials Science and Engineering Hefei University of TechnologyHefei 230009China School of Energy and Environmental Hebei University of EngineeringHandan 056038China School of Materials Science and Engineering Huazhong University of Science and TechnologyWuhan 430074China Department of Physics College of SciencesPrincess Nourah bint Abdulrahman UniversityP.O.Box 84428Riyadh 11671Saudi Arabia

Electrochemical production of hydrogen peroxide(H_(2)O_(2))via the two-electron(2e-)pathway of oxygen reduction reaction(ORR)supplies an auspicious alternative to the current industrial anthraquinone process.Nonetheless,it still lacks efficient electrocatalysts to achieve high ORR activity together with 2e-selectivity simultaneously.Herein,a boron-doped defective nanocarbon(B-DC)electrocatalyst is synthesized by using fullerene frameworks as the precursor and boric oxide as the boron source.The obtained B-DC materials have a hierarchical porous structure,befitting boron dopants,and abundant topological pentagon defects,exhibiting a high ORR onset potential of 0.78 V and a dominated 2e-selectivity(over 95%).Remarkably,when B-DC electrocatalyst is employed in a real device,it achieves a high H_(2)O_(2) yield rate(247 mg·L^(-1)·h^(-1)),quantitative Faraday efficiency(~100%),and ultrafast organic pollutant degradation rate.The theoretical calculation reveals that the synergistic effect of topological pentagon defects and the incorporation of boron dopants promote the activation of the O_(2) molecule and facilitates the desorption of oxygen intermediate.This finding will be very helpful for the comprehension of the synergistic effect of topological defects and heteroatom dopants for boosting the electrocatalytic performance of nanocarbon toward H_(2)O_(2) production.

关键词： fullerene electrochemical hydrogen peroxide production oxygen reduction reaction carbon nanomaterials

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fullerenes and derivatives as electrocatalysts: Promises and challenges

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Green Energy & Environment 2024年第1期9卷 7-27页

作者： Kun Guo Ning Li Lipiao Bao Xing Lu State Key Laboratory of Materials Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan430074China

Carbon-based metal-free nanomaterials are promising alternatives to precious metals as electrocatalysts of key energy storage and conversion technologies.Of paramount signiﬁcance are the establishment of design principles by understanding the catalytic mechanisms and identifying the active sites.Distinct from sp2-conjugated graphene and carbon nanotube,fullerene possesses unique characteristics that are growingly being discovered and exploited by the electrocatalysis community.For instance,the well-deﬁned atomic and molecular structures,the good electron afﬁnity to tune the electronic structures of other substances,the intermolecular self-assembly into superlattices,and the on-demand chemical modiﬁcation have endowed fullerene with incomparable advantages as electrocatalysts that are otherwise not applicable to other carbon ma-terials.As increasing studies are being reported on this intriguing topic,it is necessary to provide a state-of-the-art overview of the recent progress.This review takes such an initiative by summarizing the promises and challenges in the electrocatalytic applications of fullerene and its derivatives.The content is structured according to the composition and structure of fullerene,including intact fullerene(e.g.,fullerene composite and superlattices)and fullerene derivatives(e.g.,doped,endohedral,and disintegrated fullerene).The synthesis,characterization,catalytic mechanisms,and deﬁciencies of these fullerene-based materials are explicitly elaborated.We conclude it by sharing our perspectives on the key aspects that future efforts shall consider.

关键词： fullerene fullerene derivative Metal-free catalyst Structural defect Electrocatalyst

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Integrating Levels of Hierarchical Organization in Porous Organic Molecular Materials

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Nano-Micro Letters 2024年第5期16卷 134-153页

作者： Jesus Ferrando‑Soria Antonio Fernandez Instituto de Ciencia Molecular(ICMol) Universidad de Valencia46980 ValenciaSpain School of Science Loughborough UniversityLoughborough LE113TUUK

Porous organic molecular materials(POMMs)are an emergent class of molecular-based materials characterized by the formation of extended porous frameworks,mainly held by non-covalent interactions.POMMs represent a variety of chemical families,such as hydrogen-bonded organic frameworks,porous organic salts,porous organic cages,C-H···πmicroporous crystals,supramolecular organic frameworks,π-organic frameworks,halogen-bonded organic framework,and intrinsically porous molecular materials.In some porous materials such as zeolites and metal organic frameworks,the integration of multiscale has been adopted to build materials with multifunctionality and optimized properties.Therefore,considering the significant role of hierarchy in porous materials and the growing importance of POMMs in the realm of synthetic porous materials,we consider it appropriate to dedicate for the first time a critical review covering both topics.Herein,we will provide a summary of literature examples showcasing hierarchical POMMs,with a focus on their main synthetic approaches,applications,and the advantages brought forth by introducing hierarchy.

关键词： Porous organic molecular materials Hierarchy Hydrogen-bonded organic frameworks Porous cages fullerene

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Research progress on rolling superlubricity in solid lubricants

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Science China Technological Sciences 2024年第7期67卷 1980-1990页

作者： LI PanPan LI HongXuan ZHU DongXiang ZHU YongQi KANG FuYan WANG Wan ZHANG YaXin LIU XiaoHong JI Li ZHOU HuiDi CHEN JianMin State Key Laboratory of Solid Lubrication Lanzhou Institute of Chemical Physics Chinese Academy of Sciences Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences School of Chemical Engineering Northwest Minzu University

Superlubricity is an ideal lubrication state where friction nearly vanishes between contact interfaces. It has become one of the most important research topics and approaches owing to its significance in reducing energy consumption and preventing device failures. As an efficient and universal lubricating principle capable of achieving superlubricity, rolling lubrication has attracted widespread attention in recent years. In this review, the theoretical concept of rolling lubrication and the experimental research progress of spherical/scroll structures are summarized. The review focuses on the possibility of achieving rolling lubrication using spherical/scroll structures(such as spherical fullerenes, carbon nanotubes, and formed and constructed spherical/scroll structures). The challenges in achieving rolling lubrication are summarized, and the possibility of molecular rolling lubrication,as well as its potential applications in superlubrication, are discussed.

关键词： spherical/scroll structure rolling lubrication superlubricity fullerene

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Excellentπ-Bowl Semiconductors Based on C_(70)Subunit

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CCS Chemistry 2024年第2期6卷 353-364页

作者： Meng Chen Yuxiao Duan Xinyue Liu Qian Zhan Hironobu Hayashi Kyohei Matsuo Hiroko Yamada Guangpeng Gao Yonghao Zheng Lei Zhang Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical TechnologyBeijing 100029 School of Optoelectronic Science and Engineering University of Electronic Science and Technology of China(UESTC)Chengdu 610054 Division of Materials Science Nara Institute of Science and Technology(NAIST)IkomaNara 630-0192 Key Laboratory of Cluster Science of Ministry of Education Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion MaterialsSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081

As open substructures of fullerenes,aromaticπ-bowls are promising candidates as new organic semiconductors,as well as attractive hosts for fullerenes.We demonstrate herein the synthesis and characterization of a novel C_(2v)symmetricπ-bowl,pyracyleno[6,5,4,3,2,1-pqrstuv]pentaphene(3).Bowl 3 was equipped with two distinctive reactive sites,allowing for bromination and cross-coupling reactions to readily yield functionalized bowls with two 2,4,6-trimethylphenyl(5)and triethylsilyl(TES)-ethynyl(6)substituents,respectively.Variable-temperature 1H NMR analysis and density functional theory(DFT)calculations indicated bowl-to-bowl inversions of 3,5,and 6 at room temperature.By alternating the substituents,the crystal structures of the threeπ-bowls 3,5,and 6 could be controlled from 1D linear to 1D slipped to 2D herringbone packing motifs,providing insight into the packing behavior ofπ-bowls.1H NMR titration study indicated that the TES-ethynyl substituent enhanced the ability ofπ-bowl to bind C_(70)with an association constant of 2485 M−1.The C_(70)molecules withπ-bowls 3 and 6 formed 1:1 complexes,in which C_(70)molecules aggregated into zig-zag and 1D linear arrays,respectively.The hole mobility of 2.3 cm^(2)V^(−1)^s(−1)and electron mobility of 0.16 cm^(2)V^(−1)^s(−1)ofπ-bowl 3 and its complex with C_(70)were demonstrated,respectively,which proved a great value for the development of aromaticπ-bowl semiconductors with tunable properties for organic electronic devices.

关键词： organic semiconductor π-bowl fullerene crystal engineering mobility

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A strained π-extended[10]cycloparaphenylene carbon nanoring

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Chinese Chemical Letters 2024年第5期35卷 171-174页

作者： Kang Wei Jiayu Li Wen Zhang Bing Yuan Ming-De Li Pingwu Du Key Laboratory of Precision and Intelligent Chemistry Anhui Laboratory of Advanced Photon Science and TechnologyDepartment of Materials Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026China Department of Chemistry and Key Laboratory for Preparation and Application of Ordered Structural Materials of Guangdong Province Shantou UniversityShantou 515063China

Herein,we report the facile synthesis of a highly strained hexabenzocoronene-containing carbon nanoring,cyclo[4]-paraphenylene[2]-2,11-hexabenzocoronenylene([4,2]CPHBC),as the segment of a[10,10]single-walled carbon nanotube([10,10]SWNT).[4,2]CPHBC was synthesized based on the platinummediated assembly of diborylbiphenyl and diborylhexabenzocoronene,forming a tetranuclear platinum complex,followed by reductive elimination.This nanoring molecule was confirmed by NMR and HRMS,and its photophysical properties were studied using steady-state and time-resolved spectroscopies.Moreover,the selective supramolecular host-guest interaction between[4,2]CPHBC and C_(60) was also investigated.

关键词： CPP Hexabenzocoronene fullerene Supramolecular chemistry

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fullerene nanoparticles for the treatment of ulcerative colitis

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Science China(Life Sciences) 2022年第6期65卷 1146-1156页

作者： Xiaodan Liao Zhongpu Zhao Hui Li Bo Wu Jiawei Huo Lei Li Xue Li Xinran Cao Min Xia Chunru Wang Chunli Bai Beijing National Laboratory for Molecular Sciences Key Laboratory of Molecular Nanostructure and NanotechnologyCAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China Beijing FULLCAN Biotechnology Co. Ltd.Beijing 100190China

Ulcerative colitis(UC) is a long-term,recurrent inflammatory bowel disease for which no effective cure is yet available in the clinical setting.Repairing the barrier dysfunction of the colon and reducing intestinal inflammation are considered key objectives to cure UC.Here we demonstrate a novel therapeutic strategy based on a C_(60) fullerene suspension(C_(60)FS) to treat dinitrobenzene sulfonic acid-induced UC in an animal model.C_(60)FS can repair the barrier dysfunction of UC and effectively promote the healing of ulcers;it also manifests better treatment effects compared with mesalazine enema.C_(60)FS can reduce the numbers of basophils in the blood of UC rats and mast cells in the colorectal tissue,thereby effectively alleviating inflammation.The expression of H1R,H4R,and VEGFR2 receptors in colorectal tissues is inhibited by C_(60)FS,and the levels of histamine and prostaglandin in the rat blood are reduced.This work presents a reliable strategy based on fullerene to cure UC and provides a novel guide for UC treatment.

关键词： fullerene ulcerative colitis immunity

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fullerene-Intercalated Graphitic Carbon Nitride as a HighPerformance Anode Material for Sodium-Ion Batteries

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Energy & Environmental Materials 2022年第2期5卷 608-616页

作者： Pengju Li Yanglin Shen Ximing Li Wenhuan Huang Xing Lu Shaanxi Key Laboratory of Chemical Additives for Industry College of Chemistry&Chemical EngineeringShaanxi University of Science&TechnologyXi’an 710021China State Key Laboratory of Materials Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074China

Two-dimensional(2D)graphitic carbon nitride(g-CN)is a promising anode material for sodium-ion batteries(SIBs),but its insufficient interlayer spacing and poor electronic conductivity impede its sodium storage capacity and cycling stability.Herein,we report the fabrication of a fullerene(C_(60))-modified graphitic carbon nitride(C_(60)@CN)material which as an anode material for SIBs shows a high-reversible capacity(430.5 mA h g^(−1) at 0.05 A g^(−1),about 3 times higher than that of pristine g-CN),excellent rate capability(226.6 mA h g^(−1) at 1 A g^(−1))and ultra-long cycle life(101.2 mA h g^(−1) after 5000 cycles at 5 A g^(−1)).Even at a high-active mass loading of 3.7 mg cm^(−2),a reversible capacity of 316.3 mA h g^(−1) can be obtained after 100 cycles.Such outstanding performance of C_(60)@CN is attributed to the C_(60) molecules distributed in the g-CN nanosheets,which enhance the electronic conductivity and prevent g-CN sheets from restacking,thus resulting in enlarged interlayer spacing and exposed edge N defects(pyridinic N and pyrrolic N)for sodium-ion storage.Furthermore,a sodium-ion full cell combining C60@CN anode and NVPF@rGO cathode provides high-coulombic efficiency(>96.5%),exceptionally high-energy density(359.8 W h kganode−1 at power density of 105.1 W kganode−1)and excellent cycling stability(89.2%capacity retention over 500 cycles at 1Aganode−1).This work brings new insights into the field of carbon-based anode materials for SIBs.

关键词： energy storage fullerene interlayer distance nitrogen-doped carbon materials

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Double-Cable Conjugated Polymers with fullerene Pendant for Single-Component Organic Solar Cells

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Chinese Journal of Polymer Science 2022年第8期40卷 898-904,I0007页

作者： Bai-Qiao Liu Yun-Hua Xu Feng Liu Cheng-Cheng Xie Shi-Jie Liang Qiao-Mei Chen Wei-Wei Li Department of Chemistry School of ScienceBeijing Jiaotong UniversityBeijing100044China Beijing Advanced Innovation Center for Soft Matter Science and Engineering&State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing100029China

In this work,the“functionalization-polymerization”(FP)method has been used to construct fullerene-contained double-cable conjugated polymers with“donor-acceptor”backbones.It was realized via synthesizing a fullerene-contained monomer and performing Stille polymerization.With this method,a series of double-cable conjugated polymers with different fullerene contents were developed and applied into single-component organic solar cells.The power conversion efficiencies(PCEs)based on these polymers increased from 0.71%to 1.71%with the enhanced fullerene contents.The relatively low PCEs might be originated from the poor microstructure in these polymers.These new conjugated polymers with molecular heterojunction would show potential application in organic electronic devices.

关键词： Double-cable conjugated polymers Single-component organic solar cells fullerene “Donor-acceptor”conjugated polymers Microphase separation

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Plasma protein corona forming upon fullerene nanocomplex:Impact on both counterparts

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Particuology 2023年第2期73卷 26-36页

作者： Linjing Wu Fangqin Fu Wenhao Wang Wenhua Wang Zhengwei Huang Ying Huang Xin Pan Chuanbin Wu College of Pharmacy Jinan UniversityGuangzhou510632China School of Pharmaceutical Sciences Sun Yat-Sen UniversityGuangzhou510006China

Protein corona refers to the structure composed of biomolecules adsorbed on the surface of nanomaterials.The study on the effect of the interaction between protein and nanoparticles can provide an important guide for the application of nanodrug delivery.To provide a reference for the research on fullerene(C60)nanocomplex drug delivery systems,this work studied the interaction between C60 nanocomplex and a variety of plasma proteins.Research showed that the protein binding with C60 nanocomplex did not change the charge properties of protein.The proteins induced the aggregation of C60 nanocomplex.The circular dichroism spectra showed that the secondary structure of the proteins changed after binding to C60 nanocomplex.The ultraviolet-visible spectra showed that the effect of C60 nanocomplex on proteins was concentration-dependent.The fluorescence spectra showed that C60 nanocomplex could intrinsic fluorescence alteration of proteins.The adsorption capacity of C60 nanocomplex to proteins was changed at 0 h and 4 h.The interaction between nanocomplex and proteins might affect the morphological characteristics of nanocomplex and the conformation of proteins.This work could provide a reference for the research and development of C60 nanocomplex and other carbon-based nanocomplex as nanoparticulate drug delivery systems.

关键词： fullerene Nanocomplex Interaction Protein corona

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