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metal-Halide Perovskite Submicrometer-Thick Films for Ultra-Stable Self-Powered direct X-Ray Detectors

Nano-micro Letters 2024年第9期16卷 410-431页

作者： marco Girolami Fabio matteocci Sara Pettinato Valerio Serpente Eleonora Bolli Barbara Paci Amanda Generosi Stefano Salvatori Aldo di carlo Daniele m.Trucchi CNR‑ISm Consiglio Nazionale delle RicercheIstituto di Struttura della MateriaSede Secondaria di MontelibrettiDiaTHEMA LabStrada Provinciale 35D900010 MontelibrettiRomeItaly CHOSE–Centre for Hybrid and Organic Solar Energy Department of Electronic EngineeringUniversity of Rome“Tor Vergata”Via del Politecnico 100133 RomeItaly Faculty of Engineering Universita degli Studi Niccolo CusanoVia don Carlo Gnocchi 300166 RomeItaly SpecXLab CNR‑ISMConsiglio Nazionale Delle RicercheIstituto di Struttura Della MateriaArea della Ricerca di Tor VergataVia del Fosso del Cavaliere 10000133 RomeItaly

metal-halide perovskites are revolutionizing the world of X-ray detectors,due to the development of sensitive,fast,and cost-effective devices.Self-powered operation,ensuring portability and low power consumption,has also been recently demonstrated in both bulk materials and thin films.However,the signal stability and repeatability under continuous X-ray exposure has only been tested up to a few hours,often reporting degradation of the detection performance.Here it is shown that self-powered direct X-ray detectors,fabricated starting from a FAPbBr_(3)submicrometer-thick film deposition onto a mesoporous TiO_(2)scaffold,can withstand a 26-day uninterrupted X-ray exposure with negligible signal loss,demonstrating ultra-high operational stability and excellent repeatability.No structural modification is observed after irradiation with a total ionizing dose of almost 200 Gy,revealing an unexpectedly high radiation hardness for a metal-halide perovskite thin film.In addition,trap-assisted photoconductive gain enabled the device to achieve a record bulk sensitivity of 7.28 C Gy^(−1)cm^(−3)at 0 V,an unprecedented value in the field of thin-film-based photoconductors and photodiodes for“hard”X-rays.Finally,prototypal validation under the X-ray beam produced by a medical linear accelerator for cancer treatment is also introduced.

关键词： metal-halide perovskite thin films direct X-ray detectors Self-powered devices Operational stability medical linear accelerator

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On-Surface Synthesis of Anthracene-Fused Zigzag Graphene Nanoribbons from 2,7-dibromo-9,9′-bianthryl Reveals Unexpected Ring Rearrangements

Precision Chemistry

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Precision Chemistry 2024年第2期2卷 81-87页

作者： Xiushang Xu Amogh Kinikar marco di Giovannantonio carlo A.Pignedoli Pascal Ruffieux Klaus müllen Roman Fasel Akimitsu Narita max Planck Institute for Polymer Research 55128 MainzGermany Organic and Carbon Nanomaterials Unit Okinawa Institute of Science and Technology Graduate UniversityKunigami-gunOkinawa 904-0495Japan Empa Swiss Federal Laboratories for Materials Science and Technologynanotech@surfaces Laboratory8600 DübendorfSwitzerland Institute of Structure of matter-CNR(ISm-CNR) 00133 RomaItaly Institute of Physical Chemistry Johannes Gutenberg University Mainz55128 MainzGermany Department of Chemistry Biochemistry and Pharmaceutical SciencesUniversity of Bern3012 BernSwitzerland

On-surface synthesis has emerged as a powerful strategy to fabricate unprecedented forms of atomically precise graphene nanoribbons(GNRs).However,the on-surface synthesis of zigzag GNRs(ZGNR)has met with only limited success.Herein,we report the synthesis and on-surface reactions of 2,7-dibromo-9,9′-bianthryl as the precursor towardπ-extended ZGNRs.Characterization by scanning tunneling microscopy and high-resolution noncontact atomic force microscopy clearly demonstrated the formation of anthracene-fused ZGNRs.Unique skeletal rearrangements were also observed,which could be explained by intramolecular diels-Alder cycloaddition.Theoretical calculations of the electronic properties of the anthracene-fused ZGNRs revealed spin-polarized edge-states and a narrow bandgap of 0.20 eV.

关键词： On-surface synthesis Graphene nanoribbon On-surface reaction Rearrangement Edge state

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Nutrient restriction-activated Fra-2 promotes tumor progression via IGF1R in miR-15a downmodulated pancreatic ductal adenocarcinoma

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Signal Transduction and Targeted Therapy 2024年第3期9卷 1132-1146页

作者： Gian Luca Rampioni Vinciguerra marina Capece Luca Reggiani Bonetti Giovanni Nigita Federica Calore Sydney Rentsch Paolo magistri Roberto Ballarin Fabrizio di Benedetto Rosario distefano Roberto Cirombella Andrea Vecchione Barbara Belletti Gustavo Baldassarre Francesca Lovat carlo m.Croce Department of Cancer Biology and Genetics and Comprehensive Cancer Center The Ohio State UniversityColumbus 43210 OHUSA Department of Clinical and molecular medicine Faculty of Medicine and PsychologySant’Andrea HospitalUniversity of Rome“Sapienza”Rome 00189Italy Department of diagnostic Clinic and Public Health MedicineUniversity of Modena and Reggio EmiliaModena 41100Italy Hepato-pancreato-biliary Surgery and Liver Transplantation Unit University of Modena and Reggio EmiliaModena 41100Italy division of molecular Oncology Centro di Riferimento Oncologico di Aviano(CRO)Istituto di Ricovero e Cura a Carattere Scientifico(IRCCS)National Cancer InstituteAviano 33081Italy

Pancreatic ductal adenocarcinoma(PDAC)is a lethal disease,characterized by an intense desmoplastic reaction that compresses blood vessels and limits nutrient supplies.PDAC aggressiveness largely relies on its extraordinary capability to thrive and progress in a challenging tumor microenvironment.Dysregulation of the onco-suppressor miR-15a has been extensively documented in PDAC.Here,we identified the transcription factor Fos-related antigen-2(Fra-2)as a miR-15a target mediating the adaptive mechanism of PDAC to nutrient deprivation.We report that the IGF1 signaling pathway was enhanced in nutrient deprived PDAC cells and that Fra-2 and IGF1R were significantly overexpressed in miR-15a downmodulated PDAC patients.mechanistically,we discovered that miR-15a repressed IGF1R expression via Fra-2 targeting.In miR-15a-low context,IGF1R hyperactivated mTOR,modulated the autophagic flux and sustained PDAC growth in nutrient deprivation.In a genetic mouse model,mir15aKO PDAC showed Fra-2 and Igf1r upregulation and mTOR activation in response to diet restriction.Consistently,nutrient restriction improved the efficacy of IGF1R inhibition in a Fra-2 dependent manner.Overall,our results point to a crucial role of Fra-2 in the cellular stress response due to nutrient restriction typical of pancreatic cancer and support IGF1R as a promising and vulnerable target in miR-15a downmodulated PDAC.

关键词： IGF1R Fra miR

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Transperineal laser ablation of the prostate as a treatment for benign prostatic hyperplasia and prostate cancer: The results of a Delphi consensus project

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Asian Journal of Urology 2024年第2期11卷 271-279页

作者： Andrea Cocci marta Pezzoli Fernando Bianco Franco Blefari Pierluigi Bove Francois Cornud Gaetano De Rienzo Paolo Destefanis Danilo di Trapani Alessandro Giacobbe Luca Giovanessi Antonino Laganà Giovanni Lughezzani Guglielmo manenti Gianluca muto Gianluigi Patelli Novello Pinzi Stefano Regusci Giorgio I.Russo Juan I.m.Salamanca matteo Salvi Luigi Silvestri Fabrizio Verweij Eric Walser Riccardo GBertolo Valerio Iacovelli Alessandro Bertaccini Debora marchiori Hugo Davila Pasquale ditonno Paolo Gontero Gennaro Iapicca Theo m De Reijke Vito Ricapito Pierluca Pellegrini Andrea minervini Sergio Serni Francesco Sessa Department of Urology Careggi HospitalUniversity of FlorenceFlorenceItaly Urology Section University of FlorenceFlorenceItaly Urological Research Network MiamiFLUSA Urology Section Prato HospitalPratoItaly Torvergata Oncoscience Research Centre of Excellence TORDepartment of Experimental MedicineUniversity of Rome Tor VergataRomeItaly Department of Urology San Carlo di Nancy HospitalRomeItaly Department of Radiology Hôpital CochinParis Descartes UniversityParisFrance Urology and Andrology Unit II Department of Emergency and Organ TransplantationUniversity of BariBariItaly Unit of Urology Cittàdella Salute e della Scienza HospitalUniversity of TurinTurinItaly Urology Unit Buccheri La Ferla Fatebenefratelli HospitalPalermoItaly Department of Urology Humanitas Gradenigo HospitalTurinItaly Urology Unit Surgical DepartmentFondazione Poliambulanza Istituto OspedalieroBresciaItaly Departement of Urology “S.Giovanni Evangelista”HospitalTivoliItaly Humanitas Clinical and Research CentereIRCCS Department of UrologyRozzanoItaly Department of Biomedical Sciences Humanitas UniversityPieve EmanueleItaly Department of Biomedicine and Prevention University of Rome“Tor Vergata”RomeItaly Department of diagnostic Imaging and Interventional Radiology University of Rome“Tor Vergata”RomeItaly Department of Interventional Radiology Pesenti-Fenaroli Hospital-ASST Bergamo EstAlzano LombardoItaly Department of Urology University of SienaSienaItaly Swiss International Prostate Center GenevaSwitzerland Clinique Générale Beaulieu GenevaSwitzerland Department of Urology University of CataniaItaly Department of Urology Puerta de Hierro-Majadahonda University HospitalMadridSpain Lyx Institute of Urology Universidad Francisco de VitoriaMadridSpain Department of medico-Surgical Sciences and Biotechnologies Sapienza University of RomeFaculty of Pharmacy and MedicineUrology Unit ICOTLatinaItaly Department of Urology European Institute of Oncology(IEO)IRCCSMilanItaly Department of Radiology D

Objective: To evaluate transperineal laser ablation (TPLA) with Echolaser® (Echolaser® TPLA, Elesta S.p.A., Calenzano, Italy) as a treatment for benign prostatic hyperplasia (BPH) and prostate cancer (PCa) using the Delphi consensus method.methods: Italian and international experts on BPH and PCa participated in a collaborative consensus project. During two rounds, they expressed their opinions on Echolaser® TPLA for the treatment of BPH and PCa answering online questionnaires on indications, methodology, and potential complications of this technology. Level of agreement or disagreement to reach consensus was set at 75%. If the consensus was not achieved, questions were modified after each round. A final round was performed during an online meeting, in which results were discussed and finalized.Results: Thirty-two out of forty invited experts participated and consensus was reached on all topics. Agreement was achieved on recommending Echolaser® TPLA as a treatment of BPH in patients with ample range of prostate volume, from mL (80%) to >80 mL (80%), comorbidities (100%), antiplatelet or anticoagulant treatment (96%), indwelling catheter (77%), and strong will of preserving ejaculatory function (100%). majority of respondents agreed that Echolaser® TPLA is a potential option for the treatment of localized PCa (78%) and recommended it for low-risk PCa (90%). During the final round, experts concluded that it can be used for intermediate-risk PCa and it should be proposed as an effective alternative to radical prostatectomy for patients with strong will of avoiding urinary incontinence and sexual dysfunction. Almost all participants agreed that the transperineal approach of this organ-sparing technique is safer than transrectal and transurethral approaches typical of other techniques (97% of agreement among experts). Pre-procedural assessment, technical aspects, post-procedural catheterization, pharmacological therapy, and expected outcomes were discussed, leading to statements and recommendations.Conclusion: Ech

关键词： Transperineal laser ablation Prostatecancer Benignprostatic hyperplasia Delphi consensus

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Stable methylammonium-Free p-i-n Perovskite Solar Cells and mini-modules with Phenothiazine dimers as Hole-Transporting materials

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Energy & Environmental materials 2023年第6期6卷 383-392页

作者： Luigi Angelo Castriotta Rossella Infantino Luigi Vesce maurizio Stefanelli Alessio Dessì Carmen Coppola massimo Calamante Gianna Reginato Alessandro mordini Adalgisa Sinicropi Aldo di carlo Lorenzo Zani Centre for Hybrid and Organic Solar Energy(C.H.O.S.E.) Department of Electronic EngineeringUniversity of Rome Tor Vergata00133 RomeItaly Institute of Chemistry of Organometallic Compounds(CNR-ICCOm) Via Madonna del Piano 1050019 Sesto FiorentinoItaly Department of Biotechnology Chemistry and PharmacyUniversity of SienaVia Aldo Moro 253100 SienaItaly CSGI Consorzio per lo Sviluppo dei Sistemi a Grande InterfaseVia della Lastruccia 350019 Sesto FiorentinoItaly Department of Chemistry“U.Schiff” University of FlorenceVia della Lastruccia 1350019 Sesto FiorentinoItaly Institute of Structure of matter(CNR-ISm) Via del Fosso del Cavaliere 10000133 RomeItaly

During the last decade,perovskite solar technologies underwent an impressive development,with power conversion efficiencies reaching 25.5%for single-junction devices and 29.8%for Silicon-Perovskite tandem configurations.Even though research mainly focused on improving the efficiency of perovskite photovoltaics(PV),stability and scalability remain fundamental aspects of a mature photovoltaics technology.For n-i-p structure perovskite solar cells,using poly-triaryl(amine)(PTAA)as hole transport layer(HTL)allowed to achieve marked improvements in device stability compared with other common hole conductors.For p-i-n structure,poly-triaryl(amine)is also routinely used as dopant-free hole transport layer,but problems in perovskite film growth,and its limited resistance to stress and imperfect batch-to-batch reproducibility,hamper its use for device upscaling.Following previous computational investigations,in this work,we report the synthesis of two small-molecule organic hole transport layers(BPT-1,2),aiming to solve the above-mentioned issues and allow upscale to the module level.By using BPT-1 and methylammonium-free perovskite,max.Power conversion efficiencies of 17.26%and 15.42%on a small area(0.09 cm^(2))and mini-module size(2.25 cm^(2)),respectively,were obtained,with a better reproducibility than with poly-triaryl(amine).moreover,BPT-1 was demonstrated to yield more stable devices compared with poly-triaryl(amine)under ISOS-D1,T1,and L1 accelerated life-test protocols,reaching maximum T_(90)values>1000 h on all tests.

关键词： methylammonium-free perovskite mini-modules organic hole-transporting layers perovskite solar cells stability studies

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Sodium diffuses from Glass Substrates through P1 Lines and Passivates Defects in Perovskite Solar modules

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Energy & Environmental materials 2023年第6期6卷 393-401页

作者： Felix Utama Kosasih Francesco di Giacomo Jordi Ferrer Orri Kexue Li Elizabeth m.Tennyson Weiwei Li Fabio matteocci Gunnar Kusch Narges Yaghoobi Nia Rachel A.Oliver Judith L.macmanus-Driscoll Katie L.moore Samuel D.Stranks Aldo di carlo Giorgio divitini Caterina Ducati Department of materials Science and metallurgy University of Cambridge27 Charles Babbage RoadCambridge CB30FSUK Centre for Hybrid and Organic Solar Energy(CHOSE) Department of Electronic EngineeringUniversity of Rome Tor VergataRome 00133Italy Cavendish Laboratory University of CambridgeJJ Thomson AvenueCambridge CB30HEUK Department of materials and Photon Science Institute University of ManchesterOxford RoadManchester M139PLUK Department of Chemical Engineering and Biotechnology University of CambridgePhilippa Fawcett DriveCambridge CB30ASUK Laboratory for Advanced Solar Energy(LASE) National University of Science and Technology MISiSLeninskiy Prospekt 4Moscow 119049Russia Energy Research Institute@NTU Nanyang Technological University50 Nanyang DriveSingapore 637553Singapore mIIT Key Laboratory of Aerospace Information materials and Physics College of PhysicsNanjing University of Aeronautics and AstronauticsNanjing 211106China Istituto di Struttura della materia-CNR(ISm-CNR) Via del Fosso del Cavaliere 100Rome 00133Italy Electron Spectroscopy and Nanoscopy Istituto Italiano di TecnologiaVia Morego 30Genova 16163Italy

most thin-film photovoltaic modules are constructed on soda-lime glass(SLG)substrates containing alkali oxides,such as Na_(2)O.Na may diffuse from SLG into a module's active layers through P1 lines,an area between a module's constituent cells where the substrate-side charge transport layer(CTL)is in direct contact with SLG.Na diffusion from SLG is known to cause several important effects inⅡ-Ⅵand chalcogenide solar modules,but it has not been studied in perovskite solar modules(PSms).In this work,we use complementary microscopy and spectroscopy techniques to show that Na diffusion occurs in the fabrication process of PSms.Na diffuses vertically inside P1 lines and then laterally from P1 lines into the active area for up to 360 pm.We propose that this process is driven by the high temperatures the devices are exposed to during CTL and perovskite annealing.The diffused Na preferentially binds with Br,forming Br-poor,l-rich perovskite and a species rich in Na and Br(Na-Br)close to P1 lines.Na-Br passivates defect sites,reducing non-radiative recombination in the perovskite and boosting its luminescence by up to 5×.Na-Br is observed to be stable after 12 weeks of device storage,suggesting long-lasting effects of Na diffusion.Our results not only point to a potential avenue to increase PSm performance but also highlight the possibility of unabated Na diffusion throughout a module's lifetime,especially if accelerated by the electric field and elevated temperatures achievable during device operation.

关键词： defect passivation monolithic interconnection perovskite solar modules soda-lime glass sodium diffusion solar cells thin-film photovoltaics

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深海环境海洋生态系统监测与修复新技术

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Engineering 2024年第3期34卷 195-211页

作者： Jacopo Aguzzi Laurenz Thomsen Sascha Flögel Nathan J.Robinson Giacomo Picardi Damianos Chatzievangelou Nixon Bahamon Sergio Stefanni Jordi Grinyó Emanuela Fanelli Cinzia Corinaldesi Joaquin Del rio Fernandez marcello Calisti Furu mienis Elias Chatzidouros Corrado Costa Simona Violino michael Tangherlini Roberto Danovaro Instituto de Ciencias del mar(ICm-CSIC) Barcelona 08003Spain Stazione Zoologica Anton Dohrn Naples 80121Italy University of Gothenburg Göteborg 40530Sweden GEOmAR Helmholtz Centre for Ocean Research Kiel 24148Germany Fundación Oceanogràfic de la Comunitat Valenciana Valencia 46013Spain Royal Netherlands Institute for Sea Research(NIOZ) Den Burg Texel 1790 ABNetherlands Polytechnic University of marche(UNIVPm) Ancona 60131Italy SARTI-mAR of the Universitat Politecnica de Catalunya(UPC) Vilanova i la Geltrú08800Spain Lincoln Institute for Agri-food Technology University of LincolnLincoln LN22LGUK Engitec Systems International Limited Limassol 3083Cyprus Consiglio per la Ricerca in Agricoltura e L’analisi Dell’economia Agraria(CREA) Centro di Ricerca Ingegneria e Trasformazioni AgroalimentariMonterotondo 00015Italy

The United Nations(UN)’s call for a decade of“ecosystem restoration”was prompted by the need to address the extensive impact of anthropogenic activities on natural ecosystems.marine ecosystem restoration is increasingly necessary due to increasing habitat degredation in deep waters(>200 m depth).At these depths,which are far beyond those accessible by divers,only established and emerging robotic platforms such as remotely operated vehicles(ROVs),autonomous underwater vehicles(AUVs),landers,and crawlers can operate through manipulators and multiparametric sensor arrays(e.g.,optoacoustic imaging,omics,and environmental probes).The use of advanced technologies for deep-sea ecosystem restoration can provide:①high-resolution three-dimensional(3D)imaging and acoustic mapping of substrates and key taxa,②physical manipulation of substrates and key taxa,③real-time supervision of remote operations and long-term ecological monitoring,and④the potential to work autonomously.Here,we describe how robotic platforms with in situ manipulation capabilities and payloads of innovative sensors could autonomously conduct active restoration and monitoring across large spatial scales.We expect that these devices will be particularly useful in deep-sea habitats,such as①reef-building cold-water corals,②soft-bottom bamboo corals,and③soft-bottom fishery resources that have already been damaged by offshore industries(i.e.,fishing and oil/gas).

关键词： Ecosystem restoration Robotic manipulation Acoustic tracking Fishery resources Artificial reefs

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基于三维裂隙网络的岩体剪切特性尺寸效应分析

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哈尔滨工业大学学报 2024年第3期56卷 9-18页

作者：宋盛渊黄迪隋佳轩陶勇马牧野李豪杰吉林大学建设工程学院长春130000 吉林省地质环境监测总站长春130000

为研究复杂裂隙岩体剪切特性的尺寸效应,以西藏怒江松塔水电站PDC3平硐为例,在现场采集裂隙信息的基础上,基于颗粒流PFC3D软件通过统计学方法及蒙特卡洛原理生成三维裂隙网络,构建等效岩体,进行大尺度直剪模拟试验得到裂隙岩体的抗剪强... 详细信息

为研究复杂裂隙岩体剪切特性的尺寸效应,以西藏怒江松塔水电站PDC3平硐为例,在现场采集裂隙信息的基础上,基于颗粒流PFC3D软件通过统计学方法及蒙特卡洛原理生成三维裂隙网络,构建等效岩体,进行大尺度直剪模拟试验得到裂隙岩体的抗剪强度、内摩擦系数及内聚力,分别研究其尺寸效应并确定不同参数下的REV尺寸,继而对相关参数和试样尺寸分别进行非线性回归拟合,探究其函数关系。结果表明:抗剪强度、内聚力及内摩擦系数随着试样尺寸的变化而趋于稳定,且不同参数得到的REV大小不同;综合分析不同参数的REV尺寸,得出研究区裂隙岩体的剪切特性REV尺寸为11 m×11 m×11 m;通过函数关系拟合,抗剪强度、内聚力和内摩擦系数与试样尺寸之间均存在指数函数关系。该成果为研究复杂裂隙岩体的力学REV以及合理确定力学参数提供了依据。

关键词：复杂裂隙岩体尺寸效应三维裂隙网络直剪模拟剪切特性

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Respiratory muscle training with electronic devices in the postoperative period of hepatectomy:A randomized study

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World Journal of Hepatology 2023年第5期15卷 688-698页

作者： marcelo Gustavo Pereira Aurea maria Oliveira Silva Fernanda diório masi Galhardo Beatriz Dellamutta miranda Almeida Railaine Lais Lopes Ilka de Fatima Santana Ferreira Boin Hospital de Clínicas Universidade Estadual de CampinasCampinas 13076-4151São PauloBrazil Faculdade de Ciências médicas Universidade Estadual de CampinasCampinas 13083-887São PauloBrazil Hospital de Clínicas da Unicamp Universidade Estadual de CampinasCampinas 13083-888São PauloBrazil

BACKGROUND many studies have been developed with a focus on surgical techniques and drugs,but few that address the importance of rehabilitation in the pre and postoperative period,and the specific benefits for each surgical procedure or type of neoplasm,aiming to minimize respiratory complications in the postoperative period.AIm To compare the strength of the respiratory muscles in the pre and postoperative periods of hepatectomy by laparotomy and to verify the incidence of postoperative pulmonary complications among the groups studied.mETHODS Prospective,randomized,clinical trial study that compared the inspiratory muscle training group(GTmI)with the control group(CG).After the collection of sociodemographic and clinical data,in both groups,preoperatively,on the first and fifth postoperative days,vital signs and pulmonary mechanics were evaluated and recorded.Albumin and bilirubin values were recorded for the albumin-bilirubin(ALBI)score.After randomization and allocation of participants,those in the CG underwent conventional physical therapy and those in the GTmI underwent conventional physical therapy plus inspiratory muscle,in both groups for five postoperative days.RESULTS Of 76 subjects met eligibility criteria.The collection of 41 participants was completed:20 in the CG and 21 in the GTmI.The most frequent diagnosis was 41.5%with liver metastasis,followed by 26.8%with hepatocellular carcinoma.As for respiratory complications in the GTmI,there was no incidence.In the CG,there were three respiratory complications.Patients in the CG classified as ALBI score 3 presented,statistically,a higher energy value compared to patients classified as ALBI score 1 and 2(P=0.0187).Respiratory variables,measured preoperatively and on the first postoperative day,had a significant drop in both groups from the preoperative to the first postoperative day(P≤0.0001).When comparing the preoperative period and the fifth postoperative day between the GTmI and the CG,the maximal inspiratory pressure variable in the GTmI was statistic

关键词： postoperative shorter fifth

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On-surface activation of benzylic C-H bonds for the synthesis of pentagon-fused graphene nanoribbons

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Nano Research 2021年第12期14卷 4754-4759页

作者： Xiushang Xu marco di Giovannantonio José I.Urgel carlo A.Pignedoli Pascal Ruffieux Klaus müllen Roman Fasel Akimitsu Narita Present address:Istituto di Struttura della materia-CNR(ISm-CNR) via Fosso del Cavaliere 10000133RomaItaly Present address:ImDEA Nanoscience C/Faraday 9Campus de Cantoblanco28049MadridSpain max Planck Institute for Polymer Research 55128MainzGermany Empa Swiss Federal Laboratories for Materials Science and Technologynanotech@surfaces Laboratory8600DübendorfSwitzerland Organic and Carbon Nanomaterials Unit Okinawa Institute of Science and Technology Graduate University1919-1 TanchaOnna-sonKunigami-gunOkinawa904-0495Japan Institute of Physical Chemistry Johannes Gutenberg University MainzDuesbergweg 10-1455128MainzGermany

Graphene nanoribbons (GNRs) have potential for applications in electronic devices. A key issue, thereby, is the fine-tuning of their electronic characteristics, which can be achieved through subtle structural modifications. These are not limited to the conventional armchair, zigzag, and cove edges, but also possible through incorporation of non-hexagonal rings. On-surface synthesis enables the fabrication and visualization of GNRs with atomically precise chemical structures, but strategies for the incorporation of non-hexagonal rings have been underexplored. Herein, we describe the on-surface synthesis of armchair-edged GNRs with incorporated five-membered rings through the C-H activation and cyclization of benzylic methyl groups. Ortho-Tolyl-substituted dibromobianthryl was employed as the precursor monomer, and visualization of the resulting structures after annealing at 300 °C on a gold surface by high-resolution noncontact atomic force microscopy clearly revealed the formation of methylene-bridged pentagons at the GNR edges. These persisted after annealing at 340 °C, along with a few fully conjugated pentagons having singly-hydrogenated apexes. The benzylic methyl groups could also migrate or cleave-off, resulting in defects lacking the five-membered rings. moreover, unexpected and unique structural rearrangements, including the formation of embedded heptagons, were observed. Despite the coexistence of different reaction pathways that hamper selective synthesis of a uniform structure, our results provide novel insights into on-surface reactions en route to functional, non-benzenoid carbon nanomaterials.

关键词： graphene nanoribbons on-surface synthesis scanning-tunneling microscope noncontact atomic force microscope C-H activation

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