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Graphene binding on black phosphorus enables high on/off ratios and mobility

National Science Review 2024年第2期11卷 188-195页

作者： Fanrong Lin Zhonghan Cao Feiping Xiao Jiawei Liu Jiabin Qiao Minmin Xue Zhili Hu Ying Liu Huan Lu Zhuhua Zhang Jens Martin Qingjun Tong Wanlin Guo Yanpeng Liu Key Laboratory for Intelligent Nano Materials and Devices of Ministry of Education State Key Laboratory of Mechanics and Control of Mechanical Structures and Institute for Frontier Science Nanjing University of Aeronautics and Astronautics Centre for Advanced 2D Materials National University of Singapore School of Physics and Electronics Hunan University Centre for Quantum Physics Key Laboratory of Advanced Optoelectronic Quantum Architecture and MeasurementSchool of PhysicsBeijing Institute of Technology Leibniz Institute für Kristallzüchtung

Graphene is one of the most promising candidates for integrated circuits due to its robustness against short-channel effects, inherent high carrier mobility and desired gapless nature for Ohmic contact, but it is difficult to achieve satisfactory on/off ratios even at the expense of its carrier mobility, limiting its device applications. Here, we present a strategy to realize high back-gate switching ratios in a graphene monolayer with well-maintained high mobility by forming a vertical heterostructure with a black phosphorus multi-layer. By local current annealing, strain is introduced within an established area of the graphene, which forms a reflective interface with the rest of the strain-free area and thus generates a robust off-state via local current depletion. Applying a positive back-gate voltage to the heterostructure can keep the black phosphorus insulating, while a negative back-gate voltage changes the black phosphorus to be conductive because of hole accumulation. Then, a parallel channel is activated within the strain-free graphene area by edge-contacted electrodes, thereby largely inheriting the intrinsic carrier mobility of graphene in the on-state. As a result, the device can provide an on/off voltage ratio of >10～3 as well as a mobility of ～8000 cm2V-1s-1at room temperature, meeting the low-power criterion suggested by the International Roadmap for Devices and Systems.

关键词： graphene on/offratio mobility black phosphorus reflective interface

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High-throughput screening of single-atom catalysts confined in monolayer black phosphorus for efficient nitrogen reduction reaction

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Nano Research 2024年第4期17卷 2360-2367页

作者： Xiao-Yan Li Manyi Duan Pengfei Ou Department of Electrical and Computer Engineering University of TorontoTorontoOntario M5S 1A4Canada School of Physics and Electronic Engineering Sichuan Normal UniversityChengdu 610101China Department of Chemistry Northwestern UniversityEvanstonIL 60208USA

The discovery of metal-nitrogen centers as the active sites for electrolysis has aroused significant interest in utilizing single-atom catalysts for nitrogen reduction reaction(NRR).Properly designed nanostructured catalysts that strongly interact with nitrogen molecules(N_(2))can promote adsorption and activation,thereby resulting in efficient catalysts with high stability,activity,and selectivity.In this study,using density functional theory calculations,we selected monolayer black phosphorus(BP)as the substrate and screened a series of single-atom transition metals confined in tri-coordinated and tetra-coordinated active centers(without and with N dopants)to electro-catalyze NRR.As a result,we have identified two promising candidates(Hf_(1)-N_(1)P_(2)-1 and Tc_(1)-N_(4)),which exhibit not only low overpotentials of 0.56 and 0.49 V but also high thermodynamic and electrochemical stability,as well as good selectivity towards NRR over the competing hydrogen evolution reaction.We also demonstrate the ability of Hf_(1)-N_(1)P_(2)-1 and Tc_(1)-N_(4) to activate and hydrogenate N_(2) by donating electrons and regulating charge transfer.This study not only predicts new BP-based promising catalysts but also provides guidance for the rational design of high-performance NRR electrocatalysts under ambient conditions.

关键词： N_(2) electroreduction reaction single-atom catalysts black phosphorus density functional theory high-throughput calculations

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black phosphorus nanosheets-enabled DNA hydrogel integrating 3D-printed scaffold for promoting vascularized bone regeneration

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Bioactive Materials 2023年第3期21卷 97-109页

作者： Yali Miao Yunhua Chen Jinshui Luo Xiao Liu Qian Yang Xuetao Shi Yingjun Wang School of Materials Science and Engineering South China University of TechnologyGuangzhou510641China National Engineering Research Center for Tissue Restoration and Reconstruction South China University of TechnologyGuangzhou510006China Key Laboratory of Biomedical Engineering of Guangdong Province And Innovation Center for Tissue Restoration and ReconstructionSouth China University of TechnologyGuangzhou510006China Key Laboratory of Biomedical Materials and Engineering of the Ministry of Education South China University of TechnologyGuangzhou510006China

The classical 3D-printed scaffolds have attracted enormous interests in bone regeneration due to the customized structural and mechanical adaptability to bone defects.However,the pristine scaffolds still suffer from the absence of dynamic and bioactive microenvironment that is analogous to natural extracellular matrix(ECM)to regulate cell behaviour and promote tissue regeneration.To address this challenge,we develop a black phosphorus nanosheets-enabled dynamic DNA hydrogel to integrate with 3D-printed scaffold to build a bioactive gel-scaffold construct to achieve enhanced angiogenesis and bone regeneration.The black phosphorus nanosheets reinforce the mechanical strength of dynamic self-healable hydrogel and endow the gel-scaffold construct with preserved protein binding to achieve sustainable delivery of growth factor.We further explore the effects of this activated construct on both human umbilical vein endothelial cells(HUVECs)and mesenchymal stem cells(MSCs)as well as in a critical-sized rat cranial defect model.The results confirm that the gel-scaffold construct is able to promote the growth of mature blood vessels as well as induce osteogenesis to promote new bone formation,indicating that the strategy of nano-enabled dynamic hydrogel integrated with 3D-printed scaffold holds great promise for bone tissue engineering.

关键词： DNA hydrogels 3D-printed scaffold black phosphorus Vascularized bone regeneration

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black phosphorus-based heterostructures for photocatalysis and photoelectrochemical water splitting

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Journal of Energy Chemistry 2022年第4期31卷 745-779页

作者： Shutao Li Yihe Zhang Hongwei Huang Beijing Key Laboratory of Materials Utilization of Nonmetallic Minerals and Solid Wastes and School of Materials Science and Technology China University of GeosciencesBeijing 100083China

Semiconductor-based photocatalytic and photoelectrochemical(PEC) processes can convert solar energy into high-density chemical energy or for the treatment of environmental pollutants, which are ideal ways to deal with environmental and energy crises. The development of high-efficiency photocatalysts and photoelectrodes is the key to the in-depth development and practical application of the two technologies.black phosphorus(BP) has excellent physicalcochemical properties such as adjustable band gap, high carrier mobility, large specific surface area and anisotropy, making it one of the most promising catalysts.BP-based heterostructure can not only realize the effective separation of photogenerated carriers but also improve the stability of BP, and is widely used in photocatalytic and PEC reactions. In this review, we first introduce the crystal structure, band structure, anisotropy, and preparation of BP with different dimensions(bulk, zero-dimension and two-dimension). Then, according to the transfer path of the photogenerated carriers and the components, the BP-based heterostructures are divided into type I heterojunction, type II heterojunction, Z-scheme heterojunction, S-scheme heterojunction, BP/carbonbased material heterostructure, BP/metal heterostructure and multi-component heterostructure.Highlighted are the diverse photocatalytic applications of BP-based heterostructure, such as water splitting and CO_(2)reduction, N_(2)fixation, pollutant degradation, photothermal and photodynamic therapy.Finally, some concluding views and opinions are stated on the challenges and opportunities faced by the further development of BP-based heterostructures in photocatalysis and PEC water splitting.

关键词： black phosphorus Heterostructure Photocatalysis Photoelectrochemical water splitting

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black phosphorus/Nanocarbons Constructing a Dual-Carbon Conductive Network for High-Performance Sodium-Ion Batteries

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Transactions of Tianjin University 2022年第2期28卷 132-143页

作者： Leping Dang Jiawei He Hongyuan Wei School of Chemical Engineering and Technology Tianjin UniversityTianjin 300072China

black phosphorus has been recognized as a prospective candidate anode material for sodium-ion batteries(SIBs)due to its ultrahigh theoretical capacity of 2596 mA·h/g and high electric conductivity of≈300 S/m.However,its large volume expansion and contraction during sodiation/desodiation lead to poor cycling stability.In this work,a BP/graphite nanoparticle/nitrogen-doped multiwalled carbon nanotubes(BP/G/CNTs)composite with a dual-carbon conductive network is successfully fabricated as a promising anode material for SIBs through a simple two-step mechanical milling process.The unique structure can mitigate the eff ect of volume changes and provide additional electron conduction pathways during cycles.Furthermore,the formation of P–O–C bonds helps maintain the intimate connection between phosphorus and carbon,thereby improving the cycling and rate performance.As a result,the BP/G/CNTs composite delivers a high initial Coulombic efficiency(89.6%)and a high specific capacity for SIBs(1791.3 mA·h/g after 100 cycles at 519.2 mA/g and 1665.2 mA·h/g after 100 cycles at 1298 mA/g).Based on these results,the integrated strategy of one-and two-dimensional carbon materials can guide other anode materials for SIBs.

关键词： Sodium-ion batteries Anode material black phosphorus Ball milling Carbon conductive network

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black phosphorus nanosheets-based tumor microenvironment responsive multifunctional nanosystem for highly efficient photo-/sono-synergistic therapy of non-Hodgkin lymphoma

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Chinese Chemical Letters 2023年第10期34卷 223-228页

作者： Xueli Zhu Shengmin Zhang Yi Cao Xiaojiao Ge Yi Huang Feng Mao Bo Chen Juan Li Youfeng Xu Aiguo Wu Department of Ultrasound Central LaboratoryNingbo First HospitalNingbo 315000China Cixi Institute of Biomedical Engineering International Cooperation Base of Biomedical Materials Technology and ApplicationChinese Academy of Sciences(CAS)Key Laboratory of Magnetic Materials and DevicesZhejiang Engineering Research Center for Biomedical MaterialsNingbo Institute of Materials Technology and EngineeringCASNingbo 315201China University of Chinese Academy of Sciences Beijing 100049China

Finding improved therapeutic protocols against non-Hodgkin’s lymphoma(NHL) remains an unmet clinical demand. Phototherapy is a promising alternative treatment for traditional clinical therapeutic methods, but the limited tissue penetration blocks the therapeutics. Inspired by the excellent physical and chemical properties of black phosphorus nanosheets(BPNSs), a fluorescence and thermal imaging guided photo-/sono-synergistic treatment platform BPNSs@PEG-SS-IR780/RGD is developed. This ingenious multifunctional theranostic platform not only exhibits outstanding photothermal conversion efficiency and highly efficient reactive oxygen species generation, but also has good biocompatibility, tumor-targeting and tumor microenvironment responsiveness. In addition, BPNSs@PEG-SS-IR780/RGD could actively target the tumor sites and generate excellent photothermal, photodynamic and sonodynamic therapeutic efficacy. Both in vitro and in vivo experiments indicate that BPNSs@PEG-SS-IR780/RGD can be a promising nanomaterial for NHL imaging and therapy. Taken together, this study not only expands the application field of black phosphorus materials, but also provides a possibility to design a new generation of NHL treatment regimens with clinical application potential.

关键词： Non-Hodgkin’s lymphoma black phosphorus IR780 Phototherapy Sonodynamic therapy

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black-phosphorus-based materials for application in solar cells

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Chinese Journal of Structural Chemistry 2023年第7期42卷 34-46页

作者： Xiaofeng Lin Xiaoxin Li Beichi Luo Dingshan Yu School of Chemical Engineering and Light Industry Guangdong University of TechnologyGuangzhou510006PR China Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education Sun Yat-Sen University Guangzhou510275PR China

In the context of green development,the use of solar cells with renewable and environment-friendly characteristics has been rapidly growing.There has been a continuous search for materials that can enhance their performance.black phosphorus,a new type of semiconductor material,has garnered significant attention due to its distinctive properties,particularly its direct band gap with tunable layers and high optoelectronic efficiency.This review summarizes the properties of black-phosphorus-based materials and focuses on their use as doping materials in various components of solar cells,such as the electron transport layer,hole transport layer,active layer,etc.The current challenges faced by black phosphorus materials and outlook on their future development have also been discussed.

关键词： black phosphorus Solar cells Doping materials Power conversion efficiency

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Visualized SERS Imaging of Single Molecule by Ag/ black phosphorus Nanosheets

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Nano-Micro Letters 2022年第5期14卷 47-61页

作者： Chenglong Lin Shunshun Liang Yusi Peng Li Long Yanyan Li Zhengren Huang Nguyen Viet Long Xiaoying Luo Jianjun Liu Zhiyuan Li Yong Yang State Key Laboratory of High‑Performance Ceramics and Superfine Microstructures Shanghai Institute of CeramicsChinese Academy of Sciences1295 Dingxi RoadShanghai 200050People’s Republic of China Graduate School of the Chinese Academy of Sciences No.19(A)Yuquan RoadBeijing 100049People’s Republic of China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049People’s Republic of China State Key Laboratory of Oncogenes and Related Genes Shanghai Cancer InstituteRenji HospitalShanghai Jiaotong University School of Medicine200032 ShanghaiPeople’s Republic of China School of Physics and Optoelectronics South China University of TechnologyGuangzhou 510641People’s Republic of China Department of Electronics and Telecommunications Saigon UniversityHochiminh CityVietnam

Single-molecule detection and imaging are of great value in chemical analysis,biomarker identification and other trace detection fields.However,the localization and visualization of single molecule are still quite a challenge.Here,we report a special-engineered nanostructure of Ag nanoparticles embedded in multi-layer black phosphorus nanosheets(Ag/BP-NS)synthesized by a unique photoreduction method as a surfaceenhanced Raman scattering(SERS)sensor.Such a SERS substrate features the lowest detection limit of 10^(–20) mol L^(−1) for R6G,which is due to the three synergistic resonance enhancement of molecular resonance,photoinduced charge transfer resonance and electromagnetic resonance.We propose a polarization-mapping strategy to realize the detection and visualization of single molecule.In addition,combined with machine learning,Ag/BP-NS substrates are capable of recognition of different tumor exosomes,which is meaningful for monitoring and early warning of the cancer.This work provides a reliable strategy for the detection of single molecule and a potential candidate for the practical bio-application of SERS technology.

关键词： black phosphorus Single molecule SERS Exosome Machine learning

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Growth of uniformly doped black phosphorus films through versatile atomic substitution

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Science China(Information Sciences) 2023年第6期66卷 78-86页

作者： Cheng CHEN Yang LU Chang LI Xingang HOU Yongjie WANG Junrong ZHANG Junyong WANG Kai ZHANG School of Nano-Tech and Nano-Bionics University of Science and Technology of China CAS Key Laboratory of Nanophotonic Materials and Devices & Key Laboratory of Nanodevices and Applications i-LabSuzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of Sciences Nano Science and Technology Institute University of Science and Technology of China

For the emerging excellent two-dimensional semiconductor black phosphorus(BP), doping has been proven as an effective way to tune its intrinsic properties. For the further development and expansion of BP-based research and application, the direct growth of doped BP films is highly desirable but still remains a challenge. In this work, the direct growth of uniformly doped-BP films on silicon substrates is achieved by a simple one-step vapor growth. The proposed decoupled feeding strategy significantly improves the effectiveness of doping and enables uniform dopant distribution in the grown films. The substitutional doping nature and high crystal quality of the grown doped films are confirmed by microscopy and crystal structural determination. Electrical transport measurement results reveal that Se and Te dopants perform mild electron doping effect and enable improve the electron mobility relative to pristine BP, while As dopant performs mild hole doping effect. It is believed that the direct growth of doped BP films in this work will facilitate the research development of BP in electronics and optoelectronics.

关键词： black phosphorus dope vapor growth thin film two-dimensional materials

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Highly stable aqueous phase black phosphorus quantum dots with enhanced fluorescence property

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Journal of Materials Science & Technology 2022年第21期116卷 50-57页

作者： Yingli Ma Xiaoguang Xu Xiaoshuang Zhang Mayifei Rong Liying Lu Yan Li Wenhao Dai Hongwu Du Yong Jiang School of Materials Science and Engineering University of Science and Technology BeijingBeijing 100083China School of Chemistry and Biological Engineering University of Science and Technology BeijingBeijing 100083China

black phosphorus quantum dots(BPQDs)are a kind of outstanding optical material due to the tunable band structure.However,their fluorescence property and stability are obviously weakened in the aqueous phase,which extremely restricts the development of BPQDs.Here,we propose a new method to prepare stable BPQDs in an aqueous solution directly with high absolute fluorescence quantum yield.Aqueous phase BPQDs are synthesized by liquid exfoliation and hydrothermal with NH_(2)-polyethylene glycol(PEG)-NH_(2) as the modification agent to protect the BPQDs,which have high stability more than six months.In addition,NH_(2)-PEG-NH_(2) is also a surface passivation agent to enhance the emission of BPQDs by forming P-N bonds,which is confirmed by an absolute fluorescent quantum yield of 11.5%.Moreover,BPQDs show excellent resistance to a strong acid environment and high ionic strengths except for Fe^(3+).Therefore,the BPQDs are a kind of highly selective and linear response fluorescence probe for Fe^(3+).Considering the good biocompatibility of BPQDs,they are employed as cell fluorescent label probes and show excellent fluorescence imaging contrast.Based on the unique structural stability and fluorescence performance in the aqueous phase,BPQDs are potential candidates for Fe^(3+)detection and optical bio-imaging.

关键词： black phosphorus Quantum dots Fluorescence Iron detection Cell imaging

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