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Aggregate 2023年第6期4卷 101-109页

作者： Dongdong Chang Xuetao Xiao Dongyue An Rong Zhang Xianyu Song yunqi liu Yan Zhao Xuefeng Lu Department of Materials Science State Key Laboratory of Molecular Engineering of PolymersFudan UniversityShanghaiChina Key Laboratory of Water Environment Evolution and Pollution Control in Three Gorges Reservoir School of Environmental and Chemical EngineeringChongqing Three Gorges UniversityChongqingChina

A series of newπ-conjugated macrocycles(AzoM-n-E,n 1–3)incorporating=azobenzene units have been synthesized by a facile strategy in one-pot *** resultant azobenzene-embedded macrocycles feature intrinsic photoresponsive behaviors and intriguing supramolecular assembling *** smallest macro-cycle AzoM-1-E with a rigid planar conjugated backbone structure is used to prepare the single crystal transistors,showing reversible optical *** moderate size macrocycle AzoM-2-E assembles into a dimer in the form of interpenetration throughπ-πstacking between azobenzene *** largest macrocycle AzoM-3-E with enhancedﬂexibility can adaptively assemble with various types of electron-deﬁcient guests accompanied by distortion of ***,AzoM-3-E assembles with the planar F4-TCNQ to form a tetragonal geometry by C-F⋅⋅⋅π and π-π interactions,while the assembly with ellipsoidal C70 viaπ-πinteractions induces AzoM-3-E to form a boat-shaped *** work will shed new light on the development of functional conjugated macrocycles in organic electronics.

关键词： azobenzene conjugated macrocycle host-guest interaction photoresponsive transistors supramolecular assembly

A nonchlorinated solvent-processed polymer semiconductor for high-performance ambipolar transistors

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National Science Review 2022年第4期9卷 139-147页

作者： Jie Yang Yaqian Jiang Zhiyuan Zhao Xueli Yang Zheye Zhang Jinyang Chen Junyu Li Wei Shi Shuai Wang Yunlong Guo yunqi liu Beijing National Laboratory for Molecular Sciences Key Laboratory of Organic SolidsInstitute of ChemistryChinese Academy of Sciences School of Chemistry and Chemical Engineering Huazhong University of Science and Technology

Ambipolar polymer semiconductors are potentially serviceable for logic circuits, light-emitting field-effect transistors(LFETs) and polymer solar cells(PSCs). Although several high-performance ambipolar polymers have been developed, their optoelectronic devices are generally processed from toxic chlorinated solvents. To achieve the commercial applications of organic FETs(OFETs), the polymers should be processed from nonchlorinated solvents, instead of chlorinated solvents. However, most conjugated polymers show poor solubility in nonchlorinated solvents. It is of great importance to develop ambipolar polymers that can be processed from nonchlorinated solvents. Here, we develop a nonchlorinated solvent processed polymer named poly[7-fluoro-N, N′-di(4-decyltetradecyl)-7′-azaisoindigo-6′,6′′-(thieno[3,2-b]thiophene-2,5-diyl)-7′′′-fluoro-N′′, N′′′-di(4-decyltetradecyl)-7′′-azaisoindigo-6,6′′′-([2,2′′-bithiophene]-5,5′′-diyl)](PITTI-BT) by designing a monomer with a large molar mass. The polymer displays good solubility in p-xylene(PX). Well-aligned films of PITTI-BT are achieved by an off-center spin-coating(SC) method. Based on the high-quality films, the OFETs fabricated from PX solution achieve record ambipolar performance with hole and electron mobilities of 3.06 and2.81 cm~2 V-1s-1, respectively. The combination of nonchlorinated solvents and good alignment process offers an effective and eco-friendly approach to obtain high-performance ambipolar transistors.

关键词： nonchlorinated solvent high performance ambipolar transistor alignment

Olefin-linked covalent organic frameworks with twisted tertiary amine knots for enhanced ultraviolet detection

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Chinese Chemical Letters 2022年第5期33卷 2621-2624页

作者： Qianying Guo Hongyan Ji Lei Yang Daizong Ji Zhaolin Ai Shi Luo Jiatao Sun yunqi liu Dacheng Wei State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular ScienceFudan UniversityShanghai 200433China Institute of Molecular Materials and Devices Fudan UniversityShanghai 200433China MIIT Key Laboratory for Low-Dimensional Quantum Structure and Devices Beijing Institute of TechnologyBeijing 100081China

Though Olefin-linked covalent organic frameworks(oCOFs)possess excellentπ-electron delocalization,the barely reversible olefin linkage brings challenges for oCOFs’synthesis and ***,we synthesize new oCOFs with tertiary amine knots which have twisted configuration and electron-donating *** into the structural variation and photoelectric performance shows that the twisted configuration of oCOF-TFPA could favor to the intramolecular charge transfer process and reduce the pos-sibility of aggregation-caused *** measurements and electric band structure cal-culation both verify the superiority of this oCOFs’structure in photoelectric sensing.

关键词： Covalent organic frameworks Olefin linkages Tertiary amine knots Twisted intramolecular charge transfer effect Ultraviolet detection

The design and synthesis of fused thiophenes and their applications in organic field-effect transistors

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Science China Chemistry 2010年第4期53卷 779-791页

作者： liu Ying, YU Gui & liu yunqi Beijing National Laboratory for Molecular Sciences, Key Laboratory of Organic Solids, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China Beijing National Laboratory for Molecular Sciences Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences Beijing China

Fused thiophenes refer to oligothienoacenes in which several thiophenes are coupled together via twoor multi-positions and their derivatives. The synthesized organic semiconductors based on fused thiophenes exhibit excellent field effect properties due to their efficient intermolecular S…S interactions and π…π stacking. The performances of organic field-effect transistors (OFETs) depend not only on the materials but also on the devices. Such factors which influence the device performances as device structures, fabrication technologies and interface engineering are extensively investigated based on the fused thiophenes. Searching for new organic semiconductors and improving the device fabrication technologies are two major issues in the development of OFETs.

关键词： fused thiophenes oligothienoacenes organic field-effect transistors device performance

Construction of N-doped carbon frames anchored with Co single atoms and Co nanoparticles as robust electrocatalyst for hydrogen evolution in the entire pH range

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Journal of Energy Chemistry 2022年第4期31卷 147-156页

作者： Minmin Wang Min Li Yilin Zhao Naiyou Shi Hui Zhang Yuxue Zhao Yaru Zhang Haoran Zhang Wenhong Wang Kaian Sun Yuan Pan Shoujie liu Houyu Zhu Wenyue Guo Yanpeng Li yunqi liu Chenguang liu State Key Laboratory of Heavy Oil Processing China University of Petroleum(East China)Qingdao 266580ShandongChina School of Materials Science and Engineering China University of Petroleum(East China)Qingdao 266580ShandongChina College of Chemistry and Materials Science Anhui Normal UniversityWuhu 241000AnhuiChina

The development of low-cost, efficient, and high atomic economy electrocatalysts for hydrogen evolution reaction(HER) in the entire p H range for sustainable hydrogen production is of great importance but still challenging. Herein, we synthesize a highly dispersed N-doped carbon frames(NCFs) anchored with Co single atoms(SAs) and Co nanoparticles(NPs) catalyst by a doping-adsorption-pyrolysis strategy for electrocatalytic hydrogen evolution. The Co SAs-Co NPs/NCFs catalyst exhibits an excellent HER activity with small overpotential, low Tafel slope, high turnover frequency as well as remarkable stability. It also exhibits a superior HER performance in the entire p H range. Combining with experimental and theoretical calculation, we find that Co SAs with Co-N_(3) coordination structure and Co NPs have a strong interaction for promoting synergistic HER electrocatalytic process. The H_(2)O molecule is easily activated and dissociated on Co NPs, while the generated H^(*) is easily adsorbed on Co SAs for HER, which makes the Co SAs-Co NPs/NCFs catalyst exhibit more suitable H adsorption strength and more conducive to the activation and dissociation of H_(2)O molecules. This work not only proposes a novel idea for constructing coupling catalyst with atomic-level precision, but also provides strong reference for the development of high-efficiency HER electrocatalysts for practical application.

关键词： Single-atom catalyst Doping-adsorption-pyrolysis strategy Structure regulation Synergistic electrocatalysis EXAFS

Synthesis of Large-Area, Few-Layer Graphene on Iron Foil by Chemical Vapor Deposition

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Nano Research 2011年第12期4卷 1208-1214页

作者： Yunzhou Xue Bin Wu Yunlong Guo Liping Huang Lang Jiang Jianyi Chen Dechao Geng yunqi liu Wenping Hu Gui Yu Beijing National Laboratory for Molecular Sciences Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy ofSciences Beijing 100190 China

We demonstrate a simple and controllable way to synthesize large-area, few-layer graphene on iron substrates by an optimized chemical vapor deposition （CVD） method using a mixture of methane and hydrogen. Based on an analysis of the Fe-C phase diagram, a suitable procedure for the successful synthesis of graphene on Fe surfaces was designed. An appropriate temperature and cooling process were found to be very important in the synthesis of highly crystalline few-layer graphene. Graphene-based field-effect transistor （FET） devices were fabricated using the resulting few-layer graphene, and showed good quality with extracted mobilities of 300-1150 cm2/（V.s）.

关键词： Graphene iron foil chemical vapor deposition (CVD) method Raman spectroscopy field-effect transistor (FET)

Ultrahigh Density Modulation of Aligned Single-Walled Carbon Nanotube Arrays

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Nano Research 2011年第10期4卷 931-937页

作者： Bin Wu Dechao Geng Yunlong Guo Liping Huang Jianyi Chen Yunzhou Xue Gui Yu yunqi liu Hisashi Kajiura Yongming Li Beijing National Laboratory for Molecular Sciences Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China Material Laboratory Sony Corporation Atsugi Tec. No.2 4-16-10kata Atsugi Kanagawa 243-0021 Japan These authors contributed equally to this work.

Controlling the densities of aligned single-walled carbon nanotube arrays （SWNTs） on ST-cut quartz is a critical step in various applications of these materials. However the growth mechanism for tuning SWNT density using the chemical vapor deposition （CVD） method is still not well understood, preventing the development of efficient ways to obtain the desired results. Here we report a general ＂periodic＂ approach that achieves ultrahigh density modulation of SWNT arrays on ST-cut quartz substrates--with densities increased by up to -60 times compared with conventional methods using the same catalyst densities--by varying the CH4 gas ＂off＂ time. This approach is applicable to a wide range of initial catalyst densities, substrates, catalyst types and growth conditions. We propose a general mechanism for the catalyst size-dependent nucleation of SWNTs associated with different free carbon concentrations, which explains all the observations. Moreover, the validity of the model is supported by systematic experiments involving the variation of key parameters in the ＂periodic＂ CVD approach.

关键词： SWNT density chemical vapor deposition periodic growth growth mechanism

Detecting secondary spin with extreme mass ratio inspirals in scalar-tensor theory

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Chinese Physics C 2024年第9期48卷 210-224页

作者： Hong Guo Chao Zhang yunqi liu Rui-Hong Yue Yun-Gui Gong Bin Wang Center for Gravitation and Cosmology College of Physical Science and TechnologyYangzhou UniversityYangzhou 225009China Escola de Engenharia de Lorena Universidade de São PauloLorenaSP 12602-810Brazil Shanghai Frontier Research Center for Gravitational Wave Detection Shanghai Jiao Tong UniversitySha nghai 200240 China 4 School of Aeronautics and AstronauticsShanghai Jiao Tong UniversityShanghai 200240China School of Physics Huazhong University of Science and TechnologyWuhan 430074China Department of Physics School of Physical Science and TechnologyNingbo UniversityNingbo 315211China

In this study,we investigate the detectability of the secondary spin in an extreme mass ratio inspiral(EMRI) system within a modified gravity model coupled with a scalar *** central black hole,which reduces to a Kerr one,is circularly spiralled by a scalar-charged spinning secondary body on the equatorial *** analysis reveals that the presence of the scalar field amplifies the secondary spin effect,allowing for a lower limit of the detectability and an improved resolution of the secondary spin when the scalar charge is sufficiently *** findings suggest that secondary spin detection is more feasible when the primary mass is not large,and TianQin is the optimal choice for detection.

关键词： Gravitational wave EMRI secondary spin scalar radiation

Single-atomic Mn sites coupled with Fe_(3)C nanoparticles encapsulated in carbon matrixes derived from bimetallic Mn/Fe polyphthalocyanine conjugated polymer networks for accelerating electrocatalytic oxygen reduction

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Nano Research 2022年第9期15卷 7976-7985页

作者： Yuan Pan Min Li Wanliang Mi Minmin Wang Junxi Li Yilin Zhao Xuelu Ma Bin Wang Wei Zhu Zhiming Cui Hailiang Yin yunqi liu State Key Laboratory of Heavy Oil Processing China University of Petroleum(East China)Qingdao 266580China Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) College of ChemistryNankai UniversityTianjin 300071China Research Institute of Petroleum Processing SinopecBeijing 100083China School of Chemical&Environmental Engineering China University of Mining&TechnologyBeijing 100083China School of Chemistry and Chemical Engineering Shaanxi Normal UniversityXi’an 710119China State Key Lab of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China Key Laboratory of Fuel Cell Technology of Guangdong Province South China University of TechnologyGuangzhou 510641China Academy of Science&Technology China University of Petroleum(East China)Dongying 257061China

The construction of robust coupling catalysts for accelerating electrocatalytic oxygen reduction reaction(ORR)through the modulation of the electronic structure and local atomic configuration is critical but remains ***,we report a facile and effective isolation-polymerization-pyrolysis(IPP)strategy for high-precision synthesis of single-atomic Mn sites coupled with Fe_(3)C nanoparticles encapsulated in N-doped porous carbon matrixes(Mn SAs/Fe_(3)C NPs@NPC)catalyst derived from predesigned bimetallic Fe/Mn polyphthalocyanine(FeMn-BPPc)conjugated polymer networks by solid-phase reaction *** from the synergistic effects between the single-atomic Mn-N_(4)sites and Fe_(3)C NPs as well as the confinement effect of NPC,the Mn SAs/Fe_(3)C NPs@NPC catalyst exhibited excellent electrocatalytic activity and stability for *** assembled Znair battery displayed larger power density of 186 mW·cm^(−2)than that of Pt/C+Ir/C-based *** also exhibits excellent stability without obvious voltage change after 106 cycles with 36 *** in-situ Raman spectra with in-situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS)characterization results indicated that the Mn-N_(4)site as an active site for the O_(2)adsorption-activation process,which effectively facilitates the generation of key*OOH intermediates and*OH desorption to promote the multielectron reaction *** calculation reveals that the excellent electrocatalytic performance originates from the charge redistribution and the d orbital shift resulting from Mn-Fe bond,which buffers the activity of ORR through the electron reservoir capable of electron donation or *** work paves a novel IPP strategy for constructing high-performance coupling electrocatalyst towards the ORR for energy conversion devices.

关键词： single atom catalyst nanoparticles electrocatalyst oxygen reduction zinc-air battery

High-performance flexible organic field effect transistors with print-based nanowires

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Microsystems & Nanoengineering 2023年第3期9卷 83-93页

作者： Liangkun Lu Dazhi Wang Changchang Pu Yanyan Cao Yikang Li Pengfei Xu Xiangji Chen Chang liu Shiwen Liang liujia Suo Yan Cui Zhiyuan Zhao Yunlong Guo Junsheng Liang yunqi liu Laboratory for Micro/Nano Technology and System of Liaoning Province Dalian University of TechnologyDalian 116024China State Key Laboratory of High-Performance Precision Manufacturing Dalian University of TechnologyDalianChina Ningbo Institute of Dalian University of Technology Ningbo 315000China Beijing National Laboratory for Molecular Sciences Key Laboratory of Organic SolidsInstitute of ChemistryChinese Academy of SciencesBeijing 100190China

Polymer nanowire(NW)organic field-effect transistors(OFETs)integrated on highly aligned large-area flexible substrates are candidate structures for the development of high-performance flexible *** work presents a universal technique,coaxial focused electrohydrodynamic jet(CFEJ)printing technology,to fabricate highly aligned 90-nm-diameter polymer *** method allows for the preparation of uniformly shaped and precisely positioned nanowires directly on flexible substrates without transfer,thus ensuring their electrical *** indacenodithiophene-co-benzothiadiazole(IDT-BT)and poly(9,9-dioctylfluorene-co-benzothiadiazole)(F8-BT)as example materials,5 cm^(2) arrays were prepared with only minute size variations,which is extremely difficult to do using previously reported *** to 2D-GIXRD analysis,the molecules inside the nanowires mainly adopted face-onπ-stacking crystallite *** is quite different from the mixed arrangement of thin ***-based OFETs exhibited a high average hole mobility of 1.1 cm^(2) V^(−1) s^(−1) and good device uniformity,indicating the applicability of CFEJ printing as a potential batch manufacturing and integration process for high-performance,scalable polymer nanowire-based OFET *** technique can be used to fabricate various polymer arrays,enabling the use of organic polymer semiconductors in large-area,high-performance electronic devices and providing a new path for the fabrication of flexible displays and wearable electronics in the future.

关键词： performance nanowires arrangement