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| 1 | 2D graphdiyne materials:challenges and opportunities in energy field显示文摘Graphdiyne(GDY),a novel two-dimensional(2D)carbon allotrope featuring one-atom-thick planar layers of sp andhybridized carbon network,is a rapidly rising star on the horizon of materials science.Because of its unparalleled structural,electronic,chemical and physical properties,it has been receiving unprecedented increases from fundamental studies to practical applications,particularly the field of energetic materials.In this review,we aim at providing an up-to-date comprehensive overview on the state-of-the-art research into GDY,from theoretical studies to the key achievements in the development of new GDY-based energetic materials for energy storage and conversion.By reviewing the state-of-the-art achievements,we aim to address the benefits and issues of GDY-based materials,as well as highlighting the existing key challenges and future opportunities in this exciting field. | Yurui Xue Yuliang Li Jin Zhang Zhongfan Liu Yuliang Zhao | 2018 | Science China Chemistry2018，61，7： | 7 |
| 2 | Nickel(hydro)oxide/graphdiyne Catalysts for Efficient Oxygen Production Reaction显示文摘The transition metal-based materials have been regarded as promising electrocatalysts for oxygen evolution reaction(OER).However,achieving higher efficiency is largely limited by the valence states of metal species.Herein,different graphdiyne(GDY)-nickel composites were designed and synthesized[Ni(OH)_(2)/GDY,NiOOH/GDY,and NiO_(x)/GDY]as the electrocatalysts for OER.The NiO_(x)/GDY possessing the mixed valence states can drive the OER more efficiently than Ni(OH)_(2)/GDY and NiOOH/GDY.NiO_(x)/GDY gives the smallest overpotential of 310 mV at 10 mA/cm^(2) for OER,which is even superior to commercial RuO_(2)electrocatalyst.Experimental results reveal that not only the fast charge transfer induced by GDY but also the prominent roles of mixed Ni^(2+)/Ni^(3+) valence states boost the OER electrocatalytic performances.The presence of the mixed valence state was demonstrated to be helpful for the charge transfer,resulting in the enhancement of the catalytic activity.This work may provide a new direction to design and fabricate high-performance materials for OER and beyond. | LUAN Xiaoyu XUE Yurui | 2021 | Chemical Research in Chinese Universities2021，37，6： | 2 |
| 3 | Graphdiyne-based metal atomic catalysts for synthesizing ammonia显示文摘Development of novel catalysts for nitrogen reduction at ambient pressures and temperatures with ultrahigh ammonia(NH_(3))yield and selectivity is challenging.In this work,an atomic catalyst with separated Pd atoms on graphdiyne(Pd-GDY)was synthesized,which shows fascinating electrocatalytic properties for nitrogen reduction.The catalyst has the highest average NH_(3)yield of 4.45±0.30 mgNH_(3)mg Pd^(-1)h^(-1),almost tens of orders larger than for previously reported catalysts,and 100%reaction selectivity in neutral media.Pd-GDY exhibits almost no decreases in NH_(3)yield and Faradaic efficiency.Density functional theory calculations show that the reaction pathway prefers to perform at the(Pd,C1,C2)active area because of the strongly coupled(Pd,C1,C2),which elevates the selectivity via enhanced electron transfer.By adjusting the p–d coupling accurately,reduction of self-activated nitrogen is promoted by anchoring atom selection,and side effects are minimized. | Huidi Yu Yurui Xue Lan Hui Chao Zhang Yan Fang Yuxin Liu Xi Chen Danyan Zhang Bolong Huang Yuliang Li | 2021 | National Science Review2021，8，8： | 2 |
| 4 | Ir^(0)/graphdiyne atomic interface for selective epoxidation显示文摘The development of catalysts that can selectively and efficiently promote the alkene epoxidation at ambient temperatures and pressures is an important promising path to renewable synthesis of various chemical products.Here we report a new type of zerovalent atom catalysts comprised of zerovalent Ir atoms highly dispersed and anchored on graphdiyne(Ir^(0)/GDY)wherein the Ir^(0)is stabilized by the incomplete charge transfer effect and the confined effect of GDY natural cavity.The Ir^(0)/GDY can selectively and efficiently produce styrene oxides(SO)by electro-oxidizing styrene(ST)in aqueous solutions at ambient temperatures and pressures with high conversion efficiency of∼100%,high SO selectivity of 85.5%,and high Faradaic efficiency(FE)of 55%.Experimental and density functional theory(DFT)calculation results show that the intrinsic activity and stability due to the incomplete charge transfer between Ir^(0)and GDY effectively promoted the electron exchange between the catalyst and reactant molecule,and realized the selective epoxidation of ST to SO.Studies of the reaction mechanism demonstrate that Ir^(0)/GDY proceeds a distinctive pathway for highly selective and active alkene-to-epoxide conversion from the traditional processes.This work presents a new example of constructing zerovalent metal atoms within the GDY matrix toward selective electrocatalytic epoxidation. | Zhiqiang Zheng Lu Qi Yaqi Gao Xiaoyu Luan Yurui Xue Feng He Yuliang Li | 2023 | National Science Review2023，10，8： | 1 |
| 5 | Multi-heterointerfaces for selective and efficient urea production显示文摘A major impediment to industrial urea synthesis is the lack of catalysts with high selectivity and activity,which inhibits the efficient industrial production of urea.Here,we report a new catalyst system suitable for the highly selective synthesis of industrial urea by in situ growth of graphdiyne on the surface of cobalt-nickel mixed oxides.Such a catalyst is a multi-heterojunction interfacial structure resulting in the obvious incomplete charge-transfer phenomenon between a graphdiyne and metal oxide interface and multiple intermolecular interactions.These intrinsic characteristics are the origin of the high performance of the catalyst.Studies on the me chanism reve al that the catalyst could effectively optimize the adsorption/desorption capacities of the intermediate and promote direct C-N coupling by significantly suppressing by-product reactions toward the formation of H_(2),CO,N_(2)and NH_(3).The catalyst can selectively synthesize urea directly from nitrite and carbon dioxide in water at room temperature and pressure,and exhibits a record-high Faradaic efficiency of 64.3%,nitrogen selectivity(N_(urea)-selectivity)of 86.0%,carbon selectivity(C_(urea)-selectivity)of ~100%,as well as urea yield rates of 913.2μg h^(-1)mgcat^(-1)and remarkable long-term stability. | Danyan Zhang Yurui Xue Xuchen Zheng Chao Zhang Yuliang Li | 2023 | National Science Review2023，10，2： | 1 |
| 6 | Controlled Growth Interface of Charge Transfer Salts of Nickel- 7,7,8,8-Tetracyanoquinodimethane on Surface of Graphdiyne显示文摘Here we report an in situ assembly growth method that controls the growth of NiTCNQ on the surface of graphdiyne(GDY).The catalytic system of donor–acceptor–donor(GDY/TCNQ/Ni)structure with multiple charge transfer(CT)was achieved by controlling the growth of NiTCNQ on the surface of GDY.Significantly,a controlled double layer interface of GDY/TCNQ/Ni was formed.This system implemented simultaneously the two elements we expected(1)an incomplete CT,and(2)the infinite distribution of active sites originating from highly asymmetric surface charge distribution.The high conductivity and typical semiconductor characteristics of the catalyst endows it with high catalytic activity.We found that an electrolytic cell consisting of the CT salt as a catalyst provided a 1.40 V ultra-small cell voltage up to 10 mA cm−2 and the outer GDY film effectively prevented the corrosion of the catalyst.Our study is the first to introduce CT complexes to a novel catalytic material platform for high selectivity of catalysts,and undoubtedly demonstrates the high selectivity,stability,and activity of such catalytic systems,which provides a new space for the development of novel conceptual catalysts. | Yuxin Liu Yang Gao Feng He Yurui Xue Yuliang Li | 2023 | CCS Chemistry2023，5，4： | 1 |
| 7 | Controlled Growth of Multidimensional Interface for High-Selectivity Ammonia Production显示文摘The efficient production of ammonia by reducing nitrates at room temperature and ambient pressure is a promising alternative to the Haber-Bosch process and can effectively overcome the attendant water pollution issues.Herein,a new idea has been realized for rational and selective construction of the sp-carbon-metal-carbon interface,comprised of electronic-donating triple bonds in graphdiyne and electron-withdrawing iron carbides,for a highly efficient nitrate reduction reaction.The as-prepared sp-carbon-metal-carbon interfacial structures greatly increase the charge transfer ability and electrical conductivity of the system.The proposed concept of incomplete charge transfer has demonstrated significantly high selectivity,activity,and stability in catalytic system.The catalyst exhibits high Faradaic efficiency of over>95%and a NH3 yield rate up to 205.5μmolNH_(3) cm^(-2) h^(-1) in dilute nitrate conditions without any contaminant. | Xuchen Zheng Yurui Xue Chao Zhang Yuliang Li | 2023 | CCS Chemistry2023，5，7： | 1 |
| 8 | Stimuli-responsive combination therapy of cisplatin and Nrf2 siRNA for improving antitumor treatment of osteosarcoma显示文摘Cisplatin is a widely applied therapeutics for the treatment of osteosarcoma.However,its clinical applications have been hindered due to low efficacy and bioavailability,and particularly frequent emergence of reactive oxygen species(ROS)-decrease induced drug resistance.The transcription factor NF-E2-related factor 2(Nrf2)is increased in cancer patients and induces poor outcome in osteosarcoma treatment,making it a novel target to improve the efficacy of chemotherapy.Herein,a hyaluronidase-responsive multi-layer liposome(HLCN)for co-delivery of cisplatin and Nrf2 siRNA(siNrf2)is developed.It is composed of Vpr52-96 modified liposome covered with hyaluronic acid(HA).HLCN selectively accumulates in osteosarcoma by targeting tumor-specific CD44,and can be degraded by endosomal hyaluronidase to generate cationic liposome,which promotes the endosomal escape of Vpr52-96,cisplatin and siNrf2.HLCN can effectively decrease Nrf2 level,promote ROS generation,activate itochondrial apoptotic pathway,and consequently enhance anticancer efficacy of cisplatin.Particularly,HLCN shows high cytotoxicity to osteosarcoma cells with an IC50 value of about 1µM,which is four-fold lower than liposomal cisplatin(IC504µM),indicating that Nrf2 silence can significantly improve cisplatin sensitivity in cancer cells.Importantly,HLCN can remarkably inhibit tumor growth in the xenograft osteosarcoma mice with minimal systemic adverse effects.Therefore,this novel stimuli-responsive combination therapy of cisplatin and siNrf2 provides a promising strategy for the treatment of osteosarcoma. | Ting-Ting Gu Chengjun Li Yurui Xu Lei Zhang Xue Shan Xinyu Huang Leilei Guo Kerong Chen Xiaojian Wang Haixiong Ge Xinghai Ning | 2020 | Nano Research2020，13，3： | 0 |
| 9 | Themed Issue on Graphdiyne显示文摘Graphdiyne(GDY)has characteristics of one-atom-thick two-dimensional layers comprising of sp and sp^(2)hybridized carbon atoms.The chemical and electronic structure gives GDY many unique and fascinating properties,such as rich chemical bonds,highly conjugated and super-largeπstructures,infinitely distributed pores and high inhomogeneity of charge distribution,etc. | Yurui Xue Zicheng Zuo Jin Zhang Yuliang Li | 2021 | Chemical Research in Chinese Universities2021，37，6： | 0 |
| 10 | Loading Nickel Atoms on GDY for Efficient CO_(2) Fixation and Conversion显示文摘Carbon dioxide(CO_(2))is an important and valuable C1 resource for the synthesis of numerous of value-added products. However, efficient fixation and conversion of CO_(2) into organic carbonates under mild conditions remain great challenges. Herein, graphdiyne(GDY)-based nickel atomic catalysts(Ni0/GDYs) were synthesized through a facile in-situ reduction method. Experimental results showed that the obtained Ni0/GDY had outstanding catalytic performances for converting CO_(2) into cyclic carbonates with a high reaction conversion(99%) and reaction selectivity(ca. 100%) at 80℃ and under 1 atm(1 atm=101325 Pa). Specially, the activation energy (Ea) value for the Ni0/GDY is 37.05 kJ/mol, lower than those of reported catalysts. The reaction mechanism was next carefully analyzed by using density functional theory(DFT) calculations. Such an excellent catalytic property could be mainly attributed to the high dispersion of active sites on the Ni0/GDY, and the unique incomplete charge transfer properties of GDY-based zero-valent metallic catalysts. | ZHENG Zhiqiang HE Feng XUE Yurui LI Yuliang | 2022 | Chemical Research in Chinese Universities2022，38，1： | 0 |
| 11 | Bismuth/Graphdiyne Heterostructure for Electrocatalytic Conversion of CO_(2) to Formate显示文摘Electrocatalytic CO_(2) reduction is great promising in alleviating the excessive CO_(2) emission and the conversion to valuable productions.Herein we report the in-situ controlled growth of Bismuth nanoflower/graphdiyne heterostructures(Bi/GDY)for efficient CO_(2) conversion toward formate.Based on GDY,the obtained electrocatalyst exhibits a partial current density of 19.2 mA/cm^(2) and high reaction selectivity towards formate with a high Faradic efficiency of 91.7%at−1.03 V vs.RHE,and an energy efficiency of 58.8%.The high formate yield rates could be maintained at around 300µ.mol/(cm^(2)·h)over a wide potential range.Detailed characterizations show that the unique interface structures between GDY and Bi can enhance the charge transfer ability,increase the number of active sites,and improve the long-term stability,and finally reach high-performance electrocatalytic conversion of CO_(2) to formate. | DU Yuncheng ZHENG Xuchen XUE Yurui LI Yuliang | 2022 | Chemical Research in Chinese Universities2022，38，6： | 0 |
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