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Reversibly sensitizing-storing-releasing ^(1)O_(2) within a single platinum(Ⅱ)-acetylide-based metallacycle molecule via laser power modulation

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Science China Chemistry 2024年第2期67卷 604-611页

作者： Ruyi Zhou Wen Lv Bo Li Bo Yu Sudi Zhang Yucheng Zhou Shujuan Liu Qiang Zhao State Key laboratory of Organic electronics and Information Displays&Jiangsu Key laboratory for Biosensors Institute of Advanced Materials(IAM)&Institute of Flexible Electronics(Future Technology)Nanjing University of Posts and Telecommunications(NUPT)Nanjing210023China College of Electronic and Optical Engineering&College of Flexible electronics(future Technology) Jiangsu Province Engineering Research Center for Fabrication and Application of Special Optical Fiber Materials and DevicesNanjing University of Posts and Telecommunications(NUPT)Nanjing210023China

Tumor hypoxia severely limits the therapeutic efficacy of photodynamic therapy(PDT) for solid tumors,which is highly dependent on tissue oxygen *** this study,we developed a platinum(Ⅱ)-acetylide-based metallacycle compound bearing six 1,4-dimethylnaphthalenes(DMN) groups,and controlled the photodynamic and photothermal effects of the compound by adjusting the power of 730 nm laser to achieve reversible sensitization,storage and release of 1~O_(2) within a single *** compound formed nanoparticles by self-assembly and exhibited good water solubility and *** laser irradiation,the strong spin-orbit coupling of platinum atoms in the metallacycle facilitated 1~O_(2) *** produced 1~O_(2) was captured by the DMN carriers and transported into the hypoxic tumor,where 1~O_(2) release was triggered owing to the good photothermal effect of the extended conjugation of the *** therapy,the metallacycle serving as a photosensitizer,1~O_(2) carrier,and photothermal reagent,achieved the synergistic therapy of PDT/PTT,demonstrating the versatility of the *** study proposes a new strategy to develop phototherapy agents that are suitable for hypoxic tumors.

关键词： metallacycles singlet oxygen endoperoxides near-infrared absorption synergistic treatment

Materials design and preparation of ultrathin two-dimensional metal halide perovskites

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Nano Research 2024年第7期17卷 6231-6246页

作者： Xiaomin Zhang Sihan Zhao Junran Zhang Lin Wang School of Flexible electronics(future Technologies)and Institute of Advanced Materials Key Laboratory of Flexible ElectronicsJiangsu National Synergetic Innovation Center for Advanced MaterialsSchool of Physical and Mathematical SciencesNanjing Tech UniversityNanjing 211816China

Metal halide perovskites(MHPs)have emerged as highly promising candidates for the next generation of photonics and optoelectronic devices,owing to their prominent optical and excitonic properties,as well as the convenience of ***,ultrathin two-dimensional(2D)MHPs,which are generally prepared by exfoliation,solution growth,and chemical vapor deposition method,have attracted dramatically increasing attentions owing to their combined features of ultrathin 2D morphology and superior performance of *** the growing interest in ultrathin 2D MHPs,there is currently a lack of a comprehensive and systematic overview of the distinct advantages offered by each growth method for producing these *** review critically assesses the preliminary studies on the materials design and preparation of ultrathin ***,it explores heterostructures based on ultrathin MHPs and offers insights into the challenges and opportunities that lie ahead for this enticing class of 2D materials.

关键词： ultrathin perovskites material preparation exfoliation solution growth chemical vapor deposition

Solar Energy for Value-Added Chemical Production by LightPowered Microbial Factories

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CCS Chemistry 2024年第7期6卷 1776-1788页

作者： Haibo Wu Xilong Feng Liangjun Wang Cheng Chen Peng Wu Linpo Li Jinjie Xu Fan Qi Suoying Zhang Fengwei Huo Weina Zhang Key laboratory of Flexible electronics(KLOFE) Institute of Advanced Materials(IAM)School of Flexible Electronics(Future Technologies)Nanjing Tech University(NanjingTech)Nanjing 211816

The light-driven material-microorganism biohybrid system has the potential to transfer solar energy for chemical ***,few studies have reported the construction of biohybrid systems using light-responsive materials with nonmodel strains that have been widely used in practical industrial production for value-added chemicals,especially with regard to the mechanism of action of photogenerated charges in the cytoplasm,probably due to the complexity of their anabolic ***,a biohybrid system as a research mode was constructed by electrostatically self-assembling a highly efficient light-harvesting material of graphite-phase nitrided carbon(g-C_(3)N_(4))nanosheets with nonmodel strains(Phaffia rhodozyma)for synthesis of nutritional chemical *** biohybrid interface enabled efficient separation,transfer,and transport of photogenerated charges from g-C_(3)N_(4) into the interior of ***,which improved the substance metabolism and the energy metabolism of ***,photogenerated charges can significantly promote the accumulation of precursors along the astaxanthin anabolic pathway and enhance the cytoplasmic redox environment and ATP levels in the interior of ***,even under adverse conditions(such as enzyme inhibitors),thus increasing the yield of astaxanthin compared to the traditional culture of *** study not only provides new ideas for converting solar energy into value-added chemicals,but it also provides guidance for regulating microbial synthesis plants.

关键词： biohybrid system light-driven graphitephase nitrided carbon Phaffia rhodozyma astaxanthin

Coupling Au with BO_(x) matrix induced by Closo-boron cluster for electrochemical synthesis of ammonia

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Journal of Energy Chemistry 2024年第6期93卷 471-477,I0012页

作者： Wenjing Liu Nan Yang Yuao Wei Yingjie Yu Jie Chen Mo Wei Yuting Huang Xiaohan Li Linghai Zhang Faisal Saleem Weina Zhang Haibo Zhang Fengwei Huo Key laboratory of Flexible electronics(KLOFE)&Institute of Advanced Materials(IAM) School of Flexible Electronics(Future Technologies)Nanjing Tech UniversityNanjing 211816JiangsuChina College of Chemistry and Molecular Sciences Wuhan UniversityWuhan 430072HubeiChina

Au is considered as one of the most promising catalysts for nitrogen reduction reaction(NRR),however maximizing the activity utilization rate of Au and understanding the synergistic effects between Au and carriers pose ongoing ***,we systematically explore the synergistic catalytic effect of incorporating Au with boron clusters for accelerating NRR *** in-situ abinitio strategy is employed to construct B-doped Au nanoparticles(2-6 nm in diameter)loaded on BO_(x) substrates(AuBO_(x)),in which B not only modulates the surface electronic structure of Au but also forms strong coupling interactions to stabilize the *** electrochemical results show that Au-BO_(x) possesses excellent NRR activity(NH_(3) yield of 48.52μg h^(-1)mg_(cat)^(-1),Faraday efficiency of 56.18%),and exhibits high stability and reproducibility throughout the electrocatalytic NRR *** calculations reveal that the introduction of B induces the formation of both Au dangling bond and Au-B coupling *** considerably facilitates the hydrogenation of~*N_(2)^(-)~*NH_(3).The present work provides a new avenue for the preparation of metal-boron materials achieved by one-step reduction and doping process,utilizing boron clusters as reducing and stabilizing agents.

关键词： Boron clusters Nitrogen reduction reaction Au–B coupling

Deformable Catalytic Material Derived from Mechanical Flexibility for Hydrogen Evolution Reaction

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Nano-Micro Letters 2024年第2期16卷 287-311页

作者： Fengshun Wang Lingbin Xie Ning Sun Ting Zhi Mengyang Zhang Yang Liu Zhongzhong Luo Lanhua Yi Qiang Zhao Longlu Wang College of Electronic and Optical Engineering&College of Flexible electronics(future Technology) Nanjing University of Posts&Telecommunications(NJUPT)9 WenyuanNanjing 210023People’s Republic of China Key laboratory of Environmentally Friendly Chemistry and Applications of Ministry of Education School of ChemistryXiangtan UniversityXiangtan 411105People’s Republic of China State Key laboratory of Organic electronics and Information Displays&Jiangsu Key laboratory for Biosensors Institute of Advanced Materials(IAM)&Institute of Flexible Electronics(Future Technology)Nanjing University of Posts&Telecommunications9 WenyuanNanjing 210023People’s Republic of China

Deformable catalytic material with excellent flexible structure is a new type of catalyst that has been applied in various chemical reactions,especially electrocatalytic hydrogen evolution reaction(HER).In recent years,deformable catalysts for HER have made great progress and would become a research *** catalytic activities of deformable catalysts could be adjustable by the strain engineering and surface *** surface curvature of flexible catalytic materials is closely related to the electrocatalytic HER ***,firstly,we systematically summarized self-adaptive catalytic performance of deformable catalysts and various micro–nanostructures evolution in catalytic HER ***,a series of strategies to design highly active catalysts based on the mechanical flexibility of lowdimensional nanomaterials were *** but not least,we presented the challenges and prospects of the study of flexible and deformable micro–nanostructures of electrocatalysts,which would further deepen the understanding of catalytic mechanisms of deformable HER catalyst.

关键词： Deformable catalytic material Micro-nanostructures evolution Mechanical flexibility Hydrogen evolution reaction

Tailored multifunctional hydrazine derivatives for efficient printable hole-conductive-free mesoscopic perovskite solar cells via enhancing defect passivation

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Journal of Energy Chemistry 2024年第8期95卷 357-363,I0008页

作者： Minghao Xia Ziwei Zheng Yanjie Cheng Chaoyang Wang Zhaozhen Cui Guodong Zhang Jinwei Gonga Anyi Mei Hongwei Han Michael Grätzel Center for Mesoscopic Solar Cells Wuhan National Laboratory for OptoelectronicsKey Laboratory of Materials Chemistry for Energy Conversion and Storage of Ministry of EducationHuazhong University of Science and TechnologyWuhan 430074HubeiChina Key laboratory of Flexible electronics(KLoFE)&Institute of Advanced Materials(IAM) School of Flexible Electronics(Future Technologies)Nanjing Tech University(NanjingTech)Nanjing 211816JiangsuChina

The low-cost and easy large-scale fabrication advantages of printable mesoscopic perovskite solar cells(p-MPSCs)are overshadowed by their limited photovoltaic conversion efficiency(PCE).Here,we introduce the hydrazide derivative of 4-Hydroxybenzoylhydrazine(4-HBH)to improve the PCE of p-MPSCs by inducing enhanced defect *** carbonyl and hydrazine groups in hydrazide groups present strong interaction with *** hydroxyl group,as an electron donor group,increases the electron cloud density of the hydrazide group in 4-HBH under the conjugation of the benzene ring,and thus enhances its interaction with ***,the hydroxy group itself interacts with perovskite and passivates defects *** hydrazine agents can also reduce I2and suppress the loss of iodine in perovskite films,which inhibits the formation of iodine-related ***,p-MPSCs with 4-HBH achieve a high PCE of 19.21%,and present well improved stability.

关键词： Printable mesoscopic perovskite solar cells Multifunctional hydrazine derivatives Cooperative coordination Conjugation redox activity

2D all-organic perovskites refine flexible electronics

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Science China Materials 2024年第7期67卷 2365-2366页

作者： Wei Zhou Bing Chen College of Electronic and Optical Engineering and College of Flexible electronics(future Technology) Nanjing University of Posts and TelecommunicationsNanjing 210023China

Recent years have witnessed a paradigm shift with the advent of perovskites,a class of materials with a distinct CaTiO_(3)-type crystalline structure that show remarkable promise across a wide array of applications,including photovoltaics,photodetectors,lighting,lasers,and so *** them,the development of two-dimensional(2D)perovskites has garnered significant attention due to their tunable structures(mainly Dion-Jacobson and Ruddlesden-Popper structures)and enhanced stability in comparison with their 3D counterparts[1].Amidst the burgeoning research on perovskites,on the other side,all-organic perovskites stand out as a particularly intriguing subset[2].Unlike traditional perovskites that typically comprise all-inorganic(e.g.,CsPbBr_(3))or organic-inorganic hybrid components(e.g.,(PEA)_(2)PbI_(4)),all-organic perovskites are composed entirely of carbon-or nitrogen-based molecules.

关键词： perovskite inorganic entirely

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Brightening heavily doped upconversion nanoparticles by tuning characteristics of core-shell structures

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Journal of Rare Earths 2024年第5期42卷 947-954,I0005页

作者： Yangyang Niu Zhihao Bao Yuqin Gao Mengchao Guo Jingyao Liu Jinjun Shao Min Lu Ze Yuan Xiaoji Xie School of Flexible electronics(future Technologies)&Institute of Advanced Materials(IAM) Nanjing Tech UniversityNanjing211816China

Heavily doped upconversion nanoparticles(UCNPs)potentially have exceptional photon upconversion abilities that are promising for diverse applications,such as lasing and super-resolution ***,heavily doped UCNPs typically can only offer mediocre upconversion luminescence intensity,and there still lacks general guidelines for the design and synthesis of heavily doped ***,in order to boost the upconversion luminescence of heavily doped UCNPs,we studied the influence of characteristics of the core-shell structure on heavily doped UCNPs'upconversion *** find that some empirical guidelines derived from conventional UCNPs are not suitable for heavily doped *** NaYbF_(4):Tm@NaYF_(4) core-shell UCNPs with a high concentration of Yb_(3+)as a representative,our studies reveal that a rather thick inert NaYF4 shell is needed to protect the UCNPs from surface quenching,and the upconversion luminescence may undergo the cooperative sensitization process,which should be due to the highly concentrated Yb~(3+)*** addition,the upconversion luminescence of heavily doped NaYbF4:Tm UCNPs exhibits no obvious dependence on the type of inert ***,our results show that confining both Yb~(3+)and Tm~(3+)dopants in a thin layer(known as theδ-doping strategy)does not work well in the heavily doped ***,we propose a NaYbF_(4):Tm@NaYbF_(4)@NaYF_(4) core-shell-shell structure to enhance the luminescence of heavily doped UCNPs,by weakening the dissipation of excitation energy and strengthening the *** findings should be helpful to establish general design principles for developing the brightest possible UCNPs that can meet the requirements of various applications.

关键词： Luminescence Upconversion Nanomaterials Rare earths Lanthanide doping

An injectable,self-healable,and reusable PEDOT:PSS/PVA hydrogel patch electrode for epidermal electronics

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Nano Research 2024年第6期17卷 5479-5490页

作者： Yang Li Yuzhe Gu Sheng Qian Shuwen Zheng Yuncong Pang Lele Wang Baoguang Liu Shujuan Liu Qiang Zhao College of Electronic and Optical Engineering and College of Flexible electronics(future Technology) Nanjing University of Posts and Telecommunications(NJUPT)Nanjing 210023China State Key laboratory of Organic electronics and Information Displays and Jiangsu Key laboratory for Biosensors Institute of Advanced Materials(IAM)Nanjing University of Posts and Telecommunications(NJUPT)Nanjing 210023China

Injectability empowers conductive hydrogels to transcend traditional limitations,unlocking a realm of possibilities for innovative medical,wearable,and therapeutic applications that can significantly enhance patient care and quality of ***,we report an injectable,self-healable,and reusable hydrogel obtained by mixing the concentrated poly(3,4-ethylenedioxythiophene)doped with polystyrene sulfonate(PEDOT:PSS)suspension(~2 wt.%solid content),polyvinyl alcohol(PVA),and *** the presence of reversible borax/hydroxyl bonds and multiple hydrogen bonds,this PEDOT:PSS/PVA hydrogel exhibits notable shear-thinning behavior and self-healing capabilities,enabling it to be injected as a gel fiber from a ***-prepared injectable hydrogel also demonstrates an ultra-low modulus(~2.5 MPa),reduced on-skin impedance(~45%of commercial electrodes),and high signal-to-noise ratio(SNR)(~15-22 dB)in recording of electrocardiography(ECG),electromyography(EMG),and electroencephalogram(EEG)***,the injectable hydrogels can be remolded and reinjected as the reusable electrodes,maintaining nearly identical electrophysiological recording capabilities and brain-computer interface(BCI)performance compared to commercial wet *** their straightforward fabrication,excellent material properties and electronic performance,ease of cleaning,and remarkable reusability,our injectable PEDOT:PSS/PVA hydrogels hold promise for advancements in BCI based electronics and wearable bioelectronics.

关键词： epidermal hydrogel electrodes reusability injectability self-healing electrophysiological recording brain-computer interface