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Coreactant-Free and Direct Electrochemiluminescence from Dual-Stabilizer-Capped InP/ZnS Nanocrystals: A New Route Involving n-Type Luminophore

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ANALYTICAL CHEMISTRY 2022年第2期94卷 1350-1356页

作者： Fu, Li Gao, xuwen Dong, Shuangtian jia, Jingna Xu, Yuqi Wang, Dongyang Zou, Guizheng Shandong Univ Sch Chem & Chem Engn Jinan 250100 Peoples R China

Electrochemiluminescence (ECL) is conventionally generated in either an annihilation or a coreactant route, and the overwhelming majority of ECL research is conducted in the coreactant route via oxidizing or reducing the coexisting coreactant and luminophore. The coreacant-free ECL generated via merely oxidizing the luminophore would break through the ceiling of coreactant ECL via excluding the detrimental effects of exogenous coreactant and dissolved oxygen. Herein, by exploiting the rich-electron nature of n-type nanocrystals (NCs), coreacant-free ECL is achieved via merely oxidizing 3-mercaptopropionic acid (MPA) and mercaptosuccinic acid (MSA) capped InP/ZnS NCs, i.e., InP/ZnSMPA-MSA. The electron-rich InP/ZnSMPA-MSA can be electrochemically injected with holes via two oxidative processes at around +0.75 and +1.37 V (vs Ag/AgCl), respectively, and the exogenous hole can directly combine the conduction band (CB) electron of InP/ZnSMPA-MSA, resulting in two coreactant-free ECL processes without employing any exogenous coreactant. The deprotonation process for the carboxyl group of the capping agents can provide a negatively charged surface to InP/ZnSMPA-MSA and enhance the coreactant-free ECL. The hole-injecting process at +1.37 is much stronger than that at +0.75 V and eventually enables an similar to 2000-fold enhanced ECL at +1.37 V than that at +0.75 V. The ECL at +1.37 V can be utilized for coreactant-free ECL immunoassay with prostate-specific antigen (PSA) as analyte, which exhibits an acceptable linear response from 5 ***(-1) to 1 ***(-1) with a limit of detection of 0.3 ***(-1). The coreactant-free ECL route would provide an alternative to both annihilation and coreactant routes, simplify the ECL assay procedure and deepening the ECL mechanism investigations.

关键词： Electrochemiluminescence Prostate-specific antigen

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Ternary-Host and Heterojunction Enabled Eye-Visible Elastic Mechanoluminescence from (Ca0.5Sr0.5)ZnOS/xZnS/Mn2+

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JOURNAL OF PHYSICAL CHEMISTRY C 2022年第3期126卷 1523-1530页

作者： jia, Jingna Fu, Li Gao, xuwen Dong, Shuangtian Xu, Yuqi Wang, Dongyang Zou, Guizheng Shandong Univ Sch Chem & Chem Engn Jinan 250100 Peoples R China

Mechanoluminescence (ML) is one kind of mechanical-tooptical energy conversion, and a strategy toward achieving bright elastic ML emission is strongly anticipated for ML application. Herein, a ternary-host strategy is proposed for synthesizing heterojunction ML materials with eyevisible elastic ML under an ultralow pressure of 2 N, in which ZnS, CaCO3, and SrCO3 are employed as precursors to prepare the ternary-host (Ca0.5Sr0.5)ZnOS/xZnS. Upon partially substituting the precursor ZnS with MnCO3, the Mn2+ activator could introduce luminescent centers and carrier traps into the ternary-host (Ca0.3Sr0.5)ZnOS/xZnS and enable achieving a series of (Ca0.5Sr0.5)ZnOS/xZnS/Mn2+ phosphors with bright and pressure-sensitive elastic ML. The (Ca0.5Sr0.5)ZnOS/xZnS/Mn2+ phosphors not only exhibit eyevisible red ML under ambient conditions without any preirradiation but can also display a linearly enhanced ML intensity along with the enlarged external force at a 2 N interval as well as regeneratable ML upon repetitively applying an external force 20 times. The maximum emission wavelength of ML can be conveniently modulated from 623 to 658 nm by adjusting the ZnS content of (Ca0.5Sr0.5)ZnOS/xZnS/Mn2+ phosphors.

关键词： Phosphors Transition metals Elastic materials Precursors Materials

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A Heintze-Karcher-Type Inequality for Hypersurfaces with Capillary Boundary

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JOURNAL OF GEOMETRIC ANALYSIS 2023年第6期33卷 177-177页

作者： jia, Xiaohan Xia, Chao Zhang, xuwen Xiamen Univ Sch Math Sci Xiamen 361005 Peoples R China

In this paper, we establish a Heintze-Karcher-type inequality for hypersurfaces with capillary boundary of contact angle theta is an element of(0, pi\2] in the half-space or a half ball, by using solution to a mixed boundary value problem in Reilly type formula. Consequently, we give a new proof of Alexandrov-type theorem for embedded capillary constant mean curvature hypersurfaces with contact angle theta is an element of(0, pi\2] in the half-space or a half ball.

关键词： Capillary hypersurface Mixed boundary value problem Reilly's formula Heintze-Karcher inequality Alexandrov's theorem

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Glow and Flash Adjustable Chemiluminescence with Tunable Waveband from the Same CuInS2@ZnS Nanocrystal Luminophore

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ANALYTICAL CHEMISTRY 2022年第18期94卷 6902-6908页

作者： Dong, Shuangtian Wang, Dongyang Gao, xuwen Fu, Li jia, Jingna Xu, Yuqi Zhang, Bin Zou, Guizheng Shandong Univ Sch Chem & Chem Engn Jinan 250100 Peoples R China

All commercial chemiluminescence (CL) assays are conducted with either glow or flash CL of eye-visible waveband from chemical luminophores. Herein, glow and flash, as well as waveband adjustable CL from the same nanoparticle luminophore of thiol-capped CuInS2@ZnS nanocrystals (CIS@ZnS-Thiol), are proposed via extensively exploiting the differed redox nature of CL triggering reagents. Taking thiosalicylic acid (TSA) as the model thiol-capping agent, the electron-injection-initiated charge transfer between CIS@ZnS-TSA and reductant can bring out efficient glow CL while the hole-injection-initiated charge transfer between CIS@ZnS-TSA and oxidant can give off obvious flash CL under optimum conditions. The maximum emission wavelength for CL of CIS@ZnS-TSA is adjustable from 730 nm to 823 nm via employing different triggering agents. Promisingly, the coexistent reductant of N2H4 center dot H2O and oxidant of H2O2 can be employed as dual triggering reagents to trigger eye-visible and highly efficient flash CL from CIS@ZnS-TSA. The maximum emission intensity for flash CL of CIS@ZnS-TSA/N2H4-H2O2 is 101-fold greater than the glow CL of CIS@ZnS-TSA/N2H4 and 22-fold greater than the flash CL of CIS@ZnS-TSA/H2O2, respectively. The flash CL from CIS@ZnS-TSA/N2H4-H2O2 is qualified for highly sensitive and selective CL immunoassay in a commercialized typical procedure with the entire operating process manually terminated within 35 min.

关键词： Glow Luminophore Chemiluminescence Flash

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Low-Triggering-Potential Electrochemiluminescence from Surface-Confined CuInS2@ZnS Nanocrystals and their Biosensing Applications

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ANALYTICAL CHEMISTRY 2021年第36期93卷 12250-12256页

作者： Dong, Shuangtian Gao, xuwen Fu, Li jia, Jingna Zou, Guizheng Shandong Univ Sch Chem & Chem Engn Jinan 250100 Peoples R China

Electrochemiluminescence (ECL) of low triggering potential is strongly anticipated for ECL assays with less inherent electrochemical interference and improved long-term stability of the working electrode. Herein, effects of the thiol capping agents and the states of luminophores, i.e., the thiol-capped CuInS2@ZnS nanocrystals (CuInS2@ZnS-Thiol), on the ECL triggering potential of CuInS2@ZnS-Thiol/N2H4 center dot H2O were explored on the Au working electrode. The thiol capping agent of glutathione (GSH) not only enabled CuInS2@ZnS-Thiol/N2H4 center dot H2O with the stronger oxidative-reduction ECL than other thiol capping agents but also demonstrated the largest shift for the ECL triggering potential of CuInS2@ZnS-Thiol/N2H4 center dot H2O upon changing the luminophores from the monodispersed state to the surface-confined state. CuInS2@ZnS-GSH/N2H4 center dot H2O exhibited an efficient oxidative-reduction ECL around 0.78 V (vs Ag/AgCl) with CuInS2@ZnS-GSH of the monodispersed state. Upon employing CuInS2@ZnS-GSH as the ECL tag and immobilizing them onto the Au working electrode, the oxidative-reduction ECL of CuInS2@ZnS-GSH/N2H4 center dot H2O was lowered to 0.32 V (vs Ag/AgCl), which was about 0.88 V lower than that of traditional Ru(bpy)(3)(2+)/TPrA (typically similar to 1.2 V, vs Ag/AgCl). The ECL of the CuInS2@ZnS-GSH/N2H4 center dot H2O system with the luminophore of both monodispersed and surface-confined states was spectrally identical to each other, indicating that this surface-confining strategy exhibited negligible effect on the excited state for the ECL of CuInS2@ZnS-GSH. A surface-confined ECL sensor around 0.32 V was fabricated with CuInS2@ZnS-GSH as a luminophore, which could sensitively and selectively determine the K-RAS gene from 1 to 500 pM with a limit of detection at 0.5 pmol L-1 (S/N = 3).

关键词： Electrochemiluminescence Biosensor

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Alkaline-Earth-Metal-Ions Blending Enhanced Self-Activated and Bi³⁺-Activated Mechanoluminescence from Ca1-xBaxZnOS

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ADVANCED FUNCTIONAL MATERIALS 2022年第46期32卷

作者： jia, Jingna Gao, xuwen Zou, Guizheng Shandong Univ Sch Chem & Chem Engn Jinan 250100 Peoples R China

The self-activated mechanoluminescence (ML) of oxysulfides MZnOS (M = Ca, Sr, Ba) is very weak, and bright ML from these hosts is usually achieved with activator-doping strategy. Herein, a promising alkaline-earth-metal-ion blending strategy, instead of activator doping, is proposed to achieve intense and self-activated ML from MZnOS. Upon partially substituting the Ca2+ of CaZnOS with Ba2+ and vice versa, intense and eye-visible ML is achieved via exerting a small mechanical stimulus of 2 N onto the obtained Ca1-xBaxZnOS (0 x < 1). The luminescence center for ML of Ca1-xBaxZnOS is intrinsic oxygen vacancy, so that Ca1-xBaxZnOS can give off efficient and self-activated ML. Under optimum conditions, the maximum ML emission of Ca0.84Ba0.16ZnOS is about 50-folds and 170-folds to that of CaZnOS and BaZnOS, respectively. Promisingly, Bi3+ can be incorporated into the lattice of Ca1-xBaxZnOS, transferring ML center from the oxygen defects of Ca1-xBaxZnOS to the activator of Ca0.96-xBaxZnOS:Bi-0.04, and eventually enable further enhanced ML by about twofolds. This alkaline-earth-metal-ion blending strategy can also enhance Bi3+-activated ML from M0.96ZnOS:Bi-0.04, the maximum emission for ML of Ca0.80Ba0.16ZnOS:Bi-0.04 is 36-folds and 38 folds to that of Ca0.96ZnOS:Bi-0.04 and Ba0.96ZnOS:Bi-0.04, respectively. This work opens an avenue to develop new ML hosts and luminophores with efficient emission.

关键词： alkaline-earth-metal-ions blendings Ca Ba1-x xZnOS Mechanoluminescence self-activated

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Characterization of thermal neutron distribution of an Am-Be neutron source setup by CdZnTe detector

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APPLIED RADIATION AND ISOTOPES 2023年 196卷 110778页

作者： Liang, xuwen Zhao, Dong jia, Wenbao Hei, Daqian Cheng, Can Nanjing Univ Aeronaut & Astronaut Dept Nucl Sci & Technol Nanjing Peoples R China Jiangsu Higher Educ Inst Collaborat Innovat Ctr Radiat Med Suzhou 215000 Peoples R China Lanzhou Univ Sch Nucl Sci & Technol Lanzhou 730000 Peoples R China Nanjing Univ Aeronaut & Astronaut Coll Astronaut Nanjing 211106 Peoples R China

Owing to the developments in prompt gamma neutron activation analysis (PGNAA) and prompt gamma ray activation imaging (PGAI), it is necessary to develop an online thermal neutron distribution measurement method. The CdZnTe detector is considered as an alternative thermal neutron detector because of its high thermal neutron capture cross section. In this study, the thermal neutron field of an 241Am-Be neutron source was determined by CdZnTe detector. The intrinsic neutron detection efficiency of CdZnTe detector was calcu-lated by using indium foil activation, and the value was 3.65%. Then the characteristics of neutron source were conducted with the calibrated CdZnTe detector. The thermal neutron fluxes in front of beam port were measured at several distances ranging from 0 cm up to 28 cm. Thermal neutron field at distances of 1 cm and 5 cm were also measured. The experimental data were then compared with Monte Carlo simulation. The results demon-strated that the simulated data agree well with experimental measurements.

关键词： CdZnTe detector Monte Carlo simulation Am -Be neutron source Activation method Thermal neutron flux

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WILLMORE-TYPE INEQUALITY IN UNBOUNDED CONVEX SETS

arXiv

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arXiv 2024年

作者： jia, Xiaohan Wang, Guofang Xia, Chao Zhang, xuwen School of Mathematics Southeast University Nanjing211189 China Mathematisches Institut Universität Freiburg Ernst-Zermelo-Str.1 Freiburg79104 Germany School of Mathematical Sciences Xiamen University Xiamen361005 China

In this paper we prove the following Willmore-type inequality: On an unbounded closed convex set K ⊂ Rn+1 (n ≥ 2), for any embedded hypersurface Σ ⊂ K with boundary ∂Σ ⊂ ∂K satisfying a certain contact angle condition, there holds n +11∫Σ |H|n dA ≥ AVR(K)|Bn+1|. Moreover, equality holds if and only if Σ a part of a sphere and K \ Ω is a part of the solid cone determined by Σ. Here Ω is the bounded domain enclosed by Σ and ∂K, H is the normalized mean curvature of Σ, and AVR(K) is the asymptotic volume ratio of K. We also prove an anisotropic version of this Willmore-type inequality. As a special case, we obtain a Willmore-type inequality for anisotropic capillary hypersurfaces in a *** Codes 53C42, 53C20 Copyright © 2024, The Authors. All rights reserved.

关键词： Anisotropy

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Surface-Engineering Enhanced Charge Injection and Recombination of Silver Nanoclusters in an Aqueous Medium

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JOURNAL OF PHYSICAL CHEMISTRY C 2021年第40期125卷 22078-22083页

作者： Gao, xuwen Dong, Shuangtian Fu, Li Xu, Yuqi jia, Jingna Zou, Guizheng Shandong Univ Sch Chem & Chem Engn Jinan 250100 Peoples R China

An effective way to enhance the charge injection and the radiative recombination within atomically precise nanoclusters (NCs) is proposed with Ag-29(BDT)(12) (BDT = 1,3-benzenedithiol) and Ag-29(BDT)(12)(TPP)(4) (TPP = triphenylphosphine) as models. Surface-engineering Ag-29(BDT)(12) with phosphine ligands can passivate the four naked Ag atom sites on the surface of Ag-29(BDT)(12) and circumvent the geometric packing limitation induced by the wide footprint of BDT, which endows Ag-29(BDT)(12)(TPP)(4) with enhanced electrochemical redox for improved charge injection as well as boosted photoluminescence (PL) and electrochemiluminescence (ECL) for enhanced radiative charge recombination. The surface-engineering process demonstrates a negligible effect on the charge-injection potentials as well as the excited state emission for PL and ECL. Ag-29(BDT)(12) and Ag-29(BDT)(12)(TPP)(4) can be injected with holes and electrons via similar electrochemical redox processes;both annihilation ECL and co-reactant ECL of Ag-29(BDT)(12) and Ag-29(BDT)(12)(TPP)(4) match well with their valence (VB) hole/conduction (CB) electron injection-related oxidative/reductive processes and are of similar wavebands with a maximum emission wavelength around 795 nm.

关键词： Elements Redox reactions Quantum mechanics Charge recombination Recombination

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HEINTZE-KARCHER INEQUALITY FOR ANISOTROPIC FREE BOUNDARY HYPERSURFACES IN CONVEX DOMAINS

arXiv

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arXiv 2023年

作者： jia, Xiaohan Wang, Guofang Xia, Chao Zhang, xuwen School of Mathematical Sciences Xiamen University Xiamen361005 China Mathematisches Institut Universität Freiburg Ernst-Zermelo-Str.1 Freiburg79104 Germany Institut Für Mathematik Goethe-Universität Robert-Mayer-Str.10 Frankfurt60325 Germany

In this paper, we prove an optimal Heintze-Karcher-type inequality for anisotropic free boundary hypersurfaces in general convex domains. The equality is achieved for anisotropic free boundary Wulff shapes in a convex cone. As applications, we prove various Alexandrov-type *** Codes 53C45, 53A10, 53C42 Copyright © 2023, The Authors. All rights reserved.

关键词： Anisotropy

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