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SENSORS AND ACTUATORS B-CHEMICAL · 2022 · IF 9.221

High-stable perovskite nanocrystal fluorescent probe-based aptasensor for ultrasensitive detection of peanut allergen Ara h1

Shuo Qi,Anqi Sun,Xiaoze Dong,Yuhan Sun,Minwei Qin,Ning Ding,Yin Zhang,Zhouping Wang

Food allergy is a serious immune allergy reaction, that has attracted public attention all over the world due to the increasing incidence. Ara h1, the most abundant allergenic protein in peanuts, has been identified as a biomarker of peanut allergen. Therefore, a sensitive, efficient method for Ara h1 detection is urgently needed to protect allergy sufferers. In this study, a simple and efficient fluorescent aptasensor was proposed for ultrasensitive and rapid detection of peanut allergen Ara h1. The aptamer against Ara h1 was conjugated onto the surface of high-stable perovskite nanocrystal (PNCs) to serve as the fluorescence-labeled recognition probe as well as the signal probe , while the magnetic nanoparticles Fe 3 O 4 (MNPs) were functionalized with the aptamer complementary DNA (cDNA) as the separation probe. The high-stable PNCs-labeled aptasensor [email protected] gives the combined merits of the extraordinary optical properties of PNCs, the efficient magnetic separation capability of MNPs as well as the high specificity of aptamers. The developed high-stable PNCs-labeled aptasensor exhibited excellent linearity (0.1–100 ng/mL), and low limit of detection (0.04 ng/mL). The aptasensor was successfully applied for the determination of Ara h1 in food samples, implying great potential in the field of allergen assay.

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ACS Applied Nano Materials · 2023 · IF 5.9

Antisolvent-Treated MAPbI3 and PbS Quantum Dots for High-Performance Broadband Photodetectors

Zeren He,Yan Yang,Jiaxin Liu,Junyu Li,Xingyu Lu,Jikuang Zou,Shuai Yang,Yousheng Zou

Nowadays, halide perovskites have drawn extensive attention as active layers in the field of photodetectors (PDs) attributed to their optoelectric properties. However, the numerous defects in the prepared films and the lack of response in the near-infrared (NIR) range due to the intrinsic band gap limitation severely restrict the performances and applications of perovskite photodetectors. With this in mind, we introduced diethyl ether as a counter-solvent to improve the quality of the peroxide films. After comparison with chlorobenzene (CB), toluene (ToL), and ethyl acetate (EA), the mechanism by which diethyl ether (DE) as an antisolvent improves the quality of the films was explored. MAPbI3 films and lead sulfide (PbS) quantum dots (QDs) were then combined to achieve a visible (VIS)–near-infrared response. The resultant PD, with the structure of ITO/NiOx/PbS QDs/MAPbI3/PC61BM/Ag, exhibits an ultrabroad response from 300 to 1100 nm and presents high detectivity reaching 5.6 × 1011 and 6.5 × 1010 Jones in the VIS and NIR regions, respectively. The fast response time in the microsecond range and the response bandwidth of 10 kHz (f–3 dB) are comparable or even superior to counterparts. In addition, this approach provides ideas for the development of high-performance broadband perovskite-based optoelectronic devices.

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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY · 2022 · IF 4.831

Bi3+ and Tb3+ Co-doped Cs2AgInCl6 Lead-free double perovskite nanocrystals for detection of temperature and copper ions

Ruixin Song,Sai Xu,You Li,Qun Zhang,Yuefeng Gao,Hongquan Yu,Yongze Cao,Xiangping Li,Shanpeng Zhang,Baojiu Chen

The content of Cu 2+ in lubricating oil and lubricant temperature are important indicators predicting mechanical failure. Therefore, developing a nontoxic fluorescence probe is necessary to detect Cu 2+ and temperature in lubricating oil. The lead-free inorganic double perovskite nanocrystals (NCs) Cs 2 AgInCl 6 are potential candidates. However, the low fluorescence intensity and the high excitation energy required of Cs 2 AgInCl 6 NCs limit their practical applications. In this study, Bi 3+ and Tb 3+ were successfully co-doped into Cs 2 AgInCl 6 NCs via the hot-injection method. The doping of Bi 3+ produces a broad emission originating from self-trapped excitons and reduces the excitation energy, allowing commercial LEDs as excitation sources. Tb 3+ ions doping offers characteristic emission peaks ( 5 D 0 - 7 F J ) of Tb 3+ ions and improves the fluorescence intensity of Cs 2 AgInCl 6 NCs. Furthermore, the Cs 2 AgInCl 6 : Bi 3+ /Tb 3+ NCs have been employed as optical thermometry, which provide a temperature calibration curve with the maximum absolute and relative sensitivities of 2.15% K −1 at 350 K and 2.25% K −1 at 303 K in the temperature range of 303–423 K, respectively. Finally, the nanocrystals have been applied to detect Cu 2+ in lubricating oil. The fluorescent probe shows a good detection sensitivity of 8.94 × 10 -4 nM −1 and a low detection limit of 14.3 nM in the range of 10–300 nM. This work not merely offers a novel way for improving the luminescence performances of double perovskite NCs Cs 2 AgInCl 6 , but broadens their potential for detection of Cu 2+ and temperature.

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Nature Photonics · 2022 ·Vol. 16 ·期 12 ·860-868 · IF 39.728

Extreme γ-ray radiation hardness and high scintillation yield in perovskite nanocrystals

Zaffalon Matteo L.,Cova Francesca,Liu Mingming,Cemmi Alessia,Di Sarcina Ilaria,Rossi Francesca,Carulli Francesco,Erroi Andrea,Rodà Carmelita,Perego Jacopo,Comotti Angiolina,Fasoli Mauro,Meinardi Francesco,Li Liang,Vedda Anna,Brovelli Sergio

Radiation detection is of utmost importance in fundamental scientific research, as well as medical diagnostics, homeland security, environmental monitoring and industrial control. Lead halide perovskites (LHPs) are attracting growing attention as high-atomic-number materials for next-generation scintillators and photoconductors for ionizing radiation detection. To unlock their full potential as reliable and cost-effective alternatives to conventional materials, it is necessary for LHPs to conjugate high scintillation yields with emission stability under high doses of ionizing radiation. To date, no definitive solution has been devised to optimize the scintillation efficiency and kinetics of LHPs and nothing is known of their radiation hardness for doses above a few kilograys, to the best of our knowledge. Here we demonstrate that CsPbBr 3 nanocrystals exhibit exceptional radiation hardness for γ-radiation doses as high as 1 MGy. Spectroscopic and radiometric experiments highlight that despite their defect tolerance, standard CsPbBr 3 nanocrystals suffer from electron trapping in dense surface defects that are eliminated by post-synthesis fluorination. This results in >500% enhancement in scintillation efficiency, which becomes comparable to commercial scintillators, and still retaining exceptional levels of radiation hardness. These results have important implications for the widespread use of LHPs in ultrastable and efficient radiation detectors.

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INORGANIC CHEMISTRY · 2022 · IF 5.436

Suppression of Thermal Quenching for CsPbX3 (X = Cl, Br, and I) Quantum Dots via the Hollow Structure of SrTiO3 and Light-Emitting Diode Applications

Wenli Song,Bing Zhang,Wenli Zhou,Jilin Zhang,Liping Yu,Shixun Lian

All-inorganic perovskite quantum dots (PQDs, CsPbX3, X = Cl, Br, and I) show outstanding application prospects in the field of photoelectric devices. In recent years, the development of PQDs has greatly improved their stability to water, oxygen, and light. However, thermal quenching of PQDs greatly limits their practical application. Herein, we embed PQDs into ATiO3 (A = Ca, Ba, and Sr) of three different mesoporous spherical structures to explore the effect on thermal quenching of PQDs. Because of the unique mesoporous hollow microsphere structure and low thermal conductivity of SrTiO3, it can effectively block the heat transfer and improve the thermal quenching of PQDs. The photoluminescence (PL) intensity of CsPbBr3@SrTiO3 composites is 72.6% of the initial intensity after heating to 120 °C. Moreover, the PL intensity of CsPbBr3@SrTiO3 composites remains about 80% of the initial value even when stored in air for 20 days or irradiated by 365 nm UV light for 48 h. A neutral white light-emitting diode is assembled by a blue chip, CsPbBr3@SrTiO3 composites, and red phosphor of K2SiF6:Mn4+, which has a color temperature of 5389 K and a color gamut covered 133% of National Television Standards Committee (NTSC).

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CERAMICS INTERNATIONAL · 2022 · IF 5.532

Achieve high-efficiency long afterglow luminescence control using CsPbI3 quantum dots

Ou Hai,Jian Li,Mengkang Pei,Qiang Ren,Xiulan Wu

The construction of visible full-spectrum tunable afterglow luminescence is of great significance for long afterglow materials. Here we developed a new composite material whose afterglow were continuously tunable from blue to red light, we prepared CsPbI 3 quantum dots (QDs) by thermal injection method and added passivators to obtain relatively more stable QDs materials, the SDS-CsPbI 3 QDs after passivation treatment was more than twice the photoluminescent (PL) intensity of the original QDs after 10 days, which has a positive effect on the large-scale production and application of all-inorganic perovskite QDs. By uniformly distributing CsPbI 3 QDs on the surface of Sr 2 MgSi 2 O 7 :Eu 2+ ,Dy 3+ (SMS) by Stöber method, a color-tunable long-persistence luminescent material CsPbI 3 /SMS@SiO 2 was prepared, and the tunable afterglow glows from 465 nm to 700 nm was realized by optical conversion. In addition, the PL intensity of the composite material under ultraviolet light is increased by more than 50%, and it can remain stable for a long time; its high temperature resistance is also improved to 140 °C; and the luminous intensity after 10 days remains at a high level. This research also provides new ideas and methods for the development of multicolor long afterglow materials.

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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY · 2023 ·Vol. 332 ·期 4 ·1237-1244 · IF 1.6

A novel superparamagnetic iron oxide nanoparticles-based SPECT/MRI dual-modality probe for tumor imaging

Xi Wenke,Zhang Ge,Xue Jingquan,Li Juan,Liu Yu,Wang Jianjun,Yang Wenjiang

Multimodal imaging has become a trend in the development of molecular imaging. For SPECT/MRI dual-modality imaging, we developed a SPECT/MRI dual-modality probe based on superparamagnetic iron oxide nanoparticles. RGDyk peptide and DTPA chelator were used to realize the functionalization of nanoparticles. Both SPECT imaging and T2-weighted MR imaging in vivo on 4T1 tumor-bearing mice showed targeting of the probe, demonstrating the potential of the SPECT/MRI dual-modality probe as a tool for tumor evaluation and diagnosis.

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ADVANCED FUNCTIONAL MATERIALS · 2022 ·Vol. 33 ·期 7 ·2212095 · IF 19.924

Enabling Efficient Blue-Emissive Circularly Polarized Luminescence by In Situ Crafting of Chiral Quasi-2D Perovskite Nanosheets within Polymer Nanofibers

Zhangchuan Wen,Rong Lu,Fan Gu,Kai Zheng,Lijie Zhang,Huile Jin,Yihuang Chen,Shun Wang,Shuang Pan

Chiral perovskite materials have intrigued enormous interests because of their appealing chiroptical properties and tailorable non-centrosymmetric structures. However, it remains challenging to realize high-efficiency blue emissive circularly polarized luminescence (CPL) of intrinsic chiral perovskite nanomaterials at room temperature. Herein, a robust and versatile electrospinning strategy is reported for in situ construction of chiral 2D and quasi-2D perovskite nanosheets (PNSs) protected in polymer hybrid nanofibers. It is found that quasi-2D chiral PNS/polymer possesses inherent chirality and enhanced CPL properties at room temperature compared to 2D counterparts. Notably, CPL emission color of chiral quasi-2D PNS/polymer can be tuned from deep blue to sky blue, and a high luminescence dissymmetry values up to −8.0 × 10 −3 can be achieved. Different perovskites, polymers, and nanofibrous structures are expanded to explore the universality of polymer protected PNSs. Significantly, compared to spin-coated film, the stabilities of quasi-2D PNS/polymer film are greatly improved due to the effective protection of polymer. The obtained PNS/polymer hybrid nanofiber films can be conveniently implemented for circularly polarized light emitting diode devices. This study may open up a new avenue for the scalable fabrication of chiral perovskite nanomaterials of interest and their applications in the CPL related fields.

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Nanoscale · 2022 ·Vol. 15 ·期 1 ·365-375 · IF 8.307

Self-assembling ferrimagnetic fluorescent micelles for bioimaging guided efficient magnetic hyperthermia therapy

Yonghong Song,Yueqiang Zhu,Kun Jiang,Xingyu Liu,Liang Dong,Dongdong Li,Sheng Chen,Hanye Xing,Xu Yan,Yang Lu,Xianzhu Yang,Junxia Wang,Yunjun Xu

Multifunctional magnet–fluorescent nanocomposites are widely applied in biomedical applications. Incorporating biocompatible quantum dots with highly ferrimagnetic magnetic nanoparticles into one nanoplatform for achieving efficient magnetic hyperthermia therapy (MHT) is very important. Herein, we reported an amphiphilic block copolymer with a flowable hydrophobic chain to encapsulate highly ferrimagnetic magnetic nanoparticles and ZnS/InP quantum dots via a facile self-assembly method. The obtained ferrimagnetic fluorescent micelle (FMFM) exhibited a uniform diameter of about 180 nm. In stark contrast, larger aggregation (400 nm in diameter) inevitably occurred using common poly(D,L-lactide) (PLA)-based amphiphilic block copolymer with a rigid hydrophobic chain, which was readily cleared by the reticuloendothelial system (RES). The flowable FMFM exhibited long-term colloidal stability within one month and desired fluorescent stability within 84 h. Benefiting from the high ferrimagnetism, the FMFM revealed excellent magnetic heating effect and magnetic resonance imaging capability. With accurate manipulation under an external magnetic field, FMFM realized in vitro enhanced fluorescence imaging sensitivity and accumulation efficiency at the tumor region, achieving in vitro and vivo improved MHT efficacy.

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ADVANCED FUNCTIONAL MATERIALS · 2023 ·Vol. 33 ·期 7 ·2210860 · IF 19

Magnetic-Activated Nanosystem with Liver-Specific CRISPR Nonviral Vector to Achieve Spatiotemporal Liver Genome Editing as Hepatitis B Therapeutics

Chenya Zhuo,Huiming Kong,Ke Yi,Chun-Wei Chi,Jiabing Zhang,Ran Chen,Haixia Wang,Caixia Wu,Yeh-Hsing Lao,Yu Tao,Mingqiang Li

Chronic hepatitis B infection remains incurable due to the stable presence of various forms of hepatitis B virus (HBV) genome, especially the HBV covalently closed circular DNA (cccDNA). The emergence of clustered regularly interspaced short palindromic repeat (CRISPR) technology provides a new opportunity to potentially cure the HBV infection. However, the efficiency and specificity remain unsatisfactory, especially for nonviral CRISPR/Cas9 delivery. To tackle these, a liver-specific CRISPR/Cas9 magnetic nanosystem FMNP pAG333/sgXPP is constructed based on fluorinated polyethylenimine-coated magnetic nanoparticles and liver-specific ApoE.HCR.hAAT promoter-driven Cas9-T2A-EGFP plasmid with dual sgRNAs. The elaborate system enables magnetic field-induced spatially specific distribution and hepatocyte-specific promoter-driven liver-specific gene editing. Moreover, this CRISPR/Cas9 magnetic nanosystem is designed to disrupt the two conserved sites in X opening reading frame and Pol opening reading frame of the HBV genome, thereby significantly inactivating the HBV genome without showing off-target effects. Treatment with FMNP pAG333/sgXPP for 7 days reduces serum HBsAg levels by 76% with a total editing efficiency of ≈20% in the two conserved sites. Collectively, this study demonstrates spatiotemporal liver genome editing as well as the feasibility of applying a nonviral CRISPR/Cas9 vector for HBV treatment, which may open up a new application for CRISPR therapeutics.

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INORGANIC CHEMISTRY · 2023 · IF 4.6

In Situ Growth of Cs3Bi2Br9 Quantum Dots on Bi-MOF Nanosheets via Cosharing Bismuth Atoms for CO2 Capture and Photocatalytic Reduction

Lan Ding,Yongping Ding,Fenghua Bai,Gonglai Chen,Shuwei Zhang,Xiaoxue Yang,Huiqin Li,Xiaojing Wang

Given the global warming caused by excess CO2 accumulation in the atmosphere, it is essential to reduce CO2 by capturing and converting it to chemical feedstock using solar energy. Herein, a novel Cs3Bi2Br9/bismuth-based metal–organic framework (Bi-MOF) composite was prepared via an in situ growth strategy of Cs3Bi2Br9 quantum dots (QDs) on the surface of Bi-MOF nanosheets through coshared bismuth atoms. The prepared Cs3Bi2Br9/Bi-MOF exhibits bifunctional merits for both the high capture and effective conversion of CO2, among which the optimized 3Cs3Bi2Br9/Bi-MOF sample shows a CO2–CO conversion yield as high as 572.24 μmol g–1 h–1 under the irradiation of a 300 W Xe lamp. In addition, the composite shows good stability after five recycles in humid air, and the CO2 photoreduction efficiency does not decrease significantly. The mechanistic investigation uncovers that the intimate atomic-level contact between Cs3Bi2Br9 and Bi-MOF via the coshared atoms not only improves the dispersion of Cs3Bi2Br9 QDs over Bi-MOF nanosheets but also accelerates interfacial charge transfer by forming a strong bonding linkage, which endows it with the best performance of CO2 photoreduction. Our new finding of bismuth-based metal–organic framework/lead-free halide perovskite by cosharing atoms opens a new avenue for a novel preparation strategy of the heterojunction with atomic-level contact and potential applications in capture and photocatalytic conversion of CO2.

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ADVANCED MATERIALS · 2023 ·Vol. 35 ·期 15 ·2209181 · IF 29.4

An Active Pixel-Matrix Electrocaloric Device for Targeted and Differential Thermal Management

Peijia Bai,Quan Zhang,Heng Cui,Yiwen Bo,Ding Zhang,Wen He,Yongsheng Chen,Rujun Ma

More than 55% of electronic failures are caused by damage from localized overheating. Up to now, there is still no efficient method for targeted temperature control against localized overheating. Although some existing thermal management devices handle this issue by full coverage cooling, it generates a lot of useless energy consumption. Here, a highly efficient pixel-matrix electrocaloric (EC) cooling device is reported, which can realize a targeted and differential thermal management. The modified poly(vinylidene fluoride-tertrifluoroethylene-chlorofluoroethylene) reaches a large adiabatic temperature change of 7.8 K and is more suitable for thermal transfer and electrostatic actuation at high frequencies. All active pixels in the EC cooling device exhibit a stable temperature span of 4.6 K and a heat flux of 62 mW cm -2 , which is more than twice that of the one-layer EC device. Each refrigeration pixel can be independently controlled and effectively cooled down the localized overheating site(s) in situ. The surface temperature of the simulated central processing unit decreases by 33.2 K at 120 s after applying this EC device. Such a compact, embeddable, low cost, and active solid-state pixel-matrix cooling device has great potential for localized overheating protection in microelectronics.

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