CRYSTENGCOMM
·
2022
·Vol. 24
·期 17
·3230-3238
·
IF 3.756
Jingbo Huang,Liang Ji,Xiao Li,Xingqiao Wu,Ningkang Qian,Junjie Li,Yucong Yan,Deren Yang,Hui Zhang
Pd-based nanocatalysts are critical to the commercialization of direct ethanol fuel cells (DEFCs); however, the synthesis of Pd-based binary alloy nanocrystals with well-defined branches is still a great challenge. Here we report a facile seed-mediated approach for the synthesis of PdSn alloy octopods with precisely controlled branches and tunable compositions through the Stranski–Krastanov growth mode. The PdSn octopod-like catalysts exhibited prominently enhanced catalytic activity and stability towards the ethanol oxidation reaction (EOR) with respect to commercial Pd/C in alkaline solution. Specifically, Pd72Sn28 octopods exhibited the highest mass and specific activities (2701 mA mg−1 and 11.27 mA cm−2), which were 2.1 and 6.7 times higher than those of commercial Pd/C, respectively. Density functional theory (DFT) calculations reveal that the lowest d-band center of the (100) surface of Pd72Sn28 weakens the adsorption of the acetate-evolution key intermediate *CH3CO, leading to the best catalytic activity towards the EOR.
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Advanced Optical Materials
·
2022
·Vol. 10
·期 9
·2102806
·
IF 10.05
Liang-Jun Pan,Jia-Wei Tu,Ling-Ling Yang,Zhi-Quan Tian,Zhi-Ling Zhang
Ag 2 S quantum dots (QDs) with high photoluminescence quantum yield (PLQY) in the second near-infrared (NIR-II, 1000–1700 nm) window are urgently pursued. Halide atoms (especially chloride) have been studied as inorganic capping ligands on improving the PLQY of Cd-, Pb-based chalcogenide QDs; however, it remains a challenge to well replace the organic ligand with chloride ligand from silver chalcogenide QDs. Herein, a novel strategy to prepare Ag 2 S QDs with significant photoluminescence (PL) enhancement via chloride-mediated growth and passivation is demonstrated. The oleylamine and oleate ligands on the surface of silver-rich Ag 2 S QDs are readily replaced by chloride ligands due to the smaller size and higher binding affinity with Ag + . Upon partial ligand exchange and chloride passivation, the surface trap states in Ag 2 S QDs are reduced through a decrease of unsaturated surface Ag atoms. Therefore, Ag 2 S QDs with approximately 300-fold enhancement of PL intensity, and a PLQY of 47.6% at 1220 nm emission, and a lifetime of 256 ns are obtained because the nonradiative recombination is inhibited. This work reveals that the passivation of Ag 2 S QDs with chloride ligands is fully feasible, providing new insights into improving the PLQY of silver chalcogenide QDs.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Youli Xu,Shuling Shen,Long Li,Shuning Xiao,Jing Li,Zhihong Tang,Junhe Yang
Ag 2 S-ZnS (AZ) heterostructures with tunable aspect ratio (AR) and band structure were successfully synthesized by site-selective doping of metal ions. TEM and XPS results showed that by doping Cu, Mn and Cd ions in AZ heterostructures (Cu: AZ, Mn: AZ and Cd: AZ), respectively, the morphology of AZ heterostructures changed from tadpole-shape (Cu: AZ with AR of 1.2) to matchstick-shape (Cd: AZ with AR of 3.9) due to the selective doping of Cu ions in Ag 2 S head and Cd ions in ZnS tail as well as the doping of Mn ions both in Ag 2 S head and ZnS tail (Mn: AZ with AR of 2.7). All the UV-Vis spectra of doped AZ showed Urbach tail absorption, suggesting the existence of midgap-states created by metal ion dopants , which was confirmed by PL results. Cd: AZ with the largest AR values and Cd-doping induced midgap states showed the highest photocatalytic H 2 -production rate of 1443.55 μmol h −1 g −1 . The catalytic activity of the Cd: AZ can be ascribed to the synergistic effect of midgap states and aspect ratio-dependent charge transfer, which all originate from the site-selective doping of metal ions. This investigation demonstrates a facile way to manipulate the charge carrier dynamics of semiconductor heterostructures by synergistic effects through simultaneously tuning and optimizing the electronic and morphological structures.
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JOURNAL OF NANOBIOTECHNOLOGY
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2022
·Vol. 20
·期 1
·1-22
·
IF 9.429
Li Hanrui,Cai Xiaoxia,Yi Tong,Zeng Yun,Ma Jingwen,Li Lei,Pang Liaojun,Li Na,Hu Hao,Zhan Yonghua
Background Postoperative chemotherapy for gastric cancer often causes multidrug resistance (MDR), which has serious consequences for therapeutic effects. Individualized treatment based on accurate monitoring of MDR will greatly improve patient survival.Results In this article, a self-enhanced Mn3O4 nanoplatform (MPG NPs) was established, which can react with glutathione to produce Mn2+ to enhance T1-weighted magnetic resonance imaging (MRI) and mediate in vivo real-time MDR monitoring. In vitro MRI results showed that MRI signals could be enhanced in the presence of hydrogen peroxide and glutathione and at acidic pH. In vivo MRI results indicated that MPG NPs could specifically target MDR cells, thereby realizing real-time monitoring of MDR in gastric cancer. Furthermore, MPG NPs have good chemodynamic activity, which can convert the endogenous hydrogen peroxide of tumor cells into highly toxic hydroxyl radical through Fenton-like reaction at acidic pH to play the role of chemodynamic therapy. In addition, Mn3O4 can significantly enhance the chemodynamic therapy effect because of its good photothermal conversion effect. Furthermore, in situ photothermal/chemodynamic synergistic therapy obtained remarkable results, the tumors of the mice in the synergistic therapy group gradually became smaller or even disappeared.Conclusion sMPG NPs have good biocompatibility, providing a good nanoplatform for real-time monitoring and precise diagnosis and treatment of MDR in gastric cancer.Graphical Abstract
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Jing Ding,Yufeng Zhou,Ziyao He,Qingyun He,Xiaojuan Liang,Wei Xia,Weidong Xiang
All-inorganic perovskites have been considered next-generation color converters in the backlit due to their shining optical properties. However, structural instability severely limits their pragmatic applications. Here, CsPbBr 3 /Cs 4 PbBr 6 microcrystals (MCs) were successfully embedded in polydimethylsiloxane (PDMS) films by a facile two-step method. As-prepared PDMS films containing CsPbBr 3 /Cs 4 PbBr 6 MCs (CsPbBr 3 /Cs 4 PbBr 6 @PDMS) obtain high brightness and excellent stability. Meaningfully, the PDMS films not only serve as a double protective matrix that can be used to improve the stability of CsPbBr 3 /Cs 4 PbBr 6 MCs, but also a flexible substrate with high transparency that allows the CsPbBr 3 /Cs 4 PbBr 6 @PDMS films to be used as color conversion materials for backlit displays. To our surprise, when PDMS is coated with CsPbBr 3 /Cs 4 PbBr 6 MCs, the water, thermal and photostability are greatly improved, while the photoluminescence intensity only lost by 10%. Furthermore, by mixing CsPbBr 3 /Cs 4 PbBr 6 MCs with K 2 SiF 6 :Mn 4+ phosphors in PDMS, a monolithic film with high performance was obtained. Its color gamut can reach 127% of the NTSC 1953 standard and 95% of the REC. 2020 standard, exhibiting the bright prospects in the backlit display field.
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Journal of Materials Chemistry C
·
2022
·Vol. 10
·期 19
·7552-7557
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IF 8.067
Haiyan Zhao,Tianyu Lin,Shuchen Shi,Wenhao Bai,Tongtong Xuan,Tianliang Zhou,Rong-Jun Xie
Luminescent materials have been widely used in the field of information security. However, single-mode anticounterfeiting technology with the aid of UV light excitation to generate visible-light emission is rough and easily decrypted. Herein, we build a novel information encryption and decryption technology based on the reversible ON/OFF luminescence of perovskite nanocrystals (NCs) caused by the phase transformation from luminescence-free Cs4PbX6 (X = Cl, Br, I) to visible-light-emitting CsPbX3 NCs. This phase transformation is easily realized by just controlling the water content, where the Cs4PbBr6 NCs can be converted to green-emitting CsPbBr3 NCs under water vapor treatments, and the latter is quickly changed back to Cs4PbBr6 NCs by vacuum drying. The water-induced photoluminescence switch is reproducible, stable, and reliable for information encryption and decryption, as demonstrated by inkjet printing patterned films on a glass substrate using the security ink of Cs4PbBr6 NCs in cyclohexane solution. Furthermore, each pixel in the patterned film containing confidential information is quite unique in microscopic morphology, enabling multimode anti-counterfeiting if combined with artificial intelligence.
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Laser & Photonics Reviews
·
2022
·Vol. 16
·期 7
·2100736
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IF 10.947
Baiqian Wang,Jiali Peng,Xin Yang,Wensi Cai,Hongbin Xiao,Shuangyi Zhao,Qianqian Lin,Zhigang Zang
Metal halide perovskite-based high-performance X-ray scintillator is considered as one of the most favorable candidates applied in the fields of medicine, industry, and science. However, the current X-ray scilltillators based on perovskites still suffer from the issue of poor stability, which impedes their further wide applications. Herein, a template assembled method to prepare large-size, flexible, and stable CsPbBr 3 @Polymethyl methacrylate composite films in ambient conditions is developed and their detection performance is studied. The composite films can maintain 94% and 81% of the initial PL intensity after 2000 cycles bending and storing in water over 2520 h, respectively. In addition, the prepared scintillators exhibit not only a low detection limit of 40.1 nGy air s −1 and a high spatial resolution of 8.0 lp mm −1 , but also an excellent tolerance against radiation (108 h). Thus, this simple but yet effective method would not doubt pave the way for further development of scintillators and might be well applicable to other metal halides.
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Advanced Optical Materials
·
2022
·Vol. 10
·期 11
·2200189
·
IF 10.05
Shixu Yang,Chenghao Bi,Wei Dong,Xiaoyu Zhang,Weitao Zheng,Wallace C. H. Choy,Jianjun Tian
Perovskite quantum dot (QD) charging is prone to occur during light-emitting diode (LED) operation due to the electron accumulation inside the QD emitters, which is caused by the unbalanced charge injection and carrier transportation. Here in order to address this issue, an electron attractor of phenethylammonium (PEA + ) is introduced to the surface of perovskite QDs. The PEA + conjugated ligands can reversibly store and release electrons driven by the electron local density of states redistribution, which enhances the delocalization of electrons in QDs, and thus suppresses QD charging at high carrier concentrations, as evidenced by the excitation energy dependent photoluminescence. Besides, PEA + down-shifts the Fermi level of perovskite QDs, consequently increases the hole concentration, leading to greatly improved hole conduction. Halogen-rich synthesis environment also reduces the number of halogen vacancies, consequently narrows the distribution of electronic states at the band edges, leading to slightly improved electron conduction. Taking advantage of the enhanced electron delocalization and improved charge transportation, the CsPbI 3 QDs LEDs show the maximum external quantum efficiency (EQE) of 15.6% with a low efficiency roll-off, and the maximum luminance of 1634 cd m −2 .
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MATERIALS & DESIGN
·
2022
·
IF 9.417
Yanbin Zhang,Lu-Lu Qiao,Zhi-Qiang Zhang,Yong-Fang Liu,Lin-Song Li,Huaibin Shen,Mei-Xia Zhao
Numerous cellular functions are closely reliant on mitochondria and so the capability to conduct long-term stable studies of their activity is of great importance. However, current commercial mitochondrial probes are severely limited in their ability to trace mitochondria due to their inherently poor stability. Here, for the first time, we designed a novel mitochondrial fluorescent probe using InP quantum dots (QDs) as a fluorescent master and skillfully combined with (3-carboxypropyl)triphenylphosphine (TPP) for specific recognition. The bespoke InP QDs probes described here exhibited clear advantages, including simple and low-cost synthesis, high quantum yields, extremely low toxicity, good biocompatibility, and excellent photochemical stability, thus representing a versatile, novel mitochondrial fluorescent probe, particularly suitable in applications traditionally undertaken by Cd-based QDs in biological fields.
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Nanoscale Advances
·
2022
·Vol. 4
·期 13
·2884-2892
·
IF 5.598
Wei Guo,Cui Liu,Nian Li,Min Xi,Yamin Che,Changlong Jiang,Shudong Zhang,Zhenyang Wang
Anti-/de-icing of glass surfaces is of great importance in present daily life. The long-standing challenge in this field is largely due to the lack of stable multifunctional coatings that can be conveniently and economically constructed on the glass surface, and more importantly, are capable of retaining the original transparency of glass ranging from the visible to the near infrared spectrum. Herein, a direct spraying sol method on the glass surface to prepare a highly transparent and photothermal composite coating is reported. Such multifunctional coating of Cu7S4 nanoparticles/organo-silicone sols has displayed a good photothermal conversion property and hydrophobic property and therefore yields excellent anti-icing and self-melting ice properties. The condensation time of water droplets can be extended to 86 s even at −10 °C, which is 3.42 times delayed relative to ordinary blank glass. And the adhesion strength of ice is largely reduced to 72 KPa, which is as low as ∼1/3 that of ordinary glass. Meanwhile, the subcooling of adhering droplets is reduced to −12 °C under one solar illumination condition and exhibits a rapid de-icing capability. More impressively, the prepared functional coating glass shows an outstanding transmittance of more than 75% in the visible region, while it is over the minimum glass transmittance limit allowed by Safety Standards for Glass (GB9656-2016, China). In addition, the multifunctional photothermal glass coating exhibits good physical/chemical stability, which facilitates the long-term application of the coating in different environments.
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ACS Applied Nano Materials
·
2022
·
IF 6.14
Qingting Zhang,Andreas Goldbach,Na Ta,Wenjie Shen
Some of the most active catalysts for the selective oxidation of olefins are based on molybdenum oxides or silver (Ag) systems. Hence, we furnished α-MoO3 nanobelts (NBs) with size-controlled silver nanoparticles (Ag NPs) in order to explore the synergies between these materials. Intriguingly, the components reacted with each other at 350 °C to generate a Ag2Mo4O13 skin on the NBs, which turned them into a very selective catalyst for propylene conversion to acrolein. The selectivity to this aldehyde improved from less than 20% over bare NBs to ca. 75% at 350 °C, in line with the apparent intrinsic limit of other unpromoted molybdates. Propylene oxide formation appears to be completely inhibited because of the encapsulation of residual Ag NPs by silver molybdate. The reaction kinetic characteristics over Ag2Mo4O13 are consistent with a Mars–van Krevelen mechanism. However, the apparent activation energies for reoxidation of silver molybdate (86.9 kJ mol–1) and propylene activation (37.9 kJ mol–1) are considerably lower than those reported for other molybdates. The acrolein formation rate over the coated NBs exceeds that over bulk Ag2Mo4O13 by more than a factor of 10 because of the similarly enlarged surface area. On the basis of the Ag content, the rate gain is even boosted by 4 orders of magnitude because only marginal noble-metal amounts (<0.3 wt %), i.e., Ag2Mo4O13, are needed for optimum catalytic activity of the composite. Altogether, these features render Ag2Mo4O13-coated MoO3 NBs as a prototypal design for highly efficient, nanostructured selective oxidation catalysts.
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Journal of Materials Chemistry C
·
2022
·Vol. 10
·期 21
·8432-8440
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IF 8.067
Xiao Wei,Shen Zhang,Tong Wang,Aixia Chen,Jifeng Guo,Bo Bai,Shengke Yang,Yaqian Li,Xinyi Wang,Xinni Liu
All-inorganic halide perovskite quantum dots (IPQDs) have attracted considerable attention as an emerging fluorescent material owing to their excellent optical properties. However, due to the instability of IPQDs in polar solution, IPQDs have not been used in imprinting and detection in the aqueous phase. Herein, a sensitive, selective fluorescent sensor is reported, which combines luminescent CsPbBr3 quantum dots (QDs) and molecularly imprinted polymers (MIPs) for trace tetracycline (TC) detection in aqueous environments. IPQDs@MIPs were constructed by encapsulating water-soluble CsPbBr3 QDs in pre-prepared MIPs to avoid fluorescence quenching during conventional imprinted polymerization and elution, and the porous silicon matrix protected the QDs. IPQDs@MIPs solution emitted bright green fluorescence under UV lamp irradiation, confirming that IPQDs were stable in the aqueous phase and showed excellent selectivity for TC detection. Under optimal conditions, the fluorescence intensity of the IPQDs@MIPs had a good linear correlation with TC in the concentration range of 0.2–5.0 μM, and the detection limit was 28 nM. Furthermore, the imprinting factor of the IPQDs@MIPs was 4.87, and the mechanism of fluorescence quenching was mainly the electron transfer between TC and IPQDs@MIPs. The fluorescent sensor achieved satisfactory results in the standard addition recovery experiment of an actual water sample. This work paves the way for the further development of IPQDs in the field of analytical chemistry in a practical detection environment.
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