Journal of Materials Chemistry C
·
2023
·Vol. 11
·期 23
·7654-7661
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IF 6.4
Jinchan He,Xiao Zhang,Cong Xie,Hsueh Shih Chen,Ping Yang
Because of their inherent ionic properties, inorganic cesium halide lead perovskite nanocrystals (NCs) are normally unstable in light and heat environments as well as polar solvents, which seriously limit their practical application. In this paper, AlO(OH) nanosheets were assembled into hollow mesoporous spheres to encapsulate CsPbX3 NCs for increasing stability according to the powerful adsorption of AlO(OH) on Pb ions. The hollow AlO(OH) assemblies were created via hydrothermal synthesis. The in situ growth of CsPbX3 NCs in AlO(OH) assemblies was then finished in dimethylformamide solutions. After encapsulation, the stability of the NCs was greatly improved and the exchange reaction of halogen ions was effectively prevented. The NCs in the assemblies exhibited high PL quantum yields (PLQYs). Namely, blue-, green-, and red-emitting CsPbX3 (X = Cl, Br, and I)@AlO(OH) composites were fabricated. The composites were further mixed with polystyrene (PS) to prepare a flexible photoluminescent (PL) film with excellent bendable and foldable properties. The initial PLQYs of blue-, green-, and red-emitting CsPbX3@AlO(OH) composites were found to be 48.2, 96.4, and 43.7%, respectively. The films revealed high stability against water because of the excellent hydrophobic properties of PS. These emitting films were made into bands of various shapes, in which their well-flexible nature endowed the films with important applications.
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Small
·
2023
·Vol. 19
·期 33
·2302465
·
IF 13.3
Pengye Du,Pengpeng Lei,Yuan Liang,Ran An,Hongjie Zhang
Lanthanide-doped upconversion luminescent materials (LUCMs) have attracted much attention in diverse practical applications because of their superior features. However, the relatively weak luminescence intensity and low efficiency of LUCMs are the bottleneck problems that seriously limit their development. Unfortunately, most of the current major strategies of luminescence enhancement have some inherent shortcomings in their implementation. Here, a new and simple strategy of molten salt-assisted synthesis is proposed to enhance lanthanide upconversion luminescence for the first time. As a proof-of-concept, a series of rare earth oxides with obvious luminescence enhancement are prepared by a one-step method, utilizing molten NaCl as the high-temperature reaction media and rare earth chlorides as the precursors. The enhancement factors at different reaction temperatures are systematically investigated by taking Yb 3+ /Er 3+ co-doped Y 2 O 3 as an example, which can be enhanced up to more than six times. In addition, the molten salts are extended to all alkali chlorides, indicating that it is a universal strategy. Finally, the potential application of obtained UCL materials is demonstrated in near-infrared excited upconversion white light-emitting diodes (WLEDs) and other monochromatic LEDs.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Gang Yang,Songchao Bai,Xueguo Li,Hao Liang,Chao Li,Jie Sun,Yinhua Wang,Jinshu Huang,Gencai Pan,Yongsheng Zhu
Lead-free halide double perovskite, as one of the promising candidates for lead halide perovskite materials, shows great potential in light-emitting diodes (LEDs), benefiting from its environmental friendliness and high chemical stability. However, the poor regulation of the emission spectra severely limits its application range. Herein, various lanthanide ions were successfully doped in Cs2NaScCl6 double perovskite single crystals (DPSCs) to yield effective and stable emissions spanning from visible to near-infrared (NIR) regions. Notably, efficient energy transfer from the host to the dopants enables tunable emissions with good chromaticity, which is rarely reported in the field of lead-free double perovskite. Moreover, density functional theory calculations reveal that the high local electron density around the [LnCl6]3– octahedron in DPSCs plays a key role in the improvement of photoluminescence quantum yields (PLQYs). The optimal PLQYs are up to 84%, which increases around 3 times over that of the undoped sample. Finally, multicolor and NIR LEDs based on Ln3+-doped Cs2NaScCl6 DPSCs were fabricated and had different application functions. Specifically, the single-composite white LED shows adjustable coordinates and correlated color temperatures, while the NIR LED shows good night vision imaging. This work provides new inspiration for the application of efficient multifunctional LEDs based on lead-free double perovskite materials.
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Advanced Optical Materials
·
2023
·Vol. 11
·期 16
·2300187
·
IF 9
Nan Zhang,Rui Zhang,Xieming Xu,Fang Wang,Zhicheng Sun,Shuaihua Wang,Shaofan Wu
X-ray flat-panel detectors are widely used for nondestructive detection of internal information in medical radiography and industrial applications. However, a persisting challenge is the application of radiography on highly curved 3D objects to realize flexibility and information storage for the fabrication of flexible large-area X-ray detectors. This study demonstrates a halide-based double perovskite Cs 2 Na 0.9 Ag 0.1 LuCl 6 :Dy 3+ by a hydrothermal reaction. The as-prepared crystals exhibit afterglow features through a co-doping strategy of Dy 3+ and Ag + ions. The double perovskite material with doping modification exhibits excellent scintillation properties with high sensitivity, low detection limit, and high radiation stability. In addition, flexible scintillator detectors are fabricated with an area of 8.0 × 6.0 cm 2 by the blade-coating strategy, which has a high spatial resolution of 11.2 lp mm −1 @MTF = 0.2. Based on the long afterglow properties, the Cs 2 Na 0.9 Ag 0.1 LuCl 6 :Dy 3+ flexible film exhibits thermoluminescence after turning off the X-ray, thereby having strong potential for X-ray imaging of nonflat and irregular objects.
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2023
·Vol. 332
·期 7
·2589-2600
·
IF 1.6
Wang Binyan,Lu Shufan,Dai Chenjing,Ma Jianguo,Luo Jianqiang,Meng Jia,Tong Xiaolan,Liu Shujuan
In present paper, a porous carbon composite electrode, doped with nickel hexacyanoferrate, was prepared for electrochemical removal of cesium ions from aqueous solutions. Based upon the applied voltage of −3 V, a 100% adsorption was achieved in 3 h for the initial Cs + concentration of 10 ppm in solution. The maximum capacity was 155.2 mg g −1 under optimized electrochemical conditions. The electrode was regenerated by applying a reverse voltage of 3 V. The removal efficiency remained 95% even after five consecutive adsorption–desorption cycles. The results suggested that the developed electrochemical method has strong potential for extracting cesium from aqueous solutions.
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INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Meng Cheng,Congcong Jin,Wenqi Jin,Xueling Hou
Borates provide an excellent platform for investigating the optical nonlinearity and linearity of crystals as photoelectric functional materials. In our work, borate derivatives with isolated [B3O3] six-membered rings as structural features are the preferred system due to their simple functional units and excellent properties. Herein, by utilizing the target-oriented synthesis, a series of borate derivatives, A2[B3O3F4(OH)] (A= NH4, Rb, Cs) (ABOFH), K2.3Cs0.7B3O3F6 (KCsBOF), and Cs3[B3O3(OH)3]Cl3 (CsBOHCl), with novel heteroanionic groups containing [BOxF4–x] (x = 0–3) and/or [BO2(OH)] units were obtained. ABOFH, KCsBOF, and CsBOHCl construct different two-dimensional pesudolayers featuring [B3O3F4(OH)], [B3O3F6], and [B3O3(OH)3] units, respectively. Also, the optical properties and the arrangement information of these anionic groups were studied. Among the total five compounds, (NH4)2[B3O3F4(OH)] and Cs3[B3O3(OH)3]Cl3 with enlarged birefringence and sufficient band gaps were screened out as promising birefringent crystals due to the optimally aligned configuration of birefringence-active heteroanionic units. The successful results of target-oriented synthesis indicate a more profound conclusion that the borate system now has more diversified structural chemistry, and an effective strategy was proposed to modify the arrangement and species of anionic units to optimize the performance of optical crystals.
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ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Shiyao Lu,Jian Zhang,Hao Meng,Xiaoyuan Qin,Jianbin Huang,Yehao Liang,Feng-Shou Xiao
Dehydration of methyl lactate (ML) obtained from biomass is a sustainable route for the production of methyl acrylate (MA). Herein, we demonstrate that cesium-exchanged Al-rich Beta zeolite (Cs-Beta) is highly efficient for the dehydration of ML to MA, exhibiting full ML conversion with 87.4% MA yield at 340 °C. In situ FT-IR spectra and kinetic studies provide evidence that the ML dehydration on the Cs-Beta zeolite follows a forward ion-exchange/dehydration/reverse ion-exchange reaction pathway. Model experiments, DFT calculations, TG-DSC analysis, and FT-IR spectra showed that coke formation competes with the dehydration of ML to MA. Kinetic studies and theoretical simulations demonstrate that cesium cations in the micropores of Beta zeolite have a strong steric hindrance, suppressing the formation of oligomers and coke. These results offer new insights for developing highly selective and stable catalysts for the dehydration of ML to MA in the future.
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JOURNAL OF PHYSICAL CHEMISTRY B
·
2023
·
IF 3.3
Zhuanfang Jing,Yongquan Zhou,Toshio Yamaguchi,Koji Ohara,Jianming Pan,Guangguo Wang,Fayan Zhu,Hongyan Liu
The underlying recognition mechanisms of alkali metal ions by crown ethers in aqueous solutions are yet to be fully understood at the molecular level. We report direct experimental and theoretical evidence for the structure and recognition sequence of alkali metal ions (Li+, Na+, K+, Rb+, and Cs+) by 18-crown-6 in aqueous solutions by wide-angle X-ray scattering combined with an empirical potential structure refinement modeling and ab initio molecular dynamics simulation. Li+, Na+, and K+ are located in the negative potential cavity of 18-crown-6, with Li+ and Na+ deviating from the centroid of 18-crown-6 by 0.95 and 0.35 Å, respectively. Rb+ and Cs+ lie outside the 18-crown-6 ring and deviate from the centroid of 18-crown-6 by 0.05 and 1.35 Å, respectively. The formation of the 18-crown-6/alkali metal ion complexes is dominated by electrostatic attraction between the cations and the oxygen atoms (Oc) of 18-crown-6. Li+, Na+, K+, and Rb+ form the H2O···18-crown-6/cation···H2O “sandwich” hydrates, while water molecules only hydrate with Cs+ of the 18-crown-6/Cs+ complex on the same side of Cs+. Based on the local structure, the recognition sequence of 18-crown-6 for alkali metal ions in an aqueous solution follows K+ > Rb+ >Na+ >Li+, which is completely different from that (Li+ > Na+ > K+ > Rb+ > Cs+) in the gas phase, confirming that the solvation medium seriously affects the cation recognition of crown ethers. This work provides atomic insights into understanding the host–guest recognition and solvation behavior of crown ether/cation complexes.
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CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Wenfeng Sun,Xue Li,Bo Li,Caizheng Wang,Ying Zhao,Xiaotao Zu,Weilie Zhou,Xia Xiang
In this work, the carbon quantum dots@Cs 2 NaInCl 6 (CDs@CNC) composites are presented by a facile solution synthesis. The obtained CDs@CNC composites maintain the octahedral morphology of original CNC host and the characteristic functional groups of original CDs. As a result, the rare-earth-free CDs@CNC composites exhibit green light emission with good stability for UV irradiation, heat, and humidity. In addition, CDs were combined with ion-doped CNC to obtain multicolor phosphor and the corresponding white light emitting diode (WLED) devices were fabricated by coating composites on commercial UV chips. The color render index (CRI) of WLEDs increases significantly from 66.24 to 90.95 while the cold-warm white fluorescence can be flexibly tuned by the change of excitation wavelength. The combination of CDs and double perovskites provide a new route to design white light emission phosphors, which could lead to the fabrication of next generation high-quality lighting devices.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2023
·
IF 3.3
Wanlei Geng,Yinfeng Liu,Debin Wang,Mengyu Lin,Xue Yang,Limei Zhong,Runxiong Lin,Li Ding,Lianying Wu,Dianquan Dong
Radioactive Cs + is one of the most dangerous environmental pollutants . It is necessary for radioactive Cs + management and removal. Titanium-type cesium ion sieve with a strong Ti–O bond has the advantages of structural stability, radiation resistance and no secondary contamination, which is a promising adsorbent material. In this paper, The CTO (Cs 2 Ti 6 O 13 ) is prepared for the first time by sol-gel and de-templating methods, and cesium ion sieves (HTO/PMMA) are further obtained with diluted HCl elution. Compared with the ionic sieves (HTO) prepared by direct sol-gel method, the adsorption capacity is improved from 224.32 mg/g to 299.15 mg/g. The prepared HTO/PMMA has a larger specific surface area (67.282 m 2 /g). More exchange sites are provided for the adsorption of Cs ions. Moreover, Adsorption involves the cleavage of O–H bonds and the formation of O–Cs bonds, which is a typical ion exchange reaction . A series of batch experiments are carried out. The results showed that the equilibrium adsorption capacity of HTO/PMMA is 307.69 mg/g and remained high in the interfering ion solution as well (280.38 mg/g). The pseudo second order model and Freundlich model can well describe the ion exchange process. Thermodynamic study shows that adsorption is spontaneous and exothermic, and low temperature is conducive to adsorption in H + - Cs + exchange system. Finally, the reusability of HTO/PMMA is evaluated. The adsorption capacity did not decrease significantly after 5 cycles of use. Therefore, HTO/PMMA is expected to be an excellent material for recovering radioactive Cs + .
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Chi Ma,Chenyu Qi,Dingbo Wei,Zhenzhen Jiang,Yafei Guo,Nelson Belzile,Tianlong Deng
The efficient and renewable recovery of cesium and strontium by absorption from a new type of geothermal water liquid mineral resource is highly desirable but still challenging. In this work, a new Zr-doped layered potassium thiostannate adsorbent (KZrTS) was first synthesized and used for Cs+ and Sr2+ green and efficient adsorption. It was found that KZrTS had very fast adsorption kinetics toward both Cs+ and Sr2+ with an equilibrium reached within 1 min, and the theoretical maximum adsorption capacities for Cs+ and Sr2+ were 402.84 and 84.88 mg/g, respectively. Moreover, to solve the loss problem of the engineering application of the powdered adsorbent KZrTS, KZrTS was uniformly coated with polysulfone by wet spinning technology to form micrometer-level filament-like absorbents (Fiber-KZrTS), whose adsorption equilibrium rates and capacities toward Cs+ and Sr2+ are almost the same as that of powder. Furthermore, Fiber-KZrTS showed excellent reusability, and the adsorption performance remained virtually unchanged after 20 cycles. Therefore, Fiber-KZrTS has potential application for green and efficient cesium and strontium recovery from geothermal water.
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LANGMUIR
·
2023
·
IF 3.9
Zhilin Li,Qiaoqiao Li,Mengyan Cao,Zhihui Rao,Xinyu Shi,Liujiang Zhou,Xiujian Zhao,Xiao Gong
Low-dimension perovskite materials have attracted wide attention due to their excellent optical properties and stability. Herein, Sb3+-doped Cs2ZrCl6 crystals are synthesized by a coprecipitation method in which Sb3+ ions partially replace Zr4+ ions. The Cs2ZrCl6:xSb3+ powder shows blue and orange–red emissions under a 254 and 365 nm light, respectively, due to the [ZrCl6]2– octahedron and [SbCl6]3– octahedron. The photoluminescence quantum yield (PLQY) of Cs2ZrCl6:xSb3+ (x = 0.1) crystals is up to 52.5%. According to experimental and computational results, the emission mechanism of the Cs2ZrCl6:xSb3+ crystals is proposed. On the one hand, a wide blue emission with a large Stokes shift is caused by the self-trapping excitons of [ZrCl6]2– octahedra under a 260 nm excitation. On the other hand, the luminescence mechanism of [SbCl6]3– octahedron is divided into two parts: 1P1 → 1S0 (490 nm) and 3P1 → 1S0 (625 nm). The broad-band emission, high PLQY, and excellent stability endow the Cs2ZrCl6:xSb3+ powders with the potential for the fabrication of white light-emitting diodes (WLEDs). A WLED device is fabricated using a commercial 310 nm NUV chip, which shows a high color rendering index of 89.7 and a correlated color temperature of 5333 K. In addition, the synthesized Cs2ZrCl6:xSb3+ crystals can be also successfully used for information encryption. Our work will provide a deep understanding of the photophysical properties of Sb3+-doped perovskites and facilitate the development of Cs2ZrCl6:xSb3+ crystals in encrypting multilevel optical codes and WLEDs.
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