HYDROMETALLURGY
·
2022
·
IF 4.217
Wanlei Geng,Debin Wang,Yinfeng Liu,Jialing Zhang,Limei Zhong,Runxiong Lin,Li Ding,Lianying Wu,Dianquan Dong
Developing a stable and efficient adsorbent to recover Cs + from liquid resources or to remove radioactive Cs + from wastewater is challenging. In this study, the precursor Cs 2 Ti 6 O 13 (CTO) was synthesized by the solvothermal and solid-phase sintering methods for the first time, then it was acid-modified to synthesize a novel H-type titanium-based material (H-CTO nanosheets). A series of batch adsorption experiments was carried out. The adsorption of Cs + on H-CTO was evaluated under different experimental conditions, including contact time, temperature, initial Cs + concentration, pH, and interfering ions. Experiments show that H-CTO exhibits a larger adsorption capacity (329 mg/g) and better cycle performance than the currently reported titanium-based adsorbents. The cesium ions were easily eluted by the 0.2 M HCl solution; the adsorption capacity did not decrease significantly after five cycles. Furthermore, the adsorption behavior of Cs + on H-CTO can be described by the Langmuir isotherm and pseudo-second-order kinetic models. Characterization using IR and Raman spectroscopic analyses indicates that the adsorption mechanism of Cs + on H-CTO involves O H bond cleavage and O Cs bond formation. Thermodynamic studies showed that low temperatures are favorable for Cs + adsorption and are spontaneous. Overall, the results suggest that H-CTO nanosheets are promising for the recovery or removal of Cs + ions from Cs-containing liquid ores or radioactive wastewater .
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Journal of Materials Chemistry C
·
2023
·Vol. 12
·期 4
·1309-1316
·
IF 6.4
Zhichao Liu,Yuexiao Pan,Xiaoxiao Fu,Yihong Ding,Liyi Li
The development of efficient, non-toxic, and cost-effective white-light emitters is crucial for advancing lighting technology. Here, we present a groundbreaking study on a new all-inorganic perovskite crystal, CsCaCl3:Mn2+, which exhibits temperature sensing and hue-tunable white light emission. The CsCaCl3 matrix emits broad blue light at 455 nm due to self-trapped exciton (STE) emission. Upon Mn2+ doping, the CsCaCl3:Mn2+ crystal emits broad yellow light at 555 nm, originating from the Mn2+ 4T1(G)–6A1(S) transition. Increasing Mn2+ concentration led to a decrease in blue emission intensity, accompanied by enhanced yellow emission, suggesting an energy transfer from STEs to Mn2+. The enhanced stability of CsCaCl3:Mn2+ compared to pure CsCaCl3 is demonstrated through thermal analysis. The distinctive temperature-dependent responses of STE and Mn2+ emissions in CsCaCl3:Mn2+ suggest its potential application in temperature sensing. The synthesis process for this luminescent crystal is both straightforward and scalable, making it a promising candidate for large-scale applications.
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CHEMICAL ENGINEERING JOURNAL
·
2023
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IF 15.1
Xiuqiang Duan,Kun Nie,Ziyao Hu,Xiaodong Zhang,Ranran Zhou,Wubin Dai,Lefu Mei,Luoxin Wang,Hua Wang,Xiaoxue Ma
In recent years, all-inorganic perovskites have attracted considerable research attention. However, the advancement of lead-based perovskites has encountered substantial challenges, redirecting current research efforts toward lead-free alternatives. In this study, we synthesized novel Cs 4 MnBi 2 Cl 12 perovskite crystals at 80 °C. Furthermore, Tb 3+ ions were introduced to enhance the fluorescence properties and stability of the as-prepared perovskite crystals (PCs). The photoluminescence quantum yield (PLQY) of Tb 3+ -doped PCs was 25.45 % (∼598 nm), making a two-fold increase compared with the original PCs. In the PCs, [BiCl 6 ] 3− octahedrons serve as energy collectors, generating excitons, while [MnCl 6 ] 4− octahedrons function as luminescence centers of the receptor. Owing to their entirely inorganic composition, the PCs exhibited exceptional stability under sunlight and across a wide range of temperatures. Finally, we applied the PCs to fiber composite paper and an light-emitting diode (LED) device, which retained their specific stability after the modification. The findings of this study offer nover insight for incorporating perovskites into fiber applications and optoelectronic devices.
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Advanced Science
·
2023
·
IF 15.1
Bo Gao,Changqing Tian,Linfeng Guo,Jinchen Zhou,Zixian Wang,Chengfan Fu,Hongmei Ran,Wei Chen,Qiang Huang,Daofu Wu,Xiaosheng Tang,Zhongtao Luo
In order to deal with the global energy crisis and environmental problems, reducing carbon dioxide through artificial photosynthesis has become a hot topic. Lead halide perovskite is attracted people's attention because of its excellent photoelectric properties, but the toxicity and long-term instability prompt people to search for new photocatalysts. Herein, a series of <111> inorganic double perovskites Cs 4 Mn 1-x Cu x Sb 2 Cl 12 microcrystals (x = 0, 0.1, 0.2, 0.3, 0.4, and 0.5) are synthesized and characterized. Among them, Cs 4 Mn 0.7 Cu 0.3 Sb 2 Cl 12 microcrystals have the best photocatalytic performance, and the yields of CO and CH 4 are 503.86 and 68.35 µmol g −1 , respectively, after 3 h irradiation, which are the highest among pure phase perovskites reported so far. In addition, in situ Fourier transform infrared (FT-IR) spectroscopy and electron spin resonance (ESR) spectroscopy are used to explore the mechanism of the photocatalytic reaction. The results highlight the potential of this class of materials for photocatalytic reduction reactions.
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高影响因子
MOLECULES
·
2023
·Vol. 28
·期 24
·7987
·
IF 4.6
Yancheng Wu,Manyu Lian,Guotao Huang,Yangfan Zhang,Ningbo Yi,Liyong Tian,Feng Gan,Chunping Ma
Atert-butyldiphenylsilyl-containing polyimide (PI-OSi) has been established as a colorimetric and ratiometric chemosensor for rapid detecting fluoride ions (F−). The UV-vis absorbance ratio value (A322/A288) ofPI-OSiin a DMF solution displays a wide linear range change to F−concentrations with a detection limit (DL) value of 2.13 μM. Additionally, adding incremental amounts of F−to a DMF solution ofPI-OSishows an immediate color change to yellow and finally to green from colorless. More interestingly, the resultingPI-OSiplus F−system (PI-OSi·F) could detect trace water in DMF. The A292/A322value ofPI-OSi·F almost linearly increases with low water content, which suggests convenient quantitative sensing of trace water content in DMF. The DL value ofPI-OSi·F for sensing water in DMF is determined to be 0.00149% (v/v). The solution color ofPI-OSi·F returns to colorless when the water content increases, indicating thatPI-OSi·F can conveniently estimate water content in DMF by naked-eye detection. The detection mechanisms confirmed by an1H NMR study and a DFT calculation involve a F−-induced desilylation reaction ofPI-OSito form phenolate anion followed by protonation with trace water. Finally,PI-OSifilm was fabricated for the colorimetric detection of F−and water in CH3CN.Keywords:tert-butyldiphenylsilyl-containing polyimide;colorimetric and ratiometric chemosensor;fluoride ions;trace water
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Small
·
2023
·
IF 13.3
Zhihao Chen,Malik Zeeshan Shahid,Xinyan Jiang,Meng Zhang,Danrui Pan,Hongpeng Xu,Guocan Jiang,Jin Wang,Zhengquan Li
Halide perovskites exhibit outstanding optoelectronic properties, which make them an ideal choice for photocatalytic CO 2 reduction and benzyl alcohol (BA) oxidation. Nevertheless, the simultaneous realization of the above redox coupling reactions on halide perovskites remains a great challenge, as it requires distinct catalytic sites for different target reactions. Herein, the catalytic sites of Cs 2 AgBiCl 6 (CABC) are regulated by doping Fe for efficient coupling of photocatalytic CO 2 reduction and BA oxidation. The Fe-doped CABC (Fe: CABC) exhibits an enhanced visible-light response and effective charge separation. Experimental results and theoretical calculations reveal a synergistic interplay between Bi and Fe sites, where the Bi and Fe sites have lower activation energies toward CO 2 reduction and BA oxidation. Further investigations demonstrate that electrons and holes prefer to accumulate at the Bi site and Fe site under light irradiation, respectively, which creates favorable conditions for facilitating CO 2 reduction and BA oxidation. The resultant Fe: CABC achieves a high photocatalytic performance toward CO (18.5 µmol g −1 h −1 ) and BD (1.1 mmol g −1 h −1 ) generation, which surpasses most of the state-of-the-art halide photocatalysts. This work demonstrates a facile strategy for regulating the catalytic site for redox coupling reactions, which will pave a new way for designing halide perovskites for photocatalysis.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Fengmei Zhu,Yuan Gao,Chunli Zhao,Jiacheng Pi,Jianbei Qiu
Near-infrared phosphor-converted light-emitting diodes (NIR pc-LEDs) offer numerous advantages, including compact size, tunable emission spectra, energy efficiency, and high integration potential. These features make them highly promising for various applications, such as night vision monitoring, food safety inspection, biomedical imaging, and theragnostics. All-inorganic halide double-perovskite materials, known for their large absorption cross section, excellent defect tolerance, and long carrier diffusion radius, serve as unique matrices for constructing near-infrared fluorescent materials. In this study, we successfully prepared the all-inorganic metal halide double-perovskite Cs2NaYCl6:Cr3+ using a grinding–sintering method. A small fraction of the [YCl6] octahedra within the host material’s lattice was substituted with Cr3+ ions, resulting in the creation of the Cs2NaYCl6:Cr3+ phosphor. When excited with λ = 310 nm UV light, the phosphor exhibited a broad emission range spanning from 800 to 1400 nm, covering the NIR-I and NIR-II regions. It had a broad bandwidth emission of 185 nm and achieved a fluorescence quantum yield of 20.2%. The unique broadband emission of the phosphor originates from the weak crystal field environment provided by the Cs2NaYCl6 host matrix, which enhances the luminescence properties of the Cr3+ ions. To create NIR pc-LEDs, the phosphor was encapsulated onto a commercially available UV LED chip operating at 310 nm. The potential application of these NIR pc-LEDs in night vision imaging was successfully validated.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Xueguo Li,Hao Liang,Changbo Zheng,Chunxiang Zhao,Songchao Bai,Xueqing Zhao,Hao Zhang,Yongsheng Zhu
Lead-free halide double perovskites are widely used for phosphors converted light emitting diode (pc-LED) devices. However, it remains a challenge to modulate their spectra to meet different application requirements. Herein, Cs 2 NaInCl 6 :Sb 3+ double perovskite crystals with excellent blue emission of self-trapped excitons (STEs) were prepared and a lanthanide ions (Ln 3+ ) doping strategy was employed to enable multicolor emissions in this system. The emission colors can be continuously adjusted in a wide range by altering the Ln 3+ ions doping levels. Especially, white light emissions with tunable correlated color temperature were obtained in Tb 3+ , Ho 3+ ions codoped samples. Outstanding photoluminescence quantum yields of the samples are ascribed to the sensitization effect of Sb 3+ ions and the efficient energy-transfer from STEs to Ln 3+ ions. LED devices were further fabricated to demonstrate the great application potentials of the prepared phosphors. These findings provide deep insights for the designing of multicolor double perovskite phosphors.
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CHEMISTRY OF MATERIALS
·
2023
·
IF 8.6
Mengran Sun,Wenhao Xing,Shyong K. Chen,Chunxiao Li,Wenhao Liu,Ming-Hsien Lee,Jiyong Yao
Chalcogenides are promising candidates for exploring mid- and far-infrared nonlinear optical (NLO) materials. Nevertheless, although tellurides possess greater advantages in the above-mentioned spectral regions, the reports on telluride NLO materials are far fewer than those on sulfides and selenides. In this work, a new quaternary NLO-active telluride, KCd4Ga5Te12, was discovered, and its Rb and Cs analogues were successfully synthesized. They are crystallized in the trigonal R3 space group and the structure features a 3D diamond-like framework constructed by vertex-sharing asymmetric MTe4 tetrahedra (centered by disordered Cd and Ga) that are stacked along the c-axis. Moreover, a comprehensive study of their IR NLO properties, photoluminescence properties, and structural features was performed. These compounds exhibited large powder second-harmonic generation (SHG) intensities, about 2.1 (2.7, 4.4) times that of AgGaSe2 in the particle size range of 20–50 (125–150) μm and a wide transmission range (∼25 μm). The SHG-density analysis revealed that the largest component χ333(2) of KCd4Ga5Te12 originates from three types of Te in the crystal structure. More importantly, it is rare in literature to demonstrate the consistency of linear and NLO properties calculated using both ultrasoft pseudopotentials and norm-conservation pseudopotentials. Besides, the title compounds also exhibit strong luminescence emissions around 420 and 470 nm at 298 K. This work implies that title compounds are promising candidates in the IR NLO applications.
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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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iScience
·
2023
·
IF 5.8
Daofu Wu,Xiaoqing Liu,Changqing Tian,Jinchen Zhou,Junan Lai,Hongmei Ran,Bo Gao,Miao Zhou,Qiang Huang,Xiaosheng Tang
Summary Lead halide perovskites are prospective candidates for CO 2 photoconversion. Herein, we report copper-doped lead-free Cs 2 AgSbCl 6 double perovskite microcrystals (MCs) for gas-solid phase photocatalytic CO 2 reduction. The 0.2Cu@Cs 2 AgSbCl 6 double perovskite MCs display unprecedented CO 2 photoreduction capability with CO and CH 4 yields of 412 and 128 μmol g −1 , respectively. The ultrafast transient absorption spectroscopy reveals the enhanced separation of photoexcited carriers in copper-doped Cs 2 AgSbCl 6 MCs. The active sites and reaction intermediates on the surface of the doped Cs 2 AgSbCl 6 are dynamically monitored and precisely unraveled based on the in-situ Fourier transform infrared spectroscopy investigation. In combination with density functional theory calculations, it is revealed that the copper-doped Cs 2 AgSbCl 6 MCs facilitate sturdy CO 2 adsorption and activation and strikingly enhance the photocatalytic performance. This work offers an in-depth interpretation of the photocatalytic mechanism of Cs 2 AgSbCl 6 doped with copper, which may provide guidance for future design of high-performance photocatalysts for solar fuel production.
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JOURNAL OF MOLECULAR LIQUIDS
·
2023
·
IF 6
Chong Liang,Wei Zhao,Shangshang Ma,Dingkai Wang,Xutang Liu,Linyang Dong
To explore the effect of adding acidic ionic liquids (ILs) to the heteropoly acid/H 2 SO 4 catalytic system on the aerobic oxidation of lignite, acidic ILs functionalized with -SO 3 H were synthesized accordingly and mixed with H 5 PMo 10 V 2 O 40 (HPA-2) in various molar ratios. The optimum combination of HPA-2 and 1-methyl-3-(4-sulfobutyl) imidazolium (MIMBS) with molar ratio of 0.3 showed excellent performance for the catalytic oxidation of lignite, with the yields of carboxylic acids (CAs) (including benzene carboxylic acids, formic acid and acetic acid) reaching 326.21 ± 12.86 mg/g lignite, which considerably exceeded the 136.08 ± 6.23 mg/g lignite of pure HPA-2. Highest occupied molecular orbital energy of CAs calculated by Gaussian 09 on 6-31G(d) basis set and Hammett function analysis confirmed that the oxidative activity and acidity of the catalytic system could be moderately modulated by sulfonated ILs, thereby increasing the yield of CAs. In addition, the effect of H 2 SO 4 concentration on the oxidation of lignite was investigated via the HPA-2/H 2 SO 4 /MIMBS system with different molar ratios, and the results showed that CAs yield increased first and then decreased with increasing H 2 SO 4 concentration, but the concentration of H 2 SO 4 at the maximum yield of CAs was significantly reduced from 0.28 wt% to 0.14 wt% once MIMBS was added. A possible process for the catalytic oxidation of lignite by sulfonated ILs/HPA-2/H 2 SO 4 in aerobic aqueous solution is proposed, which generally involves the reactions of hydrolysis, oxidation and re-oxidation. Due to the good reproducibility, the robust homogeneous catalytic system of HPA-2/sulphonated ILs has the advantages of including increased yields of CAs and reduced H 2 SO 4 dosage, which will pave the way for the efficient utilization of lignite.
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