JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Can Liu,Yujie Li,Qi Liu,Jun Liu,Yafei Guo,Xiaoping Yu,Yingchun Xie,Tianlong Deng
The removal of 137 Cs from radioactive wastewater remains a huge challenge due to the interference of many coexisting ions. Several tin chalcogenides (X 2 Sn 3 Y 7 , X Na, K; Y Te, Se, S) were synthesized and screened for highly selective cesium removal from radioactive wastewater. It was found that Na 2 Sn 3 S 7 showed the best adsorption performance for low cesium concentrations. Especially after nickel doping, the adsorption capacity and thermal stability of the adsorbent were significantly enhanced. Its maximum adsorption capacity reached 436.72 mg·g −1 within only 5 min and adsorption performance kept active in the pH range of 2–12. After being coated with a porous polysulfone (PSF) fiber, the developed PSF-Na 2.1 Ni 0.05 Sn 2.95 S 7 was applied to natural complex water with cesium concentration of 17.58 mg·L −1 . The separation factors between Cs + and competitive ions ranged from 625.21 to 13123.21. It is noteworthy that NaNO 3 was an efficient regenerating agent and can be easily separated from the CsNO 3 mixture for cyclic utilization. Remarkably, only 45 min in each cycle of adsorption and desorption toward cesium was realized, and the adsorption properties hardly decreased even after 50 consecutive cycles. The above advantages make the proposed material an excellent candidate for efficient Cs + removal and enrichment from wastewater.
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Journal of Materials Chemistry C
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2022
·Vol. 10
·期 21
·8356-8363
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IF 8.067
Ye Li,Miaoling Cai,Mengling Shen,Yuting Cai,Rong-Jun Xie
The stability of perovskite nanocrystals (NCs) is greatly limited due to highly dynamic binding of ligands, which hinders their applications in optoelectronic devices. In this paper, a new ligand strategy was employed to prepare CsPbBr3 NCs via a facile room temperature (RT) ligand-assisted reprecipitation (LARP) method, where N1.N2-didodecyl-N1.N1.N2.N2-tetramethylethane-1.2-diaminium bromide (DTDB) as the sole capping ligand and an additional Br resource was used. Compared to other ligands with one coordinating group, this class of bidentate ligand can be tightly anchored to the surface of NCs with double N+ sites. The as-synthesized DTDB-CsPbBr3 NCs exhibited a high photoluminescence quantum yield (PLQY) of 92.3% and also showed a superior colloidal stability even under intense purification for up to ten cycles. Compared to the dodecyltrimethyl ammonium bromide (DTAB) ligand capped-CsPbBr3 NCs, the DTDB-CsPbBr3 NCs display obviously enhanced stability to light, heat and water. X-ray photoelectron spectroscopy (XPS) results revealed that the DTDB-CsPbBr3 NCs have a Br− rich surface, which accounts for the high stability and PLQY. Hence, DTDB is a promising ligand to prepare perovskite NCs with higher optical performance.
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Inorganic Chemistry Frontiers
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2022
·Vol. 9
·期 12
·2880-2894
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IF 7.779
Jia-Ying Zhu,Lin Cheng,Yi-Ming Zhao,Meng-Yu Li,Zi-Zhao Wang,Juan Wang,Cheng Wang,Kai-Yao Wang
Visualization of the ion exchange mechanism for 137Cs and 90Sr decontamination is important for safe radioactive liquid waste reprocessing and emergency response improvement in the event of a nuclear accident. Here, the remediation of Cs+ and Sr2+ was achieved through ion exchange using a cadmium selenidostannate, [CH3NH3]3[NH4]3Cd4Sn3Se13·3H2O (CdSnSe-1), with rapid exchange kinetics, high β/γ radiation resistances, broad pH durability and facile elution. The framework constructed from mono-lacunary supertetrahedral clusters features a great negative charge density of 3.27 × 10−3 that accounts for the superhigh exchange capacities of 371.4 (Cs+) and 128.4 mg g−1 (Sr2+). Single-crystal structural analysis on the exchanger during the “pristine–ion exchange–elution” cycle supplies instructive information to elucidate the uptake and recycle mechanism for Cs+ and Sr2+. The broken symmetry of the cluster caused by a vacant site, combined with the co-templating effects of mixed methylammonium/ammonium, contributes to the formation of voids I and II that show adsorption activity for both Cs+ and K+ ions. In comparison, the divalent Sr2+ ions with higher hydration degree exchange with (alkyl)ammonium cations in a 1 : 2 molar ratio, resulting in its location at a new void (III) closer to the framework and thus a higher binding strength. The energy variation during the adsorption process based on a DFT calculation illustrates the high efficiency of CdSnSe-1 for capture of both Cs+ and Sr2+. This “visualized” ion exchange underlines the robustness and flexibility of CdSnSe-1 as a Cs+ and Sr2+ trapper, and reveals the deeper structure–function relationship from a new surface interaction viewpoint.
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Frontiers in Materials
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2022
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IF 3.985
Zhou Wei,Han Peigeng,Luo Cheng,Li Cheng,Hou Jie,Yu Yang,Lu Ruifeng
Lead free double perovskites (DPs) are promising materials due to their non-toxic and tunable optical properties. In this work, a series of lead-free halide DP single crystals (SCs) and nanocrystals (NCs) (Cs4Cu1-xAg2xSb2Cl12) were reported. With alloying strategy, the optical band-gap engineering was realized and the dimension can be controlled between 2D and 3D. The Cu-alloyed SCs exhibit strong absorption from the UV-visible region to the near-infrared range (can even completely cover the bands of NIR-I and NIR-II). In addition, (Cs4Cu1-xAg2xSb2Cl12) NCs were synthesized via a top-down approach, which maintains similar optical properties and the dimensional transformation phenomenon to SCs. These results suggest the great potential of Cs4Cu1-xAg2xSb2Cl12 SCs and NCs for photovoltaic and optoelectronic applications.
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SOLVENT EXTRACTION AND ION EXCHANGE
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2022
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IF 3.695
Huifang Xing,Liangrong Yang,Lu Wang,Mengfang Li,Jiemiao Yu,Diannan Lu,Gang Ye,Huizhou Liu
The effect of ion species and concentration on the extraction percent of Cs+ by 1,3-Diisopropoxycalix [4] arenecrown-6 (BPC6) in octanol/water solvent extraction system has been studied by molecular dynamics simulations and experiments. The results show that the anionic species play an important role on the enhancement of the extraction percent of Cs+. Specifically, the order in which anions promote the extraction percent is different at different total anion concentrations. At a relatively low anion concentration of 0.5 M, the extraction percent follows the sequence: ClO4−> I−> NO3−> Br−> Cl−> SO42−> F−. At a relatively high concentration of 2 M, the extraction percent of Cs+ follows the following sequence: I−> ClO4−> Br−~ NO3−> Cl−> SO42−> F−. It is indicated that the extraction percent is dominated by the anion’s interface propensity, which is the probability of anion distribution in the interface compared to the water phase. However, at low concentration of anions, strong coordination effect of NO3− promotes the extraction effect compared to Br−. At the high anion’s concentration, the stronger salting-out capacity of Br− leads to a considerable increase of extraction percent. In addition, the cations also slightly affect the extraction percent. The extraction percent is affected by both cations’ concentration and the salt-out effect. On this basis, a neutral Cs+ extraction system has been established, and one stage extraction percent could reach 62.5%.
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Journal of Cleaner Production
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2022
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IF 11.072
Zhenzhen Jiang,Chi Ma,Yanqing He,Mingli Li,Gaoling Liu,Yafei Guo,Duo Ji,Tianlong Deng
To develop a green and efficient cesium adsorbent with high adsorption capacity , rapid kinetics, and good regeneration performance is a tremendous challenge. In this work, potassium iron antimony thiostannate (PIATS) synthesized by the hydrothermal method was utilized for green recovery cesium from geothermal water for the first time. PIATS showed a high adsorption capacity of 401.23 mg/g, which was much higher than other types of adsorbents at present. Meanwhile, PIATS showed rapid ion exchange kinetics (within 3 min) and broad pH resistance (4–12). More importantly, PIATS still showed excellent selectivity to cesium even in geothermal water containing many other coexisted ions ( K d = 1.96 × 10 4 mL/g), and the separation factors between Cs + and the coexisted competing ions were ranged from 462.77 to 963.76. Subsequently, the cesium-laden PIATS could be easily eluted with 0.50 mol/L NaNO 3 to achieve rapid desorption (within 10 min). The concentration of Cs + in the elution was enriched more than 11 times higher than that in the original solution. Furthermore, no organic solvents or other toxic reagents were involved during the whole process. Therefore, the adsorption advantages, excellent enrichment ability, and structural stability of PIATS make it a potential recyclable candidate for green cesium recovery from geothermal water.
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INORGANIC CHEMISTRY
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2022
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IF 5.436
Xiaoxi Li,Weiwei Li,Mengling Xia,Chao Liu,Neng Li,Zuhao Shi,Yinsheng Xu,Xianghua Zhang
Lead-free double perovskites (DPs) have outstanding luminescent properties, which make them excellent candidates for wide use in optoelectronics. Herein, a solvent-free melting-crystallization technique, which can produce kilogram-scale DP microcrystals (DP-MCs) in one batch, is invented to synthesize the Cs2NaxAg1–xInCl6: Bi (x = 0, 0.2, 0.4, 0.6, 0.8, and 1) DP-MCs. The structure and composition analysis confirmed the products are pure Cs2NaxAg1–xInCl6 DP-MCs. Affected by Jahn–Teller distortion of AgCl6 octahedra, self-trapped excitons appear in the excited state, resulting in the broadband emission (400–850 nm) of Cs2Ag1–xNaxInCl6: Bi DP-MCs. The enhancement of the photoluminescence quantum yield can be realized by introducing Na+ to break the parity-forbidden transition in the Cs2AgInCl6 DP. Optimized Cs2Na0.4Ag0.6InCl6: Bi DP-MC phosphors combined with commercial blue and green phosphors were coated on ultraviolet chips (365 nm) to fabricate white light-emitting diodes (WLEDs) from warm white (2930 K) to cold white (6957 K). An ultrahigh color rendering index of 97.1 and a CCT of 5548 K as well as Commission Internationale de l’Eclairage color coordinates of (0.331, 0.339) have been demonstrated. This kilogram-scale synthesis technique could stimulate the industrial development of WLEDs for general lighting based on DP-MC phosphors.
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PHYSICA B-CONDENSED MATTER
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2022
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IF 2.988
Bing Wang,Yingdu Liu,Zhiliang Deng,Pei Li,Wanfu Wang,Xiaoping Ouyang,Qiang Xu
Despite the excellent properties of perovskite materials, the strict oxygen-free atmosphere, heating temperature and a large number of toxic solvents applied during preparation obstruct their more widespread applications. Using ethanol as a green anti-solvent to successfully prepare a series of copper-based perovskite micro-phosphors. They have a luminescence peak between 445 nm and 580 nm adjusted with halogen and the highest PLQY of 81.6%. Moreover, by simply adjusting the molar ratio of CsI to CuI, white-light emission phosphors can be synthesized in one step. It exhibits a Commission Internationale de L'Eclairage (CIE) chromaticity coordinates (0.35, 0.35) and a correlated color temperature (CCT) of 4798 K. After two months of storage, there is still 97.4% of the initial light intensity . This technology offers a green and straightforward method for producing perovskite phosphors.
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Nanoscale Horizons
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2022
·Vol. 7
·期 4
·368-375
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IF 11.684
Zibo Li,Qian Liu,Deliang Zhang,Yin Wang,Yuge Zhang,Qiang Li,Mingdong Dong
Despite the extensive studies conducted in exploring friction in the aqueous environment, the mechanism of hydration friction remains not well understood. Herein, we directly probed hydration friction on mica-electrolyte interfaces with different hydrated alkali cations through a combination of three-dimensional atomic force microscopy and friction force microscopy. The atomic scale imaging of the hydration layers at the mica surface in different electrolyte solutions clearly revealed a correlation between the alkali cations and the structure of the hydration layers. Our detailed analysis showed that the hydration force was much higher at high ionic concentrations than that at low concentrations. The hydration friction coefficient was found to follow the trend K+< Na+< Li+< Cs+, which contrasts with the Hofmeister series, indicating that the hydration friction depends not only on the hydration strength of the alkali cations but also on the arrangement of the alkali cations at the interface. The results of this study provide deep insights into the origins of hydration friction, with potential implications for the development of new boundary lubrication in aqueous media.
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Advanced Science
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2022
·Vol. 9
·期 9
·2105278
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IF 17.521
Feika Bian,Lingyu Sun,Hanxu Chen,Yu Wang,Li Wang,Luoran Shang,Yuanjin Zhao
Information security occupies an important position in the era of big data. Attempts to improve the security performance tend to impart them with more additional encryption strategies. Herein, inspired by the wettability feature of Stenocara beetle elytra and signal model of traffic light, a novel array of perovskite nanocrystals (PNs)-integrated PhC microsphere for information security is presented. The photoluminescent PNs are encapsulated in angle-independent PhC microspheres to impart them with binary optical signals as coding information. Through the multimask superposition approach, PNs-integrated PhC microspheres with different codes are placed into fluorosilane-treated PDMS substrate to form different arrays. These arrays could converge moisture on PhC microspheres in wet environment, which avoids the ions loss of the PNs and effectively prevented mutual contamination. In addition, the fluorescence of the PNs inside PhC microspheres could reversibly quench or recover in response to the environmental moisture. Based on these features, it is demonstrated that the PNs-integrated PhC microsphere arrays could realize various information encryption modes, which indicate their excellent values in information security fields.
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Advanced Science
·
2022
·Vol. 9
·期 7
·2103724
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IF 17.521
Xingwen Cheng,Zhi Xie,Wei Zheng,Renfu Li,Zhonghua Deng,Datao Tu,Xiaoying Shang,Jin Xu,Zhongliang Gong,Xingjun Li,Xueyuan Chen
Fundamental understanding of the effect of doping on the optical properties of 3D double perovskites (DPs) especially the dynamics of self-trapped excitons (STEs) is of vital importance for their optoelectronic applications. Herein, a unique strategy via Cu + doping to achieve efficient STE emission in the alloyed lead-free Cs 2 (Ag/Na)InCl 6 DPs is reported. A small amount (1.0 mol%) of Cu + doping results in boosted STE emission in the crystals, with photoluminescence (PL) quantum yield increasing from 19.0% to 62.6% and excitation band shifting from 310 to 365 nm. Temperature-dependent PL and femtosecond transient absorption spectroscopies reveal that the remarkable PL enhancement originates from the increased radiative recombination rate and density of STEs, as a result of symmetry breakdown of the STE wavefunction at the octahedral Ag + site. These findings provide deep insights into the STE dynamics in Cu + -doped Cs 2 (Ag/Na)InCl 6 , thereby laying a foundation for the future design of new lead-free DPs with efficient STE emission.
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ADVANCED FUNCTIONAL MATERIALS
·
2022
·Vol. 32
·期 21
·2112717
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IF 19.924
Yi-Ming Zhao,Lin Cheng,Kai-Yao Wang,Xin Hao,Juan Wang,Jia-Ying Zhu,Meng Sun,Cheng Wang
Switchable coadsorption and separation for elimination/partitioning of Cs + and Sr 2+ is achieved by pH-controlled ion exchange using a potassium thioantimonate K 2 Sb 4 S 7 ·2H 2 O ( SbS-1K ) with fantastic pH durability from diluted NaOH (pH 12) to concentrated HCl (3 m ). At pH 6, SbS-1K exhibits ultrafast adsorption kinetics ( R ≈ 90% in 2 min for Cs + and 20 min for Sr 2+ ) and high removal rates ( R ≈ 98–99%) at equilibrium for both Cs + and Sr 2+ . At pH 2, the Sr 2+ adsorption is inhibited by H + with a great loss in R Sr to 11.18%, whereas the R Cs remains at 96.99%, contributing to a top-ranked separation factor SF Cs/Sr of 256. The SbS-1K -filled ion exchange column can be switched between the eliminating ( R Cs > 99.91%; R Sr > 98.19%) and separating ( R Cs > 98.99%; R Sr ≈ 0±3%) modes for treating continuous flow with a variation from pH 6 to pH 2 or vice versa. The SbS-1K /PTFE membrane exhibits coadsorption and separation effects for filtration of low concentrated mixed Cs + and Sr 2+ solution (1 ppm for each), even at an ultrafast vacuum filtration speed (30 mL min –1 ). Combined with easy synthesis and high β/γ irradiation resistance, SbS-1K represents a new-concept bifunctional exchanger with discriminating intelligence for equipment innovation.
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