CHEMISTRY OF MATERIALS
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2022
·
IF 10.508
Jingheng Nie,Bo Zhou,Shaofan Fang,Haizhe Zhong,Henan Li,Yumeng Shi
Inorganic lead-free halide perovskites with a broad-band emission of self-trapped excitons (STEs) have attracted great attention in lighting applications. However, it remains a fundamental challenge to expand the display color gamut because it is difficult to individually tune the emitting proportion at different wavelengths. Herein, we employ a doping route to incorporate Sb3+, Er3+, and Ho3+ ions into the Cs2NaInCl6, which enables multicolor emissions with narrow full width at half-maxima and high photoluminescence quantum yields (PLQYs). The blue emission (445 nm) originates from STEs in the [SbCl6]3– octahedrons, while the narrowband green (550 nm) and red (655 nm) emissions are mainly derived from the Er3+ and Ho3+ ions, respectively. An efficient energy transfer between multiple luminescent centers is the key point to achieve such an efficient and tunable emission. By controlling the lanthanide doping level, the emission color can be systematically modulated, and cold 10401 K (0.278, 0.286) to warm 4608 K (0.347, 0.298) adjustable white-light emission (PLQY of ∼70%) can be achieved successfully. The results provide inspiration for the material design of lead-free perovskites with efficient and tunable light-emitting properties for optoelectronic applications.
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CHEMOSPHERE
·
2022
·
IF 8.943
Zhenzhen Jiang,Gaoling Liu,Chi Ma,Yafei Guo,Ji Duo,Mingli Li,Tianlong Deng
Efficient and quick removal of radioactive Cs + from wastewater is significant for the safe use of nuclear energy and human health. A novel adsorbent K 1.93 Ti 0.22 Sn 3 S 6.43 (KTSS) was developed for Cs + removal from complex natural water systems. The working mechanism of KTSS for removing Cs + was the synergistic effect of ion exchange and the Cs⋯S binding, which was proved by several characterization techniques. KTSS showed ultrafast kinetics for Cs + adsorption within 1 min with a removal rate of 99%. Meanwhile, KTSS exhibited a higher adsorption capacity of 450.12 mg/g than many other adsorbents to remove Cs + and possessed excellent chemical stability in a wide pH range of 3–12. Thanks to the natural affinity arising from the S 2− ligands, KTSS displayed excellent selectivity for Cs + even in different complex water systems. The separation factors between Cs + and the coexisting ions of Na + , K + , Mg 2+ , Ca 2+ were ranged from 408.61 to 7448.20. Fortunately, by eluting with NaNO 3 the adsorbent could realize the green regeneration and cyclic utilization. Furthermore, it was found that KTSS had tremendous advantages in the removal of Cs + in comparison with the other adsorbents. Consequently, it should be considered that KTSS obtained in this study has great potential in applying ultrafast and high-efficient removal of Cs + from wastewater.
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2022
·Vol. 331
·期 7
·2919-2928
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IF 1.754
Jiang Yuqi,Gao Shuaibo,Li Peng,Ma Yongsong,Yin Huayi,Wang Dihua
The waste LiCl–Li 2 O oxide reduction salt was solidified and transformed into sodalite by the spark plasma sintering method. Compared with traditional solidification method, SPS operates at a lower pressure, lower temperature, shorter processing time, and without sintering additive. The SPS-solidified sodalite presents a low porosity of 0.37% and low leaching rates of 2.21 g m –2 d –1 for Cs, 3.05 × 10 –1 g m –2 d –1 for Ba, and 3.12 × 10 –1 g m –2 d –1 for Sr. Overall, the SPS is a promising method to solidify various waste OR salts.
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Advanced Optical Materials
·
2022
·Vol. 10
·期 17
·2200930
·
IF 10.05
Fei Xu,Xiang Wang,Yue Li,Beng Jiang,Zuoru Dong,Zichen Yang,Jiaxing Kang,Xin Shu,Zuimin Jiang,Feng Hong,Run Xu,Zhongquan Ma,Teng Chen,Zhan Xu,Haitao Xu
Corrugated 2D antimony-halide perovskites such as Cs 3 Sb 2 Cl 9 (CSC) are promising candidates for single-source white-light emission due to their ultra-broadband spectra. However, CSC has a serious luminescence quenching phenomenon due to inadequate confinement of excitons. By the homovalent substitution of trivalent antimony cation Sb 3+ by a small amount of trivalent rare earth (RE) cations RE 3+ , the photoluminescence intensities from high-quality Cs 3 (Sb 1− x RE x ) 2 Cl 9 (CSRC) (RE = Ce, Sm, Nd, Y, Er, etc.) films at room temperature (RT) are over two orders of magnitude higher than that of CSC film. Especially, the photoluminescence quantum yield (PLQY) for the Cs 3 (Sb 0.995 Er 0.005 ) 2 Cl 9 film is 9.5% at RT, which is much higher than A 3 B 2 X 9 perovskites previously reported for single-source white-light lighting. Furthermore, the Cs 3 (Sb 0.995 Er 0.005 ) 2 Cl 9 film exhibits an ultra-broadband emission with the full width at half maximum reaching 554 meV at RT, resulting in a “warm” white-light with the CIE coordinate (0.33, 0.46) and the correlated color temperature of 5450 K. The PLQY enhancement can be considered as the fact that a high activation energy by bandgap widening effect and Type-I-like “straddling” band alignment between Cs 3 Sb 2 Cl 9 and Cs 3 Er 2 Cl 9 lead to reducing nonradiative losses and increasing radiative recombination channels. Meanwhile, the spectral broadening can be considered to be attributed to strong effect of electron–phonon interaction.
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Yongchuan Wu,Jitao Chen,Zhongmin Liu,Ping Na,Zhibin Zhang
Removing trace radioactive 137 Cs from aquatic system is still a challenge. Herein, Zirconium Titanium Phosphate (ZTP) was prepared and utilized for Cs removal from seawater. The structure and morphology of ZTP were systematically characterized. ZTP exhibited typical feature of tetravalent metal acid, and the surface was pocked with abundant hydroxyl groups which can reacted with H 2 O to form exchangeable protons. Bench-scale to pilot-scale adsorption was carried out to assess Cs removal capacity and rate. ZTP showed a good adsorption performance for Cs + especially at trace concentration (500 ppb) and the removal rate in deionized water and seawater were 98.8 % and 83.9 %, respectively. Radioactive experiments were conducted to test the selective removal of 137 Cs + and the removal rates reached 98.3 %. Slurry-bed adsorption device was designed and used as the pilot-scale equipment. The removal rate was as high as 92.7 % after 12 cycles, indicated that ZTP is one of the promising adsorbents in industrial application. Pyridine adsorption IR spectra indicated that surface of ZTP was riddled with Brønsted and Lewis acid sites, and the protons at the Brønsted acid site exchanged with Cs + . This work will provide reference for the treatment of large-scale Cs-contaminated wastewater.
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DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 26
·10029-10035
·
IF 4.569
Xiaoxia Liu,Weibing Zhang,Rui Xu,Jiayu Tu,Guoyong Fang,Yuexiao Pan
Lead-free zero-dimensional (0D) perovskite nanocrystals (NCs) with isolated octahedral structures have attracted considerable attention due to their unique photoelectric properties, such as highly efficient emissions with broadband features. A series of phosphors composed of Sb3+-doped 0D perovskite crystals Cs3ZnCl5 with wavelength-tunable emission spectra have been obtained using a facile recrystallization method at room temperature in air. By controlling the doping concentration of Sb3+ in Cs3ZnCl5 lattice, bright emissions from red to orange have been achieved under excitation at 320 nm due to the expansion of the crystal lattice, and the emission excited at 275 nm is bluish-white, spanning the full visible region. Inductively coupled plasma emission spectrometry (ICP) demonstrates the Sb3+ substitutes for Zn2+ rather than Cs+ due to the similar charges and ionic radii. The luminescence performance of phosphor Cs3ZnCl5:Sb3+ can be improved obviously by replacing 3 mol% of Cs+ with Rb+ or K+ due to the further distortion of the crystal lattice. The present approach allows the synthesis of large-scale emissive lead-free 0D perovskites activated by Sb3+ with tunable luminescence color.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
·
IF 4.326
Yujing Chi,Yuan Xu,Chenxiang Xu,Jiming Tian,Ying Li,Boxiang Gu,Haiyan Song,Han Zhang
Selective removal of 137Cs from nuclear wastewater is still a challenge due to the issues of efficient adsorbent exploitation and high concentrations of competitive ions. In this study, two-dimensional-layered Mxene Ti3C2Tx achieved the surface alkaline modification with KOH to be used as an efficient adsorbent for Cs+ removal from model wastewater. Hydroxyl-modified Ti3C2Tx obtained improved the delamination morphology and surface structure compared with the pristine Ti3C2Tx. In addition, the F species in Ti3C2Tx were efficiently removed and the hydroxyl groups were increased after modification. The adsorption efficiency of Cs+ over the hydroxyl-modified Ti3C2Tx was significantly enhanced, being attributed to the improvements in morphology, structure, and properties. 0.05 g of an optimal adsorbent achieved 90% removal of Cs+ with 5 mg·L–1 initial concentration in 50 mL of model wastewater within 5 min at ambient temperature and neutral conditions. Hydroxyl-modified Ti3C2Tx also exhibited high adsorption selectivity for Cs+ in the presence of competitive metal ions such as K+, Na+, Mg2+, and Ca2+. The mechanism study revealed that the ion exchange between [Ti–O]−H+/Cs+ mainly contributed to Cs+ adsorption, and the complexation between the oxygen-containing groups [Ti–O] in modified Ti3C2Tx and Cs was also involved. The hydroxyl-modified Ti3C2Tx was easy to regenerate and exhibited good recyclability for Cs+ adsorption.
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Advanced Optical Materials
·
2022
·Vol. 10
·期 21
·2201053
·
IF 10.05
Xiao-Kai Gong,Lan Li,Jian-Ping Xu,Ru-Kun Ding,Zhao-Wei Zhang,Qian Li,Long Liu,Xiao-Song Zhang
Lead-free halide double perovskites continue to draw increasing attention in view of their nontoxicity and stability compared to lead-based perovskites. High-end full-color displays and white light illumination are based on blue-light excitation. However, the excitation of blue light of lead-free halide double perovskites Cs 2 AgInCl 6 at room temperature faces a great challenge, which is crucial to its commercial application. In this study, Cs 2 Ag 0.6 Na 0.4 In 0.8 Bi 0.2 Cl 6 / x KBr(KI), which can be excited under blue light, have been synthesized by solid-phase compression method. Under blue-light excitation, Cs 2 Ag 0.6 Na 0.4 In 0.8 Bi 0.2 Cl 6 /16KBr and Cs 2 Ag 0.6 Na 0.4 In 0.8 Bi 0.2 Cl 6 /16KI emit 605 nm orange light and 665 nm red light, respectively. Based on that, orange and red light-emitting devices are fabricated excited by blue light. The performance of blue-light excitation can not only make the double perovskites widely used in light-emitting devices, but also as a light-emitting down-shift layer in photovoltaic devices to improve the performance of photovoltaic modules. With the Cs 2 Ag 0.6 Na 0.4 In 0.8 Bi 0.2 Cl 6 /16KBr, the power conversion efficiency of the Si solar cell increases 4.80% and 8.14% under the sunlight and white light-emitting devices, respectively. The blue-light excitation of lead-free double perovskites at room temperature offers greater development potential in the field of display devices and optoelectronics.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
·
IF 4.326
Jiashu Liu,Shengnan Zhao,Song Song,Haifeng Cong,Wei Luo,Tong Ding,Ye Tian,Xingang Li
One-step lactide (LD) synthesis from lactic acid (LA) is a promising method for an economically viable polylactic acid (PLA) industry. However, this synthesis is based on a highly water-sensitive esterification reaction, and few studies focus on developing an efficient method to improve its activity by water removal from the reaction environment. Herein, we report a new strategy coupling salt-promoted toluene–water phase separation with heteroazeotropic distillation to enhance water removal to realize highly efficient LD synthesis. Different kinds of chloride salts (LiCl, NaCl, CsCl, MgCl2, and CaCl2) were selected to study their influence on the reaction. The highest yield of LD (84.7%) was obtained when CaCl2 was added, much higher than that of the salt-free reaction (72.3%). Hydrated Ca2+ cations with relatively large charge number and small radius can efficiently reduce the solubility of water in toluene due to their strong electrostatic force to attract more water molecules. Mechanism studies demonstrate that the increased yield of LD after adding CaCl2 was attributed to its significant inhibition of LD hydrolysis resulting from the deep water removal from the toluene solvent.
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ANALYTICA CHIMICA ACTA
·
2022
·
IF 6.911
Yiyi Liu,Fangling Wu,Jiabin Wang,Ling Pu,Chuan-Fan Ding
The separation of chiral amino acids (AAs) and their derivatives has always been a research difficulty in the field of biochemistry due to the high similarity of enantiomeric structures. In this work, a simple and quick method using natamycin (Nat) as chiral selector has been developed to simultaneously separate chiral AAs and their derivatives of carbobenzoxy/benzyl-AAs (Cbz/Bzl-AAs) by trapped ion mobility spectrometry-mass spectrometry (TIMS-MS). Specifically, 12 groups of the Cbz-AAs and Bzl-AAs can get baseline mobility separation by simple mixing with Nat to form binary diastereomeric complex ions [Nat+(Cbz-D/L-AA)+H] + and [Nat+(Bzl-D/L-AA)+H] + . While for the remained 5 groups of Bzl-D/L-AAs and 16 groups of D/L-AAs with unsatisfying separation, by further adding P-toluenesulfonic acid (PTS), the formed ternary complexes can allow their baseline chiral separation . Specifically, Bzl-D-AAs and Bzl-L-AAs get much improved separation effect by the formed diastereomeric complexes of [Nat+(Bzl-AA) 2 +PTS 2 +H] + , which the R p-p was improved from 0 to 2.40; while the D/L-AAs can get baseline separation by the formed diastereomeric complexes of [Nat + AA + PTS + H] + , [Nat + AA+(PTS) 2 +H] + , and [Nat+(AA) 2 +(PTS) 2 +H] + , with the R p-p ranged from 0.44 to 3.53. Definitely, PTS is the first time reported as the ligand to improve the separation effect for the enantiomers, and with the higher assembly of chiral analyte, Nat, and PTS might enable better chiral separation for the chiral amino acid and their derivatives. Moreover, method validation of relative quantification and accuracy for the D/L-AA and their derivatives were measured in a mixture, yielding R 2 greater than 0.99 and RSD% ≤ 2.68%. Overall, Nat and PTS as chiral selector and ligand can be widely used for chiral AAs and their derivatives mobility separation, and potentially for the separation of other AA-related chiral molecules.
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RESOURCES CONSERVATION AND RECYCLING
·
2022
·
IF 13.716
Shangqing Chen,Yanan Dong,Honghong Wang,Jingjing Sun,Junfeng Wang,Suojiang Zhang,Haifeng Dong
The selective and efficient cesium recovery from natural brines resources is a significant and challenging issue. Here we reported a green method for the facile construction of mesoporous Prussian blue analogs (PB) through an ionic liquid-assisted strategy and used for cesium recovery from salt lake brines and geothermal water. The unique nanostructures endowed this mesoporous PB with the improved cesium adsorption capacity (548.7 mg/g), which was 1.5-times as that of conventional PB (362.8 mg/g), placing it at the top level of cesium adsorbents. The adsorption experiments in salt lake brines and geothermal water were conducted and the adsorption efficiency of Cs + exceeded 90%, while those for other co-existing cations were <4.2%, demonstrating its favorable selectivity in cesium recovery from multicomponent aqueous solutions. The benign adsorption performance and adsorption-desorption stability make it a potential candidate for the sustainable recovery of cesium from different kinds of Cs-containing water resources.
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JOURNAL OF MOLECULAR LIQUIDS
·
2022
·
IF 6.633
Zhuanfang Jing,Yongquan Zhou,Wenqian Zhang,Toshio Yamaguchi,Koji Yoshida,Guangguo Wang,Li Han
Wide angle X-ray scattering (WAXS) and density functional theory (DFT) were employed to study the structures of aqueous 18-crown-6/CsCl solutions with CsCl concentrations of 0.25, 0.50 and 1.00 mol·L -1 . The empirical potential structure refinement (EPSR) modelling was adopted to get the pair distribution functions (PDFs), coordination numbers ( CN ), coordination number distributions (CND), angle distribution functions (ADFs), independent gradient model (IGM) and spatial density functions (SDFs) for the 18-crown-6 hydration, the complexation of 18-crown-6 and Cs + , the hydration of 18-crown-6/Cs + complex, and the association of Cl - and 18-crown-6/Cs + complex. Judging from the distance and orientation of water molecules, and the IGM between 18-crown-6 and water molecules, the oxygen atoms of 18-crown-6 (Oc) and the hydrogen atoms of water molecules (Hw) form strong hydrogen bonds, and these water molecules were distributed on both sides of the 18-crown-6 ring plane. However, the hydrogen atoms of 18-crown-6 (Hc) hardly form hydrogen bonds with the oxygen atoms of water molecules (Ow). Cs + is located directly above the 18-crown-6 ring plane of 0.35 to 2.05 Å away from the centroid of 18-crown-6, and forms 18-crown-6/Cs + complex with six Oc at r Cs + - O c = 3.06 Å. When the concentrations of CsCl are 0.25, 0.50 and 1.00 mol·L -1 , the complexation percentage of 18-crown-6 to Cs + are about 100%, 58% and 54%, respectively. No classic 2:1 “sandwich” 18-crown-6/Cs + complex structure was found in the solutions we surveyed. Both interaction energies and solvation stability energies reveal that the hydrates of 18-crown-6/Cs + complexes were formed in aqueous solutions. Cs + uncomplexed with 18-crown-6 hydrates with eight water molecules in aqueous solution, while Cs + can also hydrate with about four water molecules when it complexes with 18-crown-6. The results of atomic pair distances, the dipole distance of water molecules, the SDF and the IGM indicate that although water molecules can be located on both sides of the 18-crown-6 ring plane when the hydrates are formed, they hydrate with Cs + on the side where Cs + only existed. Cs + of 18-crown-6/Cs + complex associates with Cl - with the r Cs + - Cl - = 3.79 Å by electrostatic attraction.
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