Journal of Cleaner Production
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2024
·
IF 9.7
Qina Sun,Mengzhou Wang,Yujia Yang,Jinshan Song,Junfeng Li,Qingrui Zhang
Commonly used polyoxometalate (POM) adsorbents exhibit high cesium (Cs) adsorption capacity. However, its impotent ability to sequester adsorbates poses a risk of Cs migration in radioactive waste decontamination and disposal. By leveraging the cesium affinity of POMs and the regulatory properties of ionic liquids (ILs), POM-IL composites hold promise for mitigating the risk of cesium migration through efficient adsorption and retention. Herein, we designed two POM-ILs composed of the phosphotungstate anion (PW) and tetrabutylammonium cation (TBA), i.e., the {WO 6 }-saturated TBA-PW 12 and mono-lacunary TBA-PW 11 , for the capture and retention of aqueous Cs. The composites were then characterized, and the performance and mechanism of Cs uptake were investigated. TBA-PW 12 exhibited ∼300 nm aggregate of particles around 20–60 nm. TBA-PW 12 retained the Keggin structural features of PW 12 O 40 3− , which was proven essential for the binding of Cs + . With a retention efficiency of 97.3% in an NH 4 Cl eluent and a maximum adsorption capacity of 400.9 mg/g at 338 K, TBA-PW 12 exhibited superior Cs capture and retention compared to the POM-IL derived from common Cs adsorbent phosphomolybdate. The Cs adsorption onto TBA-PWs achieved equilibrium within 180 min. Cs uptake by TBA-PWs was monolayer chemisorption of Cs + accompanied by H + release, and the removal efficiencies stabilized around initial pH 5–10. Due to intense affinity between {WO 6 } and Cs + , TBA-PW 12 efficiently sequestered Cs + through {WO 6 } octahedra so that the {WO 6 }-saturated TBA-PW 12 presented better Cs uptake performance than the mono-lacunary TBA-PW 11 . The IL anion [N(C 4 H 9 ) 4 ] + provided a composite-water biphasic interface for aqueous Cs adsorption, while retaining the ability of POM cation PW 12 O 40 3− to form a stable structure with Cs via its affinity to {WO 6 } octahedra. These findings support the design of POM-IL composites as efficient adsorbents for capturing and retaining Cs, aiding in the decontamination and safe disposal of radioactive waste, thereby minimizing the risk of nuclide leakage into the environment.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 44
·18890-18899
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IF 2.7
Xuyan Xue,Changshuai Gong,Sihan Yang,Jian He,Meiting Li,Xuejiao Wang
Non-contact optical temperature measurement has attracted intense attention in recent years due to its advantages of high speed and high safety. In this work, a Lu2WO6:Er3+ phosphor was successfully prepared by a solid state reaction. The effective energy transfer from the [WO6]6− group to Er3+ was proved using the emission spectra and fluorescence lifetime measurements, with an estimated transfer efficiency of 51%. Benefiting from the self-luminescence of the [WO6]6− group, optical thermometry was established based on the fluorescence intensity ratio of [WO6]6− emission to Er3+ emission. Remarkably, strong emission color variability from blue to green was observed under 320 nm UV excitation as the temperature increases from 298 K to 548 K, while an opposite trend from green to cyan is observed under 378 nm UV excitation. The maximum relative sensitivity (SR Max) is 3.37% K−1 (298 K), which is highly superior to most of the previously reported values.
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高影响因子
CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Donglei Wei,Jingyi Fang,Jiuhui Bian,Xifeng Yang,Yushen Liu,Bo Ram Lee
Transition metal perovskite oxide is one of the most important functional materials for applications in light energy conversion due to the distinctive structures and characteristics. This work reports self-activated luminescence of Ba 3 WVO 8.5 , a hybrid hexagonal perovskite. Ba 3 WVO 8.5 acts as an indirect allowed transition, with a band gap energy of 3.2 eV. At 300 K, it exhibits a broad self-activated luminescence band peaking at 527 nm, with a decay lifetime of 0.09 μs. There are two distinct intrinsic centers, WO 6 and VO 6 , in the lattices that contribute to the self-activated luminescence. The photoluminescence (PL) and temperature-dependent spectra confirm the energy transfer process from WO 6 to VO 6 centers. The cation substitutions in Ba 3 WVO 8.5 can exert obvious effect on the luminescence efficiency. Especially, the substitution of Ba 2+ by Sr 2+ +Ca 2+ significantly enhances its self-activated luminescence. The maximum quantum efficiency (QE) in Ba 2.7 Sr 0.15 Ca 0.15 WVO 8.5 can reach up to 34 %. Moreover, Ba 3 WVO 8.5 exhibits scintillation characteristics under X-ray irradiation. Its emission efficiency is still significantly lower than that of the commercial Bi 4 Ge 3 O 12 scintillator, but Ba 3 WVO 8.5 shows advantages in QE under UV excitation and in fast decay lifetime. The experimental results may play a valuable role in the development of new luminescent materials and further understanding of the hybrid hexagonal perovskite oxides.
研究领域:
材料科学
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光学材料
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固体物理
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无机化学
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发光学
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DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-10
·
IF 14.7
Zhu Jiawei,Zhang Yu,Chen Zitao,Zhang Zhenbao,Tian Xuezeng,Huang Minghua,Bai Xuedong,Wang Xue,Zhu Yongfa,Jiang Heqing
Cu-oxide-based catalysts are promising for CO 2 electroreduction (CO 2 RR) to CH 4 , but suffer from inevitable reduction (to metallic Cu) and uncontrollable structural collapse. Here we report Cu-based rock-salt-ordered double perovskite oxides with superexchange-stabilized long-distance Cu sites for efficient and stable CO 2 -to-CH 4 conversion. For the proof-of-concept catalyst of Sr 2 CuWO 6 , its corner-linked CuO 6 and WO 6 octahedral motifs alternate in all three crystallographic dimensions, creating sufficiently long Cu-Cu distances (at least 5.4 Å) and introducing marked superexchange interaction mainly manifested by O-anion-mediated electron transfer (from Cu to W sites). In CO 2 RR, the Sr 2 CuWO 6 exhibits significant improvements (up to 14.1 folds) in activity and selectivity for CH 4 , together with well boosted stability, relative to a physical-mixture counterpart of CuO/WO 3 . Moreover, the Sr 2 CuWO 6 is the most effective Cu-based-perovskite catalyst for CO 2 methanation, achieving a remarkable selectivity of 73.1% at 400 mA cm −2 for CH 4 . Our experiments and theoretical calculations highlight the long Cu-Cu distances promoting *CO hydrogenation and the superexchange interaction stabilizing Cu sites as responsible for the superb performance.
研究领域:
材料科学
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电化学
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催化
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可持续能源
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DOI
PubMed
高影响因子
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