THERMOCHIMICA ACTA
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2025
·
IF 3.5
Shuchang Zhang,Meiqian Chen,Bingyang Li,Yuelong Pan,Linjun Yang
The treatment of spent ion exchange resins (CERs) has become a major concern with the development of nuclear industry. The migration and transformation mechanism of Cs in CERs in both pyrolysis and gasification were evaluated based on chemical equilibrium and experimental analysis. The pyrolysis and gasification temperatures should be limited below 813.15 K and 873.15 K, respectively, but after adding the fixatives, ZrO 2 or Nb 2 O 5 , the temperatures could be extended to 873.15 K, 1233.15 K (ZrO 2 ) or 1153.15 K (Nb 2 O 5 ). The kinetic and thermodynamic characteristics of CERs with metal ion catalysts in the gasification were evaluated based on thermogravimetric analysis. In 10 % O 2 /90 % N 2 , Fe 2+ and Mn 2+ metal nuclides would urge the decomposition of functional groups and polymer matrices, since they could promote the reaction in the second stage and the advance of the third stage. This study could provide basic data for the thermal treatment of CERs.
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高影响因子
CHEMISTRY OF MATERIALS
·
2026
·
IF 7.1
Luyong Zhang,Jianyi Zuo,Guangsheng Xu,Jinbin Fan,Xue Bai,Zhihua Yang,Fangfang Zhang,Shilie Pan
Deep-ultraviolet (DUV) birefringent crystals are essential for modern optical technologies, yet achieving a balance between large birefringence and a wide bandgap remains challenging. Although conventional borosulfates with alternating [BO4] and [SO4] tetrahedra connected by sharing corners possess a wide bandgap, they suffer from small birefringence due to weak optical anisotropy resulting from the presence of only tetrahedral groups. This work introduced advantageous “genes” [BO2(OH)] groups to modify the common [B(SO4)4] supertetrahedra for the first time and ultimately produced two borosulfates, Na3B3S2O11(OH)2 and K3B3S2O11(OH)2, striking the balance. Isolated fundamental building block (FBB) [B3O3(OH)2(SO4)2] was observed in the two compounds. Additionally, three conventional borosulfates featuring isolated [B(SO4)4] supertetrahedra, Na4KB(SO4)4, Na4RbB(SO4)4, and Na3Cs2B(SO4)4, were also obtained for comparison. Structural analysis and theoretical calculations reveal that the directional alignment of [BO2(OH)] groups significantly enhances the birefringence of the borosulfates. The calculated birefringence at 1064 nm increases by approximately 10-fold, specifically from 0.0035–0.0047 for the three conventional borosulfates to 0.043–0.044 for the two hydroxylated ones. This work demonstrates the effectiveness of employing [BO2(OH)] groups in optimizing the optical anisotropy of borosulfates, providing a design paradigm for exploring advanced DUV birefringent materials in borosulfates.
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CHEMISTRY OF MATERIALS
·
2025
·
IF 7
Luyong Zhang,Zhencheng Wu,Jingdong Yan,Shibin Wang,Zilong Chen,Zhihua Yang,Fangfang Zhang,Shilie Pan
Sulfates have remained promising candidates for deep-ultraviolet (DUV) optical crystals owing to the inherently wide bandgaps induced by the [SO4] tetrahedral groups. However, the structural rigidity of [SO4] tetrahedra imposes severe restrictions on the polarization anisotropy, fundamentally preventing sulfates from achieving sufficient birefringence required for regulating light polarization. Herein, by incorporating f0 rare earth metal cation Y3+ into alkali metal sulfates, we synthesized six compounds, AY(SO4)2 and A3Y(SO4)3 (A = K, Rb, Cs). They exhibit dramatically enhanced birefringence between 0.013–0.056 at 546 nm, with up to 25 times that of their parent alkali metal sulfates, which originate from the highly aberrant Y–O polyhedra and the dimensionality reduction of the Y–O–S network regulated by A-site cations. This study provides valuable insights into the further exploration of sulfate-based optical materials.
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CHEMICAL GEOLOGY
·
2022
·
IF 4.685
Hao Cui,Richen Zhong,Zimeng Li,Huan Chen,Chang Yu,Yanxia Li,Yifan Ling
Raman spectroscopy is a crucial technology in geoscience and often employed in in situ quantification experiments to investigate fluid compositions at elevated temperatures. Raman spectroscopic quantification is fundamental to understanding the hydrothermal behaviors of aqueous species, such as SO 4 2− and H 3 PO 4 0 . Considering that SO 4 2− and PO 4 3− are closely associated with metal transportation and deposition, investigating the hydrothermal behaviors of these species, via Raman spectroscopic quantification, can give an assistance for the comprehension of relative ore-forming processes. During Raman spectroscopic quantification, the accuracy of the calibration coefficient ( k ), which bridges the concentration of a species ( C species ) and its Raman peak area ( A normalized ) in the form of C species = k · A normalized , is the key to accurate measurement of fluid composition. For high-temperature experiments, quantification of fluid composition is complicated because the coefficient k varies with varying temperatures. In this study, the temperature dependence of the calibration coefficients is retrieved, based on experiments on solutions containing SO 4 2− and H 3 PO 4 0 using the fused silica capillary capsules. The results show a well-established linear relationship between the k and 1/ T (absolute temperature in Kelvin) for both SO 4 2− and H 3 PO 4 0 . The reported linear k − 1/ T relationship simplifies Raman-based fluid composition investigation at elevated temperatures: the k values throughout the whole temperature range of interest can be retrieved by measuring the room-temperature Raman intensity of a standard sample (i.e., with known composition) and one single data point at high temperature. We speculate that this linear k − 1/ T relationship method may be established for other species (e.g., carbonate ions) and can be applied for experiments using other technics (e.g., hydrothermal diamond anvil cell) or retrieving the compositions of natural or synthetic fluid inclusions . For example, the empirical linear relationship can facilitate the measurements of gas concentrations (e.g., CO 2 ) in natural fluid inclusions .
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Dayi Yang,Jingxiao Liu,Fei Shi,Yi Li,Jiaxiang Wan,Xinyu Yuan,Ziwei Tian,Meiyu Wang,Chuangchuang Ma
Synthesis of cesium tungsten bronze (Cs x WO 3 ) nanorods with excellent near-infrared shielding performance by a one-step solvothermal method from cheap tungsten source is still challenging. In this work, small-sized Cs x WO 3 nanorods with excellent transparent thermal insulation performance were synthesized by a one-step solvothermal method. It was found that halogen acids played an important role in regulating the growth and microstructure of Cs x WO 3 nanorods. Moreover, different halogen acid can regulate the content of W 5+ =O and oxygen vacancies (V O ) in Cs x WO 3 nanorods, which is helpful to further improve the near-infrared shielding performance of Cs x WO 3 particles. Compared with HF and HBr, the Cs x WO 3 nanoparticles synthesized under the regulation of HCl contain more V O s and W 5+ =O content, showing more excellent near-infrared shielding performance, and the as-prepared Cs x WO 3 -PVA composite film exhibits low haze and high transparency, with the near-infrared light shielding rate at 1500 nm attaining to 97.7% when the visible light transmittance is 71.8%. The thermal insulation test results show that the Cs x WO 3 -PVA composite film synthesized under the regulation of HCl can effectively reduce the indoor temperature by 6.9 °C under the irradiation of sunlight. After 100 cycles of thermal insulation tests, the near-infrared shielding and thermal insulation performance have not declined, showing excellent photothermal stability. This work is of great significance for promoting the industrial production of high-performance Cs x WO 3 nanoparticles and its application in energy-saving windows.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2023
·
IF 3.3
Jingxiao Liu,Dayi Yang,Fei Shi,Xiaoying Song,Guohao Cui,Huijun Sun,Chaofan Chen,Ziwei Tian,Meiyu Wang
In order to obtain high-performance energy-saving window material, Pt-Cs x WO 3 /SiO 2 composite aerogels were prepared by in-situ solvothermal synthesis and ambient pressure drying method. The relationship among the near-infrared shielding ability, thermal conductivity , thermal insulation performance and microstructure of Pt-Cs x WO 3 /SiO 2 composite aerogel was investigated. The as-prepared composite aerogel after heat-treatment at 450 °C exhibits low thermal conductivity (0.1090 W/(m·k)) of SiO 2 aerogel and near-infrared shielding ability at the same time due to its high pore volume (0.537–0.796 cm 3 /g), specific surface area (113.968–141.284 m 2 /g) and W 5+ content. The near-infrared shielding rate at 1500 nm of the composite aerogel could attain to 84% when the visible light transmittance is 72%. As Pt-Cs x WO 3 /SiO 2 composite aerogel has the synergistic effect of near-infrared shielding and low thermal conductivity, the composite aerogel heat-treated at 450 °C has excellent visible light transparency and thermal insulation performance. This research provides a new idea for developing high efficient energy-saving window glasses.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-12
·
IF 16.6
Kong Kejian,Li An-Zhen,Wang Ye,Shi Qiujin,Li Jing,Ji Kaiyue,Duan Haohong
Enzymes are characteristic of catalytic efficiency and specificity by maneuvering multiple components in concert at a confined nanoscale space. However, achieving such a configuration in artificial catalysts remains challenging. Herein, we report a microenvironment regulation strategy by modifying carbon paper with hexadecyltrimethylammonium cations, delivering electrochemical carbon–carbon coupling of benzaldehyde with enhanced activity and racemate stereoselectivity. The modified electrode–electrolyte interface creates an optimal microenvironment for electrocatalysis—it engenders dipolar interaction with the reaction intermediate, giving a 2.2-fold higher reaction rate (from 0.13 to 0.28 mmol h −1 cm −2 ); Moreover, it repels interfacial water and modulates the conformational specificity of reaction intermediate by facilitating intermolecular hydrogen bonding, affording 2.5-fold higher diastereomeric ratio of racemate to mesomer (from 0.73 to 1.82). We expect that the microenvironment regulation strategy will lead to the advanced design of electrode–electrolyte interface for enhanced activity and (stereo)selectivity that mimics enzymes.
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高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2023
·
IF 2.6
Yanfei Fan,Ziyu Zhuang,Dandan Gao,Dongdong Li,Dewen Zeng
Solid–liquid phase equilibrium data of the Li2SO4 + Rb2SO4 + H2O and Li2SO4 + Cs2SO4 + H2O systems are of importance for the design of alkali metal element extraction processes from sulfate leaching solution of lepidolite. Considering the serious inconsistency of the reported solid phases, especially double salts and solid solutions, phase diagrams of the two systems were reinvestigated experimentally. The results on the Li2SO4 + Rb2SO4 + H2O system at 298.15 K show five solids, i.e., Rb2SO4, Rb2SO4·Li2SO4, Rb2SO4·3Li2SO4·2H2O, Rb2SO4·5Li2SO4·4H2O, and a solid solution with the end members Rb2SO4·5Li2SO4·4H2O and Li2SO4·H2O. For the Li2SO4 + Cs2SO4 + H2O system at 298.15 K, the results also show five solids, i.e., Cs2SO4, Cs2SO4·Li2SO4, Cs2SO4·3Li2SO4·2H2O, Cs2SO4·5Li2SO4·4H2O, and Li2SO4·H2O, while there is no solid solution phase with the end members Cs2SO4·5Li2SO4·4H2O and Li2SO4·H2O. Moreover, the single crystal structures of Rb2SO4·3Li2SO4·2H2O and Cs2SO4·3Li2SO4·2H2O were determined.
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CHEMICAL GEOLOGY
·
2021
·
IF 4.015
Huan Chen,Richen Zhong,Yuling Xie,Hao Cui,Chang Yu,Yifan Ling,Zimeng Li,Lamei Li
Sulfate-bearing geofluids are widespread in many geological environments and play important roles in ore-forming processes. Recent experiments provide evidences that in silica-rich fluids, Na 2 SO 4 solubility exhibits a complex temperature dependence, first decreasing from 25 to 313 °C and then increasing from 313 to 425 °C. The fluid-borne silica have critical implications for sulfate-bearing hydrothermal systems and formations of rare earth element deposits. However, whether other sulfate salts share the same characteristics remains unknown. In this study, fused silica capillary capsules (FSCCs) containing K 2 SO 4 -saturated solutions and K 2 SO 4 crystals are used to quantitatively investigate the solubility of K 2 SO 4 at different temperatures in the K 2 SO 4 -SiO 2 -H 2 O system. In the K 2 SO 4 -SiO 2 -H 2 O system, K 2 SO 4 shows prograde solubility from 50 to 400 °C, and does not melt through the whole investigated temperature range. The relationship between temperature and the solubility of K 2 SO 4 can be described by a simple linear function with R 2 = 0.991: C sulfate = 4.1307 × 10 −3 × T + 0.5532, where C sulfate and T represent the solubility of K 2 SO 4 in m (mol/kg H 2 O) and temperature in °C, respectively. These results show that the solubility of K 2 SO 4 can be enhanced by 3 to 5 times at 300–400 °C by the presence of silica, compared with that in silica-absent system, even without the formation of sulfate melt. Considering that quartz is ubiquitous in the Earth's crust , the solubility of sulfate in natural geofluids may reach a much higher level than previously expected. The temperature dependences of the solubilities of K 2 SO 4 and Na 2 SO 4 in silica-saturated fluids were used to constrain the compositions of the mineralizing fluids of the synmetamorphic hematite-quartz veins at Ouro Fino (SE Brazil) and the Maoniuping REE deposit (SW China), based on the previously reported microthermometric results of fluid inclusions that contain sulfate daughter minerals. For the hematite-quartz vein at Ouro Fino, the sulfate concentration was calculated to be 8.9–19.2 wt%, which is in line with previous laser ablation measurements (~15.3 wt%). For the Maoniuping REE deposit, the total sulfate concentration was determined to be 16.3–27.4 wt%, and the REE concentration of the ore-fluid was further estimated to be 0.30–0.44 wt%.
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Nanoscale
·
2020
·Vol. 12
·期 10
·6104-6110
·
IF 6.895
Hui Chen,Yuanhang Ge,Sunjie Ye,Zhifeng Zhu,Yingfeng Tu,Denteng Ge,Zhao Xu,Wei Chen,Xiaoming Yang
Hygroresponsive actuators harness minor fluctuations in the ambient humidity to realize energy harvesting and conversion, thus they are of profound significance in the development of more energy-saving and sustainable systems. However, most of the existing hygroresponsive actuators are only adaptive to wet environments with limited moving directions and shape morphing modes. Therefore, it is highly imperative to develop a hygroresponsive actuator that works in both wet and dry environments. In this work, we present a bidirectional actuator responsive to both wet and dry stimuli. Our strategy relies on the introduction of carbon nanotubes to provide transport channels for water molecules. The actuation is enabled by the rapid transport of water in and out of the system driven by the moist/dry surroundings owing to the transport channels. The resultant actuator demonstrates reconfiguration and locomotion with turnover frequency F = 30 min−1, coupled with the capability of lifting objects 6 times heavier and transporting cargos 63 times heavier than itself. Oscillations (24°) driven by dry air flow in a cantilever display a high frequency (2 Hz) and large amplitude. Furthermore, a touchless electronic device was constructed to output varying signals in response to humid and dry environments. Our work provides valuable guidance and implications for designing and constructing hygroresponsive actuators, and paves the way for next-generation robust autonomous devices to exploit energy from natural resources.
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高影响因子
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2020
·Vol. 2020
·期 10
·854-858
·
IF 2.529
Yaoguo Shen,Xiaoling Xue,Wenyuan Tu,Zhiqun Liu,Renwen Yan,Hong Zhang,Junrong Jia
Graphical An ultraviolet-transparent sulfate Cs 2 Ca 2 (SO 4 ) 3 has been synthesized. It exhibits a moderate second harmonic generation efficiency and has good thermal stability higher than those of most nonlinear optical sulfates reported recently. The noncentrosymmetric structure is one prerequisite of a nonlinear optical (NLO) material. Here, a sulfate Cs 2 Ca 2 (SO 4 ) 3 with a noncentrosymmetric structure was synthesized by high-temperature solid-state reaction, and its crystals were grown by spontaneous crystallization. Single-crystal X-ray diffraction indicates that Cs 2 Ca 2 (SO 4 ) 3 features a three-dimensional framework constituted by corner-sharing CaO 6 octahedra and SO 4 tetrahedra. Optical characterizations suggest that Cs 2 Ca 2 (SO 4 ) 3 is transparent down to 200 nm and exhibits a moderate second-order NLO response of about 0.6 × KH 2 PO 4 . Electronic band structure calculations were performed to elucidate the optical origin. Furthermore, the title compound has good thermal stability of up to about 1000 K, which is greatly higher than those of NLO sulfates reported recently. This work may shed useful light on the development of new NLO sulfates with high thermal stability.
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JOURNAL OF CHEMICAL THERMODYNAMICS
·
2019
·
IF 2.29
Yanfei Fan,Dongdong Li,Dandan Gao,Dewen Zeng,Wu Li
Specific heat capacity of Rb 2 SO 4 (aq) and Cs 2 SO 4 (aq) solutions was determined using a Calvet-type calorimeter from 288.15 K to 338.15 K and from about 0.25 mol·kg −1 to concentration near room temperature solubility limits. For both Rb 2 SO 4 (aq) and Cs 2 SO 4 (aq) solutions, the specific heat capacity decreases with the increase of molality at constant temperature. Combining the heat capacity data determined in this study and other thermodynamic properties ( i.e. water activity, osmotic coefficient, mean ionic activity coefficient, enthalpy of dilution and solubility) reported in literature, thermodynamic and phase equilibria properties of the binary Rb 2 SO 4 + H 2 O and Cs 2 SO 4 + H 2 O systems were modelled using a comprehensive thermodynamic framework, in which a Pitzer-Simonson-Clegg model was applied to represent the non-ideality of aqueous phases. The models can represent all the properties over wide temperature and concentration ranges. This study forms a basis for solubility prediction in multi-component systems containing Rb and Cs sulfates.
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