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RADIOCHIMICA ACTA · 2022 · IF 2.083

Targeted synthesis of carbon-supported titanate nanofibers as host structure for nuclear waste immobilization

Lei Li,Ran Ma,Xuewei Liu,Tao Wen,Bo Wu,Mingtai Sun,Zheng Jiang,Suhua Wang,Xiangke Wang

Inorganic ion-exchange materials show potential application for toxic radioactive ions due to their remarkable high efficiency and selectivity features. Here, two type of carbon-supported titanate (C@TNFs and C@TNFs(H)) nanofibers have been synthesized by a cost-effective in suit growth method. The resulting C@TNFs and C@TNFs(H) microspheres present uniform flower-like morphology and large surface area. The interlayer Na + in the titanate shell provides docking sites for ion-exchange of radioactive ions (U(VI), Ba(II), and Sr(II)). Interestingly, the exceeding theoretical cation-exchange capacities (CECs) are achieved on C@TNFs for U(VI) ∼4.76 meq g −1 and Ba(II) ∼2.65 meq g −1 and C@TNFs(H) for Ba(II) ∼2.53 meq g −1 and Sr(II) ∼2.24 meq g −1 , respectively. The impressive adsorption performance is mainly attributed to the synergistic effects of ion-exchange and surface complexation. More significantly, C@TNFs and C@TNFs(H) maintain high distribution coefficients ( K d U ) of >104 mL g −1 over a wider pH range (pH = 3.5–9.0) and high adsorption rate with short equilibrium time within 50 min. Competitive ion-exchange investigation shows a selectivity order of U(VI) > Ba(II) > Sr(II) at individual 10 ppm concentration, pH = 6.0 and T = 298 K. The related spectroscopic studies reveal the intercalative mechanism of radionuclides in the deformed titanate structure, as a result of target ions firmly trapped in the interlayer of C@TNFs and C@TNFs(H). These advantageous features allow the C@TNFs and C@TNFs(H) to be promising candidates for the remediation of toxic radioactive ions polluted water.

研究领域: 材料科学 · 环境科学 · 放射化学
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CERAMICS INTERNATIONAL · 2018 · IF 3.057

Phase evolution, microstructure and chemical stability of Ca1-xZr1-xGd2xTi2O7 (0.0 ≤ x ≤ 1.0) system for immobilizing nuclear waste

Yi-Bing Zhang,Jin Wang,Jun-Xia Wang,Yi Huang,Ping Luo,Xiao-Feng Liang,Hong-Bin Tan

In order to ascertain the structural relationship of zirconolite and pyrochlore for their potential application in HLW immobilization, the Gd-doped zirconolite-pyrochlore composite ceramics (Ca 1- x Zr 1- x Gd 2 x Ti 2 O 7 ) were systematically synthesized with x  = 0.0–1.0 by traditional solid-phase reaction method. The phase evolution and microstructure of the as-prepared samples have been elucidated by XRD and Rietveld refinement , Raman spectroscopy , BSE-EDS and HRTEM analysis. The results showed that zirconolite-2M, zirconolite-4M, perovskite and pyrochlore, four phases were identified in Ca 1- x Zr 1- x Gd 2 x Ti 2 O 7 system and could be coexisted at x  = 0.4 composition. With the increase of Gd 3+ substitution, the phase evolution was followed by zirconolite-2M→zirconolite-4M→pyrochlore. It is illustrated that the phase transformation from zirconolite-2M to zirconolite-4M was promoted by the preferential substitution of Gd 3+ for Ca 2+ . And the solubility of Gd 3+ in zirconolite-2M, zirconolite-4M and pyrochlore increased in sequence. The chemical stability test was also measured by the PCT leaching method. The normalized elemental release rates of Ca, Zr, Ti and Gd in Ca 1- x Zr 1- x Gd 2 x Ti 2 O 7 system were fairly low and in the range of 10 −6 −10 −8 g m −2 d −1 , which indicated a potential ceramics composite ensemble of CaZrTi 2 O 7 -Gd 2 Ti 2 O 7 system for nuclear HLW immobilization.

研究领域: 材料科学 · 核能工程 · 化学
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CERAMICS INTERNATIONAL · 2019 · IF 3.45

Liquid–solid–solution synthesis of ultrafine Gd2Zr2O7 nanoparticles with yield enhancement

Yao Yang,Zhangyi Huang,Chen Shi,Junjing Duan,Gang Cheng,Haomin Wang,Di Wu,Jianqi Qi,Tiecheng Lu

A modified l iquid–solid–solution (LSS) phase transfer method has been applied to synthesize Gd 2 Zr 2 O 7 binary oxide nanoparticles . X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), transmission electron microscopy (TEM), thermogravimetric analysis (TG) and differential scanning calorimetry (DSC) were employed to reveal the structural, morphological and energetic evolutions of both precursors and Gd 2 Zr 2 O 7 nanoparticle products. The Gd 2 Zr 2 O 7 nanoparticles synthesized using this method exhibit an average crystallite size of 1.7 nm, which have great potential to be applied in thermal barrier coatings (TBCs), solid oxide fuel cells (SOFCs) and nuclear waste immobilizations. Moreover, the method we developed in this study has a high Gd 2 Zr 2 O 7 nanoparticle yield of up to 89%.

研究领域: 材料科学 · 纳米技术
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CERAMICS INTERNATIONAL · 2024 · IF 5.1

Phase evolution, solubility and substitution behavior of CaZrTi2O7–Ho2Ti2O7 ceramics for potential nuclear waste immobilization

Xiuhua Ji,Yanhao Song,Jiarun Wang,Yi Ding,Shiyin Ji,Tao Duan

Zirconolite and pyrochlore have been considered as the potential immobilization matrix materials of minor actinides due to their high solubility, radiation tolerance and chemical durability. In this work, a series of Ca 1-x Ho 2x Zr 1-x Ti 2 O 7 (0.1 ≤ x ≤ 1.0) ceramics were prepared by solid state synthesis and sintering at 1400 °C for 48 h twice. Powder X-ray Diffraction (XRD), Backscattered Scanning Electron Microscopy with Energy-Dispersive X-ray spectroscopy (BSEM-EDX), Transmission Electron Microscopy (TEM) were employed to investigate the phase evolution, solubility, and substitution mechanism of Ho. The results displayed that zirconolite-2M would be transformed to zirconolite-4M and then to pyrochlore with increasing Ho concentration. The initial phase transformation of zirconolite-2M to zirconolite-4M, subsequently zirconolite-4M to pyrochlore were observed in x = 0.2 and 0.4 samples, respectively. Zirconolite-4M could be synthesised at x = 0.38 sample with trace perovskite. Moreover, the semi-quantitively solubility limits of Ho in zirconolite-2M and zirconolite-4M were determined to be 27 and 41.5 at.%, respectively. Single-phase pyrochlore were fabricated after 70 at.%. In addition, the novel substitution mechanism was revealed by Rietveld refinement with Ho preferentially replacing the Ca of zirconolite-2M so that some replaced Ca occupied vacant Zr site. For pyrochlore, Ho, Ca and Zr occupied A site (16d) and Ti entered in B site (16c). The findings would provide more insights into zirconolite–pyrochlore ceramic system.

研究领域: 材料科学 · 核化学与放射化学
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Journal of Cleaner Production · 2023 · IF 11.1

Insight into immobilization mechanism of nuclear waste management by granite: Impact of waste chemical species

Guilin Wei,Shuaipeng Chen,Fen Luo,Xiaoyan Shu,Mingfen Wen,Yuexiang Lu,Wenhong Han,Jing Chen,Haijiao Xie,Faqin Dong,Xirui Lu

Nuclear waste immobilization is one of the ways to alleviate the harm of radioactive waste produced in the nuclear field to human beings and the environment. In the current study, granite was utilized as a substrate material for the immobilization of simulated radioactive waste. Based on the obtained results, the relationship between the waste chemical species and the physicochemical properties , such as solid-solubility of waste, infrared, density and leaching data, was systematically studied as well. The findings indicate that the granite substrate used for the immobilization of the simulated waste (Nd 2 O 3 ) exhibits a solid-solubility limit of 27 wt%. When the added content of waste is below 27 wt%, all Nd elements are immobilized into the glassy phase . However, when the waste content exceeds 27 wt%, in addition to being immobilized in the glassy phase, the presence of Nd 2 O 3 reacted with Ca 3 Si 3 O 9 to form Ca 2 Nd 8 (SiO 4 ) 6 O 2 . As the Nd 2 O 3 content increased from 20 wt% to 25 wt%, the microstructures related to Si-, Al-, and Fe-are more involved in the immobilization of waste. However, the appearance of Ca 2 Nd 8 (SiO 4 ) 6 O 2 and Nd 2 O 3 makes the density and Vickers hardness of the matrix not increase further. The maximum density and hardness values are 3.17 g cm −3 and 7.88 GPa, respectively. The leaching results show that the cured body has good anti-leaching performance ( L R Nd  = ∼10 −6  g cm −2  d −1 ). Finally, the comparison of vacancy formation energy of Nd in Nd 2 O 3 and Ca 2 Nd 8 (SiO 4 ) 6 O 2 proved that the formation of Ca 2 Nd 8 (SiO 4 ) 6 O 2 is beneficial to the immobilization of simulated waste. This study provides a certain reference for the selection of nuclear waste solidification substrates. This kind of granite material from nature has the potential advantages of low cost and better immobilization effect on waste, and may be more suitable for the treatment of radioactive waste in the future.

CAS / MDL: 1313-97-9
研究领域: 材料科学 · 环境科学 · 核能工程
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JOURNAL OF WUHAN UNIVERSITY OF TECHNOLOGY-MATERIALS SCIENCE EDITION · 2021 ·Vol. 36 ·期 2 ·196-202 · IF 0.957

Self-propagating High-temperature Synthesis of Sm and Zr Co-doped Gd2Ti2O7 Pyrochlore Ceramics as Nuclear Waste Forms

Xie Dayan,Zhang Kuibao,Li Weiwei,Luo Baozhu,Guo Haiyan

We reported a rapid synthesis of Sm 3+ /Zr 4+ co-doped Gd 2 Ti 2 O 7 pyrochlore simulated nuclear wastes solidification by self-propagation plus quick pressing technique. With increment excess contents of Sm 2 O 3 and ZrO 2 from 0 to 10wt%, the phase composition of the products is a mixed phase of pyrochlore structure and defective fluorite structure by X-ray diffraction (XRD) analysis and Raman spectrum. In addition, the SEM results demonstrate the fracture surface and microstructure of Gd 2 Ti 2 O 7 -based pyrochlore. The densified pyrochlore waste form exhibits high bulk density of 5.56 g·cm −3 and vickers hardness of 11.20±0.2 GPa. The leaching tests show that the elemental leaching rates of Gd, Sm, and Cu after 42 days are 1.92×10 −4 , 1.51×10 −4 , and 3.90×10 −3 g·m −2 ·d −1 , respectively.

研究领域: 材料科学 · 核化学与放射化学
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CERAMICS INTERNATIONAL · 2023 · IF 5.2

High capacity and aqueous stability immobilization of simulated trivalent actinides by zircon-based borosilicate glass-ceramics: Synergistic effect between the crystal lattice and glass network immobilization

Jiajing Li,Dandan Zhao,Yisheng Chen,Zhongxiang Guo,Hongyue Lei,Hui Dan,Yi Ding,Tao Duan

The development of matrix with high capacity and stability immobilization of nuclear waste is highly desirable. Herein, new type of zircon-based borosilicate glass-ceramics (ZBGC) with high immobilization capacity and excellent aqueous stability was prepared and applied to immobilize simulated trivalent actinide (Nd). The effects of Nd doping and sintering temperature on the microstructure and phase composition of the obtained ZBGC were researched. The experimental suggested that high ZrSiO 4 formation rate (97.49 wt%) was obtained by tuning the Nd content and sintering temperature. The record high immobilization capacity of Nd in ZGBC (18 at%) was achieved owing to the synergistic effect between the crystal lattice and glass network immobilization. Additionally, the obtained Nd-doped ZBGC exhibited excellent aqueous stability (∼10 −6  g m −2  d −1 ) due to the high compactness. The results demonstrated that ZBGC with high immobilization capacity and aqueous stability could be potential matrix for actinides immobilization.

研究领域: 材料科学 · 核化学与放射化学
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Journal of Environmental Chemical Engineering · 2025 · IF 7.2

Vanadium-driven surface engineering to suppress Sr segregation in perovskite ceramics for nuclear waste immobilization

Yinlin Chang,Tao Liu,Jingyuan Rao,Min Fu,Yijun Guo,Shuliang Zou,Dewen Tang,Zetian Tao

The safe immobilization of radiotoxic strontium (Sr) in high-level radioactive waste (HLW) remains a major challenge due to its tendency to segregate and leach under aqueous conditions. In this study, a surface vanadium (V) engineering strategy is proposed to enhance the chemical stability of Sr 2 Fe 1.5 Mo 0.5 O 6-δ (SFM) ceramics. V-doped samples (SFMV), synthesized via a sol-gel method with 0.05 mol V partially substituting Mo, show improved resistance to Sr migration. DFT calculations reveal that V modification increases the Sr migration barrier from 0.14 eV (in SFM) to 0.34 eV (in SFMV) and induces the formation of strong Fe-O-V, and Mo–O–V effectively suppressing Sr surface segregation. Additionally, the formation of SrMoO 4 phases may act as Sr sinks, further enhancing stability. Leaching tests show that the Sr release from SFMV drops from 7.43 × 10 −4 to 2.89 × 10 −6 g·cm −2 ·d −1 over 42 days, representing a 64 % reduction compared to pristine SFM. This work provides a promising strategy for designing durable ceramic hosts for Sr-containing HLW.

研究领域: 材料科学 · 核工程 · 环境化学 · 固态化学
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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY · 2025 ·Vol. 46 ·期 2 ·117844 · IF 6.2

Synthesis, microstructures, and aqueous chemical durability of high-entropy pyrochlore ceramic Eu2B2O7 (BTi, Zr, Sn, Hf, Nb, and Ce) for nuclear waste immobilization

Zhuangzhuang Ma,Yunhao Wang,Tianhao Rui,Yulin Lan,Linyuan Lu,Yang Yu,Mingxuan Deng,Tianxing Lan,Zhekang Zhao,Zhen Teng,Haibin Zhang

High-entropy pyrochlore ceramics with the nominal composition Eu 2 B 2 O 7 , incorporating up to five equiatomic B-site cations, were synthesized via a solid-state reaction method and evaluated their aqueous chemical durability for nuclear waste immobilization. Comprehensive characterization using XRD, Raman, and SEM analyses confirmed the formation of a single-phase pyrochlore structure with uniform and random elemental distribution. However, secondary phases were observed in the Ce- and Nb-doped samples, which is attributed to the larger ionic radius of Ce and the higher valence state of Nb. The 42 days leaching tests revealed normalized element release rates ranging from 10 −5 to 10 −7 g/(m 2 ∙d), significantly lower than those of conventional pyrochlore materials. This enhanced durability is attributed to synergistic effects of electronegativity, ionic radius, and atomic number, which together hinder cation diffusion and strengthen chemical durability at the B site. These findings demonstrate the potential of Eu 2 B 2 O 7 high-entropy pyrochlore ceramics as long-term host materials for high-level radioactive waste. This study provides a valuable resource for enriching the thermophysical properties database of B-site high-entropy pyrochlore solidification, thereby supporting their engineering development.

研究领域: 材料科学 · 核化学 · 无机非金属材料 · 放射性废物处理 · 固体化学
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JOURNAL OF SOLID STATE CHEMISTRY · 2021 · IF 3.498

Phase and microstructure evolution of 0.2SiO2/Zr1-xNdxSiO4-x/2 (0 ≤ x ≤ 0.1) ceramics

Zhengdi Jiang,Zhen Li,Zhenyu Chen,Xuanrui Zhang,Weijie Fan,Yuan Liu,Hui Dan,Yi Ding,Tao Duan

Zircon (ZrSiO 4 ) ceramics were widely used in the field of nuclear waste immobilization because of their excellent properties. However, the SiO 2 /ZrSiO 4 ceramics were usually obtained in the preparation of ZrSiO 4 . The actinides immobilization behavior of SiO 2 /ZrSiO 4 ceramics is unclear. Herein, Nd-doped 0.2SiO 2 /Zr 1- x Nd x SiO 4- x /2 (0≤ x  ​≤ ​0.1) ceramics were fabricated and the effects of Nd-doping and sintering temperature on their phase and microstructure evolution were investigated. The obtained ceramics were characterized by XRD , SEM, BSE and EDS . Results show that 0.2SiO 2 /Zr 1- x Nd x SiO 4- x /2 ceramics with 0≤ x  ​< ​0.04 are ZrSiO 4 phase; while with 0.04≤ x  ​≤ ​0.1 are coexistence of ZrSiO 4 and Nd 2 Si 2 O 7 phases. The solubility limit of Nd 3+ in 0.2SiO 2 /ZrSiO 4 is about 4 ​at%. The lattice volume of ZrSiO 4 increased with increasing Nd-doped content and sintering temperature. Furthermore, higher Nd-doped content and sintering temperature are beneficial to the densification of the obtained ceramics. The results demonstrate that the 0.2SiO 2 /ZrSiO 4 ceramics can be employed as waste form materials to immobilize trivalent actinides.

研究领域: 材料科学 · 核工程 · 陶瓷
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ENVIRONMENTAL RESEARCH · 2025 · IF 7.7

Optimal Si/Al molar ratio achieves ultra-high CeO2 loading and enhanced stability for nuclear waste immobilization in aluminosilicate glasses

Pan Tan,Jiaqin Wei,Sihong Luo,Guilin Wei,Xiaoan Li,Lijing Huang,Xirui Lu,Xiaoyan Shu

Glass matrices with high waste load capacity, stability, and economic viability holds significant technological implications for efficient and safe nuclear waste immobilization. Aluminosilicate glasses with various Si/Al molar ratios were successfully prepared by incorporating Al 2 O 3 into natural granite, effectively enabling precise regulation of the Si/Al ratios and overcoming the challenge of achieving complete vitrification. Here, we report a glass waste form with ultra-high CeO 2 loading (up to 20 wt .%) that exhibits excellent structural stability. At a Si/Al molar ratio of 3:1, cerium can incorporate into the glass network by forming Ce-O bonds through coordination with oxygen atoms in the [AlO 6 ] units. [AlO 6 ] is converted to more stable [AlO 4 ], thereby enhancing the stability of the glass. Up to 20 wt .% CeO 2 (9.62 mol%) can be fully incorporated into the glass system, where approximately 79.71 % of the bridging oxygen atoms form stable Si-O-Si and [AlO 4 ] units, contributing to a structurally robust glass network. The Ce-O bond length in the glass matrix is shorter (2.27 Å) than in CeO 2 , confirming enhanced coordination stability and aligning with superior chemical durability and mechanical properties. This work highlights the critical role of the Si/Al molar ratio and establishes low-cost granite could serve as a viable host material for nuclear waste immobilization.

CAS / MDL: 1306-38-3 1344-28-1
研究领域: 材料科学 · 核工程 · 玻璃化学 · 废物处理
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CERAMICS INTERNATIONAL · 2025 · IF 5.6

He2+/Xe20+ irradiation damage effects of Sr0.5Zr2(PO4)3–(Ce, Nd)PO4 composite ceramics

Yuan Liu,Junxia Wang,Jin Wang,Die Liu,Kunqi Liu,Long Kang,Tongmin Zhang

Composite ceramics, which integrate the advantages of multiple crystal structures, are considered promising candidates for nuclear waste forms capable of simultaneously immobilizing various radionuclides. In this study, a series of 0.4Sr 0.5 Zr 2 (PO 4 ) 3 –0.6Ce 1- x Nd x PO 4 composite ceramics were designed to co-immobilize the simulated fission product Sr and actinide surrogates Ce and Nd. These composite ceramics exhibited homogeneous phase distribution and high densification. Among them, the irradiation-induced damage in the representative sample, 0.4Sr 0.5 Zr 2 (PO 4 ) 3 –0.6Ce 0.6 Nd 0.4 PO 4 composite ceramic, was systematically evaluated under both He 2+ and Xe 20+ irradiation. After He 2+ irradiation, the crystallinity of the irradiated layer was retained despite the disruption of Raman-active bonding groups by point defects. Notably, the Ce 0.6 Nd 0.4 PO 4 phase exhibited significantly higher resistance to He 2+ irradiation than the Sr 0.5 Zr 2 (PO 4 ) 3 phase, as confirmed by GIXRD patterns and geometric phase analysis (GPA). Furthermore, fragmentation of Ce 0.6 Nd 0.4 PO 4 grains was observed, which was attributed to defect accumulation, the thermal spike effect, and the thermal expansion mismatch. Following Xe 20+ irradiation, the irradiated layer of the composite ceramic exhibited reduced crystallinity without complete amorphization, while the Raman-active bonding groups remained largely intact. Additionally, pore formation at grain boundaries was likely caused by the segregation and accumulation of irradiation-induced defects.

CAS / MDL: 1314-13-2
研究领域: 核材料 · 陶瓷学 · 辐射效应 · 固态物理 · 材料科学
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