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Li4SiO4
Nuclear Materials and Energy · 2023 · IF 2.6

Enhancing properties of Li2TiO3/Li4SiO4 tritium breeding ceramics by chitosan addition

Xin Chen,Yichao Gong,Kun Kang,Yuefei Wang,Jiarui Li,Zhaokun Li,Tao Wu,Guojun Zhang

Li 2 TiO 3 /Li 4 SiO 4 ceramics have been regarded as promising tritium breeders due to their numerous merits. In this work, chitosan was employed as an effective binder to provide adhesion of Li 2 TiO 3 particles to Li 4 SiO 4 particles, resulting in Li 2 TiO 3 /Li 4 SiO 4 ceramics with improved performance. Chitosan could be removed during the sintering process and had little influence on the phase composition. The resulting Li 2 TiO 3 /Li 4 SiO 4 ceramics had higher density (92.5%T.D.), greater crushing loads (115.2 ± 20.8 N) and superior thermal properties (3.61 W/m∙K) when compared to the samples prepared without chitosan. SEM analyses displayed a dual-scale structure and the inter- and trans -granular fracture mode. Thermal cycling tests revealed that the phase composition was stable but the crushing load fell slightly. The crushing load remained at 92.4 ± 17.1 N after 12 cycles. Overall, chitosan plays an important role in the amelioration of interface combination between Li 4 SiO 4 and Li 2 TiO 3 , and thus significantly improve density, crushing load and thermal conductivity of Li 2 TiO 3 /Li 4 SiO 4 .

研究领域: 材料科学 · 核能工程
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SCIENCE OF THE TOTAL ENVIRONMENT · 2022 · IF 10.753

Pore reconstruction mechanism of wheat straw-templated Li4SiO4 pellets for CO2 capture

Yingchao Hu,Hongyuan Lu,Zhe Lv,Ming Zhang,Ge Yu

The traditional Li 4 SiO 4 -based CO 2 sorbent pellets prepared from mechanical granulation methods usually presented densified microstructures. Hence, wheat straw, an agricultural waste featured with huge production and low cost, was used as porosity creator to improve the microstructures and CO 2 capture performance of Li 4 SiO 4 pellets. The results indicated that wheat straw effectively enhanced the cyclic CO 2 sorption capacity of the pellets. In particular, 30 wt% wheat straw-templated Li 4 SiO 4 pellets (LA-WS30) exhibited the capacity of ~0.15 g/g that is almost twice as high as that of unmodified pellets. The enriched porosity and improved porous structures resulted from the quick release of burning gases was considered as the main reason for the performance enhancement. In addition, the alkaline (K and Na) salts in wheat straw played a positive role in CO 2 sorption of Li 4 SiO 4 pellets due to the reduced diffusion resistance. However, the pore plugging of residual wheat straw ashes after high-temperature treatment decreased the contact areas and, thus, led to the capacity reduction. To conclude, the comprehensive performance of wheat straw-templated Li 4 SiO 4 pellets is the result of the combined effects of porosity creation, alkali doping and pore plugging by ashes.

研究领域: 材料科学 · 环境工程 · 碳捕集与封存 · 陶瓷 · 吸附材料
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ENVIRONMENTAL SCIENCE & TECHNOLOGY · 2022 · IF 11.357

From Spent Lithium-Ion Batteries to Low-Cost Li4SiO4 Sorbent for CO2 Capture

Yichao Tong,Changlei Qin,Linyan Zhu,Shuzhen Chen,Zongze Lv,Jingyu Ran

The huge consumption of fossil fuels leads to excessive CO2 emissions, and its reduction has become an urgent worldwide concern. The combination of renewable energies with battery energy storage, and carbon capture, utilization, and storage are well acknowledged as two major paths in achieving carbon neutrality. However, the former route faces the discard problem of a large amount of lithium-ion batteries (LIBs) due to their limited lifespan, while it is costly to obtain effective CO2-capturing materials to put the latter into implementation. Herein, for the first time, we propose a route to synthesize low-cost Li4SiO4 as CO2 sorbents from spent LIBs, verify the technical feasibility, and evaluate the CO2 adsorption/desorption performance. The results show that Li4SiO4 synthesized from the cathode with self-reduction by the anode graphite of LIBs has a superior CO2 capacity and cyclic stability, which is constant at around 0.19 g/g under 15 vol % CO2 after 80 cycles. Moreover, the cost of fabricating sorbents from LIBs is only 1/20–1/3 of the conventional methods. We think this work can not only promote the recycling of spent LIBs but also greatly reduce the cost of preparing Li4SiO4 sorbents, and thus could be of great significance for the development of CO2 adsorption.

研究领域: 储能 · 环境科学 · 材料科学 · 碳捕集与利用
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ENERGY & FUELS · 2017 · IF 3.091

High-Capacity Li4SiO4-Based CO2 Sorbents via a Facile Hydration–NaCl Doping Technique

Ke Wang,Wei Li,Zeguang Yin,Zhongyun Zhou,Pengfei Zhao

A sodium chloride (NaCl) doping–hydration technique was used to modify the structure of Li4SiO4 to improve its sorption properties at a low CO2 concentration. X-ray diffraction, nitrogen adsorption, scanning electron microscopy, X-ray photoelectron spectroscopy, differential scanning calorimetry, and thermogravimetric analyses were conducted to characterize the compositions, textural characteristics, morphologies, chemical valence states, molten phases, and adsorption properties of the synthesized samples. Hydration and NaCl doping produced synergistic effects. On one hand, a small particle size and large specific surface area were obtained, significantly facilitating chemisorption processes. On the other hand, co-doped sodium and chlorine induced molten phases when absorbing CO2, noticeably decreasing CO2 diffusion resistance. Thus, the CO2 absorption rate and uptake were remarkably improved. Different amounts of NaCl also greatly affected the morphology and chemisorption properties of the sorbents. At the optimized NaCl concentration, the sorbent only required 3 wt % doping to attain a maximum sorption capacity of up to 34.2 wt %. Moreover, the high capacity was maintained after 10 sorption/desorption cycles.

研究领域: 材料科学 · 环境科学
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APPLIED ENERGY · 2017 · IF 7.182

Molten sodium-fluoride-promoted high-performance Li4SiO4-based CO2 sorbents at low CO2 concentrations

Ke Wang,Zhongyun Zhou,Pengfei Zhao,Zeguang Yin,Zhen Su,Ji Sun

Highly efficient NaF-doped Li 4 SiO 4 sorbents were synthesized by sacrificial carbon template technology to overcome their typical kinetic limitations at low CO 2 concentrations. The samples were characterized by XRD , SEM , N 2 adsorption, XPS , differential scanning calorimetry (DSC), and thermogravimetric analyses (dynamic and isothermic). The results showed that co-doped sodium and fluorine were substituted for lithium and oxygen, respectively. Such doped features induced a high concentration of Li-O sites on the molten surface when absorbing CO 2 in a relatively wide temperature range (475–575   °C). This favorable characteristic greatly facilitated surface chemisorption processes, accelerated the transport of Li + and O 2− , and decreased the CO 2 diffusion resistance. Therefore, 3   wt.% NaF doping was used to reach a maximum absorption capacity (>33.0   wt.%) in a wide temperature range (475–575   °C) in 15   vol.% CO 2 . Moreover, the high capacity was maintained over 10 sorption/desorption cycles, suggesting that NaF-doped Li 4 SiO 4 sorbents have high potential for CO 2 capture.

研究领域: 材料科学 · 环境科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Unified mechanistic understanding on CO2 sorption by Na-doped Li4SiO4: Experimental and DFT study

Ke Wang,Chuanjiang Yang,Pengfei Zhao,Edward J. Anthony

The addition of molten Na 2 CO 3 can drastically accelerated the extremely slow sorption kinetics of Li 4 SiO 4 -based CO 2 sorbents in the sorption enhanced reforming process. However, the lack of a unified consensus about the effect of doped Na 2 CO 3 on the CO 2 capture process, now delays the development of more-effective Li 4 SiO 4 sorbents. Here, sorption tests, sturactural characterzations and periodic density functional theory calculations were combined to develop a better mechanistic understanding CO 2 sorption on Na-doped Li 4 SiO 4 . The Na-doped Li 4 SiO 4 exhibited a better CO 2 capture performance than pure Li 4 SiO 4 even below the melting point of any eutectic mixtures. Structural characterizations revealed that rather than generating physical favorable characteristics, the Na doping substituted at the Li site and created lithium–sodium orthosilicates (Li 4-x Na x SiO 4 ). Theoretical calculations agreeing with experimental results further demonstrated that Li 4-x Na x SiO 4 presented a weaker Na-O bond and generated more active phases (quasi Li 2 O groups) for larger sorption energies, more charge transfers and stronger CO 3 2– bond formation, in turn providing more reactive sites for enhanced CO 2 chemisorption as comparing with pure Li 4 SiO 4 . Finally, we propose a new and unified sorption mechanism independent of the traditional “melting layer” explanation.

研究领域: 材料科学 · 化学工程
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ENERGY & FUELS · 2026 ·Vol. 40 ·期 29 ·15949-15957 · IF 6

CO2 Adsorption by Low-Cost Li4SiO4 from Spent Lithium-Ion Batteries via Biomass Direct Reduction

Wang Xinmei,Ni Jianing,Han Junqiang,Qin Changlei

With the global boom in lithium-ion battery (LIB) deployment, the massive production of end-of-life LIBs has become a significant challenge for resource recycling and environmental risk mitigation. Concurrently, the advancement of carbon capture is driving an urgent demand for low-cost, high-performance CO 2 sorbents, among which Li 4 SiO 4 stands out as a promising candidate. A critical insight is that impurities such as K and Na, which are traditionally costly to remove during LIB recycling, act as effective dopants to enhance CO 2 adsorption of Li 4 SiO 4 . To address these dual needs, this work proposes an innovative strategy for the direct reduction of spent ternary cathode materials via biomass pyrolysis. By utilizing the synergistic effects of reductive gases and biochar generated in situ during pyrolysis, Li 2 CO 3 doped with Na and K is recovered and integrated into Li 4 SiO 4 sorbents. Systematic optimization identifies corn stover (20 wt % addition) as the optimal biomass feedstock, with pyrolysis-reduction at 650 ° C for 60 min as the ideal condition. The resulting sorbent exhibits exceptional durability, retaining a high CO 2 capacity of 0.190 g/g after 80 consecutive adsorption-desorption cycles. More notably, its production cost is only 19% of that via conventional routes. This study provides a sustainable pathway for valorizing spent LIBs while enabling the scalable preparation of CO 2 sorbents, bridging the gap between LIBs’ recycling and CCUS advancement.

CAS / MDL: 112945-52-5
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CERAMICS INTERNATIONAL · 2024 · IF 5.1

Nonstoichiometrically activated sintering for Li4SiO4 ceramic pebbles with a cauliflower-like nanostructure and enhanced properties

Yuefei Wang,Yichao Gong,Man Yang,Jianqi Qi,Guojun Zhang,Tiecheng Lu

The advancement of Li 4 SiO 4 ceramics with enhanced performance represents a crucial research area within the domain of solid-state tritium breeding materials. However, the mechanical and physical properties of Li 4 SiO 4 are severely constrained by the challenge of balancing between densification and grain refinement. In this study, a ceramic with a high density and a distinctive cauliflower-like nanostructure is proposed. Specifically, Li 4 SiO 4 nanopowders with varying oxygen vacancy contents were obtained via the mechanical alloying process. The issues of low diffusivity and abnormal grain growth during the sintering of Li 4 SiO 4 ceramics were effectively addressed through the nonstoichiometrically activated sintering method. The resulting Li 4 SiO 4 ceramics exhibited a high relative density (90.21 % T.D.), exceptional mechanical strength (104 N), high thermal conductivity (2.98 W/m·K at room temperature and 1.91 W/m·K at 500 °C), and good ionic conductivity (4.20 × 10 −4  S/m). The findings indicated that the oxygen vacancies in Li 4 SiO 4 powders increased with the prolongation of the mechanical alloying period. This increase contributed to enhanced relative density, crushing load, and thermal conductivity of Li 4 SiO 4 ceramics, with only a slight decline in ionic conductivity. Concurrently, the oxygen vacancies in the ceramics were almost entirely annihilated by sintering under an air atmosphere. In conclusion, the utilization of nonstoichiometrically activated sintering offers significant advantages in the fabrication of tritium breeding ceramics with superior comprehensive characteristics.

CAS / MDL: 1310-66-3
研究领域: 材料科学 · 核能工程 · 固态物理
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Environmental Progress & Sustainable Energy · 2018 ·Vol. 37 ·期 6 ·2026-2033 · IF 1.326

Understanding the flue gas components on the mechanism governing CO2 adsorption on the Li4SiO4 surface

Ke Wang,Ji Sun,Pengfei Zhao

The development of novel Li 4 SiO 4 -based sorbents is hampered by a lack of understanding of the mechanisms governing CO 2 adsorption on the Li 4 SiO 4 surface. In this work, the adsorption of CO 2 and flue gas components (such as H 2 O and SO X (SO 2 and SO 3 )) on a simulated Li 4 SiO 4 surface was investigated using ab initio-based energetic calculations. The Li 4 SiO 4 surface was modeled by a cluster of lithium silicate, in which the atoms were unsaturated to simulate the active sites. Furthermore, Fourier transform infrared (FTIR) spectra were also analyzed. The calculated results showed that three possible configurations were determined: CO 2 weakly sorbed on the oxygen sites of Li 4 SiO 4 through physisorption; a carbonate species appeared, which was characterized by chemisorption; and a linear cluster of Li + -O = C=O formed, having the largest sorption energy. These three possible pathways were likewise in accordance with the FTIR results. Moreover, a pre-chemisorption of water on Li 4 SiO 4 resulted in promoted CO 2 capture, while the presence of competitive SO X sorption on the same active sites as CO 2 sorption showed an inhibition effect. The results clarify the complex adsorption mechanisms on the Li 4 SiO 4 surface. © 2018 American Institute of Chemical Engineers Environ Prog, 37: 1901–1907, 2018

研究领域: 化学工程 · 环境科学
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CERAMICS INTERNATIONAL · 2019 · IF 3.45

Improvement of crushing strength and thermal conductivity by introduction of hetero-element Al into Li4SiO4

Yichao Gong,Junjie Li,Shenghui Yang,Mao Yang,Hao Dang,Yingying Ren,Guojun Zhang,Tiecheng Lu

Investigations on the doping modification of tritium breeding materials have been becoming one of the interesting research areas in the past few years. Recently, preparation method, mechanical and physical properties and tritium release behavior of Li 4+x Si 1-x Al x O 4 solid solution have been studied because of its potential advantages in the field of tritium breeding materials. In this paper, a facile approach was proposed to prepare Li 4+x Si 1-x Al x O 4 pebbles with a relatively small grain. TG/DSC and XRD were conducted to investigate the formation process of Li 4+x Si 1-x Al x O 4 . The results showed the crushing strength and thermal conductivity were obviously improved by introduction of hetero-element Al into Li 4 SiO 4 , and the optimal x value for Li 4+x Si 1-x Al x O 4 was 0.2 from the point of high crushing strength and thermal conductivity. This study will be expected to provide references for fabricating other solid solution tritium breeders.

研究领域: 核能科学 · 材料科学
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CERAMICS INTERNATIONAL · 2020 · IF 3.83

Preparation of Li4SiO4 pebbles with increased lithium content and crush load via molten salt assisted sintering

Yichao Gong,Junjie Li,Lin Liu,Lei Xu,Jie Cui,Guojun Zhang,Tiecheng Lu

Improving the lithium density and performance of lithium-based ceramics is the main direction for the development of advanced tritium breeder. In this work, the previously used polymers or organics were replaced by eutectic LiNO 3 –LiCl in wet process for preparing spherical green body, and then Li 4 SiO 4 pebbles were fabricated through molten salt assisted sintering. The eutectic salt used herein was eco-friendly and had little effect on the Li 4 SiO 4 pebbles. Instead, the incorporation of eutectic salt improved the lithium density and sinterability of Li 4 SiO 4 . The prepared Li 4 SiO 4 pebbles exhibited well-grained microstructure, and the grain size increased with the increasing contents of eutectic salt. Compressive tests showed that the crush load increased more than five times when 20 wt% eutectic salt was added. The proposed method may have great prospects in the preparation of tritium breeding materials.

研究领域: 核科学与技术 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Unveiling the impurity phase self-promoting mechanism in minerals-derived Li4SiO4 for enhanced CO2 capture performance

Xixuan Hu,Liang Huang,Chengbo Zhao,Qiang Wang

Although minerals-derived Li 4 SiO 4 demonstrates enhanced CO 2 capture performance and cost-effectiveness, the specific impurity-derived dopants governing cyclic stability and sorption kinetics still remain poorly understood. In this contribution, we reveal that Al doping (Si/Al = 3.76–5.68) improves cyclic stability by serving as both structural separator and support, while Na doping (Si/Na ≤20.6) enhances sorption capacity and kinetics. DFT simulations confirm Al reduces surface energy while Na increases exposure facet adsorption energy. Perlite is selected as the optimal silicon source from six minerals, and the derived perlite-Li 4 SiO 4 demonstrates superior CO 2 sorption capacities of 33.9 wt% at 650 °C and 8.3 wt% at 400 °C under 100 vol% CO 2 , maintaining 92% initial capacity even under low CO 2 concentrations (20%). Remarkable regeneration stability is observed through 100 cycles with only 1.7 wt% capacity loss. Lower activation energy (chemisorption phase) and 1.73 GJ/t CO 2 regeneration heat confirm its industrial viability. The impurity-doping synergism elucidates a self-reinforcing rationale for engineering stable high-temperature CO 2 capture materials with operational durability.

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