ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Jiaqi Ruan,Yichao Tong,Jingyu Ran,Changlei Qin
A large amount of spent lithium batteries, especially lithium iron phosphate (LiFePO4), is discarded due to their limited lifespan and poses a great threat to the environment. At the same time, the potential application of Li4SiO4, an efficient high-temperature CO2 sorbent, is largely limited by the high cost of lithium resources. Thus, the preparation of Li4SiO4 from spent LiFePO4 batteries has great potential for achieving waste recycling and reducing CO2 capture costs. However, the process of recycling spent LiFePO4 batteries to synthesize Li4SiO4 sorbents still needs to be well investigated. This work proposes to simplify the preparation scheme by combing precipitation, Na doping, and synthesis processes and further optimizing the key variables of pH, Na2CO3 ratio, and heating rate. An optimal condition is determined to be pH = 9, Na2CO3 ratio = 11 wt %, and heating rate = 5 °C/min, and the sorbent prepared shows a superior stable CO2 capacity of 0.24 g/g in 80 adsorption/desorption cycles. The work develops an effective Li4SiO4 preparation scheme from spent LiFePO4 batteries with largely enhanced CO2 adsorption performance and reduced cost and could achieve a win–win situation in waste recycling and CO2 mitigation.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Zongze Lv,Changlei Qin,Shuzhen Chen,Dawid P. Hanak,Chunfei Wu
CO 2 capture and utilization has been considered as an up-and-coming short- to mid-term approach to mitigate the excessive CO 2 emission. Comparing to the conventional separate capture, transportation and conversion arrangement, the integrated CO 2 capture and utilization (ICCU) could largely simplify the complex process and reduce the energy consumption. However, the poor stability of high-temperature CO 2 sorption/desorption severely limit the potential of ICCU. Therefore, it is indispensable to develop a new sorbent/catalyst system ensuring the high-efficiency and long-term operation of the ICCU. In this paper, we propose and demonstrate the feasibility and performance of using K 2 CO 3 -doped Li 4 SiO 4 as an efficient CO 2 sorbent for ICCU operating at a relatively low temperature by dry reforming of methane. Results show that the ratio of H 2 /CO produced is stabilized at 1 ± 0.05 in the pre-breakthrough stage, and the duration extends to be 1.6 times of the original value in the cyclic operations, displaying an excellent performance in reaction matching and process stability.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2021
·
IF 7.033
Shuzhen Chen,Changlei Qin,Weiyang Yuan,Dawid P. Hanak,Jingyu Ran
Li 4 SiO 4 is acknowledged as a promising sorbent candidate in high-temperature CO 2 adsorption. However, reaction kinetics for the regeneration process of Li 4 SiO 4 , especially its dependence on CO 2 pressure is lack of understanding. This work designed and carried out a series of isothermal tests on the regeneration of pure Li 4 SiO 4 and K-Li 4 SiO 4 under CO 2 partial pressure of 0–0.5 atm and temperature of 625–725 °C. For the first time, the expression of ( P eq − P CO 2 ) n is introduced into the regeneration rate equation so as to reveal its dependence on CO 2 pressure. The reaction order ( n ) is found to grade according to the value of ( P eq − P CO 2 ), and the apparent activation energy is calculated as 284.42 kJ•mol −1 and 146.31 kJ•mol −1 for the regeneration of Li 4 SiO 4 and K-Li 4 SiO 4 , respectively. Furthermore, this work proposes that power law model with m = 4/3 is the most probable mechanism function for the regeneration of Li 4 SiO 4 -based sorbents.
研究领域:
化学工程
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
ENERGY & FUELS
·
2017
·
IF 3.091
Yingchao Hu,Wenqiang Liu,Zijian Zhou,Yuandong Yang
Various synthesis methods, such as the combustion method, sol–gel method, impregnated suspension, precipitation, etc., have been previously proposed for the production of efficient Li4SiO4 sorbents. During these methods, the mixture of the precursors of Li and Si were usually dried through the oven, water bath, or oil bath, which are all energy-consuming and slow processes. To produce Li4SiO4 sorbents quickly and efficiently, the spray-drying technique was employed in this work. The spray-dried sorbents exhibited both excellent CO2 capture capacity and cyclic stability during the multiple cycles, indicating that the spray-drying method was effective for the preparation of efficient and durable Li4SiO4 sorbents for high-temperature CO2 removal. Especially, the sorbent using lithium tartrate as the Li source achieved a considerable first-cycle CO2 sorption capacity of ∼0.275 g of CO2/g of sorbent and still held the capacity of ∼0.248 at the 50th sorption/desorption cycle under the realistically low CO2 concentration of 15 vol %. The excellent performance of the sorbent was demonstrated to be attributed to the corresponding small crystallite size of Li4SiO4, high surface area, large pore volume, and rich porosity.
研究领域:
材料科学
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环境科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Long Ma,Changlei Qin,Shuai Pi,Henan Cui
Li 4 SiO 4 is a promising solid sorbent for high-temperature CO 2 capture due to the high and stable CO 2 adsorption performance. It is required to possess good mechanical properties in practical fluidized-bed systems and pelletization is necessary. However, pelletization generally results in a large decline in the CO 2 uptake or a continuous loss-in-capacity of Li 4 SiO 4 sorbents in cyclic reactions. In this work, three kinds of Li 4 SiO 4 powders were synthesized and screened, and spherical pellets were further prepared via an extrusion-spheronization technique using polyethylene as a pore-former to develop porous microstructure. Then sorbent pellets were systematically tested on the CO 2 adsorption performance, compression strength and attrition resistance. Results shows that the pellets modifying with 20 wt% polyethylene reach and stabilize a CO 2 sorption capacity of 0.31 g CO 2 /g sorbent in the whole 40 tested cycles under typical conditions, which is even higher than that in powder form. Moreover, the pellets are observed to have an outstanding compression strength (27.5 MPa after calcination) and an excellent attrition resistance (only 1.01 wt% mass loss in 10 h-attrition test), which are both far more better than sorbents reported in the literature. The simultaneous physiochemical performances indicate that the prepared Li 4 SiO 4 sorbent pellets could be suitable for high temperature CO 2 capture in fluidized-bed reactors.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Storage
·
2024
·
IF 8.9
Xingyu Yan,Xicheng Wang,Wentao Xia,Lin Lu,Yuandong Yang,Xiaoyu Zhang,Zijian Zhou,Wenqiang Liu
Thermochemical energy storage by using Li 4 SiO 4 TCES materials has been considered a promising technology for efficient heat storage from high temperature sources (700–900 °C). It has been proven the utilization of organic lithium precursors could effectively improve the heat storage performance of derived Li 4 SiO 4 . Hence, in this work, 7 kinds of unreported organic lithium precursors were screened for producing high-performance Li 4 SiO 4 TCES materials. The physicochemical properties, CO 2 ad-desorption capacities and the heat storage/releasing performance of as-prepared Li 4 SiO 4 were systematically evaluated by a series of experimental and kinetic investigations, and a dual modification effects of organic lithium precursor were revealed. As a consequence, 3 potential candidates including lithium benzoate, lithium oxalate and lithium citrate were screened out. Li 4 SiO 4 adsorbents derived from these precursors show great heat storage amount promotions of over 50 % in comparison with the average capacity of traditional Li 4 SiO 4 (~ 350 kJ/kg/cycle). Especially, the lithium citrate derived Li 4 SiO 4 exhibits the greatest CO 2 adsorption capacity, reaction rate and cyclic stability, leading to a cumulative storage amount of 5.9 MJ/kg within 10 cyclic heat storage/releasing processes. Above findings could provide guidance for the future development of high-performance Li 4 SiO 4 materials and Li 4 SiO 4 -CO 2 TCES systems.
研究领域:
材料科学
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能源工程
✓ 已验证
DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2019
·
IF 4.507
Hailong Li,Mingyu Qu,Yingchao Hu
Li 4 SiO 4 has been demonstrated as a promising adsorbent for CO 2 capture. However, Li 4 SiO 4 adsorbents from the conventional solid-state method usually exhibit dense microstructures and, thus, poor CO 2 capture performance. Treating Li 4 SiO 4 with organic acids has been proved effective to improve the microstructures. The commonly used acids such as acetic acid, citric acid and gluconic acid are too expensive, restricting the application of this modification technique. In addition, in the typical Li 4 SiO 4 -based CO 2 capture looping system, CO 2 usually exists in the desorption reactor. However, the effect of the existence of CO 2 at the desorption stage on adsorption performance has been rarely studied. Focusing on these two issues, this work employed pyroligneous acid (PA), a low-cost by-product of the fast pyrolysis of biomass, to modify the microstructures of Li 4 SiO 4 . It was found that modification by pyroligneous acid (PA) successfully improved the microstructures and enhanced the surface area of Li 4 SiO 4 adsorbent. As a result, the obviously improved CO 2 adsorption performance was achieved. In addition, the test results under CO 2 -containing desorption atmospheres indicated that the existence of CO 2 at the desorption stage decreased the adsorption performance due to the severe sintering caused by the existence of CO 2 at the desorption stage.
研究领域:
材料科学
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环境工程
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
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IF 7.2
Liang Cai,Sirong Tao,Zhen Shen,Li Wan,Ziao Liu,Xilin He,Yingchun Zhang
Li 4 SiO 4 ceramic pebble is deemed as the most attractive tritium breeder for fusion reactor blanket. In this work, we fabricated a novel Li 4 SiO 4 pebble with micrometer-scale pore structure by digital light processing to verify the feasibility of complex pore structure manufacturing for future breeders. The effects of processing parameters on printing accuracy, microstructure and mechanical properties of Li 4 SiO 4 pebbles were investigated. For synthesizing the pure Li 4 SiO 4 phase, the optimal stoichiometric ratio of Li 2 SiO 3 to Li 2 CO 3 was 1:1.09 in the premixed powder. The photosensitivity of dual-phase ceramic suspension was investigated according to an attenuation model, and the overgrowth was reduced to ∼50 μm by using the dimension formula. After optimizing the post-processing, the radial pore structure Li 4 SiO 4 pebbles with excellent crush load (50.3 N, standard deviation = 4.4 N) and suitable open porosity (18.3 %) can be yielded. This work provides a fresh solution to control the pore structure of tritium breeding pebbles in an unprecedented micrometer scale.
研究领域:
材料科学
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核工程
·
增材制造
✓ 已验证
DOI
高影响因子
Materials Today Chemistry
·
2025
·
IF 6.7
Jean Pierre Mwizerwa,Chenlong Gao,Changyong Liu,Wenfei Lu,Menghao Yang,Jun Shen
Constructing a robust, highly Li-ion-conductive surface layer is an effective strategy to improve the interfacial stability of nickel-rich cathodes like LiNi 0 . 8 Co 0 . 1 Mn 0 . 1 O 2 (NCM811). However, existing methods often fail to balance ion/electron conductivity with suppression of surface phase transformations, leading to poor rate capability, cycling stability, and energy density. This work introduces an in-situ solution-phase formed coating of Li 4 SiO 4 (LSO) that creates a continuous ion/electron-conductive network across NCM811 particles. This LSO enhances lithium-ion transport, builds a stable electrode/electrolyte interface, and alleviates mechanical stress during cycling. As a result, NCM811@LSO exhibits improved electrochemical performance, including reduced voltage decay and stable operation at high voltages. The LSO coating suppresses surface degradation, intergranular cracking, and parasitic reactions by shielding active sites and reducing direct electrolyte contact. It also mitigates electrode polarization and localized overcharging during long-term cycling. Full-cell tests using graphite and SiO/C anodes confirm high energy densities, reaching 765 Wh kg −1 in NCM811@LSO//graphite cells. Furthermore, density functional theory (DFT) calculations support the experimental findings, revealing that LSO promotes favorable interfacial chemistry, suppresses internal cracking, inhibits nickel migration, and prevents irreversible phase transformations. Compared to traditional coatings, the multifunctional LSO layer offers superior protection and conductivity, making it a promising approach for developing advanced, high-energy-density lithium-ion batteries.
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DOI
高影响因子
Journal of Energy Storage
·
2023
·
IF 9.4
Xiaoyu Zhang,Shimeng Zhou,Wenqiang Liu,Zijian Zhou,Yuandong Yang
Thermochemical energy storage has been considered as a promising technology for the future high-temperature solar thermal conversion and utilization in concentrated solar power plants. In this work, Li 4 SiO 4 /CO 2 thermochemical energy storage system was designed based on the reversible reaction Li 4 SiO 4 + CO 2 ↔Li 2 SiO 3 + Li 2 CO 3 . The proposed Li 4 SiO 4 -based system, which possesses a heat releasing temperature of ∼700 °C, fills in the gaps of medium temperature TCES materials. Furthermore, structure-improved, sintering-resistant Li 4 SiO 4 materials with stabilized performance were fabricated by using organic lithium precursor and cerium addition, and corresponding enhancement mechanisms were systematically studied. It is concluded that the utilization of lithium salicylate could effectively improve the surface morphology as well as the specific surface area of Li 4 SiO 4 particles. And the Ce addition could enhance the cyclic stability of Li 4 SiO 4 by forming anti-sintering CeO 2 fine particles inside. As a result, the obtained L-S-Ce2.5 exhibits an average capacity of 671.3 kJ/kg with the capacity decay as low as 13 kJ/kg per cycle, which is of great significance for the practical long-term heat storage/releasing applications at medium temperature.
研究领域:
材料科学
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可再生能源
·
太阳能
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Xinmei Wang,Junqiang Han,Jianing Ni,Jianan Li,Chang Gao,Changlei Qin
Spent lithium-ion batteries (LIBs) are expected to be discarded in huge amounts due to their limited service life, causing severe environmental problems if not properly handled. It is a promising route to obtain cheap CO2 separation materials of Li-based CO2 sorbents and Ni/Mn/Co-based oxygen carriers from spent ternary LIBs, realizing a win-win outcome in terms of waste recycling and CO2 reduction. However, the migration of key impurities during the recycling of spent LIBs and the approach to synthesizing CO2 separation materials may affect their physical and chemical characteristics. Herein, the work aims to develop CO2 separation materials from spent ternary LIBs, elaborating the migration and influence of impurities, and optimizing the performance of CO2 separation materials. Results show that Ni, Co, and Mn in spent LIB cathode enter oxygen carriers with a minor amount of Li, Al, etc., while Li mainly enters Li4SiO4 sorbents with some Na and Si. After optimization, the obtained oxygen carrier of CO–OC-0.3Al possesses a stable oxygen transport capacity of 16.3% during 30 cycles of reduction and oxidation, and the sorbent of CO-Li4SiO4-0.1Na could attain an excellent CO2 capacity of 0.26 g/g within 100 cycles of adsorption and desorption. We believe that the work could lay a foundation for the efficient construction of CO2 separation materials from spent LIBs, which is of great significance for environmental protection and low-carbon energy development.
研究领域:
能源工程
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环境科学
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材料科学
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化学工程
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可持续技术
✓ 已验证
产品关联
DOI
高影响因子
Energies
·
2025
·Vol. 18
·期 16
·4237
·
IF 3.2
Xinmei Wang,Junqiang Han,Jianing Ni,Changlei Qin
With the advancement of global carbon reduction efforts and the rapid development of battery industries, the scale of spent lithium-ion batteries (LIBs) has increased dramatically. Extracting lithium from spent LIBs to synthesize Li4SiO4sorbents not only addresses the challenge of battery recycling but also reduces the production cost of CO2sorbents, making it a research hotspot. However, the CO2adsorption behavior of these sorbents under the effect of impurities may differ from the traditional Li4SiO4, and there is a lack of systematic research on the adsorption kinetics. To address this issue, two Li4SiO4sorbents are prepared from spent ternary LIBs, and their adsorption kinetics are comprehensively investigated using classical kinetic models. Results show that the reaction order of LSO and Na-LSO is 0.41 and 1.63, respectively, with activation energies of 72.93 kJ/mol and 99.23 kJ/mol in the initial kinetic-controlled stage, and 323.15 kJ/mol and 176.79 kJ/mol in the following diffusion-controlled stage. In the cyclic processes, loss-in-capacity is observed on LSO due to the simultaneous decrease in rate constants in both the kinetic and diffusion-controlled stages, while Na-LSO could almost maintain its capacity by having a much bigger rate constant during the kinetic-controlled stage. This study reveals the adsorption kinetics of Li4SiO4prepared from spent LIBs and could provide theoretical support for the targeted design of efficient and low-cost CO2sorbents.
研究领域:
环境科学
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材料化学
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化学工程
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碳捕集与封存
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）