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.
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MACROMOLECULES
·
2025
·
IF 5.2
Fan Hu,Jinpeng Luo,Shichao Feng,Liangqiang Wei,Shinji Ando,Yinhua Wan,Yongbing Zhuang
Conventional polyimide (PI) membranes exhibit low H2/CO2 selectivity (≤3.1). To address this limitation, this study synthesized a novel diamine monomer, 5-amino-2-(4-hydroxy-3-aminobenzene)-benzoxazole (OH-BOA), specifically designed with benzoxazole and hydroxyl functionalities. Subsequently, OH-BOA and its structural counterpart 5-amino-2-(4-hydroxy-3-aminobenzene)-benzimidazole (OH-BIA) were copolymerized with pyromellitic dianhydride (PMDA) to yield four hydroxy-functionalized poly(benzoxazole-benzimidazole-imide)s (OH-CoPIs). These OH-CoPIs exhibited good solubility, robust mechanical properties (tensile strength ≥ 114.9 MPa), high glass transition temperatures (Tg > 400 °C), and low coefficients of thermal expansion (CTE ≤ 28.3 ppm/K). Notably, they achieved a significantly enhanced H2/CO2 selectivity of up to 12.2, surpassing the commercial Matrimid 5218 (3.1) by 4-fold. Systematic evaluation revealed that increasing benzoxazole content reduced the CTE while enhancing tensile strength, Young’s modulus, and H2/CO2 selectivity. The thermally rearranged membrane (TR-40CoPI-400, 400 °C) achieved high H2 permeability (26.00 Barrer) with optimal selectivity (7.6) and exceptional CO2 plasticization resistance. The synergistic integration of benzimidazole, benzoxazole, and hydroxyl groups enables high-performance PI membranes for H2/CO2 separation.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2025
·
IF 4.7
Fengming Mo,Tao Huang,Jinqiang Peng,Yaoyao Shen,Ting Wu,Yuqing Li,Fei Zhang,Xiangshu Chen,Hidetoshi Kita
ZSM-58 membranes were successfully prepared using nanosized ZSM-58 crystals as seeds via a secondary growth method. The effects of various synthesis conditions, including temperature and time, were systematically investigated to elucidate their influence on crystalline structure and morphology. The performance of the membranes synthesized by nano-crystal seeding is superior to that of the membranes synthesized by micro-crystal seeding. The results demonstrate that the ZSM-58 membrane exhibits high selectivity for CO 2 /CH 4 (142.40), CO 2 /N 2 (28.62) and CO 2 /CO (13.79). Additionally, the CO 2 permeance values for binary gas mixtures are 2.56×10 -7 mol·m -2 ·s -1 ·Pa -1 , 2.31×10 -7 mol·m -2 ·s -1 ·Pa -1 and 2.40×10 -7 mol·m -2 ·s -1 ·Pa -1 , respectively. Furthermore, under continuous operation for 100 hours with an equimolar gas mixture, the membrane's separation performance remains stable, with CO 2 permeability and CO 2 /CH 4 selectivity values of 2.42×10 -7 mol·m -2 ·s -1 ·Pa -1 and 141.53, respectively. These findings indicate that the ZSM-58 zeolite membrane possesses excellent long-term stability and holds significant potential for industrial CO 2 removal applications.
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Materials
·
2025
·Vol. 18
·期 2
·244
·
IF 3.2
Zhong Li,Zhiming Yin,Dingzhao Zhou,Zhiqiang Wu,Daohang Wang,Shuwen Guan,Guangyan Du
Ensuring long-term wellbore integrity is critical for carbon dioxide geological storage. Ordinary Portland cement (PC) is usually used for wellbore primary cementing and plug operation, and set cement is easily corroded by acidic fluids, such as carbon dioxide, in underground high-temperature and high-pressure (HTHP) environments, resulting in a decrease in the mechanical properties and an increase in permeability. In order to achieve long-term wellbore integrity in a CO2-rich environment This study introduces materials such as thermosetting vinyl ester resin (TSR), filler composite resin (FCR), and low-cost resin cement (RC). Corrosion experiments were conducted using four materials in 28 days under supercritical carbon dioxide gas and water phase conditions of 60 °C and 10 MPa. The samples were characterized through mechanical property testing machines, core permeability measuring instruments, FTIR, XRD, and SEM. The results proved that after corrosion, PC mechanical properties decreased, the permeability increased, and the microscopic composition and morphology changed greatly. Penetrating corrosion occurs in the sample in the gas phase environment, and propulsive corrosion from outside to inside occurs in the water phase environment. However, TSR, FCR, and RC materials all maintain excellent resistance to carbon dioxide corrosion in gas and water environments. They have higher compressive strength and extremely low permeability compared to ordinary Portland cement. These three materials’ compressive strengths can be maintained around 131, 99, and 58 MPa, and permeability can be stabilized at <6 × 10−7, <6 × 10−7, and 0.16 mD levels. In summary, the above three materials all show better performance than ordinary Portland cement and are promising alternative materials that can be used in primary cementing and plug operations of carbon dioxide geological storage wells.
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Foods
·
2024
·Vol. 13
·期 11
·1719
·
IF 4.7
Yadan Chen,Yanbin Wang,Liang He,Liling Wang,Jianchen Zhao,Zhenya Yang,Qin Li,Rui Shi
This study aimed to investigate the efficacy of supercritical CO2(SC-CO2) extraction in enhancing the extraction rate, purity, and antioxidant activity ofIndocalamus latifolius(Keng) McClure (Poaceae) leaf terpenoids (ILLTs). Crude extracts obtained from leaves were subjected to qualitative and quantitative analyses, revealing neophytadiene, phytol, β-sitosterol, β-amyrone, squalene, and friedelin as the primary terpenoid constituents, identified through gas chromatography–mass spectrometry (GC-MS). Compared with steam distillation extraction (SD), simultaneous distillation extraction (SDE), ultra-high pressure-assisted n-hexane extraction (UHPE-Hex), ultra-high pressure-assisted ethanol extraction (UHPE-EtOH), ultrasound-assisted n-hexane extraction (UE-Hex), and ultrasound-assisted ethanol extraction (UE-EtOH), SC-CO2exhibited a superior ILLT extraction rate, purity, and antioxidant activity. Scanning electron microscopy (SEM) observations of the residues further revealed more severe damage to both the residues and their cell walls after SC-CO2extraction. Under optimal parameters (4.5 h, 26 MPa, 39 °C, and 20% ethyl alcohol), the ILLT extraction rate with SC-CO2reached 1.44 ± 0.12 mg/g, which was significantly higher than the rates obtained by the other six methods. The subsequent separation and purification using WelFlash C18-l, BUCHI-C18, and Sephadex LH-20 led to an increase in the purity of the six terpenoid components from 12.91% to 93.34%. Furthermore, the ILLTs demonstrated cytotoxicity against HepG2 cells with an IC50value of 148.93 ± 9.93 μg/mL. Additionally, with increasing concentrations, the ILLTs exhibited an enhanced cellular antioxidant status, as evidenced by reductions in both reactive oxygen species (ROS) and malondialdehyde (MDA) levels.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Meng Linghu,Yang Jiakun,Huo Zichen,Wu Qin,Zhang Yaoyuan,Shi Daxin,Chen Kangcheng,Liu Helei,Xu Xiyan,Li Hansheng,Xu Hang
The capture and transformation of CO 2 , utilized as a C1 resource, play an integral role in mitigating CO 2 emissions and addressing the emerging 'carbon source crisis.' The CO 2 cycloaddition to cyclic carbonate is particularly noteworthy. A critical factor in optimizing the efficiency and minimizing the costs associated with CO 2 cycloaddition is the selection of an effective catalyst. A novel amine-functionalized intramolecular acid-base synergistic ZIF catalyst, designated as ABF-ZIF-X, was synthesized using a mixed ligand method, employing 2-MeIM and the larger molecular-sized ligand 2-amBzIM. The introduction of an amino active center and the strategic regulation of the active site defects in metal ions enable ABF-ZIF-X to enhance the density of Lewis acid and base sites. This enhancement facilitates intramolecular acid-base cooperation, which is pivotal for effective CO 2 cycloaddition catalysis. Notably, ABF-ZIF-X exhibits exceptional catalytic activity in the cycloaddition of EBH with CO 2 , eliminating the need for additional solvents and co-catalysts. The reaction mechanism of CO 2 cycloaddition, which is intramolecular acid-base synergistic catalysis and bimolecular activation, was proposed. Among the synthesized catalysts. ABF-ZIF-0.15 shows superior performance, achieving an impressive 96.7% conversion of EBH and a selectivity of 97.1%. Furthermore, this catalyst demonstrates remarkable reusability, maintaining high activity across five cycles.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Wanqi Lian,Ying Huang,Qiaoqiao Yin,Zhicheng Guo,Yun Xu,Tifang Miao
To enhance the economic viability of photocatalytic materials for carbon capture and conversion, the challenge of employing expensive photosensitizer must be overcome. This study aims to improve the visible light utilization with zirconium-based metal–organic frameworks (Zr-MOFs) by employing a multi-component post-synthetic modification (PSM) strategy. An economical photosensitiser and copper ions are introduced into MOF 808 to enhance its photoreduction properties. Notably, the PSM of MOF 808 shows the highest CO yield up to 236.5 μmol g −1 h −1 with a HCOOH production of 993.6 μmol g −1 h −1 under non-noble metal, and its mechanistic insight for CO 2 reaction is discussed in detail. The research results have important reference value for the potential application of photocatalytic metal–organic frameworks.
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ADVANCED MATERIALS
·
2024
·Vol. 36
·期 40
·2405492
·
IF 27.4
Long Jiang,Zihan Ma,Zhenjiang Gu,Peiliang Shen,Yong Tao,Weihua Li,Chi-Sun Poon
Superhydrophobic surfaces applying on concrete can greatly improve the durability of concrete by preventing the damage from water. However, traditional design of superhydrophobic concrete surfaces by external coating encounters to problems of flaking and poor surface robustness, while that by adding hydrophobic agents or particles faces the challenges of strength damage of concrete. Drawing inspiration from the carbonation phenomenon of concrete, here a new design of in situ growing superhydrophobic structures on concrete is proposed: The concrete sample is impregnated into Mg 2+ -containing silane–water system with continuous CO 2 injection. The contact angle of the concrete surface achieves 171.9° without obvious strength decrease after 120 min, which are mainly attributed to the formation of Ca x Mg 1−x CO 3 crystals with micro-nano-structures and the reduction of carbonates surface energy by silane. This superhydrophobic concrete structure can be divided into a superhydrophobic–hydrophobic–hydrophilic three layers structure, providing the stable water-proof protection under mechanical fatigue, capillary water absorption, UV aging, sulfate attack, and impurity water impact tests due to the in situ growing robust superhydrophobic structures. Furthermore, it captures 29.80 g m −2 CO 2 during the reaction process, providing new insights for the design and preparation of eco-friendly superhydrophobic concrete.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Wanfeng Xiong,Duanhui Si,Jundong Yi,Yuanbiao Huang,Hongfang Li,Rong Cao
Multicomponent heterogeneous catalysts present excellent catalytic performance attributed to the synergistic effect of multi-sites. Nevertheless, identifying the composition of the multi-sites and exploring the synergistic catalytic mechanisms for the multiple active sites in electrocatalytic CO 2 reduction reaction (CO 2 RR) still lack intensive study. This work regulates the chemical composition of Cu-based nanoreactors readily by adjusting the geometrical morphology of metal-organic frameworks precursor. The obtained cuboctahedron nanoreactor containing Cu-N 4 /Cu 2 O/Cu multiple active sites exhibits excellent CO 2 RR selectivity towards deep reduction product (80%) with high current density. Moreover, the tandem catalytic mechanism of multicomponent active sites has been studied intensively. The CO 2 molecule is firstly reduced in Cu-N 4 sites to form CO and then the CO is transfered to Cu 2 O/Cu sites for further deep reduction. The high concentration of CO provided by Cu-N 4 sites decreases the free energy of rate-determining step for CH 4 products in Cu 2 O sites. This work provides a promising direction for designing and synthesizing multicomponent Cu-based tandem catalysts to access high efficiency and selectivity in the electrocatalytic CO 2 reduction reaction.
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The Innovation
·
2025
·
IF 25.7
Yaoyu Yin,Zhongnan Ling,Shiqiang Liu,Jiapeng Jiao,Meng Zhou,Pei Zhang,Xing Tong,Yueqian Fan,Jiahao Yang,Huanyan Liu,Xueqing Xing,Jianling Zhang,Yi Xu,Hongyan Liang,Xinchen Kang,Buxing Han
Ionomers play a vital role in the preparation of electrodes for CO 2 electroreduction, and controlling the ionomer configuration on the catalyst surface offers an effective strategy for adjusting the surface microenvironment of the electrode, thereby influencing the distribution of CO 2 electroreduction products. In this study, we demonstrate that Nafion, a commonly used ionomer, exhibits distinct aggregation behaviors in solvents with different dielectric constant (ε) values. These differences in aggregation result in varied Nafion arrangements on the catalyst surface, which in turn affect the binding of ∗CO and ∗H intermediates, enabling control over product distribution. For example, over a Cu nanosheet catalyst at 800 mA cm −2 , the Faradaic efficiency for multicarbon products increases from 67.5% to 90.5% simply by changing the dispersion solvent from low-ε dimethyl sulfoxide to moderate-ε isopropanol. This work introduces a novel approach for fine-tuning CO 2 electroreduction product distribution through manipulation of the dispersion solvent without requiring modifications to the catalyst or ionomer.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Huiyan Ren,Liuliu Zhu,Hongbo Gu
Converting CO 2 into high-value C 2+ products under neutral conditions holds significant importance for both energy development and environmental sustainability, yet it remains a formidable challenge. In this work, we synthesize sea urchin-shaped Cu x O nanoparticles coated with polydopamine (Cu x O@PDA), in which the PDA creates a favorable local microenvironment for electrocatalytic CO 2 reduction reaction (ECO 2 RR). Specifically, PDA promotes the hydrogenation reduction of *CO, stabilizes the pivotal *CHO and *OCCHO intermediates, and reduces the energy barrier for the coupling of *CO and *CHO. Leveraging these advantages, Cu x O@PDA achieves a maximum Faraday efficiency for C 2 H 4 up to 53.4% in the neutral electrolyte at potential of -1.4 V vs . RHE, which is 22.3% higher than that of Cu x O at the same potential. This study offers new insights into enhancing the electrocatalytic CO 2 reduction performance of copper oxides through polymer modification, providing a promising strategy for improving the selectivity and efficiency of C 2 H 4 product under neutral conditions.
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Science Bulletin
·
2025
·
IF 21.1
Yiding Wang,Runyao Zhao,Jiaju Fu,Fengtao Zhang,Tianyu Yu,Linzi Wen,Yanfei Zhao,Jin-Song Hu,Buxing Han,Zhimin Liu
Cu-based catalysts have been considered promising electrocatalysts for converting CO 2 into multi-carbon products (C 2+ products). However, achieving selectivity toward a specific C 2+ product remains challenging, necessitating the delicate design of catalytic sites to regulate the energy preference of reaction pathways. Herein, we introduced catalytic sites that evolve active hydrogen atoms (*H) on Cu surfaces to regulate electrocatalytic CO 2 hydrogenation pathways to achieve the selective production of ethylene. Ru single-atom site (Ru 1 ) was theoretically screened from 17 elements with 51 structures, exhibiting optimal activity in promoting hydrogenation of CO 2 reduction intermediates. The accordingly synthesized Ru 1 -doped oxide-derived Cu (Ru 1 -ODCu) catalyst delivered an ethylene selectivity of 82% in C 2+ products with a Faradaic efficiency of 58.9% and a partial current density of 353.4 mA cm –2 in KHCO 3 electrolyte. Kinetic isotope and in situ spectroscopic analyses evidenced that the Ru 1 sites effectively promote intermediate hydrogenation by regulating *H transfer to intermediates, facilitating the energy-preferred pathway to ethylene production. These results provide insights into the design of Cu catalysts with intermediate hydrogenation sites for converting CO 2 into specific products.
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