JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Ning Li,Chao Ma,Ziyue Wang,Dudu Li,Zhihua Qiao,Chongli Zhong
The MOF crystal-glass composites (CGC) membrane, comprising a MOF crystal and MOF glass matrix, represents a novel self-supported membrane that has been effectively applied in gas separation. Nevertheless, the typical MOF glass matrix requires a higher operating temperature (>400 °C), which constrains its combination with a multitude of MOF crystals characterized by high porosity and low decomposition. In this work, Zn-P-dmbIm (coordination polymer) was chosen as the glass matrix, and MIL-101 crystal with high porosity were integrated at an operating temperature of 190 °C. Furthermore, the intrinsic low porosity of a g Zn-P-dmbIm can be enhanced by the incorporation of higher porosity MIL-101, which possessed a high specific surface area (from ∼1.7 m 2 /g to 401 m 2 /g) and porosity (from ∼0.0014 cm³/g/nm to 0.5605 cm³/g/nm) of the CGC. The intimate combination of MIL-101 and a g Zn-P-dmbIm by in - situ melting to reduce the interfacial defects, which also provides a robust foundation for effective CO 2 /N 2 separation. In CO₂/N₂ (50/50, v/v) mixed gas conditions, the MIL-101/ a g Zn-P-dmbIm membrane demonstrated a impressively high CO₂ permeability of 18670 barrer and CO₂/N₂ selectivity of 61, exceeding the CO₂/N₂ upper bound. The variable pressure (1-12 bar) and long-term stability (120 h) of the CGC membrane exhibited enhancing separation stability. Hence, the self-supported MIL-101/ a g Zn-P-dmbIm membrane demonstrated effective CO₂/N₂ separation performance, which had the potential to significantly extend the scope of applications for MOF crystal-glass matrices.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Qingping Xin,Sining Kong,Xueting Cao,Yucheng Pan,Kun Wan,Hao Chen,Huimin Jin,Ningning Gao,Xiaoli Ding,Yuzhong Zhang
At the present time, the realm of gas separation membranes is predominantly centered on the development of membrane materials that simultaneously exhibit exceptional gas permeability and selectivity. Mixed Matrix Membranes (MMMs) hold significant promise in addressing the long-standing challenge of balancing membrane selectivity with permeability. By incorporating a molecular sieving mechanism, an enhanced gas separation process is achieved. In this research endeavor, single-layer MXene nanosheets serve as an ideal substrate for the direct growth of ZIF-8 nanoparticles, yielding heterogeneously structured nanofillers, coined ZIF-8@MXene. The composite filler, ZIF-8@MXene, maintains a two-dimensional lamellar structure reminiscent of MXene, while also integrating ZIF-8 nanoparticles with their optimal pore size of 3.4 Å. This optimal pore size efficiently facilitates the unimpeded passage of CO 2 molecules through the channels, creating a preferential pathway. Conversely, N 2 molecules encounter greater difficulty traversing these channels, effectively coupling the solubility-diffusion mechanism with the molecular sieving mechanism to enhance selectivity in gas separation processes. Consequently, the mixed matrix membrane exhibits a remarkable enhancement in gas selectivity. Particularly, under sub-ambient conditions (−20 °C), the PEO/ [email protected] % membrane achieves an exceptional CO 2 /N 2 selectivity of 294.1, accompanied by a high CO 2 permeability of 115.58 Barrer. This outstanding performance surpasses the 2019 upper bound, underscoring the significant potential of heterostructured nanofillers to be harnessed in advancing various mixed matrix membranes (MMMs) towards high-performance gas separation capabilities.
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CHEMICAL PHYSICS LETTERS
·
2024
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IF 2.8
Ye Liu,Lei Zhang,Yubo Kuang,Xiaoqian Xiang,Haohan Tao,Guangran Di,Xiaojing Yin,Meicheng Li,Xiao-Jun Lv
The photocatalytic CO 2 reduction has the problems of low selectivity of single product. Here, the preparation of Cu modified tubular C 3 N 4 (CTN) was studied. The increase of the active site inhibits the recombination of electrons (e-) and holes (h + ) and improves the selectivity of CO 2 reduction products. Finally, the CO and CH 4 yields of 1.5 % CTN photocatalyst are 11.55 μmol·g −1 and 4.72 μmol·g −1 , respectively, which are 5 times higher than that of tubular C 3 N 4 photocatalyst. The selectivity of 2 % CTN to CH 4 is up to 68 %, indicating that the prepared CTN photocatalyst has high CO 2 reduction activity and CH 4 selectivity.
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Journal of Materials Chemistry A
·
2024
·Vol. 12
·期 18
·10713-10725
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IF 10.7
Xiaoling Ye,Wencheng Liu,Yan Lu,Xiaoxiao Zheng,Yijian Bi,Min Zheng,Lei Han,Benqing Liu,Yafei Ning,Syed Hassan Mujtaba Jafri,Xinyu Zhao,Shangming He,Shilin Zhang,Hu Li
Li–CO2 batteries have emerged as a potential candidate for next-generation energy storage devices due to their impressive theoretical energy density and potential for CO2 capture. However, the practical application of these batteries faces a challenge due to the sluggish CO2 reduction reaction kinetics and Li2CO3 decomposition at the cathode. Herein, graphene nanoribbons decorated with Ru nanoparticles (GNR/Ru) as cathode catalysts are reported, where dispersed Ru nanoparticles on conductive graphene networks are effective in catalyzing CO2 reduction and Li2CO3 decomposition. As a result, the cathode using GNR/Ru catalysts demonstrates a high discharge capacity of 11 470 mA h g−1 at 100 mA g−1 and exhibits excellent long-term stability (more than 1240 hours) with a low overpotential of 1.34 V at a fixed capacity of 500 mA h g−1. This study provides new insights for exploring high-performance cathodic catalysts.
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Molecular Catalysis
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2025
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IF 4.9
Rui Li,Lipeng Wang,Meilin Yin,Yangyang Lei,Shaokun Tang
CO 2 capture and utilization has received worldwide attention in view of the goals of sustainable development and carbon neutrality. Ionic liquid-functionalized covalent-organic frameworks (IL-COFs) possess high adsorption performance and catalytic activity, which overcome the drawbacks of cycling difficulty for pure ILs as homogeneous catalysts and deficient catalytic active sites for COFs. In this work, BpCOF is first rapidly synthesized by solvothermal-scCO 2 -assisted activation method. Afterwards, poly(ionic liquid)s and metal sites are introduced into BpCOF to obtain Zn-R-PIL-BpCOF (R = COOH, CH 3 ) materials through two-step modification including free radical polymerization and metallization. Then the CO 2 adsorption performance, catalytic activity for CO 2 cycloaddition with epichlorohydrin and catalytic recyclability of the materials are investigated. The excellent diffusion behavior of supercritical CO 2 and extremely low surface tension contribute to the rapid synthesis of highly crystalline BpCOF. The crystal structure and micromorphology of the materials are preserved after the two-step modification while the specific surface area and pore volume are decreased. The isosteric heat of adsorption of CO 2 for the typical sample Zn-COOH-PIL-BpCOF is higher than that of BpCOF, indicating the enhanced interaction with CO 2 by the integrated poly(ionic liquid)s and metal sites. Then Zn-COOH-PIL-BpCOF serves as catalyst and the yield of cyclic chloropropylene carbonate reaches 99.3 % at 90 °C and 2.0 MPa for 16 h under solvent-free and co-catalyst-free conditions. The carboxyl hydrogen-bond donors (HBDs), Zn 2+ Lewis acidic sites and Br − nucleophilic group in Zn-COOH-PIL-BpCOF play the roles synergistically. Zn-COOH-PIL-BpCOF exhibits excellent catalytic sustainability and reusability with the product yield exceeding 95 % after six cycles.
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ENERGY & FUELS
·
2024
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IF 5.2
Faping Liu,Yanhong Wang,Xuemei Lang,Gang Li,Shuanshi Fan
The hydrate-based CO2 sequestration (HBCS) is a potential technology that can be applied to large-scale oceanic CO2 sequestration. However, the favorable conditions of liquid CO2 to form hydrate for HBCS are rarely involved. In this work, the effect of organic matters present in the ocean on CO2 hydrate formation under liquid CO2 was investigated. Dodecylbenzenesulfonic acid and threonine were found to promote CO2 hydrate growth in seawater, while only a layer of hydrate film at the interface was formed for other organic matters by visual morphology. An interesting finding that differed from that of the seawater system was that urea and carbohydrates in quartz sand were more conducive to CO2 hydrate formation. The gas storage capacity of CO2 hydrate for urea was increased to 91.2 V/V and the hydrate growth rate reached 1.02 mmol CO2/(mol H2O·min), which significantly exceeded more than 2 times that of other organic matters. The results of visual morphology also indicated that larger chunks of white solid hydrates were observed on the surface of the quartz sand in the presence of urea. In the dissociation process of CO2 hydrate for rhamnose and urea, obvious cracks were not constructed, which is conducive to maintaining the stability of the reservoir. Therefore, the research results of organic matters on CO2 hydrate formation in seawater and quartz sand help find proper sequestration areas for real HBCS technology.
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AICHE JOURNAL
·
2025
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IF 4
Yuhan Wang,Yanxiong Ren,Yu Cao,Junyi Zhao,Jingqi Fu,Guangwei He,Ziting Zhu,Qian Sun,Fusheng Pan,Zhongyi Jiang
Hydrogen-bonded organic frameworks (HOFs) feature a highly ordered pore structure, abundant organic functional groups, and unique solution-processability, holding great promise in gas separations. In this study, we explored the fabrication of HOF membranes utilizing a dispersion-controlled deposition (DCD) method. To achieve homogeneous dispersion, the bulk HOF aggregates were initially dispersed in solvent and then switched to anti-solvent to generate the precipitated nanoparticles. Under vacuum-assisted assembly, the HOF colloidal solution containing nanoparticles was uniformly deposited, and the intracrystalline defects were spontaneously healed during the mixed-solvent evaporation. For the first time, HOF polycrystalline membranes were fabricated on flexible polymer substrates and demonstrated an ultrathin HOF selective layer of ~100 nm. The prepared HOF membranes exhibited high separation performance, with the CO 2 permeance exceeding 600 GPU and the CO 2 /N 2 selectivity exceeding 30. This work establishes a platform technology for HOF membrane fabrication and expands the families of carbon capture membranes.
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Greenhouse Gases-Science and Technology
·
2024
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IF 2.7
Fa-Ping Liu,Ai-Rong Li,Cheng Wang,Yu-Ling Ma
CO 2 hydrate technology can be applied to seawater desalination. However, the kinetics of CO 2 hydrate formation were inhibited in the aqueous solution with inorganic salts, and the kinetic mechanism of CO 2 hydrate formation for inorganic salts with different metal cations and anions was still unclear. In this work, CO 2 hydrate nucleation and growth were studied in aqueous solutions of metal chlorides. Instead of Na + and K + ions, CO 2 hydrate nucleation was promoted in the presence of Ni 2+ , Mn 2+ , Zn 2+ and Fe 3+ ions due to the co-ordination bonds between transition metal ions and water molecules to enhance the formation of the critical crystal nuclei. The induction time was increased by 61.1% in aqueous solution with 0.32 mol/L NaCl, while it was shortened by 55.6% in FeCl 3 aqueous solution at the same concentration of Cl − anions. In the process of CO 2 hydrate growth, Cl − ions played a more important role than the metal ions in affecting the stability of CO 2 hydrate cages. The gas storage capacity was reduced by 10.3% in the presence of NaCl, and was lower than that of other metal chlorides. Cl − anions were absorbed on the hydrate surface and involved in hydrate cages to inhibit the hydrate growth due to the hydrogen bonds between the Cl − ions and water molecules of the hydrate cages. © 2024 Society of Chemical Industry and John Wiley & Sons, Ltd.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Zezhong Xie,Qiushi Wang,Rongge Yang,Jingnan Zhang,Shanqiang Ou,Gangfeng Ouyang,Mingyang Li,Jianxin Shi,Yexiang Tong
Local pH near the catalyst surface exerts a substantial influence on both catalytic selectivity and activity in electrocatalytic CO 2 reduction (CO 2 RR). While the investigation of local pH remains challenging in the aspect of in-situ imaging and monitoring. In this study, a novel lateral-type surface-enhanced Raman spectroscopy (L-SERS) system with a wide pH testing range from acidic to alkaline, is developed for the in-situ observation of local pH distributions with high spatial and temporal resolution during CO 2 RR. Excellent in-situ imaging of local pH near the catalyst surface is obtained, showing good consistency with simulation results. Besides, the gradual pH elevation and stabilization can be monitored via this time-resolved local pH investigation. This study presents a direct visualization of local pH distribution and variation at the Nernst layer during CO 2 RR, providing direct evidence in local pH for the feasibility of acidic electrolyte and offering theoretical guidance for optimizing CO 2 RR conditions.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Gangan Wang,Chaoyi Chen,Junqi Li,Yuanpei Lan,Xin Lin
Red mud and carbide slag, strongly alkaline solid wastes, are produced during the manufacturing of alumina and acetylene gas, respectively. Improper management of these wastes can pose significant environmental hazards. This study proposed a novel method for the collaborative treatment of red mud and carbide slag, enabling the recovery of constituent elements with CO 2 sequestration. During the hydrochloric acid leaching process, Si was reclaimed as Si-rich residue, whereas Ti, Al, Ga, Fe, and Sc were stepwise recovered as Ti-rich product, Al/Ga-rich filtrate, and Fe/Sc-rich product via the subsequent hydrolysis, co-precipitation, and alkali leaching processes, respectively. Utilizing carbide slag to replace the energy-intensive NaOH for pH adjustment in the leaching solution resulted in a Ca 2+ concentration of 21,922 mg/L in the filtrate after co-precipitation. Through further mineralization process, CO 2 sequestration was achieved alongside the production of CaCO 3 with the content reaching 98.5 % along with a whiteness of 94.4 %. Furthermore, by adjusting the experimental parameters in the mineralization process, controlled manipulation of the phase and morphology of the CaCO 3 product could be achieved to meet various industry requirements. To summarize, the complete resource recovery of red mud and carbide slag was achieved in this study, demonstrating the promising potential in practical applications.
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POLYMER
·
2024
·
IF 4.1
Biao Li,Hao Li,Dexuan Xiang,Yuejun Ouyang,Jingao Wu,Gui Chen,Zaixing Zhang,Hongwei Lin,Nonglin Zhou
Converting CO 2 into precious chemicals is considered to be a fundamental and effective tool for controlling the abundant CO 2 emitted. One of the most compelling methods for CO 2 conversion is the synthesis of cyclic carbonates by cycloaddition of CO 2 with epoxides. However, the development of materials with specific functionalities for CO 2 capture and conversion is still considered to be a significant challenge. Herein, a novel imidazolium salts and pyridine skeleton bifunctionalized hypercrosslinked polymers were prepared by FeCl 3 -catalyted Friedel-Crafts alkylation reaction. Various analytical techniques were used to investigate the properties of the catalysts. The bifunctionalized heterogeneous catalysts exhibited outstanding catalytic performances for CO 2 cycloaddition under mild conditions with an excellent yield of up to 99 %. Besides, the catalyst could bear various epoxides and no significant loss of activity after 6 cycles. The properties of metal-free, solvent-free, cocatalyst-free, easy-to-prepare, mild conditions, facility separation and recyclability make the bifunctionalized hypercrosslinked polymers useful for CO 2 cycloaddition.
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ACTA PHYSICO-CHIMICA SINICA
·
2025
·
IF 13.5
Xianghai Song,Xiaoying Liu,Zhixiang Ren,Xiang Liu,Mei Wang,Yuanfeng Wu,Weiqiang Zhou,Zhi Zhu,Pengwei Huo
Photocatalytic carbon dioxide (CO 2 ) reduction represents a hopeful approach to addressing global energy and environmental issues. The quest for catalysts that demonstrate both high activity and selectivity for CO 2 conversion has attracted significant attention. In this study, ultrathin N-doped BiOBr was synthesized using a simple straightforward method. Systematic experimental results indicated that N-doping reduced the thickness of the BiOBr nanosheets and increased their specific surface area. Moreover, the efficiency of photogenerated charge carrier migration and the CO 2 adsorption capacity were significantly enhanced, contributing to improved CO 2 photoreduction performance. Experimental results showed that the 2N-BiOBr exhibited the best catalytic performance, with a CO evolution rate of 18.28 μmol·g −1 ·h −1 and nearly 100% CO selectivity in water, which was three times higher than that of pure BiOBr. The potential photocatalytic mechanism was investigated using in situ FTIR analysis and DFT simulations. Mechanistic studies revealed that N atoms replaced O atoms as adsorption centers, enhancing the strong adsorption selectivity towards CO 2 over O–H in BiOBr and facilitating the formation of key reaction intermediates. This study provides new perspectives on the creation and developmen of effective photocatalytic materials, offering theoretical support for the application of photocatalytic technology in energy and environmental science.
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