Journal of Materials Chemistry A
·
2021
·Vol. 10
·期 2
·881-890
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IF 12.732
Peng Hu,Hao Liu,Hao Wang,Jie Zhou,Yongqing Wang,Hongbing Ji
CO2 capture, especially under ultralow-pressure regions (400–10 000 ppm), is extremely essential and challenging to keep the prolonged manual operation in confined spaces and reduce CO2 corrosion in natural gas. Although many MOFs have been covered for CO2 capture, they usually suffered from unheeded morphology engineering associated with diffusion kinetics and unbridgeable CO2 adsorption under ultralow pressure. Herein, we have successfully targeted pyrazine-functionalized Co-MOF (1a′) nanocrystals having dapper hexahedral morphology through skillfully integrating morphology engineering and pore functionality. The yielded 1a′ paradigm with snug pore microenvironment afforded record-high adsorption performance for trace CO2 capture (1.36 mmol g−1 at 400 ppm and 5.7 mmol g−1 at 10 000 ppm), yet eclipsed adsorption behavior for CH4 and N2 at 298 K. The decent pore geometry awarded 1a′ with superior property for CO2/CH4 and CO2/N2 separation, giving higher IAST selectivity (1454 for 15/85 CO2/N2 and 494 for 50/50 CO2/CH4). Besides, 1a′ showed an improved hydrophobic nature, with a desired CO2/H2O uptake ratio of 0.45 and improved diffusion selectivity (DM,CO2/DM,H2O) of 17.7. Breakthrough tests visualized that 1a′ could realize high-purity CO2 (>96%), yielding maximum CO2 productivity (162 and 164.9 litres per kilogram for 18/85 CO2/N2 and 50/50 CO2/CH4). Modeling simulations have cooperatively revealed the structure–property relationship between guest molecules and the framework. This work presents an advanced benchmark adsorbent for low-concentration CO2 capture from flue gas and natural gas.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
ACS Applied Energy Materials
·
2021
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IF 6.024
Mengde Li,Junjie Liu,Shuping Deng,Qian Liu,Ning Qi,Zhiquan Chen
In this paper, three kinds of zeolite imidazole frameworks (ZIF-90, ZIF-93, and ZIF-94) were synthesized through hydrothermal reactions. Positron lifetime results reveal two kinds of pores corresponding to the channel in the windows and central cavity of ZIFs. The average diameters of the cavities are 1.12, 1.54, and 0.80 nm in ZIF-90, ZIF-93, and ZIF-94, respectively, while the average diameters of channels are between 0.55 and 0.60 nm. CO2 adsorption results show that ZIF-90 has the highest CO2 adsorption capacities (64.4 cm3 g–1 at 298 K and 104.7 cm3 g–1 at 273 K) at 1 bar, followed by ZIF-94 (57.9 cm3 g–1 at 298 K and 79.4 cm3 g–1 at 273 K) and ZIF-93 (41.5 cm3 g–1 at 298 K and 62.5 cm3 g–1 at 273 K). This shows inconsistency with the total pore volume but is in good agreement with relative volumes of pores smaller than 1.2 nm, which are 6.55, 2.06, and 5.60% for ZIF-90, ZIF-93, and ZIF-94, respectively. Further investigation reveals that an even smaller pore size is required for CO2 adsorption under ultralow pressure. At a pressure of 0.1 bar, ZIF-94 exhibits an ultrahigh CO2 adsorption capacity (21.2 cm3 g–1 at 298 K and 32.1 cm3 g–1 at 273 K) compared with ZIF-93 (10.1 cm3 g–1 at 298 K and 14.9 cm3 g–1 at 273 K) and ZIF-90 (5.9 cm3 g–1 at 298 K and 11.6 cm3 g–1 at 273 K). These quantities coincide well with the relative volumes of pores smaller than 0.8 nm, which are 5.60, 2.06, and 1.18% for ZIF-94, ZIF-93, and ZIF-90, respectively. Our results demonstrate that at atmospheric pressure, CO2 molecules are more effectively captured by micropores, while at extremely low pressures, CO2 molecules are mainly enriched around ultramicropores such as the channels and small cavities in ZIFs.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 24
·2214661
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IF 19
Jing Yang,Ligang Lin,Fengling Tang,Zixu Zhang,Zitian Liu,Meina Xu,Xu Yang,Qiying Wang,Aishan He,Qi Cheng,Chunhong Wang
The development of low-pressure or pressureless self-driven membranes is important for saving energy and overcoming the critical trade-off effect in membrane separation processes. However, conventional self-driven membranes rely on gravity, which is effective in the separation of large-sized materials but is still ineffective in the fine separation of small molecules. Herein, inspired by the capillary effect that exists in nature, a capillary force-induced membrane-driving strategy for fine separation at ultra-low pressures is demonstrated. Hydrophilic nanoparticles are prepared by a cross-linking reaction between tannic acid and 3-aminopropyltriethoxysilane and then introduce them into membrane pores to simulate sand accumulation with an aim to generate the capillary force. The membrane is then used in ultra-low pressure membrane separation. Interestingly, it is found that the membrane has excellent performance in the separation of dye/salt mixtures (dye rejection > 99%, salt rejection < 10%) and a high permeate flux (160 L m −2 h −1 ) under near “zero pressure” conditions. Moreover, the structural stability of the membrane is verified. Introducing capillary forces into membranes as an autonomous driving force can be a promising universal approach that can be added up to the toolbox for the efficient preparation of separation membranes.
研究领域:
材料科学
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环境工程
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膜技术
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Peng Wu,Zai-Dong Shao,George Z. Chen,Jun He,Yu-Ming Zheng
Ammonia (NH 3 ) is a prevalent indoor pollutant, particularly in semiconductor cleanrooms, where it is essential to adhere to stringent regulations that maintain concentration levels below parts per million (ppm). The development of sustainable adsorbents exhibiting high selectivity and adsorption capacity for NH 3 at low partial pressures constitutes a critical yet challenging endeavor within this field. Herein, we introduce a class of isostructural gallate-based metal–organic frameworks (M−GA MOFs, M = Co, Mg, and Mn) endowed with abundant hydrogen bond donors within the pore channels. Notably, the Co-GA MOF exhibits an exceptionally high NH 3 uptake of 3 mmol g −1 at an ultralow pressure of 0.001 mbar, surpassing all previously reported MOFs. Density-functional theory (DFT), independent gradient model based on Hirshfeld partition (IGMH), and quantum theory of atoms in molecules (QTAIM) analyses reveal the presence of strong O-H···N and N-H···O hydrogen bonds between NH 3 and the MOF framework. These interactions, combined with van der Waals forces, contributed to exceptional NH 3 selectivity over CO 2 and N 2 , with selectivity exceeding 10 4 for NH 3 /CO 2 = 0.1 %:99.9 %. Breakthrough experiments validate the exceptional removal performance of Co-GA MOFs for trace amounts of NH 3 , with a breakthrough point observed at 14 d g −1 for a concentration of 10 ppm NH 3 . This work not only advances our understanding of ultralow-pressure gas separation mechanisms but also offers a scalable solution for efficient separation and purification of trace contaminants in environmentally relevant settings.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
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IF 7.7
Fengling Tang,Jing Yang,Ligang Lin,Zitian Liu,Qiying Wang,Wensong Ma,Huiyang Shang,Hao Wu,Aishan He
In the field of wastewater treatment, the efficient separation of dyes/salts and the high-pressure drive easily results in concentration polarization and membrane contamination. In this study, inspired by the capillary effect of natural sponge structure, an aerogel layer with a bionic three-dimensional mesh porous sponge structure was designed to construct an ultra-low-pressure membrane. With the assistance of tannic acid, the carboxymethyl cellulose (CMC) aerogel layer were constructed on the surface of polyvinylidene fluoride (PVDF) membrane using the layer-by-layer cross-linking and freeze-drying methods. The unique three-dimensional mesh structure of the aerogel provides a capillary effect that accelerates the rapid transport of water molecules. The introduction of polypyrrole (PPy) to the aerogel improves the mechanical properties of the aerogel, helping avoid the collapse during the separation process. Meanwhile, the formed PPy improves the membrane separation performance. The results showed, that under near-zero pressure conditions, the modified membrane had excellent dye/salt separation performance (dye rejection >99 %, salt rejection <10 %) and high flux of pure water (101.3 L·m −2 ·h −1 ). Moreover, the membrane also maintained good long-term stability. The study demonstrated the potential of using membrane for dye/salt separation applications by constructing bionic sponge-structured aerogels having capillary effect and good mechanical strength on membrane.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Fu Yang,Li-an Xing,Kwame Nana Opoku,Hongyao Zhao,Zhenxiao Wang,Ruiting Ni,Qiang Gao,Zengjing Guo,Feng Zeng,Aihua Yuan,Jianming Pan
The utilization of ambient low-pressure CO 2 adsorption for carbon neutrality initiatives holds great potential. However, conventional liquid amine absorption methods for CO 2 capture are plagued by high energy consumption and equipment corrosion issues. In this study, we present a novel approach using industrial waste silica fume (SF) as a precursor and tetraethylenepentamine (TEPA) as a chemical modifying agent to efficiently synthesize low-cost mesoporous solid amine adsorbents within the waste-derived mesoporous powder sorbents (MPS) series. Employing the static adsorption technique, the impact of both adsorption temperature and amine loading on the CO 2 adsorption efficacy was comprehensively investigated. The optimized sample, MPS-TEPA-30, demonstrated a superior CO 2 adsorption capacity, achieving 2.22 mmol g −1 at 323 K and 1 bar, a significant 6.8-fold increase compared to the unmodified MPS material (0.326 mmol g −1 ). Additionally, MPS-TEPA-30 demonstrated notable performance advantages, surpassing SBA15-TEPA-30 and MCM41-TEPA-30 with near 1.49- and 2.12-fold increases in adsorption capacity, respectively. Impressively, MPS-TEPA-30 exhibited remarkable adsorption ability beyond 1.5 mmol g −1 at ultralow pressures (<0.01 bar), suggesting its potential for ambient ultralow-pressure CO 2 capture. Moreover, MPS-TEPA-30 showed exceptional stability over multiple adsorption–desorption cycles, with only a marginal 6 % decrease in CO 2 capture efficiency after the seventh cycle. Thermogravimetric analysis confirmed the robust thermal stability of the amine-functionalized adsorbent (∼473 K), rendering it suitable for high-temperature adsorption–desorption processes. The Ideal Adsorbed Solution Theory (IAST) equation predicted an excellent adsorption selectivity of 1600 for the CO 2 /N 2 (1:1) mixture at 323 K and 10 mbar, underscoring the promising prospects of MPS-TEPA-30 in CO 2 capture and selective separation applications from ambient condition.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
WATER RESEARCH
·
2019
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IF 7.913
Caihong Liu,Dan Song,Wenjuan Zhang,Qiang He,Xiaoliu Huangfu,Shaofang Sun,Zhiqiang Sun,Wei Cheng,Jun Ma
In this study, zwitterionic polymer brushes with controlled architecture were grafted on the surface of gravity-driven membrane (GDM) via surface-initiated reaction to impart antifouling property. A variety of membrane characterization techniques were conducted to demonstrate the successful functionalization of zwitterionic polymers on PVDF hollow fiber membrane. The membrane underwent 90 min of reaction time possessing strong hydrophilicity and high permeability was determined as the optimal modified membrane. Long-term GDM dynamic fouling experiments operated for 30 days using sewage wastewater as feed solution indicated zwitterionic polymer modified membrane exhibit excellent membrane fouling resistance thus enhanced stable flux. Confocal laser scanning microscopy (CLSM) imaging implied that zwitterionic polymer modification significantly inhibit the adsorption of extracellular polymeric substances (EPS) which dominates fouling propensity, resulting in the formation of a thin biofilm with high porosity under synthetic functions of foulants deposition and microbial activities . Interfacial free energy prediction affirmed the presence of zwitterionic functional layer on membrane surface could substantially decrease the interactions (e.g., electrostatic attractions and hydrophobic effects) between membrane and foulants, thereby reduced flux decline and high stable flux. Our study suggests surface hydrophilic functionalization shows promising potential for improving the performance of ultra-low pressure filtration.
研究领域:
环境科学
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材料科学
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生物学
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DOI
PubMed
高影响因子
DESALINATION
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2022
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IF 11.211
Cunxian Lai,Xuewu Zhu,Jinyu Li,Weiwei Zhou,Jingtao Xu,Junwen Ding,Jialin Song,Daoji Wu,Heng Liang,Xiaoxiang Cheng
Highly permeable nanofiltration (NF) membranes with efficient natural organic matter (NOM) removal yet preserving essential minerals are of great significance for purifying ground water. In this work, a novel pH-regulated interfacial polymerization (PRIP) strategy was proposed to fabricate ultra-low pressure NF membranes. This strategy was achieved by changing the aqueous solution pH (5, 7, 9, and 11) during IP process. The effects of pH-regulated processes on the structure, chargeability, and physicochemical properties of NF membranes were systematically investigated. Tailored NF membranes under acidic conditions (TFC-pH 5) achieved the ultrahigh permeability of 42.9 L m −2 h −1 bar −1 and 83.3 % moderate rejection of Na 2 SO 4 . For the NF membranes prepared under alkaline conditions (TFC-pH 11), the sieving capacity was obviously improved with fewer defects, and 99.4 % rejection of Na 2 SO 4 was observed. In addition, the purification performance of NF membranes in ground water treatment was further studied. Modified NF membranes showed significant removal of NOM and retain moderate amounts of mineral salts. Finally, the mechanism of the pH-regulated influence on the polyamide active layer formation process was proposed. This study provides a feasible and facile design idea for ultralow-pressure NF membranes in purifying ground water.
研究领域:
环境科学
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材料科学
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水处理
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DOI
高影响因子
危险品化学品经营许可证（带存储）