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Nature Communications · 2024 ·Vol. 15 ·期 1 ·1-10 · IF 14.7

Anomalous enhancement of humid CO2 capture by local surface bound water in polar carbon nanopores

Zheng Zhe,Wang Yong-Sheng,Wang Miao,Zhao Guo-Hua,Hao Guang-Ping,Lu An-Hui

Removal of confined space carbon dioxide (CO 2 ) that is in low concentration and with coexisting water is necessary but challenging by physical adsorption method. To make the removal process effective, rendering the nanopore surface hydrophobic to resist water is the popular way. Instead of preventing water from occupying the nanopores, in this work, we propose to utilize the guest water for the spatially selective formation of local surface bound water and further induce the preferential CO 2 capture. We observe an anomalous enhancement of CO 2 capture performance under humid conditions over carbon nanopores with spatially selective polar sites. It is evidenced that the surface bound water is formed at non-CO 2 -selective areas of polar carbon nanopores, thus creating additional CO 2 trapping sites. This work may inspire the design of environment tolerable materials for molecular separation and purification under harsh conditions.

CAS / MDL: 553-26-4
研究领域: 材料科学 · 环境科学
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ENERGY & FUELS · 2024 · IF 5.2

Design of Hyperbranched Amine Polymer-Functionalized PolyHIPEs for Rapid CO2 Capture and Separation

Haorui Liu,Xiaoqiong Wang,Shixun Chen,Shuixia Chen

A novel solid amine adsorbent meso-PDVB@HBPE-x was prepared by impregnating and cross-linking the hyperbranched amine polymer (HBP-NH2) in a mesoporous polydivinylbenzene (meso-PDVB) substrate with an open-cell structure. The optimum preparation conditions were investigated in detail, and the CO2 adsorption performance of prepared adsorbents was conducted by a fixed bed dynamic adsorption system. It is suggested that beneficial from the low viscosity, the intramolecular cavity of HBP-NH2, and the open-cell structure of meso-PDVB, the best adsorbent meso-PDVB@HBPE-8, which was slightly cross-linked with ethylene glycol diglycidyl ether (EGDE), exhibited a high CO2 adsorption capacity of 5.64 mmol/g under 25 °C and wet conditions and quick adsorption kinetics (a high Qb/Qe ratio of 0.92). Compared with the low-molecular-weight amine tetraethylene pentaamine, HBP-NH2 processes a higher molecular weight and is easily modified. Through cross-linking with EGDE, the N content and CO2 adsorption capacity of meso-PDVB@HBPE-8 remained stable during 20 absorption (at 25 °C)–desorption (at 90 °C) cycles under wet conditions, showing great regeneration stability. The adsorbents showed great potential in CO2/CH4 separation, achieving a CH4 productivity of 18.86 mmol/g from a 15 mL of CO2/CH4 (20:80, v:v) mixed gas. The strategy of synergistically designing the amine and substrate porous structures demonstrates its advantage in the practical application of CO2 adsorption and separation.

研究领域: 材料科学 · 环境科学 · 化学工程
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ACS Sustainable Chemistry & Engineering · 2024 · IF 7.1

Experimental Study of Sulfoaluminate Cement-Based Rapid Repair Mortar Undergoing Hot/Wet Harsh Conditions: Mechanical Strengths, Hydration Products, and Ettringite Evolution Mechanism

Xiangshan Hou,Jingwei Li,Jianwei Xu,Xin Xiao,Jianyong Wang,Yanhui Liu,Mona Ossman,Fawei Lin,Xujiang Wang,Yuzhong Li,Wenlong Wang

Rapid repair mortar (RRM) is widely used to repair infrastructures, which must achieve high early strength and long-term service. This study investigated the influence of hot/wet harsh environmental conditions on RRM prepared using solid-waste-based sulfoaluminate cement (WSAC). Orthogonal experiments were conducted to obtain the optimized WSAC-based RRM. Then, the impact of simulated harsh conditions (cross-combination of 20/60 °C and 10/40/90%RH humidity) on RRM and synthetic ettringite was studied. High temperature and low humidity restrained the volume deformation and promoted the growth of the later-age compressive strength of the RRM, but reduced the flexural strength. In this case, ettringite lost some water molecules in the Ca–H2O groups and transformed into amorphous meta-ettringite, which retained its needle-rod morphology. A small amount of ettringite decomposed into gypsum, AH3, and Ca(OH)2 under high-humidity conditions, which caused a slight expansion and reduced the compressive strength of the RRM. Fortunately, most ettringite was well protected by the dense RRM matrix, and harsh temperature and humidity conditions could only slowly promote the transformation of ettringite in RRM over a long period. Therefore, short-term rain or hot weather has little effect on the mechanical properties of WSAC-based RRM. This study provides a theoretical basis and data support for the promotion of industrialization of WSAC-based RRM, which is in line with the concept of green and sustainable development.

CAS / MDL: 7784-31-8
研究领域: 土木工程 · 材料科学 · 环境科学
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Facile synthesis of hydrophobic amine-functionalized silica aerogel with low regeneration temperature and long-term stability for efficient direct air capture

Yong Kong,Zhiting Tan,Fangchen Tang,Xiaodong Shen

The objective of this research is to develop an adsorbent with long-term stability for direct air capture of CO 2 (DAC) under humid conditions. Silica aerogel with amine and methyl hybridized (SA-AM) was synthesized to achieve long-term stability and high CO 2 adsorption performance under humid conditions. SA-AM-M with a moderate precursor concentration exhibited well-developed nanostructure and hydrophobicity, achieving a specific surface area of 306 m 2 /g and a water contact angle of 133°. The CO 2 adsorption capacity of SA-AM-M is 0.97 and 1.14 mmol/g at 25 °C with dry and humid 400 ppm CO 2 , respectively. The CO 2 adsorption capacity mainly depends on the temperature, and lower temperature leads to higher CO 2 adsorption capacity in the range of 5–45 °C. The average adsorption rate shows a positive dependency with gas flow rate, indicating that the working capacity can be improved by increasing gas flow rate significantly. SA-AM-M exhibited the lowest regeneration temperature (65 °C) among reported adsorbents for DAC. The diminishment of CO 2 adsorption capacity is only 35 % after the long-term aging for equivalent 18 months at 25 °C and 65 % relative humidity. This study smoothly combines two different functional groups within the silica aerogel, offering significant guidance towards the development of durable aerogels with high performance for practical DAC.

CAS / MDL: 1185-55-3 13822-56-5
研究领域: 材料科学 · 环境科学 · 化学工程 · 纳米技术
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Mixed matrix membranes (MMMs) with amine-functionalized ZIF-L for enhanced CO2 separation performance

Zikang Qin,Yulei Ma,Wentao Du,Jing Wei,Jia Song,Xinyue Fan,Lu Yao,Lin Yang,Yuanfa Zhuang,Wenju Jiang,Zhongde Dai

Amine-functionalized Metal-Organic Frameworks (MOFs) stand out as highly promising materials in membrane separation technology. Nevertheless, the incorporation of amine-functionalized additives may lead to uncontrollable alterations in MOF morphology. Two intact blade-like MOFs (PEI (Polyethylenimine)-ZIF-L and PAMAM (Polyamidoamine)-ZIF-L) were successfully synthesized by controlling the conditions and then introduced into Pebax 2533 to fabricate Mixed Matrix Membranes (MMMs). Hydrogen bonding and other interactions with Pebax can be formed by PEI-ZIF-L and PAMAM-ZIF-L to enhance interfacial compatibility. Simultaneously, a reversible reaction with CO 2 molecules can be undergone by the amine groups, resulting in facilitated transport in MMMs. The CO 2 separation performance of the MMMs is enhanced by this process, with the facilitation being more pronounced under humid conditions. Under humid conditions, the CO 2 permeabilities of Pebax-PEI-ZIF-L (2 wt%) and Pebax-PAMAM-ZIF-L (2 wt%) MMMs were 639.4 Barrer and 702.7 Barrer, respectively, while the CO 2 /N 2 selectivities were 26.68 and 24.35, respectively. Both permeability and selectivity exhibited a significant increase of 200% and 130%, respectively, compared to pure Pebax. Furthermore, the MMMs demonstrated excellent long-term stability during 72 h of continuous operation in a humid environment, showcasing significant potential for industrial applications, particularly in humid flue gas carbon capture.

CAS / MDL: 155773-72-1
研究领域: 膜科学 · 材料科学 · 环境工程 · 化学工程
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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Tuning the Pore Environment of MOFs toward Efficient CH4/N2 Separation under Humid Conditions

Tong Li,Xiaoxia Jia,Hui Chen,Zeyu Chang,Libo Li,Yong Wang,Jinping Li

Adsorption separation technology using adsorbents is promising as an alternative to the energy-demanding cryogenic distillation of natural gas (CH4/N2) separation. Although a few adsorbents, such as metal–organic frameworks (MOFs), with high performance for CH4/N2 separation, have been reported, it is still challenging to target the desired adsorbents for the actual CH4/N2 separation under humid conditions because the adsorption capacity and selectivity of the adsorbents might be mainly dampened by water vapor. Except for the high CH4 uptake and CH4/N2 selectivity, the adsorption material should simultaneously have excellent stability against moisture and relatively low-water absorption affinity. Here, we tuned the ligands and metal sites of reticular MOFs, Zn-benzene-1,4-dicarboxylic acid–1,4-diazabicyclo[2.2.2]octane (Zn-BDC–DABCO) (DMOF), affording a series of isostructural MOFs (DMOF-N, DMOF-A1, DMOF-A2, and DMOF-A3). Because of the finely engineered pore size and introduced aromatic rings in the functional DMOF, gas sorption results reveal that the materials show improved performance with a benchmark CH4 uptake of 37 cm3/g and a high CH4/N2 adsorption selectivity of 7.2 for DMOF-A2 at 298 K and 1.0 bar. Moisture stability experiments show that DMOF-A2 is a robust MOF with low water vapor capacity even at ∼40% relative humidity (RH) because of the presence of more hydrophobic aromatic rings. Breakthrough experiments verify the excellent CH4/N2 separation performances of DMOF-A2 under high humidity.

研究领域: 材料科学 · 化学工程 · 环境科学
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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Synthesis of a Quaternary Ammonium-Halamine and Preparation on the Modified Nanofibrous Filter with Superior Sterilization, Air Filtration, and Biodegradability

Xin Tang,Zaixing Zhang,Lingxiao Jing,Kun Luan,Tonghua Zhang,Sha Zhou,Yifan Zhu,Lifan Li,Jiapeng Ye

The outbreak of the 2019 coronavirus pandemic has raised worldwide attention about self-protection from airborne diseases. Air filtration and wearing mask have been proven to be effective measures in reducing the pathogenic aerosol’s transmission. Those lead to an increasing demand of high-efficient filters. However, the nonbiodegradable polymeric materials used in filters can accumulate in landfills or ecosystems, potentially causing pollution after improper disposals. Sustainable and biodegradable alternatives to current filter materials are urgently needed. Yet, very few commercial filters meet these needs. In this paper, a novel quaternary ammonium-halamine compound containing Schiff base and a sandwich-structured preparation strategy were developed. The obtained multifunctional filter consists of a PLA fleece as a support layer, an antimicrobial coating for bactericidal function, and a nanofibrous membrane for the particle removal. The filter demonstrates strong bactericidal properties, killing 97% of Escherichia coli and Staphylococcus aureus at a biocide concentration of only 1 mg/mL. It can rapidly kill bacteria within 5 min contact without leaching antimicrobial substances. Furthermore, it boasts a filtration performance with a success rate over 99.99% and a pressure drop of 45 Pa, which surpasses that of commercial N95 filters for PM0.3. Even under humid conditions, it maintains excellent filtration performance. Our reusability testing result of the developed filters shows that a simple halogenation treatment can renew the halamines and restore the filter’s antimicrobial activity. The filters can degrade in natural soil. The successful development of this sustainable and biodegradable filter material offers a new alternative for high-performance air quality control that protect public health.

CAS / MDL: 590-14-7 9002-89-5
研究领域: 材料科学 · 环境科学 · 生物技术 · 公共卫生
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