Sustainable Chemistry for Climate Action
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2023
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IF 0
Ya-Qi Ba,Yong-Sheng Wang,Tian-Yi Li,Zhe Zheng,Guang-Ping Hao,An-Hui Lu
CO 2 capture from flue gas is one of the global urgent tasks. Adsorption separation of CO 2 is an energy-efficient way as compared to the absorption method. The central issue is to devise efficient adsorbents that work well under flue gas conditions with temperatures of 323–348 K and low CO 2 concentrations of 15%. In this work, we targeted this issue and proposed a well-controlled diffusion strategy, which is achieved over a series of poly(furfuryl alcohol)-derived carbons (PFCs) with dense and abundant ultra-micropores. As the adsorption temperature increased from 298 to 348 K, the CO 2 capture capacity is 54% kept for PFC-800, which is 1.2 times higher than that for samples without diffusion limitation. The capture of CO 2 is kinetics control at ambient temperature, however, at 348 K CO 2 with higher kinetic energy can overcome the restriction of the narrow pore entrance and the CO 2 /N 2 selectivity for simulated flue gas composition increases from 20 to 40. Furthermore, the PFCs exhibit a high CO 2 volumetric adsorption capacity of 97 cm 3 cm −3 at 298 K and 1 bar, benefiting the practical application deployed with an integrated adsorption column. The diffusion kinetics can be further tuned when altering the bulk phase into nanocoating, which would inspire their application in different scenarios.
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
Journal of Materials Chemistry A
·
2025
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IF 9.5
Hu Zhang,Jian Yin,Dandan Ouyang,Yu Liu,Ruiyao Wu,Rui Zhang,Ruiqiang Huo,Gaixiu Yang,Yanjun Cai,Jiao Yin
The plateau capacity of a hard carbon anode plays a crucial role in achieving the high energy density of sodium-ion batteries. However, the loss of plateau capacity due to polarization at high current densities imposes significant limitations on hard carbon applications. Ultra-micropores could maintain plateau capacity at high current densities but are generally prepared accompanied by micropores and mesopores that deteriorate the Na-ion storage performance. Herein, a hard carbon with ultra-micropores is prepared by a protonation-mediated strategy using an N, P co-doped biomass precursor. The P dopants favor reducing the interaction between N and C so that the confined volatiles of NH3 could be utilized to create ultra-micropores concentrated at 0.4–0.8 nm. These ultra-micropores enable the hard carbon to deliver a reversible capacity of 386 mA h g−1 at 20 mA g−1, a high plateau capacity of 173 mA h g−1, and an excellent rate capability of 106 mA h g−1 at 2 A g−1. The plateau capacity and rate capability are superior to those of the reported hard carbons. This work provides a new approach for ultra-micropore construction within hard carbons and a new perspective for sodium-ion batteries toward high energy and power densities.
研究领域:
材料科学
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能源存储
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Li Xu,Qiye Ju,Haiyan Jiang,Na Geng,Jianze Xiao,Ziqian Xue,Tingyu Zhu,Yangyang Guo
Heavy water (D 2 O) electrolysis is the primary technology for D 2 production, playing an irreplaceable role in fields such as nuclear fusion research and isotope tracing. However, the inherent similarity in chemical properties between H 2 O and D 2 O (with only a 1.4 °C difference in boiling points) poses significant challenges to their separation. Furthermore, the extremely low natural abundance of D 2 O (0.015 %) increases the difficulty and cost of separation, while traditional electrolysis and distillation techniques are highly energy intensive. Therefore, there is an urgent need to develop novel adsorbents for efficient and environmentally sustainable H 2 O/D 2 O separation. Herein, we used polydentate ligand 2, 5-dihydroxyterephthalic acid (DOBDC) and its derivatives 4,4́-(anthracene-9,10-diyl) bis (2-hydroxybenzoic acid (ABHB) as raw materials to prepare two novel high coordination Sr-MOFs namely IPE-1 and IPE-2, respectively. These MOFs were applied for efficient separation of H 2 O and D 2 O at room temperature. X-ray diffraction results reveal that one Sr atom in IPE-1 is coordinated with 9 oxygen atoms. This high coordination number results in the formation of ultra-small rectangular pores of approximately 2.5 Å. Adsorption isotherms of N 2 , CO 2 , H 2 O, and D 2 O indicate that the ultramicroporous structure of IPE-1 precludes efficient diffusion of CO 2 and H 2 O molecules into the MOF channels. In contrast, the activated IPE-2 exhibits good CO 2 , H 2 O, and D 2 O uptake capacities of 3 mmol/g, 8.38 mmol/g, and 6.51 mmol/g at 298 K, respectively. The Q st values and K sap values of H 2 O and D 2 O indicate that the adsorption rates of H 2 O were much higher than D 2 O under 0.2 < P/P 0 < 0.7, with a calculated ratio of approximately 1.26. This study not only provides appealing MOFs materials for efficient H 2 O/D 2 O separation at room temperature but also provides a new avenue for preparing adsorbents with high stability and high separation performance.
研究领域:
材料科学
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环境科学
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高影响因子
ACS Applied Materials & Interfaces
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2020
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IF 8.758
Gen Li,Zhonggang Wang
This paper presents a series of micro- and ultramicroporous polyaminals with BET surface areas up to 1304 m2 g–1, which are prepared from two triazine-based tetraamines and three dialdehydes or monoaldehyde through the A4 + B2 or A4 + B1 aminalization reaction. It is interesting to find that the para-substituted monomers are favorable to force the linking struts apart in the network to generate micropores (1.22 nm), whereas the meta-substituted monomers make the pores in the network squeezed by the twisted linking struts, resulting in the formation of ultramicropores (0.52 nm). Besides, the adsorption behaviors of the major components of natural gas, such as propane (C3H8), ethane (C2H6), methane (CH4), and carbon dioxide (CO2), are significantly different, strongly depending on the polarizabilities, critical temperatures, molecular sizes of gases, porosity parameters of polymers, and the interaction between gases and the polymer skeleton. At 298 K/1 bar, the polymers show high uptake for C3H8 (114.5 cm3 g–1) and C2H6 (84.2 cm3 g–1). Moreover, the adsorption selectivities of C3H8/CH4, C2H6/CH4, C3H8/C2H6, C3H8/CO2, C2H6/CO2, and CO2/CH4 also reach 296.3, 23.1, 9.0, 22.1, 4.1, and 5.0, respectively, exhibiting promising applications in adsorption/separation of C1–C3 hydrocarbons and stripping CO2 gas from natural gas under the ambient condition.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
Materials
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2020
·Vol. 13
·期 5
·1126
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IF 3.057
Yongfeng Li,Jiaojiao Su,Guiping Li,Xiufeng Meng
Super-microporous material (pore size 1–2 nm) can bridge the pore size gap between the zeolites (<1 nm) and the mesoporous oxides (>2 nm). A series of super-microporous titania–alumina materials has been successfully prepared via a facile one-pot evaporation-induced self-assembly (EISA) strategy by different solvents using fatty alcohol polyoxyethylene ether (AEO-7) as the template. Moreover, no extra acid or base is added in our synthesis process. When titanium isopropylate is used as the titanium source, these materials exhibit high BET surface areas (from 275 to 396 m2/g) and pore volumes (from 0.14 to 0.18 cm3/g). The sample prepared using methanol as the solvent shows the largest Brunauer–Emmett–Teller (BET) surface area of 396 m2/g. When tetrabutyl titanate is used as the titanium source, these materials exhibit high BET surface areas (from 282 to 396 m2/g) and pore volumes (from 0.13 to 0.18 cm3/g). The sample prepared using ethanol as the solvent shows the largest BET surface area of 396 m2/g.Keywords:super-microporous alumina–titania;different solvents;fatty alcohol polyoxyethylene ether;high BET surface areas
研究领域:
材料科学
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化学工程
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DOI
PubMed
高影响因子
AICHE JOURNAL
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2023
·Vol. 69
·期 6
·e18046
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IF 3.7
Zhiwei Zhao,Yueyue Liu,Xing Liu,Yuan Liu,Jingwen Chen,Shixia Chen,Shuguang Deng,Jun Wang
The one-step adsorptive separation of high-purity ethylene (C 2 H 4 ) from a ternary gas mixture (C 2 H 2 /C 2 H 4 /CO 2 ) is challenging and has not been reported on porous carbons. Herein, we report camphor seeds husk-derived ultramicroporous carbons (CSHs) show high affinities toward acetylene (C 2 H 2 ) and carbon dioxide (CO 2 ) over C 2 H 4 . The optimized CSH-2-700 with high heteroatom contents and centered pore size distributions shows high C 2 H 2 adsorption capacity (2.24 mmol g −1 ) and record ideal adsorbed solution theory (IAST) C 2 H 2 /C 2 H 4 selectivity (10.2) among one-step C 2 H 4 purification adsorbents. Meanwhile, CSH carbons are the only carbon adsorbents that preferentially adsorb CO 2 over C 2 H 4 , with a CO 2 /C 2 H 4 selectivity of 1.9 under ambient conditions. Furthermore, dynamic breakthrough experiments verified its feasibility for one-step C 2 H 4 purification from a three-component C 2 H 2 /C 2 H 4 /CO 2 gas-mixture.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
LANGMUIR
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2025
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IF 3.9
Chenxiang Feng,Wei Jian,Junxiu Chen,Agula Bao
The environmental problems caused by excessive CO2 emissions have made the development of adsorbent materials for capturing CO2 an important topic. N-doped porous carbon materials are attractive for CO2 adsorption because of their large specific surface area, porous structure, and multiple active sites. S and N are known to work well together as codopants, but the effects of S on N and the synergistic effects of S and N on carbon materials need to be clarified. In this study, N and S codoped porous carbon samples with an ultramicroporous structure were prepared by using lignin as the carbon source and thiourea as the sulfur source. The prepared samples had a specific surface area of up to 1723 m2/g and N and S contents of up to 1.60 at % and 0.23 at %, respectively. In tests, the best-performing sample had a CO2 adsorption capacity of 3.58 mmol/g at 298 K and 1 bar, which can be attributed to ultramicropores (<1 nm) making up 67.8% of the pore volume. S doping had the synergistic effect of increasing the pyrrole N content on the sample surface, which increased the CO2 adsorption capacity. The present study provides insights into using N and S codoping to develop high-efficiency carbon-based adsorbents for CO2 capture.
研究领域:
材料科学
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环境科学
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DOI
PubMed
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
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2024
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IF 4.8
Kunpeng Liu,Yixuan Yu,Qi Wang,Lingtong Kong,Tianjun Sun
A comprehensive investigation was conducted to explore the adsorption behaviors of CH 4 over N 2 on ultra-microporous Al/Zr-FDCA frameworks, which were synthesized specifically using the eco-friendly and bio-sourced 2,5-furandicarboxylic acid (FDCA). Characterization results revealed that both Al-FDCA and Zr-FDCA exhibited similar specific surface area and surface groups, leading to comparable methane uptake per-unit mass at atmospheric pressure. However, the presence of Zr nodes generated ultra-micropores around 0.43 nm in size, leading to a pronounced affinity for CH 4 . Zr-FDCA demonstrated a higher CH 4 /N 2 selectivity (8.90) calculated from the isotherms compared to Al-FDCA (3.86). Furthermore, breakthrough experiments indicated that under the same dynamic conditions, Zr-FDCA exhibited 1.5 times higher CH 4 uptake per unit volume and 2.5 times higher CH 4 /N 2 selectivity when compared to Al-FDCA. Initially, a four-step VPSA process was simulated to investigate the separation of CH 4 /N 2 mixture, in which the effects of feed-gas flow rate, adsorption time, adsorption pressure, and desorption pressure in VPSA cycle were extensively evaluated to enhance the purity and recovery of methane. Subsequently, a six-step process was employed for further optimization, achieving a purity of 95.9 % and a recovery of 99.1 %. The obtained results demonstrated the reliability of the established model and highlighted the significant potential of Zr-FDCA for CH 4 /N 2 separation.
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
Nature Energy
·
2022
·Vol. 7
·期 2
·153-162
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IF 67.439
Tang Hongying,Geng Kang,Wu Lei,Liu Junjie,Chen Zhiquan,You Wei,Yan Feng,Guiver Michael D.,Li Nanwen
Conventional proton exchange membrane fuel cells (PEMFCs) operate within narrow temperature ranges. Typically, they are run at either 80‒90 °C using fully humidified perfluorosulfonic acid membranes, or at 140‒180 °C using non-humidified phosphoric acid (PA)-doped membranes, to avoid water condensation-induced PA leaching. However, the ability to function over a broader range of temperature and humidity could simplify heat and water management, thus reducing costs. Here we present PA-doped intrinsically ultramicroporous membranes constructed from rigid, high free volume, Tröger’s base-derived polymers, which allow operation from −20 to 200 °C. Membranes with an average ultramicropore radius of 3.3 Å show a syphoning effect that allows high retention of PA even under highly humidified conditions and present more than three orders of magnitude higher proton conductivity retention than conventional dense PA-doped polybenzimidazole membranes. The resulting PA-doped PEMFCs display 95% peak power density retention after 150 start-up/shut-down cycles at 15 °C and can accomplish over 100 cycles, even at −20 °C.
研究领域:
材料科学
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能源工程
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化学工程
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DOI
高影响因子
MACROMOLECULES
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2025
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IF 5.2
Mengtao Wang,Luxin Sun,Chen Luo,Jiachen Chu,Congcong Wu,Kunying Li,Xuepeng Li,Kai Song,Jianxin Li,Xiaohua Ma
Formation of porous organic polymer (POP) membranes is a great challenge due to their highly cross-linked nature that prevents film formability. Here, we reported a series of mechanically strong POP membranes derived from a cross-linked Tröger’s base using 3,3′-dimethylbiphenyl-4,4′-diamine as a linear monomer and 1,3,5-tris(4-aminophenyl)benzene (TPB) as a cross-linking node. As the TPB content increased from 0% (TPB-0) to 75% (TPB-75), these POP membranes show a continuously decreased chain spacing from 7.96 to 6.22 Å, increased Brunauer–Emmet–Teller surface areas from 250 to 531 m2 g–1, and enhanced ultramicropore volumes from 0.046 to 0.143 cm3. Thereby, a huge increase in permeability without sacrificing selectivity was observed for these TPB-based POP membranes. For example, TPB-75 exhibited not only over 19 times larger O2 permeability (790 vs 50.3 Barrer) but also slightly higher O2/N2 selectivity (4.8 vs 4.5) than the linear TPB-0. The overall separation performances quickly improved from below the 2008 trade-off curves for TPB-0 to near the latest 2015 curves for O2/N2, H2/N2, and H2/CH4 as the TPB content increased. These results are attributed to the significantly improved ultramicroporosity that enhanced the molecular sieving effect by the POP structure induced by in situ cross-linking. This design protocol and the POP membranes provide a novel direction for advanced gas separation membranes.
研究领域:
材料科学
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化学工程
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高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2022
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IF 8.025
Linghong Yin,Pengyu Hu,Chen Liang,Jie Wang,Ming Li,Wangda Qu
Lignin is a renewable biomacromolecule that can be used as precursors for carbon materials. In this work, highly flexible lignin-based carbon nanofibers with abundant ultra-micropores are constructed via electrospinning, oxidative stabilization and carbonization. The results indicate that replacing PAN with 80 % lignin is feasible in regulating ultra-micropores. The synthesized L4P1-CNFs possess many attractive properties (e.g., pore size distribution , electrochemical and deionization property) compared with that produced from other non-renewable precursors or more-complexed processes. It shows excellent electrochemical double-layer capacitance in 6 M KOH (233 to 162 F g −1 at 0.5 to 5 A g −1 ) and 1 M NaCl (158 to 82 F g −1 at 0.5 to 5 A g −1 ) electrolytes. Upon assembling into CDI cells, the average salt adsorption rate could reach 1.79 mg g −1 min −1 at 1.2 V and 3.32 mg g −1 min −1 at 2 V in 500 mg L −1 . Benefiting from the excellent flexibility, we innovatively stack four layers of L4P1-CNFs to improve the areal electrosorption capacity to 0.0817 mg cm −2 at 500 mg L −1 , significantly higher than that of traditional carbon-based electrodes. The good desalination property makes lignin-based carbon nanofibers ideal for practical, low-cost capacitive deionization applications.
研究领域:
材料科学
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环境工程
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化学工程
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PubMed
高影响因子
ACS Applied Engineering Materials
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2023
·
IF 0
Xue Han,Ruisheng Xue
Hypercross-linked porous polymer materials have good stability and can be used as needed by adjusting the hydrophobic/hydrophilic degree of its functional groups/ions and surface, and they can achieve high gas adsorption. In this study, a series of hypercross-linked porous polymer materials with a rich pore structure and excellent gas adsorption ability were synthesized from polynaphthalene and dimethoxymethane by adjusting the added amount of the catalyst and cross-linker. The sample prepared under the optimized conditions of adding 18 mmol catalyst and 9 mmol cross-linker gained the specific surface area of 786 m2 g–1 and 0.58 nm ultramicropores taking up 80% of total pores. In addition, its CO2 uptake was up to 2.75 mmol g–1 at 273.15 K/1.0 bar. After carbonization at 800 °C, this sample had a 710 m2 g–1 specific surface area and a monodisperse pore structure with a pore diameter of about 0.4 nm, and its CO2 uptake increased to 3.81 mmol g–1 at 273.15 K/1.0 bar. The adsorption selectivity coefficients of CO2/N2 and CO2/CH4 for the carbonized sample were 8.5 and 2.3, respectively, by using Henry’s law initial slope method.
研究领域:
材料科学
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化学工程
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环境科学
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DOI
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