Porous materials with pre-designed single-molecule traps for CO2 selective adsorption

Lǐ, Jiànróng; Yu, Jiamei; Lü, Weigang; Sun, Lin‐Bing; Sculley, Julian P.; Balbuena, Perla B.; Zhou, Hong‐Cai

doi:10.1038/ncomms2552

Cited by 545 publications

(334 citation statements)

References 44 publications

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“…Adsorption enthalpy of R22 (34.6 kJ mol À 1 ) is considerably higher in magnitude compared with R12, R13, R14 and R32 (refs 25,26). The Qst values are higher than the standard enthalpy of vaporization for R12, R22 (20 and 28.2 kJ mol À 1 ) and similar to the Qst for MOFs with open metal sites such as MDOBDC (CO 2 as sorbate) 14,29,30 .…”

Section: Mof Selectionmentioning

confidence: 95%

“…Sorbents examined for fluorocarbon-based adsorption chillers have thus far been limited to activated carbon 7,8 and zeolites 9 . Although the literature on gas adsorption in MOFs is very extensive [10][11][12][13][14][15][16][17][18][19] , fluorocarbon adsorption has been limited to zeolites and activated carbons [7][8][9] . The adsorption behaviour of the MOFs with high capacity at very low vapor pressures suggests MOFs can, in principle, be used in fluorocarbon-based adsorption heat pumps, separation of fluorocarbons from azeotrope mixture, removal of environmentally hazardous gases from atmosphere.…”

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confidence: 99%

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Fluorocarbon adsorption in hierarchical porous frameworks

et al. 2014

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Metal-organic frameworks comprise an important class of solid-state materials and have potential for many emerging applications such as energy storage, separation, catalysis and bio-medical. Here we report the adsorption behaviour of a series of fluorocarbon derivatives on a set of microporous and hierarchical mesoporous frameworks. The microporous frameworks show a saturation uptake capacity for dichlorodifluoromethane of 44 mmol g À 1 at a very low relative saturation pressure (P/P o ) of 0.02. In contrast, the mesoporous framework shows an exceptionally high uptake capacity reaching 414 mmol g À 1 at P/P o of 0.4. Adsorption affinity in terms of mass loading and isosteric heats of adsorption is found to generally correlate with the polarizability and boiling point of the refrigerant, with dichlorodifluoromethane 4chlorodifluoromethane 4chlorotrifluoromethane 4tetrafluoromethane 4methane. These results suggest the possibility of exploiting these sorbents for separation of azeotropic mixtures of fluorocarbons and use in eco-friendly fluorocarbon-based adsorption cooling.

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Section: Mof Selectionmentioning

confidence: 95%

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confidence: 99%

Fluorocarbon adsorption in hierarchical porous frameworks

et al. 2014

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“…Several types of MOFs have been proposed for CO 2 capture, including (i) MOFs with open metal sites, [25][26][27][28][29][30][31][32][33][34][35][36][37] (ii) MOFs without open metals sites, [38][39][40][41][42][43][44][45][46][47][48][49][50][51][52][53][54][55] (iii) MOFs with narrow pore size via interpenetration 10,56,57 or shortening the size of the ligands, 10,41 and (iv) MOFs decorated with specific functional groups, including (NH 2 , OH, etc.). 23,51,[58][59][60][61][62][63][64] Functionalization of these types of MOFs may be carried out by post-synthetic modification (PSM) on the open metal sites, 47,[65][66]…”

Section: Discussionmentioning

confidence: 99%

Low concentration CO2 capture using physical adsorbents: Are metal–organic frameworks becoming the new benchmark materials?

Belmabkhout¹,

Guillerm²,

Eddaoudi³

2016

Chemical Engineering Journal

297

168

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KeywordsCO 2 capture, traces CO 2 removal, air capture, physical adsorbents, MOFs AbstractThe capture and separation of traces and concentrated CO 2 from important commodities such as CH 4 , H 2 , O 2 and N 2, is becoming important in many areas related to energy security and environmental sustainability. While trace CO 2 concentration removal applications have been modestly studied for decades, the spike in interest in the capture of concentrated CO 2 was motivated by the need for new energy vectors to replace highly concentrated carbon fuels and the necessity to reduce emissions from fossil fuel-fired power plants. CO 2 capture from various gas streams, at different concentrations, using physical adsorbents, such as activated carbon, zeolites, and metal-organic frameworks (MOFs), is attractive. However, the adsorbents must be designed with consideration of many parameters including CO 2 affinity, kinetics, energetics, stability, capture mechanism, in addition to cost. Here, we perform a systematic analysis regarding the key technical parameters that are required for the best CO 2 capture performance using physical adsorbents. We also experimentally demonstrate a suitable 2 material model of Metal Organic Framework as advanced adsorbents with unprecedented properties for CO 2 capture in a wide range of CO 2 concentration. These recently developed class of MOF adsorbents represent a breakthrough finding in the removal of traces CO 2 using physical adsorption.This platform shows colossal tuning potential for more efficient separation agents.

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“…Recently, we studied MOFs containing predesigned singlemolecule traps (SMTs) for carbon capture, wherein each SMT can trap one CO 2 molecule 10 . If the same concept is applied in enzyme immobilization, we can potentially diminish leaching and encapsulate each enzyme molecule in a SMT to eliminate aggregation, optimizing the catalytic environment.…”

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confidence: 99%

Stable metal-organic frameworks containing single-molecule traps for enzyme encapsulation

et al. 2015

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. However, the engineering of enzymes is severely hampered due to their low operational stability and difficulty of reuse. Here, we develop a series of stable metal-organic frameworks with rationally designed ultra-large mesoporous cages as single-molecule traps (SMTs) for enzyme encapsulation. With a high concentration of mesoporous cages as SMTs, PCN-333(Al) encapsulates three enzymes with record-high loadings and recyclability. Immobilized enzymes that most likely undergo single-enzyme encapsulation (SEE) show smaller K m than free enzymes while maintaining comparable catalytic efficiency. Under harsh conditions, the enzyme in SEE exhibits better performance than free enzyme, showing the effectiveness of SEE in preventing enzyme aggregation or denaturation. With extraordinarily large pore size and excellent chemical stability, PCN-333 may be of interest not only for enzyme encapsulation, but also for entrapment of other nanoscaled functional moieties.

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Porous materials with pre-designed single-molecule traps for CO2 selective adsorption

Cited by 545 publications

References 44 publications

Fluorocarbon adsorption in hierarchical porous frameworks

Fluorocarbon adsorption in hierarchical porous frameworks

Low concentration CO2 capture using physical adsorbents: Are metal–organic frameworks becoming the new benchmark materials?

Stable metal-organic frameworks containing single-molecule traps for enzyme encapsulation

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