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1.
ACS Appl Mater Interfaces ; 10(3): 2414-2422, 2018 Jan 24.
Article in English | MEDLINE | ID: mdl-29278323

ABSTRACT

Eutectic mixtures of alkali nitrates are known to increase the sorption capacity and kinetics of MgO-based sorbents. Underlying principles and mechanisms for CO2 capture on such sorbents have already been established; however, real-time observation of the system was not yet accomplished. In this work, we present the direct-observation of the CO2 capture phenomenon on a KNO3-LiNO3 eutectic mixture (EM)-promoted MgO sample, denoted as KLM, via in situ transmission electron microscopy (in situ TEM). Results revealed that the pseudoliquid EM undergoes structural rearrangement as MgCO3 evolves from the surface of MgO, resulting in surface roughening and evolution of cloudy structures that stay finely distributed after regeneration. From this, we propose a nucleation and structural rearrangement scheme for MgCO3 and EM, which involves the rearrangement of bulk EM to evenly distributed EM clusters due to MgCO3 saturation as adsorption proceeds. We also conducted studies on the interface between EM over solid MgO and MgCO3 formed during sorption, which further clarifies the interaction between MgO and EM. This study provides better insight into the sorption and regeneration mechanism, as well as the structural rearrangements involved in EM-promoted sorbents by basing not only on intrinsic evolutions but also on real-time observation of the system as a whole.

2.
ChemSusChem ; 10(3): 541-550, 2017 02 08.
Article in English | MEDLINE | ID: mdl-28004886

ABSTRACT

A combined sonication and microwave irradiation procedure provides the most effective functionalization of ethylenediamine (en) and branched primary diamines of 1-methylethylenediamine (men) and 1,1-dimethylethylenediamine (den) onto the open metal sites of Mg2 (dobpdc) (1). The CO2 capacities of the advanced adsorbents 1-en and 1-men under simulated flue gas conditions are 19 wt % and 17.4 wt %, respectively, which are the highest values reported among amine-functionalized metal-organic frameworks (MOFs) to date. Moreover, 1-den exhibits both a significant working capacity (12.2 wt %) and superb CO2 uptake (11 wt %) at 3 % CO2 . Additionally, this framework showcases the superior recyclability; ultrahigh stability after exposure to O2 , moisture, and SO2 ; and exceptional CO2 adsorption capacity under humid conditions, which are unprecedented among MOFs. We also elucidate that the performance of CO2 adsorption can be controlled by the structure of the diamine ligands grafted such as the number of amine end groups or the presence of side groups, which provides the first systematic and comprehensive demonstration of fine-tuning of CO2 uptake capability using different amines.


Subject(s)
Carbon Dioxide/chemistry , Diamines/chemistry , Organometallic Compounds/chemistry , Adsorption , Carbon Dioxide/isolation & purification , Models, Molecular , Molecular Conformation , Oxygen/chemistry , Quantum Theory , Steam , Sulfur Dioxide/chemistry , Temperature
3.
J Nanosci Nanotechnol ; 15(10): 7980-7, 2015 Oct.
Article in English | MEDLINE | ID: mdl-26726451

ABSTRACT

Palmitoyl grafted modified cellulose were prepared by simple chemical grafting method and applied as nano adsorbent for removal of pyrene from aqueous solution. The chemical properties and morphology of prepared nano-adsorbent were characterized by FT-IR, XRD, SEM, EDX, TGA, and contact angle. Results showed that palmitoyl successfully grafted on the surface of cellulose and possess effective organic functional groups for the adsorption of pyrene from aqueous solution. The adsorption performance of modified cellulose was significantly improved toward pyrene in aqueous solution. It is worthy to note that 0.25 g of palmitoyl grafted cellulose (PMC) removed 92% pyrene compared to unmodified cellulose which adsorbed 36% pyrene from 1.65 ppm aqueous solution of pyrene in very short contact time at room temperature. Results showed that, presence of various organic functional groups from palmitoyl chains grafted on cellulose backbone affected to pyrene removal. After completion of adsorption phenomenon nano-adsorbent can be removed by simply filtration process and reused several times. The adsorption capacity was studied under different experimental conditions and their effects on adsorption such as temperature, pH, and contact time were also studied. The kinetics and isotherms of material were also determined.


Subject(s)
Cellulose/chemistry , Nanoparticles/chemistry , Palmitic Acid/chemistry , Pyrenes/chemistry , Water Purification/methods , Adsorption
4.
Chem Sci ; 6(7): 3697-3705, 2015 Jul 15.
Article in English | MEDLINE | ID: mdl-28706716

ABSTRACT

An amine-functionalized metal-organic framework (MOF), dmen-Mg2(dobpdc) (dmen = N,N-dimethylethylenediamine), which contains a heterodiamine with both primary and tertiary amines, was prepared via a post-synthetic method. This material exhibits a significant selectivity factor for CO2 over N2 that is commensurate with top-performing MOFs. It is remarkable that the solid is fully regenerated under vacuum or flowing Ar at low desorption temperatures, and following this can take up CO2 at more than 13 wt%. An exceptionally high working capacity is achieved at low regeneration temperatures and after exposure to humid conditions, which are important parameters for a real post-combustion CO2 capture process.

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