Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 11, Issue 1, Pages 1426-1439Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.8b17479
Keywords
adsorption; MOFs; COPs; formaldehyde; HPLC
Funding
- R&D Center for Green Patrol Technologies through the R&D for Global Top Environmental Technologies - Ministry of Environment (MOE) [2018001850001]
- National Research Foundation of Korea (NRF) - Ministry of Science, ICT, & Future Planning [2016R1E1A1A01940995]
- Korea Ministry of Environment (MOE) as part of The Chemical Accident Prevention Technology Development Project [2015001950001]
- Department of Science and Technology (DST) [JNC/AO/A.0610(36)2017-2620]
- SERB, Government of India [YSS/2015/000212]
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Porous materials have been identified as efficient sorbent media to remove volatile organic compounds. To evaluate their potential as adsorbents, the adsorptive removal of formaldehyde (FA) in aqueous environments was investigated using four materials, two water-stable metal organic frameworks (MOFs) of UiO-66 (U6) and U6-NH2 (U6N) and two covalent organic polymers (COPs) with amine-functionality, CBAP-1-EDA (CE) and CBAP-1-DETA (CD). U6N exhibited the highest removal capacity of 93% (0.56 mg g(-1)) of the tested materials [e.g., CE (81.1%, 0.53 mg g(-1)) > CD (67.2%, 0.43 mg g(-1)) > U6 (66.9%, 0.42 mg g(-1))], which was 2 times higher than that of the reference sorbent, activated carbon (AC: 50%, 0.30 mg g(-1)). The results of Fourier transform infrared and powder X-ray diffraction analyses confirmed the interactions between FA molecules and the amine components of the materials (U6N, CD, and CE). According to density functional theory calculations, the formation of hydrogen bonds between FA molecules and amine components was apparent and was further verified by FA/amine distance (CD: 2.83, CE: 2.88, and U6N: 2.66 A) along with enthalpy values (CD: 32.4, CE: 45.5, and U6N: 272 kJ mol(-1)). In case of U6, the major interactions occurred in the metal clusters (-19.3 kJ mol(-1)) via electrostatic interactions (distance: 5.49 A). Furthermore, the sorption by amine-functionalized materials such as U6N is suggested to be dominated by hydrogen bonding which ultimately led to the formation of imine. If the performance of the tested materials is evaluated in terms of partition coefficient, U6N (1153 mg g(-1) mM(-1)) is found as the outperformer in all tested subjects. Regeneration of spent MOFs/COPs was also plausible in the presence of ethanol to maintain their structural integrity even after 10 adsorption desorption cycles. Overall, the selected MOFs/COPs were seen to have very high removal capacity for hazardous FA molecules in aqueous phase.
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