6533b83afe1ef96bd12a702d

RESEARCH PRODUCT

Fine-tuning of the confined space in microporous metal–organic frameworks for efficient mercury removal

Xiaoni QuXiaoni QuEmilio PardoDonatella ArmentanoEnrique V. Ramos-fernandezJohannes C. JansenIsaac Pellicer-carreñoAntonio Sepúlveda-escribanoJesús Ferrando-soriaMarta Mon

subject

Fine-tuningmercuryInorganic chemistrychemistry.chemical_element02 engineering and technology010402 general chemistry01 natural sciencesmetal organic frameworkMercury removalAdsorptionOrganic chemistryGeneral Materials ScienceConfined spaceMOFQuímica InorgánicaMetal–organic frameworksAqueous mediumRenewable Energy Sustainability and the EnvironmentGeneral ChemistryMicroporous materialheavy metal021001 nanoscience & nanotechnology0104 chemical sciencesMercury (element)Contaminated waterAqueous mediachemistryMetal-organic framework0210 nano-technology

description

Offsetting the impact of human activities on the biogeochemical cycle of mercury has become necessary for a sustainable planet. Herein, we report the development of a water-stable and eco-friendly metal–organic framework, which has the formula {Cu4II[(S,S)-methox]2}·5H2O (1), where methox is bis[(S)-methionine]oxalyl diamide. Its features include narrow functional channels decorated with thioalkyl chains, which are able to capture HgCl2 from aqueous media in an efficient, selective, and rapid manner. The conscious design effort in terms of size, shape, and reactivity of the channels results in extremely efficient immobilization of HgCl2 guest species in a very stable conformation, similar to that of the enzyme mercury reductase. Thus, 1 enables the highly efficient removal of toxic HgCl2 from aqueous media and reduces the [Hg2+] concentration from the dangerous level of 10 ppm to acceptable limits of below 2 ppb in drinking water. The unusual combination of a low-cost straightforward synthetic procedure and high stability under environmental conditions, together with its ability to efficiently and rapidly remove poisonous mercury ions, places 1 among the most attractive adsorbents reported to date for the purification of contaminated water. This work was supported by the MINECO (Spain) (Project CTQ2016-75671-P and Excellence Unit “Maria de Maeztu” MDM-2015-0538), the Generalitat Valenciana (Spain) (Project PROMETEOII/2014/070), and the Ministero dell'Istruzione, dell'Università e della Ricerca (Italy). M. M. and X. Q. thank the MINECO and the China Scholarship Council for grants. Thanks are also extended to the Ramón y Cajal program (E. P and E. V. R.-F.).

https://doi.org/10.1039/c7ta06199d