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Abstract
Herein, we present a scalable approach for the synthesis of a hydrogen-bonded organic–inorganic framework via coordination-driven supramolecular chemistry, for efficient remediation of trace heavy metal ions from water. In particular, using copper as our model ion of interest and inspired by nature’s use of histidine residues within the active sites of various copper binding proteins, we design a framework featuring pendant imidazole rings and copper-chelating salicylaldoxime, known as zinc imidazole salicylaldoxime supramolecule. This material is water-stable and exhibits unprecedented adsorption kinetics, up to 50 times faster than state-of-the-art materials for selective copper ion capture from water. Furthermore, selective copper removal is achieved using this material in a pH range that was proven ineffective with previously reported metal–organic frameworks. Molecular dynamics simulations show that this supramolecule can reversibly breathe water through lattice expansion and contraction, and that water is initially transported into the lattice through hopping between hydrogen-bond sites.
Heavy metals and metalloids pose major threats to health and environmental ecosystems, thus systems for low-cost remediation are needed. Here the authors report the scalable design of a hydrogen-bonded organic–inorganic framework for selective removal of trace heavy metal ions from water.
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1 The Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, USA (GRID:grid.184769.5) (ISNI:0000 0001 2231 4551); The School of Chemical, Biological and Materials Engineering and the School of Civil Engineering and Environmental Science, the University of Oklahoma, Norman, USA (GRID:grid.266900.b) (ISNI:0000 0004 0447 0018)
2 The Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, USA (GRID:grid.184769.5) (ISNI:0000 0001 2231 4551); Department of Mechanical Engineering, University of California, Berkeley, USA (GRID:grid.47840.3f) (ISNI:0000 0001 2181 7878)
3 Advanced Light Sources, Lawrence Berkeley National Laboratory, Berkeley, USA (GRID:grid.184769.5) (ISNI:0000 0001 2231 4551)
4 National Synchrotron Radiation Research Center, Hsinchu Science Park, Hsinchu, Taiwan (GRID:grid.410766.2) (ISNI:0000 0001 0749 1496)
5 The Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, USA (GRID:grid.184769.5) (ISNI:0000 0001 2231 4551)
6 Departments of Chemistry, University of California, Berkeley, USA (GRID:grid.47840.3f) (ISNI:0000 0001 2181 7878)
7 Departments of Chemistry, University of California, Berkeley, USA (GRID:grid.47840.3f) (ISNI:0000 0001 2181 7878); Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, USA (GRID:grid.184769.5) (ISNI:0000 0001 2231 4551); Chemical and Biomolecular Engineering, University of California, Berkeley, USA (GRID:grid.47840.3f) (ISNI:0000 0001 2181 7878)
8 Water-Energy Resilience Research Institute, Lawrence Berkeley National Laboratory, Berkeley, USA (GRID:grid.184769.5) (ISNI:0000 0001 2231 4551)
9 Energy Storage and Distributed Resources Division, Lawrence Berkeley National Laboratory, Berkeley, USA (GRID:grid.184769.5) (ISNI:0000 0001 2231 4551)