Abstract
Achieving structural requirements for the exclusive selectivity of adsorbent to a specific metal remains challenging, as certain metal ions show similar adsorptive behaviors and preference toward a given site. We reported the morphology and oxidation state-dependent selectivity manipulating of layered oxides by controlling the dynamic evolution of different adsorptive sites. The computational investigation predicted the site-specific partitioning trends of metal ions at two sites of manganese oxide (MnO2) layers: the lateral edge sites (LESs) and octahedral vacancy sites (OVSs). In contrast to the predominant occupation of the OVSs for other metal ions, the binding of lead (Pb) ions was energetically favored at both the sites. We assembled ultrathin MnO2 nanosheets on the magnetic iron oxides to first enhance the accessibility of the LESs. A sequential ligand-promoted partial reduction of the atomic MnO2 layers induced the edge-to-interlayer migration of Mn atoms to block the nonspecific OVSs and activate the LESs, enabling a superior selectivity to Pb. In addition, the iron oxides helped construct a multifunctional adsorptive/electrosensing platform for Pb regarding their facile magnetic separation and electrochemical activity. Simultaneous selective adsorption and on-site monitoring of Pb(II) were achieved on this nanoplatform, owing to its satisfactory stability and sensitivity without an obvious matrix effect.
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