Resource utilization of organic spent adsorbent to prepare three-dimensional sulfate-functionalized layered double oxide for superior removal of azo dye.

Developing superior, rapid, cost-effective adsorbents derived from organic spent adsorbent is an economically sustainable way for purifying azo dye wastewater. Herein, we report a precursor-calcination strategy for the recycle of the organic spent adsorbent to a high value-added three-dimensional sulfate-functionalized MgAl-layered double oxide (3S-LDO). Thanks to the unique property of the sulfate group and LDO, 3S-LDO exhibited a superior (4340.71 mg/g) and ultrafast (<1 h) adsorption toward methyl orange (MO, as the representative of azo dye). A thermodynamic study revealed that the reaction process was spontaneous and exothermic. FT-IR, XPS, and XRD results confirmed that the sulfate from 3S-LDO played a vital role in MO removal wherein the S=O bond (with the electrophilic character) from SO interacted with the N=N double bond (with rich electron) in MO through the electron donor-acceptor mechanism. And the "memory effect" and surface complexation of 3S-LDO further strengthened the MO adsorption. More importantly, 3S-LDO could work efficiently in a wide pH range and even in the presence of competitive anions (e.g., Cl, NO, and CO). Multiple cyclic runs and selective tests demonstrated the excellent reusability and explicit selectivity of 3S-LDO. This work not only provides a prospective sulfate-functionalized adsorbent from organic waste for rapid azo dye removal from wastewater but also achieves the high value-added utilization of organic waste.