High-performance biochar-loaded MgAl-layered double oxide adsorbents derived from sewage sludge towards nanoplastics removal: Mechanism elucidation and QSAR modeling

Utilization of sewage sludge for the fabrication of environmental functional materials is highly desirable to achieve pollution mitigation and resource recovery. In the present work, we introduced a novel MgAl-layered double oxide (LDO)@biochar composite adsorbent in-situ fabricated from Al-rich sewage sludge, and its excellent application in nanoplastics adsorption. Initially, fifteen model contaminants with varied conjugate structures, hydrogen bonding and ionic properties were selected for an investigation of adsorption behavior and adsorption selectivity on LDO@biochar. Structural variation of LDO@biochar suggested reconstruction of the layered double hydroxide (LDH) during the adsorption process due to the "memory effect". Under the synergy of LDH and biochar, the contaminants were adsorbed via multiple adsorbent-adsorbate interactions, including anion exchange, electrostatic interaction, hydrogen bonding and π-π conjugation. Then, a quantitative structure-activity relationship (QSAR) model was constructed by integrating the number of hydrogen bond acceptors, polarity surface area, number of aromatic rings, and Fukui index f(-) together to reflect the affinity of each contaminant to the adsorbent. Guided by the QSAR model, the negatively charged polystyrene nanoplastics with continuously conjugated aromatic rings were predicted to be effectively adsorbed on LDO@biochar. Experimental tests confirmed a great capacity of LDO@biochar towards the polystyrene nanoplastics, given the equilibrium adsorption capacity as high as 360 mg g at 30-50 °C. This work not only opened up a new avenue for sustainable utilization of sewage sludge towards high-performance environmental functional materials, but also demonstrated the potential of the QSAR analysis as a rapid and accurate approach for guiding the application of an adsorbent to new emerging containments.