X-ray Absorption Spectroscopy Reveals Mechanisms of Calcium and Silicon Fouling on Reverse Osmosis Membranes Used in Wastewater Reclamation

Reverse osmosis (RO) is widely employed to provide clean water from nontraditional sources (e.g., seawater or municipal wastewater). One of its key challenges is membrane fouling, which leads to reduced flux and increased operational costs. Despite its practical relevance, fundamental understanding of membrane fouling is limited. Toward this end, we investigated calcium (Ca) and silicon (Si) fouling under real RO feed conditions using mu-X-ray fluorescence (mu-XRF) mapping and mu-X-ray absorption near-edge fine structure (mu-XANES) spectroscopy. These techniques are distinctly suited to identify the spatial distribution and (local) chemical speciation of foulants, thereby providing unique insight into the mechanisms of fouling under realistic conditions. Specifically, we investigated RO membranes harvested from a pilot-scale RO system operated at the Orange County Water District (OCWD) Ground water Replenishment System (GWRS) Advanced Water Purification (AWP) Facility, which received the same feed water as the full-scale plant. Both Ca and Si were found to be abundant in the fouling layer. Despite the use of a commercial antiscalant to inhibit mineral formation, several Ca minerals were present in the fouling layer as minority species, including sulfates, phosphates, and carbonates; most of these minerals were found in particles that were aligned with the feed spacer used to separate the membranes. In contrast, organic-bound Ca and silica occurred across the entire membrane. Our work provides novel insight into the synergistic mechanism of RO fouling by Ca, Si, and organics on RO membranes.