Quantum chemistry unifies phosphorus removal and recovery through environmental affinity

Phosphorus is both a finite resource and a driver of eutrophication, making its sustainable management a persistent challenge. Efficient removal and recovery require a mechanistic understanding of how phosphate speciation, surface chemistry, interfacial water, and coexisting solutes regulate phosphorus adsorption, transformation, and release at solid-liquid interfaces. These interactions create competing requirements, where strong binding favors removal but may hinder recovery, whereas excessive mobility enhances availability but increases environmental risk. These trade-offs are governed by environmental affinity, which describes how thermodynamic retention, kinetic accessibility, reversibility, selectivity, and structural stability jointly regulate phosphorus behavior at environmental interfaces. Quantum-chemical (QC) descriptors such as adsorption free energy, activation barriers, desorption energetics, and structural stability metrics provide molecular-level measures of this affinity and link interfacial interactions to removal efficiency, recovery feasibility, and environmental persistence. This review reframes phosphorus removal and recovery as an interaction-controlled problem and positions QC as a unifying tool to resolve the trade-offs between binding, release, and environmental stability. Methodologically, this review combines bibliometric mapping of 350 phosphorus-related studies retrieved from the Web of Science database with a critical synthesis of 144 studies explicitly using QC, organized by target system, research theme, computational method, and reported descriptors. This synthesis shows that current QC studies are dominated by adsorption-oriented applications, particularly phosphate binding on metal oxides, hydroxides, and framework materials, as well as organophosphorus transformation pathways. By contrast, recovery-oriented descriptors, including desorption free energy, regenerant-surface interactions, and cycling-related structural stability, remain much less systematically reported. Across these studies, phosphate speciation, surface protonation, solvation, ion pairing, and interfacial water emerge as major factors that can shift predicted binding modes, reaction barriers, and reversibility. The review further identifies inconsistent environmental representations and non-standardized computational protocols as key sources of uncertainty and highlights standardized QC datasets and active-learning workflows as near-term priorities for QC-AI integration. These insights enable a unified understanding of how interfacial interactions control phosphorus binding, release, and transformation, providing a basis for tuning reversibility and selectivity across environmental conditions and thereby advancing both phosphorus recovery and pollution control.