The activation of inert oxygen (O<sub>2</sub>) often consumes enormous amounts of energy and resources, which is a global challenge in the field of environmental remediation and fuel cells. Organic pollutants are abundant in electrons and promising as alternative donors. Here, we implement the sustainable micro-activation of dissolved oxygen (DO) by using the electrons and adsorption energy of pollutants through creating nonequilibrium micro-surface on nanoparticle-integrated molybdenum lattice-doped zinc sulfide composites (MZS-1). It is found that organic pollutants can be quickly removed by DO micro-activation in the MZS-1 system under natural conditions without any additional energy and electron donor. The turnover frequency (TOF, per Mo atom basis) is 5 orders of magnitude higher compared to homogeneous systems. Structural and electronic characterization technologies reveal the change in crystalline phase (Zn-S-Mo) and the activation of the π-electrons on six-membered rings of ZnS after Mo doping, which resulting in the formation of nonequilibrium micro-surface on MZS-1. It is the key for the strong interfacial interaction and directional electron transfer from pollutants to MZS-1 through delocalized π-π conjugation effect and from MZS-1 to DO via Zn-S-Mo, as demonstrated by electron paramagnetic resonance (EPR) techniques and density functional theory (DFT) calculations. This process achieves the efficient use of pollutants and the low-energy activation of O<sub>2</sub> through the construction of nonequilibrium micro-surface, which shows new significance for water treatment.

Sustainable micro-activation of dissolved oxygen driving pollutant conversion on Mo-enhanced zinc sulfide surface in natural conditions

ACS Spring 2022

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