Conspectus Providing access to safe drinking water is a prerequisite for protecting public health. Vast improvements in drinking water quality have been witnessed during the last century, particularly in urban areas, thanks to the successful implementation of large, centralized water treatment plants and the distribution of treated water via underground networks of pipes. Nevertheless, infection by waterborne pathogens through the consumption of biologically unsafe drinking water remains one of the most significant causes of morbidity and mortality in developing rural areas. In these areas, the construction of centralized water treatment and distribution systems is impractical due to high capital costs and lack of existing infrastructure. Improving drinking water quality in developing rural areas demands a paradigm shift to unconventional, innovative water disinfection strategies that are low cost and simple to implement and maintain, while also requiring minimal infrastructure. The implementation of point-of-use (POU) disinfection techniques at the household- or community-scale is the most promising intervention strategy for producing immediate health benefits in the most vulnerable rural populations. Among POU techniques, solar-driven processes are considered particularly instrumental to this strategy, as developing rural areas that lack safe drinking water typically receive higher than average surface sunlight irradiation. Materials that can efficiently harvest sunlight to produce disinfecting agents are pivotal for surpassing the disinfection performance of conventional POU techniques. In this account, we highlight recent advances in materials and processes that can harness sunlight to disinfect water. We describe the physicochemical properties and molecular disinfection mechanisms for four categories of disinfectants that can be generated by harvesting sunlight: heat, germicidal UV radiation, strong oxidants, and mild oxidants. Our recent work in developing materials-based solar disinfection technologies is discussed in detail, with particular focus on the materials’ mechanistic functions and their modes of action for inactivation of three common types of waterborne pathogens (i.e., bacteria, virus, and protozoa). We conclude that different solar disinfection technologies should be applied depending on the source water quality and target pathogen due to significant variations on susceptibility of microbial components to disparate disinfectants. In addition, we expect that ample research opportunities exist on reactor design and process engineering for scale-up and improved performance of these solar materials, while accounting for the infrastructure demand and capital input. Although the practical implementation of new treatment techniques will face social and economic challenges that cannot be overlooked, novel technologies such as these can play a pivotal role in reducing water borne disease burden in rural communities in the developing world.

Separating the redox sites of photocatalysts is one of most promising strategies to promote an efficient photoinduced charge transfer of semiconductor photocatalysis. Herein, we present a site-selective loading of single-atom Pt (Pt1) on facet-engineered TiO2 to achieve decomposition of recalcitrant halogenated water pollutants, including perfluorooctanoic acid (PFOA). Positively charged Pt1 are atomically dispersed catalytic sites that are selectively loaded onto the reductive sites of tailored TiO2 to attract the photoinduced electrons efficiently. This enhances the number of holes, and consequently hydroxyl radicals, remaining on the sites of facet-engineered TiO2, confirmed by the enhancement of degradation of sulfamethoxazole and 2,4-dichlorophenoxyacetic acid. While Pt nanoparticle cocatalysts consume photoinduced electrons for the reduction of oxygen molecules, site-specifically loaded Pt1 produce surface hydrogen atoms and enhance hydrogen spillover onto the TiO2 surface, to achieve efficient hydrodefluorination of PFOA via the cleavage of the C–F bond with the Ti–H bond. The site-selective loading of Pt1 on facet-engineered TiO2 serves as a versatile platform that harnesses both reductive and oxidative degradation of emerging aqueous pollutants.

Although adsorption has gained favor among numerous water treatment technologies as an effective pollutant removal method, its application is often hindered by challenges with its resource- and energy-intensive regeneration procedure once the available adsorption sites are exhausted. Herein, we present adsorption–photocatalysis composite materials combining layered double hydroxides (LDHs) and titanium dioxide (TiO2) for water treatment. Incorporation of the photocatalyst into the material opens opportunities to harness light from the sun or lamps for oxidative degradation of the adsorbed contaminants on the material surface, to free adsorption sites for material reuse. In addition to allowing photocatalytic regeneration, the addition of TiO2 to colloidal suspensions of delaminated LDH enabled the formation of TiO2–LDH composites with far superior adsorptive performances compared to their parent LDH compounds. During the material synthesis, positively charged LDH layers and negatively charged TiO2 particles combine through electrostatic attraction to yield composites with dramatically enhanced adsorption capacities toward model contaminants, methyl orange and 2,4-dichlorophenoxyacetic acid, by 16.0 and 76.7 times, respectively. Combining delaminated LDH with TiO2 allowed us to maximize the exposure of positively charged surfaces to the contaminants, in a form that can be used as a solid adsorbent. After regeneration, the material regained up to 92% of its adsorption efficiency toward model contaminants. In light of our findings showing significantly different kinetics of adsorption and photocatalytic regeneration, we propose a new scheme to utilize adsorption–photocatalysis systems, in which the two processes are separated to better utilize their unique strengths.

High chlorine doses (50–200 mg/L) are used in postharvest washing facilities to control foodborne pathogen outbreaks. However, chlorine can react with biopolymers (e.g., lipids) within the produce to form chlorinated byproducts that remain in the food. During chlorination of micelles of oleic acid, an 18-carbon alkene fatty acid, chlorine added rapidly across the double bond to form the two 9,10-chlorohydrin isomers at a 100% yield. The molar conversion of lipid-bound oleic acid to 9,10-chlorohydrins in chlorine-treated glyceryl trioleate and produce was much lower, reflecting the restricted access of chlorine to lipids. Yields from spinach treated with 100 mg/L chlorine at 7.5 °C for 2 min increased from 0.05% (0.9 nmol/g-spinach) for whole leaf spinach to 0.11% (2 nmol/g) when shredding increased chlorine access. Increasing temperature (21 °C) and chlorine contact time (15 min) increased yields from shredded spinach to 0.83% (22 nmol/g) at 100 mg/L chlorine and to 1.8% (53 nmol/g) for 200 mg/L chlorine. Oleic acid 9,10-chlorohydrin concentrations were 2.4–2.7 nmol/g for chlorine-treated (100 mg/L chlorine at 7.5 °C for 2 min) broccoli, carrots, and butterhead lettuce, but 0.5–1 nmol/g for cabbage, kale, and red leaf lettuce. Protein-bound chlorotyrosine formation was higher in the same vegetables (5–32 nmol/g). The Chinese hamster ovary cell chronic cytotoxicity LC50 value for oleic acid 9,10-chlorohydrins was 0.106 mM. The cytotoxicity associated with the chlorohydrins and chlorotyrosines in low masses (9–52 g) of chlorine-washed vegetables would be comparable to that associated with trihalomethanes and haloacetic acids at levels of regulatory concern in drinking water.

No abstract