Environmental Science & Technology

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ISSN / EISSN : 0013-936X / 1520-5851
Published by: American Chemical Society (ACS) (10.1021)
Total articles ≅ 50,191
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Qiyang Yan, , Ye Cheng,
Environmental Science & Technology; https://doi.org/10.1021/acs.est.1c03035

Background ozone in this study is defined as the amount of ozone that is not affected by the emissions of ozone precursors in the region of study and is transported from the distant troposphere or the stratosphere. It is one of the factors that must be considered in regional ozone control strategies. Different methods have been applied to define the background ozone level. We develop a new method based on the O3–CO–HCHO relationships, which can be applied to both observation and modeling data for regions with high isoprene emission ozone, such as the Southeast United States. We make use of the extensive aircraft and surface observations in the Southeast in the summer of 2013. Compared to the diagnostic results using the relationship of O3–NOz (total reactive nitrogen excluding nitrogen oxides), zero-emission (model-only), and 5th percentile methods, the new method is most consistent using observation or model data and the resulting background ozone concentrations are 4–50% lower than the other methods for field campaigns. Using this method, we find that the summertime background ozone at the surface is in the range of 10–15 ppbv in the inland areas of the Southeast, which is lower than that reported in previous studies. This background ozone tends to increase from urban centers to rural regions and from the surface to higher altitude due to changing ozone lifetime driven by anthropogenic emissions and dry deposition to the surface. The better quantification of background ozone using the new method highlights the importance of the contributions by natural emissions to ozone and the necessity to control anthropogenic emissions in ozone nonattainment areas of the Southeast.
Kyungho Kim, Jothikumar Narayanan, Anindito Sen,
Environmental Science & Technology; https://doi.org/10.1021/acs.est.0c04438

Virus destabilization and inactivation are critical considerations in providing safe drinking water. We demonstrate that iron electrocoagulation simultaneously removed (via sweep flocculation) and inactivated a non-enveloped virus surrogate (MS2 bacteriophage) under slightly acidic conditions, resulting in highly effective virus control (e.g., 5-logs at 20 mg Fe/L and pH 6.4 in 30 min). Electrocoagulation simultaneously generated H2O2 and Fe(II) that can potentially trigger electro-Fenton reactions to produce reactive oxygen species such as •OH and high valent oxoiron(IV) that are capable of inactivating viruses. To date, viral attenuation during water treatment has been largely probed by evaluating infective virions (as plaque forming units) or genomic damage (via the quantitative polymerase chain reaction). In addition to these existing means of assessing virus attenuation, a novel technique of correlating transmission electron micrographs of electrocoagulated MS2 with their computationally altered three-dimensional electron density maps was developed to provide direct visual evidence of capsid morphological damages during electrocoagulation. The majority of coliphages lost at least 10–60% of the capsid protein missing a minimum of one of the 5-fold and two of 3- and 2-fold regions upon electrocoagulation, revealing substantial localized capsid deformation. Attenuated total reflectance–Fourier transform infrared spectroscopy revealed potential oxidation of viral coat proteins and modification of their secondary structures that were attributed to reactive oxygen species. Iron electrocoagulation simultaneously disinfects and coagulates non-enveloped viruses (unlike conventional coagulation), adding to the robustness of multiple barriers necessary for public health protection and appears to be a promising technology for small-scale distributed water treatment.
Dahong Huang, David J. Kim, Kali Rigby, Xuechen Zhou, Xuanhao Wu, Aidan Meese, , Eli Stavitski,
Environmental Science & Technology; https://doi.org/10.1021/acs.est.1c04294

In this study, we loaded Pd catalysts onto a reduced graphene oxide (rGO) support in an atomically dispersed fashion [i.e., Pd single-atom catalysts (SACs) on rGO or Pd1/rGO] via a facile and scalable synthesis based on anchor-site and photoreduction techniques. The as-synthesized Pd1/rGO significantly outperformed the Pd nanoparticle (Pdnano) counterparts in the electrocatalytic hydrodechlorination of chlorinated phenols. Downsizing Pdnano to Pd1 leads to a substantially higher Pd atomic efficiency (14 times that of Pdnano), remarkably reducing the cost for practical applications. The unique single-atom architecture of Pd1 additionally affects the desorption energy of the intermediate, suppressing the catalyst poisoning by Cl–, which is a prevalent challenge with Pdnano. Characterization and experimental results demonstrate that the superior performance of Pd1/rGO originates from (1) enhanced interfacial electron transfer through Pd–O bonds due to the electronic metal–support interaction and (2) increased atomic H (H*) utilization efficiency by inhibiting H2 evolution on Pd1. This work presents an important example of how the unique geometric and electronic structure of SACs can tune their catalytic performance toward beneficial use in environmental remediation applications.
Xiaochi Liu, , C. Marjorie Aelion, Chenyin Dong
Environmental Science & Technology; https://doi.org/10.1021/acs.est.1c01097

Blood lead (Pb) poisoning remains a global concern, particularly for children in their early developmental years. Broken Hill is Australia’s oldest operating silver–zinc–lead mine. In this study, we utilized recent advances in machine learning to assess multiple algorithms and identify the most optimal model for predicting childhood blood Pb levels (BLL) using Broken Hill children’s (<5 years of age) data (n = 23,749) from 1991 to 2015, combined with demographic, socio-economic, and environmental influencing factors. We applied model-agnostic methods to interpret the most optimal model, investigating different environmental and human factors influencing childhood BLL. Algorithm assessment showed that stacked ensemble, a method for automatically and optimally combining multiple prediction algorithms, enhanced predictive performance by 1.1% with respect to mean absolute error (p < 0.01) and 2.6% for root-mean-squared error (p < 0.01) compared to the best performing constituent algorithm (random forest). By interpreting the model, the following information was acquired: children had higher BLL if they resided within 1.0 km to the central mine area or 1.37 km to the railroad; year of testing had the greatest interactive strength with all other factors; BLL increased faster in Aboriginal than in non-Aboriginal children at 9–10 and 12–18 months of age. This “stacked ensemble + model-agnostic interpretation” framework achieved both prediction accuracy and model interpretability, identifying previously unconnected variables associated with elevated childhood BLL, offering a marked advantage over previous works. Thus, this approach has a clear value and potential for application to other environmental health issues.
Rachel T. Mason, , Hung Tan, Jack A. Brand, Michael G. Bertram, Reid Tingley, Andrew Todd-Weckmann, Bob B. M. Wong
Environmental Science & Technology; https://doi.org/10.1021/acs.est.1c04084

Behavior-modifying drugs, such as antidepressants, are increasingly being detected in waterways and aquatic wildlife around the globe. Typically, behavioral effects of these contaminants are assessed using animals tested in social isolation. However, for group-living species, effects seen in isolation may not reflect those occurring in realistic social settings. Furthermore, interactions between chemical pollution and other stressors, such as predation risk, are seldom considered. This is true even though animals in the wild are rarely, if ever, confronted by chemical pollution as a single stressor. Here, in a 2 year multigenerational experiment, we tested for effects of the antidepressant fluoxetine (measured concentrations [±SD]: 42.27 ± 36.14 and 359.06 ± 262.65 ng/L) on shoaling behavior in guppies (Poecilia reticulata) across different social contexts and under varying levels of perceived predation risk. Shoaling propensity and shoal choice (choice of groups with different densities) were assessed in a Y-maze under the presence of a predatory or nonpredatory heterospecific, with guppies tested individually and in male–female pairs. When tested individually, no effect of fluoxetine was seen on shoaling behavior. However, in paired trials, high-fluoxetine-exposed fish exhibited a significantly greater shoaling propensity. Hence, effects of fluoxetine were mediated by social context, highlighting the importance of this fundamental but rarely considered factor when evaluating impacts of environmental pollution.
Environmental Science & Technology; https://doi.org/10.1021/acs.est.1c04370

Iron oxychloride (FeOCl) has been reported to be a highly efficient heterogeneous Fenton catalyst over a wide pH range. In order to determine the true catalytic performance of FeOCl, we simultaneously quantified the adsorptive and oxidative removal of formate, oxalate, and rhodamine-B (RhB) and the formation of RhB oxidation products at both pH 4.0 and 7.0. FeOCl was found to be a poor Fenton catalyst at either pH, as gauged by the oxidation of formate, oxalate, and rhodamine B and the decomposition of H2O2, in comparison with ferrihydrite (Fhy), one of the most common Fe-containing Fenton catalysts. The adsorption of target contaminants to FeOCl and homogeneous Fenton processes, induced by dissolved iron, resulted in overevaluation of the catalytic performance of FeOCl, especially for (i) the use of strongly adsorbing target compounds, without consideration of the role of adsorption in their removal and (ii) exceedingly high concentrations of H2O2 to remove trace quantities of target contaminants. Overall, this study highlights that the systematic quantification of H2O2 decomposition, target compound adsorption, and oxidation as well as the concentrations of oxidized products formed are prerequisites for unequivocal elucidation of the catalytic nature and reaction mechanism of solid Fenton catalysts.
Environmental Science & Technology; https://doi.org/10.1021/acs.est.1c01641

On-demand ridesourcing services from transportation network companies (TNCs), such as Uber and Lyft, have reshaped urban travel and changed externality costs from vehicle emissions, congestion, crashes, and noise. To quantify these changes, we simulate replacing private vehicle travel with TNCs in six U.S. cities. On average, we find a 50–60% decline in air pollutant emission externalities from NOx, PM2.5, and VOCs due to avoided “cold starts” and relatively newer, lower-emitting TNC vehicles. However, increased vehicle travel from deadheading creates a ∼20% increase in fuel consumption and associated greenhouse gas emissions and a ∼60% increase in external costs from congestion, crashes, and noise. Overall, shifting private travel to TNCs increases external costs by 30–35% (adding 32–37 ¢ of external costs per trip, on average). This change in externalities increases threefold when TNCs displace transit or active transport, drops by 16–17% when TNC vehicles are zero-emission electric, and potentially results in reduced externalities when TNC rides are pooled.
Shuhan Liu, , Xiaoxuan Bai, Chuanyong Zhu, Bobo Wu, Lining Luo, Yan Hao, Wei Liu, Shumin Lin, Shuang Zhao, et al.
Environmental Science & Technology; https://doi.org/10.1021/acs.est.1c01775

Airborne trace elements (TEs) pose a notable threat to human health due to their toxicity and carcinogenicity, whereas their exposures and associated health risks in China remain unclear. Here, we present the first nationwide assessment of spatiotemporal exposure to 11 TEs in China by coupling a bottom-up emission inventory with a modified CMAQ model capable of TE simulation. Associated health risks of 11 TEs are then evaluated using a set of risk assessment models. Our results show that the CMAQ model could reasonably reproduce the spatiotemporal variations of 11 TEs in China compared to observations. We find significant but spatiotemporal-heterogeneous cancer risks associated with high-level exposure of TEs in China. Gridded cell concentrations of hexavalent chromium, arsenic, and nickel in eastern and central China usually exceed China’s air quality standard limits, resulting in significant cancer risks that affected over 85% of the entire population in China in 2015. National annual mean population-weighted concentrations of 11 TEs decrease by 9.8–35.6% from 2012 to 2015, largely attributed to emission reduction from coal combustion. Our study provides critical insights for policymakers to implement stricter measures to alleviate health burdens and benefit relevant epidemiological research on airborne TEs.
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