{"title":"Accelerated Indirect Photodegradation of Organic Pollutants at the Soil–Water Interface","authors":"Binbin Wu, Jingyi Wang, Xingyi He, Hengyi Dai, Xiaoshan Zheng, Junye Ma, Yu Yao, Dantong Liu, Wanchao Yu, Baoliang Chen and Chiheng Chu*, ","doi":"10.1021/acs.est.4c0699310.1021/acs.est.4c06993","DOIUrl":"https://doi.org/10.1021/acs.est.4c06993https://doi.org/10.1021/acs.est.4c06993","url":null,"abstract":"<p >Indirect photolysis driven by photochemically produced reactive intermediates (PPRIs) is pivotal for the transformations and fates of pollutants in nature. While well-studied in bulk water, indirect photolysis processes at environmental interfaces remain largely unexplored. This study reveals a significant acceleration of indirect photodegradation of organic pollutants at the soil–water interface of wetlands. Organic pollutants experienced ubiquitously enhanced indirect photodegradation at the soil–water interfaces, with rates 1.41 ± 0.01 to 4.27 ± 0.03-fold higher than those in bulk water. This enhancement was observed across various natural and artificial wetlands, including coastal wetlands and rice paddies. <i>In situ</i> mapping indicated that soil–water interfaces act as hotspots, concentrating both organic pollutants and PPRIs by 9.30- and 4.27-folds, respectively. This synchronized colocation is the primary cause of the accelerated pollutant photolysis. Additionally, the contribution of each PPRI species to pollutant photolysis and a coupled transformation pathway at the soil–water interface significantly differed from those in bulk water. For instance, the contribution of singlet oxygen to metoxuron photolysis increased from 10.1% in bulk water to 44.4% at the soil–water interface. Our study highlights the rapid indirect photolysis of organic pollutants at the soil–water interfaces, offering new insights into the natural purification processes in wetlands as “Earth’s kidneys.”</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 45","pages":"20181–20189 20181–20189"},"PeriodicalIF":10.8,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609047","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Central SciencePub Date : 2024-10-29DOI: 10.1021/acs.est.4c0773710.1021/acs.est.4c07737
Qiong Zhang*, Matthew J. Eckelman, Guangtao Fu, Sai Liang, James R. Mihelcic, Weiwei Mo and Julie B. Zimmerman,
{"title":"Systems Approaches for Addressing Complex Environmental Problems","authors":"Qiong Zhang*, Matthew J. Eckelman, Guangtao Fu, Sai Liang, James R. Mihelcic, Weiwei Mo and Julie B. Zimmerman, ","doi":"10.1021/acs.est.4c0773710.1021/acs.est.4c07737","DOIUrl":"https://doi.org/10.1021/acs.est.4c07737https://doi.org/10.1021/acs.est.4c07737","url":null,"abstract":"","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 43","pages":"19093–19094 19093–19094"},"PeriodicalIF":10.8,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142550295","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Central SciencePub Date : 2024-10-29DOI: 10.1021/acs.est.4c0637110.1021/acs.est.4c06371
Brendan P. Harrison*, Wilson H. McNeil, Tao Dai, J. Elliott Campbell and Corinne D. Scown,
{"title":"Site Suitability and Air Pollution Impacts of Composting Infrastructure for California’s Organic Waste Diversion Law","authors":"Brendan P. Harrison*, Wilson H. McNeil, Tao Dai, J. Elliott Campbell and Corinne D. Scown, ","doi":"10.1021/acs.est.4c0637110.1021/acs.est.4c06371","DOIUrl":"https://doi.org/10.1021/acs.est.4c06371https://doi.org/10.1021/acs.est.4c06371","url":null,"abstract":"<p >California’s organic waste diversion law, SB 1383, mandates a 75% reduction in organics disposal by 2025 to reduce landfill methane emissions. Composting will likely be the primary alternative to landfilling, and 75–100 new large-scale composting facilities must be sited in the state to meet its diversion goal. We developed a strategy for evaluating site suitability for commercial composting by incorporating land-use, economic, and environmental justice criteria. In our Baseline scenario, we identified 899 candidate sites, and nearly all are within a cost-effective hauling distance of cropland and rangelands for compost application. About half of sites, mostly in rural areas, are not within a cost-effective collection distance of enough municipal organics to supply an average-sized facility. Conversely, sites near cities have greater access to organics but cause greater health damages from ammonia and volatile organic compounds emitted during the composting process. The additional required composting capacity corresponds to $266–355 million in annual damages from air pollution. However, this excludes avoided emissions from landfilling, and damages could be reduced by 56% if aerated static piles are used instead of windrows. Siting a higher number of smaller decentralized facilities could also help equally distribute air pollution to avoid concentrating burdens in certain communities.</p><p >We identified and analyzed suitable compost facility sites in California to help the state meet its organic waste diversion law.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 45","pages":"19913–19924 19913–19924"},"PeriodicalIF":10.8,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.est.4c06371","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608960","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Central SciencePub Date : 2024-10-29DOI: 10.1021/acs.est.4c0656610.1021/acs.est.4c06566
Yuna Gu, Qiancheng Xia, Bin Liu, Yang Zhao, Liangtao Pu, Jie Ding, Yanbiao Liu, Enze Li, Chad D. Vecitis* and Guandao Gao*,
{"title":"Electric Demulsification Membrane Technology for Confined Separation of Oil–Water Emulsions","authors":"Yuna Gu, Qiancheng Xia, Bin Liu, Yang Zhao, Liangtao Pu, Jie Ding, Yanbiao Liu, Enze Li, Chad D. Vecitis* and Guandao Gao*, ","doi":"10.1021/acs.est.4c0656610.1021/acs.est.4c06566","DOIUrl":"https://doi.org/10.1021/acs.est.4c06566https://doi.org/10.1021/acs.est.4c06566","url":null,"abstract":"<p >Demulsification technology for separation of oil–water (O/W) emulsions, especially those stabilized by surfactants, is urgently needed yet remains highly challenging due to their inherent stability characteristics. Electrocoalescence has emerged as a promising solution owing to its simplicity, efficacy, and versatility, yet hindered by substantial energy consumption (e.g., >50 kWh/m<sup>3</sup>) along with undesirable Faradic reactions. Herein, we propose an innovative electric demulsification technology that leverages conductive membrane microchannels to confine oil droplets from the oil–water emulsion for achieving high energy-efficient coalescence of oil droplets. The proposed system reduces the required voltage down to 12 V, 2 orders of magnitude lower than that of conventional electrocoalescence systems, while achieving a similar separation efficacy of 91.4 ± 3.0% at a low energy consumption (3 kWh/m<sup>3</sup>) and an ultrahigh permeability >3000 L/(m<sup>2</sup>·h·bar). <i>In situ</i> fluorescence microscopy combined with COMSOL simulations provided insight into the fundamental mechanistic steps of an electric demulsification process confined to membrane microchannels: (1) rapid electric-field redistribution of oil droplet surfactant molecules, (2) enhanced collision probability due to confined oil droplet concentration under dielectrophoretic forces, and (3) increased collision efficacy facilitated by the membrane pore structure. This strategy may revolutionize the next generation of demulsification and oil–water separation innovations.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 45","pages":"20277–20288 20277–20288"},"PeriodicalIF":10.8,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609694","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Central SciencePub Date : 2024-10-29DOI: 10.1021/acs.est.4c0961110.1021/acs.est.4c09611
Jun-Jie Zhu, Alexandria B. Boehm and Zhiyong Jason Ren*,
{"title":"Environmental Machine Learning, Baseline Reporting, and Comprehensive Evaluation: The EMBRACE Checklist","authors":"Jun-Jie Zhu, Alexandria B. Boehm and Zhiyong Jason Ren*, ","doi":"10.1021/acs.est.4c0961110.1021/acs.est.4c09611","DOIUrl":"https://doi.org/10.1021/acs.est.4c09611https://doi.org/10.1021/acs.est.4c09611","url":null,"abstract":"","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 45","pages":"19909–19912 19909–19912"},"PeriodicalIF":10.8,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609692","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Central SciencePub Date : 2024-10-29DOI: 10.1021/acs.est.4c1115710.1021/acs.est.4c11157
Xiao-Na Zhao, Yu-Lei Liu, Zhuang-Song Huang, Jinfeng Lu, Yue Cao, Jing-Xiao Wang, Zhiqiang Chen, Jun Ma and Lu Wang*,
{"title":"Correction to “Understanding Variations in Ferrate Detection through the ABTS Method in the Presence of Electron-Rich Organic Compounds”","authors":"Xiao-Na Zhao, Yu-Lei Liu, Zhuang-Song Huang, Jinfeng Lu, Yue Cao, Jing-Xiao Wang, Zhiqiang Chen, Jun Ma and Lu Wang*, ","doi":"10.1021/acs.est.4c1115710.1021/acs.est.4c11157","DOIUrl":"https://doi.org/10.1021/acs.est.4c11157https://doi.org/10.1021/acs.est.4c11157","url":null,"abstract":"","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 45","pages":"20328 20328"},"PeriodicalIF":10.8,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609695","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Central SciencePub Date : 2024-10-29DOI: 10.1021/acs.est.4c0003910.1021/acs.est.4c00039
Colleen E. Yancey, Lauren Hart, Apurva Chandrakant Lad, Johnna A. Birbeck, Siliang Song, Osama G. Mohamed, Andrew M. Fribley, Steven T. Haller, Ashootosh Tripathi, David J. Kennedy, Judy A. Westrick, David H. Sherman and Gregory J. Dick*,
{"title":"Synthesis of a Truncated Microcystin Tetrapeptide Molecule from a Partial Mcy Gene Cluster in Microcystis Cultures and Blooms","authors":"Colleen E. Yancey, Lauren Hart, Apurva Chandrakant Lad, Johnna A. Birbeck, Siliang Song, Osama G. Mohamed, Andrew M. Fribley, Steven T. Haller, Ashootosh Tripathi, David J. Kennedy, Judy A. Westrick, David H. Sherman and Gregory J. Dick*, ","doi":"10.1021/acs.est.4c0003910.1021/acs.est.4c00039","DOIUrl":"https://doi.org/10.1021/acs.est.4c00039https://doi.org/10.1021/acs.est.4c00039","url":null,"abstract":"<p ><i>Microcystis</i> spp. threaten freshwater ecosystems through the proliferation of cyanobacterial harmful algal blooms (cyanoHABs) and production of the hepatotoxin, microcystin. While microcystin and its biosynthesis pathway, encoded by the <i>mcy</i> genes, have been well studied for over 50 years, a recent study found that <i>Microcystis</i> populations in western Lake Erie contain a transcriptionally active partial <i>mcy</i> operon, in which the A2 domain of <i>mcyA</i> and <i>mcyB-C</i> are present but the <i>mcyD-J</i> genes are absent. Here, we investigate the potential biosynthetic products and the evolutionary history of this partial operon. Our results reveal two candidate tetrapeptide constructs, with an X variable position, to be produced by strains with the partial operon. The partial operon appears necessary and sufficient for tetrapeptide biosynthesis and likely evolved from a single ancestor hundreds to tens of thousands of years ago. Bioactivity screens using Hep3B cells indicate a mild elevation of some markers of hepatotoxicity and inflammation, suggesting the need to further assess the effects of these novel secondary metabolites on freshwater ecosystems and public health. The need to assess these effects is even more pressing given the detection of tetrapeptides in both culture and western Lake Erie, which is a vital source of fresh water. Results from this study emphasize previous findings in which novel bacterial secondary metabolites may be derived from the molecular evolution of existing biosynthetic machinery under different environmental forcings.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 45","pages":"19936–19947 19936–19947"},"PeriodicalIF":10.8,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608959","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Central SciencePub Date : 2024-10-29DOI: 10.1021/acs.est.4c0609310.1021/acs.est.4c06093
Ying Yu*, Xijing Li, Angel Hsu and Noah Kittner*,
{"title":"Mapping Spatiotemporal Disparities in Residential Electricity Inequality Using Machine Learning","authors":"Ying Yu*, Xijing Li, Angel Hsu and Noah Kittner*, ","doi":"10.1021/acs.est.4c0609310.1021/acs.est.4c06093","DOIUrl":"https://doi.org/10.1021/acs.est.4c06093https://doi.org/10.1021/acs.est.4c06093","url":null,"abstract":"<p >The move toward electrification is critical for decarbonizing the energy sector but may exacerbate energy unaffordability without proper safeguards. Addressing this challenge requires capturing neighborhood-scale dynamics to uncover the blind spots in residential electricity inequality. Based on publicly available, multisourced remote sensing and census data, we develop a high-resolution, spatiotemporally explicit machine learning (ML) framework to predict tract-level monthly electricity consumption across the conterminous U.S. from 2013–2020. We then construct the electricity affordability gap (EAG) metric, defined as the gap between electricity bills and 3% of household income, to better identify energy-vulnerable communities over space and time. The results show that our framework largely improves the resolution of electricity consumption data while achieving an <i>R</i><sup>2</sup> of 0.82 compared to the Low-Income Energy Affordability Data (LEAD). We estimate an annual $16.18 billion economic burden on the ability to afford electricity bills, exceeding current federal appropriations in alleviating energy difficulties. We also observe pronounced seasonal and urban-rural disparities, with monthly EAG in summer and winter being 2–3 times greater than other seasons and rural residents facing burdens up to 1.7 times higher than their urban counterparts. These insights inform equitable electrification by addressing spatiotemporal mismatches and multiple jurisdictional challenges in energy justice efforts.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 45","pages":"19999–20008 19999–20008"},"PeriodicalIF":10.8,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609693","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Central SciencePub Date : 2024-10-29DOI: 10.1021/acs.est.4c0650310.1021/acs.est.4c06503
Ziyan Wu, Sarah E. Janssen, Michael T. Tate, Haoran Wei* and Mohan Qin*,
{"title":"Adaptable Plasmonic Membrane Sensors for Fast and Reliable Detection of Trace Low-Micrometer Microplastics in Lake Water","authors":"Ziyan Wu, Sarah E. Janssen, Michael T. Tate, Haoran Wei* and Mohan Qin*, ","doi":"10.1021/acs.est.4c0650310.1021/acs.est.4c06503","DOIUrl":"https://doi.org/10.1021/acs.est.4c06503https://doi.org/10.1021/acs.est.4c06503","url":null,"abstract":"<p >In freshwater environments, low-micrometer microplastics (LMMPs) have captured significant attention due to their prevalence and toxicity. Yet, rapid detection of LMMPs (1–10 μm) at the single-particle level within complex freshwater matrices remains a hurdle. We developed an adaptable plasmonic membrane sensor for fast detection of individual LMMPs in eutrophic lake waters. The plasmonic membrane sensor functions both as a membrane filter and as a sensor for LMMP collection and analysis. Among the four types of membrane sensors, polycarbonate track-etch (PCTE) membrane sensors exhibit superior imaging quality for LMMPs due to their flat and homogeneous surfaces. Besides the significantly improved imaging contrast and reduced background interferences, the Raman intensity of LMMPs is enhanced by 48% ± 25% on PCTE membrane sensors compared to unmodified membranes. The increased Raman intensities of a chemical probe with an increasing gold layer thickness and a decreasing membrane pore size suggest a surface-enhanced Raman scattering effect from the membrane sensors. The membrane sensors achieve a detection limit of 1 μg/L and an ultrafast scanning time of 0.01 s for individual LMMPs across natural eutrophic lake water. The developed membrane sensors offer an adaptable tool for the swift and reliable detection of individual LMMPs in complex environmental matrices.</p><p >This study developed a dual-function plasmonic membrane sensor for rapid detection of low-micrometer microplastics in a lake water matrix at the single-particle level.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 45","pages":"20172–20180 20172–20180"},"PeriodicalIF":10.8,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.est.4c06503","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608796","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Central SciencePub Date : 2024-10-28DOI: 10.1021/acs.est.4c0550410.1021/acs.est.4c05504
Liuwei Wang, Jing Gao, Wei-Min Wu, Jian Luo, Michael S. Bank, Albert A. Koelmans, John J. Boland and Deyi Hou*,
{"title":"Rapid Generation of Microplastics and Plastic-Derived Dissolved Organic Matter from Food Packaging Films under Simulated Aging Conditions","authors":"Liuwei Wang, Jing Gao, Wei-Min Wu, Jian Luo, Michael S. Bank, Albert A. Koelmans, John J. Boland and Deyi Hou*, ","doi":"10.1021/acs.est.4c0550410.1021/acs.est.4c05504","DOIUrl":"https://doi.org/10.1021/acs.est.4c05504https://doi.org/10.1021/acs.est.4c05504","url":null,"abstract":"<p >In this study, we show that low-density polyethylene films, a prevalent choice for food packaging in everyday life, generated high numbers of microplastics (MPs) and hundreds to thousands of plastic-derived dissolved organic matter (DOM) substances under simulated food preparation and storage conditions. Specifically, the plastic film generated 66–2034 MPs/cm<sup>2</sup> (size range 10–5000 μm) under simulated aging conditions involving microwave irradiation, heating, steaming, UV irradiation, refrigeration, freezing, and freeze–thaw cycling alongside contact with water, which were 15–453 times that of the control (plastic film immersed in water without aging). We also noticed a substantial release of plastic-derived DOM. Using ultrahigh-resolution mass spectrometry, we identified 321–1414 analytes with molecular weights ranging from 200 to 800 Da, representing plastic-derived DOM containing C, H, and O. The DOM substances included both degradation products of polyethylene (including oxidized forms of oligomers) and toxic plastic additives. Interestingly, although no apparent oxidation was observed for the plastic film under aging conditions, plastic-derived DOM was more oxidized (average O/C increased by 27–46%) following aging with a higher state of carbon saturation and higher polarity. These findings highlight the future need to assess risks associated with MP and DOM release from plastic wraps.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 45","pages":"20147–20159 20147–20159"},"PeriodicalIF":10.8,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609028","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}