环境科学与技术最新文献

Dimethyl selenide (DMSe) is the simplest volatile organoselenium compound that can undergo atmospheric oxidation to form secondary aerosols. While the oxidative potential of DMSe-derived aerosols has been shown to be greater compared to that of ambient aerosols from various sources, the role of selenium (Se) in processes governing reactive oxygen species (ROS) production remains unclear. Utilizing dimethyl sulfide (DMS) as a chemical analogue and mechanistic control of DMSe, we detected, quantified, and contrasted ROS produced by DMSe- and DMS-derived aerosols in aqueous solutions and confirmed the changes in Se oxidation state after dissolution. DMSe- and DMS-derived aerosols produced 9.0 ± 2.1 nmol ·OH/μg-aerosol and 0.29 nmol ± 0.11 ·OH/μg-aerosol, respectively. The average 33-fold difference in ·OH produced in these systems implies different dominating mechanisms of formation. DMS-derived aerosols can generate ·OH through organic hydroperoxide decomposition, whereas DMSe-derived aerosols are additionally capable of producing ·OH through Fenton-like reactions by cycling among Se(0), Se(IV), and Se(VI). Selenate (SeO₄^2-), selenite (SeO₃^2-), selenium dioxide (SeO₂), and methane seleninic acid (CH₄O₂Se) were redox-active compounds confirmed within DMSe-derived aerosols. This study highlights the redox cycling of particulate Se and the production of aqueous ·OH, which have important implications for atmospheric aqueous chemistry and Se biogeochemical cycles.

Decarbonizing the iron and steel industry (ISI) reduces air pollutant emissions, yielding substantial public health cobenefits. Existing assessments fail to account for plant-level heterogeneity in production routes and geographic settings─critical determinants of health impacts─hindering the formulation of targeted decarbonization strategies that maximize health gains. Here, by integrating a facility-level emission inventory with inverse atmospheric modeling, we estimate that the Chinese ISI emits 1.56 Pg of CO₂ and 0.85 Tg of PM_2.5 annually, with 147,000 (IQR: 121,000-184,000) annual PM_2.5-attributable premature deaths linked to ISI emissions, and the health burdens varying by 77,500-fold across individual plants. Blast furnace-basic oxygen furnace (BF-BOF) processes impose 3.8 times higher mortality intensity than electric arc furnaces (EAFs) (172 vs 45 deaths per 1000 Gg steel produced), with 80% of mortality concentrated in 21% of plants─predominantly large BF-BOF complexes in densely populated eastern China. Strategically relocating 30 Tg eastern BF-BOF capacity (3.6% of the national total) to scrap-based EAFs in low-carbon southwestern power grids could prevent 12,300 (IQR: 9500-16,100) annual deaths (8.4% reduction), generating USD 24.5 (IQR: 20.0-30.4) billion in combined climate-health benefits. Natural gas-based direct reduced iron-electric arc furnace (DRI-EAF) integration offers a scrap-independent alternative, achieving ∼50% lower mortality than BF-BOF. These findings advance targeted strategies to optimize health outcomes during ISI decarbonization in China.

Synchronous sulfidogenesis and acidogenesis (SSA) are critical for pollutant removal and resource recovery. However, inefficient electron transfer and metabolic imbalance between acidogenic bacteria and sulfidogens limit SSA performance, especially from mariculture solid wastes (MSW) containing high-strength sulfate. This work unveiled the neglected role and mechanism of rhamnolipid (RL) in modulating microbial interspecies electron transfer for SSA during MSW anaerobic fermentation. RL, at environmentally relevant levels of 20-200 mg/g suspended solids, simultaneously improved sulfide (40.1-87.9%) and short-chain fatty acids (8.0-19.3-fold) yield. Extracellular polymeric substances (EPSs) exhibited higher capacitance and electroactivity to store or transfer electrons in the presence of RL. Proper RL facilitated pili-like filament formation and redox mediator secretion. The flavins and cytochrome c combination was promoted by RL to mediate one-electron transfer with a higher transfer rate via the flavin semiquinone intermediate. RL increased the dipole moment of the α-helix peptide and spontaneously interacted with the C═O of amide groups, enabling efficient electron hopping in EPSs. RL also activated key components in the intracellular electron transfer system, delivering more electron flow to sulfate reductase. Metagenomic and metatranscriptomic analyses verified the differential enrichment of microorganisms and key gene upregulation related to SSA, EPS secretion, quorum sensing, ATP, type IV pili, and electron shuttle synthesis. These findings provide new insight into the roles and interactive mechanisms of biosurfactants in modulating microbial electron transfer.

The rapid iteration of electronics and semiconductor technologies has brought convenience to daily life. However, the resulting large-scale production may pose health risks due to per- and polyfluoroalkyl substances (PFAS) emissions. Here, we present the first trade-off analysis between PFAS wastewater treatment burdens and associated health benefits in electronics and semiconductor manufacturing and benchmark the costs against market values. Specifically, by 2035, the rapid expansion of these sectors is projected to discharge 4.4-10.9 kilotons of PFAS annually into wastewater, resulting in an estimated upper-bound range of 25-103 million comparative toxic units for human toxicity (CTUh) in the absence of treatment. Achieving the toxicity reduction via granular activated carbon (GAC), ion-exchange resin (IER), or reverse osmosis (RO) membranes will require annual investments of $16.5-50.0 billion across regions in 2035, equivalent to ∼0.5% of the respective electronics market value via IER. Moreover, we find that variations in breakthrough performance substantially alter both economic and environmental burdens, particularly in electronics wastewater, which is dominated by short-chain PFAS, whose limited removal efficiency amplifies these effects. By quantifying the cost-health nexus, our findings provide actionable insights for PFAS governance and reinforce the urgency of globally coordinated efforts to align industrial growth with environmental and public health protection.

Whether used as an alternative fuel or a clean feedstock, renewable hydrogen (H₂) could facilitate the deep decarbonization of hard-to-abate sectors, which is essential to meet China's carbon neutrality target. Nevertheless, the nationwide H₂ backbone networks required have not yet been fully investigated. Employing a techno-economic analysis of solar photovoltaic and wind power on a scale of 1 km combined with source-sink matching among potential multisectoral H₂ hubs, this study develops a decision support system (dubbed China Shared Hydrogen Infrastructure Network Enabler (SHINE)) to explore renewable H₂ layouts commensurate with China's climate ambition, accounting for varying degrees of H₂ demand and reuse of oil and gas pipeline corridors. Given total H₂ demand scenarios of 54, 77, and 100 Mt/yr in 2060, the total length of the proposed trunkline networks will reach roughly 11,700, 18,300, and 29,900 km, with a levelized cost of production and transport of 1.55, 1.62, and 1.72 USD/kg, respectively. Additionally, by incorporating the spatial heterogeneities and sectoral disparities of H₂ deployment expansion into the model, distinct policy instruments can be crafted for the shared nationwide H₂ network.

Coastal salt marshes (CSMs) are vital blue carbon (BC) reservoirs, yet accurately quantifying their gross primary productivity (GPP) remains challenging due to limitations in terrestrial biosphere models (TBMs), which often overlook coastal-specific processes. Here, we present SAL-GPP, a process-based model that incorporates coastal-specific modules to capture the effects of salinity and temperature stress on photosynthesis, as well as light-use efficiency across salinity gradients in diverse CSM plant species. Model validation showed strong agreement with observations, with R² of 0.82 and model efficiencies of 0.82 and 0.74 for daily and seasonal GPP, respectively. Driven with global inputs, SAL-GPP produced high-resolution global simulations, yielding a mean annual GPP of 66.89 ± 11.68 TgC yr^-1 (2011-2020), with 64% concentrated in key hotspots across the southeastern United States, western Europe, southeastern China, and Australia. From 2011 to 2016, global CSM GPP increased by 1.56 TgC yr^-1, then declined, rebounded after 2018, and peaked at 71.45 ± 12.02 TgC yr^-1 in 2020. Model evaluation showed that SAL-GPP outperformed existing remote sensing-based GPP products and TBMs at both site and grid levels. By explicitly incorporating coastal ecosystem dynamics, SAL-GPP supports global BC accounting and climate mitigation strategies aligned with nature-based solutions for carbon neutrality.

Non-targeted liquid chromatography tandem high-resolution mass spectrometry (LC-MS/MS) is increasingly applied for the structure-resolved chemical analysis of dissolved organic matter (DOM). With new developments in MS instrumentation and analysis software, the approach has gained substantial momentum over the past decade. However, achieving high-quality analytical data that is reproducible and comparable across laboratories can be a bottleneck in non-targeted metabolomics and organic matter chemical analysis, especially for data reuse in repository-scale analyses. Understanding the capabilities as well as challenges of comparing LC-MS/MS data from different laboratories is necessary for inferring global trends from public data sets. To illuminate instrumentation factors that drive differences and variability, we used a standardized data analysis pipeline, including classical (CMN) and feature-based molecular networking (FBMN), to analyze data from a ring trial by 24 laboratories on identical sample sets of algal and DOM extracts that were mixed in predefined concentrations and spiked with standards. Our results showed that data sets from similar mass spectrometer types with unified instrument parameters were qualitatively comparable, resolving the same general trends and shared mass spectral features. Interlaboratory comparability was best for high-intensity features, while low-intensity features showed greater detection variability. Our analysis also highlights challenges when comparing data from instruments with different acquisition rates or operating with less standardized methods. Lastly, we provide recommendations for data integration, public data sharing, standardization, and best practices for standardized LC-MS/MS data acquisition, which will be critical for long-term time series and intercomparability of DOM chemical analyses.

The obesity epidemic is increasingly linked to environmental factors like endocrine disrupting chemicals (EDCs). Bisphenol A (BPA), a known EDC, has been suspected to be linked to adiposity through activation of peroxisome proliferator activated receptor gamma (PPARγ), a key regulator of adipogenesis. Though many BPA alternatives have been introduced as substitutes, their effects on metabolic health remain unclear. This study aimed to investigate the mechanistic interactions of 11 BPA alternatives with PPARγ and their adipogenic potential. Using a PPARγ reporter assay, we assessed the binding affinity and activation potential of BPA alternatives, followed by X-ray crystallography of two potent activators, 4-benzyloxyphenyl 4-hydroxyphenyl sulfone (BPS4BE) and bisphenol PH (BPPH). Additionally, adipogenesis was assessed via a human mesenchymal stem cells (hMSCs) differentiation assay. Results revealed that the alternatives BPPH and BPS4BE potently activated PPARγ (BMD20 (μM): 0.23 and 0.34 respectively). Both significantly induced adipogenesis and a positive correlation was found between PPARγ activation and adipogenic differentiation. Crystallography revealed distinct binding modes for BPPH and BPS4BE compared to rosiglitazone, indicating partial agonism. These findings raise significant concerns about the safety of BPA alternatives and underscore the need for structure-based risk assessment to ensure safer substitutes.

Plastic particles present in soil are exposed to soil solutions containing a mixture of microbial metabolites, dissolved organic matter, mineral and organic colloids, as well as inorganic ions. These components can interact with plastic particles in different ways that may alter their surface properties and environmental behavior. In this study, we examined how soil solution affects the aggregation kinetics and colloidal stability of nanoplastics made from a soil-biodegradable plastic (poly(butylene adipate-co-terephthalate), PBAT) and a conventional plastic (polyethylene). Without the soil solution, both PBAT and polyethylene nanoplastics aggregated more readily in CaCl₂ than in NaCl, with critical coagulation concentrations of 344 and 284 mM in NaCl and 31 and 36 mM in CaCl₂, respectively. The addition of the soil solution promoted the aggregation of both nanoplastics, as evidenced by the larger aggregate sizes, despite that the critical coagulation concentrations did not decrease correspondingly. Such an increase in aggregate sizes was induced not only by the formation of an eco-corona on nanoplastics, which enhanced aggregation through polymer bridging and attractive patch-charge interactions, but also by the heteroaggregation between nanoplastics and colloids present in the soil solution. These results suggest that interaction with soil solution can promote the aggregation of nanoplastics through eco-corona formation and heteroaggregation, underlining the role of the complex interactions between nanoplastics and their surrounding matrices on the environmental behavior of nanoplastics.