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1.
Nature ; 627(8005): 797-804, 2024 Mar.
Article in English | MEDLINE | ID: mdl-38480894

ABSTRACT

Evidence shows a continuing increase in the frequency and severity of global heatwaves1,2, raising concerns about the future impacts of climate change and the associated socioeconomic costs3,4. Here we develop a disaster footprint analytical framework by integrating climate, epidemiological and hybrid input-output and computable general equilibrium global trade models to estimate the midcentury socioeconomic impacts of heat stress. We consider health costs related to heat exposure, the value of heat-induced labour productivity loss and indirect losses due to economic disruptions cascading through supply chains. Here we show that the global annual incremental gross domestic product loss increases exponentially from 0.03 ± 0.01 (SSP 245)-0.05 ± 0.03 (SSP 585) percentage points during 2030-2040 to 0.05 ± 0.01-0.15 ± 0.04 percentage points during 2050-2060. By 2060, the expected global economic losses reach a total of 0.6-4.6% with losses attributed to health loss (37-45%), labour productivity loss (18-37%) and indirect loss (12-43%) under different shared socioeconomic pathways. Small- and medium-sized developing countries suffer disproportionately from higher health loss in South-Central Africa (2.1 to 4.0 times above global average) and labour productivity loss in West Africa and Southeast Asia (2.0-3.3 times above global average). The supply-chain disruption effects are much more widespread with strong hit to those manufacturing-heavy countries such as China and the USA, leading to soaring economic losses of 2.7 ± 0.7% and 1.8 ± 0.5%, respectively.

2.
Nature ; 626(8000): 792-798, 2024 Feb.
Article in English | MEDLINE | ID: mdl-38297125

ABSTRACT

Crop production is a large source of atmospheric ammonia (NH3), which poses risks to air quality, human health and ecosystems1-5. However, estimating global NH3 emissions from croplands is subject to uncertainties because of data limitations, thereby limiting the accurate identification of mitigation options and efficacy4,5. Here we develop a machine learning model for generating crop-specific and spatially explicit NH3 emission factors globally (5-arcmin resolution) based on a compiled dataset of field observations. We show that global NH3 emissions from rice, wheat and maize fields in 2018 were 4.3 ± 1.0 Tg N yr-1, lower than previous estimates that did not fully consider fertilizer management practices6-9. Furthermore, spatially optimizing fertilizer management, as guided by the machine learning model, has the potential to reduce the NH3 emissions by about 38% (1.6 ± 0.4 Tg N yr-1) without altering total fertilizer nitrogen inputs. Specifically, we estimate potential NH3 emissions reductions of 47% (44-56%) for rice, 27% (24-28%) for maize and 26% (20-28%) for wheat cultivation, respectively. Under future climate change scenarios, we estimate that NH3 emissions could increase by 4.0 ± 2.7% under SSP1-2.6 and 5.5 ± 5.7% under SSP5-8.5 by 2030-2060. However, targeted fertilizer management has the potential to mitigate these increases.


Subject(s)
Ammonia , Crop Production , Fertilizers , Ammonia/analysis , Ammonia/metabolism , Crop Production/methods , Crop Production/statistics & numerical data , Crop Production/trends , Datasets as Topic , Ecosystem , Fertilizers/adverse effects , Fertilizers/analysis , Fertilizers/statistics & numerical data , Machine Learning , Nitrogen/analysis , Nitrogen/metabolism , Oryza/metabolism , Soil/chemistry , Triticum/metabolism , Zea mays/metabolism , Climate Change/statistics & numerical data
3.
Nature ; 622(7983): 514-520, 2023 Oct.
Article in English | MEDLINE | ID: mdl-37731002

ABSTRACT

The highly energy-intensive iron and steel industry contributed about 25% (ref. 1) of global industrial CO2 emissions in 2019 and is therefore critical for climate-change mitigation. Despite discussions of decarbonization potentials at national and global levels2-6, plant-specific mitigation potentials and technologically driven pathways remain unclear, which cumulatively determines the progress of net-zero transition of the global iron and steel sector. Here we develop a CO2 emissions inventory of 4,883 individual iron and steel plants along with their technical characteristics, including processing routes and operating details (status, age, operation-years etc.). We identify and match appropriate emission-removal or zero-emission technologies to specific possessing routes, or what we define thereafter as a techno-specific decarbonization road map for every plant. We find that 57% of global plants have 8-24 operational years, which is the retrofitting window for low-carbon technologies. Low-carbon retrofitting following the operational characteristics of plants is key for limiting warming to 2 °C, whereas advanced retrofitting may help limit warming to 1.5 °C. If each plant were retrofitted 5 years earlier than the planned retrofitting schedule, this could lead to cumulative global emissions reductions of 69.6 (±52%) gigatonnes (Gt) CO2 from 2020 to 2050, almost double that of global CO2 emissions in 2021. Our results provide a detailed picture of CO2 emission patterns associated with production processing of iron and steel plants, illustrating the decarbonization pathway to the net-zero-emissions target with the efforts from each plant.

4.
Nature ; 567(7748): 414-419, 2019 03.
Article in English | MEDLINE | ID: mdl-30867593

ABSTRACT

DNA and histone modifications have notable effects on gene expression1. Being the most prevalent internal modification in mRNA, the N6-methyladenosine (m6A) mRNA modification is as an important post-transcriptional mechanism of gene regulation2-4 and has crucial roles in various normal and pathological processes5-12. However, it is unclear how m6A is specifically and dynamically deposited in the transcriptome. Here we report that histone H3 trimethylation at Lys36 (H3K36me3), a marker for transcription elongation, guides m6A deposition globally. We show that m6A modifications are enriched in the vicinity of H3K36me3 peaks, and are reduced globally when cellular H3K36me3 is depleted. Mechanistically, H3K36me3 is recognized and bound directly by METTL14, a crucial component of the m6A methyltransferase complex (MTC), which in turn facilitates the binding of the m6A MTC to adjacent RNA polymerase II, thereby delivering the m6A MTC to actively transcribed nascent RNAs to deposit m6A co-transcriptionally. In mouse embryonic stem cells, phenocopying METTL14 knockdown, H3K36me3 depletion also markedly reduces m6A abundance transcriptome-wide and in pluripotency transcripts, resulting in increased cell stemness. Collectively, our studies reveal the important roles of H3K36me3 and METTL14 in determining specific and dynamic deposition of m6A in mRNA, and uncover another layer of gene expression regulation that involves crosstalk between histone modification and RNA methylation.


Subject(s)
Adenosine/analogs & derivatives , Histones/chemistry , Histones/metabolism , Lysine/metabolism , RNA, Messenger/chemistry , RNA, Messenger/metabolism , Transcription, Genetic , Adenosine/metabolism , Animals , Cell Differentiation , Cell Line , Embryonic Stem Cells/metabolism , Humans , Lysine/chemistry , Methylation , Methyltransferases/deficiency , Methyltransferases/genetics , Methyltransferases/metabolism , Mice , RNA Polymerase II/metabolism , Transcription Elongation, Genetic , Transcriptome/genetics
5.
Environ Sci Technol ; 58(19): 8326-8335, 2024 May 14.
Article in English | MEDLINE | ID: mdl-38696616

ABSTRACT

China, especially the densely populated North China region, experienced severe haze events in the past decade that concerned the public. Although the most extreme cases have been largely eliminated through recent mitigation measures, severe outdoor air pollution persists and its environmental impact needs to be understood. Severe indoor pollution draws less public attention due to the short visible distance indoors, but its public health impacts cannot be ignored. Herein, we assess the trends and impacts of severe outdoor and indoor air pollution in North China from 2014 to 2021. Our results demonstrate the uneven contribution of severe hazy days to ambient and exposure concentrations of particulate matter with an aerodynamic diameter <2.5 (PM2.5). Although severe indoor pollution contributes to indoor PM2.5 concentrations (23%) to a similar extent as severe haze contributes to ambient PM2.5 concentrations (21%), the former's contribution to premature deaths was significantly higher. Furthermore, residential emissions contributed more in the higher PM2.5 concentration range both indoors and outdoors. Notably, severe haze had greater health impacts on urban residents, while severe indoor pollution was more impactful in rural areas. Our findings suggest that, besides reducing severe haze, mitigating severe indoor pollution is an important aspect of combating air pollution, especially toward improving public health.


Subject(s)
Air Pollutants , Air Pollution, Indoor , Environmental Monitoring , Particulate Matter , China , Particulate Matter/analysis , Air Pollutants/analysis , Air Pollution , Humans
6.
Environ Sci Technol ; 58(31): 13950-13960, 2024 Aug 06.
Article in English | MEDLINE | ID: mdl-39051425

ABSTRACT

Phototransformation is a key process affecting the fate of many antibiotics in the environment, but little is known about whether their photoproducts exert selective pressure on bacteria by inducing antibiotic resistance genes (ARGs). Here, we examined the expression of tetracycline resistance gene tet(M) of a fluorescent Escherichia coli whole-cell bioreporter influenced by the phototransformation of tetracycline. The presence of suspended smectite clay (montmorillonite or hectorite, 1.75 g/L) or dissolved humic substance (Pahokee Peat humic acid or Pahokee peat fulvic acid, 10 mg C/L) in aqueous solutions markedly facilitated the transformation of tetracycline (initially at 400 µg/L) with half-life shortened by 1.4-2.6 times. Despite the similar phototransformation ratios (80-90%) of the total loaded tetracycline after 60 min irradiation, the decreased ratios of cell fluorescence intensity (which was proportional to the expression amount of ARG tet(M)) were much higher with the two clays (94 and 93%) than with the two humic substances (44 and 69%) when compared to the respective dark controls. As illustrated by mass spectroscopic and chemical analyses, tetracycline was proposed to be mainly transformed to amide (ineffective in inducing ARGs) with the presence of clays by reaction with self-photosensitized singlet oxygen (1O2), while the humic substances might catalyze the production of another two demethylated and/or deaminated compounds (still effective in inducing ARGs) in addition to the amide compound via reaction with triplet excited state dissolved organic matter (3DOM*). As clay minerals and humic substances are important soil constituents and ubiquitously present in surface environments, the observed clay and humic-dependent photooxidation pathways of tetracycline and the differing selective pressures of the associated products highlight the need for monitoring the transformation compounds of antibiotics and provide critical insight into the development of antibiotic treatment protocols.


Subject(s)
Clay , Escherichia coli , Humic Substances , Photolysis , Tetracycline , Tetracycline/chemistry , Clay/chemistry , Aluminum Silicates/chemistry , Anti-Bacterial Agents/chemistry , Anti-Bacterial Agents/pharmacology , Tetracycline Resistance
7.
Environ Sci Technol ; 58(27): 11998-12007, 2024 Jul 09.
Article in English | MEDLINE | ID: mdl-38935345

ABSTRACT

Landscape wildfires generate a substantial amount of dissolved black carbon (DBC) annually, yet the molecular nitrogen (N) structures in DBC are poorly understood. Here, we systematically compared the chemodiversity of N-containing molecules among three different DBC samples from rice straw biochar pyrolyzed at 300, 400, and 500 °C, one leached dissolved organic carbon (LDOC) sample from composted rice straw, and one fire-affected soil dissolved organic matter (SDOMFire) sample using Fourier-transform ion cyclotron resonance mass spectrometry (FT-ICR MS). N-Containing molecules contributed 20.0%, 36.1%, and 43.7% of total compounds in Combined DBC (pooling together the three DBC), LDOC, and SDOMFire, respectively, and molecules with fewer N atoms had higher proportions (i.e., N1 > N2 > N3). The N-containing molecules in Combined DBC were dominated by polycyclic aromatic (62.2%) and aromatic (14.4%) components, while those in LDOC were dominated by lignin-like (50.4%) and aromatic (30.1%) components. The composition and structures of N-containing molecules in SDOMFire were more similar to those in DBC than in LDOC. As the temperature rose, the proportion of the nitrogenous polycyclic aromatic component in DBC significantly increased with concurrent enhanced oxidation and unsaturation of N. As indicated by density functional theory (DFT)-based thermodynamic calculations, the proportion of aliphatic amide N decreased from 23.2% to 7.9%, whereas that of nitroaromatic N increased from 10.0% to 39.5% as the temperature increased from 300 to 500 °C; alternatively, the proportion of aromatic N in the 5/6 membered ring remained relatively stable (∼31%) and that of aromatic amide N peaked at 400 °C (32.7%). Our work first provides a comprehensive and thorough description of molecular N structures of DBC, which helps to better understand and predict their fate and biogeochemical behavior.


Subject(s)
Mass Spectrometry , Nitrogen , Thermodynamics , Nitrogen/chemistry , Molecular Structure , Carbon/chemistry , Soil/chemistry
8.
Environ Sci Technol ; 58(2): 1142-1151, 2024 Jan 16.
Article in English | MEDLINE | ID: mdl-38159290

ABSTRACT

Landscape fires annually generate large quantities of black carbon. The water-soluble fraction of black carbon (i.e., dissolved black carbon/DBC) is an important constituent of the dissolved organic carbon (DOC) pool, playing a crucial role in the global budget of refractory carbon and climate change. A key challenge in constraining the flux and fate of riverine DBC is to develop targeted and accurate quantification methods. Herein, we report that benzenepentacarboxylic acid (B5CA) intrinsically present in DBC can be used as an exclusive and holistic marker (representing both condensed aromatics and less-/nonaromatic fractions) for DBC quantification. B5CA was universally detected in water extractions of biochar and fire-affected soils with relatively large abundance but not produced by nonthermogenic processes. It has good mobility in the environment as it is not readily precipitated by cations or adsorbed by common geosorbents. B5CA also represents the recalcitrant components of DBC with excellent stability against photodegradation and biodegradation. Applying B5CA as the DBC marker in surface waters of the Changjiang River (i.e., the third largest river in the world), we calculate the DBC concentration in the downstream Changjiang River to be 4.8 ± 5.5% of the DOC flux. Our work provides a simple and reliable approach for the accurate quantification and source tracking of DBC in the soil and aquatic carbon pools.


Subject(s)
Carbon , Carboxylic Acids , Soil , Rivers , Soot , Water
9.
Environ Sci Technol ; 2024 Aug 14.
Article in English | MEDLINE | ID: mdl-39140482

ABSTRACT

Mercury, a neurotoxic substance, circulates globally, significantly stored in soils through atmospheric deposition and plant decay. Despite being deposited, mercury can be remobilized and released into the atmosphere and water, enhancing its global cycle. Recent research suggests that climate warming may amplify the remobilization of soil mercury, facilitating its incorporation into food webs that humans exploit. However, the potential geospatial feedback of soil mercury levels in response to warming remains unclear. By leveraging up-to-date soil measurements and observation-driven models, we determined the amount of mercury stored in global 0-100 cm soils to be 4.3 Tg (interquartile range: 2.5-6.3 Tg). Furthermore, our analysis indicates that warming likely aggravates global soil mercury levels, particularly in many temperate areas in East Asia, North Europe, and North America (>20 ng g-1 increase by 2100) due to warming-induced vegetation greening. Critically, observation-driven models raise the possibility that implementing ambitious mercury-emission-control schemes alone may be insufficient to counterbalance the positive feedback of soil mercury concentration, while process-based biogeochemical modeling demonstrates consistent patterns that reinforce this concern. These findings hold broad implications; for example, such feedback may catalyze mercury remobilization in land-ocean continuums and exacerbate human risks, stressing the necessity for continued reductions in greenhouse gas and mercury emissions.

10.
Environ Sci Technol ; 2024 Aug 05.
Article in English | MEDLINE | ID: mdl-39102498

ABSTRACT

Residential solid fuel combustion significantly impacts air quality and human health. Pelletized biomass fuels are promoted as a cleaner alternative, particularly for those who cannot afford the high costs of gas/electricity, but their emission characteristics and potential effects remain poorly understood. The present laboratory-based study evaluated pollution emissions from pelletized biomass burning, including CH4 (methane), NMHC (nonmethane hydrocarbon compounds), CO, SO2, NOx, PM2.5 (particulate matter with an aerodynamic diameter ≤2.5 µm), OC (organic carbon), EC (element carbon), PAHs (polycyclic aromatic hydrocarbons), EPFRs (environmentally persistent free radicals), and OP (oxidative potential) of PM2.5, and compared with those from raw biomass burning. For most targets, except for SO2 and NOx, the mass-based emission factors for pelletized biomass were 62-96% lower than those for raw biomass. SO2 and NOx levels were negatively correlated with other air pollutants (p < 0.05). Based on real-world daily consumption data, this study estimated that households using pelletized biomass could achieve significant reductions (51-95%) in emissions of CH4, NMHC, CO, PM2.5, OC, EC, PAHs, and EPFRs compared to those using raw biomass, while the differences in emissions of NOx and SO2 were statistically insignificant. The reduction rate of benzo(a)pyrene-equivalent emissions was only 16%, much lower than the reduction in the total PAH mass (78%). This is primarily attributed to the more PAHs with high toxic potentials, such as dibenz(a,h)anthracene, in the pelletized biomass emissions. Consequently, impacts on human health associated with PAHs might be overestimated if only the mass of total PAHs was counted. The OP of particles from the pellet burning was also significantly lower than that from raw biomass by 96%. The results suggested that pelletized biomass could be a transitional substitution option that can significantly improve air quality and mitigate human exposure.

11.
Environ Sci Technol ; 2024 Mar 15.
Article in English | MEDLINE | ID: mdl-38485962

ABSTRACT

Ozone pollution is profoundly modulated by meteorological features such as temperature, air pressure, wind, and humidity. While many studies have developed empirical models to elucidate the effects of meteorology on ozone variability, they predominantly focus on local weather conditions, overlooking the influences from high-altitude and broader regional meteorological patterns. Here, we employ convolutional neural networks (CNNs), a technique typically applied to image recognition, to investigate the influence of three-dimensional spatial variations in meteorological fields on the daily, seasonal, and interannual dynamics of ozone in Shenzhen, a major coastal urban center in China. Our optimized CNNs model, covering a 13° × 13° spatial domain, effectively explains over 70% of daily ozone variability, outperforming alternative empirical approaches by 7 to 62%. Model interpretations reveal the crucial roles of 2-m temperature and humidity as primary drivers, contributing 16% and 15% to daily ozone fluctuations, respectively. Regional wind fields account for up to 40% of ozone changes during the episodes. CNNs successfully replicate observed ozone temporal patterns, attributing -5-6 µg·m-3 of interannual ozone variability to weather anomalies. Our interpretable CNNs framework enables quantitative attribution of historical ozone fluctuations to nonlinear meteorological effects across spatiotemporal scales, offering vital process-based insights for managing megacity air quality amidst changing climate regimes.

12.
Proc Natl Acad Sci U S A ; 118(51)2021 12 21.
Article in English | MEDLINE | ID: mdl-34903647

ABSTRACT

Anthropogenic activities have led to widespread contamination with mercury (Hg), a potent neurotoxin that bioaccumulates through food webs. Recent models estimated that, presently, 200 to 600 t of Hg is sequestered annually in deep-sea sediments, approximately doubling since industrialization. However, most studies did not extend to the hadal zone (6,000- to 11,000-m depth), the deepest ocean realm. Here, we report on measurements of Hg and related parameters in sediment cores from four trench regions (1,560 to 10,840 m), showing that the world's deepest ocean realm is accumulating Hg at remarkably high rates (depth-integrated minimum-maximum: 24 to 220 µg ⋅ m-2 ⋅ y-1) greater than the global deep-sea average by a factor of up to 400, with most Hg in these trenches being derived from the surface ocean. Furthermore, vertical profiles of Hg concentrations in trench cores show notable increasing trends from pre-1900 [average 51 ± 14 (1σ) ng ⋅ g-1] to post-1950 (81 ± 32 ng ⋅ g-1). This increase cannot be explained by changes in the delivery rate of organic carbon alone but also need increasing Hg delivery from anthropogenic sources. This evidence, along with recent findings on the high abundance of methylmercury in hadal biota [R. Sun et al, Nat. Commun. 11, 3389 (2020); J. D. Blum et al, Proc. Natl. Acad. Sci. U. S. A. 117, 29292-29298 (2020)], leads us to propose that hadal trenches are a large marine sink for Hg and may play an important role in the regulation of the global biogeochemical cycle of Hg.


Subject(s)
Geologic Sediments/chemistry , Mercury , Ecosystem , Oceans and Seas
13.
Proc Natl Acad Sci U S A ; 118(15)2021 04 13.
Article in English | MEDLINE | ID: mdl-33876752

ABSTRACT

Knowing the historical relative contribution of greenhouse gases (GHGs) and short-lived climate forcers (SLCFs) to global radiative forcing (RF) at the regional level can help understand how future GHGs emission reductions and associated or independent reductions in SLCFs will affect the ultimate purpose of the Paris Agreement. In this study, we use a compact Earth system model to quantify the global RF and attribute global RF to individual countries and regions. As our evaluation, the United States, the first 15 European Union members, and China are the top three contributors, accounting for 21.9 ± 3.1%, 13.7 ± 1.6%, and 8.6 ± 7.0% of global RF in 2014, respectively. We also find a contrast between developed countries where GHGs dominate the RF and developing countries where SLCFs including aerosols and ozone are more dominant. In developing countries, negative RF caused by aerosols largely masks the positive RF from GHGs. As developing countries take measures to improve the air quality, their negative contributions from aerosols will likely be reduced in the future, which will in turn enhance global warming. This underlines the importance of reducing GHG emissions in parallel to avoid any detrimental consequences from air quality policies.

14.
J Environ Manage ; 350: 119695, 2024 Jan 15.
Article in English | MEDLINE | ID: mdl-38035506

ABSTRACT

Interactions between dissolved organic matter (DOM) and surrounding environments are highly complex. Understanding DOM at the molecular level can contribute to the management of soil pollution and safeguarding agricultural fields. Fourier transform ion cyclotron resonance mass spectrometry (FTICR-MS) has enabled a molecular-level understanding of DOM. Accordingly, in this study, we investigated soil samples from 27 different regions of mainland China with various soil types and climatic characteristics. Based on the geographical features of the four typical climatic zones in mainland China (temperate monsoon, temperate continental, subtropical monsoon, and Qinghai-Tibet Plateau climates), we employed high-resolution mass spectrometry to determine the molecular diversity of DOM under different climatic conditions. The results indicated that lignin and tannin-like substances were the most active categories of DOM in the soils. Collectively, the composition and unsaturation of DOM molecules are influenced by sunlight, precipitation, temperature, and human activity. All climatic regions contained a substantial number of characteristic molecules, with CHO and CHON constituting over 80%, and DOM containing nitrogen and sulfur was relatively more abundant in the monsoon regions. The complex composition of DOM incorporates various active functional groups, such as -NO2 and -ONO2. Furthermore, soil DOM in the monsoon regions showed higher unsaturation and facilitated various (bio) biochemical reactions in the soil.


Subject(s)
Dissolved Organic Matter , Soil , Farms , Organic Chemicals/analysis , Soil/chemistry , China
15.
Environ Geochem Health ; 46(4): 135, 2024 Mar 14.
Article in English | MEDLINE | ID: mdl-38483670

ABSTRACT

Some Polycyclic Aromatic Compounds (PACs) such as nitrated-PAHs (NPAHs), oxygenated-PAHs (OPAHs) and methyl-PAHs (MPAHs) have attracted significant concern due to derivatives have greater potential to be more toxic at low environmental concentrations compared to their PPAHs, particularly in petrochemical industrial region and its surrounding areas surface soils in China. Hence, this article provides an insight into the fate, sources, impacts, and relevance to the external environment of PAH-derivatives based on important emissions source. Moreover, prospective health risk due to their exposure has also been discussed. In this study, the concentration (10-3 ng/g) of Æ©18PPAHs, Æ©11MPAHs, Æ©12NPAHs, and Æ©4OPAHs in the park were 9.67 ± 1.40, 3.24 ± 0.54, 0.03 ± 0.02 and 0.19 ± 0.65, respectively, which were 4.47, 3.89, 2.04 and 1.17 times than of them surrounding the region. A decreasing trend of the low molecular weight (2-4Rings) contribution to the total amount of PAHs, while the fraction of high molecular weight (5-6Rings) species showed the opposite trend. According to the principal component analysis (PCA) and diagnostic ratios indicated PAHs in the soil samples have mixed sources from industrial activities, solid fuel combustion, and heavy traffic. Despite the high concentrations of MPAHs and OPAHs, the toxicity equivalency quotients (TEQs) of them were not calculated due to the lack of toxic equivalent factors (TEF), thus current studies on PAH and derivatives could have underestimated their exposure risks. The quality and sustainable management of soils are crucial for human health and sustainable development, while there is lack of public awareness of the severe issue of soil pollution. It is recommended to conduct more intensive monitoring and regional assessments in the future.


Subject(s)
Polycyclic Aromatic Hydrocarbons , Polycyclic Compounds , Soil Pollutants , Humans , Polycyclic Compounds/analysis , Environmental Monitoring , Soil , Polycyclic Aromatic Hydrocarbons/toxicity , Polycyclic Aromatic Hydrocarbons/analysis , China , Soil Pollutants/toxicity , Soil Pollutants/analysis , Risk Assessment
16.
Environ Sci Technol ; 57(40): 15223-15231, 2023 Oct 10.
Article in English | MEDLINE | ID: mdl-37771096

ABSTRACT

Although activated carbon (AC) is widely used as an adsorbent and barrier for contaminated sediment remediation, little attention has been paid to its mediation effects on reductive dechlorination of chlorinated solvents by commonly presenting sulfide. Here, we reported that highly porous, graphitized AC (250 mg L-1) suspended in deoxygenated aqueous solutions could increase the pseudo-first-order rate constant of sulfide-induced dechlorination of carbon tetrachloride (CCl4) by more than 1 order of magnitude. Carbon disulfide (CS2) was the only main product, with no production of chloroform or dichloromethane. The minimum promotion of CCl4 reduction observed with electro-conductive but nonporous graphite and a microporous but electro-insulative resin (XAD-4) indicates that graphitic carbons and micropores both play key roles in AC-mediated dechlorination of CCl4 by sulfide. The detection of dichlorocarbene (:CCl2) by free radical trapping experiments combined with the high suitability of the Langmuir-Hinshelwood model led us to propose a new mediation mechanism: CCl4 molecules adsorbed within the deep regions of AC micropores formed by graphitic carbons accept two electrons transferred from sulfide to form :CCl2, which is impeded from hydrolysis and hydrogenolysis by the hydrophobic micropore and further reacts with sulfide to generate CS2. Consistently, the production of :CCl2 was very low when AC was replaced with graphite or XAD-4. The proposed mechanism was further validated by the enhanced mediation effects of another two carbonaceous materials (template-synthesized mesoporous carbon and covalent triazine-based framework) that are electro-conductive and have well-developed micropore structures. These findings highlight the importance of pore properties of carbonaceous materials as mediators or catalysts for reductive dechlorination reactions and shed light on the development of coupled adsorption-reaction systems for remediation.

17.
Environ Sci Technol ; 57(6): 2506-2515, 2023 02 14.
Article in English | MEDLINE | ID: mdl-36734358

ABSTRACT

Fuel combustion provides basic energy for the society but also produces CO2 and incomplete combustion products that threaten human survival, climate change, and global sustainability. A variety of fuels burned in different facilities expectedly have distinct impacts on climate, which remains to be quantitatively assessed. This study uses updated emission inventories and an earth system model to evaluate absolute and relative contributions in combustion emission-associated climate forcing by fuels, sectors, and regions. We showed that, from 1970 to 2014, coal burned in the energy sector and oil used in the transportation sector contributed comparable energies consumed (24 and 20% of the total) but had distinct climate forcing (1 and 40%, respectively). Globally, coal burned for energy production had negative impacts on climate forcing but positive effects in the residential sector. In many developing countries, coal combustion in the energy sector had negative radiative forcing (RF) per unit energy consumed due to insufficient controls on sulfur and scattering aerosol levels, but oils in the transportation sector had high positive RF values. These results had important implications on the energy transition and emission reduction actions in response to climate change. Distinct climate efficiencies of energies and the spatial heterogeneity implied differentiated energy utilization strategies and pollution control policies by region and sector.


Subject(s)
Air Pollution , Coal , Humans , Coal/analysis , Physical Phenomena
18.
Environ Sci Technol ; 57(48): 20010-20023, 2023 Dec 05.
Article in English | MEDLINE | ID: mdl-37909663

ABSTRACT

Outdoor air pollution causes millions of premature deaths annually worldwide. Sulfate is a major component of particulate pollution. Winter sulfate observations in China show both high concentrations and an accumulation mode with a modal size >1 µm. However, we find that this observed size distribution cannot be simulated using classical gaseous and aqueous phase formation (CSF) or proposed aerosol-processing formation (APF) mechanisms. Specifically, the CSF simulation underestimates sulfate concentrations by 76% over megacities in China and predicts particle size distributions with a modal size of ∼0.35 µm, significantly smaller than observations. Although incorporating the APF mechanism in the atmospheric chemical model notably improves sulfate concentration simulation with reasonable parameters, the simulated sulfate particle size distribution remains similar to that using the CSF mechanism. We further conduct theoretical analyses and show that particles with diameters <0.3 µm grow rapidly (2-3 s) to 1 µm through the condensation of sulfuric acid in fresh high-temperature exhaust plumes, referred to as in-source formation (ISF). An ISF sulfate source equivalent to 15% of sulfur emissions from fossil fuel combustion largely explains both observed size distributions and mass concentrations of sulfate particles. The findings imply that ISF is a major source of wintertime micron-sized sulfate in China and underscore the importance of considering the size distribution of aerosols for accurately assessing the impacts of inorganic aerosols on radiative forcing and human health.


Subject(s)
Air Pollutants , Humans , Air Pollutants/analysis , Particulate Matter/analysis , Sulfates/analysis , Seasons , China , Aerosols/analysis , Environmental Monitoring , Particle Size
19.
Environ Sci Technol ; 57(51): 21662-21672, 2023 Dec 26.
Article in English | MEDLINE | ID: mdl-38079372

ABSTRACT

Air pollution is still one of the most severe problems in northern China, especially in the Jing-Jin-Ji region around Beijing. In recent years, China has implemented many stringent policies to address the air quality issue, including promoting energy transition toward cleaner fuels in residential sectors. But until 2020, even in the Jing-Jin-Ji region, nearly half of the rural households still use solid fuels for heating. For residents who are not covered by the clean heating campaign, we analyze five potential mitigation strategies and evaluate their environmental effects as well as the associated health benefits and costs. We estimate that substitution with electricity or gas would reduce air pollution and premature mortality more strongly, while the relatively low investment costs of implementing clean coal or biomass pellet lead to a larger benefit-cost ratio, indicating higher cost efficiency. Hence, clean coal or biomass pellet could be transitional substitution options for the less developed or remote areas which cannot afford a total transition toward electricity or natural gas in the short term.


Subject(s)
Air Pollutants , Air Pollution, Indoor , Air Pollution , Air Pollutants/analysis , Particulate Matter/analysis , Cost-Benefit Analysis , Air Pollution/analysis , China , Coal/analysis , Policy , Air Pollution, Indoor/analysis , Cooking
20.
Environ Sci Technol ; 57(16): 6465-6473, 2023 04 25.
Article in English | MEDLINE | ID: mdl-37040484

ABSTRACT

Access to safe drinking water is a major public concern in China. A national survey of 57 029 households was conducted to fill major knowledge gaps on drinking water sources, end-of-use treatment methods, and energy used to boil water. Herein, we show that surface water and well water were frequently used by >147 million rural residents living in low-income inland and mountainous areas. Driven by socioeconomic development and government intervention, the level of access to tap water in rural China increased to 70% by 2017. Nevertheless, the rate was considerably lower than that in cities and unevenly distributed across the country. Approximately 90% of drinking water was boiled, an increase from 85% a decade ago. The contribution of electricity, mainly electric kettles, to the boiling of water was 69%. Similar to cooking, living conditions and heating requirements are the main influencing indicators of energy used to boil water. In addition to socioeconomic development, government intervention is a key factor driving the transition to safe water sources, universal access to tap water, and clean energy. Further improvement in drinking water safety in poor and remote rural areas remains challenging, and more intervention and more investment are needed.


Subject(s)
Drinking Water , Water Supply , Humans , China , Cities , Family Characteristics , Rural Population
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