State Key Laboratory of Pollution Control and Resource Reuse

Microplastics have become emerging contaminants, causing widespread concern about their potential toxic effects. In this study, the uptake and tissue accumulation of polystyrene microplastics (PS-MPs) in zebrafish were detected, and the toxic effects in liver were investigated. The results showed that after 7 days of exposure, 5 μm diameter MPs accumulated in fish gills, liver, and gut, while 20 μm diameter MPs accumulated only in fish gills and gut. Histopathological analysis showed that both 5 μm and 70 nm PS-MPs caused inflammation and lipid accumulation in fish liver. PS-MPs also induced significantly increased activities of superoxide dismutase and catalase, indicating that oxidative stress was induced after treatment with MPs. In addition, metabolomic analysis suggested that exposure to MPs induced alterations of metabolic profiles in fish liver and disturbed the lipid and energy metabolism. These findings provide new insights into the toxic effects of MPs on fish.

Adsorption is one of the most widely applied techniques for environmental remediation. Its kinetics are of great significance to evaluate the performance of a given adsorbent and gain insight into the underlying mechanisms. There are lots of references available concerning adsorption kinetics, and several mathematic models have been developed to describe adsorption reaction and diffusion processes. However, these models were frequently employed to fit the kinetic data in an unsuitable or improper manner. This is mainly because the boundary conditions of the associated models were, to a considerable extent, ignored for data modeling. Here we reviewed several widely-used adsorption kinetic models and paid more attention to their boundary conditions. We believe that the review is of certain significance and improvement for adsorption kinetic modeling.

Microplastics (MPs) are a significant environmental health issue and increasingly greater source of concern. MPs have been detected in oceans, rivers, sediments, sewages, soil and even table salts. MPs exposure on marine organisms and humans has been documented, but information about the toxicity of MPs in mammal is limited. Here we used fluorescent and pristine polystyrene microplastics (PS-MPs) particles with two diameters (5 μm and 20 μm) to investigate the tissue distribution, accumulation, and tissue-specific health risk of MPs in mice. Results indicated that MPs accumulated in liver, kidney and gut, with a tissue-accumulation kinetics and distribution pattern that was strongly depended on the MPs particle size. In addition, analyses of multiple biochemical biomarkers and metabolomic profiles suggested that MPs exposure induced disturbance of energy and lipid metabolism as well as oxidative stress. Interestingly, blood biomarkers of neurotoxicity were also altered. Our results uncovered the distribution and accumulation of MPs across mice tissues and revealed significant alteration in several biomarkers that indicate potential toxicity from MPs exposure. Collectively, our data provided new evidence for the adverse consequences of MPs.

Rare species are increasingly recognized as crucial, yet vulnerable components of Earth's ecosystems. This is also true for microbial communities, which are typically composed of a high number of relatively rare species. Recent studies have demonstrated that rare species can have an over-proportional role in biogeochemical cycles and may be a hidden driver of microbiome function. In this review, we provide an ecological overview of the rare microbial biosphere, including causes of rarity and the impacts of rare species on ecosystem functioning. We discuss how rare species can have a preponderant role for local biodiversity and species turnover with rarity potentially bound to phylogenetically conserved features. Rare microbes may therefore be overlooked keystone species regulating the functioning of host-associated, terrestrial and aquatic environments. We conclude this review with recommendations to guide scientists interested in investigating this rapidly emerging research area.

This review provides an overview of electrocatalytic reduction of nitrate, including the reaction mechanisms, reactor design principles, product detection methods, and performance evaluation methods, which can provide a sustainable nitrogen cycle.

Herein, we proposed a new peroxymonosulfate (PMS) activation system employing the Fe(III) doped g-C3N4 (CNF) as catalyst. Quite different from traditional sulfate radical-based advanced oxidation processes (SR-AOPs), the PMS/CNF system was capable of selectively degrading phenolic compounds (e.g., p-chlorophenol, 4-CP) in a wide pH range (3–9) via nonradical pathway. The generated singlet oxygen (1O2) in the PMS/CNF3 (3.46 wt % Fe) system played negligible role in removing 4-CP, and high-valent iron-oxo species fixated in the nitrogen pots of g-C3N4 (≡FeV═O) was proposed as the dominant reactive species by using dimethyl sulfoxide as a probe compound. The mechanism was hypothesized that PMS was first bound to the Fe(III)-N moieties to generate ≡FeV═O, which effectively reacted with 4-CP via electron transfer. GC-MS analysis indicated that 4-chlorocatechol and 1,4-benzoquinone were the major intermediates, which could be further degraded to carboxylates. The kinetic results suggested that the formation of ≡FeV═O was proportional to the dosages of PMS and CNF3 under the experimental conditions. Also, the PMS/CNF3 system exhibited satisfactory removal of 4-CP in the presence of inorganic anions and natural organic matters. We believe that this study will provide a new routine for effective PMS activation by heterogeneous iron-complexed catalysts to efficiently degrade organic contaminants via nonradical pathway.

In the environment, microplastics are subjected to multiple aging processes; however, information regarding the impact of aging on the environmental behavior of microplastics is still lacking. This study investigated the alteration properties of polystyrene and high-density polyethylene microplastics by heat-activated K2S2O8 and Fenton treatments to improve the understanding of their long-term natural aging in aquatic environments. Our results indicated that the O/C ratio was an alternative parameter to the carbonyl index (CI) to quantitatively describe the surface alteration properties of microplastics. The correlation model of the O/C ratio or CI versus alteration time was developed and compared by natural alteration of microplastics in freshwater samples. Moreover, the regression equation of the equilibrium adsorption capacity of altered microplastics versus the O/C ratio and average size was proposed. This study is the first effort in differentiating the relationships between the alteration properties and alteration time/adsorption capacity of microplastics, which would be helpful for predicting the weathering degree and accumulation of hydrophilic antibiotics onto aged microplastics in aquatic environments. This research develops promising strategies to accelerate the aging reactions using advanced oxidation processes, which would provide further information to assess the microplastic pollution in actual environments.

nanoparticles distributed inside multiwalled carbon nanotubes with inner diameter of ∼7 nm. Unlike the traditional Fenton-like processes, this delicately designed system was shown to selectively oxidize the organic dyes that could be adsorbed with oxidation rates linearly proportional to the adsorption affinity. It also exhibited remarkably higher degradation activity (22.5 times faster) toward a model pollutant methylene blue than its nonconfined analog. Strikingly, the unforeseen stability at pH value up to 9.0 greatly expands the use of Fenton-like catalysts in alkaline conditions. This work represents a fundamental breakthrough toward the design and understanding of the Fenton-like system under nanoconfinement, might cause implications in other fields, especially in biological systems.

Eutrophication of water bodies is a serious and widespread environmental problem. Achieving low levels of phosphate concentration to prevent eutrophication is one of the important goals of the wastewater engineering and surface water management. Meeting the increasingly stringent standards is feasible in using a phosphate-selective sorption system. This critical review discusses the most fundamental aspects of selective phosphate removal processes and highlights gains from the latest developments of phosphate-selective sorbents. Selective sorption of phosphate over other competing anions can be achieved based on their differences in acid-base properties, geometric shapes, and metal complexing abilities. Correspondingly, interaction mechanisms between the phosphate and sorbent are categorized as hydrogen bonding, shape complementarity, and inner-sphere complexation, and their representative sorbents are organic-functionalized materials, molecularly imprinted polymers, and metal-based materials, respectively. Dominating factors affecting the phosphate sorption performance of these sorbents are critically examined, along with a discussion of some overlooked facts regarding the development of high-performance sorbents for selective phosphate removal from water and wastewater.

Significant concerns have been raised over the presence of antibiotics including tetracyclines in aquatic environments. We herein studied single-walled carbon nanotubes (SWNT) and multi-walled carbon nanotubes (MWNT) as potential effective adsorbents for removal of tetracycline from aqueous solution. In comparison, a nonpolar adsorbate, naphthalene, and two other carbonaceous adsorbents, pulverized activated carbon (AC) and nonporous graphite, were used. The observed adsorbent-to-solution distribution coefficient (Kd, L/kg) of tetracycline was in the order of 10(4)-10(6) L/kg for SWNT, 10(3)-10(4) L/kg for MWNT, 10(3)-10(4) L/kg for AC, and 10(3)-10(5) L/kg for graphite. Upon normalization for adsorbent surface area, the adsorption affinity of tetracycline decreased in the order of graphite/ SWNT > MWNT >> AC. The weaker adsorption of tetracycline to AC indicates that for bulky adsorbates adsorption affinity is greatly affected by the accessibility of available adsorption sites. The remarkably strong adsorption of tetracycline to the carbon nanotubes and to graphite can be attributed to the strong adsorptive interactions (van der Waals forces, pi-pi electron-donor-acceptor interactions, cation-pi bonding) with the graphene surface. Complexation between tetracycline and model graphene compounds (naphthalene, phenanthrene, pyrene) in solution phase was verified by ring current-induced 1H NMR upfield chemical shifts of tetracycline moieties.

Abstract The COVID-19 pandemic is impacting human activities, and in turn energy use and carbon dioxide (CO 2 ) emissions. Here we present daily estimates of country-level CO 2 emissions for different sectors based on near-real-time activity data. The key result is an abrupt 8.8% decrease in global CO 2 emissions (−1551 Mt CO 2 ) in the first half of 2020 compared to the same period in 2019. The magnitude of this decrease is larger than during previous economic downturns or World War II. The timing of emissions decreases corresponds to lockdown measures in each country. By July 1st, the pandemic’s effects on global emissions diminished as lockdown restrictions relaxed and some economic activities restarted, especially in China and several European countries, but substantial differences persist between countries, with continuing emission declines in the U.S. where coronavirus cases are still increasing substantially.

We demonstrated high-performance gas sensors based on graphene oxide (GO) sheets partially reduced via low-temperature thermal treatments. Hydrophilic graphene oxide sheets uniformly suspended in water were first dispersed onto gold interdigitated electrodes. The partial reduction of the GO sheets was then achieved through low-temperature, multi-step annealing (100, 200, and 300 degrees C) or one-step heating (200 degrees C) of the device in argon flow at atmospheric pressure. The electrical conductance of GO was measured after each heating cycle to interpret the level of reduction. The thermally-reduced GO showed p-type semiconducting behavior in ambient conditions and was responsive to low-concentration NO2 and NH3 gases diluted in air at room temperature. The sensitivity can be attributed mainly to the electron transfer between the reduced GO and adsorbed gaseous molecules (NO2/NH3). Additionally, the contact between GO and the Au electrode is likely to contribute to the overall sensing response because of the adsorbates-induced Schottky barrier variation. A simplified model is used to explain the experimental observations.

Abstract Rationale Evidence concerning the acute health effects of air pollution caused by fine particulate matter (PM2.5) in developing countries is quite limited. Objectives To evaluate short-term associations between PM2.5 and daily cause-specific mortality in China. Methods A nationwide time-series analysis was performed in 272 representative Chinese cities from 2013 to 2015. Two-stage Bayesian hierarchical models were applied to estimate regional- and national-average associations between PM2.5 concentrations and daily cause-specific mortality. City-specific effects of PM2.5 were estimated using the overdispersed generalized additive models after adjusting for time trends, day of the week, and weather conditions. Exposure–response relationship curves and potential effect modifiers were also evaluated. Measurements and Main Results The average of annual mean PM2.5 concentration in each city was 56 μg/m3 (minimum, 18 μg/m3; maximum, 127 μg/m3). Each 10-μg/m3 increase in 2-day moving average of PM2.5 concentrations was significantly associated with increments in mortality of 0.22% from total nonaccidental causes, 0.27% from cardiovascular diseases, 0.39% from hypertension, 0.30% from coronary heart diseases, 0.23% from stroke, 0.29% from respiratory diseases, and 0.38% from chronic obstructive pulmonary disease. There was a leveling off in the exposure–response curves at high concentrations in most, but not all, regions. The associations were stronger in cities with lower PM2.5 levels or higher temperatures, and in subpopulations with elder age or less education. Conclusions This nationwide investigation provided robust evidence of the associations between short-term exposure to PM2.5 and increased mortality from various cardiopulmonary diseases in China. The magnitude of associations was lower than those reported in Europe and North America.

Human ingestion of microplastics (MPs) is inevitable due to the ubiquity of MPs in various foods and drinking water. Whether the ingestion of MPs poses a substantial risk to human health is far from understood. Here, by analyzing the characteristics of MPs in the feces of patients with inflammatory bowel disease (IBD) and healthy people, for the first time, we found that the fecal MP concentration in IBD patients (41.8 items/g dm) was significantly higher than that in healthy people (28.0 items/g dm). In total, 15 types of MPs were detected in feces, with poly(ethylene terephthalate) (22.3-34.0%) and polyamide (8.9-12.4%) being dominant, and their primary shapes were sheets and fibers, respectively. We present evidence indicating that a positive correlation exists between the concentration of fecal MPs and the severity of IBD. Combining a questionnaire survey and the characteristics of fecal MPs, we conclude that the plastic packaging of drinking water and food and dust exposure are important sources of human exposure to MPs. Furthermore, the positive correlation between fecal MPs and IBD status suggests that MP exposure may be related to the disease process or that IBD exacerbates the retention of MPs. The relative mechanisms deserve further studies. Our results also highlight that fecal MPs are useful for assessing human MP exposure and potential health risks.

Understanding adsorptive interactions between organic contaminants and carbon nanotubes is critical to both the environmental application of carbon nanotubes as special adsorbents and the assessment of the potential impact of carbon nanotubes on the fate and transport of organic contaminants in the environment. The adsorption of organic compounds with varied physical-chemical properties (hydrophobicity, polarity, electron polarizability, and size) to one single-walled carbon nanotube (SWNT) and two multiwalled carbon nanotubes (MWNTs) was evaluated. For a given carbon nanotube, the adsorption affinity correlated poorly with hydrophobicity but increased in the order of nonpolar aliphatic < nonpolar aromatics < nitroaromatics, and within the group of nitroaromatics, the adsorption affinity increased with the number of nitrofunctional groups. We propose that the strong adsorptive interaction between carbon nanotubes and nitroaromatics was due to the pi-pi electron-donor-acceptor (EDA) interaction between nitroaromatic molecules (electron acceptors) and the highly polarizable graphene sheets (electron donors) of carbon nanotubes. Additionally, we attribute the stronger adsorption of nonpolar aromatics compared to that of nonpolar aliphatics to the pi-electron coupling between the flat surfaces of both aromatic molecules and carbon nanotubes. For tetrachlorobenzene, the bulkiest adsorbate, adsorption affinity (on a unit surface area basis) to the SWNT was much stronger than to the two MWNTs, indicating a probable molecular sieving effect.

An alkali-acitvated method was explored to synthesize activated carbon nanotubes (CNTs-A) with a high specific surface area (SSA), and a large number of mesopores. The resulting CNTs-A were used as an adsorbent material for removal of anionic and cationic dyes in aqueous solutions. Experimental results indicated that CNTs-A have excellent adsorption capacity for methyl orange (149 mg/g) and methylene blue (399 mg/g). Alkali-activation treatment of CNTs increased the SSA and pore volume (PV), and introduced oxygen-containing functional groups on the surface of CNTs-A, which would be beneficial to improving the adsorption affinity of CNTs-A for removal of dyes. Kinetic regression results shown that the adsorption kinetic was more accurately represented by a pseudo second-order model. The overall adsorption process was jointly controlled by external mass transfer and intra-particle diffusion, and intra-particle diffusion played a dominant role. Freundlich isotherm model showed a better fit with adsorption data than Langmuir isotherm model. Adsorption interactions of dyes onto CNTs-A from aqueous solutions were investigated using Fourier transform infrared (FT-IR) spectroscopy, scanning electron microscopy (SEM), X-ray diffraction (XRD), and Brunauer-Emmett-Teller (BET) method. The remarkable adsorption capacity of dye onto CNTs-A can be attributed to the multiple adsorption interaction mechanisms (hydrogen bonding, π-π electron-donor-acceptor interactions, electrostatic interactions, mesopore filling) on the CNTs-A. Results of this work are of great significance for environmental applications of activated CNTs as a promising adsorbent nanomaterial for organic pollutants from aqueous solutions.

Metal-organic frameworks (MOFs) represent a fascinating class of solid crystalline materials which can be self-assembled in a straightforward manner by the coordination of metal ions or clusters with organic ligands. Owing to their intrinsic porous characteristics, unique chemical versatility and abundant functionalities, MOFs have received substantial attention for diverse industrial applications, including membrane separation. Exciting research activities ranging from fabrication strategies to separation applications of MOF-based membranes have appeared. Inspired by the marvelous achievements of MOF-based membranes in gas separations, liquid separations are also being explored for the purpose of constructing continuous MOFs membranes or MOF-based mixed matrix membranes. Although these are in an emerging stage of vigorous development, most efforts are directed towards improving the liquid separation efficiency with well-designed MOF-based membranes. Therefore, as an increasing trend in membrane separation, the field of MOF-based membranes for liquid separation is highlighted in this review. The criteria for judicious selection of MOFs in fabricating MOF-based membranes are given. Special attention is paid to rational design strategies for MOF-based membranes, along with the latest application progress in the area of liquid separations, such as pervaporation, water treatment, and organic solvent nanofiltration. Moreover, some attractive dual-function applications of MOF-based membranes in the removal of micropollutants, degradation, and antibacterial activity are also reviewed. Finally, we define the remaining challenges and future opportunities in this field. This Tutorial Review provides an overview and outlook for MOF-based membranes for liquid separations. Further development of MOF-based membranes for liquid separation must consider the demands of strict separation standards and environmental safety for industrial application.

Abstract Traditionally, the selective preservation of certain recalcitrant organic compounds and the formation of recalcitrant humic substances have been regarded as an important mechanism for soil organic matter (SOM) stabilization. Based on a critical overview of available methods and on results from a cooperative research program, this paper evaluates how relevant recalcitrance is for the long‐term stabilization of SOM or its fractions. Methodologically, recalcitrance is difficult to assess, since the persistence of certain SOM fractions or specific compounds may also be caused by other stabilization mechanisms, such as physical protection or chemical interactions with mineral surfaces. If only free particulate SOM obtained from density fractionation is considered, it rarely reaches ages exceeding 50 y. Older light particles have often been identified as charred plant residues or as fossil C. The degradability of the readily bioavailable dissolved or water‐extractable OM fraction is often negatively correlated with its content in aromatic compounds, which therefore has been associated with recalcitrance. But in subsoils, dissolved organic matter aromaticity and biodegradability both are very low, indicating that other factors or compounds limit its degradation. Among the investigated specific compounds, lignin, lipids, and their derivatives have mean turnover times faster or similar as that of bulk SOM. Only a small fraction of the lignin inputs seems to persist in soils and is mainly found in the fine textural size fraction (&lt;20 µm), indicating physico‐chemical stabilization. Compound‐specific analysis of 13 C : 12 C ratios of SOM pyrolysis products in soils with C3‐C4 crop changes revealed no compounds with mean residence times of &gt; 40–50 y, unless fossil C was present in substantial amounts, as at a site exposed to lignite inputs in the past. Here, turnover of pyrolysis products seemed to be much longer, even for those attributed to carbohydrates or proteins. Apparently, fossil C from lignite coal is also utilized by soil organisms, which is further evidenced by low 14 C concentrations in microbial phospholipid fatty acids from this site. Also, black C from charred plant materials was susceptible to microbial degradation in a short‐term (60 d) and a long‐term (2 y) incubation experiment. This degradation was enhanced, when glucose was supplied as an easily available microbial substrate. Similarly, SOM mineralization in many soils generally increased after addition of carbohydrates, amino acids, or simple organic acids, thus indicating that stability may also be caused by substrate limitations. It is concluded that the presented results do not provide much evidence that the selective preservation of recalcitrant primary biogenic compounds is a major SOM‐stabilization mechanism. Old SOM fractions with slow turnover rates were generally only found in association with soil minerals. The only not mineral‐associated SOM components that may be persistent in soils appear to be black and fossil C.

Electrochemical energy storage and conversion through hydrogen is essential for a clean and sustainable energy system. Highly efficient hydrogen electrocatalysts play a key role in the electrochemical transformation reactions. A comprehensive understanding of the hydrogen reaction kinetics and mechanisms is critical for the catalyst design and development. Especially pH-dependent hydrogen evolution and oxidation reaction (HER/HOR) kinetics receives increasing interest, and understanding its origin adds new knowledge to fundamental hydrogen electrocatalysis. Here, a detailed description of kinetic analysis and reaction mechanisms for HER/HOR, and a brief summary about recent development of highly efficient and cost-effective hydrogen electrocatalysts are presented. Lastly, recent advances in the fundamental understanding of pH-dependent hydrogen electrocatalysis are discussed.

Sustainable agriculture is a key component of the effort to meet the increased food demand of a rapidly increasing global population. Nano-biotechnology is a promising tool for sustainable agriculture. However, rather than acting as nanocarriers, some nanoparticles (NPs) with unique physiochemical properties inherently enhance plant growth and stress tolerance. This biological role of nanoparticles depends on their physiochemical properties, application method (foliar delivery, hydroponics, soil), and the applied concentration. Here we review the effects of the different types, properties, and concentrations of nanoparticles on plant growth and on various abiotic (salinity, drought, heat, high light, and heavy metals) and biotic (pathogens and herbivores) stresses. The ability of nanoparticles to stimulate plant growth by positive effects on seed germination, root or shoot growth, and biomass or grain yield is also considered. The information presented herein will allow researchers within and outside the nano-biotechnology field to better select the appropriate nanoparticles as starting materials in agricultural applications. Ultimately, a shift from testing/utilizing existing nanoparticles to designing specific nanoparticles based on agriculture needs will facilitate the use of nanotechnology in sustainable agriculture.