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1.
Sci Total Environ ; 932: 173033, 2024 May 07.
Artigo em Inglês | MEDLINE | ID: mdl-38723954

RESUMO

Microplastics (MPs) pollution has emerged as a global concern, and wastewater treatment plants (WWTPs) are one of the potential sources of MPs in the environment. However, the effect of polyethylene MPs (PE) on nitrogen (N) removal in moving bed biofilm reactor (MBBR) remains unclear. We hypothesized that PE would affect N removal in MBBR by influencing its microbial community. In this study, we investigated the impacts of different PE concentrations (100, 500, and 1000 µg/L) on N removal, enzyme activities, and microbial community in MBBR. Folin-phenol and anthrone colorimetric methods, oxidative stress and enzyme activity tests, and high-throughput sequencing combined with bioinformation analysis were used to decipher the potential mechanisms. The results demonstrated that 1000 µg/L PE had the greatest effect on NH4+-N and TN removal, with a decrease of 33.5 % and 35.2 %, and nitrifying and denitrifying enzyme activities were restrained by 29.5-39.6 % and 24.6-47.4 %. Polysaccharide and protein contents were enhanced by PE, except for 1000 µg/L PE, which decreased protein content by 65.4 mg/g VSS. The positive links of species interactions under 1000 µg/L PE exposure was 52.07 %, higher than under 500 µg/L (51.05 %) and 100 µg/L PE (50.35 %). Relative abundance of some metabolism pathways like carbohydrate metabolism and energy metabolism were restrained by 0.07-0.11 % and 0.27-0.4 %. Moreover, the total abundance of nitrification and denitrification genes both decreased under PE exposure. Overall, PE reduced N removal by affecting microbial community structure and species interactions, inhibiting some key metabolic pathways, and suppressing key enzyme activity and functional gene abundance. This paper provides new insights into assessing the risk of MPs to WWTPs, contributing to ensuring the health of aquatic ecosystems.

2.
Water Res ; 257: 121700, 2024 Apr 30.
Artigo em Inglês | MEDLINE | ID: mdl-38705068

RESUMO

Sulfur-based denitrification is a promising technology in treatments of nitrate-contaminated wastewaters. However, due to weak bioavailability and electron-donating capability of elemental sulfur, its sulfur-to-nitrate ratio has long been low, limiting the support for dissimilatory nitrate reduction to ammonium (DNRA) process. Using a long-term sulfur-packed reactor, we demonstrate here for the first time that DNRA in sulfur-based system is not negligible, but rather contributes a remarkable 40.5 %-61.1 % of the total nitrate biotransformation for ammonium production. Through combination of kinetic experiments, electron flow analysis, 16S rRNA amplicon, and microbial network succession, we unveil a cryptic in-situ sulfur disproportionation (SDP) process which significantly facilitates DNRA via enhancing mass transfer and multiplying 86.7-210.9 % of bioavailable electrons. Metagenome assembly and single-copy gene phylogenetic analysis elucidate the abundant genomes, including uc_VadinHA17, PHOS-HE36, JALNZU01, Thiobacillus, and Rubrivivax, harboring complete genes for ammonification. Notably, a unique group of self-SDP-coupled DNRA microorganism was identified. This study unravels a previously concealed fate of DNRA, which highlights the tremendous potential for ammonium recovery and greenhouse gas mitigation. Discovery of a new coupling between nitrogen and sulfur cycles underscores great revision needs of sulfur-driven denitrification technology.

3.
Sci Total Environ ; 931: 172901, 2024 Apr 30.
Artigo em Inglês | MEDLINE | ID: mdl-38697549

RESUMO

High nitrate pollution in agriculture and industry poses a challenge to emerging methane oxidation coupled denitrification. In this study, an efficient nitrate removal efficiency of 100 % was achieved at an influent loading rate of 400 mg-N/L·d, accompanied by the production of short chain fatty acids (SCFAs) with a maximum value of 80.9 mg/L. Batch tests confirmed that methane was initially converted to acetate, which then served as a carbon source for denitrification. Microbial community characterization revealed the dominance of heterotrophic denitrifiers, including Simplicispira (22.8 %), Stappia (4.9 %), and the high­nitrogen-tolerant heterotrophic denitrifier Diaphorobacter (19.0 %), at the nitrate removal rate of 400 mg-N/L·d. Notably, the low abundance of methanotrophs ranging from 0.24 % to 3.75 % across all operational stages does not fully align with the abundance of pmoA genes, suggesting the presence of other functional microorganisms capable of methane oxidation and SCFAs production. These findings could facilitate highly efficient denitrification driven by methane and contributed to the development of denitrification using methane as an electron donor.

4.
Sci Total Environ ; 929: 172598, 2024 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-38642769

RESUMO

Wastewater treatment is an important source of non-CO2 greenhouse gases (GHGs). However, current quantification of these GHG emissions mainly employs unit-based measurements, where emissions from individual process units are identified, leading to large uncertainties of overall emissions. Here we introduce plant-integrated measurements, where emissions from the whole plant are measured through the off-gas pipelines of the enclosed facility, to quantify methane (CH4) and nitrous oxide (N2O) emissions from an underground municipal wastewater treatment plant (WWTP) in southern China. Our results show that the primary oxic tank contributes the largest in total CH4 and N2O emissions, with an average fraction of over 80 % and over 90 %, respectively. This can be attributed to the vigorous aeration process, which facilitates the transfer of dissolved CH4 and N2O from the liquid phase to the atmosphere through intensive air stripping. The plant-integrated measurements yield around 3-9 times higher emission factors of CH4 and N2O than the unit-based measurements. This difference in emission accounting is attributed to both varying survey durations of the two approaches and the omission of uncertain emission sources during unit-based measurements. The comparison between these two approaches indicates that plant-integrated measurements are more applicable for emission quantification of the whole plant whereas unit-based measurements provide insights into the emission characteristics of individual process units. More plant-integrated measurements are needed in the future for more accurate emission accounting of WWTPs.

5.
Sci Total Environ ; 929: 172651, 2024 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-38653406

RESUMO

The widespread use of microplastics (MPs) has led to an increase in their discharge to wastewater treatment plants. However, the knowledge of impact of MPs on macro-performance and micro-ecology in simultaneous nitrification, denitrification, and phosphorus removal (SNDPR) systems is limited, hampering the understanding of potential risks posed by MPs. This study firstly comprehensively investigated the performance, species interactions, and community assembly under polystyrene (PS) and polyvinyl chloride (PVC) exposure in SNDPR systems. The results showed under PS (1, 10 mg/L) and PVC (1, 10 mg/L) exposure, total nitrogen removal was reduced by 3.38-10.15 %. PS and PVC restrained the specific rates of nitrite and nitrate reduction (SNIRR, SNRR), as well as the activities of nitrite and nitrate reductase enzymes (NIR, NR). The specific ammonia oxidation rate (SAOR) and activity of ammonia oxidase enzyme (AMO) were reduced only at 10 mg/L PVC. PS and PVC enhanced the size of co-occurrence networks, niche breadth, and number of key species while decreasing microbial cooperation by 5.85-13.48 %. Heterogeneous selection dominated microbial community assembly, and PS and PVC strengthened the contribution of stochastic processes. PICRUSt prediction further revealed some important pathways were blocked by PS and PVC. Together, the reduced TN removal under PS and PVC exposure can be attributed to the inhibition of SAOR, SNRR, and SNIRR, the restrained activities of NIR, NR, and AMO, the changes in species interactions and community assembly mechanisms, and the suppression of some essential metabolic pathways. This paper offers a new perspective on comprehending the effects of MPs on SNDPR systems.


Assuntos
Desnitrificação , Microplásticos , Nitrificação , Fósforo , Eliminação de Resíduos Líquidos , Poluentes Químicos da Água , Fósforo/metabolismo , Poluentes Químicos da Água/metabolismo , Poluentes Químicos da Água/análise , Eliminação de Resíduos Líquidos/métodos , Águas Residuárias , Microbiota
6.
Environ Sci Technol ; 58(16): 6998-7009, 2024 Apr 23.
Artigo em Inglês | MEDLINE | ID: mdl-38602777

RESUMO

Phosphorus (P) is the key in maintaining food security and ecosystem functions. Population growth and economic development have increased the demand for phosphate rocks. China has gradually developed from zero phosphate mining to the world's leading P miner, fertilizer, and agricultural producer since 1949. China released policies, such as designating phosphate rock as a strategic resource, promoting eco-agricultural policies, and encouraging the use of solid wastes produced in mining and the phosphorus chemical industry as construction materials. However, methodological and data gaps remain in the mapping of the long-term effects of policies on P resource efficiency. Here, P resource efficiency can be represented by the potential of the P cycle to concentrate or dilute P as assessed by substance flow analysis (SFA) complemented by statistical entropy analysis (SEA). P-flow quantification over the past 70 years in China revealed that both resource utilization and waste generation peaked around 2015, with 20 and 11 Mt of mined and wasted P, respectively. Additionally, rapidly increasing aquaculture wastewater has exacerbated pollution. The resource efficiency of the Chinese P cycle showed a U-shaped change with an overall improvement of 22.7%, except for a temporary trough in 1975. The driving force behind the efficiency decline was the roaring phosphate fertilizer industry, as confirmed by the sharp increase in P flows for both resource utilization and waste generation from the mid-1960s to 1975. The positive driving forces behind the 30.7% efficiency increase from 1975 to 2018 were the implementation of the resource conservation policy, downstream pollution control, and, especially, the circular agro-food system strategy. However, not all current management practices improve the P resource efficiency. Mixing P industry waste with construction materials and the development of aquaculture to complement offshore fisheries erode P resource efficiency by 2.12% and 9.19%, respectively. With the promotion of a zero-waste society in China, effective P-cycle management is expected.


Assuntos
Desenvolvimento Econômico , Fósforo , China , Fertilizantes , Agricultura
7.
Environ Sci Technol ; 58(15): 6647-6658, 2024 Apr 16.
Artigo em Inglês | MEDLINE | ID: mdl-38563431

RESUMO

The biodegradation of polypropylene (PP), a highly persistent nonhydrolyzable polymer, by Tenebrio molitor has been confirmed using commercial PP microplastics (MPs) (Mn 26.59 and Mw 187.12 kDa). This confirmation was based on the reduction of the PP mass, change in molecular weight (MW), and a positive Δδ13C in the residual PP. A MW-dependent biodegradation mechanism was investigated using five high-purity PP MPs, classified into low (0.83 and 6.20 kDa), medium (50.40 and 108.0 kDa), and high (575.0 kDa) MW categories to access the impact of MW on the depolymerization pattern and associated gene expression of gut bacteria and the larval host. The larvae can depolymerize/biodegrade PP polymers with high MW although the consumption rate and weight losses increased, and survival rates declined with increasing PP MW. This pattern is similar to observations with polystyrene (PS) and polyethylene (PE), i.e., both Mn and Mw decreased after being fed low MW PP, while Mn and/or Mw increased after high MW PP was fed. The gut microbiota exhibited specific bacteria associations, such as Kluyvera sp. and Pediococcus sp. for high MW PP degradation, Acinetobacter sp. for medium MW PP, and Bacillus sp. alongside three other bacteria for low MW PP metabolism. In the host transcriptome, digestive enzymes and plastic degradation-related bacterial enzymes were up-regulated after feeding on PP depending on different MWs. The T. molitor host exhibited both defensive function and degradation capability during the biodegradation of plastics, with high MW PP showing a relatively negative impact on the larvae.


Assuntos
Microbiota , Tenebrio , Animais , Tenebrio/metabolismo , Tenebrio/microbiologia , Plásticos , Polipropilenos/metabolismo , Microplásticos , Peso Molecular , Poliestirenos , Larva/metabolismo , Bactérias/metabolismo , Biodegradação Ambiental
8.
Environ Sci Ecotechnol ; 20: 100412, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38560759

RESUMO

Effective management of large basins necessitates pinpointing the spatial and temporal drivers of primary index exceedances and urban risk factors, offering crucial insights for basin administrators. Yet, comprehensive examinations of multiple pollutants within the Yangtze River Basin remain scarce. Here we introduce a pollution inventory for urban clusters surrounding the Yangtze River Basin, analyzing water quality data from 102 cities during 2018-2019. We assessed the exceedance rates for six pivotal indicators: dissolved oxygen (DO), ammonia nitrogen (NH3-N), chemical oxygen demand (COD), biochemical oxygen demand (BOD), total phosphorus (TP), and the permanganate index (CODMn) for each city. Employing random forest regression and SHapley Additive exPlanations (SHAP) analyses, we identified the spatiotemporal factors influencing these key indicators. Our results highlight agricultural activities as the primary contributors to the exceedance of all six indicators, thus pinpointing them as the leading pollution source in the basin. Additionally, forest coverage, livestock farming, chemical and pharmaceutical sectors, along with meteorological elements like precipitation and temperature, significantly impacted various indicators' exceedances. Furthermore, we delineate five core urban risk components through principal component analysis, which are (1) anthropogenic and industrial activities, (2) agricultural practices and forest extent, (3) climatic variables, (4) livestock rearing, and (5) principal polluting sectors. The cities were subsequently evaluated and categorized based on these risk components, incorporating policy interventions and administrative performance within each region. The comprehensive analysis advocates for a customized strategy in addressing the discerned risk factors, especially for cities presenting elevated risk levels.

9.
Environ Res ; 252(Pt 1): 118834, 2024 Mar 31.
Artigo em Inglês | MEDLINE | ID: mdl-38565414

RESUMO

Iron-doped biochar has been widely used as an adsorbent to remove contaminants due to the high adsorption performance, but it still suffers from complicated preparation methods, unstable iron loading, unsatisfactory specific surface area, and uneven distribution of active sites. Here, a novel magnetic porous biochar (FeCS800) with nanostructure on surface was synthesized by one-pot pyrolysis method of corn straw with K2FeO4, and used in orange G (OG) and tetracycline (TC) adsorption. FeCS800 exhibited outstanding adsorption capacities for OG and TC after K2FeO4 activation and the adsorption data were fitted satisfactorily to Langmuir isotherm and Pseudo-second-order kinetic model. The maximum adsorption capacities of FeCS800 for OG and TC were around 303.03 mg/g and 322.58 mg/g, respectively, at 25 °C and pH 7.0, which were 16.27 and 24.61 times higher than that before modification. Thermodynamic studies showed that the adsorption of OG/TC by FeCS800 were thermodynamically favorable and highly spontaneous. And the adsorption capacity of OG and TC by FeCS800 remained 77% and 81% after 5 cycles, respectively, indicating that FeCS800 had good stability. The outstanding adsorption properties and remarkable reusability of FeCS800 show its great potential to be an economic and environmental adsorbent in contaminants removal.

10.
Water Res ; 256: 121571, 2024 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-38583332

RESUMO

'Candidatus Methanoperedens nitroreducens' is an archaeal methanotroph with global importance that links carbon and nitrogen cycles and great potential for sustainable operation of wastewater treatment. It has been reported to mediate the anaerobic oxidation of methane through a reverse methanogenesis pathway while reducing nitrate to nitrite. Here, we demonstrate that 'Ca. M. nitroreducens' reduces ferric iron forming ammonium (23.1 %) and nitrous oxide (N2O, 46.5 %) from nitrate. These results are supported with the upregulation of genes coding for proteins responsible for dissimilatory nitrate reduction to ammonium (nrfA), N2O formation (norV, cyt P460), and multiple multiheme c-type cytochromes for ferric iron reduction. Concomitantly, an increase in the N2O-reducing SJA-28 lineage and a decrease in the nitrite-reducing 'Candidatus Methylomirabilis oxyfera' are consistent with the changes in 'Ca. M. nitroreducens' end products. These findings demonstrate the highly flexible physiology of 'Ca. M. nitroreducens' in anaerobic ecosystems with diverse electron acceptor conditions, and further reveals its roles in linking methane oxidation to global biogeochemical cycles. 'Ca. M. nitroreducens' could significantly affect the bioavailability of nitrogen sources as well as the emission of greenhouse gas in natural ecosystems and wastewater treatment plants.


Assuntos
Compostos de Amônio , Metano , Nitratos , Óxido Nitroso , Oxirredução , Metano/metabolismo , Óxido Nitroso/metabolismo , Compostos de Amônio/metabolismo , Anaerobiose , Nitratos/metabolismo , Compostos Férricos/metabolismo
11.
Water Res ; 256: 121600, 2024 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-38640563

RESUMO

A limited understanding of microbial interactions and community assembly mechanisms in constructed wetlands (CWs), particularly with different substrates, has hampered the establishment of ecological connections between micro-level interactions and macro-level wetland performance. In this study, CWs with distinct substrates (zeolite, CW_A; manganese ore, CW_B) were constructed to investigate the nutrient removal efficiency, microbial interactions, metabolic mechanisms, and ecological assembly for treating rural sewage with a low carbon-to-nitrogen ratio. CW_B showed higher removal of ammonia nitrogen and total nitrogen by about 1.75-6.75 % and 3.42-5.18 %, respectively, compared to CW_A. Candidatus_Competibacter (denitrifying glycogen-accumulating bacteria) was the dominant microbial genus in CW_A, whereas unclassified_f_Blastocatellaceae (involved in carbon and nitrogen transformation) dominated in CW_B. The null model revealed that stochastic processes (drift) dominated community assembly in both CWs; however, deterministic selection accounted for a higher proportion in CW_B. Compared to those in CW_A, the interactions between microbes in CW_B were more complex, with more key microbes involved in carbon, nitrogen, and phosphorus conversion; the synergistic cooperation of functional bacteria facilitated simultaneous nitrification-denitrification. Manganese ores favour biofilm formation, increase the activity of the electron transport system, and enhance ammonia oxidation and nitrate reduction. These results elucidated the ecological patterns exhibited by microbes under different substrate conditions thereby contributing to our understanding of how substrates shape distinct microcosms in CW systems. This study provides valuable insights for guiding the future construction and management of CWs.


Assuntos
Carbono , Nitrogênio , Eliminação de Resíduos Líquidos , Águas Residuárias , Áreas Alagadas , Nitrogênio/metabolismo , Carbono/metabolismo , Eliminação de Resíduos Líquidos/métodos , Bactérias/metabolismo
12.
Sci Total Environ ; 931: 172466, 2024 Apr 16.
Artigo em Inglês | MEDLINE | ID: mdl-38626826

RESUMO

The burgeoning issue of plasmid-mediated resistance genes (ARGs) dissemination poses a significant threat to environmental integrity. However, the prediction of ARGs prevalence is overlooked, especially for emerging ARGs that are potentially evolving gene exchange hotspot. Here, we explored to classify plasmid or chromosome sequences and detect resistance gene prevalence by using DNABERT. Initially, the DNABERT fine-tuned in plasmid and chromosome sequences followed by multilayer perceptron (MLP) classifier could achieve 0.764 AUC (Area under curve) on external datasets across 23 genera, outperforming 0.02 AUC than traditional statistic-based model. Furthermore, Escherichia, Pseudomonas single genera based model were also be trained to explore its predict performance to ARGs prevalence detection. By integrating K-mer frequency attributes, our model could boost the performance to predict the prevalence of ARGs in an external dataset in Escherichia with 0.0281-0.0615 AUC and Pseudomonas with 0.0196-0.0928 AUC. Finally, we established a random forest model aimed at forecasting the relative conjugation transfer rate of plasmids with 0.7956 AUC, drawing on data from existing literature. It identifies the plasmid's repression status, cellular density, and temperature as the most important factors influencing transfer frequency. With these two models combined, they provide useful reference for quick and low-cost integrated evaluation of resistance gene transfer, accelerating the process of computer-assisted quantitative risk assessment of ARGs transfer in environmental field.

13.
J Environ Manage ; 358: 120832, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38599089

RESUMO

Polyethylene (PE) is the most productive plastic product and includes three major polymers including high-density polyethylene (HDPE), linear low-density polyethylene (LLDPE) and low-density polyethylene (LDPE) variation in the PE depends on the branching of the polymer chain and its crystallinity. Tenebrio obscurus and Tenebrio molitor larvae biodegrade PE. We subsequently tested larval physiology, gut microbiome, oxidative stress, and PE degradation capability and degradation products under high-purity HDPE, LLDPE, and LDPE powders (<300 µm) diets for 21 days at 65 ± 5% humidity and 25 ± 0.5 °C. Our results demonstrated the specific PE consumption rates by T. molitor was 8.04-8.73 mg PE ∙ 100 larvae-1⋅day-1 and by T. obscurus was 7.68-9.31 for LDPE, LLDPE and HDPE, respectively. The larvae digested nearly 40% of the ingested three PE and showed similar survival rates and weight changes but their fat content decreased by 30-50% over 21-day period. All the PE-fed groups exhibited adverse effects, such as increased benzoquinone concentrations, intestinal tissue damage and elevated oxidative stress indicators, compared with bran-fed control. In the current study, the digestive tract or gut microbiome exhibited a high level of adaptability to PE exposure, altering the width of the gut microbial ecological niche and community diversity, revealing notable correlations between Tenebrio species and the physical and chemical properties (PCPs) of PE-MPs, with the gut microbiome and molecular weight change due to biodegradation. An ecotoxicological simulation by T.E.S.T. confirmed that PE degradation products were little ecotoxic to Daphnia magna and Rattus norvegicus providing important novel insights for future investigations into the environmentally-friendly approach of insect-mediated biodegradation of persistent plastics.


Assuntos
Biodegradação Ambiental , Larva , Microplásticos , Polietileno , Tenebrio , Animais , Tenebrio/metabolismo , Polietileno/metabolismo , Microplásticos/toxicidade , Microbioma Gastrointestinal/efeitos dos fármacos , Estresse Oxidativo
14.
Environ Res ; 252(Pt 1): 118810, 2024 Mar 28.
Artigo em Inglês | MEDLINE | ID: mdl-38552829

RESUMO

Nitrate/nitrite-dependent anaerobic methane oxidation (n-DAMO) process offers a promising solution for simultaneously achieving methane emissions reduction and efficient nitrogen removal in wastewater treatment. Although nitrogen removal at a practical rate has been achieved by n-DAMO biofilm process, the mechanisms of biofilm formation and nitrogen transformation remain to be elucidated. In this study, n-DAMO biofilms were successfully developed in the membrane aerated moving bed biofilm reactor (MAMBBR) and removed nitrate at a rate of 159 mg NO3--N L-1 d-1. The obvious increase in the content of extracellular polymeric substances (EPS) indicated that EPS production was important for biofilm development. n-DAMO microorganisms dominated the microbial community, and n-DAMO bacteria were the most abundant microorganisms. However, the expression of biosynthesis genes for proteins and polysaccharides encoded by n-DAMO archaea was significantly more active compared to other microorganisms, suggesting the central role of n-DAMO archaea in EPS production and biofilm formation. In addition to nitrate reduction, n-DAMO archaea were revealed to actively express dissimilatory nitrate reduction to ammonium and nitrogen fixation. The produced ammonium was putatively converted to dinitrogen gas through the joint function of n-DAMO archaea and n-DAMO bacteria. This study revealed the biofilm formation mechanism and nitrogen-transformation network in n-DAMO biofilm systems, shedding new light on promoting the application of n-DAMO process.

15.
Bioresour Technol ; 399: 130643, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38552855

RESUMO

This study proposed an efficient framework for optimizing the design and operation of combined systems of wastewater treatment plants (WWTP) and constructed wetlands (CW). The framework coupled a WWTP model with a CW model and used a multi-objective evolutionary algorithm to identify trade-offs between energy consumption, effluent quality, and construction cost. Compared to traditional design and management approaches, the framework achieved a 27 % reduction in WWTP energy consumption or a 44 % reduction in CW cost while meeting strict effluent discharge limits for Chinese WWTP. The framework also identified feasible decision variable ranges and demonstrated the impact of different optimization strategies on system performance. Furthermore, the contributions of WWTP and CW in pollutant degradation were analyzed. Overall, the proposed framework offers a highly efficient and cost-effective solution for optimizing the design and operation of a combined WWTP and CW system.


Assuntos
Eliminação de Resíduos Líquidos , Purificação da Água , Áreas Alagadas , Águas Residuárias , Aprendizado de Máquina
16.
Water Res ; 254: 121417, 2024 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-38461597

RESUMO

Single-atom catalysts (SACs) have emerged as competitive candidates for Fenton-like oxidation of micro-pollutants in water. However, the impact of metal insertion on the intrinsic catalytic activity of carrier materials has been commonly overlooked, and the environmental risk due to metal leaching still requires attention. In contrast to previous reports, where metal sites were conventionally considered as catalytic centers, our study investigates, for the first time, the crucial catalytic role of the carbon carrier modulated through hetero-single-atom dispersion and the regulation of Fenton-like oxidation pathways. The inherent differences in electronic properties between Fe and Co can effectively trigger long-range electron rearrangement in the sp2-carbon-conjugated structure, creating more electron-rich regions for peroxymonosulfate (PMS) complexation and initiating the electron transfer process (ETP) for pollutant degradation, which imparts the synthesized catalyst (FeCo-NCB) with exceptional catalytic efficiency despite its relatively low metal content. Moreover, the FeCo-NCB/PMS system exhibits enduring decontamination efficiency in complex water matrices, satisfactory catalytic stability, and low metal leaching, signifying promising practical applications. More impressively, the spatial relationship between metal sites and electron density clouds is revealed to determine whether high-valent metal-oxo species (HVMO) are involved during the decomposition of surface complexes. Unlike single-type single-atom dispersion, where metal sites are situated within electron-rich regions, hetero-single-atom dispersion can cause the deviation of electron density clouds from the metal sites, thus hindering the in-situ oxidation of metal within the complexes and minimizing the contribution of HVMO. These findings provide new insights into the development of carbon-based SACs and advance the understanding of nonradical mechanisms underpinning Fenton-like treatments.


Assuntos
Carbono , Poluentes Ambientais , Peróxidos , Oxirredução , Transporte de Elétrons , Eletrônica , Água
17.
Environ Sci Technol ; 58(11): 4844-4851, 2024 Mar 19.
Artigo em Inglês | MEDLINE | ID: mdl-38385614

RESUMO

This perspective presents the latest advancements in selective polymerization pathways in advanced oxidation processes (AOPs) for removal of featured organic pollutants in wastewater. In radical-based homogeneous reactions, SO4• --based systems exhibit superior oxidative activity toward aromatics with electron-donating substituents via single electron transfer and radical adduct formation (RAF). The produced organic radical cations subsequently undergo coupling and polymerization reactions to produce polymers. For •OH-based oxidation, metal ions facilitate the production of monomer radicals via RAF. Additionally, heterogeneous catalysts can mediate both coupling and polymerization reactions via persulfate activation without generating inorganic radicals. Metal-based catalysts will mediate a direct oxidation pathway toward polymerization. In contrast, carbon-based catalysts will induce coupling reactions to produce low-molecular-weight oligomers (≤4 units) via an electron transfer process. In comparison to mineralization, polymerization pathways remarkably reduce peroxide usage, quickly separate pollutants from the aqueous phase, and generate polymeric byproducts. Thus, AOP-driven polymerization systems hold significant promise in reducing carbon emission and realizing carbon recycling in water treatment processes.


Assuntos
Poluentes Químicos da Água , Oxirredução , Carbono , Águas Residuárias , Metais , Polímeros
18.
Bioresour Technol ; 396: 130383, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38316227

RESUMO

The addition of biochar resulted in a 31.5 % to 44.6 % increase in decolorization efficiency and favorable decolorization stability. Biochar promoted extracellular polymeric substances (EPS) secretion, especially humic-like and fulvic-like substances. Additionally, biochar enhanced the electron transfer capacity of anaerobic sludge and facilitated surface attachment of microbial cells. 16S rRNA gene sequencing analysis indicated that biochar reduced microbial species diversity, enriching fermentative bacteria such as Trichococcus. Finally, a machine learning model was employed to establish a predictive model for biochar characteristics and decolorization efficiency. Biochar electrical conductivity, H/C ratio, and O/C ratio had the most significant impact on RR2 anaerobic decolorization efficiency. According to the results, the possible mechanism of RR2 anaerobic decolorization enhanced by different types of biochar was proposed.


Assuntos
Compostos Azo , Carvão Vegetal , Corantes , Compostos Azo/metabolismo , Corantes/metabolismo , Anaerobiose , RNA Ribossômico 16S/genética , Esgotos
19.
J Colloid Interface Sci ; 662: 357-366, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38354562

RESUMO

The rational design of efficient photocatalysts to achieve artificial nitrogen fixation is an urgent challenge. Herein, we combined donor-acceptor covalent organic framework with iron-doped nitrogen vacancy graphitized carbon nitride (D-A COF/Fe-g-C3Nx) for photocatalytic nitrogen fixation. The photocatalyst exhibited good crystallinity, high porosity, and a large specific surface area. Without a sacrificial agent, the optimal 40 % D-A COF/Fe-g-C3Nx exhibited an excellent rate of ammonia production (646 µmol h-1 g-1) at 420 nm, and durable stability after successive cycling. Exhaustive experimental research and theory calculations verified that the D-A unit and Fe doping redistributed the distribution of the charge, which enhanced the visible light utilization and provided chemisorption sites for further polarization. Besides N-vacancies can serve as electron-trapping active sites to promote the directional migration of carriers. The reaction mechanism demonstrated that superoxide radical and hydrogen peroxide were formed by electron and hole, respectively, which promote the reduction of nitrogen to ammonia. This work provides a new idea for the rationalizing design of efficient catalysts for photocatalytic nitrogen fixation under mild conditions.

20.
Environ Sci Ecotechnol ; 20: 100374, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38283868

RESUMO

Microalgal-indigenous bacterial wastewater treatment (MBWT) emerges as a promising approach for the concurrent removal of nitrogen (N) and phosphorus (P). Despite its potential, the prevalent use of MBWT in batch systems limits its broader application. Furthermore, the success of MBWT critically depends on the stable self-adaptation and synergistic interactions between microalgae and indigenous bacteria, yet the underlying biological mechanisms are not fully understood. Here we explore the viability and microbial dynamics of a continuous flow microalgae-indigenous bacteria advanced wastewater treatment system (CFMBAWTS) in processing actual secondary effluent, with a focus on varying hydraulic retention times (HRTs). The research highlights a stable, mutually beneficial relationship between indigenous bacteria and microalgae. Microalgae and indigenous bacteria can create an optimal environment for each other by providing essential cofactors (like iron, vitamins, and indole-3-acetic acid), oxygen, dissolved organic matter, and tryptophan. This collaboration leads to effective microbial growth, enhanced N and P removal, and energy generation. The study also uncovers crucial metabolic pathways, functional genes, and patterns of microbial succession. Significantly, the effluent NH4+-N and P levels complied with the Chinese national Class-II, Class-V, Class-IA, and Class-IB wastewater discharge standards when the HRT was reduced from 15 to 6 h. Optimal results, including the highest rates of CO2 fixation (1.23 g L-1), total energy yield (32.35 kJ L-1), and the maximal lipid (33.91%) and carbohydrate (41.91%) content, were observed at an HRT of 15 h. Overall, this study not only confirms the feasibility of CFMBAWTS but also lays a crucial foundation for enhancing our understanding of this technology and propelling its practical application in wastewater treatment plants.

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