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Balancing catalyst-intermediate interactions: Unlocking high-performance MXene-supported catalysts for two-electron water oxidation reaction from single atoms to nanoparticles
IF 7.7 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2025-02-21 DOI: 10.1016/j.envres.2025.121207
Jiangtao Wei , Pengyang Ye , Yaqian Zhang, Jiayu Zheng, Qinglan Hao, Weiyi Zhang, Haihong Bao, Botao Teng
Two-electron water oxidation reaction (2e-WOR) provides an eco-friendly and cost-efficient approach to H2O2 synthesis. ZnO-based catalysts exhibit outstanding H2O2 activity and selectivity. Exploring the relationship between the structure of different zinc-based catalysts and their 2e-WOR performance is crucial for the rational design and development of high-performance catalysts. In this work, MXene (Ti3C2Tx) nanosheets were employed as supports to prepare zinc single atoms, ZnO nanoclusters and nanoparticles on MXene. Structural characterization, electrocatalytic evaluation, and density functional theory (DFT) calculations revealed distinct differences in catalyst performance. Zn-SA/MXene and ZnO-NC/MXene exhibit strong interactions with OH radicals, resulting in adsorption energies that greatly exceed the optimal range of −2.4∼−1.6 eV. This excessive interaction hinders efficient hydrogen peroxide production. In contrast, ZnO-NP/MXene achieves a balanced interaction with OH, with adsorption energy approaching the optimal range, leading to superior 2e-WOR activity. These findings highlight the critical role of tuning the interaction strength between active sites and OH radicals to achieve optimal catalytic performance. This work offers valuable theoretical insights and experimental validation for designing high-performance 2e-WOR catalysts, demonstrating that neither excessively strong nor weak interactions are conducive to maximizing efficiency.
{"title":"Balancing catalyst-intermediate interactions: Unlocking high-performance MXene-supported catalysts for two-electron water oxidation reaction from single atoms to nanoparticles","authors":"Jiangtao Wei ,&nbsp;Pengyang Ye ,&nbsp;Yaqian Zhang,&nbsp;Jiayu Zheng,&nbsp;Qinglan Hao,&nbsp;Weiyi Zhang,&nbsp;Haihong Bao,&nbsp;Botao Teng","doi":"10.1016/j.envres.2025.121207","DOIUrl":"10.1016/j.envres.2025.121207","url":null,"abstract":"<div><div>Two-electron water oxidation reaction (2e-WOR) provides an eco-friendly and cost-efficient approach to H<sub>2</sub>O<sub>2</sub> synthesis. ZnO-based catalysts exhibit outstanding H<sub>2</sub>O<sub>2</sub> activity and selectivity. Exploring the relationship between the structure of different zinc-based catalysts and their 2e-WOR performance is crucial for the rational design and development of high-performance catalysts. In this work, MXene (Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>) nanosheets were employed as supports to prepare zinc single atoms, ZnO nanoclusters and nanoparticles on MXene. Structural characterization, electrocatalytic evaluation, and density functional theory (DFT) calculations revealed distinct differences in catalyst performance. Zn-SA/MXene and ZnO-NC/MXene exhibit strong interactions with OH radicals, resulting in adsorption energies that greatly exceed the optimal range of −2.4∼−1.6 eV. This excessive interaction hinders efficient hydrogen peroxide production. In contrast, ZnO-NP/MXene achieves a balanced interaction with OH, with adsorption energy approaching the optimal range, leading to superior 2e-WOR activity. These findings highlight the critical role of tuning the interaction strength between active sites and OH radicals to achieve optimal catalytic performance. This work offers valuable theoretical insights and experimental validation for designing high-performance 2e-WOR catalysts, demonstrating that neither excessively strong nor weak interactions are conducive to maximizing efficiency.</div></div>","PeriodicalId":312,"journal":{"name":"Environmental Research","volume":"272 ","pages":"Article 121207"},"PeriodicalIF":7.7,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143479578","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Hierarchical Cu-doped MoS2 microspheres with efficient visible-light-driven peroxymonosulfate activation for micropollutant degradation: Nanostructure engineering and reaction mechanism
IF 7.7 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2025-02-21 DOI: 10.1016/j.envres.2025.121205
Bao Pan , Ge Jin , Wen Chen , Jiani Qin , Fei Li , Chuanyi Wang
Transition metal doping and nanostructure engineering are effective strategies to overcome the limitations of photocatalysts in peroxomonosulfate (PMS) activation. In this study, Cu-doped MoS2 with a hierarchical microspheric architecture was synthesized via a one-step hydrothermal method and employed for tetracycline (TC) degradation through PMS activation. Under visible light irradiation, the Cu0.06-MoS2 catalyst achieved an 86.2% TC removal efficiency within 40 min, which was 2.3 times higher than that of pristine MoS2. The effects of various operation parameters, including initial PMS concentration, reaction temperature, solution pH, and coexisting inorganic anions on the TC degradation efficiency were thoroughly investigated. Characterization results and theoretical calculations demonstrated that the redox cycles of Cu2+/Cu+ and Mo6+/Mo4+, as well as the 3D microspheric structure of Cu0.06-MoS2, support its ultra-high charge transfer capability and abundant exposure of active sites, thereby promoting efficient photocatalytic activation of PMS for TC degradation. Reactive species quenching experiments and EPR analysis revealed that ·O2, •OH, and SO4•− are the primary reactive oxygen species involved in TC degradation. This study provides a promising direction for the development of highly efficient micropollutant degradation utilizing transition metals-modified sulfide photocatalysts with a 3D architecture.
{"title":"Hierarchical Cu-doped MoS2 microspheres with efficient visible-light-driven peroxymonosulfate activation for micropollutant degradation: Nanostructure engineering and reaction mechanism","authors":"Bao Pan ,&nbsp;Ge Jin ,&nbsp;Wen Chen ,&nbsp;Jiani Qin ,&nbsp;Fei Li ,&nbsp;Chuanyi Wang","doi":"10.1016/j.envres.2025.121205","DOIUrl":"10.1016/j.envres.2025.121205","url":null,"abstract":"<div><div>Transition metal doping and nanostructure engineering are effective strategies to overcome the limitations of photocatalysts in peroxomonosulfate (PMS) activation. In this study, Cu-doped MoS<sub>2</sub> with a hierarchical microspheric architecture was synthesized via a one-step hydrothermal method and employed for tetracycline (TC) degradation through PMS activation. Under visible light irradiation, the Cu<sub>0.06</sub>-MoS<sub>2</sub> catalyst achieved an 86.2% TC removal efficiency within 40 min, which was 2.3 times higher than that of pristine MoS<sub>2</sub>. The effects of various operation parameters, including initial PMS concentration, reaction temperature, solution pH, and coexisting inorganic anions on the TC degradation efficiency were thoroughly investigated. Characterization results and theoretical calculations demonstrated that the redox cycles of Cu<sup>2+</sup>/Cu<sup>+</sup> and Mo<sup>6+</sup>/Mo<sup>4+</sup>, as well as the 3D microspheric structure of Cu<sub>0.06</sub>-MoS<sub>2</sub>, support its ultra-high charge transfer capability and abundant exposure of active sites, thereby promoting efficient photocatalytic activation of PMS for TC degradation. Reactive species quenching experiments and EPR analysis revealed that ·O<sub>2</sub><sup>−</sup>, •OH, and SO<sub>4</sub><sup>•−</sup> are the primary reactive oxygen species involved in TC degradation. This study provides a promising direction for the development of highly efficient micropollutant degradation utilizing transition metals-modified sulfide photocatalysts with a 3D architecture.</div></div>","PeriodicalId":312,"journal":{"name":"Environmental Research","volume":"272 ","pages":"Article 121205"},"PeriodicalIF":7.7,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143479577","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Effects of neonicotinoid pesticide exposure in the first trimester on gestational diabetes mellitus based on interpretable machine learning
IF 7.7 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2025-02-20 DOI: 10.1016/j.envres.2025.121168
Dongxiang Pan , Lihong Zhou , Changhui Mu , Mengrui Lin , Yonghong Sheng , Yang Xu , Dongping Huang , Shun Liu , Xiaoyun Zeng , Virasakdi Chongsuvivatwong , Xiaoqiang Qiu

Background

Gestational diabetes mellitus (GDM) is one of the most common pregnancy complications and seriously threatens the health of mothers and offspring. Neonicotinoids (NEOs) is a new class of pesticide and widely used worldwide. Prenatal NEOs exposure had negative effects on fetal growth, but the potential effect of NEOs exposure on pregnancy complications remain unclear.

Objectives

To examine the individual and jointed effects of serum neonicotinoids (NEOs) pesticide exposure on gestational diabetes mellitus (GDM), and explore the application of NEOs exposure levels as predictor of GDM.

Methods

We conducted a prospective cohort study based on Guangxi Zhuang Birth Cohort, China. A total of 1450 mather-infant pairs were included from 2015 to 2019. Ten NEOs were measured by UPLC-MS. Maternal serum samples were collected during gestational age 0–12 weeks. Individual and jointed effects of NEOs on GDM were assessed through binomial regressions, Bayesian Kernel Machine Regression and quantile g-computation. Prediction of GDM using XGboost machine learning and SHapley Additive exPlanations (SHAP).

Results

A total of 122 (8.4%) mothers were diagnosed with GDM. In the individual exposure models, sulfoxaflor and thiamethoxam exposure in the first trimester significantly increased the risk of GDM (OR = 1.48, 95%CI: 1.21, 1.82; OR = 1.42, 95%CI: 1.14, 1.78). Moreover, GDM risk increased significantly with NEOs mixture concentration was above 75th percentile, compared with the 50th percentile. Sulfoxaflor and thiamethoxam as the main positive contributing factors in NEOs mixture to increase the GDM with a weight of 29.3% and 27.6%, respectively. Furthermore, sulfoxaflor and thiamethoxam were the most important contributing factors for predicting GDM after combining traditional risk factors in machine learning model, with predicted contribution values of 0.79 and 0.46, respectively.

Conclusion

Our findings suggested that elevated maternal serum sulfoxaflor, thiamethoxam and NEOs mixture were positively associated with GDM, and sulfoxaflor, thiamethoxam were the important contributing factors for predicting GDM.
{"title":"Effects of neonicotinoid pesticide exposure in the first trimester on gestational diabetes mellitus based on interpretable machine learning","authors":"Dongxiang Pan ,&nbsp;Lihong Zhou ,&nbsp;Changhui Mu ,&nbsp;Mengrui Lin ,&nbsp;Yonghong Sheng ,&nbsp;Yang Xu ,&nbsp;Dongping Huang ,&nbsp;Shun Liu ,&nbsp;Xiaoyun Zeng ,&nbsp;Virasakdi Chongsuvivatwong ,&nbsp;Xiaoqiang Qiu","doi":"10.1016/j.envres.2025.121168","DOIUrl":"10.1016/j.envres.2025.121168","url":null,"abstract":"<div><h3>Background</h3><div>Gestational diabetes mellitus (GDM) is one of the most common pregnancy complications and seriously threatens the health of mothers and offspring. Neonicotinoids (NEOs) is a new class of pesticide and widely used worldwide. Prenatal NEOs exposure had negative effects on fetal growth, but the potential effect of NEOs exposure on pregnancy complications remain unclear.</div></div><div><h3>Objectives</h3><div>To examine the individual and jointed effects of serum neonicotinoids (NEOs) pesticide exposure on gestational diabetes mellitus (GDM), and explore the application of NEOs exposure levels as predictor of GDM.</div></div><div><h3>Methods</h3><div>We conducted a prospective cohort study based on Guangxi Zhuang Birth Cohort, China. A total of 1450 mather-infant pairs were included from 2015 to 2019. Ten NEOs were measured by UPLC-MS. Maternal serum samples were collected during gestational age 0–12 weeks. Individual and jointed effects of NEOs on GDM were assessed through binomial regressions, Bayesian Kernel Machine Regression and quantile g-computation. Prediction of GDM using XGboost machine learning and SHapley Additive exPlanations (SHAP).</div></div><div><h3>Results</h3><div>A total of 122 (8.4%) mothers were diagnosed with GDM. In the individual exposure models, sulfoxaflor and thiamethoxam exposure in the first trimester significantly increased the risk of GDM (OR = 1.48, 95%CI: 1.21, 1.82; OR = 1.42, 95%CI: 1.14, 1.78). Moreover, GDM risk increased significantly with NEOs mixture concentration was above 75th percentile, compared with the 50th percentile. Sulfoxaflor and thiamethoxam as the main positive contributing factors in NEOs mixture to increase the GDM with a weight of 29.3% and 27.6%, respectively. Furthermore, sulfoxaflor and thiamethoxam were the most important contributing factors for predicting GDM after combining traditional risk factors in machine learning model, with predicted contribution values of 0.79 and 0.46, respectively.</div></div><div><h3>Conclusion</h3><div>Our findings suggested that elevated maternal serum sulfoxaflor, thiamethoxam and NEOs mixture were positively associated with GDM, and sulfoxaflor, thiamethoxam were the important contributing factors for predicting GDM.</div></div>","PeriodicalId":312,"journal":{"name":"Environmental Research","volume":"273 ","pages":"Article 121168"},"PeriodicalIF":7.7,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143475974","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Windows of Susceptibility to Air Pollution During and Surrounding Pregnancy in Relation to Longitudinal Maternal Measures of Adiposity and Lipid Profiles.
IF 7.7 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2025-02-20 DOI: 10.1016/j.envres.2025.121198
Sandra India Aldana, Danielle Demateis, Damaskini Valvi, Allan C Just, Iván Gutiérrez-Avila, Guadalupe Estrada-Gutierrez, Martha María Téllez Rojo, Robert O Wright, Andrea A Baccarelli, Haotian Wu, Kayleigh P Keller, Ander Wilson, Elena Colicino

Pregnancy is a critical window for long-term metabolic programming of fetal effects stemming from airborne particulate matter ≤2.5μm (PM2.5) exposure. Yet, little is known about long-term metabolic effects of PM2.5 exposure during and surrounding pregnancy in mothers. We assessed potential critical windows of PM2.5 exposure during and surrounding pregnancy with maternal adiposity and lipid measures later in life. We included 517 pregnant women from the PROGRESS cohort with adiposity [body mass index (BMI), waist circumference (WC), % body fat] and lipids [total cholesterol, high-density-lipoprotein (HDL), low-density-lipoprotein (LDL)] measured repeatedly at 4, 6 and 8 years post-delivery. Monthly average PM2.5 exposure was estimated at each participant's address using a validated spatiotemporal model. We employed distributed lag interaction models (DLIMs) adjusting for socio-demographics and clinical covariates. We found that a 1 μg/m3 increase in PM2.5 exposure throughout mid-/late-pregnancy was associated with higher WC at 6-years post-delivery, peaking at 6 months of gestation: 0.04 cm (95%CI: 0.01, 0.06). We also identified critical windows of PM2.5 exposure during and surrounding pregnancy associated with higher LDL and lower HDL both measured at 4 years post-delivery with peaks at pre-conception for LDL [0.17 mg/dL (95%CI: 0.00, 0.34)] and at the 11th month after conception for HDL [-0.07 mg/dL (95%CI: -0.11, -0.02)]. Stratified analyses by fetal sex indicated stronger associations with adiposity measures in mothers carrying a male, while with lipids in mothers carrying a female fetus. Stratified analyses also indicated potential stronger deleterious lagged effects in women with folic acid intake lower than 600mcg/day during pregnancy.

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引用次数: 0
Enhancing methane production in anaerobic digestion via improved electron transfer with dual-reaction-centers catalyst
IF 7.7 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2025-02-20 DOI: 10.1016/j.envres.2025.121190
Congfeng Xu , Wenrui Cao , Fangxing Guo , Chun Hu , Lai Lyu
The recovery of methane from waste-activated sludge and rice straw often encounters challenges due to inefficient electron transfer between microorganisms. To break through this bottleneck, a novel and effective strategy is urgently needed. Here, we propose adding dual reaction centers (DRCs) catalyst with electron-rich and electron-poor microregions into the anaerobic digestion (AD) system. Pigeon manure was transformed into a novel DRCs catalyst, Fe-PMC, through pyrolysis and doping. Our findings indicate that the micro-electric field on the surface of Fe-PMC effectively aggregated humic acid-like substances and increased sludge conductivity. Compared to the control group (0 mg/L), adding trace amounts of Fe-PMC (40 mg/L) significantly increased methane production by 27.45%. High-throughput sequencing analyses revealed that Fe-PMC enhanced the relative abundance of functional microorganisms, such as Geobacter (23.62%) and Methanobacterium (35.53%), thereby promoting methanogenic co-metabolism. Furthermore, functional genes associated with carbon dioxide reduction to methane and direct interspecific electron transfer were upregulated by 3.41%–297.66%. This study provides a valuable reference for recovering renewable energy from waste using DRCs catalysts.
{"title":"Enhancing methane production in anaerobic digestion via improved electron transfer with dual-reaction-centers catalyst","authors":"Congfeng Xu ,&nbsp;Wenrui Cao ,&nbsp;Fangxing Guo ,&nbsp;Chun Hu ,&nbsp;Lai Lyu","doi":"10.1016/j.envres.2025.121190","DOIUrl":"10.1016/j.envres.2025.121190","url":null,"abstract":"<div><div>The recovery of methane from waste-activated sludge and rice straw often encounters challenges due to inefficient electron transfer between microorganisms. To break through this bottleneck, a novel and effective strategy is urgently needed. Here, we propose adding dual reaction centers (DRCs) catalyst with electron-rich and electron-poor microregions into the anaerobic digestion (AD) system. Pigeon manure was transformed into a novel DRCs catalyst, Fe-PMC, through pyrolysis and doping. Our findings indicate that the micro-electric field on the surface of Fe-PMC effectively aggregated humic acid-like substances and increased sludge conductivity. Compared to the control group (0 mg/L), adding trace amounts of Fe-PMC (40 mg/L) significantly increased methane production by 27.45%. High-throughput sequencing analyses revealed that Fe-PMC enhanced the relative abundance of functional microorganisms, such as <em>Geobacter</em> (23.62%) and <em>Methanobacterium</em> (35.53%), thereby promoting methanogenic co-metabolism. Furthermore, functional genes associated with carbon dioxide reduction to methane and direct interspecific electron transfer were upregulated by 3.41%–297.66%. This study provides a valuable reference for recovering renewable energy from waste using DRCs catalysts.</div></div>","PeriodicalId":312,"journal":{"name":"Environmental Research","volume":"272 ","pages":"Article 121190"},"PeriodicalIF":7.7,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143472024","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Selective removal of cesium ions from aqueous solution by different metal (Zn2+/Ni2+) hexacyanocobaltate
IF 7.7 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2025-02-20 DOI: 10.1016/j.envres.2025.121192
Kang Li , Yisa Liu , Jiong Dong , Lili Xu , Chenxi Li , Ruixin Ma , Shina Li
Radioactive 137Cs removal and treatment have attracted widespread attention since the Chernobyl disaster and the Fukushima Daiichi nuclear plant accident. So far, Prussian blue analogs (PBAs) are recognized as the most effective Cs+ adsorbents possessing excellent sorption ability and radiation resistance. Here, two types of PBA-based Cs+ adsorbents, potassium zinc hexacyanocobaltate (Zn-Co PBA) and potassium nickel hexacyanocobaltate (Ni-Co PBA), were prepared by chemical precipitation method. Consequently, Zn-Co PBA and Ni-Co PBA had fast adsorption kinetics, and could remove 86.12% and 91.49% of Cs+ within 5 min, respectively. Zn-Co PBA and Ni-Co PBA were stable in a wide pH range, with Qmax of 96.53 and 77.52 mg/g for Cs+, respectively, both removing 98.5% of Cs+. In addition, Zn-Co PBA can eliminate 93.79% of Cs+ even in Cs+ spiked seawater containing high concentration of competitive cations. The adsorption mechanism indicates that the primary process involves ion exchange between K+ in the adsorbent and Cs+.
{"title":"Selective removal of cesium ions from aqueous solution by different metal (Zn2+/Ni2+) hexacyanocobaltate","authors":"Kang Li ,&nbsp;Yisa Liu ,&nbsp;Jiong Dong ,&nbsp;Lili Xu ,&nbsp;Chenxi Li ,&nbsp;Ruixin Ma ,&nbsp;Shina Li","doi":"10.1016/j.envres.2025.121192","DOIUrl":"10.1016/j.envres.2025.121192","url":null,"abstract":"<div><div>Radioactive <sup>137</sup>Cs removal and treatment have attracted widespread attention since the Chernobyl disaster and the Fukushima Daiichi nuclear plant accident. So far, Prussian blue analogs (PBAs) are recognized as the most effective Cs<sup>+</sup> adsorbents possessing excellent sorption ability and radiation resistance. Here, two types of PBA-based Cs<sup>+</sup> adsorbents, potassium zinc hexacyanocobaltate (Zn-Co PBA) and potassium nickel hexacyanocobaltate (Ni-Co PBA), were prepared by chemical precipitation method. Consequently, Zn-Co PBA and Ni-Co PBA had fast adsorption kinetics, and could remove 86.12% and 91.49% of Cs<sup>+</sup> within 5 min, respectively. Zn-Co PBA and Ni-Co PBA were stable in a wide pH range, with <em>Q</em><sub>max</sub> of 96.53 and 77.52 mg/g for Cs<sup>+</sup>, respectively, both removing 98.5% of Cs<sup>+</sup>. In addition, Zn-Co PBA can eliminate 93.79% of Cs<sup>+</sup> even in Cs<sup>+</sup> spiked seawater containing high concentration of competitive cations. The adsorption mechanism indicates that the primary process involves ion exchange between K<sup>+</sup> in the adsorbent and Cs<sup>+</sup>.</div></div>","PeriodicalId":312,"journal":{"name":"Environmental Research","volume":"272 ","pages":"Article 121192"},"PeriodicalIF":7.7,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143471147","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Biochar-amended constructed wetlands enhance sulfadiazine removal and reduce resistance genes accumulation in treatment of mariculture wastewater
IF 7.7 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2025-02-20 DOI: 10.1016/j.envres.2025.121161
Yuan-yuan Gao , Yu-xin Wu , Wang-chao Chu , Li Lai , Jia-hao Sun , Lin-lan Zhuang , Fei-fei Liu
With the rapid development of mariculture, an increasing amount of antibiotics are being discharged into the marine environment. Effectively removing antibiotics and antibiotic resistance genes (ARGs) in mariculture wastewater with a relatively high salinity and low C/N presents challenges. Biochar-amended constructed wetlands (CWs) can effectively remove antibiotics, However, few studies have compared the impacts of biochar-amended CWs pyrolyzed at different temperatures on the treatment of mariculture wastewater. Thus, this study utilized biochar prepared at three temperatures as substrate for CWs (CW-300, CW-500, and CW-700), aiming to evaluate their efficiency to treat mariculture wastewater containing antibiotic sulfadiazine (SDZ). The results demonstrated that compared to traditional quartz sand-filled CW (NCW), the addition of biochar with a larger specific surface area significantly enhanced the removal efficiency of SDZ by 21.72%–46.96%. Additionally, the addition of biochar effectively reduced the relative abundance of one integron gene (int1) and antibiotic resistance genes (ARGs) including sul1, sul2, and sul3 in both effluent and substrates. The addition of biochar reduced the accumulation of extracellular polymeric substances within the substrate of CWs, thereby mitigating the proliferation and spread of ARGs. The microbial community structure indicated that the addition of biochar increased the abundance of the potential antibiotic-degrading bacteria such as Proteobacteria and Bacteroidota, facilitating the degradation of SDZ and mitigating the accumulation of ARGs. This study demonstrated that biochar can be a promising substrate in CWs for treating mariculture wastewater containing antibiotics.
{"title":"Biochar-amended constructed wetlands enhance sulfadiazine removal and reduce resistance genes accumulation in treatment of mariculture wastewater","authors":"Yuan-yuan Gao ,&nbsp;Yu-xin Wu ,&nbsp;Wang-chao Chu ,&nbsp;Li Lai ,&nbsp;Jia-hao Sun ,&nbsp;Lin-lan Zhuang ,&nbsp;Fei-fei Liu","doi":"10.1016/j.envres.2025.121161","DOIUrl":"10.1016/j.envres.2025.121161","url":null,"abstract":"<div><div>With the rapid development of mariculture, an increasing amount of antibiotics are being discharged into the marine environment. Effectively removing antibiotics and antibiotic resistance genes (ARGs) in mariculture wastewater with a relatively high salinity and low C/N presents challenges. Biochar-amended constructed wetlands (CWs) can effectively remove antibiotics, However, few studies have compared the impacts of biochar-amended CWs pyrolyzed at different temperatures on the treatment of mariculture wastewater. Thus, this study utilized biochar prepared at three temperatures as substrate for CWs (CW-300, CW-500, and CW-700), aiming to evaluate their efficiency to treat mariculture wastewater containing antibiotic sulfadiazine (SDZ). The results demonstrated that compared to traditional quartz sand-filled CW (NCW), the addition of biochar with a larger specific surface area significantly enhanced the removal efficiency of SDZ by 21.72%–46.96%. Additionally, the addition of biochar effectively reduced the relative abundance of one integron gene (<em>int1</em>) and antibiotic resistance genes (ARGs) including <em>sul1</em>, <em>sul2</em>, and <em>sul3</em> in both effluent and substrates. The addition of biochar reduced the accumulation of extracellular polymeric substances within the substrate of CWs, thereby mitigating the proliferation and spread of ARGs. The microbial community structure indicated that the addition of biochar increased the abundance of the potential antibiotic-degrading bacteria such as <em>Proteobacteria</em> and <em>Bacteroidota</em>, facilitating the degradation of SDZ and mitigating the accumulation of ARGs. This study demonstrated that biochar can be a promising substrate in CWs for treating mariculture wastewater containing antibiotics.</div></div>","PeriodicalId":312,"journal":{"name":"Environmental Research","volume":"273 ","pages":"Article 121161"},"PeriodicalIF":7.7,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143475968","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Catalytic ozonation of sulfamethoxazole using loaded CuOx/MgO-SiO2 silica aerogel catalyst: Performance, mechanisms and toxicity
IF 7.7 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2025-02-20 DOI: 10.1016/j.envres.2025.121155
Lanhe Zhang , Jiaming Wu , Jian Zhang , Jingbo Guo
Catalytic ozonation technology can quickly and inexpensively treat antibiotic wastewater, where the performance of catalysts determines the level of catalytic efficiency. In this study, CuOx/MgO-SiO2 (represented by CuMgSiO) catalysts were prepared using hydrothermal method. Their structure and properties were analyzed by X-ray diffractometer (XRD), X-ray photoelectron spectroscopy (XPS) and automatic specific surface area analyzer. The effects of O3 concentration, catalyst dosage and initial pH on the degradation of Sulfamethoxazole (SMX) were investigated. Catalytic ozonation mechanisms and degradation pathways of the pollutants were revealed by quenching experiments and liquid chromatography-mass spectrometry analysis. The toxicity of SMX and its intermediates was analyzed by ECOSAR software. The results showed that CuOx/MgO was successfully loaded onto SiO2 aerogel and the catalyst exhibited a porous network structure. The highest removal efficiency of SMX reached 87.92% and Kobs was 0.07045 min−1 under the optimum conditions, which was 35.9% and 2.77 times higher than those of ozonation alone. The ·OH, ·O2 and 1O2 were active species for the degradation of SMX, and 1O2 played a dominant role. Valence cycling between Cu2+/Cu+ and Mg2+/Mg and adsorption of O3 by surface hydroxyl groups were key steps in catalytic ozonation, and the toxicity of wastewater after treatment was greatly reduced. This study not only provides an economically feasible catalyst, but also offers a new perspective in the field of antibiotic wastewater treatment.
{"title":"Catalytic ozonation of sulfamethoxazole using loaded CuOx/MgO-SiO2 silica aerogel catalyst: Performance, mechanisms and toxicity","authors":"Lanhe Zhang ,&nbsp;Jiaming Wu ,&nbsp;Jian Zhang ,&nbsp;Jingbo Guo","doi":"10.1016/j.envres.2025.121155","DOIUrl":"10.1016/j.envres.2025.121155","url":null,"abstract":"<div><div>Catalytic ozonation technology can quickly and inexpensively treat antibiotic wastewater, where the performance of catalysts determines the level of catalytic efficiency. In this study, CuO<sub>x</sub>/MgO-SiO<sub>2</sub> (represented by CuMgSiO) catalysts were prepared using hydrothermal method. Their structure and properties were analyzed by X-ray diffractometer (XRD), X-ray photoelectron spectroscopy (XPS) and automatic specific surface area analyzer. The effects of O<sub>3</sub> concentration, catalyst dosage and initial pH on the degradation of Sulfamethoxazole (SMX) were investigated. Catalytic ozonation mechanisms and degradation pathways of the pollutants were revealed by quenching experiments and liquid chromatography-mass spectrometry analysis. The toxicity of SMX and its intermediates was analyzed by ECOSAR software. The results showed that CuO<sub>x</sub>/MgO was successfully loaded onto SiO<sub>2</sub> aerogel and the catalyst exhibited a porous network structure. The highest removal efficiency of SMX reached 87.92% and K<sub>obs</sub> was 0.07045 min<sup>−1</sup> under the optimum conditions, which was 35.9% and 2.77 times higher than those of ozonation alone. The ·OH, ·O<sub>2</sub><sup>−</sup> and <sup>1</sup>O<sub>2</sub> were active species for the degradation of SMX, and <sup>1</sup>O<sub>2</sub> played a dominant role. Valence cycling between Cu<sup>2+</sup>/Cu<sup>+</sup> and Mg<sup>2+</sup>/Mg and adsorption of O<sub>3</sub> by surface hydroxyl groups were key steps in catalytic ozonation, and the toxicity of wastewater after treatment was greatly reduced. This study not only provides an economically feasible catalyst, but also offers a new perspective in the field of antibiotic wastewater treatment.</div></div>","PeriodicalId":312,"journal":{"name":"Environmental Research","volume":"272 ","pages":"Article 121155"},"PeriodicalIF":7.7,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143475970","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Seawater nanoarchitectonics for an eco-friendly dual-function activator-catalyst producing graphene-decorated activated biochar for applications in electrochemical energy storage 海水纳米结构用于生态友好型双功能活化剂-催化剂,产生石墨烯装饰的活化生物炭,应用于电化学储能。
IF 7.7 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2025-02-20 DOI: 10.1016/j.envres.2025.121176
Authit Phakkhawan , Suppanat Kosolwattana , Morakot Sakulsombat , Samuk Pimanpang , Pawinee Klangtakai , Vittaya Amornkitbamrung
Activated biochar (AB) powder derived from sawdust was prepared using 0.6 M NaCl as a dual-function activator-catalyst at temperatures ranging from 500 to 1000 °C. The AB synthesized at 900 °C (NaCl-AB-900) shows the highest specific surface area (880.05 m2 g−1). Seawater was then used as the dual activator-catalyst to explore sustainable alternatives, producing Seawater-AB-900 powder with a specific surface area similar to the NaCl-AB-900 powder (890.34 m2 g−1). In contrast, the non-activated biochar (Non-AB-900, 782.45 m2 g−1) has a smaller specific surface area than both AB powders. SEM and TEM analyses reveal that both AB powders have graphene decoration and porosity, whereas the Non-AB-900 powder only exhibits porosity. Electrodes made from NaCl-AB-900 and Seawater-AB-900 powders demonstrate higher specific capacitances (81.42 and 84.45 F g−1) compared to Non-AB-900 (64.39 F g−1) at 0.3 A g−1 in a three-electrode system using 6 M KOH. They also exhibit better rate capability (76.54% and 70.44%) than Non-AB-900 (65.24%). In a two-electrode mode, NaCl-AB-900 and Seawater-AB-900 supercapacitors outperform Non-AB-900 in capacitance (51.76 F g−1, 50.68 F g−1 vs. 25.96 F g−1 at 0.3 A g−1) and rate capability (64.50%, 65.20% vs. 27.59% at 10 A g−1). In a Zn-ion battery system, NaCl-AB-900 (137.07 mAh g−1) and Seawater-AB-900 (142.29 mAh g−1) deliver higher specific capacities than Non-AB-900 (69.03 mAh g−1) at 0.3 A g−1. Both AB electrodes show excellent cycle stability, with over 70% retention after 40000 supercapacitor cycles and 90% after 7000 battery cycles. The Seawater-AB-900-powered supercapacitors and batteries successfully lit an LED for over 2 min.
{"title":"Seawater nanoarchitectonics for an eco-friendly dual-function activator-catalyst producing graphene-decorated activated biochar for applications in electrochemical energy storage","authors":"Authit Phakkhawan ,&nbsp;Suppanat Kosolwattana ,&nbsp;Morakot Sakulsombat ,&nbsp;Samuk Pimanpang ,&nbsp;Pawinee Klangtakai ,&nbsp;Vittaya Amornkitbamrung","doi":"10.1016/j.envres.2025.121176","DOIUrl":"10.1016/j.envres.2025.121176","url":null,"abstract":"<div><div>Activated biochar (AB) powder derived from sawdust was prepared using 0.6 M NaCl as a dual-function activator-catalyst at temperatures ranging from 500 to 1000 °C. The AB synthesized at 900 °C (NaCl-AB-900) shows the highest specific surface area (880.05 m<sup>2</sup> g<sup>−1</sup>). Seawater was then used as the dual activator-catalyst to explore sustainable alternatives, producing Seawater-AB-900 powder with a specific surface area similar to the NaCl-AB-900 powder (890.34 m<sup>2</sup> g<sup>−1</sup>). In contrast, the non-activated biochar (Non-AB-900, 782.45 m<sup>2</sup> g<sup>−1</sup>) has a smaller specific surface area than both AB powders. SEM and TEM analyses reveal that both AB powders have graphene decoration and porosity, whereas the Non-AB-900 powder only exhibits porosity. Electrodes made from NaCl-AB-900 and Seawater-AB-900 powders demonstrate higher specific capacitances (81.42 and 84.45 F g<sup>−1</sup>) compared to Non-AB-900 (64.39 F g<sup>−1</sup>) at 0.3 A g<sup>−1</sup> in a three-electrode system using 6 M KOH. They also exhibit better rate capability (76.54% and 70.44%) than Non-AB-900 (65.24%). In a two-electrode mode, NaCl-AB-900 and Seawater-AB-900 supercapacitors outperform Non-AB-900 in capacitance (51.76 F g<sup>−1</sup>, 50.68 F g<sup>−1</sup> vs. 25.96 F g<sup>−1</sup> at 0.3 A g<sup>−1</sup>) and rate capability (64.50%, 65.20% vs. 27.59% at 10 A g<sup>−1</sup>). In a Zn-ion battery system, NaCl-AB-900 (137.07 mAh g<sup>−1</sup>) and Seawater-AB-900 (142.29 mAh g<sup>−1</sup>) deliver higher specific capacities than Non-AB-900 (69.03 mAh g<sup>−1</sup>) at 0.3 A g<sup>−1</sup>. Both AB electrodes show excellent cycle stability, with over 70% retention after 40000 supercapacitor cycles and 90% after 7000 battery cycles. The Seawater-AB-900-powered supercapacitors and batteries successfully lit an LED for over 2 min.</div></div>","PeriodicalId":312,"journal":{"name":"Environmental Research","volume":"272 ","pages":"Article 121176"},"PeriodicalIF":7.7,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143475989","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Simultaneously ammonium and perchlorate remove via the partial nitrification-anammox coupled sulfur autotrophic system
IF 7.7 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2025-02-20 DOI: 10.1016/j.envres.2025.121195
Guiying Zhang , Jingmei Liu , Yi Han , Liang Xia , Jianbing Zhang , Jianbo Guo , Haibo Li , Yanan Hou , Yuanyuan Song
In this study, partial nitrification-anammox coupled sulfur autotrophic (PNA-SA) system was constructed for removing ammonium and perchlorate from composite wastewater simultaneously. The removal rates of ammonium and perchlorate could reach 94.2% and 93.1%, respectively, at an ammonium concentration of 60 mg N∙L−1 and a perchlorate concentration of 30 mg N∙L−1. Ammonium was mainly removed by anammox bacteria (AnAOB) in PNA reactor, while perchlorate removal was attributed to perchlorate reducing bacteria (PRB) in SA reactor. Furthermore, combined with Pearson analysis, N-acylhomoserine lactones (AHLs)-mediated quorum sensing regulated the production of TB-EPS, improving biofilm stability and thus ensuring the removal performance of reactors. 16sRNA gene sequencing results indicated that the key functional bacteria in the PNA reactor were Comamonas and Candidatus Kuenenia, and the key functional bacteria in the SA reactor were Sulfurimonas, Thiobacillus, and Defluviimonas. These key functional bacteria ensured PNA-SA system feasibility and stability. Such results indicated that PNA-SA system could be used to treat ammonium and perchlorate composite wastewater, thereby providing a new strategy for removing such composite wastewater.
{"title":"Simultaneously ammonium and perchlorate remove via the partial nitrification-anammox coupled sulfur autotrophic system","authors":"Guiying Zhang ,&nbsp;Jingmei Liu ,&nbsp;Yi Han ,&nbsp;Liang Xia ,&nbsp;Jianbing Zhang ,&nbsp;Jianbo Guo ,&nbsp;Haibo Li ,&nbsp;Yanan Hou ,&nbsp;Yuanyuan Song","doi":"10.1016/j.envres.2025.121195","DOIUrl":"10.1016/j.envres.2025.121195","url":null,"abstract":"<div><div>In this study, partial nitrification-anammox coupled sulfur autotrophic (PNA-SA) system was constructed for removing ammonium and perchlorate from composite wastewater simultaneously. The removal rates of ammonium and perchlorate could reach 94.2% and 93.1%, respectively, at an ammonium concentration of 60 mg N∙L<sup>−1</sup> and a perchlorate concentration of 30 mg N∙L<sup>−1</sup>. Ammonium was mainly removed by anammox bacteria (AnAOB) in PNA reactor, while perchlorate removal was attributed to perchlorate reducing bacteria (PRB) in SA reactor. Furthermore, combined with Pearson analysis, N-acylhomoserine lactones (AHLs)-mediated quorum sensing regulated the production of TB-EPS, improving biofilm stability and thus ensuring the removal performance of reactors. 16sRNA gene sequencing results indicated that the key functional bacteria in the PNA reactor were <em>Comamonas</em> and <em>Candidatus Kuenenia</em>, and the key functional bacteria in the SA reactor were <em>Sulfurimonas</em>, <em>Thiobacillus</em>, and <em>Defluviimonas</em>. These key functional bacteria ensured PNA-SA system feasibility and stability. Such results indicated that PNA-SA system could be used to treat ammonium and perchlorate composite wastewater, thereby providing a new strategy for removing such composite wastewater.</div></div>","PeriodicalId":312,"journal":{"name":"Environmental Research","volume":"272 ","pages":"Article 121195"},"PeriodicalIF":7.7,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143474746","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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Environmental Research
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