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Removal and Oxidation of Low Concentration tert-Butanol from Potable Water using Nonthermal Plasma Coupled with Metal Oxide Adsorption 利用非热等离子体和金属氧化物吸附技术去除和氧化饮用水中的低浓度叔丁醇
IF 7.1 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-08-20 DOI: 10.1021/acsestengg.4c00166
Cristina E. Stere, Maicon Delarmelina, Mbongiseni W. Dlamini, Sarayute Chansai, Philip R. Davies, Graham J. Hutchings, C. Richard A. Catlow, Christopher Hardacre
Taste and odor are crucial factors in evaluating the quality of drinking water for consumers. Geosmin is an example of a pollutant commonly found in potable water responsible for earthy and musty taste, and odor even at low concentrations. We have investigated the use of a hybrid two-step adsorption-mineralization process for low-level volatile organic compounds removal from potable water using dielectric barrier discharge over common metal oxides (MO). The system proposed is a proof of principle with tert-butanol (TBA) used as a model compound for geosmin removal/degradation during wastewater treatment when combined with an appropriate metal oxide adsorbent. Initial assessments of the adsorption properties of titania by density functional theory (DFT) calculations and experimental tests indicated that the adsorption of geosmin and TBA with water present results in only weak interactions between the sorbate and the metal oxide. In contrast, the DFT results show that alumina could be a suitable adsorbent for these tertiary alcohols and were reinforced by experimental studies. We find that while there is a competitive effect between the water and TBA adsorption from gaseous/liquid feed, the VOC can be removed, and the alumina will be regenerated by the reactive oxygen species (ROS) produced by a dielectric barrier discharge (DBD). The use of alumina in conjunction with NTP leads to efficient degradation of the adsorbate and the formation of oxygenated intermediates (formates, carbonates, and carboxylate-type species), which could then be mineralized for the regeneration of the adsorbent. A reaction mechanism has been proposed based on the in-situ infrared measurements and DFT calculations, while the removal of TBA with conventional heating is indicative of a gradual desorption process as a function of temperature rather than the destruction of the adsorbate. Furthermore, steady performance was observed after several adsorption–regeneration cycles, indicating no alteration of the adsorption properties of alumina during the NTP treatment and demonstrating the potential of the approach to be applied in the treatment of high throughput of water, without the challenges faced by the biocatalysts or formation of toxic byproducts.
味道和气味是评估消费者饮用水质量的关键因素。土臭素是饮用水中常见的一种污染物,即使浓度很低,也会产生泥土味和霉味以及异味。我们研究了在普通金属氧化物(MO)上使用电介质阻挡放电的两步吸附-矿化混合工艺来去除饮用水中的低浓度挥发性有机化合物。提出的系统是一个原理验证,以叔丁醇(TBA)为模型化合物,与适当的金属氧化物吸附剂相结合,在废水处理过程中去除/降解地奥辛。通过密度泛函理论(DFT)计算和实验测试对二氧化钛的吸附特性进行的初步评估表明,地奥司明和叔丁醇与水的吸附只会导致吸附剂和金属氧化物之间产生微弱的相互作用。与此相反,DFT 结果表明,氧化铝可能是这些叔醇的合适吸附剂,实验研究也证实了这一点。我们发现,虽然气态/液态进料中的水和 TBA 吸附之间存在竞争效应,但挥发性有机化合物可以被去除,而且氧化铝会被介质阻挡放电(DBD)产生的活性氧(ROS)再生。将氧化铝与 NTP 结合使用,可有效降解吸附剂并形成含氧中间产物(甲酸盐、碳酸盐和羧酸盐类),然后将其矿化,用于吸附剂的再生。根据原位红外测量和 DFT 计算提出了一种反应机制,而传统加热法去除 TBA 的过程表明,这是一个随温度变化而逐渐解吸的过程,而不是吸附剂被破坏的过程。此外,经过几个吸附-再生周期后,观察到了稳定的性能,这表明氧化铝的吸附特性在 NTP 处理过程中没有发生改变,并证明了该方法在处理高吞吐量水方面的应用潜力,同时还避免了生物催化剂所面临的挑战或有毒副产品的形成。
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引用次数: 0
Co-valorization of Food Waste and CO2 to Produce Volatile Fatty Acids Using Liter-Scale Tubular Microbial Electrosynthesis Cells 利用升级管式微生物电合成电池将厨余垃圾和二氧化碳共价生成挥发性脂肪酸
IF 7.4 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-08-20 DOI: 10.1021/acsestengg.4c0021810.1021/acsestengg.4c00218
Yanhong Bian, Aaron M. Leininger, Weilan Zhang, Yanna Liang and Zhiyong Jason Ren*, 

This study presents the simultaneous conversion of food waste and CO2 into volatile fatty acids (VFAs) using a 6 L tubular microbial electrosynthesis cell (MES). The MES reactor uses a bioanode to convert food waste into current and CO2, while on the cathode, H2 is produced and subsequently consumed by cathode microbes for the conversion of CO2 to VFAs. The study reveals that system performance is impacted by organic loading, applied voltage, and flow rate, and optimal operational conditions achieve a VFA titer of 1763 mg/L with the Coulombic efficiency (CE) exceeding 90% at the anode, highlighting efficient electron recovery from food waste. Resistance analysis indicates that the cathode contributed most to system resistance, while microbial community analysis shows a synergy between fermentative and electroactive bacteria in the anode and dominant acetogens in the cathode, facilitating efficient electron recovery and VFA synthesis, respectively. The research underscores the tubular MES’s potential for sustainable food waste treatment and CO2 valorization into valuable VFAs, contributing to waste management and greenhouse gas mitigation strategies.

本研究介绍了利用 6 升管式微生物电合成池(MES)将食物垃圾和二氧化碳同时转化为挥发性脂肪酸(VFAs)的方法。MES 反应器使用生物阳极将食物垃圾转化为电流和 CO2,同时在阴极产生 H2,随后阴极微生物消耗 H2 将 CO2 转化为挥发性脂肪酸。研究表明,系统性能受有机负载、应用电压和流速的影响,最佳运行条件下的 VFA 滴度为 1763 毫克/升,阳极的库仑效率(CE)超过 90%,突出显示了从食物垃圾中回收电子的效率。阻力分析表明,阴极对系统阻力的影响最大,而微生物群落分析表明,阳极的发酵菌和电活性菌与阴极的优势醋酸菌之间存在协同作用,分别促进了高效电子回收和 VFA 合成。这项研究强调了管式 MES 在可持续食品废物处理和将二氧化碳转化为有价值的 VFA 方面的潜力,有助于废物管理和温室气体减排战略。
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引用次数: 0
Surface Complexation and Packed Bed Mass Transport Models Enable Adsorbent Design for Arsenate and Vanadate Removal 表面络合和堆积床质量迁移模型有助于设计用于去除砷酸盐和钒酸盐的吸附剂
IF 7.1 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-08-19 DOI: 10.1021/acsestengg.4c00315
Emily Briese, Ken Niimi, Annika Hjelmstad, Paul Westerhoff
Co-occurrence of metal oxo-anions (e.g., arsenate) in drinking water poses human health risks. To understand and predict competition and breakthrough for individual or mixtures of oxo-anions in continuous-flow packed bed adsorption systems, we linked equilibrium surface complexation models (SCMs) with a pore surface diffusion model (PSDM). After parametrization, using data for two commercial adsorbents, the SCM and PSDM predicted well the adsorption isotherm data and column breakthrough curves, respectively, for single-solute (arsenate) and bisolute water chemistries (arsenate, vanadate) as well as chromatographic displacement of previously adsorbed arsenate by vanadate. Surface and pore diffusivities for both commercial adsorbents were 3.0 to 3.5 x10–12 cm2/s and 1.1 to 0.8 x10–6 cm2/s, respectively. After validation, SCM + PSDM was used in silico to evaluate adsorbent media characteristics, variable water chemistries, and reactor configurations. When contrasting hypothetical crystalline versus amorphous metal (hydr)oxide adsorbents, increasing surface site density resulted in higher Freundlich isotherm capacity (KF) but did not impact 1/n. Increasing surface binding affinities beneficially impacted both the KF and 1/n isotherms and would improve the performance of point-of-use (POU) adsorbent system applications. In silico simulation results suggest prioritizing enhancing adsorbent capacity (q) through improved surface reactivity in the design of new POU adsorbent materials rather than focusing on reducing mass transport limitations through intraparticle pore design. For municipal-scale adsorption systems, the PSDM simulation of the mass transfer zone shape was evaluated for hypothetical adsorbent pore designs (i.e., intraparticle porosity (εp) and tortuosity) and demonstrated that εp control was a key strategy to improve performance.
饮用水中金属氧化阴离子(如砷酸盐)的共存会对人类健康造成危害。为了了解和预测连续流填料床吸附系统中单个或混合氧化阴离子的竞争和突破情况,我们将平衡表面络合模型(SCM)与孔隙表面扩散模型(PSDM)联系起来。参数化后,利用两种商用吸附剂的数据,SCM 和 PSDM 分别很好地预测了单固态(砷酸盐)和双固态水化学(砷酸盐、钒酸盐)的吸附等温线数据和色谱柱突破曲线,以及钒酸盐对先前吸附的砷酸盐的色谱置换。两种商用吸附剂的表面和孔隙扩散率分别为 3.0 至 3.5 x10-12 cm2/s 和 1.1 至 0.8 x10-6 cm2/s。经过验证后,SCM + PSDM 被用于评估吸附剂介质特性、不同的水化学成分和反应器配置。在对比假定的结晶与无定形金属(水)氧化物吸附剂时,增加表面位点密度可提高 Freundlich 等温线容量 (KF),但对 1/n 没有影响。增加表面结合亲和力会对 KF 和 1/n 等温线产生有利影响,并能提高使用点 (POU) 吸附剂系统的应用性能。硅学模拟结果表明,在设计新型 POU 吸附材料时,应优先考虑通过提高表面反应速度来增强吸附容量(q),而不是通过粒子内孔隙设计来减少质量传输限制。对于市政规模的吸附系统,针对假设的吸附剂孔隙设计(即颗粒内孔隙率(εp)和迂回度),对传质区形状的 PSDM 仿真进行了评估,结果表明εp 控制是提高性能的关键策略。
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引用次数: 0
Biological Waste-Derived Dual-Site Catalyst Empowers Electro-Fenton Systems to Sustainably Decontaminate Livestock Wastewater 生物废料衍生的双位催化剂推动电-芬顿系统以可持续的方式净化禽畜废水
IF 7.1 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-08-15 DOI: 10.1021/acsestengg.4c00413
Ke-Yu Chen, Yun-Xin Huang, Qian Zhang, Shou-Yan Zhao, Wen-Ting Liu, Qi Wang, Bao-Cheng Huang, Ren-Cun Jin
Livestock and poultry industries are pivotal for meat production, but produced wastewater with heavy pollution challenges environmental sustainability and public health. The electro-Fenton (EF) process, capable of in situ production and activation of hydrogen peroxide, is promising for decontaminating recalcitrant pollutants, yet fabricating a highly active bifunctional cathode catalyst across a broad pH range remains a bottleneck. Guided by green chemistry principles, we synthesized a dual-site catalyst from biological waste to facilitate hydroxyl radical production. Combined experimental and theoretical investigations unveiled that the Fe2O3 sites facilitated H2O2 generation via catalyzing the oxygen reduction reaction, whereas Fe3N sites promoted in situ H2O2 activation into hydroxyl radicals. This electrocatalyst, integrated into a gas diffusion electrode, achieved stable, aeration-free mineralization of antibiotic contaminants at neutral pH with a low energy consumption of just 0.94 kWh/g of removed total organic carbon. The further development of a tandem system that coupled the anammox bioprocess with the EF process exhibited exceptional efficiency in both nitrogen removal and tertiary purification of actual livestock wastewater, obviating the need for pH adjustments or Fenton reagent additives. These findings underscore the potential scalability and application of our proposed approach in promoting sustainable wastewater management practices.
畜禽养殖业在肉类生产中举足轻重,但其产生的废水污染严重,对环境的可持续发展和公众健康构成了挑战。电-芬顿(EF)工艺能够原位产生和活化过氧化氢,在净化难降解污染物方面前景广阔,但在广泛的 pH 值范围内制造高活性双功能阴极催化剂仍是一个瓶颈。在绿色化学原理的指导下,我们从生物废料中合成了一种双位点催化剂,以促进羟基自由基的产生。结合实验和理论研究发现,Fe2O3 位点通过催化氧还原反应促进 H2O2 生成,而 Fe3N 位点则促进 H2O2 就地活化为羟基自由基。这种集成到气体扩散电极中的电催化剂实现了抗生素污染物在中性 pH 值下的稳定、无曝气矿化,且能耗低,仅为 0.94 千瓦时/克去除的总有机碳。进一步开发的串联系统将 Anammox 生物工艺与 EF 工艺相结合,在实际畜牧业废水的脱氮和三级净化方面都表现出卓越的效率,无需调节 pH 值或添加芬顿试剂。这些发现强调了我们提出的方法在促进可持续废水管理实践中的潜在可扩展性和应用性。
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引用次数: 0
Enhancing Anaerobic Digestion of Food Waste by Combining Carriers and Microaeration: Performance and Potential Mechanisms 通过结合载体和微曝气加强厨余垃圾的厌氧消化:性能和潜在机制
IF 7.1 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-08-13 DOI: 10.1021/acsestengg.4c00298
Baocun Wu, Yi Wang, Linyan He, Miao Liu, Jinjing Xiang, Yongdong Chen, Li Gu, Jinze Li, Lin Li, Weiliang Pan, Qiang He
Enhancing the anaerobic digestion (AD) of organic wastes has been a widely discussed topic. This study aims to enhance AD performance by combining microaeration with conductive or nonconductive carriers, using food waste as the substrate. The use of carriers alone enhanced methane production, and microaeration further improved performance. The conductive carrier showed significant enhancement with microaeration, achieving a daily methane yield of 478 ± 11.3 mL CH4/g VS, which was 1.1 and 1.3 times higher than that of the nonconductive carrier and the control digester, respectively. Furthermore, the study explored various aspects, including oxidative stress, antioxidant capacity, and microbial community structure during digestion. The results demonstrated that combining microaeration with a conductive carrier improved hydrolytic-acidification efficiency and promoted direct interspecies electron transfer among syntrophic microorganisms. Methanogenic archaea aggregated on the carrier surface and formed consortia with facultative anaerobes, thereby mitigating oxidative stress effects on cells and enhancing total methane production. Moreover, metabolomics analysis showed that combining conductive carriers with microaeration enhanced ATP transport across the bacterial membrane, accelerated nutrient conversion, and caused significant changes in metabolites and intermediates related to glycerophospholipids, amino acids, and signal transduction pathways.
加强有机废物的厌氧消化(AD)一直是一个广泛讨论的话题。本研究旨在以厨余为基质,通过将微曝气与导电或不导电载体相结合来提高厌氧消化性能。单独使用载体可提高甲烷产量,而微曝气可进一步提高性能。在微曝气的作用下,导电载体的甲烷产量显著提高,日甲烷产量达到 478 ± 11.3 mL CH4/g VS,分别是非导电载体和对照消化器的 1.1 倍和 1.3 倍。此外,研究还探讨了消化过程中的氧化应激、抗氧化能力和微生物群落结构等各个方面。结果表明,将微曝气与导电载体相结合可提高水解酸化效率,并促进合成微生物之间的种间直接电子传递。产甲烷古细菌聚集在载体表面,与兼性厌氧菌形成联合体,从而减轻了氧化应激对细胞的影响,提高了甲烷总产量。此外,代谢组学分析表明,导电载体与微通气的结合增强了 ATP 在细菌膜上的传输,加速了营养物质的转化,并导致与甘油磷脂、氨基酸和信号转导途径有关的代谢物和中间产物发生显著变化。
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引用次数: 0
Nanoconfined Cobalt Ferrite Composite Carbon Nanotube Membrane Oxidation-Filtration System for Water Decontamination 用于水净化的纳米钴铁氧体复合碳纳米管膜氧化-过滤系统
IF 7.1 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-08-12 DOI: 10.1021/acsestengg.4c00282
Huanran Ma, Lijun Zhang, Xiao Zhang, Zonglin Pan, Ruisong Xu, Guanlong Wang, Xinfei Fan, Huixia Lu, Shuaifei Zhao, Chengwen Song
Constructing a membrane-confined peroxymonosulfate (PMS) activation system has emerged as a promising strategy for efficient water decontamination. Herein, a novel cobalt ferrite (CoFe2O4)-filled open-end carbon nanotube (OCNT) membrane filtration system was proposed, aiming to integrate dual metal centers and nanoconfinement for enhancing PMS activation (MFPA) toward water decontamination. The optimal CoFe2O4@OCNT MFPA process displayed 100% phenol removal within a residence time of 5.7 s, whose k (1.17 s–1) was 3.0, 5.6, and 3.9 times higher than that of CoO@OCNT, FeO@OCNT, and CoFe2O4/CCNT (surface-loaded closed end cap CNT), respectively. Experimental results and theoretical calculations jointly unravel the nonradical-dominated (1O2 and electron transfer) oxidation mechanism, leading to the wide-pH adaptation and superior stability in the complex water matrix. Mechanism analysis showed that fast cycling of Co2+/Co3+ was achieved via synergistic promotion between dual metal centers and the nanoconfinement effect, which coboosted the PMS consumption as well as reactive oxygen species generation (especially 1O2). Compared with the single metal center, the dual metal centers of internal CoFe2O4 exhibited coenhanced electron cloud density (amount of charge transfer) and adsorption energy for PMS, resulting in O–O cleavage and elongated O–H. Meanwhile, the oxygen vacancy defect (Odef) on CoFe2O4 also contributed to the nonradical process, which not only served as the precursor of 1O2 generation but also acted as a transfer station for electrons.
构建膜封闭式过一硫酸盐(PMS)活化系统已成为一种很有前途的高效水净化策略。本文提出了一种新型的铁氧体钴(CoFe2O4)填充开口碳纳米管(OCNT)膜过滤系统,旨在整合双金属中心和纳米细化技术,以增强过硫酸盐活化(MFPA),从而达到净化水的目的。最佳的 CoFe2O4@OCNT MFPA 工艺在 5.7 秒的停留时间内实现了 100% 的苯酚去除率,其 k 值(1.17 s-1)分别是 CoO@OCNT、FeO@OCNT 和 CoFe2O4/CCNT(表面负载封闭端盖 CNT)的 3.0、5.6 和 3.9 倍。实验结果和理论计算共同揭示了非自由基主导(1O2 和电子传递)的氧化机理,从而使其在复杂的水基质中具有较宽的 pH 适应性和优异的稳定性。机理分析表明,Co2+/Co3+ 的快速循环是通过双金属中心之间的协同促进作用和纳米融合效应实现的,这共同促进了 PMS 的消耗和活性氧(尤其是 1O2)的生成。与单金属中心相比,内部 CoFe2O4 的双金属中心表现出共同增强的电子云密度(电荷转移量)和对 PMS 的吸附能,从而导致 O-O 裂解和 O-H 拉伸。同时,CoFe2O4 上的氧空位缺陷(Odef)也促进了非辐射过程,它不仅是生成 1O2 的前体,也是电子的中转站。
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引用次数: 0
Vital Threshold and Underlying Mechanism for the Complete Remediation of Oil and Microplastic Co-Contaminated Soil by Fast Pyrolysis 通过快速热解完全修复油类和微塑料共污染土壤的重要阈值和基本机制
IF 7.4 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-08-11 DOI: 10.1021/acsestengg.4c0020410.1021/acsestengg.4c00204
Zi-Ying Hu,  and , Hong Jiang*, 

The coexistence of microplastics (MPs) and oil contaminants in soil has led to a new pollution scenario around the oil-production region, yet how to cost-effectively remediate soil with combined pollutants has rarely been explored. Herein, we propose a fast pyrolysis technique to perfectly remediate MPS-oil copresence soil (MPs-oil-soil). The experimental data showed that pyrolysis at 500 °C for 15 min is a key threshold for the complete removal of MPs and petroleum contaminants from soil. Above this threshold, seed germination and the growth of wheat in the soil increased, and the rhizosphere microbial population decreased with increasing abundance of beneficial microbial flora, such as Proteobacteria, Actinobacteria and Bacteroidetes (which promote the circulation of nutrients and help to strengthen plant resistance). Structural equation modeling revealed that temperature had a more significant positive effect on the remediation effect than did time. Two-dimensional correlation spectroscopy combined with synchronous fluorescence spectroscopy showed that the presence of MPs was the main factor affecting the pyrolysis threshold. Three-dimensional excitation–emission matrix and UV–visible absorption spectroscopy revealed large differences in the aromaticity and relative molecular weight of dissolved organic matter before and after the pyrolysis threshold. These findings shed light on the mechanistic understanding of the pyrolytic remediation of microplastics and oil-contaminated soils.

微塑料(MPs)和石油污染物在土壤中的共存导致了产油区周围出现了一种新的污染情况,但如何经济有效地修复混合污染物的土壤却鲜有人问津。在此,我们提出了一种快速热解技术来完美修复 MPS-石油共存土壤(MPs-土壤-土壤)。实验数据表明,在 500 °C 下热解 15 分钟是完全去除土壤中 MPs 和石油污染物的关键阈值。超过这一临界值,种子发芽率和小麦在土壤中的生长速度均有所提高,根圈微生物数量减少,有益微生物菌群数量增加,如变形菌、放线菌和类杆菌(促进养分循环,有助于增强植物抵抗力)。结构方程模型显示,温度对修复效果的积极影响比时间更显著。二维相关光谱与同步荧光光谱相结合显示,MPs 的存在是影响热解阈值的主要因素。三维激发-发射矩阵和紫外-可见吸收光谱显示,在热解阈值前后,溶解有机物的芳香度和相对分子量存在很大差异。这些发现有助于从机理上理解微塑料和油污染土壤的热解修复。
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引用次数: 0
Vital Threshold and Underlying Mechanism for the Complete Remediation of Oil and Microplastic Co-Contaminated Soil by Fast Pyrolysis 通过快速热解完全修复油类和微塑料共污染土壤的重要阈值和基本机制
IF 7.1 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-08-11 DOI: 10.1021/acsestengg.4c00204
Zi-Ying Hu, Hong Jiang
The coexistence of microplastics (MPs) and oil contaminants in soil has led to a new pollution scenario around the oil-production region, yet how to cost-effectively remediate soil with combined pollutants has rarely been explored. Herein, we propose a fast pyrolysis technique to perfectly remediate MPS-oil copresence soil (MPs-oil-soil). The experimental data showed that pyrolysis at 500 °C for 15 min is a key threshold for the complete removal of MPs and petroleum contaminants from soil. Above this threshold, seed germination and the growth of wheat in the soil increased, and the rhizosphere microbial population decreased with increasing abundance of beneficial microbial flora, such as Proteobacteria, Actinobacteria and Bacteroidetes (which promote the circulation of nutrients and help to strengthen plant resistance). Structural equation modeling revealed that temperature had a more significant positive effect on the remediation effect than did time. Two-dimensional correlation spectroscopy combined with synchronous fluorescence spectroscopy showed that the presence of MPs was the main factor affecting the pyrolysis threshold. Three-dimensional excitation–emission matrix and UV–visible absorption spectroscopy revealed large differences in the aromaticity and relative molecular weight of dissolved organic matter before and after the pyrolysis threshold. These findings shed light on the mechanistic understanding of the pyrolytic remediation of microplastics and oil-contaminated soils.
微塑料(MPs)和石油污染物在土壤中的共存导致了产油区周围出现了一种新的污染情况,但如何经济有效地修复混合污染物的土壤却鲜有人问津。在此,我们提出了一种快速热解技术来完美修复 MPS-石油共存土壤(MPs-土壤-土壤)。实验数据表明,在 500 °C 下热解 15 分钟是完全去除土壤中 MPs 和石油污染物的关键阈值。超过这一临界值,种子发芽率和小麦在土壤中的生长速度均有所提高,根圈微生物数量减少,有益微生物菌群数量增加,如变形菌、放线菌和类杆菌(促进养分循环,有助于增强植物抵抗力)。结构方程模型显示,温度对修复效果的积极影响比时间更显著。二维相关光谱与同步荧光光谱相结合显示,MPs 的存在是影响热解阈值的主要因素。三维激发-发射矩阵和紫外-可见吸收光谱显示,在热解阈值前后,溶解有机物的芳香度和相对分子量存在很大差异。这些发现有助于从机理上理解微塑料和油污染土壤的热解修复。
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引用次数: 0
Enhanced Detection of Primary Biological Aerosol Particles Using Machine Learning and Single-Particle Measurement 利用机器学习和单粒子测量增强对初级生物气溶胶粒子的检测
IF 7.1 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-08-07 DOI: 10.1021/acsestengg.4c00262
Ashfiqur Rahman, Nurun Nahar Lata, Bruna Grasielli Sebben, Darielle Dexheimer, Zezhen Cheng, Ricardo Henrique Moreton Godoi, Aivett Bilbao, Swarup China
Accurately identifying primary biological aerosol particles (PBAPs) using analytical techniques poses inherent challenges due to their resemblance to other atmospheric carbonaceous particles. We present a study of an enhanced method for detecting PBAPs by combining single-particle measurement with advanced supervised machine learning (SML) techniques. We analyzed ambient particles from a variety of environments and lab-generated standards, focusing on chemical composition for traditional rule-based and clustering approaches and incorporating morphological features into the SML approaches, neural networks and XGBoost, for improved accuracy. This study demonstrates that SML methods outperform traditional methods in quantifying PBAPs, achieving significant improvements in precision, recall, F1-score, and accuracy, leading to an increased number of detected PBAPs by at least 19%. The adaptability of the proposed XGBoost-based SML model is showcased in comparison to traditional methods in categorizing PBAPs for blind data sets from different geographical locations. Two field case studies were investigated, over agricultural land and Amazonia rain forest, representing relatively low and high concentrations of PBAPs, respectively, where XGBoost consistently detected up to 3.5 times more PBAPs than traditional methods. Precise detection of PBAPs in the atmosphere could significantly improve the prediction of climatic impacts by them.
由于原生生物气溶胶粒子(PBAPs)与大气中的其他碳质粒子相似,因此使用分析技术准确识别这些粒子存在固有的挑战。我们通过将单颗粒测量与先进的监督机器学习(SML)技术相结合,研究了一种检测 PBAP 的增强型方法。我们分析了各种环境中的环境颗粒和实验室生成的标准颗粒,在传统的基于规则的方法和聚类方法中重点关注化学成分,在 SML 方法、神经网络和 XGBoost 中加入形态特征以提高准确性。这项研究表明,在量化 PBAP 方面,SML 方法优于传统方法,在精确度、召回率、F1 分数和准确度方面都有显著提高,使检测到的 PBAP 数量至少增加了 19%。与传统方法相比,所提出的基于 XGBoost 的 SML 模型在对来自不同地理位置的盲数据集进行 PBAP 分类时,展示了其适应性。对农业用地和亚马逊热带雨林的两个实地案例进行了研究,这两个地方分别代表了相对较低和较高的 PBAP 浓度,XGBoost 检测到的 PBAP 始终是传统方法的 3.5 倍。精确检测大气中的多溴联苯醚可大大改善对其气候影响的预测。
{"title":"Enhanced Detection of Primary Biological Aerosol Particles Using Machine Learning and Single-Particle Measurement","authors":"Ashfiqur Rahman, Nurun Nahar Lata, Bruna Grasielli Sebben, Darielle Dexheimer, Zezhen Cheng, Ricardo Henrique Moreton Godoi, Aivett Bilbao, Swarup China","doi":"10.1021/acsestengg.4c00262","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00262","url":null,"abstract":"Accurately identifying primary biological aerosol particles (PBAPs) using analytical techniques poses inherent challenges due to their resemblance to other atmospheric carbonaceous particles. We present a study of an enhanced method for detecting PBAPs by combining single-particle measurement with advanced supervised machine learning (SML) techniques. We analyzed ambient particles from a variety of environments and lab-generated standards, focusing on chemical composition for traditional rule-based and clustering approaches and incorporating morphological features into the SML approaches, neural networks and XGBoost, for improved accuracy. This study demonstrates that SML methods outperform traditional methods in quantifying PBAPs, achieving significant improvements in precision, recall, F1-score, and accuracy, leading to an increased number of detected PBAPs by at least 19%. The adaptability of the proposed XGBoost-based SML model is showcased in comparison to traditional methods in categorizing PBAPs for blind data sets from different geographical locations. Two field case studies were investigated, over agricultural land and Amazonia rain forest, representing relatively low and high concentrations of PBAPs, respectively, where XGBoost consistently detected up to 3.5 times more PBAPs than traditional methods. Precise detection of PBAPs in the atmosphere could significantly improve the prediction of climatic impacts by them.","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.1,"publicationDate":"2024-08-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141948905","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Energy-Efficient Nutrient Recovery from Real Urine for Hydroponics Based on Alkalinization, Full Nitrification in a Trickling Filter and Limited Supplementations 基于涓流过滤器中的碱化、完全硝化和有限补充,从真实尿液中为水培法回收高能效养分
IF 7.4 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-08-06 DOI: 10.1021/acsestengg.4c0018810.1021/acsestengg.4c00188
Yankai Xie, Mingsheng Jia, Patricia Gutiérrez Lozano, Marijn Juliaan Timmer, Marc Spiller, Jolien De Paepe and Siegfried E. Vlaeminck*, 

Human urine is considered a major stream of nitrogen mass flow in domestic wastewater, which is widely available and rich in valuable nutrient resources for hydroponic cultivation. In this study, a promising concept of nutrient recovery from real urine was proposed, including urine alkalinization by Ca(OH)2, full nitrification in a trickling filter, and chemical supplementations. The steady performance of urine nitrification among different urine-collecting batches indicates the robustness of the trickling filter. An optimal hydraulic loading rate of 2.1 m3 m–2 h–1 sufficed the dissolved oxygen and urine circulation in the trickling filter, achieving a nitrate production rate of 223 ± 2 mg N L–1 d–1 with an efficiency of 90 ± 2% at pH 6 and 21 °C. The electrical energy consumption was only 1.15 kWh kg–1 NO3-N production at a short hydraulic retention time of 1 day. Among all of the three types of pH control reagents (i.e., Ca(OH)2, CaCO3, and K2CO3), K2CO3 could enhance the activity of ammonium-oxidizing bacteria by raising the inorganic carbon level in the trickling filter and subsequently result in the lowest supplementation of extra macronutrients (i.e., nitrogen, phosphorus, and magnesium) to the urine-sourced nutrient solution. Batch tests showed that the highest activity of ammonium-oxidizing and nitrite-oxidizing bacteria was in the bottom compartment of the trickling filter, consistent with the vertical stratification of their relative abundance. Overall, the proposed novel concept was demonstrated to be robust and energy-efficient in nutrient recovery from real urine for hydroponics.

人尿被认为是生活废水中氮质量流的主要来源,其来源广泛且富含宝贵的营养资源,可用于水培栽培。本研究提出了一种从真实尿液中回收营养物质的可行概念,包括用 Ca(OH)2 碱化尿液、在滴流过滤器中充分硝化尿液以及补充化学物质。在不同的尿液收集批次中,尿液硝化的稳定表现表明了滴流过滤器的稳健性。最佳水力负荷率为 2.1 m3 m-2 h-1,足以满足滴流过滤器中的溶解氧和尿液循环,在 pH 值为 6 和温度为 21 ℃ 的条件下,硝酸盐产生率为 223 ± 2 mg N L-1 d-1,效率为 90 ± 2%。在 1 天的短水力停留时间内,电能消耗仅为 1.15 kWh kg-1 NO3--N。在所有三种 pH 值控制试剂(即 Ca(OH)2、CaCO3 和 K2CO3)中,K2CO3 可通过提高滴流滤池中的无机碳含量来增强铵氧化细菌的活性,从而使尿液营养液中额外大量营养元素(即氮、磷和镁)的补充量最低。批量测试表明,氨氧化细菌和亚硝酸盐氧化细菌的最高活性位于滴流式过滤器的底层,这与它们相对丰度的垂直分层是一致的。总之,在从真实尿液中回收营养物质用于水培方面,所提出的新概念被证明是稳健而节能的。
{"title":"Energy-Efficient Nutrient Recovery from Real Urine for Hydroponics Based on Alkalinization, Full Nitrification in a Trickling Filter and Limited Supplementations","authors":"Yankai Xie,&nbsp;Mingsheng Jia,&nbsp;Patricia Gutiérrez Lozano,&nbsp;Marijn Juliaan Timmer,&nbsp;Marc Spiller,&nbsp;Jolien De Paepe and Siegfried E. Vlaeminck*,&nbsp;","doi":"10.1021/acsestengg.4c0018810.1021/acsestengg.4c00188","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00188https://doi.org/10.1021/acsestengg.4c00188","url":null,"abstract":"<p >Human urine is considered a major stream of nitrogen mass flow in domestic wastewater, which is widely available and rich in valuable nutrient resources for hydroponic cultivation. In this study, a promising concept of nutrient recovery from real urine was proposed, including urine alkalinization by Ca(OH)<sub>2</sub>, full nitrification in a trickling filter, and chemical supplementations. The steady performance of urine nitrification among different urine-collecting batches indicates the robustness of the trickling filter. An optimal hydraulic loading rate of 2.1 m<sup>3</sup> m<sup>–2</sup> h<sup>–1</sup> sufficed the dissolved oxygen and urine circulation in the trickling filter, achieving a nitrate production rate of 223 ± 2 mg N L<sup>–1</sup> d<sup>–1</sup> with an efficiency of 90 ± 2% at pH 6 and 21 °C. The electrical energy consumption was only 1.15 kWh kg<sup>–1</sup> NO<sub>3</sub><sup>–</sup>-N production at a short hydraulic retention time of 1 day. Among all of the three types of pH control reagents (i.e., Ca(OH)<sub>2</sub>, CaCO<sub>3</sub>, and K<sub>2</sub>CO<sub>3</sub>), K<sub>2</sub>CO<sub>3</sub> could enhance the activity of ammonium-oxidizing bacteria by raising the inorganic carbon level in the trickling filter and subsequently result in the lowest supplementation of extra macronutrients (i.e., nitrogen, phosphorus, and magnesium) to the urine-sourced nutrient solution. Batch tests showed that the highest activity of ammonium-oxidizing and nitrite-oxidizing bacteria was in the bottom compartment of the trickling filter, consistent with the vertical stratification of their relative abundance. Overall, the proposed novel concept was demonstrated to be robust and energy-efficient in nutrient recovery from real urine for hydroponics.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.4,"publicationDate":"2024-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142228300","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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ACS ES&T engineering
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