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Flexible Electrochemical Stripping for Wastewater Ammonia Recovery with On-Demand Product Tunability 用于废水氨回收的灵活电化学剥离,可按需进行产品调整
IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-07-05 DOI: 10.1021/acs.estlett.4c0036610.1021/acs.estlett.4c00366
Anna Kogler, Meili Gong, Kindle S. Williams and William A. Tarpeh*, 

Nitrogen in wastewater can be recovered to prevent negative environmental, human health, and economic impacts and to enable distributed chemical manufacturing. We developed novel flexible electrochemical stripping (FECS) for tunable recovery of ammonia/ammonium (total ammonia nitrogen, TAN) from urine as (NH4)2SO4 and aqueous NH3. Batch and continuous experiments demonstrated that product speciation could be readily controlled by modifying electrochemical cell operation frequency, duration, and applied current without affecting TAN removal. During continuous experiments, FECS recovered NH3 solutions with concentrations similar to ready-to-use cleaners (1% and 2% NH3 (w/w) or 8.22 and 16.4 g/L TAN) and cleaner concentrates (5% NH3 (w/w) or 41.1 g/L TAN), as well as (NH4)2SO4 solutions between 5 and 18.4 g/L TAN, approaching commercial fertilizer concentrations (28.4 g/L TAN). Beyond modifying applied current, future process engineering and operating condition optimization should reduce energy consumption, increase recovery efficiency, and enhance economic viability of FECS. Our findings will enable the development and deployment of electrochemical nitrogen recovery in contexts with varying needs for ammonia-based products, paving the way for circular economies that integrate distributed chemical manufacturing with sanitation systems.

废水中的氮可以回收,以防止对环境、人类健康和经济造成负面影响,并实现分布式化学制造。我们开发了新型柔性电化学剥离 (FECS),用于以 (NH4)2SO4 和 NH3 水溶液的形式从尿液中回收氨/铵(总氨氮,TAN)。批量和连续实验表明,通过改变电化学电池的运行频率、持续时间和外加电流,可以轻松控制产物的种类,而不会影响总氨氮的去除。在连续实验中,FECS 回收的 NH3 溶液浓度类似于即用型清洁剂(1% 和 2% NH3(w/w)或 8.22 和 16.4 克/升 TAN)和清洁剂浓缩物(5% NH3(w/w)或 41.1 克/升 TAN),以及 5 至 18.4 克/升 TAN 的 (NH4)2SO4 溶液,接近商用肥料浓度(28.4 克/升 TAN)。除了修改应用电流,未来的工艺工程和操作条件优化还将降低能耗,提高回收效率,并增强 FECS 的经济可行性。我们的研究结果将使电化学氮回收技术得以在对氨基产品有不同需求的环境中开发和应用,从而为将分布式化学制造与卫生系统相结合的循环经济铺平道路。
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引用次数: 0
Assessing the Relative Concentration Efficiency and Spatial–Temporal Distribution of Plasmid pBI143 in Raw Wastewater 评估原废水中质粒 pBI143 的相对浓度效率和时空分布情况
IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-07-02 DOI: 10.1021/acs.estlett.4c0048510.1021/acs.estlett.4c00485
Bethany Oceguera Johnson, Marlee Shaffer, Devin North, Kien Vu and Kyle Bibby*, 

Plasmid pBI143 has recently been identified as being highly abundant in the human gut microbiome, suggesting potential as a fecal water quality indicator and normalization marker in wastewater-based surveillance. We evaluated the relative concentration efficiency and spatial–temporal distribution in raw wastewater to inform its development as a marker. The results showed significantly higher (p < 0.01) enrichment in raw wastewater solids (mean of 9.2 × 107 GC/mL) than in liquid fractions [mean of 2.3 × 106 genome copies (GC)/mL]. The relative concentration efficiencies were 28% for nanotrap particles, 23% for Amicon ultrafiltration, 3.6% for pH drop and filtration, 4% for skim milk flocculation, and 0.04% for poly(ethylene glycol) precipitation compared to direct wastewater extraction. DNase pretreatment reduced pBI143 levels by 90.3%, indicating that it is mainly extracellular in raw wastewater. Over 21 days, pBI143 levels remained stable and were consistently a mean of 1.3 log10 higher than other fecal indicators (Carjivirus, PMMoV, and HF183). In raw wastewater from eight states (n = 16), pBI143 concentrations averaged 2.2 × 106 GC/mL (95% confidence interval of 1.7–2.7 × 106) and pBI143 was detected in all samples. The findings support pBI143’s potential as a fecal indicator and normalization marker, though further validation is needed to confirm its specificity to humans.

最近发现质粒 pBI143 在人类肠道微生物组中含量很高,这表明它有可能成为粪便水质指标和废水监测中的正常化标记。我们对其在原废水中的相对浓度效率和时空分布进行了评估,以便为其作为标记物的开发提供依据。结果显示,原废水固体(平均 9.2 × 107 GC/mL)中的富集度(p < 0.01)明显高于液体馏分(平均 2.3 × 106 基因组拷贝 (GC)/mL)。与直接提取废水相比,纳米捕集颗粒的相对浓缩效率为 28%,Amicon 超滤为 23%,pH 值下降和过滤为 3.6%,脱脂乳絮凝为 4%,聚乙二醇沉淀为 0.04%。DNase 预处理可使 pBI143 的含量降低 90.3%,这表明它在原废水中主要存在于细胞外。在 21 天的时间里,pBI143 的水平保持稳定,并且一直比其他粪便指标(Carjivirus、PMMoV 和 HF183)平均高出 1.3 log10。在八个州(n = 16)的原始废水中,pBI143 的平均浓度为 2.2 × 106 GC/mL(95% 置信区间为 1.7-2.7 × 106),所有样本中都检测到了 pBI143。研究结果支持 pBI143 作为粪便指示剂和正常化标记物的潜力,不过还需要进一步验证以确认其对人类的特异性。
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引用次数: 0
Multisatellite Data Depicts a Record-Breaking Methane Leak from a Well Blowout 多卫星数据描绘了破纪录的井喷甲烷泄漏事件
IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-30 DOI: 10.1021/acs.estlett.4c0039910.1021/acs.estlett.4c00399
Luis Guanter*, Javier Roger, Shubham Sharma, Adriana Valverde, Itziar Irakulis-Loitxate, Javier Gorroño, Xin Zhang, Berend J. Schuit, Joannes D. Maasakkers, Ilse Aben, Alexis Groshenry, Antoine Benoit, Quentin Peyle and Daniel Zavala-Araiza, 

Accidental blowouts in oil and gas wells can result in large and prolonged methane emissions, which are often unreported when happening in remote places. The rapid advancement of space-based methods for detecting and quantifying methane plumes provides an essential tool for uncovering these superemission events. We use a number of methane-sensitive satellite missions, including the Sentinel-5P/TROPOMI global mapper and several high-resolution instruments, to document a methane leak from a well blowout happening in Kazakhstan’s Karaturun East oil field in 2023. A dense time series of plume detections from those satellites shows that the leak was active during 205 days and that most of the emissions were in the range 20–50 t/h. Using 48 high-quality emission rate estimates, we calculate that a total of 131 ± 34 kt of methane was released to the atmosphere during this leak, which exceeds the total emissions from all previously documented accidents. Our study characterizes the evolution and magnitude of the 2023 Karaturun East methane leak and showcases how different types of satellite instruments can be combined to document and quantify methane leaks active during long time periods.

石油和天然气井的意外井喷会导致大量和长时间的甲烷排放,而这种情况如果发生在偏远地区,往往不会被报告。用于探测和量化甲烷羽流的天基方法的快速发展为揭示这些超高排放事件提供了重要工具。我们利用一些对甲烷敏感的卫星任务,包括哨兵-5P/TROPOMI 全球绘图仪和一些高分辨率仪器,记录了 2023 年在哈萨克斯坦卡拉图伦东油田发生的井喷造成的甲烷泄漏。从这些卫星探测到的密集羽流时间序列显示,泄漏活跃期为 205 天,大部分排放量在 20-50 吨/小时之间。利用 48 个高质量的排放率估算值,我们计算出在这次泄漏过程中,共有 131 ± 34 千吨甲烷被释放到大气中,这超过了之前记录的所有事故的总排放量。我们的研究描述了 2023 年卡拉图伦东部甲烷泄漏的演变过程和规模,并展示了如何将不同类型的卫星仪器结合起来,记录和量化长期活跃的甲烷泄漏。
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引用次数: 0
Cysteine-Protected Antibacterial Spheroids of Atomically Precise Copper Clusters for Direct and Affordable Arsenic Detection from Drinking Water 受半胱氨酸保护的抗菌球状原子团簇铜,用于直接、经济地检测饮用水中的砷含量
IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-28 DOI: 10.1021/acs.estlett.4c0026410.1021/acs.estlett.4c00264
Jenifer Shantha Kumar, Arijit Jana, Jayathraa Raman, Hema Madhuri Veera, Amoghavarsha Ramachandra Kini, Jayoti Roy, Saurav Kanti Jana, Tiju Thomas and Thalappil Pradeep*, 

Rapid and naked-eye detection of water-borne contaminants using molecularly precise nanomaterials has emerged as a promising strategy to reduce the impact of chemical pollution. This study presents a luminescence-based arsenic (As) sensor, eliminating the need for sample preparation. Incorporating red-emitting spheroidal cluster-assembled superstructures (CASs), comprised of Cu17 nanoclusters (Cu17NCs), coprotected by l-cysteine (l-Cys) and 1,2-bis(diphenylphosphino) ethane (DPPE) ligands, the sensor exhibits notable sensitivity toward arsenite (As3+) and (As5+) ions. A detection limit of 1 ppb in tap water was achieved through luminescence-based quenching. Remarkably, it demonstrates selective detection of As amidst common interfering metal ions such as Cd2+, Hg2+, Fe3+, Pb2+, Cu2+, and Cr3+. A sensor disc made of CASs coated on nonwoven polypropylene (PP) mats has been devised for practical field applications. Electron microscopy reveals disrupted morphology of the spheroids due to As interaction. Moreover, the CASs exhibit significant antibacterial efficacy against Gram-negative Escherichia coli and Gram-positive Staphylococcus aureus and antibiofilm properties against Bacillus subtilis. This research highlights the effectiveness of atomically precise clusters for a practical application with direct societal relevance.

利用分子精确纳米材料对水体污染物进行快速肉眼检测,已成为减少化学污染影响的一项前景广阔的策略。本研究提出了一种基于发光的砷(As)传感器,无需进行样品制备。该传感器由 Cu17 纳米团簇(Cu17NCs)组成,并由 l-半胱氨酸(l-Cys)和 1,2-双(二苯基膦)乙烷(DPPE)配体共同保护,具有红色发光的球状团簇组装超结构(CASs),对亚砷酸盐(As3+)和(As5+)离子具有显著的灵敏度。通过发光淬火,自来水中的检测限达到了 1 ppb。值得注意的是,它还能在 Cd2+、Hg2+、Fe3+、Pb2+、Cu2+ 和 Cr3+ 等常见干扰金属离子中选择性地检测砷。我们设计了一种由涂覆在聚丙烯(PP)无纺布垫上的 CASs 制成的传感器圆盘,用于实际现场应用。电子显微镜显示,由于砷的相互作用,球体的形态发生了破坏。此外,CAS 对革兰氏阴性大肠杆菌和革兰氏阳性金黄色葡萄球菌具有显著的抗菌效果,对枯草杆菌具有抗生物膜特性。这项研究凸显了原子级精确团簇在与社会直接相关的实际应用中的有效性。
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引用次数: 0
New Insights into the Mechanism of the UV/Sulfite Process: Formation of SO2•– Radicals and Their Derivatives under Acidic Conditions 紫外线/亚硫酸盐过程机理的新见解:酸性条件下二氧化硫自由基及其衍生物的形成
IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-26 DOI: 10.1021/acs.estlett.4c00251
Linghao Kong, Zhe Jin, Feng Zhu, Mengchang He, Feng Qian and Xianjia Peng*, 

The UV/sulfite process shows great potential for reductively degrading or eliminating pollutants. While its mechanism in neutral and alkaline environments has been well-elucidated, the reaction pathway under acidic conditions remains unclear. Herein, we report the novel findings of the formation of reductive SO2•– radicals and their derivatives in the UV/sulfite process at pH levels below 4. Mechanistic investigation revealed that H• radicals and SO3•– radicals formed by the photolysis of sulfite under acidic conditions, with the H• radicals being scavenged by sulfite to produce SO2•– radicals. Subsequently, these SO2•– radicals are transformed into dithionite, thiosulfate, hydrogen sulfide, and elemental sulfur through a series of intricate reactions. This study is expected to expand the potential application of the UV/sulfite process under acid conditions.

紫外线/亚硫酸盐工艺在还原降解或消除污染物方面显示出巨大的潜力。虽然其在中性和碱性环境中的机理已被充分阐明,但在酸性条件下的反应途径仍不清楚。在此,我们报告了在 pH 值低于 4 的紫外线/亚硫酸盐过程中形成还原性 SO2 自由基及其衍生物的新发现。机理研究发现,在酸性条件下亚硫酸盐光解形成 H- 自由基和 SO3--自由基,其中 H- 自由基被亚硫酸盐清除后生成 SO2--自由基。随后,这些 SO2--自由基通过一系列错综复杂的反应转化为二亚硫酸盐、硫代硫酸盐、硫化氢和元素硫。这项研究有望拓展紫外线/亚硫酸盐工艺在酸性条件下的潜在应用。
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引用次数: 0
Whale Baleen To Monitor Per- and Polyfluoroalkyl Substances (PFAS) in Marine Environments 用鲸须监测海洋环境中的全氟和多氟烷基物质 (PFAS)
IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-26 DOI: 10.1021/acs.estlett.4c0040910.1021/acs.estlett.4c00409
Matthew S. Savoca*, Anna R. Robuck, Michaela A. Cashman, Mark G. Cantwell, Lindsay C. Agvent, David N. Wiley, Rachel Rice, Sean Todd, Nicole E. Hunter, Jooke Robbins, Jeremy A. Goldbogen and Rainer Lohmann, 

Per- and polyfluoroalkyl substances (PFAS) comprise >10 000 synthetic compounds that are globally distributed and highly persistent but remain challenging to monitor. Here we assess the utility of baleen─an accreting, keratinaceous tissue that baleen whales use for filter-feeding─to track PFAS dynamics in marine food webs. In six species investigated, PFAS were detected in all baleen tested (n = 18 plates, 220 samples, ∑10PFAS range of 0.02–60.5 ng/g of dry weight), at levels higher than those of other tissue types besides liver. Three of the species in our data set had not been tested for PFAS contamination previously, and two of those species (blue whale and North Atlantic right whale) are internationally endangered species. Apparent links were observed between PFAS and life-history events by testing successive subsamples along the growth axis of the baleen plates. These results establish baleen as a viable sample matrix for assessing PFAS contamination in marine ecosystems by enabling multiyear time-series analyses through single-tissue sampling with seasonal resolution.

全氟烷基和多氟烷基物质(PFAS)包括 1 万种合成化合物,它们分布于全球各地,具有很强的持久性,但对它们的监测仍然具有挑战性。在这里,我们评估了须鲸的须膜(一种增生的角质组织,须鲸利用这种组织进行滤食)在跟踪海洋食物网中 PFAS 动态方面的作用。在所调查的六个物种中,所有检测到的须鲸组织中都检测到了 PFAS(n = 18 个平板,220 个样本,∑10PFAS 范围为 0.02-60.5 纳克/克干重),其水平高于除肝脏以外的其他组织类型。在我们的数据集中,有三个物种以前未检测过 PFAS 污染,其中两个物种(蓝鲸和北大西洋露脊鲸)是国际濒危物种。通过沿鲸须板生长轴连续检测子样本,可以观察到 PFAS 与生命史事件之间的明显联系。这些结果确立了须鲸作为评估海洋生态系统中 PFAS 污染的可行样本基质的地位,通过具有季节分辨率的单组织采样,实现了多年时间序列分析。
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引用次数: 0
Landfill Gas: A Major Pathway for Neutral Per- and Polyfluoroalkyl Substance (PFAS) Release 垃圾填埋气:中性全氟和多氟烷基物质 (PFAS) 释放的主要途径
IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-26 DOI: 10.1021/acs.estlett.4c00364
Ashley M. Lin, Jake T. Thompson, Jeremy P. Koelmel, Yalan Liu, John A. Bowden and Timothy G. Townsend*, 

The undisclosed and ubiquitous use of perfluoroalkyl and polyfluoroalkyl substances (PFAS) in consumer products has led to a growing issue of environmental pollution, particularly within the solid waste community, where the fate of volatile (neutral) PFAS in landfilled refuse is not well understood. Here, three municipal solid waste landfills in Florida were assessed for neutral PFAS in landfill gas and ionic PFAS in landfill leachate to compare the relative mobility between the two pathways. Landfill gas was directly sampled using a high volume, XAD-2 resin based sampling approach developed for adsorption and analysis of 27 neutral PFAS. Across sites, 13 neutral PFAS were identified from fluorotelomer alcohol (FTOH), fluorotelomer olefin (FTO), secondary FTOH, fluorotelomer acetate (FTOAc), and fluorotelomer methyl acrylate (FTMAc) classes; however, FTOHs dominated concentrations (87–97% total neutral PFAS), with most detections surpassing utilized calibration levels. Even under conservative assumptions, the mass of fluorine leaving in landfill gas (32–76%) was comparable to or greater than the mass leaving in landfill leachate (24–68%). These findings suggest that landfill gas, a less scrutinized byproduct, serves as a major pathway for the mobility of PFAS from landfills.

全氟烷基和多氟烷基物质 (PFAS) 在消费品中的未公开和普遍使用导致环境污染问题日益严重,尤其是在固体废物领域,人们对垃圾填埋场中挥发性(中性)PFAS 的去向还不甚了解。在此,我们对佛罗里达州的三个城市固体废物填埋场进行了评估,检测填埋气体中的中性全氟辛烷磺酸和填埋沥滤液中的离子全氟辛烷磺酸,以比较这两种途径之间的相对流动性。垃圾填埋场气体采用大容量、基于 XAD-2 树脂的采样方法直接采样,该方法是为吸附和分析 27 种中性全氟辛烷磺酸而开发的。在各个地点,从氟醚醇 (FTOH)、氟醚烯烃 (FTO)、仲氟醚醇 (FTOH)、氟醚醋酸酯 (FTOAc) 和氟醚丙烯酸甲酯 (FTMAc) 类别中鉴定出 13 种中性全氟辛烷磺酸;不过,氟醚醇的浓度占主导地位(占中性全氟辛烷磺酸总量的 87-97%),大多数检测结果都超过了使用的校准水平。即使按照保守的假设,垃圾填埋气中的氟残留量(32-76%)与垃圾填埋场渗滤液中的氟残留量(24-68%)相当或更大。这些研究结果表明,垃圾填埋气这一不太受关注的副产品是 PFAS 从垃圾填埋场迁移的主要途径。
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引用次数: 0
Control of Micropollutants in Water by Far-UVC Photolysis of Peracetic Acid 通过远紫外光分解过乙酸控制水中的微污染物
IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-25 DOI: 10.1021/acs.estlett.4c00384
Ran Yin*, Xinyi Ruan, Jiadong Peng, Jing Zhao, Yuliang Zhang, Arnaud Heuzard and Chii Shang, 

Increasing radical yields to reduce energy consumption for micropollutant degradation would make advanced oxidation processes more sustainable in the context of the United Nations’ Sustainable Development Goals and carbon neutrality. We herein demonstrate that switching the UV radiation source from conventional low-pressure UV (UV254) to far-UVC (UV222) increases the UV fluence-based concentration of hydroxyl radicals (HO) in the UV/peracetic acid (UV/PAA) process by 4.1-fold and 27.9-fold in deionized water and real surface water, respectively. Acetyloxyl radicals (CH3C(O)O) are generated in the UV222/PAA process at a steady-state concentration of 2.4 × 10–12 M in deionized water, while they are undetectable in the UV254/PAA process under the comparable conditions. The enhancement to radical production is mainly attributed to the 15.7-fold higher molar absorption coefficients of PAA0 at 222 nm than 254 nm (50 vs 3.5 M–1 cm–1), which suppresses the compromised 1.1-fold lower innate quantum yield at 222 nm than 254 nm (0.78 vs 0.86 mol einstein–1). The enhanced radical generation and direct photolysis promote the fluence-based degradation rate constants of bisphenol A, phenol, and nitrobenzene by 4.1-fold, 3.3-fold, and 2.9-fold in the UV222/PAA process than the UV254/PAA process.

在联合国可持续发展目标和碳中和的背景下,提高自由基产量以降低微污染物降解的能耗,将使高级氧化工艺更具可持续性。我们在本文中证明,将紫外线辐射源从传统的低压紫外线(UV254)切换到远紫外线(UV222)后,紫外线/过乙酸(UV/PAA)过程中基于紫外线通量的羟基自由基(HO-)浓度在去离子水和实际地表水中分别增加了 4.1 倍和 27.9 倍。UV222/PAA 过程中产生的乙酰氧基(CH3C(O)O-)在去离子水中的稳态浓度为 2.4 × 10-12 M,而在 UV254/PAA 过程中,在类似条件下检测不到乙酰氧基。自由基生成的增强主要归因于 PAA0 在 222 纳米波段的摩尔吸收系数比 254 纳米波段高 15.7 倍(50 对 3.5 M-1 cm-1),从而抑制了在 222 纳米波段比 254 纳米波段低 1.1 倍的先天量子产率(0.78 对 0.86 摩尔爱因斯坦-1)。与 UV254/PAA 工艺相比,UV222/PAA 工艺中增强的自由基生成和直接光解促进了双酚 A、苯酚和硝基苯的基于通量的降解速率常数,分别提高了 4.1 倍、3.3 倍和 2.9 倍。
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引用次数: 0
Response to Comment on “Size-Resolved Elemental Composition of Respiratory Particles in Three Healthy Subjects” 对 "三位健康受试者呼吸道粒子的尺寸分辨元素组成 "评论的回应
IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-25 DOI: 10.1021/acs.estlett.4c00484
Linsey C. Marr*, Zezhen Cheng, Weinan Leng, Swarup China and Aaron J. Prussin II, 
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引用次数: 0
Comment on “Size-Resolved Elemental Composition of Respiratory Particles in Three Healthy Subjects” 关于 "三名健康受试者呼吸道颗粒的尺寸分辨元素组成 "的评论
IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-25 DOI: 10.1021/acs.estlett.4c00243
Steven C. Hill*,  and , David C. Doughty*, 
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引用次数: 0
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