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Achieving cycling catalysis of electro-Fenton treatment 实现电-芬顿处理的循环催化
Pub Date : 2024-08-16 DOI: 10.1038/s44221-024-00284-9
Ming Chen, J. Paul Chen
The electro-Fenton process offers great potential for the treatment of contaminated water, but its industrial applications are limited due to a lack of electrocatalysts with effective cycling functionality. The electro-responsive catalyst enables continuous cycling of Fe(III)/Fe(II) species for electro-driven regeneration of the Fe(II) catalyst, leading to stable and efficient degradation of organic pollutants.
电-芬顿工艺在处理污染水方面具有巨大潜力,但由于缺乏具有有效循环功能的电催化剂,其工业应用受到限制。这种电反应催化剂能使铁(III)/铁(II)物种持续循环,从而实现铁(II)催化剂的电驱动再生,从而稳定、高效地降解有机污染物。
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引用次数: 0
Wastewater production footprint of conventional and unconventional oil and gas wells in North America 北美常规和非常规油气井的废水生产足迹
Pub Date : 2024-08-14 DOI: 10.1038/s44221-024-00286-7
Ashkan Zolfaghari, Joel Gehman, Andrew J. Kondash, Kurt O. Konhauser, Yong Sik Ok, Avner Vengosh, Daniel S. Alessi
Hydrocarbon recovery from conventional and unconventional wells, such as those using hydraulic fracturing (HF), generates substantial volumes of highly saline wastewater, known as flowback and produced water (FPW). Traditional evaluations of FPW management have focused on volume and chemical additives in HF fluids, neglecting variations in FPW volumetric production and salinity. Here we introduce two parameters to better assess the environmental impact of FPW: total produced salts (TPS), which accounts for both volume and salinity, and produced salts intensity, the ratio of TPS to the energy content of recovered hydrocarbons. Analysing a database of over 620,000 HF and conventional wells in North America, we found that more than 355 billion tonnes of salts were produced from 2005 to 2019, with HF wells contributing over 85%. Projections indicate that more than 1.5 trillion tonnes of salts will be produced by wells drilled between 2019 and 2050, predominantly from HF wells. TPS and produced salts intensity are crucial for assessing environmental risks, treatment costs and resource extraction potential, providing valuable metrics for regulators and planners. Recovering hydrocarbons from oil and gas wells results in highly saline wastewater, also known as flowback and produced water. The introduction of two parameters to estimate the environmental impact of these by-products, relative to energy produced, provides an important tool for assessing the risks associated with the planning and use of wells.
常规和非常规油井(如使用水力压裂法(HF)的油井)的碳氢化合物回收会产生大量高含盐废水,即回流水和生产水(FPW)。传统的 FPW 管理评估主要关注 HF 流体的体积和化学添加剂,而忽略了 FPW 体积产量和盐度的变化。在此,我们引入了两个参数,以更好地评估 FPW 对环境的影响:总产盐量(TPS)(同时考虑体积和盐度)和产盐强度(TPS 与回收碳氢化合物能量含量之比)。通过分析北美超过 62 万口高含盐量油井和常规油井的数据库,我们发现从 2005 年到 2019 年,盐的产量超过 3550 亿吨,其中高含盐量油井占 85% 以上。据预测,2019 年至 2050 年间钻探的油井将生产超过 1.5 万亿吨盐分,其中主要来自高频油井。TPS 和产盐强度对于评估环境风险、处理成本和资源开采潜力至关重要,为监管机构和规划人员提供了宝贵的衡量标准。从油气井中开采碳氢化合物会产生高含盐废水,也称为回流水和采出水。引入两个参数来估算这些副产品对环境的影响(相对于所生产的能源),为评估与油井规划和使用相关的风险提供了一个重要工具。
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引用次数: 0
Global inland-water nitrogen cycling has accelerated in the Anthropocene 人类世加速了全球内陆水域的氮循环
Pub Date : 2024-08-09 DOI: 10.1038/s44221-024-00282-x
Junjie Wang, Alexander F. Bouwman, Lauriane Vilmin, Arthur H. W. Beusen, Wim J. van Hoek, Xiaochen Liu, Jack J. Middelburg
Inland waters are an important component of the global nitrogen (N) cycle, functioning not only as land-to-sea transporters but also as active biogeochemical reactors. However, the latter role is not well understood regarding mechanisms, quantities or on a global scale. It remains unclear whether, when, how and why global inland-water biogeochemical N cycling has changed. Here we analyse the dynamic global inland-water N cycling processes in the Anthropocene by quantifying the long-term changes in different N forms, including their inputs to inland waters, transformation pathways, retention within inland waters, and river export to oceans. Using a spatially explicit, mechanistic, coupled hydrology and biogeochemistry model, we show that, during 1900–2010, the increase in total nitrogen (TN) river loading (from 27 to 68 Tg yr−1) resulted in an increase in TN export to oceans (from 20 to 42 Tg yr−1), despite an increase in inland-water retention (from 25% to 39%) primarily due to gaseous loss and burial. Moreover, the relative contributions of ammonium (NH4+), nitrate/nitrite (NOx−) and organic nitrogen (ON) changed because of threefold increases in global inland-water mineralization (transforming ON to NH4+) and N burial in sediments, a fourfold increase in nitrification (transforming NH4+ to NOx−) and a sixfold increase in denitrification (transforming NOx− to mainly N2). This Article presents a comprehensive analysis of the dynamic global inland-water N cycling processes using a coupled model of hydrology, nutrient loading and biogeochemical transformation, showing that N export increased more slowly than loading due to increased inland-water retention via enhanced transformation and burial.
内陆水域是全球氮(N)循环的重要组成部分,它不仅是陆地到海洋的运输工具,还是活跃的生物地球化学反应器。然而,人们对后者的作用机制、数量或在全球范围内的作用还不甚了解。目前仍不清楚全球内陆水体生物地球化学氮循环是否、何时、如何以及为何发生了变化。在此,我们通过量化不同氮形式的长期变化,包括其对内陆水域的输入、转化途径、在内陆水域的滞留以及向海洋的河流输出,分析了人类世全球内陆水域氮循环的动态过程。通过使用空间明确、机械耦合的水文和生物地球化学模型,我们发现在 1900-2010 年期间,尽管主要由于气态流失和掩埋,内陆水域的保留率有所提高(从 25% 提高到 39%),但河流总氮(TN)负荷的增加(从 27 吨/年增加到 68 吨/年)导致向海洋输出的 TN 增加(从 20 吨/年增加到 42 吨/年)。此外,铵(NH4+)、硝酸盐/亚硝酸盐(NOx-)和有机氮(ON)的相对贡献也发生了变化,这是因为全球内陆水矿化(将ON转化为NH4+)和沉积物中氮埋藏量增加了三倍,硝化(将NH4+转化为NOx-)增加了四倍,反硝化(将NOx-主要转化为N2)增加了六倍。本文利用水文、营养物质负荷和生物地球化学转化的耦合模型,对全球内陆水体氮的动态循环过程进行了全面分析,结果表明,由于转化和掩埋作用增强,内陆水体的氮截留量增加,氮出口量的增加速度比负荷量的增加速度要慢。
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引用次数: 0
It’s too soon to stop studying the potential effects of PFAS on human health 停止研究全氟辛烷磺酸对人类健康的潜在影响为时尚早
Pub Date : 2024-08-09 DOI: 10.1038/s44221-024-00294-7
Jamie C. DeWitt
Despite positive signs regarding the decreasing presence of specific PFAS in the blood of sampled humans, we do not know enough about this broad class of substances to justify stopping research on their toxicity.
尽管出现了一些积极的迹象,表明特定全氟辛烷磺酸在采样人体血液中的含量有所下降,但我们对这一大类物质的了解还不够,因此没有理由停止对其毒性的研究。
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引用次数: 0
Designing membranes with specific binding sites for selective ion separations 设计具有特定结合位点的膜,实现选择性离子分离
Pub Date : 2024-08-08 DOI: 10.1038/s44221-024-00279-6
Camille Violet, Akash Ball, Mohammad Heiranian, Luis Francisco Villalobos, Junwei Zhang, Betul Uralcan, Heather Kulik, Amir Haji-Akbari, Menachem Elimelech
A new class of membranes that can separate ions of similar size and charge is highly desired for resource recovery, water reuse and energy storage technologies. These separations require membrane nanochannels with simultaneous ångström-scale confinement and ion-selective binding sites. Conventional membrane material design uses continuous, volume-averaged properties that cannot account for discrete chemical interactions between ions and binding sites. In this Perspective, we present a design framework for ultraselective membranes by describing how to select and incorporate ion-specific binding sites into membrane nanochannels. We begin by discussing how the chemical features of ions, functional groups and solvents impact ion-binding energy. We then describe the role of binding energy in selective ion transport through nanochannels and discuss the critical importance of intersite spacing. Subsequently, we draw inspiration from machine learning methods used for drug discovery and suggest a similar approach to identify functional groups with optimal ion-binding affinity. We conclude by outlining synthetic methods to incorporate ion-specific binding sites into prevalent nanostructured materials such as covalent organic frameworks, metal–organic frameworks, two-dimensional materials and polymers. This Perspective proposes a way to design membranes to separate ions of similar size and charge with a view to their use in resource recovery, water reuse and energy storage technologies.
资源回收、中水回用和能源存储技术非常需要一种能够分离大小和电荷相近的离子的新型膜。这些分离要求膜纳米通道同时具有盎司尺度的封闭性和离子选择性结合位点。传统的膜材料设计采用连续、体积平均的特性,无法考虑离子与结合位点之间离散的化学作用。在本视角中,我们介绍了超选择性膜的设计框架,描述了如何选择离子特异性结合位点并将其纳入膜纳米通道。我们首先讨论了离子、官能团和溶剂的化学特征如何影响离子结合能。然后,我们描述了结合能在纳米通道选择性离子传输中的作用,并讨论了位点间距的关键重要性。随后,我们从用于药物发现的机器学习方法中汲取灵感,提出了一种类似的方法来识别具有最佳离子结合亲和力的功能基团。最后,我们概述了在共价有机框架、金属有机框架、二维材料和聚合物等常见纳米结构材料中加入离子特异性结合位点的合成方法。
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引用次数: 0
Metal oxyhalide-based heterogeneous catalytic water purification with ultralow H2O2 consumption 超低 H2O2 消耗量的金属氧卤化物基异相催化水净化技术
Pub Date : 2024-08-08 DOI: 10.1038/s44221-024-00281-y
Ying-Jie Zhang, Jia-Shu Tao, Yi Hu, Gui-Xiang Huang, Yuan Pan, Wen-Wei Li, Jie-Jie Chen, Han-Qing Yu
In the quest for advanced water treatment via Fenton and Fenton-like reactions, minimizing the hydrogen peroxide (H2O2) usage by improving its activation efficiency is a critical goal. Here we report a metal oxyhalide (MOX)-based Fenton reaction system that differs fundamentally from traditional ones in pollutant removal pathway and mechanism. The MOX/H2O2 system enables efficient coupling and polymerization of organic pollutants via mild surface direct oxidation, bypassing the generation of reactive oxygen species. As a result, pollutants are translocated and removed from water with ultralow H2O2 consumption, avoiding the formation of toxic by-products. It achieves up to 80% pollutant (50% total organic carbon) removal at a H2O2-to-pollutants molar ratio of 2:1, outperforming conventional Fenton systems, which are operated at ratios ranging from 20:1 to 1,000:1. The success of these catalytic systems is attributed to the synergistic actions of O-bridging M and X sites on the catalyst surface, which selectively activate pollutants and H2O2, respectively. The catalyst could be extended to low-cost and environmentally benign MOX materials such as BiOI, FeOCl and VOCl, and be adopted to construct a dynamic membrane filtration catalytic system for high-performance and energy-saving abatement of micropollutants in water, providing a promising water purification paradigm. Traditional Fenton and Fenton-like reactions for pollutant removal require a substantial amount of H2O2. In contrast, the heterogeneous metal oxyhalide-based Fenton catalytic approach achieves organic pollutant removal by concentrating and activating them on the catalyst, significantly minimizing H2O2 consumption.
在寻求通过芬顿和类芬顿反应进行先进水处理的过程中,通过提高过氧化氢(H2O2)的活化效率最大限度地减少其用量是一个关键目标。在此,我们报告了一种基于金属氧卤化物(MOX)的芬顿反应系统,该系统在污染物去除途径和机理方面与传统的芬顿反应系统有着本质区别。MOX/H2O2 系统通过温和的表面直接氧化作用,绕过活性氧的生成,实现了有机污染物的高效耦合和聚合。因此,污染物从水中转移和清除的 H2O2 消耗量极低,避免了有毒副产品的形成。当 H2O2 与污染物的摩尔比为 2:1 时,它的污染物(50% 总有机碳)去除率高达 80%,优于传统的 Fenton 系统,后者的比率从 20:1 到 1,000:1 不等。这些催化系统的成功归功于催化剂表面的 O 桥 M 位点和 X 位点的协同作用,它们分别选择性地激活污染物和 H2O2。该催化剂可推广到 BiOI、FeOCl 和 VOCl 等低成本、对环境无害的 MOX 材料上,并可用于构建动态膜过滤催化系统,以高性能、节能地去除水中的微污染物,提供一种前景广阔的水净化范例。
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引用次数: 0
Elemental sulfur–siderite composite filler empowers sustainable tertiary treatment of municipal wastewater even at an ultra-low temperature of 7.3 °C 元素硫-菱铁矿复合填料即使在 7.3 °C 的超低温条件下也能对城市污水进行可持续的三级处理
Pub Date : 2024-08-02 DOI: 10.1038/s44221-024-00285-8
Qi Zhao, Luyao Wang, Tipei Jia, Xiyao Li, Qiong Zhang, Yongzhen Peng
Tertiary treatment, the ‘polisher’ for wastewater nutrients, has assumed an increasingly greater role in municipal wastewater treatment plants, particularly given the growing demands for wastewater treatment worldwide and more stringent discharge standards. However, most municipal wastewater treatment plants in service use first-generation tertiary treatment processes (for example, additional carbon source-dependent denitrification and chemical dephosphorization), raising significant sustainability concerns. For effective, yet sustainable nutrient polishing, we develop an elemental sulfur (S0)–siderite composite filler (S0SCF) using a melting–embedding strategy based on the liquid immersion granulation technique. As a prerequisite for engineering use, S0SCF overcomes the poor mechanical properties and safety concerns plaguing traditional S0-based reactive fillers. S0SCF inherits efficient S0-driven autotrophic denitrification and acquires an effective dephosphorization capability, with the dephosphorization mechanism linked to S0-driven autotrophic denitrification-induced Fe2+ leaching from siderite and subsequent Fe2+–PO43− coprecipitation. During ultra-low temperature tests (7.3 ± 0.3 °C), the S0SCF-packed bed bioreactor demonstrated robust removal rates for NOx− (NO3− and NO2−) (0.29 ± 0.02 kg N m−3 per day) and PO43− (0.014 ± 0.004 kg P m−3 per day), with removal efficiencies reaching 91.2 ± 3.2% and 81.4 ± 7.8%, respectively. Meanwhile, the low levels of nitrous oxide emissions and free sulfide generation further highlight the sustainability implications of S0SCF-based nutrient polishing. This work sheds fresh light on developing low-carbon and eco-friendly tertiary treatment processes, taking a necessary step towards addressing the sustainability crisis in the wastewater treatment sector. Tertiary treatment in wastewater treatment plants serves as the final barrier against the discharge of nutrients into natural waters but requires large inputs of chemical agents. An elemental sulfur–siderite composite filler demonstrates efficient and sustainable denitrification and dephosphorization, even at ultra-low temperatures.
三级处理是废水营养物质的 "抛光剂",在城市污水处理厂中发挥着越来越重要的作用,特别是考虑到全球对污水处理的需求不断增长,排放标准也更加严格。然而,大多数投入使用的城市污水处理厂使用的是第一代三级处理工艺(例如,依赖碳源的额外反硝化和化学除磷),这引起了人们对可持续发展的极大关注。为了实现有效且可持续的营养抛光,我们开发了一种元素硫(S0)-菱镁矿复合填料(S0SCF),采用基于液态浸泡造粒技术的熔融-嵌入策略。作为工程应用的先决条件,S0SCF 克服了困扰传统 S0 反应填料的机械性能差和安全问题。S0SCF 继承了 S0 驱动的高效自养反硝化作用,并获得了有效的脱磷能力,其脱磷机制与 S0 驱动的自养反硝化作用引起的菱铁矿中 Fe2+ 浸出和随后的 Fe2+-PO43- 共沉淀有关。在超低温试验中(7.3 ± 0.3 °C),S0SCF-堆积床生物反应器对氮氧化物(NO3- 和 NO2-)(每天 0.29 ± 0.02 千克 N m-3)和 PO43-(每天 0.014 ± 0.004 千克 P m-3)的去除率很高,去除效率分别达到 91.2 ± 3.2% 和 81.4 ± 7.8%。同时,氧化亚氮的排放量和游离硫化物的生成量都很低,这进一步凸显了基于 S0SCF 的营养液抛光技术的可持续发展意义。这项研究为开发低碳环保的三级处理工艺提供了新的思路,为解决污水处理领域的可持续发展危机迈出了必要的一步。
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引用次数: 0
Hotspots of irrigation-related US greenhouse gas emissions from multiple sources 与灌溉相关的美国温室气体多源排放热点
Pub Date : 2024-08-01 DOI: 10.1038/s44221-024-00283-w
Avery W. Driscoll, Landon T. Marston, Stephen M. Ogle, Noah J. Planavsky, Md Abu Bakar Siddik, Shannon Spencer, Shuang Zhang, Nathaniel D. Mueller
Irrigation effectively increases yields and buffers against intensifying climatic stressors to crop productivity but also produces greenhouse gas (GHG) emissions through several pathways including energy use for pumping (on farm and for interbasin water transfers), N2O emissions from increased denitrification under elevated soil moisture, and degassing of groundwater supersaturated in CO2. Despite irrigation’s climate adaptation potential, associated GHG emissions remain unquantified. Here we conduct a comprehensive, county-level assessment of US GHG emissions from these irrigation-related pathways, estimating that irrigation produces 18.9 MtCO2e annually (95% confidence interval 15.2–23.5 Mt), with 12.6 Mt from on-farm pumping, 1.1 Mt from pumping for interbasin transfers, 2.9 Mt from elevated N2O and 2.4 Mt from groundwater degassing. These emissions are highly spatially concentrated, revealing opportunities for geographically targeted and source-specific GHG mitigation actions. These findings enable strategic consideration of GHG emissions in decision-making associated with irrigation expansion for climate adaptation. Despite its utility for climate change adaptation, US irrigation produces 18.9 MtCO2e yr−1 from groundwater degassing, elevated N2O and energy use. This county-level analysis reveals opportunities for geographically targeted emissions mitigation.
灌溉可有效提高产量,缓冲气候对作物生产率造成的日益加剧的压力,但也会通过多种途径产生温室气体(GHG)排放,包括抽水(农田抽水和流域间调水)的能源消耗、土壤水分升高导致的反硝化作用增加所产生的一氧化二氮排放,以及二氧化碳过饱和地下水的脱气。尽管灌溉具有气候适应潜力,但相关的温室气体排放仍未量化。在此,我们对这些灌溉相关途径产生的美国温室气体排放进行了全面的县级评估,估计灌溉每年产生 1890 万吨 CO2e(95% 置信区间为 15.2-23.5 万吨),其中 1260 万吨来自农场抽水,110 万吨来自流域间调水,290 万吨来自 N2O 升高,240 万吨来自地下水脱气。这些排放在空间上高度集中,揭示了采取有地理针对性和特定来源的温室气体减排行动的机会。这些发现有助于在与扩大灌溉以适应气候相关的决策中对温室气体排放进行战略性考虑。
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引用次数: 0
Author Correction: Simultaneous time-resolved inorganic haloamine measurements enable analysis of disinfectant degradation kinetics and by-product formation 作者更正:同步时间分辨无机卤胺测量可分析消毒剂降解动力学和副产品的形成
Pub Date : 2024-08-01 DOI: 10.1038/s44221-024-00295-6
Samuel H. Brodfuehrer, Daniel C. Blomdahl, David G. Wahman, Gerald E. Speitel Jr., Pawel K. Misztal, Lynn E. Katz
{"title":"Author Correction: Simultaneous time-resolved inorganic haloamine measurements enable analysis of disinfectant degradation kinetics and by-product formation","authors":"Samuel H. Brodfuehrer, Daniel C. Blomdahl, David G. Wahman, Gerald E. Speitel Jr., Pawel K. Misztal, Lynn E. Katz","doi":"10.1038/s44221-024-00295-6","DOIUrl":"10.1038/s44221-024-00295-6","url":null,"abstract":"","PeriodicalId":74252,"journal":{"name":"Nature water","volume":"2 10","pages":"1038-1038"},"PeriodicalIF":0.0,"publicationDate":"2024-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s44221-024-00295-6.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142451324","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Frozen water on Earth 地球上的冰冻水
Pub Date : 2024-07-23 DOI: 10.1038/s44221-024-00287-6
The shrinking cryosphere demands collaborative and inclusive approaches to improve our knowledge of its dynamics amidst climate change.
不断缩小的冰冻圈要求我们采取协作和包容的方法,以增进我们对气候变化中冰冻圈动态的了解。
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引用次数: 0
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Nature water
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