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Highly efficient metal-free nitrate reduction enabled by electrified membrane filtration 电动膜过滤实现高效无金属硝酸盐还原
Pub Date : 2024-07-04 DOI: 10.1038/s44221-024-00278-7
Yingzheng Fan, Xiaoxiong Wang, Claire Butler, Amma Kankam, Abdessamad Belgada, Julia Simon, Yuanzuo Gao, Eric Chen, Lea R. Winter
Current methods for electrocatalytic destruction of nitrate in drinking water require metal catalysts to achieve sufficient nitrate removal. However, metal-based catalysts involve complicated synthesis, increase treatment costs and can lead to leaching of metals into treated water. Here we achieved nitrate reduction performance comparable to that of metal-based catalysts via electrofiltration through a metal-free nanoporous electrified membrane (EM) containing unmodified pristine carbon nanotubes (CNTs). Experimental results coupled with computational fluid dynamics simulations elucidated how the decreased diffusion boundary layer in the flow-through CNT-EM mitigates diffusion limitations to enhance overall nitrate reaction activity. Furthermore, defects in CNTs were identified as the catalytic active sites by comparing the activity of EMs containing acid-treated metal-free CNTs and CNTs with added defects. Through density functional theory and molecular dynamics calculations, we demonstrated enhanced *NO2 and *NO adsorption energies at intrinsic defect sites, which are present in most commercial CNTs and become more accessible to nitrate ions under flow-through operation. Finally, the long-term stability, tolerance of environmental interferences, and sufficient nitrate removal and scalability to meet drinking water standards were demonstrated in real surface water, exhibiting the outstanding performance of the metal-free CNT-EM for practical applications. By elucidating how nanoporous electrofiltration enables dynamic matching of reaction and transport rates, this study demonstrates a new strategy to drastically improve electrocatalytic reaction performance without complex catalyst materials innovation, bridging existing gaps for nitrate removal in drinking water treatment related to the use of metal-based catalysts. Current methods for electrocatalytic destruction of nitrate in drinking water require metal catalysts to achieve sufficient nitrate removal. Electrified membranes containing pristine carbon nanotubes operated under flow-through mode provide an alternative approach for efficient nitrate reduction without the use of metals.
目前,饮用水中硝酸盐的电催化破坏方法需要使用金属催化剂才能充分去除硝酸盐。然而,金属催化剂涉及复杂的合成,会增加处理成本,并可能导致金属渗入处理过的水中。在这里,我们通过含有未经改性的原始碳纳米管(CNTs)的无金属纳米多孔电化膜(EM)进行电过滤,实现了与金属催化剂相当的硝酸盐还原性能。实验结果与计算流体动力学模拟相结合,阐明了流动的 CNT-EM 中扩散边界层的减少如何缓解扩散限制,从而提高整体硝酸盐反应活性。此外,通过比较含有经酸处理的无金属 CNT 和添加了缺陷的 CNT 的 EM 的活性,确定了 CNT 中的缺陷是催化活性位点。通过密度泛函理论和分子动力学计算,我们证明了内在缺陷位点的*NO2 和*NO 吸附能增强,这些缺陷位点存在于大多数商用 CNT 中,在流动操作下更容易被硝酸根离子吸附。最后,研究人员在实际地表水中演示了这种无金属 CNT-EM 的长期稳定性、对环境干扰的耐受性、足够的硝酸盐去除率以及满足饮用水标准的可扩展性,从而展示了其在实际应用中的卓越性能。通过阐明纳米多孔电过滤如何实现反应和传输速率的动态匹配,本研究展示了一种无需创新复杂催化剂材料就能大幅提高电催化反应性能的新策略,弥补了饮用水处理中与使用金属基催化剂有关的硝酸盐去除方面的现有差距。
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引用次数: 0
Rising food and water insecurity among US children 美国儿童的食物和水不安全问题日益严重
Pub Date : 2024-07-02 DOI: 10.1038/s44221-024-00267-w
J. Tom Mueller
Concurrent food and water insecurity doubled among children from 2005 to 2020, with minoritized children facing far more insecurity than their white counterparts.
从 2005 年到 2020 年,儿童同时面临的粮食和水不安全问题增加了一倍,少数族裔儿童面临的不安全问题远远高于白人儿童。
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引用次数: 0
Electro-driven cycling Fenton catalysis through two-dimensional electroresponsive metal–organic frameworks for water purification 通过二维电响应金属有机框架进行电驱动循环芬顿催化,实现水净化
Pub Date : 2024-07-01 DOI: 10.1038/s44221-024-00262-1
Chao Yang, Shanshan Shang, Lin Lin, Pei Wang, Zhihong Ye, Yixuan Wang, Kaimin Shih, Lianpeng Sun, Xiao-yan Li
The electro-Fenton process is a promising technology for eliminating emerging organic pollutants from water. However, its potential is hindered by the lack of cathode materials with the essential cycling catalytic functionality for sustained Fenton reactions. In this study, we developed an innovative catalytic cathode comprising a two-dimensional electroresponsive ferrocene metal–organic framework (ER-Fc-MOF) for effective H2O2 activation in a reagent-free dual-cathode electro-Fenton process. The ER-Fc-MOF cathode also enables the electro-driven regeneration of the Fe(II) sites through direct electron transfer within the ferrocene sandwich structure, achieving continuous cycling of the Fc+-Fe(III)/Fc-Fe(II) species for Fenton reactions. Electron paramagnetic resonance and quenching tests confirmed that the ER-Fc-MOF catalytic cathode generates both radical (HO·) and non-radical (1O2) species for highly efficient degradation of organic pollutants across a broad pH range in diverse water matrices. This novel electroresponsive cycling catalyst for the electro-Fenton process presents a promising route towards the development of green and sustainable oxidation technologies for water purification and wastewater treatment. Electro-Fenton treatment holds great promise as an advanced oxidation process for removing emerging organic pollutants, but achieving sustained Fenton reactions remains a challenge. An electroresponsive ferrocene metal–organic framework cathode now enables continuous cycling of the catalytic species for Fenton reactions and achieves efficient water purification.
电-芬顿工艺是一种消除水中新出现的有机污染物的前景广阔的技术。然而,由于缺乏具有持续芬顿反应所必需的循环催化功能的阴极材料,该技术的潜力受到了阻碍。在本研究中,我们开发了一种创新的催化阴极,由二维电响应二茂铁金属有机框架(ER-Fc-MOF)组成,可在无试剂双阴极电-芬顿过程中有效激活 H2O2。ER-Fc-MOF 阴极还能通过二茂铁夹层结构内的直接电子传递实现铁(II)位点的电驱动再生,从而实现 Fc+-Fe(III)/Fc-Fe(II) 物种在芬顿反应中的连续循环。电子顺磁共振和淬灭试验证实,ER-Fc-MOF 催化阴极可产生自由基(HO-)和非自由基(1O2)物种,在各种水基质中的宽 pH 值范围内高效降解有机污染物。这种用于电-芬顿过程的新型电反应循环催化剂为开发用于水净化和废水处理的绿色可持续氧化技术提供了一条前景广阔的途径。
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引用次数: 0
Accelerating Antarctic research amid rapid changes 在快速变化中加速南极研究
Pub Date : 2024-07-01 DOI: 10.1038/s44221-024-00266-x
Lettie A. Roach
We must prioritize diversity, scientific communication and team-based science to keep up with rapid Antarctic ice and climate change.
我们必须优先考虑多样性、科学交流和以团队为基础的科学,以跟上南极冰川和气候变化的快速发展。
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引用次数: 0
MnO2-modified activated carbon and granular nano-TiO2 in tandem succeed in treating domestic well water arsenic at point of use 二氧化锰改性活性炭和颗粒纳米二氧化钛串联使用,成功处理了家用井水中的砷
Pub Date : 2024-06-24 DOI: 10.1038/s44221-024-00268-9
Yanhua Duan, Yuqin Sun, Alejandro Palomo, Zengyi Li, Baoling Yang, Qiantao Shi, Derek Z. Zhang, Qiang Yang, Xiaoguang Meng, Yan Zheng
Globally, millions of rural households that use groundwater for drinking are exposed to inorganic arsenic, frequently as arsenite (As(III)). Crucial for health protection, adsorption-based treatment works well for arsenate (As(V)) but not for slower-adsorbing As(III). Liquid oxidants, though impractical for point of use, are widely used to pre-oxidize As(III) to As(V) in point-of-entry treatment for better performance and cost saving. Here MnO2-modified activated carbon, a solid oxidant, was integrated into a point-of-use system with granular nano-TiO2 as the main adsorbent for two real-world tests, supplying As-safe water at less than US$0.01 l−1. One 4-month deployment treated 4,200 bed volumes (~2.1 m3) of groundwater with 69 ± 16 μg l−1 As (78 ± 5% As(III)). Another 28-month deployment treated 10,000 bed volumes (~5.0 m3) of groundwater with 42 ± 21 μg l−1 As (33 ± 21% As(III)). Interactions between the groundwater matrix and filter media affect performance, highlighting the need to verify household As removal technologies through long-term deployments. Drinking well water with unsafe levels of arsenic is a considerable public health concern, and conventional point-of-use (POU) treatment often falls short in real-world household utilizations. Integrating a solid oxidant into the POU system has proven to be a successful strategy through long-term field deployment, ensuring drinking-water safety.
在全球范围内,数百万使用地下水饮用的农村家庭接触到无机砷,通常是亚砷酸盐(As(III))。吸附式处理对健康保护至关重要,它对砷酸盐(As(V))效果良好,但对吸附速度较慢的 As(III) 却效果不佳。液体氧化剂虽然在使用点上不切实际,但在入口点处理中被广泛用于将 As(III)预氧化为 As(V),以获得更好的性能并节约成本。在这里,二氧化锰改性活性炭(一种固体氧化剂)与粒状纳米二氧化钛(作为主要吸附剂)被整合到一个使用点系统中,进行了两次实际测试,以低于 0.01 美元/升的价格供应 As-safe 水。其中一次为期 4 个月的部署处理了 4,200 个床体积(约 2.1 立方米)的地下水,As 含量为 69 ± 16 μg l-1 (78 ± 5% As(III))。另一个为期 28 个月的部署处理了 10,000 个床层(约 5.0 立方米)的地下水,As 含量为 42 ± 21 μg l-1 (33 ± 21% As(III))。地下水基质和过滤介质之间的相互作用会影响其性能,因此需要通过长期部署来验证家用砷去除技术。
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引用次数: 0
Taking selectivity to a new high 将选择性提升到新高度
Pub Date : 2024-06-21 DOI: 10.1038/s44221-024-00271-0
The ideal sharp cutoff of solutes by a porous membrane is not achievable yet. Prolonging the interactions between solutes and pores in isoporous membranes pushes the precise separation abilities further.
多孔膜还无法实现理想的溶质截流。延长等孔膜中溶质与孔之间的相互作用时间,可以进一步提高精确分离能力。
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引用次数: 0
Pushing the limits of size selectivity in nanoscale solute separations 突破纳米级溶质分离中尺寸选择性的极限
Pub Date : 2024-06-20 DOI: 10.1038/s44221-024-00252-3
Feng Gao, Wen Chen, Jamila G. Eatman, Ruben Z. Waldman, Nestor J. Zaluzec, Ruilin Dong, Paul F. Nealey, Seth B. Darling
Transport of a spherical solute through a cylindrical pore has been modelled for decades using well-established hindered transport theory, predicting solutes with a size smaller than the pore to be rejected nonetheless because of convective and diffusive hindrance; this rejection mechanism prevents extremely sharp solute separations by a membrane. Whereas the model has been historically verified, solute transport through near-perfect isoporous membranes may finally overcome this limitation. Here encouraging solute rejections are achieved using nanofabricated, defect-free silicon nitride isoporous membranes. The membrane is challenged by a recirculated feed to increase the opportunity for interactions between solutes and the pore array. Results show the membrane completely reject solutes with greater size than the pore size while effectively allowing smaller solutes to permeate through. With effectively increasing the number of interactions, we propose that a steeper size-selective rejection curve may be achieved. With this traditional hurdle overcome, there is new promise for unprecedented membrane separations through judicious process design and extremely tight pore-size distributions. Membrane separations are foundational to water treatment processes, and the traditional solute transport theory is limited in predicting the sharp separation of solutes by a membrane. By the proper design of the porous membranes and filtration processes, a sharp rejection curve may be achieved using isoporous membranes with an infinite number of interactions between solutes and membranes.
几十年来,球形溶质通过圆柱形孔隙的传输一直是利用成熟的受阻传输理论来模拟的,该理论预测,由于对流和扩散阻碍,尺寸小于孔隙的溶质仍会被排斥;这种排斥机制阻止了膜对溶质的极度分离。虽然该模型已在历史上得到验证,但通过近乎完美的等孔膜进行溶质传输可能最终会克服这一限制。在这里,使用纳米制造的无缺陷氮化硅等孔膜实现了令人鼓舞的溶质分离。膜受到循环进料的挑战,以增加溶质与孔阵列之间相互作用的机会。结果表明,膜能完全阻挡尺寸大于孔径的溶质,同时有效地允许较小的溶质通过。通过有效增加相互作用的数量,我们建议可以实现更陡峭的尺寸选择性排斥曲线。在克服了这一传统障碍后,通过合理的工艺设计和极其严格的孔径分布,有望实现前所未有的膜分离。膜分离是水处理过程的基础,而传统的溶质传输理论在预测膜对溶质的急剧分离方面是有限的。通过对多孔膜和过滤过程的合理设计,可以利用溶质与膜之间无限多的相互作用,使用等孔膜实现锐利的剔除曲线。
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引用次数: 0
Perfecting size-selective membrane separations 完善尺寸选择性膜分离技术
Pub Date : 2024-06-20 DOI: 10.1038/s44221-024-00260-3
Anthony P. Straub
Porous membranes struggle to achieve tight size exclusion. Membranes with uniform pore sizes and flow regimes that maximize interactions offer a path to unprecedented selectivity.
多孔膜难以实现严格的尺寸排除。具有均匀孔径和最大化相互作用的流动机制的膜为实现前所未有的选择性提供了途径。
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引用次数: 0
Viral metagenome reveals microbial hosts and the associated antibiotic resistome on microplastics 病毒元基因组揭示微塑料上的微生物宿主及相关抗生素耐药性基因组
Pub Date : 2024-06-14 DOI: 10.1038/s44221-024-00249-y
Ruilong Li, Xin-Li An, Yijin Wang, Zhugen Yang, Jian-Qiang Su, Jonathan Cooper, Yong-Guan Zhu
Microplastics provide a unique niche for viruses, promoting viral interactions with hosts and accelerating the rapid ‘horizontal’ spread of antibiotic resistance genes (ARGs). Currently, however, there is a lack of knowledge concerning the main drivers for viral distribution on microplastics and on the resulting patterns of viral biogeographic distributions and the spread of the associated ARGs. Here we performed metagenomic and virus enrichment-based viromic sequencings on both polyethylene and polypropylene microplastics along a river. Experimental results show that Proteobacteria, Firmicutes, Actinobacteria and Cyanobacteria were the potential hosts of viruses on microplastics, but only approximately 4.1% of viral variations were associated with a bacterial community. Notably, two shared ARGs and six metal resistance genes were identified in both viral and their host bacterial genomes, indicating the occurrence of horizontal gene transfer between viruses and bacteria. Furthermore, microplastics introduce more distinctive elements to viral ecology, fostering viral diversification and virus–host linkage while refraining from an escalated level of horizontal gene transfer of ARGs in contrast to natural matrixes. Our study provides comprehensive profiles of viral communities, virus-related ARGs and their driving factors on microplastics, highlighting how these anthropogenic niches provide unique interfaces that comprise highly defined viral ecological features in the environment. The combination of metagenome and virus-enriched virome sequencing provides comprehensive profiles of viral communities and their associated antibiotic resistance genes and reveals the factors driving changes in the plastisphere.
微塑料为病毒提供了一个独特的生存环境,促进了病毒与宿主的相互作用,并加速了抗生素抗性基因(ARGs)的快速 "水平 "传播。然而,目前人们对微塑料上病毒分布的主要驱动因素、由此产生的病毒生物地理分布模式以及相关 ARGs 的传播还缺乏了解。在此,我们对河流沿岸的聚乙烯和聚丙烯微塑料进行了元基因组学和基于病毒富集的病毒组测序。实验结果表明,变形菌、固着菌、放线菌和蓝细菌是微塑料上病毒的潜在宿主,但只有约 4.1% 的病毒变异与细菌群落有关。值得注意的是,在病毒及其宿主细菌基因组中发现了两个共享的ARGs和六个抗金属基因,这表明病毒和细菌之间存在水平基因转移。此外,微塑料还为病毒生态学引入了更多独特的元素,促进了病毒的多样化和病毒-宿主联系,同时与自然基质相比,ARGs 的水平基因转移没有升级。我们的研究提供了微塑料上病毒群落、与病毒相关的ARGs及其驱动因素的综合概况,强调了这些人为壁龛如何提供独特的界面,构成环境中高度确定的病毒生态特征。元基因组测序与富集病毒的病毒组测序相结合,提供了病毒群落及其相关抗生素耐药基因的全面概况,并揭示了驱动塑界变化的因素。
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引用次数: 0
Microplastics, microfibres and marine snows 微塑料、微纤维和海雪
Pub Date : 2024-06-13 DOI: 10.1038/s44221-024-00263-0
Tamara S. Galloway, Adam Porter
A digital method of studying the dynamic behaviours of marine and lake snows in the water column will help to speed up investigations of their behaviour and of the ecological impact of microplastics and microfibres in water bodies.
研究海雪和湖雪在水体中的动态行为的数字化方法将有助于加快对它们的行为以及微塑料和微纤维在水体中的生态影响的研究。
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引用次数: 0
期刊
Nature water
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