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Stronger biogeographical pattern of bacterioplankton communities than biofilm communities along a riverine ecosystem: a local scale study of the Kaidu river in the arid and semi-arid northwest of China. 沿河生态系统中浮游细菌群落的生物地理格局强于生物膜群落:对中国西北干旱半干旱地区开都河的局部尺度研究。
IF 7.7 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-11-04 DOI: 10.1016/j.envres.2024.120294
Yang Hu, Yifu Song, Jian Cai, Jianying Chao, Yi Gong, Xingyu Jiang, Keqiang Shao, Xiangming Tang, Guang Gao

Although the biogeographical pattern and mechanisms underlying microbial assembly have been well-explored in lentic ecosystems, the relevant scenarios in lotic ecosystems remain poorly understood. By sequencing the bacterial communities in bacterioplankton and biofilm, our study detected their distance-decay relationship (DDR), and the balance between deterministic and stochastic processes, along the Kaidu river in an arid and semi-arid region of northwest China. Our results revealed that bacterioplankton and biofilm had significantly contrasting community structures. The bacterioplankton communities showed a gradually decreasing trend in alpha-diversity from the headwater to the river mouth, contrasting with the alpha-diversity of biofilm communities which was constant along the river length. Both bacterioplankton and biofilm showed significant DDRs along the 500-km river corridor with the slope of the bacterioplankton DDR being steeper than that of the biofilm DDR, which implies a stronger biogeography of bacterioplankton than biofilm. Relative to biofilm communities, the species interactions formed a denser and more complex network in the bacterioplankton communities than in the biofilm communities. Our results also revealed that there was a transition of community assembly from deterministic to stochastic processes upstream to downstream, although both the bacterioplankton and biofilm communities were mainly regulated by deterministic processes within the entire river. All these empirical results expand our knowledge of microbial ecology in an arid and semi-arid lotic ecosystem.

尽管人们已经对借水生态系统的生物地理格局和微生物集结的内在机制进行了深入探讨,但对地段生态系统的相关情况仍然知之甚少。通过对浮游细菌和生物膜中的细菌群落进行测序,我们的研究检测了中国西北干旱和半干旱地区开都河沿岸细菌群落的距离-衰减关系(DDR),以及确定性过程和随机过程之间的平衡。我们的研究结果表明,浮游细菌和生物膜的群落结构具有明显的反差。从源头到河口,浮游细菌群落的α-多样性呈逐渐降低的趋势,而生物膜群落的α-多样性在整个河段保持不变。在 500 公里的河流走廊上,浮游细菌和生物膜都表现出显著的 DDR,浮游细菌 DDR 的斜率比生物膜 DDR 的斜率陡峭,这意味着浮游细菌的生物地理学特征比生物膜更强。与生物膜群落相比,浮游细菌群落中物种间的相互作用形成了更密集、更复杂的网络。我们的研究结果还显示,虽然在整条河流中,浮游细菌群落和生物膜群落主要受确定性过程的调节,但群落的组成存在着从上游到下游从确定性过程到随机过程的过渡。所有这些实证结果拓展了我们对干旱和半干旱地段生态系统微生物生态学的认识。
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引用次数: 0
Bisphenol S exposure promotes stemness of triple-negative breast cancer cells via regulating Gli1-mediated Sonic hedgehog pathway 双酚 S 暴露通过调节 Gli1 介导的声子刺猬通路促进三阴性乳腺癌细胞的干性。
IF 7.7 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-11-04 DOI: 10.1016/j.envres.2024.120293
Kefan Yi , Weiyi Chen , Xu Zhou , Chunfeng Xie , Caiyun Zhong , Jianyun Zhu
Bisphenol S (BPS), one of the most common alternatives for bisphenol A (BPA), has been implied to increase the risk of breast cancer. Triple-negative breast cancer (TNBC) is a highly aggressive type of breast cancer with a poor prognosis. However, the association between BPS and TNBC remains unclear. Cancer stem cells (CSCs) have a crucial role in breast cancer initiation, metastasis, and recurrence. Here, we proposed that BPS, equivalent to the human internal exposure and the environmental concentrations, enhanced CSC-like properties by upregulating sphere formation, self-renewal, the percentage of CD44+/CD24- cells, and the expression of CSC markers. Moreover, BPS promoted the migration, invasion, and epithelial-mesenchymal transition (EMT) in TNBC cells. Mechanistically, BPS activated the Sonic Hedgehog (SHH) signaling pathway in TNBC cells. Molecular docking analysis further showed that BPS upregulated SHH signaling pathway via directly binding Gli1 protein. Furthermore, inhibitor of SHH pathway or Gli1 siRNA attenuated the promoting effects of BPS on stemness, invasion, and migration of TNBC cells. In summary, our data firstly provide evidence that environmentally relevant BPS concentration treatment significantly enhanced TNBC malignant phenotype by activating the Sonic Hedgehog/Gli1 signaling pathway, raising high concerns about the potential population biology hazards of BPS.
双酚 S(BPS)是双酚 A(BPA)最常见的替代品之一,被认为会增加罹患乳腺癌的风险。三阴性乳腺癌(TNBC)是一种侵袭性很强的乳腺癌,预后较差。然而,BPS 与 TNBC 之间的关系仍不清楚。癌症干细胞(CSCs)在乳腺癌的发生、转移和复发中起着至关重要的作用。在此,我们提出,相当于人体内部暴露和环境浓度的BPS可通过上调球体形成、自我更新、CD44+/CD24-细胞百分比和CSC标志物的表达来增强CSC样特性。此外,BPS 还能促进 TNBC 细胞的迁移、侵袭和上皮-间质转化(EMT)。从机理上讲,BPS激活了TNBC细胞中的Sonic Hedgehog(SHH)信号通路。分子对接分析进一步表明,BPS通过直接结合Gli1蛋白上调SHH信号通路。此外,SHH通路抑制剂或Gli1 siRNA减弱了BPS对TNBC细胞干性、侵袭和迁移的促进作用。总之,我们的数据首次证明了环境相关浓度的BPS处理可通过激活Sonic Hedgehog/Gli1信号通路显著增强TNBC的恶性表型,引起了人们对BPS潜在群体生物学危害的高度关注。
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引用次数: 0
Effects of the combined use of lanthanum carbonate and activated carbon capping materials on phosphorus and dissolved organic matter in lake sediments 联合使用碳酸镧和活性炭封盖材料对湖泊沉积物中磷和溶解有机物的影响。
IF 7.7 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-11-04 DOI: 10.1016/j.envres.2024.120291
Chenjun Yang , Qi Li , Xiang Chen , Minjuan Li , Xiangyu He , Gaoxiang Li , Yichun Shao , Jingwei Wu
Lanthanum carbonate (LC) represents a novel material for the immobilization of internal phosphorus (P) in sediments. Activated carbon (AC) is a traditional adsorbent that has been employed in the remediation of sediments on a wide scale. The objective of this study is to examine the mechanisms and effects of the combined use of LC and AC capping materials on the immobilization of P and dissolved organic matter (DOM) in sediments, through a 90-day incubation experiment. The results of isotherm experiments showed that the adsorption mechanism of P on LC and AC was mainly chemisorption. The XPS analyses showed the adsorption mechanism of P on LC was mainly ligand exchange and inner-sphere complexation; while the adsorption mechanism of P on AC was mainly ligand exchange and electrostatic adsorption. The results demonstrated that the concentrations of soluble reactive phosphorus (SRP) and DOM in the 0 to −100 mm sediment layer were reduced by 69.79% and 33.93%, respectively, in comparison to the control group with the LC + AC group. Moreover, the HCl-P and Res-P (stable P) in the 0–5 cm sediment layer were increased by 50.07% and 21.04%, respectively, in the LC + AC group. This indicates that the combined application of LC and AC has the potential to reduce the risk of P release. Furthermore, the formation of Fe(III)/Mn(IV) oxyhydroxides by LC + AC treatment resulted in an increased adsorption of SRP and DOM. Moreover, the effect of LC + AC capping on microbial community was smaller than that of LC/AC capping alone. The findings of this study indicated that the combined use of LC and AC represents a novel approach to the effective treatment of internal P and DOM in eutrophic lake sediments.
碳酸镧(LC)是一种固定沉积物中内磷(P)的新型材料。活性炭(AC)是一种传统的吸附剂,已被广泛用于沉积物的修复。本研究的目的是通过为期 90 天的培养实验,考察 LC 和 AC 盖层材料联合使用对沉积物中磷和溶解有机物 (DOM) 固定化的机理和影响。等温线实验结果表明,LC 和 AC 对 P 的吸附机理主要是化学吸附。XPS 分析表明,P 在 LC 上的吸附机理主要是配体交换和内球络合;而 P 在 AC 上的吸附机理主要是配体交换和静电吸附。结果表明,与对照组相比,LC+AC 组 0 至 -100 mm 沉积层中可溶性活性磷(SRP)和 DOM 的浓度分别降低了 69.18% 和 33.93%。此外,在 LC+AC 组中,0∼5 厘米沉积层中的 HCl-P 和 Res-P(稳定 P)分别增加了 50.07% 和 21.04%。这表明结合施用 LC 和 AC 有可能降低 P 释放的风险。此外,LC+AC 处理形成的铁(III)/锰(IV)氧氢氧化物增加了对 SRP 和 DOM 的吸附。此外,LC + AC 覆膜对微生物群落的影响小于单独使用 LC/AC 覆膜的影响。该研究结果表明,结合使用 LC 和 AC 是有效处理富营养化湖泊沉积物中内部 P 和 DOM 的一种新方法。
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引用次数: 0
Differences in the regulation of soil carbon pool quality and stability by leaf-litter and root-litter decomposition 叶屑和根屑分解对土壤碳库质量和稳定性的调节差异。
IF 7.7 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-11-02 DOI: 10.1016/j.envres.2024.120285
Jia Zeng , Xiangyang Li , Junnan Jian , Liheng Xing , Yu Li , Xing Wang , Qi Zhang , Chengjie Ren , Gaihe Yang , Xinhui Han
Litter plays a crucial role in soil ecosystems. However, the differences in decomposition between leaf-litter and root-litter and their relative contributions to soil carbon pools and stability are not yet clear. Therefore, we conducted a 450-day in situ decomposition experiment in a semi-arid grassland to investigate the effects of soil biophysical and chemical properties on litter decomposition and to elucidate the dynamics of soil carbon pools during the decomposition process. The results showed that the decomposition rate (K) of leaf-litter was significantly higher than that of root-litter, and litter quality was the most important factor affecting the K of leaf-litter (58%) and root-litter (63%). Leaf-litter decomposition was more effective in promoting the increase in soil leucine aminopeptidase and β-1,4-glucosidase activities, as well as the accumulation of microbial biomass carbon (MBC), particulate organic carbon (POC), and dissolved organic carbon (DOC), compared to root-litter. However, the difference in the impact of leaf-litter and root-litter on soil organic carbon (SOC) was not significant. The decomposition of leaf-litter contributed more significantly to enhancing the soil carbon pool management index (CPMI) compared to root-litter, with increases of 39% and 25%, respectively. In contrast, leaf-litter decomposition significantly reduced the mineral-associated organic carbon (MAOC) and the MAOC/POC ratio, while root-litter decomposition significantly increased the MAOC and MAOC/POC. Random forest, partial correlation, and path analysis indicated that the effects of leaf-litter and root-litter decomposition on CPMI were mainly regulated by decomposition time and soil carbon components, while the effects on MAOC/POC were mainly controlled by litter quality. The results demonstrate that both leaf-litter and root-litter can enhance soil carbon storage and CPMI, but root-litter may be more beneficial for soil carbon pool stability. These results further contribute to the understanding of the continuous system of litter-soil carbon pools.
腐殖质在土壤生态系统中起着至关重要的作用。然而,叶状废弃物和根状废弃物的分解差异及其对土壤碳库和稳定性的相对贡献尚不清楚。因此,我们在半干旱草地上进行了为期 450 天的原位分解实验,以研究土壤生物物理和化学特性对枯落物分解的影响,并阐明分解过程中土壤碳库的动态变化。结果表明,叶状废弃物的分解率(K)明显高于根状废弃物,废弃物质量是影响叶状废弃物分解率(58%)和根状废弃物分解率(63%)的最重要因素。与根状废弃物相比,叶状废弃物的分解更能促进土壤亮氨酸氨肽酶和β-1,4-葡萄糖苷酶活性的提高,以及微生物生物量碳(MBC)、颗粒有机碳(POC)和溶解有机碳(DOC)的积累。然而,叶屑和根屑对土壤有机碳(SOC)的影响差异并不显著。与根部残留物相比,叶片残留物的分解对提高土壤碳库管理指数(CPMI)的贡献更大,分别提高了 39% 和 25%。相比之下,叶片分解显著降低了矿质相关有机碳(MAOC)和MAOC/POC比率,而根叶分解则显著提高了MAOC和MAOC/POC。随机森林分析、偏相关分析和路径分析表明,叶屑和根屑分解对 CPMI 的影响主要受分解时间和土壤碳组分的调控,而对 MAOC/POC 的影响主要受枯落物质量的控制。研究结果表明,叶屑和根屑都能提高土壤碳储量和CPMI,但根屑可能更有利于土壤碳库的稳定。这些结果进一步加深了人们对废弃物-土壤碳库连续系统的理解。
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引用次数: 0
Effect of iron-based nanomaterials on organic carbon dynamics and greenhouse gas emissions during composting process 铁基纳米材料对堆肥过程中有机碳动态和温室气体排放的影响
IF 7.7 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-11-02 DOI: 10.1016/j.envres.2024.120281
Pengjiao Tian, Shentao Yang, Mingxin Yang, Duo Xie, Haizhong Yu, Xiqing Wang
Iron-based nanomaterials as effective additives can enhance the quality and safety of compost. However, their influence on organic carbon fractions changes and greenhouse gas emissions during composting remains unclear. This study demonstrated that iron-based nanomaterials facilitate the conversion of light organic carbon fraction into heavy organic carbon fraction, with the iron-based nanomaterials group showing a significantly higher heavy organic carbon fraction content (41.88%) compared to the control group (35.71%). This shift led to an increase in humic substance content (77.5 g/kg) and a reduction in greenhouse gas emissions, with CO2, CH4, and N2O emissions decreasing by 20.5%, 39.7%, and 55.4%, respectively. Additionally, CO2-equivalent emissions were reduced by 42.9%. Microbial analysis revealed that iron-based nanomaterials increased the abundance of Bacillus and reduced the abundance of methane-producing archaea such as Methanothermobacter and Methanomassiliicoccus. These results indicated that the role of iron-based nanomaterials in regulating reactive oxygen species production and specific microbial communities involved in humification process. This study provides a practical strategy for improving waste utilization efficiency and mitigating climate change.
铁基纳米材料作为有效的添加剂,可以提高堆肥的质量和安全性。然而,它们对堆肥过程中有机碳组分变化和温室气体排放的影响仍不清楚。本研究表明,铁基纳米材料可促进轻质有机碳组分向重质有机碳组分的转化,与对照组(35.71%)相比,铁基纳米材料组的重质有机碳组分含量(41.88%)显著提高。这种变化导致腐殖质含量增加(77.5 克/千克),温室气体排放量减少,二氧化碳、甲烷和氧化亚氮排放量分别减少了 20.5%、39.7% 和 55.4%。此外,二氧化碳当量排放量减少了 42.9%。微生物分析表明,铁基纳米材料增加了芽孢杆菌的数量,降低了产甲烷古细菌(如甲烷热杆菌和甲烷嗜热球菌)的数量。这些结果表明,铁基纳米材料在调节活性氧生成和参与腐殖化过程的特定微生物群落方面发挥了作用。这项研究为提高废物利用效率和减缓气候变化提供了一种实用策略。
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引用次数: 0
Reduced primary productivity and notable resilience of phytoplankton community in the coastal water of southern China under a marine heatwave 海洋热浪下中国南方沿海水域浮游植物群落初级生产力下降和显著的恢复能力。
IF 7.7 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-11-02 DOI: 10.1016/j.envres.2024.120286
Yukun Zhang , Guang Gao , Huijie Xue , Kunshan Gao
Increasing frequency, intensity and duration of marine heatwaves (MHWs) are supposed to affect coastal biological production in different regions to different extents. To understand how MHWs impact coastal primary productivity and community succession of phytoplankton and assess the changes in resilience of phytoplankton communities, we conducted a mesoscale enclosure experiment simulating a MHW in the coastal water of southern China. After 8 days of the MHW (+3 °C) treatment, community biomass was significantly lower than the control's, and primary productivity per volume of water was reduced by about 56%. Nevertheless, the phytoplankton community retrieved its biomass and primary productivity after the temperature was subsequently reset to that of the control. Although the MHW treatment decreased the abundance of diatom and increased the percentages of Synechococcus and Prasinophytes, the main phytoplankton functional types showed positive resilience that allowed the recovery of the phytoplankton community after the MHW. Our results indicate that key phytoplankton functional types in the southern coastal waters of China exhibited significant resilience, recovery, and temporal stability under the influence of the marine MHW by 3 °C rise. However, reduced primary productivity during the MHW period, along with decreased biomass density, might significantly influence secondary producers. In addition, the altered phytoplankton community structure may affect coastal food web processes at least during the MHW period.
海洋热浪(MHWs)的频率、强度和持续时间的增加会对不同地区的沿岸生物生产产生 不同程度的影响。为了了解海洋热浪对沿岸初级生产力和浮游植物群落演替的影响,并评估浮游植物群落恢复能力的变化,我们在中国南方沿岸水域进行了模拟海洋热浪的中尺度围隔实验。经过 8 天的 MHW(+3 oC)处理后,群落生物量明显低于对照组,单位体积水体的初级生产力降低了约 56%。然而,当温度恢复到对照组的水平后,浮游植物群落的生物量和初级生产力又恢复了。虽然高温热浪处理降低了硅藻的丰度,增加了 Synechococcus 和 Prasinophytes 的比例,但主要浮游植物功能类型表现出了积极的恢复能力,使浮游植物群落在高温热浪后得以恢复。我们的研究结果表明,在海洋 MHW 上升 3 oC 的影响下,中国南部沿岸海域的主要浮游植物功能类型表现出显著的恢复力、复原力和时间稳定性。然而,MHW 期间初级生产力的降低以及生物量密度的下降可能会严重影响次级生产者。此外,浮游植物群落结构的改变可能至少在 MHW 期间影响沿岸食物网过程。
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引用次数: 0
Physiological plasticity and life history traits affect Chamelea gallina acclimatory responses during a marine heatwave 生理可塑性和生活史特征影响五步蛇在海洋热浪中的适应性反应。
IF 7.7 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-11-02 DOI: 10.1016/j.envres.2024.120287
Letizia Iuffrida , Rachele Spezzano , Giulia Trapella , Nicolo Cinti , Luca Parma , Antonina De Marco , Giorgia Palladino , Alessio Bonaldo , Marco Candela , Silvia Franzellitti
The striped venus clam (Chamelea gallina) is a relevant economic resource in the Adriatic Sea. This study explored the physiological status of C. gallina at four sites selected along a gradient from high to low incidence of recorded historical mortality events and low to high productivity in the Northwestern Adriatic Sea. Investigations were performed during the marine heatwave in 2022 (from July to November). The optimal temperature range for C. gallina was exceeded in July and September, exacerbating stress conditions and a poor nutritional status, particularly at the low productivity sites. Transcriptional profiles assessed in digestive glands showed that clams from the low productivity sites up-regulated transcripts related to feeding/digestive functions as a possible compensatory mechanism to withstand adverse environmental conditions. Clams from the high productivity sites, that in a previous study showed enrichment of health-promoting microbiome components, displayed a healthier metabolic makeup (IDH up-regulation) and induction of protective antioxidant and immune responses. These features are hallmarks of putative enhanced resilience of the species towards environmental stress. Despite the well-known high sensitivity of C. gallina to environmental variations and its narrow window of acclimatory potential, results highlight that local conditions may influence physiological plasticity of this clam species and shape either positively or negatively its response capabilities to environmental changes. The identification of health-promoting endogenous mechanisms both from the animal (this study) and from its associated microbiome may provide the foundation for developing novel tools and strategies to improve clam health and production in low productivity areas or under adverse environmental conditions.
条纹文蛤(Chamelea gallina)是亚得里亚海的一种相关经济资源。本研究在亚得里亚海西北部从有历史记录的死亡事件高发地到低发地、从低生产力到高生产力的梯度上选定的四个地点,探讨了条纹文蛤的生理状态。调查是在 2022 年海洋热浪期间(7 月至 11 月)进行的。七月和九月的温度超过了 C. gallina 的最适温度范围,加剧了应激条件和营养状况,尤其是在低生产力地点。对消化腺转录谱的评估表明,低生产力地点的蛤蜊上调了与摄食/消化功能有关的转录本,这可能是一种抵御不利环境条件的补偿机制。在之前的一项研究中,高生产力地点的蛤蜊富含促进健康的微生物组成分,显示出更健康的新陈代谢结构(IDH 上调),并诱导保护性抗氧化和免疫反应。这些特征表明,该物种对环境压力的适应能力可能有所增强。尽管众所周知五倍子蛤对环境变化高度敏感,而且其适应潜力窗口很窄,但研究结果突出表明,当地条件可能会影响这种蛤类的生理可塑性,并对其应对环境变化的能力产生积极或消极的影响。从动物(本研究)及其相关微生物组中发现促进健康的内源机制,可为开发新的工具和战略奠定基础,以改善低生产力地区或不利环境条件下的蛤蜊健康和产量。
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引用次数: 0
Electrocatalytic conversion of nitrate to ammonia on the oxygen vacancy engineering of zinc oxide for nitrogen recovery from nitrate-polluted surface water 在氧化锌氧空位工程上将硝酸盐电催化转化为氨,以从受硝酸盐污染的地表水中回收氮。
IF 7.7 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-11-02 DOI: 10.1016/j.envres.2024.120279
Wenyang Fu, Yanjun Yin, Shuxian He, Xiangyi Tang, Yinan Liu, Fei Shen, Yan Zou, Guangming Jiang
Nitrate pollution in surface water poses a significant threat to drinking water safety. The integration of electrocatalytic reduction reaction of nitrate (NO3RR) to ammonia with ammonia collection processes offers a sustainable approach to nitrogen recovery from nitrate-polluted surface water. However, the low catalytic activity of existing catalysts has resulted in excessive energy consumption for NO3RR. Herein, we developed a facile approach of electrochemical reduction to generate oxygen vacancy (Ov) on zinc oxide nanoparticles (ZnO1-x NPs) to enhance catalytic activity. The ZnO1-x NPs achieved a high NH3-N selectivity of 92.4% and NH3-N production rate of 1007.9 mgNH3N h−1 m−2 at −0.65 V vs. RHE in 22.5 mg L−1 NO3N, surpassing both pristine ZnO and the majority of catalysts reported in the literature. DFT calculations with in-situ Raman spectroscopy and ESR analysis revealed that the presence of Ov significantly increased the affinity for the NO3 (nitrate) and key intermediate of NO2 (nitrite). The strong adsorption of NO3 on Ov decreased the energy barrier of potential determining step (NO3 →∗NO3) from 0.49 to 0.1 eV, boosting the reaction rate. Furthermore, the strong adsorption of NO2 on Ov prevented its escape from the active sites, thereby minimizing NO2 by-product formation and enhancing ammonia selectivity. Moreover, the NO3RR, when coupled with a membrane separation process, achieved a 100% nitrogen recycling efficiency with low energy consumption of 0.55 kWh molN1 at a flow rate below 112 mL min−1 for the treatment of nitrate-polluted lake water. These results demonstrate that ZnO1-x NPs are a reliable catalytic material for NO₃RR, enabling the development of a sustainable technology for nitrogen recovery from nitrate-polluted surface water.
地表水中的硝酸盐污染对饮用水安全构成严重威胁。将硝酸盐的电催化还原反应(NO3RR)与氨气收集工艺相结合,为从硝酸盐污染的地表水中回收氮提供了一种可持续的方法。然而,现有催化剂的催化活性较低,导致 NO3RR 的能耗过高。在此,我们开发了一种简便的电化学还原方法,在氧化锌纳米颗粒(ZnO1-x NPs)上生成氧空位(Ov),以提高催化活性。ZnO1-x NPs 的 NH3-N 选择性高达 92.4%,在 -0.65 V 对 22.5 mg L-1 的 RHE 条件下,NH3-N 产率为 1007.9 h-1 m-2,超过了原始 ZnO 和文献报道的大多数催化剂。利用原位拉曼光谱和 ESR 分析进行的 DFT 计算表明,Ov 的存在显著提高了(硝酸盐)和(亚硝酸盐)关键中间产物的亲和力。Ov 的强吸附作用使潜在决定步骤(→*NO3)的能量势垒从 0.49 eV 降至 0.1 eV,从而提高了反应速率。此外,Ov 的强吸附性阻止了其从活性位点逸出,从而最大限度地减少了副产物的形成,提高了氨的选择性。此外,NO3RR 与膜分离过程相结合,在处理硝酸盐污染的湖水时,在低于 112 mL min-1 的流速下,实现了 100% 的氮回收效率和 0.55 kWh 的低能耗。这些结果表明,ZnO1-x NPs 是一种可靠的 NO₃RR 催化材料,有助于开发一种可持续的硝酸盐污染地表水氮回收技术。
{"title":"Electrocatalytic conversion of nitrate to ammonia on the oxygen vacancy engineering of zinc oxide for nitrogen recovery from nitrate-polluted surface water","authors":"Wenyang Fu,&nbsp;Yanjun Yin,&nbsp;Shuxian He,&nbsp;Xiangyi Tang,&nbsp;Yinan Liu,&nbsp;Fei Shen,&nbsp;Yan Zou,&nbsp;Guangming Jiang","doi":"10.1016/j.envres.2024.120279","DOIUrl":"10.1016/j.envres.2024.120279","url":null,"abstract":"<div><div>Nitrate pollution in surface water poses a significant threat to drinking water safety. The integration of electrocatalytic reduction reaction of nitrate (NO<sub>3</sub>RR) to ammonia with ammonia collection processes offers a sustainable approach to nitrogen recovery from nitrate-polluted surface water. However, the low catalytic activity of existing catalysts has resulted in excessive energy consumption for NO<sub>3</sub>RR. Herein, we developed a facile approach of electrochemical reduction to generate oxygen vacancy (Ov) on zinc oxide nanoparticles (ZnO<sub>1-x</sub> NPs) to enhance catalytic activity. The ZnO<sub>1-x</sub> NPs achieved a high NH<sub>3</sub>-N selectivity of 92.4% and NH<sub>3</sub>-N production rate of 1007.9 <span><math><mrow><msub><mtext>mg</mtext><mrow><msub><mtext>NH</mtext><mn>3</mn></msub><mo>‐</mo><mi>N</mi></mrow></msub></mrow></math></span> h<sup>−1</sup> m<sup>−2</sup> at −0.65 V <em>vs.</em> RHE in 22.5 mg L<sup>−1</sup> <span><math><mrow><msubsup><mtext>NO</mtext><mn>3</mn><mo>‐</mo></msubsup><mo>‐</mo><mi>N</mi></mrow></math></span>, surpassing both pristine ZnO and the majority of catalysts reported in the literature. DFT calculations with <em>in-situ</em> Raman spectroscopy and ESR analysis revealed that the presence of Ov significantly increased the affinity for the <span><math><mrow><msubsup><mtext>NO</mtext><mn>3</mn><mo>‐</mo></msubsup></mrow></math></span> (nitrate) and key intermediate of <span><math><mrow><msubsup><mtext>NO</mtext><mn>2</mn><mo>‐</mo></msubsup></mrow></math></span> (nitrite). The strong adsorption of <span><math><mrow><msubsup><mtext>NO</mtext><mn>3</mn><mo>‐</mo></msubsup></mrow></math></span> on Ov decreased the energy barrier of potential determining step (<span><math><mrow><msubsup><mtext>NO</mtext><mn>3</mn><mo>‐</mo></msubsup></mrow></math></span> →∗NO<sub>3</sub>) from 0.49 to 0.1 eV, boosting the reaction rate. Furthermore, the strong adsorption of <span><math><mrow><msubsup><mtext>NO</mtext><mn>2</mn><mo>‐</mo></msubsup></mrow></math></span> on Ov prevented its escape from the active sites, thereby minimizing <span><math><mrow><msubsup><mtext>NO</mtext><mn>2</mn><mo>‐</mo></msubsup></mrow></math></span> by-product formation and enhancing ammonia selectivity. Moreover, the NO<sub>3</sub>RR, when coupled with a membrane separation process, achieved a 100% nitrogen recycling efficiency with low energy consumption of 0.55 kWh <span><math><msubsup><mi>mol</mi><mi>N</mi><mrow><mo>−</mo><mn>1</mn></mrow></msubsup></math></span> at a flow rate below 112 mL min<sup>−1</sup> for the treatment of nitrate-polluted lake water. These results demonstrate that ZnO<sub>1-x</sub> NPs are a reliable catalytic material for NO₃RR, enabling the development of a sustainable technology for nitrogen recovery from nitrate-polluted surface water.</div></div>","PeriodicalId":312,"journal":{"name":"Environmental Research","volume":"264 ","pages":"Article 120279"},"PeriodicalIF":7.7,"publicationDate":"2024-11-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142566860","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
Meadows or asphalt road – Does momentary affective well-being vary with immediate physical environment? Results from a geographic ecological momentary assessment study in three metropolitan areas in Germany 草地还是沥青路--瞬间的情感幸福感会随直接的物理环境而变化吗?德国三个大都市地区的地理生态瞬间评估研究结果。
IF 7.7 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-11-02 DOI: 10.1016/j.envres.2024.120283
Anna Mascherek , Gloria Luong , Cornelia Wrzus , Michaela Riediger , Simone Kühn
We investigated the association between the immediate physical environment of individuals and individual fluctuations of momentary affective well-being in everyday life with a focus on medium sized metropolitan areas in Europe representing a typical living environment of a large proportion of the world’s population. The sample comprised 365 individuals (54.8 % female) with participants ranging from 14.08 to 88.27 years of age (M = 43.9, SD = 20.9). In an geographic ecological momentary assessment (GEMA), participants were prompted six times a day on at least 9 days over the course of 3 weeks, covering a total of six weekdays and three weekend days on mobile phones to report their momentary affective well-being. Urban land use categories (forest, water, urban green) were assessed with GPS-localization as environmental variables. Additionally, sunshine, rainfall, whether participants were inside or outside as well as whether they were alone or had company were included into the analyses.
We used dynamic structural equation modelling to model the inter- and intraindividual differences as well as fluctuations and assess potential covariates while acknowledging the autoregressive nature of affect.
The results showed that on individual level, fluctuations of momentary affective well-being were associated with sunshine, having company and travelling. No significant association emerged for urban green, forest, and water neither within individuals nor between. Methodological as well as conceptual implications are discussed and an interpretation of the present findings are provided.
我们以欧洲中等大都市地区为研究对象,调查了日常生活中个人的直接物理环境与个人瞬间情感幸福感波动之间的关系,这些地区代表了世界上大部分人口的典型生活环境。样本包括 365 人(54.8% 为女性),年龄从 14.08 岁到 88.27 岁不等(M = 43.9,SD = 20.9)。在地理生态瞬间评估(GEMA)中,参与者在 3 周内至少有 9 天每天接受 6 次手机提示,共涵盖 6 个工作日和 3 个周末,以报告他们的瞬间情感幸福感。城市土地利用类别(森林、水域、城市绿化)作为环境变量通过 GPS 定位进行评估。此外,日照、降雨量、参与者是在室内还是室外,以及他们是独自一人还是有人陪伴,都被纳入了分析范围。我们使用动态结构方程模型来模拟个体间和个体内的差异以及波动,并评估潜在的协变量,同时承认情感的自回归性质。结果显示,在个体层面上,瞬间情感幸福感的波动与阳光、有人陪伴和旅行有关。在个体内部或个体之间,城市绿化、森林和水都没有出现明显的关联。本文讨论了研究方法和概念上的影响,并对目前的研究结果进行了解释。
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引用次数: 0
Surfactant-modified zein nanoparticles adsorbents for ultrafast and efficient removal of Cr(VI) 超快高效去除六价铬的表面活性剂改性玉米蛋白纳米颗粒吸附剂。
IF 7.7 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-11-02 DOI: 10.1016/j.envres.2024.120284
Qing Shen , Xiaomeng Xu , Xiaojing Liang , Cong Tang , Xiaoping Bai , Shijun Shao , Qing Liang , Shuqing Dong
The adsorption and removal of heavy metal ions Cr(VI) is of great significance for human health and ecological environment. Here, an ultrafast and high efficient adsorbent for Cr(VI) was developed based on cetyltrimethylammonium bromide (CTAB)-modified zein nanoparticles (C-ZNPs). In comparison to pristine zein nanoparticles (ZNPs) (11.199 m2 g−1), the surfactant-modified C-ZNPs exhibited larger specific surface area (17.002 m2 g−1). Moreover, C-ZNPs had superior dispersion and more positive charge distribution, which contributed to the improvement for adsorption performance. The results showed that the saturated adsorption of Cr(VI) was reached up to 192.27 mg/g using the C-ZNPs nanosorbent at T = 298 K, pH = 4, t = 10s, and C0 = 125 mg/L. The removal rate was significantly faster than that reported natural polymer-based adsorbents. The experimental values were followed Freundich isothermal model and pseudo-second-order kinetic model, indicating that the adsorption occurred primarily through a multimolecular layer adsorption process, with a strong emphasis on chemisorption. Mechanistic investigations further revealed that the adsorption of Cr(VI) onto C-ZNPs was mediated by various interactions, including electrostatic attraction, complexation, and ion exchange. These findings provide insights into the efficient removal of Cr(VI) by C-ZNPs and suggest potential applications in water treatment and environmental remediation.
重金属离子 Cr(VI) 的吸附和去除对人类健康和生态环境具有重要意义。本文以十六烷基三甲基溴化铵(CTAB)修饰的玉米蛋白纳米颗粒(C-ZNPs)为基础,开发了一种超快速、高效的 Cr(VI) 吸附剂。与原始玉米蛋白纳米颗粒(ZNPs)(11.199 m2-g-1)相比,表面活性剂修饰的 C-ZNPs 具有更大的比表面积(17.002 m2-g-1)。此外,C-ZNPs 具有更好的分散性和更多的正电荷分布,这有助于改善吸附性能。结果表明,在 T = 298 K、pH = 4、t = 10s 和 C0 = 125 mg/L 条件下,C-ZNPs 纳米吸附剂对 Cr(VI) 的饱和吸附达到 192.27 mg/g。其去除率明显快于所报道的天然聚合物基吸附剂。实验值遵循弗兰迪奇等温模型和伪秒阶动力学模型,表明吸附主要通过多分子层吸附过程进行,化学吸附作用十分突出。机理研究进一步表明,C-ZNPs 对 Cr(VI) 的吸附是由各种相互作用介导的,包括静电吸引、络合和离子交换。这些发现为 C-ZNPs 高效去除六价铬提供了启示,并提出了在水处理和环境修复中的潜在应用。
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Environmental Research
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