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Understanding filamentous cyanobacteria and their adaptive niches in Lake Honghu, a shallow eutrophic lake 了解洪湖浅富营养化湖泊中的丝状蓝藻及其适应性生态位
2区 环境科学与生态学 Pub Date : 2024-05-14 DOI: 10.1016/j.jes.2024.05.010
Guangbin Gao , Dong Bai , Tianli Li , Jie Li , Yunlu Jia , Jing Li , Zhi Wang , Xiuyun Cao , Lirong Song

Freshwater lakes globally are witnessing an escalation in the frequency and intensity of cyanobacterial harmful blooms. However, underlying factors influencing the succession or coexistence of cyanobacteria, especially filamentous ones, remain poorly understood. Lake Honghu, a Ramsar Wetland of International Importance with degrading aquatic ecological quality, served as a case study to elucidate the intricate relationship between environmental changes and cyanobacterial dynamics. Our analysis revealed a significant increase in the dominance of filamentous cyanobacteria, marked by high spatiotemporal variability in community structure. This dominance of filamentous diazotrophic cyanobacteria is attributed to a decrease in the ratio of dissolved inorganic nitrogen to total phosphorus and their capacity to utilize organic phosphorus in phosphorus-deficient conditions. Species-specific density variations were linked to diverse environmental factors, with total nitrogen or total phosphorus concentration remaining as a crucial factor influencing dominant cyanobacterial density fluctuations. The dominance of low-temperature-tolerant Aphanizomenon and Pseudanabaena was evident in spring and winter, whereas Dolichospermum and Cylindrospermopsis, which prefer higher temperatures, thrived in summer and autumn. Additionally, non-algal turbidity and heterogeneity can potentially alter the competitive outcome among filamentous cyanobacteria or foster coexistence under conditions of elevated temperatures and nutrient limitation. This study predicts that filamentous cyanobacteria may spread and persist in lakes spanning a wide trophic range. Current findings enhance our comprehension of the dynamic responses exhibited by filamentous bloom-forming cyanobacteria in the face of environmental changes within shallow eutrophic lakes and provide valuable insights for lake managers involved in the remediation of degraded shallow lakes.

全球淡水湖蓝藻有害藻华的发生频率和强度都在不断上升。然而,人们对影响蓝藻(尤其是丝状蓝藻)演替或共存的潜在因素仍然知之甚少。洪湖是拉姆萨尔国际重要湿地,其水生生态质量不断恶化,我们以洪湖为案例,阐明了环境变化与蓝藻动态之间错综复杂的关系。我们的分析表明,丝状蓝藻的优势度明显增加,群落结构的时空变异性很高。丝状重氮蓝藻占优势的原因是溶解无机氮与总磷的比例下降,以及它们在缺磷条件下利用有机磷的能力下降。物种特异性密度变化与多种环境因素有关,总氮或总磷浓度仍然是影响优势蓝藻密度波动的关键因素。耐低温的 Aphanizomenon 和 Pseudanabaena 在春季和冬季明显占优势,而喜欢较高温度的 Dolichospermum 和 Cylindrospermopsis 则在夏季和秋季生长旺盛。此外,在温度升高和营养限制条件下,非海藻浊度和异质性可能会改变丝状蓝藻之间的竞争结果或促进共存。本研究预测,丝状蓝藻可能会在跨度很大的营养级范围的湖泊中传播和持续存在。目前的研究结果加深了我们对丝状蓝藻面对浅表富营养化湖泊环境变化所表现出的动态响应的理解,并为湖泊管理者参与退化浅表湖泊的修复工作提供了宝贵的见解。
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引用次数: 0
Ammonium removal through anaerobic ammonium oxidation coupled to iron(III) reduction along the Yangtze river–estuary continuum 通过厌氧氨氧化与铁(III)还原作用去除长江-河口连续体中的氨氮
2区 环境科学与生态学 Pub Date : 2024-05-13 DOI: 10.1016/j.jes.2024.05.006
Anxing Lai , Shiming Fan , Jingya Xue , Hongwei Wang , Ke Xie , Huabing Li , Hai Xu , Biao Li , Qinglong L. Wu

Anaerobic ammonium oxidation coupled to iron(III) reduction (Feammox) process has recently been recognized as an important pathway for removing ammonium in various natural habitats. However, our understanding for Feammox in river–estuary continuum is limited. In this study, stable isotope tracers and high-throughput amplicon sequencing were employed to determine Feammox rates and identify associated microbial communities in sediments along the Yangtze river–estuary continuum. Feammox rates averaged 0.0058 ± 0.0069 mg N/(kg·d) and accounted for approximately 22.3% of the ammonium removed from the sediments. Sediment Fe(III), ammonium (NH4+), total organic carbon (TOC), and pH were identified as important factors influencing Feammox rates. Additionally, Spirochaeta, Caldilineaceae_uncultured, and Ignavibacterium were found potentially associated with Feammox, which had not been documented as Feammox-associated microbial taxa previously. This study demonstrates that Feammox plays a vital role in ammonium removal within the Yangtze river–estuary continuum, providing greater insight into nitrogen removal and cycling in aquatic ecosystems.

厌氧氨氧化与铁(III)还原(Feammox)过程最近被认为是各种自然生境中去除氨的重要途径。然而,我们对河流-河口连续体中 Feammox 过程的了解还很有限。本研究采用稳定同位素示踪剂和高通量扩增子测序技术来测定长江-河口连续沉积物中的Feammox速率并识别相关微生物群落。铁氧率平均为 0.0058 ± 0.0069 mg N/(kg-d),约占沉积物中氨去除量的 22.3%。沉积物中的铁(III)、铵(NH4+)、总有机碳(TOC)和 pH 值被认为是影响 Feammox 氧化率的重要因素。此外,研究还发现 Spirochaeta、Caldilineaceae_uncultured 和 Ignavibacterium 可能与 Feammox 相关,而这些微生物类群以前从未作为与 Feammox 相关的微生物类群被记录在案。这项研究表明,Feammox 在长江-河口连续水域的氨去除过程中发挥了重要作用,为水生生态系统的氮去除和循环提供了更深入的见解。
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引用次数: 0
Catalytic performance of Pd catalyst supported on CeO2 or ZrO2 modified beta zeolite for methane oxidation 以 CeO2 或 ZrO2 改性 beta 沸石为载体的 Pd 催化剂在甲烷氧化中的催化性能
2区 环境科学与生态学 Pub Date : 2024-05-10 DOI: 10.1016/j.jes.2024.05.005
Yingao Zhang , Zidi Yan , Min Xiao , Chunlei Zhang , Luna Ruan , Yanshuang Zhang , Yun Zhong , Yong Yan , Yunbo Yu , Hong He

Two kinds of oxide-zeolite composite support, Ce-beta and Zr-beta were prepared by a simple wet impregnation method and adopted for the preparation of palladium-based catalysts for catalytic oxidation of methane. The Pd/6.8Zr-beta catalyst showed superior methane oxidation performance, achieving T50 and T90 of 417 °C and 451 °C, respectively, together with robust hydrothermal stability. Kinetic analysis has shown that incorporating Zr into the catalyst significantly enhanced its efficiency, nearly tripling the turnover frequency (TOF) for methane combustion compared to the Pd/beta catalyst. This enhanced performance was attributed to the dispersion of Zr on the zeolite surface, which not only promoted the formation of active PdO sites but also helped maintain the high Pd2+ content via facilitating the oxygen migration during the reaction, thus improving both the catalyst's activity and stability. In the Pd/8.6Ce-beta catalyst, doped CeO2 tended to aggregate in the zeolite's pores, adversely affecting the catalyst's efficiency. This aggregation promoted the formation of inactive Pd4+ species, a result of the enhanced metal-support interaction. This finding is critical for understanding the implications of dopant selection in the design of high-activity methane oxidation catalysts.

通过简单的湿法浸渍制备了两种氧化物-沸石复合载体(Ce-beta 和 Zr-beta),并将其用于制备甲烷催化氧化的钯基催化剂。Pd/6.8Zr-beta 催化剂表现出优异的甲烷氧化性能,T50 和 T90 分别达到 417 ℃ 和 451 ℃,并具有很强的水热稳定性。动力学分析表明,在催化剂中加入 Zr 能显著提高催化剂的效率,与 Pd/beta 催化剂相比,甲烷燃烧的翻转频率 (TOF) 几乎提高了两倍。这种性能的提高归功于 Zr 在沸石表面的分散,它不仅促进了活性 PdO 位点的形成,还通过促进反应过程中的氧迁移帮助维持了高 Pd2+ 含量,从而提高了催化剂的活性和稳定性。在 Pd/8.6Ce-beta 催化剂中,掺杂的 CeO2 容易在沸石孔隙中聚集,从而对催化剂的效率产生不利影响。这种聚集促进了非活性 Pd4+ 物种的形成,这是金属与支撑相互作用增强的结果。这一发现对于理解设计高活性甲烷氧化催化剂时选择掺杂剂的意义至关重要。
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引用次数: 0
The cGAS−STING-mediated ROS and ferroptosis are involved in manganese neurotoxicity cGAS-STING 介导的 ROS 和铁变态反应参与了锰的神经毒性作用
2区 环境科学与生态学 Pub Date : 2024-05-09 DOI: 10.1016/j.jes.2024.05.003
Zhimin Zhang, Jirui Yang, Qiongli Zhou, Shiyin Zhong, Jingjing Liu, Xin Zhang, Xuhong Chang, Hui Wang

Manganese (Mn) has been characterized as an environmental pollutant. Excessive releases of Mn due to human activities have increased Mn levels in the environment over the years, posing a threat to human health and the environment. Long-term exposure to high concentrations of Mn can induce neurotoxicity. Therefore, toxicological studies on Mn are of paramount importance. Mn induces oxidative stress through affecting the level of reactive oxygen species (ROS), and the overabundance of ROS further triggers ferroptosis. Additionally, Mn2+ was found to be a novel activator of the cyclic guanosine-adenosine synthase (cGAS)−stimulator of interferon genes (STING) pathway in the innate immune system. Thus, we speculate that Mn exposure may promote ROS production by activating the cGAS−STING pathway, which further induces oxidative stress and ferroptosis, and ultimately triggers Mn neurotoxicity. This review discusses the mechanism between Mn-induced oxidative stress and ferroptosis via activation of the cGAS−STING pathway, which may offer a prospective direction for future in-depth studies on the mechanism of Mn neurotoxicity.

锰(Mn)已被定性为一种环境污染物。多年来,人类活动导致的锰过量排放增加了环境中的锰含量,对人类健康和环境构成威胁。长期接触高浓度的锰会引起神经中毒。因此,对锰进行毒理学研究至关重要。锰通过影响活性氧(ROS)的水平诱导氧化应激,而过量的 ROS 会进一步引发铁变态反应。此外,研究还发现 Mn2+ 是先天免疫系统中环鸟苷腺苷合成酶(cGAS)-干扰素基因刺激器(STING)通路的新型激活剂。因此,我们推测锰暴露可能会通过激活 cGAS-STING 通路促进 ROS 的产生,从而进一步诱导氧化应激和铁变态反应,最终引发锰神经毒性。本综述探讨了锰通过激活 cGAS-STING 通路诱导氧化应激和铁变态反应之间的机制,为今后深入研究锰的神经毒性机制提供了一个前瞻性的方向。
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引用次数: 0
Effect of temperature on surface fluid sediment properties with cyanobacterial bloom biomass accumulation 温度对蓝藻水华生物量积累的表层流体沉积物特性的影响
2区 环境科学与生态学 Pub Date : 2024-05-09 DOI: 10.1016/j.jes.2024.05.001
Chunliu Wang , Da Xu , Bosong Zhu , Leilie Bai , Lei Huang , Helong Jiang

In eutrophic shallow lakes, cyanobacterial blooms will occur frequently and then settle into sediment, leading the formation of fluid sediment. Several factors including temperature can influence surface sediment properties. In this study, the influence of temperatures on surface sediment properties was determined in microcosm experiments through monitoring sediment physicochemical and rheological properties. During one-month incubation, it was found that surface sediment density and water content varied exponentially with increase in temperatures from 10 to 35 ℃. The results of particle size distribution indicated that cyanobacterial blooms biomass (CBB) degradation in sediment led to sediment flocculation and agglomeration. In the meantime, there were high ratios polysaccharide/protein in extracellular polymeric substances (EPSs), which enhanced the sediment particle agglomeration. Further, the yield stress in rheological test for sediment with (R2 = 0.97) and without (R2 = 0.85) CBB presented an exponential decay with increase in temperatures. And a threshold value at 20 ℃ for sediment critical shear stress (τcr) indicated that sediment could be resuspended easier when temperature was more than 20 ℃. Altogether, this study showed that the increase in temperatures with a threshold at 20 ℃, can cause sediment particle flocculation, resulting in a loose and fragile structure. And the results would be helpful to sediment management considering environmental effects of sediment suspension for eutrophication shallow lakes.

在富营养化的浅水湖泊中,蓝藻会频繁繁殖,然后沉淀到沉积物中,形成流动沉积物。包括温度在内的多种因素都会影响表层沉积物的性质。本研究通过监测沉积物的物理化学和流变特性,在微观世界实验中确定了温度对表层沉积物特性的影响。在为期一个月的培养过程中发现,表层沉积物的密度和含水量随着温度从 10 ℃ 到 35 ℃ 的升高呈指数变化。粒径分布结果表明,沉积物中蓝藻生物量(CBB)的降解导致了沉积物的絮凝和团聚。同时,细胞外高分子物质(EPSs)中的多糖/蛋白质比例较高,增强了沉积物颗粒的团聚。此外,含(R2 = 0.97)和不含(R2 = 0.85)CBB 的沉积物在流变测试中的屈服应力随温度升高呈指数衰减。沉积物临界剪切应力(τcr)的临界值为 20 ℃,这表明当温度超过 20 ℃ 时,沉积物更容易被重新悬浮。总之,这项研究表明,温度升高到 20 ℃ 时,会引起沉积物颗粒絮凝,导致结构松散和脆弱。考虑到沉积物悬浮对浅水湖泊富营养化的环境影响,该研究结果将有助于沉积物管理。
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引用次数: 0
Development of a UAV-borne sorbent tube sampler and its application on the vertical profile measurement of volatile organic compounds 无人机载吸附管采样器的开发及其在挥发性有机化合物垂直剖面测量中的应用
2区 环境科学与生态学 Pub Date : 2024-05-07 DOI: 10.1016/j.jes.2024.04.016
Haiyue Zhai , Jiacheng Zhou , Weixiong Zhao , Wanli Du , Nana Wei , Qianqian Liu , Shuo Wang , Jianguo Zhang , Weihua Cui , Weijun Zhang , Yanyu Lu , Zhu Zhu , Yue Liu

Vertical detection of volatile organic compounds (VOCs) is essential to expend our understanding of the distribution characteristics of VOCs and improve the predictive ability of existing air quality models. In this work, we report the development of a sorbent tube sampler based on an unmanned aerial vehicle (UAV) platform. Vertical profile measurement of VOCs with a vertical resolution of 25 m was achieved. The sampler consists of five lightweight VOC sorbent tubes and a 5-way solenoid valve, making it available for collecting five atmospheric VOC samples in a single flight with a time response of less than 30 min. The sampler weighed ∼ 1.45 kg and had dimensions of 240 mm × 220 mm × 100 mm with small penetration loss (< 10%) under 4-liter sampling conditions (flow rate of 200 mL/min). Commercialized SUMMA canisters were used as experimental controls to investigate the possible loss of self-made sampler for target compounds in the same sampling process. Comparison experiment on the ground showed that the concentration differences for all VOC species were lower than 0.14 μg/m3, proving the good reliability for VOCs measurements using sorbent tube sampler. The UAV platform also incorporated online instruments for meteorological parameters and O3 measurement. The sampler was successfully applied to characterize the vertical profiles of VOCs up to 100 m in October 2023 in the Huaihe River Basin of China. The UAV platform and the sorbent tube sampler demonstrate good performance and will be a valuable and reliable tool for vertical VOCs measurement.

挥发性有机化合物(VOC)的垂直探测对于加深我们对 VOC 分布特征的了解和提高现有空气质量模型的预测能力至关重要。在这项工作中,我们报告了基于无人飞行器(UAV)平台的吸附管采样器的开发情况。实现了垂直分辨率为 25 米的挥发性有机化合物垂直剖面测量。采样器由五个轻型挥发性有机化合物吸附管和一个五通电磁阀组成,一次飞行可采集五个大气挥发性有机化合物样本,时间响应小于 30 分钟。采样器重量为 1.45 千克,尺寸为 240 毫米 × 220 毫米 × 100 毫米,在 4 升采样条件下(流速为 200 毫升/分钟)穿透损失较小(< 10%)。为了研究自制采样器在相同采样过程中对目标化合物可能造成的损耗,使用了商品化的 SUMMA 罐作为实验对照。地面对比实验表明,所有挥发性有机化合物的浓度差异均低于 0.14 μg/m3 ,证明使用吸附剂管采样器测量挥发性有机化合物具有良好的可靠性。无人机平台还集成了气象参数和臭氧测量在线仪器。2023 年 10 月,该采样器成功应用于中国淮河流域 100 米范围内的 VOCs 垂直剖面表征。无人机平台和吸附管采样器表现出良好的性能,将成为垂直 VOCs 测量的可靠工具。
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引用次数: 0
Strategies for efficient enrichment of anaerobic ammonia oxidizing bacteria in activated sludge 活性污泥中厌氧氨氧化菌的高效增殖策略
2区 环境科学与生态学 Pub Date : 2024-05-07 DOI: 10.1016/j.jes.2024.04.046
Bin Tang , Jin Wang , Xingdong Gao , Zhihua Li

Anaerobic ammonia oxidation (Anammox) is an economical and sustainable wastewater nitrogen removal technology, and its application in the mainstream process is the inevitable trend of the development of Anammox. However, how to effectively enriching Anammox bacteria from the activated sludge remains challenging and restricts its extensive applications. In this study, the rapid and efficient enrichment of Anammox bacteria was achieved by raising the reflux ratio and nitrogen loading rate (NLR) using conventional activated sludge as the inoculant. In the screening phase (days 1–90), the reflux ratio was increased to discharge partial floc sludge, resulting in the relative abundance of Candidatus Brocadiaceae increased from 0.04% to 22.54%, which effectively reduced the matrix and spatial competition between other microorganisms and Anammox bacteria. On day 90, the stoichiometric ratio of the Anammox process closely approached the theoretical value of 1:1.32:0.26, indicating that the Anammox reaction was the primary nitrogen removal process in the system. In the enrichment phase (days 91–238), the NLR increased from 0.43 to 1.20 kgN/(m3·d) and removal efficiency was 71.89%, resulting in the relative abundance of Candidatus Brocadiaceae increased to 61.27% on day 180. The reactor operated steadily from days 444 to 498, maintaining the nitrogen removal rate (NRR) of 3.00 kgN/(m3·d) and achieving successful sludge granulation with the particle size of 392.4 µm. In short, this study provided a simple and efficient approach for enriching Anammox bacteria from the activated sludge, supporting to start an Anammox process efficiently.

厌氧氨氧化(Anammox)是一种经济、可持续的污水脱氮技术,将其应用于主流工艺是厌氧氨氧化发展的必然趋势。然而,如何有效地从活性污泥中富集 Anammox 细菌仍是一项挑战,限制了其广泛应用。本研究以传统活性污泥为接种剂,通过提高回流比和氮负荷率(NLR)实现了 Anammox 细菌的快速高效富集。在筛选阶段(第 1-90 天),通过提高回流比来排放部分絮状污泥,从而使 Candidatus Brocadiaceae 的相对丰度从 0.04% 提高到 22.54%,有效减少了其他微生物与 Anammox 菌之间的基质和空间竞争。第 90 天,Anammox 过程的化学计量比接近理论值 1:1.32:0.26,表明 Anammox 反应是系统中主要的脱氮过程。在富集阶段(第 91-238 天),NLR 从 0.43 kgN/(m3-d) 增加到 1.20 kgN/(m3-d),去除效率为 71.89%,因此在第 180 天,Candidatus Brocadiaceae 的相对丰度增加到 61.27%。反应器在第 444 天至第 498 天稳定运行,氮去除率(NRR)保持在 3.00 kgN/(m3-d),并成功实现了污泥颗粒化,颗粒大小为 392.4 µm。总之,这项研究为从活性污泥中富集 Anammox 细菌提供了一种简单而有效的方法,为高效启动 Anammox 工艺提供了支持。
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引用次数: 0
Magnetic iron oxide nanoparticles: An emerging threat for the environment and human health 磁性氧化铁纳米粒子:对环境和人类健康的新威胁
2区 环境科学与生态学 Pub Date : 2024-05-07 DOI: 10.1016/j.jes.2024.04.045
Hang Yang , Lin Liu , Zhao Shu , Weican Zhang , Cha Huang , Yanhuan Zhu , Si Li , Weichao Wang , Gang Li , Qinghua Zhang , Qian Liu , Guibin Jiang

Magnetic iron oxide nanoparticles (FexOy NPs, mainly Fe3O4 and γ-Fe2O3) are nanomaterials ubiquitously present in aquatic, terrestrial, and atmospheric environments, with a high prevalence and complex sources. Over the past decade, numerous reports have emerged on the presence of exogenous particles in human body, facilitated by the rapid development of separation and detection methods. The health risk associated with magnetic FexOy NP have garnered escalating attention due to their presence in human blood and brain tissues, especially for their potential association with neurodegenerative diseases like Alzheimer's disease. In this paper, we provide a comprehensive overview of sources, analysis methods, environmental impacts, and health risks of magnetic FexOy NP. Currently, most researches are primarily based on engineered FexOy NP, while reports about magnetic FexOy NP existing in real-world environments are still limited, especially for their occurrence levels in various environmental matrices, environmental transformation behavior, and biotoxic effects. Our study reviews this emerging pollutant, providing insights to address current research deficiencies and chart the course for future studies.

磁性氧化铁纳米粒子(FexOy NPs,主要是 Fe3O4 和 γ-Fe2O3)是一种普遍存在于水生、陆地和大气环境中的纳米材料,具有高普遍性和复杂的来源。过去十年间,随着分离和检测方法的快速发展,关于人体内存在外源粒子的报道层出不穷。由于磁性非氧化物 NP 存在于人体血液和脑组织中,特别是可能与阿尔茨海默病等神经退行性疾病相关,因此其对健康的危害日益受到关注。本文全面概述了磁性 FexOy NP 的来源、分析方法、环境影响和健康风险。目前,大多数研究主要基于工程化的 FexOy NP,而关于实际环境中存在的磁性 FexOy NP 的报道仍然有限,特别是关于它们在各种环境基质中的出现水平、环境转化行为和生物毒性效应的报道。我们的研究回顾了这种新兴污染物,为解决当前研究的不足提供了见解,并为未来的研究指明了方向。
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引用次数: 0
Promoting effect of potassium over Pd/SiO2 catalyst for ambient formaldehyde oxidation 钾对 Pd/SiO2 催化剂在环境甲醛氧化中的促进作用
2区 环境科学与生态学 Pub Date : 2024-05-07 DOI: 10.1016/j.jes.2024.04.027
Xiaofeng Liu , Chunying Wang , Xudong Chen , Jingyi Wang , Yaobin Li

Highly dispersed noble metals are acknowledged for its pivotal role in influencing the efficiency of catalysts during the HCHO oxidation process. Interestingly, in this work, an innovative approach was employed to augmenting the stabilization of noble metals on irreducible carriers supported noble metal catalyst (Pd/SiO2) by adding alkali metal potassium (K). A formidable promotion effect was observed when the K doping to Pd/SiO2 catalysts. It achieves a conversion rate of 93% for 270 ppmV of HCHO to harmless CO2 and H2O at a weight hourly space velocity (WHSV) of 300,000 mL/(g·hr) at 25°C. Multiple characterization results illustrated that a strong interaction between added K and Pd species was formed after K addition, which not only stabilized Pd species on the carrier surface but also markedly enhanced its dispersal on the SiO2 carrier. The increasing Pd dispersion induced more oxygen vacancies on the surfaces of the Pd/SiO2 catalysts. The formation of these oxygen vacancies can be attributed to the phenomenon of hydrogen spillover, which also contributed to elevating the electron density on the Pd sites. Meanwhile, the oxygen vacancies favored the O2 activation to form more reactive oxygen species participating in the HCHO oxidation reaction, thus improving the performance of Pd/SiO2 catalysts displayed for HCHO oxidation. This study provides a simple strategy to design high-performance irreducible carriers supported noble metal catalysts for HCHO catalytic oxidation.

高度分散的贵金属在影响 HCHO 氧化过程中催化剂的效率方面发挥着关键作用,这一点已得到公认。有趣的是,在这项工作中,采用了一种创新方法,通过添加碱金属钾(K)来增强不可还原载体支撑贵金属催化剂(Pd/SiO2)上贵金属的稳定性。当 K 掺杂到 Pd/SiO2 催化剂中时,观察到了强大的促进作用。在 25°C 条件下,重量小时空间速度(WHSV)为 300,000 mL/(g-hr)时,270 ppmV 的 HCHO 转化为无害的 CO2 和 H2O 的转化率达到 93%。多重表征结果表明,添加 K 后,添加的 K 与钯元素之间形成了强烈的相互作用,这不仅使钯元素稳定在载体表面,还显著提高了钯元素在二氧化硅载体上的分散度。随着钯分散度的增加,Pd/SiO2 催化剂表面出现了更多的氧空位。这些氧空位的形成可归因于氢溢出现象,这也有助于提高钯位点上的电子密度。同时,氧空位有利于 O2 活化,形成更多的活性氧参与 HCHO 氧化反应,从而提高了 Pd/SiO2 催化剂在 HCHO 氧化中的性能。这项研究为设计用于 HCHO 催化氧化的高性能不可还原载体支撑贵金属催化剂提供了一种简单的策略。
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引用次数: 0
Ingenious construction of a magnetic-recyclable photo-Fenton catalyst ZnFe2O4@MIL-88A(Fe) and its adsorption-degradation activity toward levofloxacin 巧妙构建磁性可回收光芬顿催化剂 ZnFe2O4@MIL-88A(Fe)及其对左氧氟沙星的吸附降解活性
2区 环境科学与生态学 Pub Date : 2024-05-07 DOI: 10.1016/j.jes.2024.04.043
Xichen Mi , Tingwei Wang , Yitong Chen , Dan Cao , Na Ma , Wei Dai

Monotonic pore size and particles inseparability of metal-organic frameworks (MOFs) caused serious effects on its light absorption ability and charge separation, restricting its application for antibiotic such as levofloxacin (LEV) degradation in water. In this study, a magnetically detachable nano-photocatalyst (ZnFe2O4@MIL-88A(Fe)) was synthesized using a simple two-step hydrothermal technique. The morphology and microstructure analyses showed that n-type ZnFe2O4 catalyst particles were efficiently assembled onto the surface of MIL-88A(Fe) crystal. Photocatalytic activity studies indicated that the ZnFe2O4@MIL-88A(Fe) plus H2O2 exhibiting a significantly boosted photo-Fenton activity toward LEV at visible light irradiation, compared to the pure ZnFe2O4 and MIL-88A(Fe), the degradation efficiency accordingly reached up to nearly 82% and 25% within 60 min. This excellent photocatalytic performance was ascribed to the synergistic effects of the heterogeneous structure of ZnFe2O4 and MIL-88A(Fe), whereby the efficient separation of charge carriers in the catalytic system is mutually reinforced with the efficient reduction of Fe3+ and Fe2+. Meanwhile, the degradation mechanism and intermediates of LEV during the photo-Fenton reaction process were also studied in depth through free radical burst, electron paramagnetic resonance, and mass spectrometry analyses, etc. Additionally, the ZnFe2O4@MIL-88A(Fe) composite catalyst displayed significant stability and ease of separation, indicating potential for the photo-oxidative degradation of organic pollutants.

金属有机框架(MOFs)的单调孔径和颗粒不可分离性严重影响了其光吸收能力和电荷分离能力,限制了其在水中降解左氧氟沙星等抗生素方面的应用。本研究采用简单的两步水热技术合成了一种磁性可分离纳米光催化剂(ZnFe2O4@MIL-88A(Fe))。形貌和微观结构分析表明,n 型 ZnFe2O4 催化剂颗粒被有效地组装在 MIL-88A(Fe) 晶体表面。光催化活性研究表明,与纯 ZnFe2O4 和 MIL-88A(Fe)相比,ZnFe2O4@MIL-88A(Fe) 加 H2O2 在可见光照射下对 LEV 的光 Fenton 活性显著提高,60 分钟内降解效率分别达到近 82% 和 25%。这种优异的光催化性能归功于 ZnFe2O4 和 MIL-88A(Fe)异质结构的协同效应,即催化体系中电荷载体的高效分离与 Fe3+ 和 Fe2+ 的高效还原相互促进。同时,还通过自由基猝灭、电子顺磁共振和质谱分析等方法深入研究了光-芬顿反应过程中 LEV 的降解机理和中间产物。此外,ZnFe2O4@MIL-88A(Fe)复合催化剂显示出显著的稳定性和易分离性,表明其具有光氧化降解有机污染物的潜力。
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Journal of Environmental Sciences-china
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