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Passivation Performance and Mechanism of a Novel Self-Healing Composite Passivator on Pyrite 新型自愈合复合钝化剂在黄铁矿上的钝化性能与机理
IF 8.131 2区 环境科学与生态学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-12 DOI: 10.1039/d4en00404c
Weifeng Wu, Mengke Li, Jiang Tian, Feng Li, Yun Liu
Acid mine drainage (AMD) is a harmful effluent from mining activities. Surface passivation technology can prevent AMD production by coating minerals with passivation films. Previous study reported a composite passivator comprising γ-mercaptopropyltrimethoxysilane (PropS-SH) and halloysite loaded with benzotriazole (BTA). However, two issues persist in this work: the organosilane-based passivator requires passivating pyrite at 50~100 °C, and the encapsulation method for the guest passivator in halloysite is limited. To address these challenges, a novel self-healing composite passivator (PLHP passivator) was synthesized, using PropS-SH and lawsone as the main passivation agents and halloysite loaded with 8-HQ as the nanofillers. Polyelectrolytes were employed as the encapsulant within the nanofillers. The formation of a hydrophobic coating on the PLHP coated pyrite surface was revealed by SEM and contact angle tests. The enhanced oxidation resistance of PLHP coated pyrite over raw pyrite and other coated pyrite was verified by electrochemical measurements and chemical leaching tests. Notably, the PLHP coatings could passivate pyrite at room temperature, exhibiting excellent long-term stability and self-healing ability. Furthermore, the incorporation of polyelectrolytes expanded the application range of guest passivator. This paper provides new insights into overcoming the limitations of organosilane-based passivation and self-healing methods in current technology.
酸性矿井排水(AMD)是采矿活动产生的一种有害废水。表面钝化技术可以通过在矿物表面镀上钝化膜来防止酸性矿井排水的产生。之前的研究报道了一种复合钝化剂,由γ-巯丙基三甲氧基硅烷(PropS-SH)和负载苯并三唑(BTA)的哈洛伊特组成。然而,这项工作仍存在两个问题:有机硅烷基钝化剂需要在 50~100 °C的温度下钝化黄铁矿,而将客体钝化剂封装在哈洛来石中的方法有限。为解决这些难题,研究人员以 PropS-SH 和 lawsone 为主要钝化剂,以含 8-HQ 的哈洛来石为纳米填料,合成了一种新型自修复复合钝化剂(PLHP 钝化剂)。纳米填料中使用了聚电解质作为封装剂。SEM 和接触角测试表明,PLHP 涂层黄铁矿表面形成了疏水涂层。电化学测量和化学浸出试验证实,PLHP 涂层黄铁矿的抗氧化性优于未加工的黄铁矿和其他涂层黄铁矿。值得注意的是,PLHP 涂层可在室温下钝化黄铁矿,表现出优异的长期稳定性和自修复能力。此外,聚电解质的加入扩大了客体钝化剂的应用范围。本文为克服现有技术中基于有机硅的钝化和自修复方法的局限性提供了新的见解。
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引用次数: 0
A design-phase Environmental Safe-and-Sustainable-by-Design Categorization Tool for the Development and Innovation of Nano-enabled Advanced Materials (AdMaCat) 用于纳米先进材料开发与创新的设计阶段环境安全与可持续设计分类工具 (AdMaCat)
IF 8.131 2区 环境科学与生态学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-12 DOI: 10.1039/d4en00068d
Analuisa Rubalcaba Medina, Fernando J. Rodríguez-Macías, Anders Baun, Steffen Foss Hansen
In support of the European Union’s circular economy action plans and its chemical strategy for sustainability, initiatives are being developed aimed at integrating ‘safe and sustainable by design’ (SSbD) principles and approaches in the development of chemicals and materials to promote a toxic-free environment. The expected widespread use of advanced materials (AdMa) underlines the need for addressing sustainability and environmental safety as early as possible in the material design. Here, we present AdMaCat, which is a SSbD first-tier screening categorization tool addressing environmental concerns of AdMa. The tool is aimed at the early design-phase in materials development, to enable a transparent and systematic evaluation of the functionality, safety, and sustainability of AdMa in a circular economy context. AdMaCat delivers a color coded output with design recommendations covering the material life-cycle stages manufacturing, use, and end-of-life. The applicability of AdMaCat is illustrated through a case study on organic aerogels for insulation purposes focusing on material and process selections, application, and waste management options. We conclude that AdMaCat can assist in identifying data gaps and inform decisions regarding the design of tailored AdMa by optimizing the balance of functionality, safety, and sustainability in a circular economy.
为支持欧盟的循环经济行动计划及其化学可持续发展战略,目前正在制定相关倡议,旨在将 "安全和可持续设计"(SSbD)原则和方法纳入化学品和材料的开发中,以促进无毒环境的形成。先进材料(AdMa)的预期广泛使用突出表明,有必要在材料设计中尽早解决可持续性和环境安全问题。在此,我们介绍 AdMaCat,这是一种 SSbD 一级筛选分类工具,用于解决 AdMa 的环境问题。该工具针对材料开发的早期设计阶段,能够在循环经济背景下对 AdMa 的功能性、安全性和可持续性进行透明、系统的评估。AdMaCat 以彩色编码输出设计建议,涵盖材料生命周期的制造、使用和报废阶段。AdMaCat 的适用性通过对用于绝缘目的的有机气凝胶的案例研究加以说明,重点关注材料和工艺选择、应用和废物管理选项。我们的结论是,AdMaCat 可以通过优化循环经济中的功能性、安全性和可持续性之间的平衡,帮助确定数据缺口,并为量身定制的 AdMa 设计提供决策依据。
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引用次数: 0
Outstanding Reviewers for Environmental Science: Nano in 2023 环境科学》杰出评审员:2023 年的纳米
IF 8.131 2区 环境科学与生态学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-12 DOI: 10.1039/d4en90023e
We would like to take this opportunity to thank all of Environmental Science: Nano's reviewers for helping to preserve quality and integrity in chemical science literature. We would also like to highlight the Outstanding Reviewers for Environmental Science: Nano in 2023.
我们想借此机会感谢《环境科学》杂志的所有审稿人,感谢他们帮助保持化学科学文献的质量和完整性:纳米》的审稿人帮助维护了化学科学文献的质量和完整性。我们还想特别提到《环境科学:纳米》的杰出审稿人:2023 年纳米》的杰出审稿人。
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引用次数: 0
Enhanced removal of As(III) by manganese-doped defective UiO-66 coupled peroxymonosulfate: multiple reactive oxygen species and system stability 锰掺杂缺陷 UiO-66 耦合过氧单硫酸盐增强对 As(III) 的去除:多种活性氧物种和系统稳定性
IF 8.131 2区 环境科学与生态学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-12 DOI: 10.1039/d4en00194j
Zihao Xie, Qingyun He, Shaobo Liu, Xinyi Huang, Mingyang Dai, Qiang Chen, Ang Sun, Jian Ye, Xiaofei Tan, Weihua Xu
Structurally defective UiO-66 has garnered significant interest due to its remarkable performance in the domains of adsorption and catalysis. In this research, the successful synthesis of Mn-doped defective UiO-66 (Mn1D40UiO-66) was confirmed by XRD and FTIR characterization. More than 95% of As(III) (C0 = 1.1 mg L−1) was removed in 1 h (Ccatalyst = 0.2 g L−1, CPMS = 0.1 mM). Compared with the original UiO-66, when coupled with peroxymonosulfate (PMS), Mn1D40UiO-66 accelerated the generation of reactive oxygen species (ROS), resulting in an increase in As(III) removal efficiency by about 50%. XPS spectra and EXAFS spectra indicated that As(III) adsorbed in the Mn1D40UiO-66/PMS system was fully oxidized to As(V) and the adsorption was attributed to As–O–Zr coordination. Several types of ROS (·OH, SO4˙, and O2˙) generated by PMS activation acted collectively on As(III) oxidation, so a single ROS scavenger did not have a marked inhibitory effect on As(III) removal. In addition, the system maintained efficiency over a broad pH range (3–11), and retained an arsenic removal rate higher than 89.8% even in the presence of high concentrations of several anions (SO42−/Cl/NO3, 10 mM). Meanwhile, 99.3% of the As(III) could be removed by Mn1D40UiO-66 at extremely high humic acid concentrations (100 mg L−1). Due to the excellent stability of the material, only trace amounts of metal leaching were detected (Mn ion ≤ 3 μg L−1) during the whole experiment. The whole oxidation and adsorption process demonstrated excellent anti-interference ability and stability. This study shows the great potential of transition metal doped defective metal–organic frameworks in the field of adsorption and catalysis and provides a novel idea for the high-efficiency management of As(III) pollution in water environments.
结构上有缺陷的 UiO-66 由于在吸附和催化领域的卓越性能而备受关注。本研究通过 XRD 和 FTIR 表征证实了掺锰缺陷 UiO-66 (Mn1D40UiO-66)的成功合成。在 1 小时内,95% 以上的 As(III)(C0 = 1.1 mg L-1)被去除(Ccatalyst = 0.2 g L-1,CPMS = 0.1 mM)。与原来的 UiO-66 相比,Mn1D40UiO-66 与过一硫酸盐 (PMS) 结合使用时,可加速活性氧 (ROS) 的生成,从而使 As(III) 的去除效率提高约 50%。XPS 光谱和 EXAFS 光谱表明,Mn1D40UiO-66/PMS 系统中吸附的 As(III) 被完全氧化为 As(V),吸附作用归因于 As-O-Zr 配位。PMS 活化产生的几种 ROS(-OH、SO4˙- 和 O2˙-)共同作用于 As(III)的氧化,因此单一的 ROS 清除剂对 As(III)的去除没有明显的抑制作用。此外,该系统在较宽的 pH 值范围(3-11)内都能保持高效率,即使在高浓度的几种阴离子(SO42-/Cl-/NO3-,10 mM)存在的情况下,砷去除率也能保持在 89.8%以上。同时,在腐殖酸浓度极高(100 mg L-1)的情况下,Mn1D40UiO-66 可以去除 99.3% 的 As(III)。由于该材料具有极佳的稳定性,在整个实验过程中仅检测到微量的金属浸出(锰离子≤ 3 μg L-1)。整个氧化和吸附过程表现出了卓越的抗干扰能力和稳定性。该研究显示了掺杂过渡金属的缺陷金属有机框架在吸附催化领域的巨大潜力,为高效治理水环境中的 As(III) 污染提供了新思路。
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引用次数: 0
A metal-free photocatalytic active hybrid fiber as a novel self-cleaning adsorbent for enhanced tetracycline removal 一种作为新型自清洁吸附剂的无金属光催化活性杂化纤维,可提高四环素的去除率
IF 8.131 2区 环境科学与生态学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-12 DOI: 10.1039/d4en00387j
Kaijie Ni, Ruiqi Xu, Yanlong Chen, Ming Guo
Metal-free photocatalytic degradation of pollutant is an eco-friendly green method for wastewater remediation. Herein we reported using amine modified alginate as anchor line, graphene oxide (GO) and carbon nanotubes (CNT) as photoactive units to fabricate a recyclable metal-free photocatalytic active hybrid fiber via facile carbodiimine-mediated amide coupling and calcium ion crosslinking. The results show that the photoactive fiber with unique microporosity and enhanced thermal stability has been successfully prepared. The prepared fiber presented a significantly photo-enhanced removal effect on tetracycline (TC). The efficiency of TC removal promoted by the fiber under solar irradiation is 10 times higher than that under dark. In the photocatalytic treatment of TC, the fiber also showed higher TC removal efficiency than that of GO and CNT alone synergistic effect of GO/CNT. Electron spin resonance analysis confirmed that the fiber under solar irradiation induced to the generation of 1O2 and hole (h+) which degraded TC. UV-vis spectra analysis indicated that GO and CNT components in the fiber promoted TC to undergo oxidative degradation. Major transformation products during TC removal were identified with Liquid chromatography mass spectrometry. Finally, such photoactivity of the fiber can be utilized to develop a convenient irradiation/agitation regeneration approach to make the fiber adsorbent reusable. The recycled fiber maintained an excellent level of TC removal performance after multiple recycling steps. Overall, this study provides a new strategy of preparing a recycled metal-free photocatalytic material for water treatment, and is of great reference value for research in this field.
无金属光催化降解污染物是一种环保的绿色废水修复方法。本文报道了以胺修饰的海藻酸盐为锚线,氧化石墨烯(GO)和碳纳米管(CNT)为光活性单元,通过简便的碳化二亚胺介导的酰胺偶联和钙离子交联,制备出一种可回收的无金属光催化活性杂化纤维。结果表明,所制备的光活性纤维具有独特的微孔和更高的热稳定性。所制备的纤维对四环素(TC)具有明显的光增强去除效果。该纤维在太阳光照射下对四环素(TC)的去除效率是黑暗环境下的 10 倍。在光催化处理四环素的过程中,纤维对四环素的去除效率也高于单独使用 GO 和 CNT 的效果。电子自旋共振分析证实,在太阳光照射下,纤维会诱导产生 1O2 和空穴(h+),从而降解 TC。紫外-可见光谱分析表明,纤维中的 GO 和 CNT 成分促进了 TC 的氧化降解。液相色谱质谱法确定了去除 TC 过程中的主要转化产物。最后,纤维的这种光活性可用于开发一种方便的辐照/搅拌再生方法,使纤维吸附剂可重复使用。再生纤维在经过多个再生步骤后,仍能保持出色的三氯乙酸去除性能。总之,本研究为制备用于水处理的再生无金属光催化材料提供了一种新策略,对该领域的研究具有重要的参考价值。
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引用次数: 0
MOF-5 Fortified Fiber Optic Plasmonic Absorption-based Pb(II) Ion Sensor for Rapid Water Quality Monitoring 用于快速水质监测的 MOF-5 强化光纤质子吸收型铅(II)离子传感器
IF 8.131 2区 环境科学与生态学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-11 DOI: 10.1039/d4en00197d
Swetha Menon, Sourav Dutta, Narayanan Madaboosi, V. V. R. Sai
Precise detection of heavy metal ions in water is of paramount importance owing to its detrimental effects on human health, especially with spectroscopically silent ions such as lead ions (Pb(II)). This study demonstrates the design and development of a novel portable and field-deployable fiber optic plasmonic absorption-based chemical sensor (PACS) for Pb(II) ion detection using a metal-organic framework (MOF-5) as a highly selective chemoreceptor. MOF-5 was grown in situ over the tannic acid-capped gold nanoparticles (AuNP, 20 nm) of the plasmonic U-bent fiber optic sensor (U-FOS) probes. The Pb(II) ion binding to MOF-5 was detected and quantified as an increase in the plasmonic absorption of the light by AuNP due to significant refractive index changes at the AuNP surface. Besides an excellent selectivity (Pb(II) vs. 11 potential interfering metal ions at 1:50 ppm), these sensors manifest a detection limit down to 0.5 ppb (20 times below the maximum contaminant level of 10 ppb), a wide dynamic range (0.5 ppb to 50 ppm). The sensor was challenged with filtered sewage samples (neat and spiked with 10 ppb) yielded recovery rates within 91% to 105% with respect to the standard ICP-MS analysis. With the notable merits of a facile and scalable probe fabrication process, long shelf-life (at least 12 weeks moisture-free storage), and simpler instrumentation (only with an LED-photodetector pair), the PACS/MOF-5 platform is highly promising for water quality measurements on-site.
由于水中重金属离子对人体健康的有害影响,尤其是铅离子(Pb(II))等光谱上无声的离子,因此精确检测水中的重金属离子至关重要。本研究利用金属有机框架(MOF-5)作为高选择性化学感受器,设计并开发了一种新型便携式、可现场部署的光纤质子吸收型化学传感器(PACS),用于检测铅(II)离子。MOF-5 是在等离子 U 型弯曲光纤传感器(U-FOS)探针的单宁酸封端金纳米粒子(AuNP,20 nm)上原位生长的。由于 AuNP 表面的折射率发生了显著变化,因此 AuNP 对光的等离子吸收增加,从而检测并量化了与 MOF-5 结合的铅(II)离子。除了出色的选择性(Pb(II) 与 11 种潜在干扰金属离子的比值为 1:50 ppm)外,这些传感器的检测限低至 0.5 ppb(比 10 ppb 的最大污染物水平低 20 倍),动态范围宽(0.5 ppb 至 50 ppm)。与标准的 ICP-MS 分析相比,该传感器对过滤后的污水样本(纯净样本和添加了 10 ppb 的样本)的回收率在 91% 至 105% 之间。PACS/MOF-5 平台具有以下显著优点:探头制造工艺简单、可扩展、保存期长(至少 12 周无湿储存)、仪器更简单(仅使用一对 LED 光电探测器),因此非常适合现场水质测量。
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引用次数: 0
Uptake and physiological impacts of nanoplastics in trees with divergent water use strategies 不同用水策略的树木对纳米塑料的吸收和生理影响
IF 8.131 2区 环境科学与生态学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-11 DOI: 10.1039/d4en00286e
Maria Elvira Murazzi, Alice Pradel, Roman B. Schefer, Arthur Gessler, Denise M. Mitrano
Anthropogenic contaminants can place significant stress on vegetation, especially when they are taken up into plants. Plastic pollution, including nanoplastics (NPs), could be detrimental to tree functioning, by causing, for example, oxidative stress or reducing photosynthesis. While a number of studies have explored the capacity of plants to take up NPs, few have simultaneously assessed the functional damage due to particulate matter uptake. To quantify NPs uptake by tree roots and to determine whether this resulted in subsequent physiological damage, we exposed the roots of two tree species with different water use strategies in hydroponic cultures to two concentrations (10 mg L−1 and 30 mg L−1) of model metal-doped polystyrene NPs. This approach allowed us to accurately quantify low concentrations of NPs in tissues using standard approaches for metal analysis. The two contrasting tree species included Norway spruce (Picea abies [L.] Karst), a water conservative tree, and wild service tree (Sorbus torminalis [L.] Crantz), an early successional tree with a rather water spending strategy. At both exposure concentrations and at each of the experimental time points (two and four weeks), NPs were highly associated and/or concentrated inside the tree roots. In both species, maximum concentrations were observed after 2 weeks in the roots of the high concentration (HC) treatment (spruce: 2512 ± 304 μg NPs per g DW (dry weight), wild service tree: 1190 ± 823 μg NPs per g DW). In the aboveground organs (stems and leaves or needles), concentrations were one to two orders of magnitude lower than in the roots. Despite relatively similar NPs concentrations in the tree aboveground organs across treatments, there were different temporal impacts on tree physiology of the given species. Photosynthetic efficiency was reduced faster (after 2 weeks of NPs exposure) and more intensively (by 28% in the HC treatment) in wild service trees compared to Norway spruce (ca. 10% reduction only after 4 weeks). Our study shows that both, evergreen coniferous as well as deciduous broadleaf tree species are negatively affected in their photosynthesis by NPs uptake and transport to aboveground organs. Given the likelihood of trees facing multiple, concurrent stressors from anthropogenic pollution and climate change, including the impact of NPs, it is crucial to consider the cumulative effects on vegetation in future.
人为污染物会对植被造成巨大压力,尤其是当它们被植物吸收时。包括纳米塑料(NPs)在内的塑料污染可能会对树木的功能造成损害,例如造成氧化应激或降低光合作用。虽然许多研究都探讨了植物吸收 NPs 的能力,但很少有研究同时评估了吸收颗粒物质所造成的功能损害。为了量化树木根系对 NPs 的吸收,并确定这是否会导致随后的生理损害,我们将水培法培养的两种不同用水策略的树木根系暴露于两种浓度(10 毫克/升-1 和 30 毫克/升-1)的模型掺金属聚苯乙烯 NPs 中。这种方法使我们能够利用金属分析的标准方法准确量化组织中的低浓度 NPs。两种截然不同的树种包括挪威云杉(Picea abies [L.] Karst)和野役树(Sorbus torminalis [L.] Crantz),前者是一种节约用水的树种,后者则是一种早期演替树种,具有相当的耗水策略。在两种接触浓度和每个实验时间点(两周和四周),NPs 都与树根高度相关和/或集中在树根内部。在这两种树种中,高浓度(HC)处理的树根在 2 周后浓度最高(云杉:2512 ± 304 μg NPs per g DW(干重);野役树:1190 ± 823 μg NPs per g DW(干重)):1190 ± 823 μg NPs/克干重)。地上部分(茎、叶或针叶)的 NPs 浓度比根部低一到两个数量级。尽管不同处理中树木地上器官中的 NPs 浓度相对相似,但对特定物种的树木生理产生的时间影响却不同。与挪威云杉(4 周后才降低约 10%)相比,野生役用树的光合作用效率降低得更快(接触 NPs 2 周后)、更严重(在 HC 处理中降低了 28%)。我们的研究表明,常绿针叶树种和落叶阔叶树种的光合作用都会受到 NPs 吸收和传输到地上器官的负面影响。鉴于树木可能同时面临人为污染和气候变化等多重压力,包括氮磷的影响,因此考虑未来对植被的累积影响至关重要。
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引用次数: 0
Self-cycled photocatalytic Fenton system and rapid degradation of organic pollutants over magnetic 3D MnS nanosheet/iron-nickel foam 自循环光催化 Fenton 系统和磁性 3D MnS 纳米片/铁-镍泡沫对有机污染物的快速降解
IF 8.131 2区 环境科学与生态学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-11 DOI: 10.1039/d4en00452c
Xiaoqian Ma, Yu Liu, Yi Zhao, Xiaohong Chen, Junyang Leng, Anlong Zhang, Daomei Chen, Kai Xiong, Jiaqiang Wang
The photocatalysis self-Fenton systems by coupling photocatalysis and Fenton technology overcome the limitations of conventional Fenton reactions by in-situ generation and activation of H2O2. While a considerable amount of iron sludge is still produced. In this study, we develop a novel self-cycled photocatalytic Fenton process for the degradation of organic pollutants via an iron-nickel foam-supported MnS nanosheet (MnS/INF). Without the external addition of both H2O2 and ferrous ions, MnS/INF 3D Z-scheme heterojunction exhibited an extremely high H2O2 production rate of 25.4 mM h-1 g-1 under visible light irradiation, which is 2119 times than those reported photocatalysis self-Fenton system in the literature. The photogenerated electrons of MnS/INF can participate in the Fe2+/Fe3+ cycle process to promote H2O2 activation, significantly enhancing the catalytic performance owing to the formation of a 3D Z-scheme heterojunction. DFT calculations indicate that MnS/INF can lower the energy barrier of *OOH formation and result in an enhanced photocatalytic activity of H2O2 production. Magnetic MnS/INF was easily recycled, remained very stable, and mitigated the extra undesirable Fe-containing sludge and only little iron sludge (0.43 mmol/L) is produced after nine cycles of reuse. Furthermore, a large (100 cm2) MnS/INF was used for an unassisted solar-driven in situ photocatalytic H2O2 production and rapid degradation of RhB with requirements for only water, oxygen and sunlight. In addition, MnS/INF also exhibited good performance in real wastewater containing fluoronitrobenzene from a factory (initial COD 2310 mg/L) and wastewater from sewage treatment station (initial COD 106 mg/L). This work may provide leverage to minimize iron sludge from the Fenton reaction's source.
光催化自 Fenton 系统将光催化和 Fenton 技术相结合,通过原位生成和活化 H2O2,克服了传统 Fenton 反应的局限性。尽管如此,仍会产生大量铁污泥。在本研究中,我们开发了一种新型自循环光催化 Fenton 工艺,通过铁镍泡沫支撑的 MnS 纳米片(MnS/INF)降解有机污染物。在不外加 H2O2 和亚铁离子的情况下,MnS/INF 三维 Z 型异质结在可见光照射下的 H2O2 产率高达 25.4 mM h-1 g-1,是文献报道的光催化自 Fenton 系统的 2119 倍。由于形成了三维 Z 型异质结,MnS/INF 光生电子可参与 Fe2+/Fe3+ 循环过程,促进 H2O2 活化,显著提高催化性能。DFT 计算表明,MnS/INF 可以降低 *OOH 形成的能垒,从而提高产生 H2O2 的光催化活性。磁性 MnS/INF 易于循环使用,保持非常稳定,并能减少额外的不良含铁污泥,在循环使用九次后仅产生少量铁污泥(0.43 mmol/L)。此外,大型(100 平方厘米)MnS/INF 被用于无辅助太阳能驱动的原位光催化 H2O2 生产和 RhB 的快速降解,只需要水、氧气和阳光。此外,MnS/INF 在处理来自工厂的含氟硝基苯废水(初始 COD 2310 mg/L)和来自污水处理站的废水(初始 COD 106 mg/L)时也表现出良好的性能。这项工作可为尽量减少来自 Fenton 反应源的铁污泥提供杠杆作用。
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引用次数: 0
Synthesis of N-doped porous carbon derived from biomass waste for activating peroxymonosulfate in water decontamination: Mechanism insight and biotoxicity assessment 从生物质废弃物中合成掺杂 N 的多孔碳,用于活化水污染中的过硫酸盐:机理研究与生物毒性评估
IF 8.131 2区 环境科学与生态学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-10 DOI: 10.1039/d4en00481g
Shun Ding, FANGYU FU, Huibin Niu, Jiaying Yan, Yanfen Fang, Xiang Liu
N-doping is a widely used strategy for the synthesis of highly efficient carbon nanocatalysts, however, an in-depth understanding of the effect of nitrogen source on the intrinsic structure and catalytic performance is highly desired. Therefore, to kill two birds with one stone, a series of N-doped carbon nanomaterials were synthesized from the pyrolysis of biomass waste (dealkali lignin) and various nitrogen sources (including melamine, dicyandiamide, and urea). Even though N-doping nanocatalysts showed better catalytic activity than the HCNs (pyrolysis form only dealkali lignin) for sulfamethoxazole (SMX) degradation via peroxymonosulfate (PMS) activation, NCN-1 and NCN-2 presented contractive and small spherical structures when melamine and dicyandiamide with high nitrogen content were added, showing relatively low catalytic efficiency. NPCN derived from dealkali lignin and urea led to the formation of a porous cluster structure with abundant active species of graphitic C/N and C-OH, which showed the best catalytic performance for SMX degradation. Significantly, NPCN exhibited excellent universality, adaptability, and reusability. Moreover, the possible mechanism was proposed based on the quenching study, EPR analysis, electronic quenching experiment, DFT calculation, and HR-MS, confirming that e−, 1O2, •OH, SO4•−, and O2•− were the active species, of which 1O2 was the dominating one in NPCN/PMS system. In addition, the biotoxicity of SMX was evaluated by the ECOSAR analysis and germination tests of wheat seeds. This work provides how the nitrogen source would affect the microstructure-dependent catalytic activity of metal-free carbon nanocatalysts for water decontamination.
氮掺杂是合成高效碳纳米催化剂的一种广泛应用的策略,然而,深入了解氮源对其内在结构和催化性能的影响是非常必要的。因此,为了一石二鸟,研究人员利用生物质废料(脱碱木质素)热解和各种氮源(包括三聚氰胺、双氰胺和尿素)合成了一系列氮掺杂碳纳米材料。在通过过一硫酸盐(PMS)活化降解磺胺甲噁唑(SMX)方面,尽管掺杂氮的纳米催化剂比 HCN(热解形式仅为脱碱木质素)显示出更好的催化活性,但当添加含氮量较高的三聚氰胺和双氰胺时,NCN-1 和 NCN-2 出现收缩和小球形结构,显示出相对较低的催化效率。从脱碱木质素和尿素中提取的 NPCN 可形成多孔团簇结构,其中含有丰富的石墨 C/N 和 C-OH 活性物种,对 SMX 降解具有最佳催化性能。值得注意的是,NPCN 具有优异的通用性、适应性和可重复使用性。此外,根据淬灭研究、EPR分析、电子淬灭实验、DFT计算和HR-MS,提出了可能的机理,证实了e-、1O2、-OH、SO4-和O2-是活性物种,其中1O2在NPCN/PMS体系中占主导地位。此外,还通过 ECOSAR 分析和小麦种子发芽试验评估了 SMX 的生物毒性。这项研究提供了氮源如何影响用于水净化的无金属碳纳米催化剂的微结构催化活性。
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引用次数: 0
Catalytic activity of Cu-cysteine coated on Ti3C2MXene toward peroxymonosulfate activation for carbamazepine degradation 涂覆在 Ti3C2MXene 上的半胱氨酸铜对过一硫酸活化降解卡马西平的催化活性
IF 8.131 2区 环境科学与生态学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-10 DOI: 10.1039/d4en00342j
Pascaline Sanga, Haitham Saad Al-mashriqi, Jing Xiao, Jia Chen, Hongdeng Qiu
The growing prevalence of pharmaceutical pollutants in water bodies poses a significant threat to the enviromnent, underscoring the urgent need for more effective and sustainable methods for removing these pollutants. This study introduces a novel technique for degrading carbamazepine (CBZ), based on a peroxymonosulfate (PMS) oxidation system catalysed by a Copper-cysteine/Ti3C2MXene composite (Cu-cy/Ti3C2MXene), denoted as CCM. CCM was initially prepared by growing Cu-cy nanoparticles on MXene sheet to make Cu-cy/Ti3C2MXene. CCM was then utilized to activate PMS, facilitating the generation of reactive oxygen species necessary for decomposing CBZ. The CCM+PMS system demonstrated a remarkable 98.6% degradation rate of CBZ within 20 min, outperforming the pristine Cu-cy nanoparticles and Ti3C2MXene when applied in same conditions. Furthermore, to examine the vital contribution of reactive oxygen species in the degradation process, experiments focused on quenching reactions and electron paramagnetic resonance (EPR) analysis demonstrated that both radical species, including sulfate radicals (SO4•-) and hydroxyl radicals (•OH), and non-radical species such as singlet oxygen (1O2), were involved in the degradation of CBZ with non-radical species (1O2) exerting a predominant role. Notably, the synthesized material showed excellent reusability and stability in multiple cycles of CBZ degradation. These findings highlight the effectiveness of the CCM+PMS system in addressing water pollution issues caused by CBZ.
水体中的药物污染物日益普遍,对环境构成了严重威胁,因此迫切需要更有效、更可持续的方法来清除这些污染物。本研究介绍了一种降解卡马西平(CBZ)的新技术,该技术基于由铜-半胱氨酸/Ti3C2MXene 复合材料(Cu-cy/Ti3C2MXene)催化的过一硫酸盐(PMS)氧化系统,简称 CCM。CCM 最初是通过在 MXene 片材上生长 Cu-cy 纳米颗粒来制备 Cu-cy/Ti3C2MXene。然后利用 CCM 激活 PMS,促进产生分解 CBZ 所需的活性氧。CCM+PMS 系统在 20 分钟内对 CBZ 的降解率高达 98.6%,在相同条件下优于原始 Cu-cy 纳米粒子和 Ti3C2MXene。此外,为了研究活性氧在降解过程中的重要作用,实验重点放在淬灭反应和电子顺磁共振(EPR)分析上,结果表明硫酸根自由基(SO4--)和羟基自由基(-OH)等自由基物种和单线态氧(1O2)等非自由基物种都参与了 CBZ 的降解,其中非自由基物种(1O2)发挥了主要作用。值得注意的是,合成的材料在 CBZ 的多次降解循环中表现出卓越的可重复使用性和稳定性。这些发现凸显了 CCM+PMS 系统在解决 CBZ 造成的水污染问题方面的有效性。
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引用次数: 0
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Environmental Science: Nano
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