{"title":"饱和多孔介质中铁水有机物胶体与锑(V)的共迁移:对锑迁移率的影响","authors":"Wenjian Mao, Dengjun Wang, Pan Wu, Jian Zhu, Peng Liao, Kaidi Lai, Zihan Ding, Yuqin Zhang, Zhongxu He, Ruyi Zheng and Yonglin Chen","doi":"10.1039/D3EN00701D","DOIUrl":null,"url":null,"abstract":"<p >Both iron (Fe) and organic matter (OM) occur ubiquitously in the subsurface environment that draws tremendous attention for its impact on the fate and transport of antimony (Sb). The importance of Fe–OM colloids on the transport of Sb(<small>V</small>) is severely unappreciated. This study provides new insight regarding the mechanisms of FH–OM colloids (ferrihydrite–humic acid (FH–HA)) on the transport of Sb(<small>V</small>) in a water-saturated sand column. Batch experiments in conjunction with characterization show that Sb(<small>V</small>) can bind with FH–HA colloids over a range of pH (3.0–7.5), ionic strength (IS, 1–5 mM NaCl), and HA and FH concentrations. Results show that the transport of FH–HA colloids loaded with Sb(<small>V</small>) is highly dependent on pH and IS. The presence of 1 mg C per L HA or low pH (3.0 and 4.5) significantly hindered FH–HA–Sb(<small>V</small>) transport with most particles being retained on the quartz sand surface. Increasing pH and HA concentrations enhanced the transport of FH–HA colloids and thus promoted Sb(<small>V</small>) mobility because of the increasing electrostatic repulsion. Colloid filtration theory (CFT) calculations show the maximum transport distance (<em>L</em><small><sub>0.01</sub></small> >59.6 m) of colloids under favorable conditions (<em>e.g.</em>, HA ≥5 mg C per L at pH ≥6.0), as also reflected by the low attachment efficiency (<em>α</em> <1.2 × 10<small><sup>−8</sup></small>) and low deposition rate coefficient (<em>k</em><small><sub>d</sub></small> <1.3 × 10<small><sup>−6</sup></small>). Additionally, Derjaguin–Landau–Verwey–Overbeek (DLVO) theory calculations elucidate the interaction energy between colloids and quartz sand, showing higher repulsive energy barriers (54.6 <em>kT</em> for ≥5.0 mg C per L HA) under unfavorable retention conditions. Further, a non-equilibrium two-site model and a two-site kinetic attachment/detachment model successfully captured the breakthrough curves of FH–HA colloids with Sb(<small>V</small>). Collectively, our findings update crucial perception into the importance of FH–OM colloids on the mobility of Sb(<small>V</small>), which is valuable for the management and remediation of Sb-contaminated sites.</p>","PeriodicalId":73,"journal":{"name":"Environmental Science: Nano","volume":" 4","pages":" 1462-1476"},"PeriodicalIF":5.8000,"publicationDate":"2024-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Co-transport of ferrihydrite–organic matter colloids with Sb(v) in saturated porous media: implications for antimony mobility†\",\"authors\":\"Wenjian Mao, Dengjun Wang, Pan Wu, Jian Zhu, Peng Liao, Kaidi Lai, Zihan Ding, Yuqin Zhang, Zhongxu He, Ruyi Zheng and Yonglin Chen\",\"doi\":\"10.1039/D3EN00701D\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Both iron (Fe) and organic matter (OM) occur ubiquitously in the subsurface environment that draws tremendous attention for its impact on the fate and transport of antimony (Sb). The importance of Fe–OM colloids on the transport of Sb(<small>V</small>) is severely unappreciated. This study provides new insight regarding the mechanisms of FH–OM colloids (ferrihydrite–humic acid (FH–HA)) on the transport of Sb(<small>V</small>) in a water-saturated sand column. Batch experiments in conjunction with characterization show that Sb(<small>V</small>) can bind with FH–HA colloids over a range of pH (3.0–7.5), ionic strength (IS, 1–5 mM NaCl), and HA and FH concentrations. Results show that the transport of FH–HA colloids loaded with Sb(<small>V</small>) is highly dependent on pH and IS. The presence of 1 mg C per L HA or low pH (3.0 and 4.5) significantly hindered FH–HA–Sb(<small>V</small>) transport with most particles being retained on the quartz sand surface. Increasing pH and HA concentrations enhanced the transport of FH–HA colloids and thus promoted Sb(<small>V</small>) mobility because of the increasing electrostatic repulsion. Colloid filtration theory (CFT) calculations show the maximum transport distance (<em>L</em><small><sub>0.01</sub></small> >59.6 m) of colloids under favorable conditions (<em>e.g.</em>, HA ≥5 mg C per L at pH ≥6.0), as also reflected by the low attachment efficiency (<em>α</em> <1.2 × 10<small><sup>−8</sup></small>) and low deposition rate coefficient (<em>k</em><small><sub>d</sub></small> <1.3 × 10<small><sup>−6</sup></small>). Additionally, Derjaguin–Landau–Verwey–Overbeek (DLVO) theory calculations elucidate the interaction energy between colloids and quartz sand, showing higher repulsive energy barriers (54.6 <em>kT</em> for ≥5.0 mg C per L HA) under unfavorable retention conditions. Further, a non-equilibrium two-site model and a two-site kinetic attachment/detachment model successfully captured the breakthrough curves of FH–HA colloids with Sb(<small>V</small>). 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引用次数: 0
摘要
铁(Fe)和有机物(OM)在地下环境中无处不在,它们对锑(Sb)的归宿和迁移的影响引起了人们的极大关注。铁-有机质胶体对锑(V)迁移的重要性还没有得到充分认识。本研究提供了有关 FH-OM 胶体(铁矾土-腐植酸(FH-HA))对水饱和砂柱中 Sb(V)迁移机制的新见解。结合表征进行的批量实验表明,在一定的 pH 值(3.0-7.5)、离子强度(IS,1-5 mM NaCl)以及 HA 和 FH 浓度范围内,Sb(V) 可与 FH-HA 胶体结合。结果表明,装载了 Sb(V)的 FH-HA 胶体的传输高度依赖于 pH 值和 IS。每升 HA 含 1 毫克 C 或低 pH 值(3.0 和 4.5)明显阻碍了 FH-HA-Sb(V) 的迁移,大多数颗粒被保留在石英砂表面。提高 pH 值和 HA 浓度可增强 FH-HA 胶体的迁移,从而促进 Sb(V) 的迁移,因为静电排斥力在增加。胶体过滤理论(CFT)计算显示,在有利条件下(例如,pH ≥6.0 时 HA ≥5 mg C per L),胶体的最大传输距离(L0.01 >59.6 m),这也反映在低附着效率(α <1.2×10-8)和低沉积速率系数(kd <1.3×10-6)上。此外,Derjaguin-Landau-Verwey-Overbeek(DLVO)理论计算阐明了胶体与石英砂之间的相互作用能,显示出在不利的保留条件下存在较高的排斥能垒(54.6 kT,每升 HA 含≥5.0 mg C)。此外,非平衡双位点模型和双位点动力学附着/脱离模型成功地捕捉到了 FH-HA 胶体与 Sb(V) 的突破曲线。总之,我们的研究结果更新了人们对 FH-OM 胶体对锑(V)迁移率重要性的重要认识,这对锑污染场地的管理和修复很有价值。
Co-transport of ferrihydrite–organic matter colloids with Sb(v) in saturated porous media: implications for antimony mobility†
Both iron (Fe) and organic matter (OM) occur ubiquitously in the subsurface environment that draws tremendous attention for its impact on the fate and transport of antimony (Sb). The importance of Fe–OM colloids on the transport of Sb(V) is severely unappreciated. This study provides new insight regarding the mechanisms of FH–OM colloids (ferrihydrite–humic acid (FH–HA)) on the transport of Sb(V) in a water-saturated sand column. Batch experiments in conjunction with characterization show that Sb(V) can bind with FH–HA colloids over a range of pH (3.0–7.5), ionic strength (IS, 1–5 mM NaCl), and HA and FH concentrations. Results show that the transport of FH–HA colloids loaded with Sb(V) is highly dependent on pH and IS. The presence of 1 mg C per L HA or low pH (3.0 and 4.5) significantly hindered FH–HA–Sb(V) transport with most particles being retained on the quartz sand surface. Increasing pH and HA concentrations enhanced the transport of FH–HA colloids and thus promoted Sb(V) mobility because of the increasing electrostatic repulsion. Colloid filtration theory (CFT) calculations show the maximum transport distance (L0.01 >59.6 m) of colloids under favorable conditions (e.g., HA ≥5 mg C per L at pH ≥6.0), as also reflected by the low attachment efficiency (α <1.2 × 10−8) and low deposition rate coefficient (kd <1.3 × 10−6). Additionally, Derjaguin–Landau–Verwey–Overbeek (DLVO) theory calculations elucidate the interaction energy between colloids and quartz sand, showing higher repulsive energy barriers (54.6 kT for ≥5.0 mg C per L HA) under unfavorable retention conditions. Further, a non-equilibrium two-site model and a two-site kinetic attachment/detachment model successfully captured the breakthrough curves of FH–HA colloids with Sb(V). Collectively, our findings update crucial perception into the importance of FH–OM colloids on the mobility of Sb(V), which is valuable for the management and remediation of Sb-contaminated sites.
期刊介绍:
Environmental Science: Nano serves as a comprehensive and high-impact peer-reviewed source of information on the design and demonstration of engineered nanomaterials for environment-based applications. It also covers the interactions between engineered, natural, and incidental nanomaterials with biological and environmental systems. This scope includes, but is not limited to, the following topic areas:
Novel nanomaterial-based applications for water, air, soil, food, and energy sustainability
Nanomaterial interactions with biological systems and nanotoxicology
Environmental fate, reactivity, and transformations of nanoscale materials
Nanoscale processes in the environment
Sustainable nanotechnology including rational nanomaterial design, life cycle assessment, risk/benefit analysis