Reducing Arsenic Mobilization in Sediments: A Synergistic Effect of Oxidation and Adsorption with Zirconium-Manganese Binary Metal Oxides

IF 11.4 1区环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL

Water Research Pub Date : 2025-05-09 DOI:10.1016/j.watres.2025.123798

Xue Jiang, Youzi Gong, Jiaxing Xiong, Boxian Ren, Yewei Qiu, Zhiguo Lin, Ying Tang, Shixiong Wang, Xiaolong Wang, Cai Li, Xiangjun Yang, Shiming Ding

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Abstract

Remediation of arsenic (As)-contaminated sediments is challenging, due to surface sediment often being subjected to hypoxic/anoxic conditions where As(Ⅲ) is the dominant species. In this study, a novel capping material comprising zirconium-manganese binary oxides (ZMBO) was synthesized and its feasibility in controlling sedimentary As release investigated using high-resolution sampling, X-ray absorption near edge structure (XANES) spectroscopy, and scanning electron microscopy (SEM) techniques. Results showed ZMBO exhibited both high oxidation efficiency (94%) and strong adsorption capacity (151.8 mg As/g) for As(Ⅲ). Capping As-contaminated sediments with ZMBO resulted in a negative diffusive flux of −0.08 ng/cm²/s, effectively maintaining low As levels in the overlying water over 150 days. XANES spectra showed As in surface sediments existed predominantly as As(V), consistent with high-resolution data indicating ∼90% of labile As(Ⅲ) was oxidized and adsorbed by ZMBO. Furthermore, ZMBO also promoted Fe(Ⅱ) oxidation to stable hematite in sediments, providing additional adsorption sites for As. By comparing with current capping materials, ZMBO exhibited a balanced performance in terms of its cost-effectiveness, adsorption capacity, remediation effects, and environmental adaptability. This study highlights the potential of ZMBO as a promising capping material for remediating As-contaminated sediments through combined chemical oxidation and adsorption mechanisms, offering sustainable solutions for improving water quality management worldwide.

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还原沉积物中砷的动员：氧化和吸附与锆锰二元金属氧化物的协同作用

砷（As）污染沉积物的修复具有挑战性，因为地表沉积物经常处于缺氧/缺氧条件下，其中As（Ⅲ）是优势物种。在这项研究中，合成了一种由锆锰二元氧化物（ZMBO）组成的新型盖层材料，并利用高分辨率采样、x射线吸收近边缘结构（XANES）光谱和扫描电子显微镜（SEM）技术研究了其控制沉积砷释放的可行性。结果表明，ZMBO对As（Ⅲ）具有较高的氧化效率（94%）和较强的吸附能力（151.8 mg As/g）。用ZMBO覆盖受砷污染的沉积物，导致−0.08 ng/cm2/s的负扩散通量，在150天内有效地维持了上覆水体的低砷水平。XANES光谱显示，表面沉积物中的As主要以As(V)的形式存在，这与高分辨率数据一致，表明~ 90%的活性As（Ⅲ）被ZMBO氧化和吸附。此外，ZMBO还促进了沉积物中Fe（Ⅱ）氧化为稳定的赤铁矿，为As提供了额外的吸附位点。与现有封盖材料相比，ZMBO在成本效益、吸附能力、修复效果和环境适应性方面表现出平衡的性能。该研究强调了ZMBO作为一种有前途的封盖材料的潜力，它可以通过化学氧化和吸附机制联合修复砷污染的沉积物，为改善全球水质管理提供可持续的解决方案。

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来源期刊

Water Research 环境科学-工程：环境

CiteScore

20.80

自引率

9.40%

发文量

1307

审稿时长

38 days

期刊介绍： Water Research, along with its open access companion journal Water Research X, serves as a platform for publishing original research papers covering various aspects of the science and technology related to the anthropogenic water cycle, water quality, and its management worldwide. The audience targeted by the journal comprises biologists, chemical engineers, chemists, civil engineers, environmental engineers, limnologists, and microbiologists. The scope of the journal include: •Treatment processes for water and wastewaters (municipal, agricultural, industrial, and on-site treatment), including resource recovery and residuals management; •Urban hydrology including sewer systems, stormwater management, and green infrastructure; •Drinking water treatment and distribution; •Potable and non-potable water reuse; •Sanitation, public health, and risk assessment; •Anaerobic digestion, solid and hazardous waste management, including source characterization and the effects and control of leachates and gaseous emissions; •Contaminants (chemical, microbial, anthropogenic particles such as nanoparticles or microplastics) and related water quality sensing, monitoring, fate, and assessment; •Anthropogenic impacts on inland, tidal, coastal and urban waters, focusing on surface and ground waters, and point and non-point sources of pollution; •Environmental restoration, linked to surface water, groundwater and groundwater remediation; •Analysis of the interfaces between sediments and water, and between water and atmosphere, focusing specifically on anthropogenic impacts; •Mathematical modelling, systems analysis, machine learning, and beneficial use of big data related to the anthropogenic water cycle; •Socio-economic, policy, and regulations studies.