Microenvironment modulation of two-dimensional defective carbon nitride with extended nanoporous furnished oxygen-enriched sites for efficient recovery of rare earth elements

IF 11.3 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Journal of Hazardous Materials Pub Date : 2025-06-05 Epub Date: 2025-02-10 DOI:10.1016/j.jhazmat.2025.137568
Hui Cai , Meng Rong , Siqi Liang , Qike Wang , Qiyu Meng , Shan Ni , Huizhou Liu , Liangrong Yang
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Abstract

Efficient recovery of rare earth elements (REEs) from wastewater is crucial for environmental remediation and the sustainable development of resources. Nevertheless, achieving efficient and selective REEs extraction in the systems containing low-concentration REEs and high-concentration competing metal ions remains a challenge. Here, we report on the fabrication of two-dimensional defective carbon nitride (DGCN-K) with extended nanoporous furnished oxygen-enriched sites, which is achieved through re-arrangement of framework structural unit using a flexible polycondensation-ion-thermal strategy. The extended nanoporous and continuous transmission nanochannels establish a dedicated structure microenvironment surrounding the active sites center, promoting the effective ion diffusion and increasing the accessibility of active sites. Meanwhile, the incorporation of abundant electronegative cyano and hydroxyl group modifies coordination microenvironment, improving hydrophilicity and strengthening interaction affinity with REEs. Consequently, DGCN-K shows excellent REEs adsorption performance, achieving high adsorption capacity (Nd(III) 146.25 mg/g, Dy(III) 180.82 mg/g, Lu(III) 204.34 mg/g,) within short adsorption equilibrium time (30 min). Furthermore, DGCN-K possesses high REEs selective removal rate in the mixed binary system and actual leaching tailings. This study provides a feasible microenvironment regulation strategy for the construction of 2D defective carbon nitride with oxygen-enriched sites and extended nanoporous for synergistically enabling efficient recovery of REEs.

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扩展纳米孔富氧位点对二维缺陷氮化碳微环境的调控及稀土元素的高效回收
废水中稀土元素的高效回收是环境修复和资源可持续发展的重要手段。然而,在含有低浓度稀土和高浓度竞争金属离子的系统中实现高效和选择性的稀土提取仍然是一个挑战。在这里,我们报道了二维缺陷氮化碳(DGCN-K)的制备,其具有扩展的纳米多孔富氧位点,这是通过使用柔性缩聚-离子-热策略重新排列框架结构单元来实现的。扩展的纳米孔和连续传输的纳米通道在活性位点中心周围建立了专用的结构微环境,促进了离子的有效扩散,增加了活性位点的可达性。同时,丰富的电负性氰基和羟基的加入改变了配位微环境,改善了亲水性,增强了与稀土的相互作用亲和力。DGCN-K表现出优异的稀土吸附性能,在较短的吸附平衡时间(30 min)内达到较高的吸附容量(Nd(III) 146.25 mg/g, Dy(III) 180.82 mg/g, Lu(III) 204.34 mg/g)。DGCN-K在混合二元体系和实际浸出尾矿中均具有较高的稀土选择性去除率。本研究提供了一种可行的微环境调控策略,用于构建富氧位点和扩展纳米孔的二维缺陷氮化碳,以协同有效地回收稀土。
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来源期刊
Journal of Hazardous Materials
Journal of Hazardous Materials 工程技术-工程:环境
CiteScore
25.40
自引率
5.90%
发文量
3059
审稿时长
58 days
期刊介绍: The Journal of Hazardous Materials serves as a global platform for promoting cutting-edge research in the field of Environmental Science and Engineering. Our publication features a wide range of articles, including full-length research papers, review articles, and perspectives, with the aim of enhancing our understanding of the dangers and risks associated with various materials concerning public health and the environment. It is important to note that the term "environmental contaminants" refers specifically to substances that pose hazardous effects through contamination, while excluding those that do not have such impacts on the environment or human health. Moreover, we emphasize the distinction between wastes and hazardous materials in order to provide further clarity on the scope of the journal. We have a keen interest in exploring specific compounds and microbial agents that have adverse effects on the environment.
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