Nitrite-driven hydrochemical regulation for enhanced ruthenium separation in a pyridine-based sorbent framework

IF 9.8 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Science China Chemistry Pub Date : 2026-09-01 DOI:10.1007/s11426-026-3427-x

Yan Wu, Zhennan Wu, Tianming Qi, Hongji Sang, Luyu Zhang, Hao Wu, Weiqun Shi

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引用次数: 0

Abstract

This study introduces a nitrite-driven hydrochemical regulation strategy to reconfigure the ligand environment of ruthenium (Ru), transforming it from heterogeneous species into a uniform and stable anionic complex, [Ru(NO)(NO₂)_x(OH)_5−x]²⁻. This transformation significantly enhances the homogeneity and reactivity of Ru, enabling highly efficient separation from high-level liquid waste (HLLW) using a pyridine-based resin. Combined density functional theory (DFT) and X-ray absorption fine structure (XAFS) analyses identified the dominant complex as [Ru(NO)(NO₂)_2.2(ONO)_1.8(OH)]²⁻. To counteract the inherent instability of the nitrite-nitric acid system, a silicon-based composite adsorbent (N3/SiO₂) was developed, providing protective barriers against deterioration. Under optimized conditions, the adsorbent achieved a maximum capacity of 69.20 mg/g at 298 K—a 65% improvement over conventional systems. Adsorption and desorption mechanisms were elucidated, and a reusable ion-exchange-complexation cycle was proposed. This work offers an innovative strategy for Ru separation in HLLW, with strong potential for industrial scale-up applications.

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亚硝酸盐驱动的水化学调节在吡啶基吸附剂框架中增强钌分离

本研究介绍了一种亚硝酸盐驱动的水化学调节策略，以重新配置钌（Ru）的配体环境，将其从异相物质转化为均匀稳定的阴离子配合物[Ru(NO)(NO2)x(OH)5−x]2−。这一转变显著提高了Ru的均匀性和反应性，使使用吡啶基树脂从高放射性废液（HLLW）中高效分离成为可能。结合密度泛函理论（DFT）和x射线吸收精细结构（XAFS）分析，确定了优势配合物为[Ru(NO)(NO2)2.2(ONO)1.8(OH)]2−。为了抵消亚硝酸盐-硝酸体系固有的不稳定性，开发了一种硅基复合吸附剂（N3/SiO2），提供了防止变质的保护屏障。在优化条件下，吸附剂在298 k下的最大吸附容量为69.20 mg/g，比常规体系提高了65%。阐明了吸附和解吸机理，并提出了一个可重复使用的离子交换络合循环。这项工作提供了一种创新的策略，在高废液中分离钌，具有强大的工业规模应用潜力。

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来源期刊

Science China Chemistry CHEMISTRY, MULTIDISCIPLINARY-

CiteScore

14.40

自引率

7.30%

发文量

3787

审稿时长

2.2 months

期刊介绍： Science China Chemistry, co-sponsored by the Chinese Academy of Sciences and the National Natural Science Foundation of China and published by Science China Press, publishes high-quality original research in both basic and applied chemistry. Indexed by Science Citation Index, it is a premier academic journal in the field. Categories of articles include: Highlights. Brief summaries and scholarly comments on recent research achievements in any field of chemistry. Perspectives. Concise reports on thelatest chemistry trends of interest to scientists worldwide, including discussions of research breakthroughs and interpretations of important science and funding policies. Reviews. In-depth summaries of representative results and achievements of the past 5–10 years in selected topics based on or closely related to the research expertise of the authors, providing a thorough assessment of the significance, current status, and future research directions of the field.