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Coordination engineering strategy of iron single-atom catalysts boosts anti-Cu(II) interference detection of As(III) with a high sensitivity
Journal of Hazardous Materials ( IF 12.2 ) Pub Date : 2022-10-04 , DOI: 10.1016/j.jhazmat.2022.130122
Pei-Hua Li 1 , Zong-Yin Song 2 , Xiang-Yu Xiao 2 , Bo Liang 2 , Meng Yang 1 , Shi-Hua Chen 1 , Wen-Qing Liu 3 , Xing-Jiu Huang 2
Affiliation  

Mutual interference issues between heavy metal ions tremendously affect the detection reliability and accuracy in water quality analysis, especially the serious interference of Cu(II) on the detection of As(III) is greatly hard to overcome, which needs to be solved urgently. Herein, iron single-atom catalysts with different coordination structures of FeN2C2 and FeN3P are constructed to selectively catalyze the detection of As(III) in the coexistence of Cu(II). FeN3P achieves a high sensitivity of 3.90 µA ppb-1 toward As(III) in NH4Cl/NH3·H2O electrolyte (pH 8.0), completely avoiding Cu(II)-interference. Moreover, the turnover frequency (TOF) of FeN3P is an order of magnitude higher than that of FeN2C2. X-ray absorption fine structure (XAFS) spectroscopy and density functional theory (DFT) calculations demonstrate that an As-O bond of H3AsO3 is broken by the strong affinities between both P and O atoms and Fe and As atoms, and H3AsO3 are preferentially reduced by FeN3P during adsorptive process. Meanwhile, the low reaction energy barrier of the rate-determined step for As(III) reduction over FeN3P also accelerates the deposition of As(III) and enhances its response signals. The free-Cu(II) are difficult to adsorb on FeN3P and do not compete with As(III) for Fe active sites, which contributes to the excellent anti-Cu(II) interference capability.



中文翻译:

铁单原子催化剂的配位工程策略促进了高灵敏度As(III)的抗Cu(II)干扰检测

重金属离子之间的相互干扰问题极大地影响了水质分析中检测的可靠性和准确性,尤其是Cu(II)对As(III)检测的严重干扰难以克服,亟待解决。在此,本文构建了具有不同配位结构的FeN 2 C 2和FeN 3 P 的铁单原子催化剂,以选择性催化Cu(II)共存中As(III)的检测。FeN 3 P 对 NH 4 Cl/NH 3 ·H 2中的 As(III)具有 3.90  µA ppb -1的高灵敏度O 电解质(pH 8.0),完全避免 Cu(II) 干扰。此外,FeN 3 P 的转换频率(TOF) 比FeN 2 C 2高一个数量级。X 射线吸收精细结构 (XAFS) 光谱和密度泛函理论 (DFT) 计算表明,H 3 AsO 3的 As-O 键因P 和 O 原子与 Fe 和 As 原子之间的强亲和力而断裂,而 H 3 AsO 3在吸附过程中优先被FeN 3 P还原。同时,FeN 3上 As(III) 还原的速率决定步骤的低反应能垒P 还加速 As(III) 的沉积并增强其响应信号。游离Cu(II)难以吸附在FeN 3 P上,不与As(III)竞争Fe活性位点,具有优异的抗Cu(II)干扰能力。

更新日期:2022-10-05
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