增加 P 掺杂 FeCo2O4-x 纳米片上的还原性 Fe(II)/Co(II) 位点以加速 As(III) 电分析的价态循环,Environmental Science: Nano

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增加 P 掺杂 FeCo2O4-x 纳米片上的还原性 Fe(II)/Co(II) 位点以加速 As(III) 电分析的价态循环
Environmental Science: Nano ( IF 5.8 ) Pub Date : 2023-02-01 , DOI: 10.1039/d2en01104b
Yuan-Fan Yang _{1,

2,

3} , Hong-Qi Huang ₁ , Zong-Yin Song _{1,

2} , Hui-Quan Li ₄ , Xin-Yu Yu ₅ , Yu-Min Cui ₄ , Meng Yang ₁ , Shi-Hua Chen _{1,

3} , Xing-Jiu Huang _{1,

2,

3}

Affiliation

通过掺杂杂原子调节活性位点以提高纳米材料的催化能力受到了各个领域的关注。然而，优异的催化性能与掺杂引起的材料结构变化之间的关系却被忽略了。在此，我们设计了一种有效的策略来促进FeCo ₂ O ₄₋_x与 P 掺杂 (P-FeCo ₂ O ₄₋_x ) 对 As( III )的电化学分析。P-FeCo ₂ O ₄₋_x改性玻碳电极 (P-FeCo ₂ O ₄₋_x/GCE) 对 As( III ) 表现出 1.240 μA ppb ^-1的优异灵敏度，这几乎比 FeCo ₂ O _{4- x} /GCE 高一个数量级。此外，与其他典型重金属离子（HMIs）相比，P-FeCo ₂ O _{4− x}对As（ III ）表现出优异的选择性，具有优异的稳定性、可重复性、实用性和抗干扰能力。X射线光电子能谱表明，P掺杂使更多的电子通过Fe-P和Co-P键从P转移到相邻的Fe( III )和Co( III ) ，从而获得更多的高活性离子Fe( II )) 和P–FeCo ₂ O ₄₋_x中的Co( II ) ，以及丰富的氧空位 (Ov) 的形成。吸附在Ov上的As( III )在检测过程中与P位相互作用形成Fe-P-As和Co-P-As键。随后，由增加的还原离子引起的 Fe( II )/Fe( III ) 和 Co( II )/Co( III ) 的增强价态循环进一步改善了表面氧化还原，以高效电催化 As( III )), 从而获得令人满意的电化学性能。该工作有助于理解杂原子掺杂引起的敏感界面内部变化与优异催化性能之间的关系，为设计用于超灵敏环境HMIs分析的高活性电催化界面提供指导。

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Increasing reductive Fe(II)/Co(II) sites on P-doped FeCo2O4−x nanosheets to accelerate the valence cycle for the electroanalysis of As(III)

Modulating active sites via doping heteroatoms to improve the catalytic capabilities of nanomaterials has attracted attention from various fields. However, the relationship between the excellent catalytic performance and the changes in the structures of materials caused by doping was ignored. Herein, we designed a competent strategy for promoting the electrochemical analysis of As(III) by FeCo₂O_4−x with P-doping (P-FeCo₂O_4−x). P-FeCo₂O_4−x modified glassy carbon electrodes (P-FeCo₂O_4−x/GCE) exhibited an excellent sensitivity for As(III) of 1.240 μA ppb⁻¹, which was almost one order of magnitude higher than that of FeCo₂O_4−x/GCE. Besides, P-FeCo₂O_4−x displayed excellent selectivity toward As(III) compared to other typical heavy metal ions (HMIs), with excellent stability, repeatability, practicality, and anti-interference ability. X-ray photoelectron spectroscopy revealed that P-doping made more electrons transfer from P to adjacent Fe(III) and Co(III) via Fe–P and Co–P bonds, thus obtaining more high-activity ions of Fe(II) and Co(II) in P–FeCo₂O_4−x, along with the formation of abundant oxygen vacancies (Ov). As(III) adsorbed on Ov interacted with P sites to form Fe–P–As and Co–P–As bonds, during the process of detection. Subsequently, the enhanced valance cycle of Fe(II)/Fe(III) and Co(II)/Co(III) caused by increasing reduction ions further improved the surficial redox for highly-efficient electrocatalysis of As(III), thereby acquiring a satisfactory electrochemical performance. This work helps to understand the relationship between the internal change of sensitive interfaces caused by heteroatomic doping and excellent catalytic performance, which provides guidance for designing high-activity electrocatalytic interfaces for ultrasensitive environmental HMIs analysis.

更新日期：2023-02-01

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