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掺氟 BiVO4 光催化剂:优先切断 C-N 键实现草甘膦的绿色降解。

Fluorine-doped BiVO photocatalyst: Preferential cleavage of C-N bond for green degradation of glyphosate.

机构信息

College of Materials and Chemical Engineering, China Three Gorges University, Yichang 443002, China; Engineering Research Center of Eco-environment in Three Gorges Reservoir Region, Ministry of Education, China Three Gorges University, Yichang 443002, China.

Engineering Research Center of Eco-environment in Three Gorges Reservoir Region, Ministry of Education, China Three Gorges University, Yichang 443002, China; College of Biology & Pharmacy, China Three Gorges University, Yichang 443002, China.

出版信息

J Environ Sci (China). 2023 May;127:60-68. doi: 10.1016/j.jes.2022.04.013. Epub 2022 Apr 18.

DOI:10.1016/j.jes.2022.04.013
PMID:36522089
Abstract

With increasing concerns on the environment and human health, the degradation of glyphosate through the formation of less toxic intermediates is of great importance. Among the developed methods for the degradation of glyphosate, photodegradation is a clean and efficient strategy. In this work, we report a new photocatalyst by doping F ion on BiVO that can efficiently degrade glyphosate and reduce the toxic emissions of aminomethylphosphonic acid (AMPA) through the selective (P)-C-N cleavage in comparison of BiVO catalyst. The results demonstrate that the best suppression of AMPA formation was achieved by the catalyst of 0.3F@BiVO at pH = 9 (AMPA formation below 10%). In situ attenuated total reflectance Fourier transforms infrared (ATR-FTIR) spectroscopy indicates that the adsorption sites of glyphosate on BiVO and 0.3F@BiVO are altered due to the difference in electrostatic interactions. Such an absorption alteration leads to the preferential cleavage of the C-N bond on the N-C-P skeleton, thereby inhibiting the formation of toxic AMPA. These results improve our understanding of the photodegradation process of glyphosate catalyzed by BiVO-based catalysts and pave a safe way for abiotic degradation of glyphosate.

摘要

随着人们对环境和人类健康的关注日益增加,通过形成毒性较小的中间体来降解草甘膦变得尤为重要。在已开发的草甘膦降解方法中,光降解是一种清洁高效的策略。在这项工作中,我们通过在 BiVO 上掺杂 F 离子报告了一种新型光催化剂,该催化剂可以有效地降解草甘膦,并通过选择性(P)-C-N 断裂减少有毒的氨甲基膦酸(AMPA)的排放,与 BiVO 催化剂相比。结果表明,在 pH = 9 时,最佳的 AMPA 形成抑制效果是通过 0.3F@BiVO 催化剂实现的(AMP A 形成低于 10%)。原位衰减全反射傅里叶变换红外(ATR-FTIR)光谱表明,由于静电相互作用的差异,草甘膦在 BiVO 和 0.3F@BiVO 上的吸附位点发生了改变。这种吸收的改变导致 N-C-P 骨架上的 C-N 键优先断裂,从而抑制了有毒 AMPA 的形成。这些结果提高了我们对基于 BiVO 的催化剂催化草甘膦光降解过程的理解,并为草甘膦的非生物降解铺平了安全的道路。

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