Biomimetic Photodegradation of Glyphosate in Carborane-Functionalized Nanoconfined Spaces,Journal of the American Chemical Society

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Biomimetic Photodegradation of Glyphosate in Carborane-Functionalized Nanoconfined Spaces
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-06-20 , DOI: 10.1021/jacs.3c02019
Lei Gan _{1,

2} , Makenzie T Nord ₃ , Jacob M Lessard ₃ , Noah Q Tufts ₃ , Arunraj Chidambaram _{4,

5} , Mark E Light ₆ , Hongliang Huang ₇ , Eduardo Solano ₈ , Julio Fraile ₁ , Fabián Suárez-García ₉ , Clara Viñas ₁ , Francesc Teixidor ₁ , Kyriakos C Stylianou ₃ , José G Planas ₁

Affiliation

Institut de Ciència de Materials de Barcelona (ICMAB-CSIC), Bellaterra 08193, Spain.
Institute of Physical and Theoretical Chemistry, Graz University of Technology, Graz 8010, Austria.
Materials Discovery Laboratory (MaD Lab), Department of Chemistry, Oregon State University, 153 Gilbert Hall, Corvallis, Oregon OR 97331, United States.
Institute of Chemical Sciences and Engineering, École Polytechnique Fedérale de Lausanne (EPFL Valais), Rue de l'Industrie 17, Sion 1951, Switzerland.
Chemspeed Technologies AG, Wölferstrasse 8, Füllinsdorf 4414, Switzerland.
Department of Chemistry, University of Southampton, Highfield, Southampton SO17 1BJ, U.K.
State Key Laboratory of Separation Membranes and Membrane Processes, School of Chemistry and Chemical Engineering, Tiangong University, Tianjin 300387, China.
NCD-SWEET Beamline, ALBA Synchrotron Light Source, Cerdanyola del Vallès 08290, Spain.
Departament of Material Chemistry, Instituto de Ciencia y Tecnología del Carbono, INCAR-CSIC, Oviedo 33011, Spain.

The removal of organophosphorus (OP) herbicides from water has been studied using adsorptive removal, chemical oxidation, electrooxidation, enzymatic degradation, and photodegradation. The OP herbicide glyphosate (GP) is one of the most used herbicides worldwide, leading to excess GP in wastewater and soil. GP is commonly broken down in environmental conditions to compounds such as aminomethylphosphonic acid (AMPA) or sarcosine, with AMPA having a longer half-life and similar toxicity to GP. Metal–organic frameworks (MOFs) are excellent materials for purifying OP herbicides from water due to their ability to combine adsorption and photoactivity within one material. Herein, we report the use of a robust Zr-based MOF with a meta-carborane carboxylate ligand (mCB-MOF-2) to examine the adsorption and photodegradation of GP. The maximum adsorption capacity of mCB-MOF-2 for GP was determined to be 11.4 mmol/g. Non-covalent intermolecular forces between the carborane-based ligand and GP within the micropores of mCB-MOF-2 are thought to be responsible for strong binding affinity and capture of GP. After 24 h of irradiation with ultraviolet–visible (UV–vis) light, mCB-MOF-2 selectively converts 69% of GP to sarcosine and orthophosphate, following the C–P lyase enzymatic pathway and biomimetically photodegrading GP. Circumventing the production of AMPA is desirable, as it has a longer half-life and similar toxicity to GP. The exceptional adsorption capacity of GP by mCB-MOF-2 and its biomimetic photodegradation to non-toxic sarcosine make it a promising material for removing OP herbicides from water.

中文翻译：

碳硼烷功能化纳米受限空间中草甘膦的仿生光降解

人们利用吸附去除、化学氧化、电氧化、酶降解和光降解等方法研究了去除水中有机磷 (OP) 除草剂的方法。OP 除草剂草甘膦 (GP) 是全球最常用的除草剂之一，导致废水和土壤中 GP 过量。GP 通常在环境条件下分解为氨甲基膦酸 (AMPA) 或肌氨酸等化合物，其中 AMPA 的半衰期较长，且毒性与 GP 相似。金属有机框架 (MOF) 是从水中纯化 OP 除草剂的优异材料，因为它们能够在一种材料中结合吸附和光活性。在此，我们报告了使用具有间碳硼烷羧酸盐配体的稳健的 Zr 基 MOF（m CB-MOF-2）来检查GP的吸附和光降解。m CB-MOF-2对 GP的最大吸附容量测定为 11.4 mmol/g。m CB-MOF-2微孔内基于碳硼烷的配体和 GP 之间的非共价分子间力被认为是造成 GP 强结合亲和力和捕获的原因。在紫外可见 (UV-vis) 光照射 24 小时后，m CB-MOF-2遵循 C-P 裂合酶途径和仿生光降解 GP，选择性地将 69% 的 GP 转化为肌氨酸和正磷酸盐。避免 AMPA 的产生是可取的，因为它具有更长的半衰期和与 GP 相似的毒性。GP 的卓越吸附能力CB-MOF-2及其仿生光降解作用使其成为无毒肌氨酸，使其成为去除水中 OP 除草剂的有前途的材料。

更新日期：2023-06-20

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