Department of Chemistry and Green-Nano Materials Research Center, Kyungpook National University, Daegu, 41566, South Korea.
Department of Chemistry and Green-Nano Materials Research Center, Kyungpook National University, Daegu, 41566, South Korea.
Environ Res. 2022 Mar;204(Pt A):111991. doi: 10.1016/j.envres.2021.111991. Epub 2021 Aug 31.
Based on the recent concern on the pollution of water bodies with herbicides, adsorptive removal of typical herbicides with similar chemical structures, e. g. clofibric acid (CLFA), methylchlorophenoxypropionic acid or mecoprop (MCPP) and 2,4-dichlorophenoxyacetic acid (2,4-D) from water was studied using a porous nitrogen-enriched carbon. To prepare the nitrogen-enriched carbon, pyrolysis of a melamine (MLM) incorporated metal-azolate framework-6 (MLM(x)@MAF6; x = 0-50 M % of the ligand 2-ethylimidazole for MAF6), that was prepared for the first time via an in situ method, was carried out. The MLM(x)@MAF6-derived carbons (MDC6M(x)s) were characterized and used in the removal of CLFA, MCPP and 2,4-D from water. We found that the MDC6M(25), obtained from MLM(25)@MAF6 with 25% MLM (as the optimum precursor composition), showed the highest maximum adsorption capacity (Q) of 1031 mg/g for CLFA, compared with any reported adsorbents, so far. The physicochemical properties of CLFA, as well as adsorbents and adsorptions under wide pH conditions, were employed to propose a plausible adsorption mechanism including hydrogen bonding. Remarkably, the porous carbon with enriched nitrogen, derived from MAF6 loaded MLM via in situ method, was very competitive in herbicides adsorption because of the contribution of well-dispersed nitrogen sties on the adsorbent. Finally, MDC6M(25) was suggested as a potential adsorbent for the removal of herbcides, including CLFA, MCPP and 2,4-D, from water, which is highly attractive to mitigate the environmental issue, especially, water pollution by various herbicides.
基于最近对水体中除草剂污染的关注,本研究采用一种多孔富氮碳材料,研究了具有相似化学结构的典型除草剂(如氯苯氧丁酸(CLFA)、甲基氯苯氧丙酸或麦草畏(MCPP)和 2,4-二氯苯氧乙酸(2,4-D))在水中的吸附去除。为了制备富氮碳,首次采用原位法制备了三聚氰胺(MLM)掺入金属-唑啉骨架-6(MLM(x)@MAF6;x = 0-50 mol%配体 2-乙基咪唑的 MAF6),然后对其进行热解。对 MLM(x)@MAF6 衍生的碳(MDC6M(x)s)进行了表征,并将其用于从水中去除 CLFA、MCPP 和 2,4-D。结果表明,由 MLM(25)@MAF6 制得的 MDC6M(25)(最佳前驱体组成中 MLM 的含量为 25%)对 CLFA 的最大吸附容量(Q)最高,为 1031 mg/g,这一值高于迄今为止报道的任何吸附剂。本研究通过研究 CLFA、吸附剂以及宽 pH 条件下的吸附情况,提出了一种可能的吸附机制,其中包括氢键作用。值得注意的是,通过原位法将 MLM 负载到 MAF6 上制得的富氮多孔碳,由于吸附剂上分散良好的氮位的贡献,在除草剂吸附方面具有很强的竞争力。最后,建议将 MDC6M(25)作为一种有潜力的吸附剂,用于从水中去除除草剂,包括 CLFA、MCPP 和 2,4-D,这对于缓解环境问题,特别是各种除草剂造成的水污染问题具有重要意义。