4.7 Article

Construction of a novel metal-organic framework adenine-UiO-66 piezocatalyst for efficient diclofenac removal

期刊

出版社

ELSEVIER
DOI: 10.1016/j.seppur.2022.120743

关键词

Piezoelectric; Metal-organic frame; Adenine-UiO-66; Stirring; Diclofenac

资金

  1. Changzhou University, Advanced Catalysis and Green Manufacturing Collaborative Innovation Center, National-local Joint Engineering Research Center of Biomass Refining and High-quality Utilization and Industry Supporting Project of Changzhou of Jiangsu Prov [CE20195022]
  2. National key research and development program of Zhejiang Province [2019C01083]
  3. Scientific Research Foundation of Jiangsu Provincial Education Department [21KJB430035]

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Piezoelectric materials, such as UiO-66, have shown promising potential in catalyzing the sustained removal of pollutants. In this study, the introduction of the polar molecule adenine in the synthesis process of UiO-66 led to enhanced piezoelectric properties and structure asymmetry. The optimized catalyst, AD U, exhibited improved piezoelectric potential and charge separation efficiency compared to UiO-66. Additionally, AD U demonstrated enhanced piezoelectric degradation efficiency for diclofenac sodium (DCF) compared to pure UiO-66, and the major role of h+ in destroying DCF molecules was confirmed through experiments. Three possible degradation pathways for DCF were proposed using DFT and LC-MS. This work provides a new pathway to enhance the piezoelectric properties of MOFs and expands their applications in the field of piezocatalysis.
Piezoelectric materials, which could collect and convert mechanical energy into electrical energy, have recently emerged as promising catalysts for pollutants removal sustainably. Unfortunately, it remains a challenge to enhance the intrinsic piezoelectric property of piezoelectric materials. Herein, for the first time, the polar molecule adenine was introduced as a linking agent in the synthesis process of Zr-based UiO-66 (denoted as AD U) to enhance the structure asymmetry and piezoelectric properties of UiO-66. The piezoresponse force microscopy (PFM) and ferroelectric hysteresis loop demonstrated that AD-U catalyst exhibited significantly enhanced piezoelectric potential than UiO-66. Furthermore, a series of electrochemical characterization evidenced that AD U displayed higher charge separation efficiency than UiO-66. As expect, the optimized AD-U shown promoted diclofenac sodium (DCF) piezoelectric degradation efficiency by harvesting stirring energy compared with pure UiO-66. The electron paramagnetic resonance (EPR) spectra and trapping agent experiments convinced that h+ play the major role for destroying the DCF molecules. Moreover, three possible degradation pathways of DCF were put forward by DFT and liquid chromatography mass system (LC-MS). Our work offers a new pathway to enhance piezoelectric property of MOFs and extend the application of MOFs in the field of piezocatalysis.

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