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通过前驱体的超分子自模板结构制备的微米级垂直MoS/多孔g-CN压电催化剂:降解与析氢

Micron-Scale Vertical MoS/Porous g-CN Piezocatalyst via a Precursor's Supramolecular Self-Template Architecture: Degradation and Hydrogen Evolution.

作者信息

Wang Yimeng, Ma Hecheng, Liu Jianjun, Yu Yingchun, Zuo Shengli

机构信息

State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China.

出版信息

ACS Appl Mater Interfaces. 2024 Oct 16;16(41):55325-55342. doi: 10.1021/acsami.4c10981. Epub 2024 Oct 7.

DOI:10.1021/acsami.4c10981
PMID:39374064
Abstract

Piezocatalysis can effectively harvest various kinds of mechanical energy with high entropy from the environment and drive some redox reactions without light irradiation, where MoS- and g-CN-based piezocatalysts are recent research hotspots. This study constructs an architecture of ordered melamine hydrochloride-cyanuric acid/MoO supramolecular precursor via self-assembly, serving as a self-template for in situ tight growth of vertically aligned micron-scale MoS on porous foam-like g-CN(CM) under S vapor with a bioinspired rooting and sprouting-like process. Experiments, DFT calculations, and finite element simulations collectively confirm the high piezoresponse of the CM with high exposure of active sites and enhanced mechanical energy collection. The vertical interfaces and built-in electric fields in the composite induce efficient charge carrier separation and transfer. The optimized CM0.77 efficiently degrades various organic dyes and antibiotic under dark ultrasound [rhodamine B (RhB): 0.47 s, methyl orange (MO): 0.05 s, methylene blue (MB): 0.21 s, and tetracycline hydrochloride (TC): 0.03 s] and achieves hydrogen evolution (2431 μmol·g·h). Under simulated water flow (10 L/min), the expanded CM0.77/AlO porous foam ceramic (CM/alumina ceramic) purifier device degrades 95% of 400 mL of RhB within 25 min. The developed ordered vertical MoS/g-CN piezocatalyst demonstrates rapid pollutant degradation and efficient hydrogen evolution under water flow and ultrasound, providing new insights for constructing multidimensional piezoelectric composites for environmental remediation and clean energy production.

摘要

压电催化能够有效地从环境中收集各种具有高熵的机械能,并在无光照的情况下驱动一些氧化还原反应,其中基于MoS和g-CN的压电催化剂是近期的研究热点。本研究通过自组装构建了有序的盐酸三聚氰胺-氰尿酸/MoO超分子前驱体结构,在S蒸汽下,以一种受生物启发的生根发芽状过程,作为在多孔泡沫状g-CN(CM)上原位紧密生长垂直排列的微米级MoS的自模板。实验、密度泛函理论计算和有限元模拟共同证实了CM具有高活性位点暴露和增强机械能收集的高压电响应。复合材料中的垂直界面和内建电场诱导了有效的电荷载流子分离和转移。优化后的CM0.77在黑暗超声条件下能有效降解各种有机染料和抗生素[罗丹明B(RhB):0.47 s,甲基橙(MO):0.05 s,亚甲基蓝(MB):0.21 s,盐酸四环素(TC):0.03 s],并实现析氢(2431 μmol·g·h)。在模拟水流(10 L/min)下,膨胀后的CM0.77/AlO多孔泡沫陶瓷(CM/氧化铝陶瓷)净化装置在25分钟内可降解400 mL RhB中的95%。所开发的有序垂直MoS/g-CN压电催化剂在水流和超声作用下表现出快速的污染物降解和高效的析氢性能,为构建用于环境修复和清洁能源生产的多维压电复合材料提供了新的见解。

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