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Bidirectional Progressive Optimization of Carbon and Nitrogen Defects in Solar-Driven Regenerable Adsorbent to Remove UV-Filters from Water
ACS ES&T Engineering Pub Date : 2021-01-15 , DOI: 10.1021/acsestengg.0c00176
Chao Zhu 1 , Yi Shen 1 , Shaobin Wang 2 , Shuang Song 1 , Qile Fang 3 , Da Wang 1 , Haomiao Xu 4 , Renlan Liu 5 , Zhiqiao He 1
Affiliation  

Defect engineering of nanomaterials has emerged as a promising approach to improve their performance for pollutant removal. However, various nanomaterial defects play variant roles in environmental applications. It is still a challenge to construct multiple defects of composite materials into advantageous aggregates to deal with complicated matrix pollution. In this work, we investigated a series of three-dimensional defect-optimized aerogels (3D DOAs) of graphene oxide (GO) with a covalent triazine framework (CTF) for improved adsorption and photoregeneration performance via tailoring duet carbon and nitrogen defects. Using chemical reduction, carbon defects in GO were gradually repaired and nitrogen defects in CTF were created simultaneously. The carbon defect engineering generated additional nonpolarized electron-depleted sites in GO of 3D DOA for increased adsorption capacities (2417 μmol/g for benzophenone, 2209 μmol/g for 4-hydroxybenzophenone, 1957 μmol/g for 2,2′,4,4′-tetrahydroxybenzophenone). Meanwhile, increasing nitrogen defects of the CTF in 3D DOA would produce midgap states for an extended absorption range of visible light and increased photocatalytic activity to remove adsorbed pollutants. The enhanced adsorption and the superior photocatalytic regeneration soundly corroborated that the performance of 3D DOA was improved effectively by the defect optimization strategy. Moreover, the high stability of 3D DOA and its practical usage were verified in a real water matrix with a 7-day cycle test. The present work highlights an approach of defect optimization for development of a solar-driven, self-regenerative adsorbent for water purification with high efficiency.

中文翻译:

太阳能驱动可再生吸附剂中碳和氮缺陷的双向渐进优化,以去除水中的紫外线滤光片

纳米材料的缺陷工程已经成为提高其去除污染物性能的一种有前途的方法。但是,各种纳米材料缺陷在环境应用中起着不同的作用。将复合材料的多个缺陷构造成有利的聚集体以应对复杂的基质污染仍然是一个挑战。在这项工作中,我们研究了一系列具有共价三嗪骨架(CTF)的氧化石墨烯(GO)的三维缺陷优化气凝胶(3D DOA),以通过调整二重碳和氮缺陷来改善吸附和光再生性能。通过化学还原,逐渐修复了GO中的碳缺陷,同时创建了CTF中的氮缺陷。碳缺陷工程在3D DOA的GO中生成了额外的非极化电子耗尽位点,以提高吸附能力(二苯甲酮为2417μmol/ g,4-羟基二苯甲酮为2209μmol/ g,2,2',4,4为1957μmol/ g '-四羟基二苯甲酮)。同时,在3D DOA中增加CTF的氮缺陷会产生中间能隙状态,从而扩大了可见光的吸收范围,并提高了光催化活性以去除吸附的污染物。增强的吸附能力和出色的光催化再生性能得到了有力的佐证,该缺陷优化策略有效地提高了3D DOA的性能。此外,在7天的循环测试中,在真实的水基质中验证了3D DOA的高稳定性及其实际使用。
更新日期:2021-03-12
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