Construction of photothermal hybrid with surface-polarized carbon nanotube twined oxygen-vacancy engineered cuprous oxide for improved PMS activation and water purification

IF 4.9 2区 化学 Q2 CHEMISTRY, PHYSICAL Molecular Catalysis Pub Date : 2025-03-06 DOI:10.1016/j.mcat.2025.114994
Yarao Gao , Hongyao Zhao , Mengting Liu , Yanyun Wang , Yangping Zhang , Linzhi Zhai , Xiang Liu , Feng Zeng , Jianming Pan , Danhong Shang , Fu Yang
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Abstract

Photothermal hybrids composed of nanocarbon and metal species are promising in solar-driven photothermal conversion and later application of water purification. Herein, the photothermal hybrid with surface-polarized carbon nanotube (CNT) twined oxygen vacancy-engineered cuprous oxides was constructed. The surface polar oxygen and nitrogen moieties were introduced onto the CNT, enriching the surface polarity of the nanocarbon, which further twined the in-situ generated oxygen vacancy-engineered cuprous oxides. The constructed catalyst was endowed with abundant Cu(I) reactive sites and oxygen vacancy, providing the efficient trapping effect and enough exposed active sites to trigger improved peroxymonosulfate (PMS) activation. In addition, the obtained catalyst affords superior photothermal conversion efficiency, thereby showcasing the great potential in solar-driven water purification. Therefore, the catalyst shows excellent bisphenol A (BPA) degradation performance with a reaction rate constant of 0.47 min-1, and activation energy (Ea=9.38 kJ·mol-1).. The reaction mechanism study indicates the main contribution of singlet oxygen and superoxide radicals in the BPA degradation. More importantly, the obtained catalyst affords the excellent total organic carbon (TOC) removal ability for mixed contaminants, higher than that of single contaminant removal, which shows great potential for practical complicated wastewater purification. Finally, the obtained photothermal hybrids were anchored onto the tailored sponge through a hydrogel tethering strategy, which acts as a monolith evaporator to enable cleanwater regeneration and contaminant degradation.

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表面极化碳纳米管缠绕氧空位工程氧化亚铜光热杂化物的构建及其对PMS活化和水净化的改善
由纳米碳和金属组成的光热杂化材料在太阳能光热转换和水净化方面具有广阔的应用前景。本文构建了表面极化碳纳米管(CNT)缠绕氧空位工程氧化亚铜的光热杂化材料。将表面极性氧和氮基团引入碳纳米管中,使纳米碳的表面极性丰富,从而进一步缠绕原位生成的氧空位工程亚铜氧化物。所构建的催化剂具有丰富的Cu(I)活性位点和氧空位,提供了高效的捕获效果和足够的暴露活性位点,以触发改进的过氧单硫酸盐(PMS)活化。此外,所获得的催化剂具有优异的光热转换效率,因此在太阳能驱动的水净化中显示出巨大的潜力。因此,该催化剂具有良好的双酚A (BPA)降解性能,反应速率常数为0.47 min-1,活化能Ea=9.38 kJ·mol-1。反应机理研究表明,单线态氧和超氧自由基在双酚a降解过程中起主要作用。更重要的是,所制备的催化剂对混合污染物具有优异的总有机碳(TOC)去除能力,高于对单一污染物的去除能力,在实际复杂废水净化中具有很大的潜力。最后,通过水凝胶系结策略将获得的光热杂交体固定在定制的海绵上,作为一个整体蒸发器,实现清洁水再生和污染物降解。
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来源期刊
Molecular Catalysis
Molecular Catalysis Chemical Engineering-Process Chemistry and Technology
CiteScore
6.90
自引率
10.90%
发文量
700
审稿时长
40 days
期刊介绍: Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are: Heterogeneous catalysis including immobilized molecular catalysts Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis Photo- and electrochemistry Theoretical aspects of catalysis analyzed by computational methods
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