Catalysis Science & Technology
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2020
·Vol. 11
·期 5
·1899-1913
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IF 5.721
Xiaojuan Bai,Cong Wang,Xuyu Wang,Tianqi Jia,Boxuan Sun,Shengqi Yang,Di Li,Junqi Li,Haiyan Li
Pharmaceutical and personal care products (PPCPs) are the most common hazardous environmental pollutants. Accordingly, PDI anion radicals are promising photocatalysts to transform PPCPs into non-toxic CO2 and H2O for their clean and efficient production. In the present work, we successfully synthesized an electrophilic PDI supramolecular (sEACA-PDI) compound with high electron affinity through a simple gelation process. Its electron affinity is contributed by its side chain, which enhances the electrophilicity of its perylene core edge. Consequently, sEACA-PDI tends to form anion radicals to provide a SOMO orbital, which allows sEACA-PDI to obtain electrons successively from organic pollutants. Its side chain also generates a polarized surface electric field, building an efficient pathway for electron transfer. The high flexibility and freedom of the sEACA-PDI side chain is beneficial to form a cluster structure. Numerous strongly electrophilic groups are exposed on the surface of sEACA-PDI, which further enhance its electron affinity. sEACA-PDI exhibited high photocatalytic degradation efficiency for classical organic pollutants via successive electrophilic attack, i.e. the k for DCF was 0.923 h−1. Also, sEACA-PDI achieved a k value of 0.351 h−1 for the degradation of MB. This work proposes a promising strategy for developing PDI anion radicals with high electron affinity, and also provides new insights for the treatment of environmental pollutants.
研究领域:
环境科学
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材料科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Yuhang Ren,Yu Tian,Yating Lu,Dongyu Nie,Huayi Zhu,Xia Yang
Malathion (MA) is a widely used organophosphorus pesticide globally. Developing efficient photocatalysts is crucial for eliminating MA pollution in water by photocatalytic technology. This study focuses on preparing a series of H-PDI supermolecule/NH 2 -MIL-101(Fe) (PM) materials by amidating NH 2 -MIL-101(Fe) with the more stable H-PDI supermolecule, forming a covalent O C–NH bond. Among these materials, 40 %PM (indicating a mass percentage content of 40 % H-PDI supermolecule in PM) exhibited the best performance for degradation of MA. Under simulated sunlight irradiation of a 10 mg·L 1 MA solution for 180 min, the reaction rate constants of 40 %PM were 5.95 times and 3.13 times higher than those of NH 2 -MIL-101(Fe) and H-PDI supermolecule, respectively. The enhanced performance is attributed to the formation of Z-scheme heterojunctions in the 40 %PM composite lead to fast separation of photogenerated e − and h + . Combining the results of HPLC-MS with Fukui Function, the HOMO, LUMO, and pathway of degradation of MA attracted by 1 O 2 , •OH, and h + were speculated. The pathway involves oxidation, demethylation, P-S bond breakage, decarboxylation, and final conversion to some inorganic molecules. The toxicity of the degradation byproducts were lower than that of MA estimated by Toxicity Estimation Software Tool.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Tao Cai,Wengao Zeng,Yutang Liu,Longlu Wang,Wanyue Dong,Hui Chen,Xinnian Xia
Silver orthophosphate (Ag 3 PO 4 ) based semiconductor photocatalysis have been widely investigated for environmental purification due to its strong oxidation ability. Yet, its poor photostability and low photoactivity hamper its extensive applications. Here, an inorganic-organic Z-scheme photocatalytic system for antibiotic degradation demonstrated high photoactivity and stability through the use of Ag 3 PO 4 /Perylene diimide organic supermolecule (PDIsm). The apparent rate constant of tetracycline hydrochloride (TC-H) degradation with Ag 3 PO 4 /PDIsm was 1.5 times that of Ag 3 PO 4 and 8 times that of PDIsm. The photocatalytic activity of Ag 3 PO 4 /PDIsm toward TC-H still kept 65 % after four reuses, while pure Ag 3 PO 4 only kept 22 %. We revealed that this high photoactivity and photostability arisen from the efficient carriers separation and the formation of direct Z-scheme junction. Importantly, this Z-scheme electron transfer pathway was confirmed by thorough experimental study and density functional theory (DFT) calculation. This work demonstrated the significant potential of Ag 3 PO 4 -based inorganic-organic Z-scheme photocatalyst in environmental remediation.
研究领域:
环境科学
·
材料科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Wenwu Zhou,Bing Yang,Guo Liu,Chenmin Xu,Qiuyi Ji,Weiming Xiang,Dunyu Sun,Qiang Zhong,Huan He,Liu Yazi,Zhe Xu,Chengdu Qi,Shiyin Li,Shaogui Yang
Employing perylene diimide supermolecule (PDI) as metal-free cocatalyst, a novel PDI/g-C 3 N 4 /Bi 2 WO 6 (PCB) photocatalyst was constructed for the effective degradation of antibiotics. Both the photocatalytic activity and photostability of g-C 3 N 4 /Bi 2 WO 6 (gCB) were further improved after loading PDI. Under simulated sunlight illumination, the apparent rate constant of tetracycline (TC) degradation by PCB reached 2.6 times that of gCB. The photocatalytic activity of PCB still kept over 80% after 4 cycle experiments, while gCB only remained around 21%. The superior activity of PCB was ascribed to the synergism between the extended visible light absorption range through the participation of PDI cocatalyst and facilitated gCB-to-PDI photoelectron transfer. TC would finally be transformed into non-toxic ring opening products and mineralized. This work demonstrated that PDI was an excellent metal-free cocatalyst and exhibited great potential to boost the activity of photocatalysts.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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