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Ultrafine copper nanoclusters and single sites for Fenton-like reactions with high atom utilities
Environmental Science: Nano ( IF 7.3 ) Pub Date : 2020-07-22 , DOI: 10.1039/d0en00505c
Yu Yin 1, 2, 3, 4, 5 , Wenlang Li 6, 7, 8, 9, 10 , Chunli Xu 1, 2, 3, 4 , Lei Shi 5, 11, 12, 13 , Lai-Chang Zhang 5, 11, 12, 13 , Zhimin Ao 6, 7, 8, 9, 10 , Mengxuan Liu 1, 2, 3, 4 , Min Lu 1, 2, 3, 4 , Xiaoguang Duan 13, 14, 15, 16 , Shaobin Wang 13, 14, 15, 16 , Shaomin Liu 4, 17, 18, 19 , Hongqi Sun 5, 11, 12, 13
Affiliation  

Catalysts containing both nanoclusters and single atom metal sites have received increasing attention because of their superior catalytic activities to their aggregated counterparts. Herein, ultrafine CuO nanoclusters along with Cu single atoms were anchored onto typical mesoporous silica SBA-15 for Fenton-like reactions, and the obtained catalysts were named UNCu-SBA. Both advanced characterization and computational studies offered convincing evidence for the unique structural feature. XPS and XANES identified the valence state of Cu(II) on UNCu-SBA. Fenton-like reactions further demonstrated that UNCu-SBA manifested higher activities in comparison with APCu-SBA, which contained aggregated CuO particles. Moreover, the Cu mass normalized rate constant of UNCu-SBA was 18 times larger than that of APCu-SBA, suggesting an exceptional Cu atom utility in UNCu-SBA. The UNCu-SBA catalyst was able to activate H2O2 to generate ˙OH in a wider pH range of 4–7 than in typical Fenton reactions (2–4). This may direct future advances toward AOP nanocatalysis.

中文翻译:

超细铜纳米簇和单个位点,可实现高原子效用的芬顿样反应

包含纳米团簇和单原子金属位点的催化剂因其比聚集的同类物优越的催化活性而受到越来越多的关注。在此,将超细的CuO纳米团簇与Cu单原子一起固定在典型的介孔二氧化硅SBA-15上进行Fenton样反应,并将得到的催化剂命名为UNCu-SBA。先进的表征和计算研究都为独特的结构特征提供了令人信服的证据。XPS和XANES鉴定了Cu(II)在UNCu-SBA上。类似于Fenton的反应进一步表明,与包含聚集的CuO颗粒的APCu-SBA相比,UNCu-SBA表现出更高的活性。此外,UNCu-SBA的铜质量归一化速率常数是APCu-SBA的18倍,这表明UNCu-SBA中具有优异的Cu原子效用。与典型的Fenton反应(2-4)相比,UNCu-SBA催化剂能够活化H 2 O 2以在4-7的较宽pH范围内生成˙OH。这可能会指导AOP纳米催化的未来发展。
更新日期:2020-09-18
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