Origin of the Excellent Activity and Selectivity of a Single-Atom Copper Catalyst with Unsaturated Cu-N2 Sites via Peroxydisulfate Activation: Cu(III) as a Dominant Oxidizing Species,Environmental Science & Technology

当前位置： X-MOL 学术 › Environ. Sci. Technol. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Origin of the Excellent Activity and Selectivity of a Single-Atom Copper Catalyst with Unsaturated Cu-N2 Sites via Peroxydisulfate Activation: Cu(III) as a Dominant Oxidizing Species
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2022-05-12 , DOI: 10.1021/acs.est.2c00369
Fan Li ₁ , Zhicong Lu ₁ , Tong Li ₁ , Peng Zhang ₁ , Chun Hu ₁

Affiliation

As an efficient active oxidant for the selective degradation of pollutants in wastewater, the high-valent copper species Cu(III) with persulfate activation has attracted substantial attention in some Cu-based catalysts. However, the systematic study of a catalyst structure and mechanism about Cu(III) with peroxydisulfate (PDS) activation is challenging owing to the coexistence of multiple Cu species and the structural symmetry of PDS. Herein, we anchored a Cu atom with two pyridinic N atoms to synthesize a single-atom Cu catalyst (Cu_SA-NC). Experimental characterizations and theoretical calculations complemented each other well because of the uniform atomic active sites. The single-atom Cu was identified as the active site, and the unsaturated Cu-N₂ configuration was more conductive to PDS activation than the saturated Cu-N₄ configuration. Benefiting from the generation of Cu(III), Cu_SA-NC exhibited an obvious selective and anti-interference performance for pollutant degradation in a complex matrix. The superior catalytic activity of Cu_SA-NC compared with that of other reported Cu-based catalysts and good durability in a continuous-flow experiment further revealed the potential of Cu_SA-NC for practical applications. This work strongly deepens the understanding of the generation of Cu(III) in a single-atom Cu catalyst with unsaturated Cu-N₂ sites under PDS activation and develops an efficient approach for actual water purification.

中文翻译：

通过过二硫酸盐活化具有不饱和 Cu-N2 位点的单原子铜催化剂具有优异活性和选择性的原因：Cu(III) 作为主要的氧化物质

作为选择性降解废水中污染物的有效活性氧化剂，具有过硫酸盐活化的高价铜物种Cu(III)在一些Cu基催化剂中引起了广泛关注。然而，由于多种Cu物种的共存和PDS的结构对称性，对Cu(III)与过二硫酸盐(PDS)活化的催化剂结构和机理的系统研究具有挑战性。在此，我们用两个吡啶N原子锚定了一个Cu原子，合成了一种单原子Cu催化剂（Cu _SA -NC）。由于均匀的原子活性位点，实验表征和理论计算相得益彰。单原子Cu被确定为活性位点，不饱和Cu-N ₂构型比饱和Cu-N ₄构型更能促进PDS活化。受益于 Cu(III) 的生成，Cu _SA -NC 在复杂基质中对污染物降解表现出明显的选择性和抗干扰性能。与其他报道的铜基催化剂相比， Cu _SA -NC的优异催化活性和连续流动实验中良好的耐久性进一步揭示了 Cu _SA -NC 在实际应用中的潜力。_{这项工作极大地加深了对在 PDS 活化下具有不饱和 Cu-N 2}位点的单原子 Cu 催化剂中 Cu(III) 生成的理解，并开发了一种有效的实际水净化方法。

更新日期：2022-05-12

点击分享查看原文

点击收藏

阅读更多本刊新发论文本刊介绍/投稿指南