Details

Autor(en) / Beteiligte

• Xu, Junjie
• Yao, Yanchi
• Zhu, Chao
• Lu, Lun
• Fang, Qile
• He, Zhiqiao
• Song, Shuang
• Chen, Baoliang
• Shen, Yi

Titel

Unveiling enhanced electron-mediated peroxymonosulfate activation for degradation of emerging organic pollutants

Ist Teil von

• Applied catalysis. B, Environmental, 2024-02, Vol.341, p.123356, Article 123356

Ort / Verlag

Elsevier B.V

Erscheinungsjahr

2024

Quelle

Alma/SFX Local Collection

Beschreibungen/Notizen

• The electron transfer pathway activated by peroxymonosulfate (PMS) has garnered significant attention for the removal of emerging organic pollutants from water. However, overcoming the two-step energy barriers involved in electron transport across reaction interfaces presents a formidable challenge. To surmount the two-step energy barriers of pollutant-catalyst and catalyst-PMS, a catalyst with nano-island structure was developed, forming efficient ternary catalytic interfaces with PMS and pollutants. The presence of atomic pairs within the catalyst punched through the electron transport channels, resulting in a pseudo-first-order kinetic rate of 2.06 min−1 for bisphenol A, which was 5.1 times higher than that of the control sample. The electronic coupling of atomic pairs exerted a profound impact on the splitting of d-orbitals, effectively elevating the d-orbital unoccupancy and reducing the two-step energy barriers encountered by electrons from pollutants to catalysts, and subsequently to PMS, which promoted efficient degradation of pollutants. Furthermore, through the association of two-step energy barrier, the feasibility of utilizing the orbital interaction as a descriptor of the degradation rate by electron-mediated PMS activation was demonstrated. Additionally, the intermediates generated through electron transfer pathway exhibited a lower risk of bioaccumulation. This work inspires insights into the electron-mediated mechanism of multinary catalytic interface reactions. [Display omitted] Co-Fe atomic pairs with electronic coupling were constructed on a nano-island structure to overcome the two-step energy barriers during electron-mediated peroxymonosulfate activation. The electronic coupling induces variations in d-orbitals and reduces the two-step energy barriers, facilitating electron transport from pollutants to PMS through catalyst, leading to the accelerated degradation of emerging organic pollutants. •The effective ternary catalytic interfaces were readily established.•The two-step energy barriers were reduced by electronic coupling.•Electronic coupling punched through the electron transport channels.•This work offers insights into the multinary catalytic interface reactions.