<br>了解类芬顿反应中单原子活性位点的距离效应，以实现有效的水体修复,Advanced Science

当前位置： X-MOL 学术 › Adv. Sci. › 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.)

了解类芬顿反应中单原子活性位点的距离效应，以实现有效的水体修复
Advanced Science ( IF 14.3 ) Pub Date : 2024-01-15 , DOI: 10.1002/advs.202307151
Shuaiqi Zhang ₁ , Zhicong Lu ₁ , Chun Hu ₁ , Fan Li ₁

Affiliation

新兴的单原子催化剂（SAC）在通过类芬顿反应进行水修复方面前景广阔。尽管通过增加单原子活性位点的密度显着增强了催化活性，但性能的提高并不仅仅归因于活性位点数量的增加。由于原子密度增加而引起的催化行为的变化特别难以捉摸，值得深入研究。在此，通过控制Fe负载量构建了相邻单原子Fe位点之间具有不同距离（ d_位点）的单原子Fe催化剂（Fe _SA -CN）。随着d_位值的降低，通过过一硫酸盐 (PMS) 活化的电子转移机制实现了 Fe _SA -CN 的催化活性显着增强。 d_位点值的降低促进电子通讯并进一步改变电子结构，有利于 PMS 激活。此外，两个相邻的单原子Fe位点共同吸附PMS并实现PMS分解产物的单位点解吸，保持持续的PMS激活和污染物去除。此外，Fe _SA -CN/PMS系统对各种水生系统表现出优异的抗干扰性能，并且在连续流实验中具有良好的耐用性，表明其在水处理应用中具有巨大的潜力。本研究通过设计密集的 SAC，深入了解单原子活性位点对水体修复的距离影响。

"点击查看英文标题和摘要"

Understanding the Distance Effect of the Single-Atom Active Sites in Fenton-Like Reactions for Efficient Water Remediation

Emerging single-atom catalysts (SACs) are promising in water remediation through Fenton-like reactions. Despite the notable enhancement of catalytic activity through increasing the density of single-atom active sites, the performance improvement is not solely attributed to the increase in the number of active sites. The variation of catalytic behaviors stemming from the increased atomic density is particularly elusive and deserves an in-depth study. Herein, single-atom Fe catalysts (Fe_SA-CN) with different distances (d_site) between the adjacent single-atom Fe sites are constructed by controlling Fe loading. With the decrease in d_site value, remarkably enhanced catalytic activity of Fe_SA-CN is realized via the electron transfer regime with peroxymonosulfate (PMS) activation. The decrease in d_site value promotes electronic communication and further alters the electronic structure in favor of PMS activation. Moreover, the two adjacent single-atom Fe sites collectively adsorb PMS and achieve single-site desorption of the PMS decomposition products, maintaining continuous PMS activation and contaminant removal. Moreover, the Fe_SA-CN/PMS system exhibits excellent anti-interference performance for various aquatic systems and good durability in continuous-flow experiments, indicating its great potential for water treatment applications. This study provides an in-depth understanding of the distance effect of single-atom active sites on water remediation by designing densely populated SACs.

更新日期：2024-01-15

点击分享查看原文

点击收藏

公开下载

阅读更多本刊新发论文本刊介绍/投稿指南