Quantifying the contribution of lanthanum single atoms in photocatalytic Fenton-like processes with a rigorous benchmarking protocol

IF 7.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Cell Reports Physical Science Pub Date : 2024-08-27 DOI:10.1016/j.xcrp.2024.102170
Xinyu Bai, Meiting Ju, Hengli Qian, Chao Xie, Ruite Lai, Tianliang Xia, Guanjie Yu, Yao Tang, Chengxu Wang, Fei Qu, Haijiao Xie, Qidong Hou
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Abstract

Single-atom catalysts (SACs) are increasingly of interest for Fenton-like processes for water treatment due to maximized metal utilization. However, their feasibility has not been conclusively demonstrated, partly due to inconsistent preparation and benchmarking. Here, we verify the catalytic activity of lanthanum single atoms for pollutant degradation by a rigorous benchmarking protocol that considers the contributions of adsorption, catalytic activity of supports, and leached ions. The reaction rate constant increases linearly with lanthanum loading up to 9 wt %, illustrating the viability of synchronously realizing high specific activity and maximized atom utilization. In addition, we show that the synergetic activation of peroxymonosulfate (PMS) and oxygen to produce multiple reactive oxygen species (ROS) is responsible for the catalytic performance, revealing the previously ignored contributions of air in catalytic systems. We anticipate that this protocol will aid in the development of SACs to realize their full prospects.

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用严格的基准协议量化镧单质原子在光催化 Fenton-like 过程中的贡献
单原子催化剂(SAC)可最大限度地利用金属,因此在类似芬顿的水处理过程中越来越受到关注。然而,它们的可行性尚未得到确证,部分原因是制备和基准不一致。在此,我们采用严格的基准测试方法验证了单原子镧对污染物降解的催化活性,该方法考虑了吸附、支撑物的催化活性和浸出离子的贡献。反应速率常数随着镧负载量的增加而线性增加,最高可达 9 wt %,这说明了同步实现高比活度和原子利用率最大化的可行性。此外,我们还表明,过氧单硫酸盐(PMS)和氧气的协同活化产生多种活性氧(ROS)是催化性能的原因,揭示了空气在催化系统中以往被忽视的贡献。我们预计,该方案将有助于开发 SAC,以实现其全部前景。
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来源期刊
Cell Reports Physical Science
Cell Reports Physical Science Energy-Energy (all)
CiteScore
11.40
自引率
2.20%
发文量
388
审稿时长
62 days
期刊介绍: Cell Reports Physical Science, a premium open-access journal from Cell Press, features high-quality, cutting-edge research spanning the physical sciences. It serves as an open forum fostering collaboration among physical scientists while championing open science principles. Published works must signify significant advancements in fundamental insight or technological applications within fields such as chemistry, physics, materials science, energy science, engineering, and related interdisciplinary studies. In addition to longer articles, the journal considers impactful short-form reports and short reviews covering recent literature in emerging fields. Continually adapting to the evolving open science landscape, the journal reviews its policies to align with community consensus and best practices.
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