Precise manipulation of iron spin states in single-atom catalytic membranes for singlet oxygen selective production.

IF 12.2 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Na Lu, Yanle Li, Jianqiang Wang, Guiliang Li, Guowei Li, Fu Liu, Chuyang Y Tang
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引用次数: 0

Abstract

Heterogeneous single-atom catalysts are attracting substantial attention for selectively generating singlet oxygen (1O2). However, precise manipulation of atom coordination structures remains challenging. Here, the fine coordination structure of iron single-atom carbon-nitride catalysts (Fe-CNs) was manipulated by precisely tuning the heating rate with 1 °C min-1 difference. Multiple techniques in combination with density functional theory (DFT) calculations reveal that FeN6 coordination sites with high Fe spin states promote the adsorption, electron transfer, and dissociation of peroxymonosulfate (PMS), resulting in nearly 100% selection of 1O2 generation. A lamellar single atom catalytic membrane is constructed, exhibiting high permeance, high degradation, high-salinity resistance and sustained operation stability. This work provides ideas for regulating spin states of the metal site to fabricate catalysts with selective 1O2 generation for membrane separation and environment catalysis applications.

用于单线态氧选择性生产的单原子催化膜中铁自旋态的精确操纵。
非均相单原子催化剂在选择性生成单线态氧(1O2)方面受到广泛关注。然而,原子配位结构的精确操作仍然具有挑战性。本文采用1°C min-1差精确调节升温速率的方法,对铁单原子碳氮化催化剂(Fe-CNs)的精细配位结构进行了调控。多种技术结合密度泛函数理论(DFT)计算表明,具有高铁自旋态的FeN6配位位点促进了过氧单硫酸根(PMS)的吸附、电子转移和解离,导致1O2生成的选择接近100%。构造了一种具有高渗透、高降解、高耐盐性和持续运行稳定性的层状单原子催化膜。本研究为调节金属位点的自旋态,制备选择性生成1O2的催化剂,用于膜分离和环境催化提供了思路。
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来源期刊
Materials Horizons
Materials Horizons CHEMISTRY, MULTIDISCIPLINARY-MATERIALS SCIENCE, MULTIDISCIPLINARY
CiteScore
18.90
自引率
2.30%
发文量
306
审稿时长
1.3 months
期刊介绍: Materials Horizons is a leading journal in materials science that focuses on publishing exceptionally high-quality and innovative research. The journal prioritizes original research that introduces new concepts or ways of thinking, rather than solely reporting technological advancements. However, groundbreaking articles featuring record-breaking material performance may also be published. To be considered for publication, the work must be of significant interest to our community-spanning readership. Starting from 2021, all articles published in Materials Horizons will be indexed in MEDLINE©. The journal publishes various types of articles, including Communications, Reviews, Opinion pieces, Focus articles, and Comments. It serves as a core journal for researchers from academia, government, and industry across all areas of materials research. Materials Horizons is a Transformative Journal and compliant with Plan S. It has an impact factor of 13.3 and is indexed in MEDLINE.
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