Regulation of the Electronic Structure and Charge Behaviors Derived from Single-Atom Iron for Photocatalytic Water Purification

IF 6.7 Q1 ENGINEERING, ENVIRONMENTAL
Min Dai, Zhihui Yin, Shuaiqi Zhang, Fengming Situ, Xiaoyue Zhou, Jun Xiong, Ning Jiang, Peng Zhang*, Chun Hu and Fan Li*, 
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引用次数: 0

Abstract

Large-scale and sustainable photocatalytic water treatment requires semiconductors with appropriate band structures and efficient charge transfer properties. Motivated by this point, a facial method is reported for synthesizing an efficient single-atom photocatalyst (FeSA-PCN) consisting of polymeric graphitic carbon nitride (g-C3N4) rationally integrated with Fe single atoms (Fe SAs). Fe SAs not only enhance the oxidation ability of the holes on the valence band but also introduce a doping energy level directly into the band gap, significantly expanding the light absorption range of FeSA-PCN. The density functional theory (DFT) calculations and characterization results such as Kelvin probe force microscopy (KPFM) imply that a significant polarized distribution of surface charges is constructed owing to the electronic interaction between Fe SAs and g-C3N4. This enables the efficient separation and transfer of photogenerated charge carriers for surface reactions. Subsequently, high-oxidation-capability holes directly oxidize adsorbed pollutants, while electrons are captured by oxygen, reduced via a two-electron process to H2O2, and further activated into OH for pollutant degradation. Consequently, FeSA-PCN demonstrates outstanding efficiency in pollutant degradation, resistance to interference, and stability, which proposes a promising strategy for developing g–C3N4–based photocatalysts for applications in environmental remediation.

Abstract Image

光催化水净化中单原子铁电子结构和电荷行为的调控
大规模、可持续的光催化水处理需要具有合适能带结构和高效电荷转移特性的半导体。基于此,本文报道了一种由石墨化氮化碳(g-C3N4)与铁单原子(Fe SAs)合理结合而成的高效单原子光催化剂(FeSA-PCN)的合成方法。Fe - SAs不仅增强了价带上空穴的氧化能力,而且在带隙中直接引入了掺杂能级,显著扩大了FeSA-PCN的光吸收范围。密度泛函理论(DFT)计算和表征结果(如开尔文探针力显微镜(KPFM))表明,由于Fe - sa和g-C3N4之间的电子相互作用,表面电荷形成了明显的极化分布。这使得光生载流子的有效分离和转移表面反应成为可能。随后,高氧化能力的空穴直接氧化被吸附的污染物,而电子被氧捕获,通过双电子过程还原为H2O2,并进一步活化成•OH,用于污染物降解。因此,FeSA-PCN在污染物降解、抗干扰和稳定性方面表现出卓越的效率,这为开发基于g - c3n4的光催化剂用于环境修复提供了一个有前途的策略。
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来源期刊
ACS ES&T engineering
ACS ES&T engineering ENGINEERING, ENVIRONMENTAL-
CiteScore
8.50
自引率
0.00%
发文量
0
期刊介绍: ACS ES&T Engineering publishes impactful research and review articles across all realms of environmental technology and engineering, employing a rigorous peer-review process. As a specialized journal, it aims to provide an international platform for research and innovation, inviting contributions on materials technologies, processes, data analytics, and engineering systems that can effectively manage, protect, and remediate air, water, and soil quality, as well as treat wastes and recover resources. The journal encourages research that supports informed decision-making within complex engineered systems and is grounded in mechanistic science and analytics, describing intricate environmental engineering systems. It considers papers presenting novel advancements, spanning from laboratory discovery to field-based application. However, case or demonstration studies lacking significant scientific advancements and technological innovations are not within its scope. Contributions containing experimental and/or theoretical methods, rooted in engineering principles and integrated with knowledge from other disciplines, are welcomed.
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