Min Dai, Zhihui Yin, Shuaiqi Zhang, Fengming Situ, Xiaoyue Zhou, Jun Xiong, Ning Jiang, Peng Zhang*, Chun Hu and Fan Li*,
{"title":"光催化水净化中单原子铁电子结构和电荷行为的调控","authors":"Min Dai, Zhihui Yin, Shuaiqi Zhang, Fengming Situ, Xiaoyue Zhou, Jun Xiong, Ning Jiang, Peng Zhang*, Chun Hu and Fan Li*, ","doi":"10.1021/acsestengg.5c00206","DOIUrl":null,"url":null,"abstract":"<p >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 (Fe<sub>SA</sub>-PCN) consisting of polymeric graphitic carbon nitride (g-C<sub>3</sub>N<sub>4</sub>) 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 Fe<sub>SA</sub>-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-C<sub>3</sub>N<sub>4</sub>. 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 H<sub>2</sub>O<sub>2</sub>, and further activated into <sup>•</sup>OH for pollutant degradation. Consequently, Fe<sub>SA</sub>-PCN demonstrates outstanding efficiency in pollutant degradation, resistance to interference, and stability, which proposes a promising strategy for developing g–C<sub>3</sub>N<sub>4</sub>–based photocatalysts for applications in environmental remediation.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":"5 9","pages":"2294–2304"},"PeriodicalIF":6.7000,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Regulation of the Electronic Structure and Charge Behaviors Derived from Single-Atom Iron for Photocatalytic Water Purification\",\"authors\":\"Min Dai, Zhihui Yin, Shuaiqi Zhang, Fengming Situ, Xiaoyue Zhou, Jun Xiong, Ning Jiang, Peng Zhang*, Chun Hu and Fan Li*, \",\"doi\":\"10.1021/acsestengg.5c00206\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >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 (Fe<sub>SA</sub>-PCN) consisting of polymeric graphitic carbon nitride (g-C<sub>3</sub>N<sub>4</sub>) 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 Fe<sub>SA</sub>-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-C<sub>3</sub>N<sub>4</sub>. 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 H<sub>2</sub>O<sub>2</sub>, and further activated into <sup>•</sup>OH for pollutant degradation. 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Regulation of the Electronic Structure and Charge Behaviors Derived from Single-Atom Iron for Photocatalytic Water Purification
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.
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.