High-loading inducing Fe-dimer on carbon nitride promotes the generation of ·O2−
The research on metal dimer clusters is of great importance, owing to the potential in modulating the adsorption behavior towards reaction intermediates. Here, we develop a loading heightening strategy to obtain a 32.5 wt% Fe-dimer catalyst (Fe-32.5). The co-anchoring of two Fe atoms in a single tr...
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| Format: | Article |
| Language: | English |
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KeAi Communications Co. Ltd.
2025-10-01
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| Series: | Advanced Powder Materials |
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| Online Access: | http://www.sciencedirect.com/science/article/pii/S2772834X25000442 |
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| author | Xinran Zheng Yuchao Wang Jianping Guan Xu Liu Yu Bai Yingbi Chen Peiyao Yang Jing Zhang Houzheng Ou Meng Wang Yu Xiong Haozhi Wang Yongpeng Lei |
| author_facet | Xinran Zheng Yuchao Wang Jianping Guan Xu Liu Yu Bai Yingbi Chen Peiyao Yang Jing Zhang Houzheng Ou Meng Wang Yu Xiong Haozhi Wang Yongpeng Lei |
| author_sort | Xinran Zheng |
| collection | DOAJ |
| description | The research on metal dimer clusters is of great importance, owing to the potential in modulating the adsorption behavior towards reaction intermediates. Here, we develop a loading heightening strategy to obtain a 32.5 wt% Fe-dimer catalyst (Fe-32.5). The co-anchoring of two Fe atoms in a single triazine ring of carbon nitride with an atomic spacing of ∼0.23 nm is proved. Fe atoms occupy the pores of the triazine ring in the lower iron content sample (Fe-12.9 and Fe-17.1). However, with the increase of iron content to 32.5 wt%, two Fe atoms simultaneously occupy one triazine ring. For Fe-32.5, besides the main peak located at ∼1.5 Å corresponding to the Fe–N interaction, a peak attributed to Fe–Fe bonding is observed at ∼2.2 Å in Fourier-transformed k3-weithted extended X-ray absorption fine structure. Density functional theoretical calculations reveal that Fe-dimer in Fe-32.5 induces a charge redistribution compared with that in Fe-12.9 and Fe-17.1. H2O∗ is adsorbed on O∗ via hydrogen bonding in Fe-12.9 and Fe-17.1. However, H2O∗and O∗ in Fe-32.5 are adsorbed on Fe–Fe dimer, resulting in a decrease in the total energy of the reaction process. For the two former, O2−∗ adsorbs on individual Fe atoms. Fe-dimer in Fe-32.5 adsorbs O2−∗ in the form of bridge bonds, which facilitates the ·O2− release. Furthermore, an enhanced affinity for the substrate 3,3′,5,5′-tetramethylbenzidine and higher peroxidase-like activity were displayed. This work provides an effective mean to synthesize metal dimer clusters through high loading. |
| format | Article |
| id | doaj-art-dc09b0cf6b5848ebbaff249bc5632c71 |
| institution | DOAJ |
| issn | 2772-834X |
| language | English |
| publishDate | 2025-10-01 |
| publisher | KeAi Communications Co. Ltd. |
| record_format | Article |
| series | Advanced Powder Materials |
| spelling | doaj-art-dc09b0cf6b5848ebbaff249bc5632c712025-08-20T02:44:20ZengKeAi Communications Co. Ltd.Advanced Powder Materials2772-834X2025-10-014510030810.1016/j.apmate.2025.100308High-loading inducing Fe-dimer on carbon nitride promotes the generation of ·O2−Xinran Zheng0Yuchao Wang1Jianping Guan2Xu Liu3Yu Bai4Yingbi Chen5Peiyao Yang6Jing Zhang7Houzheng Ou8Meng Wang9Yu Xiong10Haozhi Wang11Yongpeng Lei12State Key Laboratory of Powder Metallurgy, Central South University, Changsha 410083, ChinaState Key Laboratory of Powder Metallurgy, Central South University, Changsha 410083, ChinaCollege of Chemistry and Chemical Engineering, Central South University, Changsha 410083, ChinaCollege of Chemistry and Chemical Engineering, Central South University, Changsha 410083, ChinaState Key Laboratory of Powder Metallurgy, Central South University, Changsha 410083, ChinaState Key Laboratory of Powder Metallurgy, Central South University, Changsha 410083, ChinaState Key Laboratory of Powder Metallurgy, Central South University, Changsha 410083, ChinaState Key Laboratory of Powder Metallurgy, Central South University, Changsha 410083, ChinaState Key Laboratory of Powder Metallurgy, Central South University, Changsha 410083, ChinaState Key Laboratory of Powder Metallurgy, Central South University, Changsha 410083, ChinaCollege of Chemistry and Chemical Engineering, Central South University, Changsha 410083, China; Corresponding author.School of Materials Science and Engineering, Hainan University, Haikou 570228, China; Corresponding author.State Key Laboratory of Powder Metallurgy, Central South University, Changsha 410083, China; Corresponding author.The research on metal dimer clusters is of great importance, owing to the potential in modulating the adsorption behavior towards reaction intermediates. Here, we develop a loading heightening strategy to obtain a 32.5 wt% Fe-dimer catalyst (Fe-32.5). The co-anchoring of two Fe atoms in a single triazine ring of carbon nitride with an atomic spacing of ∼0.23 nm is proved. Fe atoms occupy the pores of the triazine ring in the lower iron content sample (Fe-12.9 and Fe-17.1). However, with the increase of iron content to 32.5 wt%, two Fe atoms simultaneously occupy one triazine ring. For Fe-32.5, besides the main peak located at ∼1.5 Å corresponding to the Fe–N interaction, a peak attributed to Fe–Fe bonding is observed at ∼2.2 Å in Fourier-transformed k3-weithted extended X-ray absorption fine structure. Density functional theoretical calculations reveal that Fe-dimer in Fe-32.5 induces a charge redistribution compared with that in Fe-12.9 and Fe-17.1. H2O∗ is adsorbed on O∗ via hydrogen bonding in Fe-12.9 and Fe-17.1. However, H2O∗and O∗ in Fe-32.5 are adsorbed on Fe–Fe dimer, resulting in a decrease in the total energy of the reaction process. For the two former, O2−∗ adsorbs on individual Fe atoms. Fe-dimer in Fe-32.5 adsorbs O2−∗ in the form of bridge bonds, which facilitates the ·O2− release. Furthermore, an enhanced affinity for the substrate 3,3′,5,5′-tetramethylbenzidine and higher peroxidase-like activity were displayed. This work provides an effective mean to synthesize metal dimer clusters through high loading.http://www.sciencedirect.com/science/article/pii/S2772834X25000442Single atom catalystsHigh loadingDimerAdsorption strengthIntermediate |
| spellingShingle | Xinran Zheng Yuchao Wang Jianping Guan Xu Liu Yu Bai Yingbi Chen Peiyao Yang Jing Zhang Houzheng Ou Meng Wang Yu Xiong Haozhi Wang Yongpeng Lei High-loading inducing Fe-dimer on carbon nitride promotes the generation of ·O2− Advanced Powder Materials Single atom catalysts High loading Dimer Adsorption strength Intermediate |
| title | High-loading inducing Fe-dimer on carbon nitride promotes the generation of ·O2− |
| title_full | High-loading inducing Fe-dimer on carbon nitride promotes the generation of ·O2− |
| title_fullStr | High-loading inducing Fe-dimer on carbon nitride promotes the generation of ·O2− |
| title_full_unstemmed | High-loading inducing Fe-dimer on carbon nitride promotes the generation of ·O2− |
| title_short | High-loading inducing Fe-dimer on carbon nitride promotes the generation of ·O2− |
| title_sort | high loading inducing fe dimer on carbon nitride promotes the generation of ·o2 |
| topic | Single atom catalysts High loading Dimer Adsorption strength Intermediate |
| url | http://www.sciencedirect.com/science/article/pii/S2772834X25000442 |
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