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Highly efficient nitrogen fixation over S-scheme heterojunction photocatalysts with enhanced active hydrogen supply.

ABSTRACT: Photocatalytic N₂ fixation is a promising strategy for ammonia (NH₃) synthesis; however, it suffers from relatively low ammonia yield due to the difficulty in the design of photocatalysts with both high charge transfer efficiency and desirable N₂ adsorption/activation capability. Herein, an S-scheme CoS_x/ZnS heterojunction with dual active sites is designed as an efficient N₂ fixation photocatalyst. The CoS_x/ZnS heterojunction exhibits a unique pocket-like nanostructure with small ZnS nanocrystals adhered on a single-hole CoS_x hollow dodecahedron. Within the heterojunction, the electronic interaction between ZnS and CoS_x creates electron-deficient Zn sites with enhanced N₂ chemisorption and electron-sufficient Co sites with active hydrogen supply for N₂ hydrogenation, cooperatively reducing the energy barrier for N₂ activation. In combination with the promoted photogenerated electron-hole separation of the S-scheme heterojunction and facilitated mass transfer by the pocket-like nanostructure, an excellent N₂ fixation performance with a high NH₃ yield of 1175.37 μmol g^-1 h^-1 is achieved. This study provides new insights into the design of heterojunction photocatalysts for N₂ fixation.

SUBMITTER: Bao T

PROVIDER: S-EPMC10989659 | biostudies-literature | 2024 May

REPOSITORIES: biostudies-literature

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Highly efficient nitrogen fixation over S-scheme heterojunction photocatalysts with enhanced active hydrogen supply.

Bao Tong T Xi Yamin Y Zhang Chaoqi C Du Peiyang P Xiang Yitong Y Li Jiaxin J Yuan Ling L Yu Chengzhong C Liu Chao C

National science review 20240309 5

Photocatalytic N2 fixation is a promising strategy for ammonia (NH3) synthesis; however, it suffers from relatively low ammonia yield due to the difficulty in the design of photocatalysts with both high charge transfer efficiency and desirable N2 adsorption/activation capability. Herein, an S-scheme CoSx/ZnS heterojunction with dual active sites is designed as an efficient N2 fixation photocatalyst. The CoSx/ZnS heterojunction exh ...[more]

PMID: 38577667

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Project description:The preparation of visible light-responsive efficient photocatalysts for removing organic contaminants from water and killing cancer cells has gotten a lot of attention due to the growing global concern. In this study, we have successfully fabricated an efficient AgBr/β-MnO2 nanocomposite via a facile deposition and precipitation method at room temperature. Techniques such as XRD, SEM-EDS, TEM, DRS, PL, EIS, ESR, and FTIR were used to determine the crystalline, structural, morphological, optical, and other properties. The SEM and TEM analyses reveal that AgBr NPs are decorated on the surface of β-MnO2, which possesses rods with a sphere-like structure for AgBr/β-MnO2. The EDX analysis confirms the existence of Mn, O, Ag, and Br elements in the nanocomposites without an extra peak, indicating that the synthesized samples are highly pure. The high photocatalytic performance of AgBr/β-MnO2 could be attributed to the formation of Ag NPs and the construction of the Z-scheme heterojunction between AgBr and β-MnO2. This may enhance fast light absorption and efficient photogenerated (e-/h+) pairs, as indicated by EIS and photoluminescence measurements, which in turn achieved high activity for the decomposition of MB (97%, in 12 min), RhB (98.9%, in 9 min), and paracetamol (80%, in 180 min), respectively. The kinetic model study proposed that the first-order model showed a better fit than the zero- and second-order for the photocatalytic decolorization of RhB dye. XRD analysis of 0.2 AgBr/β-MnO2 before and after recycling confirms the high stability of the catalyst. HPLC results showed that no detectable by-products are produced through the decomposition of paracetamol. Interestingly, 0.2 AgBr/β-MnO2 nanocomposites showed visible light-induced anticancer activity against A549 cancer cell lines. The mechanistic degradation pathway has been proposed using the involvement of active species like superoxide radicals (-•O2) and photoinduced holes (h+). The proposed work focuses on synthesizing effective photocatalysts in a less hazardous environment with superior biological activity.

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Highly efficient nitrogen fixation over S-scheme heterojunction photocatalysts with enhanced active hydrogen supply.

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Highly efficient nitrogen fixation over S-scheme heterojunction photocatalysts with enhanced active hydrogen supply.

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