Abstract
Two-dimensional porous nanosheet heterostructure materials, which combine the advantages of both architecture and components, are expected to feature a significant photocatalytic performance toward CO2 conversion into useful fuels. Herein, we provide a facile strategy for fabricating sulfur-doped C3N4 porous nanosheets with embedded SnO2-SnS2 nanojunctions (S-C3N4/SnO2-SnS2) via liquid impregnation-pyrolysis and subsequent sulfidation treatment using a layered supramolecular structure as the precursor of C3N4. A hexagonal layered supramolecular structure was first prepared as the precursor of C3N4. Then Sn4+ ions were intercalated into the supramolecular interlayers through the liquid impregnation method. The subsequent annealing treatment in air simultaneously realized the fabrication and efficient exfoliation of layered C3N4 porous nanosheets. Moreover, SnO2 nanoparticles were formed and embedded in situ in the porous C3N4 nanosheets. In the following sulfidation process under a nitrogen atmosphere, sulfur powder can react with SnO2 nanoparticles to form SnO2-SnS2 nanojunctions. As expected, the exfoliation of sulfur-doped C3N4 porous nanosheets and ternary heterostructure construction could be simultaneously achieved in this work. Sulfur-doped C3N4 porous nanosheets with embedded SnO2-SnS2 nanojunctions featured abundant active sites, enhanced visible light absorption, and efficient interfacial charge transfer. As expected, the optimized S-C3N4/SnO2-SnS2 achieved a much higher gas-phase photocatalytic CO2 reduction performance with high yields of CO (21.68 μmolg−1 h−1) and CH4 (22.09 μmolg−1 h−1) compared with the control C3N4, C3N4/SnO2, and S-C3N4/SnS2 photocatalysts. The selectivity of CH4 reached 80.30%. Such a promising synthetic strategy can be expected to inspire the design of other robust C3N4-based porous nanosheet heterostructures for a broad range of applications.
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摘要
结合了多孔纳米片和异质结优点的二维多孔纳米片异质结构材 料预计能在CO2光催化还原为燃料过程中表现出优异的性能. 本文中, 我们提出了一种简便的合成方案, 即通过液体浸渍-热解和后续的硫化 处理, 将层状结构的超分子前驱体转变成C3N4, 形成了硫掺杂的原位嵌 入的SnO2-SnS2纳米异质结C3N4多孔纳米片(S-C3N4/SnO2-SnS2). 在这 项研究中, 硫掺杂的C3N4多孔纳米片的剥离和SnO2-SnS2纳米异质结同 时获得. SnO2-SnS2纳米异质结的硫掺杂C3N4多孔纳米片具有丰富的活 性位点、增**的可见光吸收能力和界面电荷转移效率. **如预期, 与 C3N4, C3N4/SnO2和S-C3N4/SnS2光催化剂相比, 优化的S-C3N4/SnO2-SnS2具有更高的气相光催化还原CO2性能, CO产率(21.68 μmol g−1 h−1) 和CH4产率(22.09 μmol g−1 h−1)显著提高. CH4的选择性可达80.30%. 这 种合成策略有望推动其他C3N4基多孔纳米片异质结构的研究, 以实现 更广泛的应用.
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Acknowledgements
This work was supported by the National Natural Science Foundation of China (22072037 and 51772079) and the Natural Science Foundation of Heilongjiang Province of China (LH2020B018).
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Author contributions Tian G and Chen Y designed the project; Chen X and Liu X performed the experiments; Li L and Du L performed the data analysis; Tian G, Chen Y and Chen X wrote the paper. All authors contributed to the general discussion.
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** new photocatalysts for CO2 reduction.
Guohui Tian received his BSc degree in chemistry from Heilongjiang University in 1998. In 2008, he received his PhD degree in inorganic chemistry from Heilongjiang University. Then he worked at Heilongjiang University. He is currently a researcher at Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education of China, Heilongjiang University. His research interests focus on energy-related inorganic functional materials.
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Boosted Charge Transfer and Photocatalytic CO2 Reduction over Sulfur-Doped C3N4 Porous Nanosheets with Embedded SnS2-SnO2 Nanojunctions
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Chen, X., Chen, Y., Liu, X. et al. Boosted charge transfer and photocatalytic CO2 reduction over sulfur-doped C3N4 porous nanosheets with embedded SnS2-SnO2 nanojunctions. Sci. China Mater. 65, 400–412 (2022). https://doi.org/10.1007/s40843-021-1744-5
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DOI: https://doi.org/10.1007/s40843-021-1744-5