Abstract
Using solar energy to convert CO2 into value-added fuel is crucial for the goal of global carbon neutrality. Effective separation of photogenerated charges is important for improving photocatalytic CO2 reduction efficiency. Herein, we report a facile in situ exfoliation and conversion strategy to synthesize a novel CeO2/C3N4 heterostructure by uniformly distributing CeO2 nanoparticles onto ultrathin porous C3N4 nanosheets. The ultrathin porous structure of C3N4 not only increases the specific surface area to provide more active sites but also effectively shortens the migration distance of photogenerated electron holes to avoid their recombination. In addition, the well-dispersed CeO2 on C3N4 shows an intimate interface contact, which allows more charges to be transferred through the increased interface surface area. The as-synthesized CeO2/C3N4 heterojunction with well-matched band gaps and a Z-scheme structure prolongs the lifetime of photo-induced charge carriers and maximizes the redox ability of the photocatalyst. Without a noble metal cocatalyst or a sacrificial agent, the CO2 photoreduction performance of the CeO2/C3N4 heterojunction is approximately 5-fold enhanced compared with that of bulk C3N4. This study provides a facile strategy for the design and practical application of direct Z-scheme pho-tocatalysts for sustainable energy conversion.
摘要
利用太阳能将CO2转化为增值燃料, 对于实现全球碳中和的目标 ¾ßÓÐÖØÒªÒâÒå, ¶ø¹âÉúµçºÉµÄÓÐЧ·ÖÀëÊÇÌá¸ß¹â´ß»¯CO2»¹ÔЧC2;ʵÄÖØ 要影响因素. 在此, 我们报道了一种简易的原位剥离和转化策略, 将 CeO2ÄÉÃ׿ÅÁ£¾ùÔÈ·Ö²¼ÔÚ³¬±¡¶à¿×C3N4ÄÉÃ×ƬÉÏ, ºÏ³ÉÁËÐÂÐ굀 CeO2/C3N4异质结构. C3N4的超薄多孔结构不仅可以增加比表面积以 提供更多的活性位点, 还可以有效缩短光生电子空穴的迁移距离以避 免复合. 此外, 高度分散的CeO2与C3N4之间具有紧密的界面接触, 使更 多的电荷通过界面进行转移. 合成的CeO2/C3N4异质结构具有带隙匹配 的Z型结构, 可以有效延长光诱导电荷载流子的寿命并提升光催化剂的 氧化还原能力. 与传统块状C3N4相比, 合成的CeO2/C3N4异质结在没有 贵金属作为助催化剂和没有牺牲剂条件下显示出约5倍的CO2光还原 性能的提升. 这项工作为用于可持续能源转换的直接Z型光催化剂的设 计和实际应用提供了一种新策略.
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Acknowledgements
This work was supported by the National Key R&D Program of China (2022YFA1503003), the National Natural Science Foundation of China (U20A20250, 21801069 and 91961111), the Natural Science Foundation of Heilongjiang Province (YQ2021B008), the Basic Research Fund of Heilongjiang University in Heilongjiang Province (2022-KYYWF-1036 and 2021-KYYWF-0039), and Heilongjiang University Excellent Youth Foundation.
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Chen J conducted the synthesis of materials and performed the characterizations and photocatalytic tests. Xiao Y, Wang N and Kang X analyzed partial experimental data. Wang D, Wang C and Jiang Y assisted with the experiments and characterizations. Chen J wrote the paper with support from Liu J and Fu H. All authors contributed to the general discussion.
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Jie Chen is currently an MSc candidate in inorganic chemistry under the supervision of associate Prof. Jian-cong Liu and Prof. Honggang Fu at Heilongjiang University. Her research focuses on novel photocatalytic materials.
Jiancong Liu received her BSc and PhD degrees in 2012 and 2017, respectively, from Jilin University. Then, she joined Heilongjiang University as an assistant professor in 2018. Her interests focus on zeolite-based nanocomposites for hydrogenation catalysis and porous materials with long afterglow luminescence properties.
Honggang Fu received his BSc and MSc degrees in 1984 and 1987, respectively, from Jilin University. He joined Heilongjiang University as an assistant professor in 1988. In 1999, he received a PhD degree from Harbin Institute of Technology. He became a full professor in 2000. His interests focus on oxide-based nanomaterials for solar energy conversion and photocatalysis, carbon-based nanomaterials for energy conversion and storage, and electrocatalysis.
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Chen, J., Xiao, Y., Wang, N. et al. Facile synthesis of a Z-scheme CeO2/C3N4 heterojunction with enhanced charge transfer for CO2 photoreduction. Sci. China Mater. 66, 3165–3175 (2023). https://doi.org/10.1007/s40843-023-2443-0
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DOI: https://doi.org/10.1007/s40843-023-2443-0