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Selective Photocatalytic Dehydrogenation of Formic Acid on Graphite Carbon Nitride with Dual-Sited Cobalt and Platinum Cocatalysts
ACS Applied Nano Materials ( IF 5.9 ) Pub Date : 2024-04-16 , DOI: 10.1021/acsanm.4c00279
Hang Xu 1, 2 , Heng Zhao 2, 3 , Jian Xu 3 , Mehdi Eisapour 2 , Zechuan Yu 4 , Hang Su 5 , Yuan Li 6 , Fujian Zhou 1 , Jinguang Hu 2 , Zhangxing Chen 2, 3
Affiliation  

Photocatalytic hydrogen production from the selective dehydrogenation of liquid organic hydrogen carriers is emerging as a promising alternative for green hydrogen generation. In this work, graphite carbon nitride (CN)-based photocatalyst is rationally designed by photodeposition of cobalt oxide nanoparticles as the hole trapper for the deprotonation of formic acid (FA), while the photogenerated electrons collected by in situ photodeposited platinum (Pt) nanoparticles reduce these protons to produce sustainable hydrogen. As a result, the well-designed photocatalyst (Co-CN) exhibits excellent hydrogen evolution activity (9039 μmol/h/g) and >99.98% dehydrogenation selectivity. Besides, Co-CN shows great durability in the long-time cycling test. Density functional theory reveals the contribution of Pt and cobalt oxide on the deprotonation from O–H and C–H breakage, respectively. Technoeconomic analysis demonstrates the potential of this reaction system for scale-up application. This present work demonstrates a great example for green hydrogen production from dehydrogenation of liquid organic hydrogen carriers under a mild condition.

中文翻译:

双位钴和铂助催化剂在石墨碳氮化物上选择性光催化甲酸脱氢

通过液态有机氢载体的选择性脱氢来光催化制氢正在成为绿色制氢的一种有前途的替代方案。在这项工作中,合理设计了石墨氮化碳(CN)基光催化剂,通过光沉积氧化钴纳米颗粒作为甲酸(FA)去质子化的空穴捕获剂,同时通过原位光沉积铂(Pt)纳米颗粒收集光生电子减少这些质子以产生可持续的氢气。因此,精心设计的光催化剂(Co-CN)表现出优异的析氢活性(9039 μmol/h/g)和>99.98%的脱氢选择性。此外,Co-CN在长时间循环测试中表现出良好的耐久性。密度泛函理论揭示了 Pt 和氧化钴分别对 O-H 和 C-H 断裂去质子化的贡献。技术经济分析证明了该反应系统具有放大应用的潜力。目前的工作展示了在温和条件下通过液态有机氢载体脱氢生产绿色氢气的一个很好的例子。
更新日期:2024-04-16
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