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一种铂-卟啉锆金属有机框架作为用于氢气生成的有效光催化剂。

A platinum-porphyrin zirconium metal-organic framework as an effective photocatalyst for hydrogen generation.

作者信息

Xiao Lina, Zhang Qiuping, Wang Xinzhi, Zhang Huan, Li Wenxuan, Zhang Hao, Li Bowen

机构信息

Analysis and Testing Center, Xinyang University, Xinyang, 464000, PR China.

Institute for Ocean Engineering, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, PR China; Department of Civil and Environmental Engineering, Hanyang University, 222 Wangsimni-Ro, Seoul, 04763, Republic of Korea.

出版信息

Environ Res. 2025 Aug 1;278:121710. doi: 10.1016/j.envres.2025.121710. Epub 2025 Apr 25.

Abstract

Efficient solar energy storage via light-driven hydrogen (H) production presents a promising and attractive strategy for addressing the global energy crisis. The integration of platinum (Pt) co-catalyst into metal-organic frameworks (MOFs) to enhance photoinduced charge separation and transfer remains a significant challenge. Herein, a platinum-porphyrin zirconium metal-organic framework (MOF) PCN-223(Pt) is reported, and synthesized using a facile two-solvent strategy. The prepared PCN-223(Pt) is self-sensitized and contains a platinum (Pt) electron-trapping center, which confers excellent visible-light catalytic activity. Under visible-light irradiation, PCN-223(Pt) produced 732 μmol g h of H, a 7.6-fold increase compared to the isostructural PCN-223, which lacks Pt coordination in its porphyrin rings. This improvement results from the photogenerated electrons' efficient transport to the Pt electron-trapping centers, which improves charge carrier separation. Density functional theory calculations demonstrate the positive role that Pt in PCN-223(Pt) play in optimizing the corresponding hydrogen binding energy. PCN-223(Pt) exhibits excellent recyclability, maintaining its catalytic performance across five cycles without significant degradation. These results offer a new approach for designing MOF-based highly efficient visible-light active catalysts.

摘要

通过光驱动产氢实现高效太阳能存储是应对全球能源危机的一种有前景且具吸引力的策略。将铂(Pt)助催化剂整合到金属有机框架(MOF)中以增强光生电荷的分离和转移仍然是一项重大挑战。在此,报道了一种铂卟啉锆金属有机框架(MOF)PCN - 223(Pt),并采用简便的双溶剂策略合成。所制备的PCN - 223(Pt)是自敏化的,且含有铂(Pt)电子捕获中心,赋予其优异的可见光催化活性。在可见光照射下,PCN - 223(Pt)产氢量为732 μmol g⁻¹ h⁻¹,相较于在卟啉环中缺乏Pt配位的同结构PCN - 223增加了7.6倍。这种改善源于光生电子向Pt电子捕获中心的有效传输,从而改善了电荷载流子的分离。密度泛函理论计算表明PCN - 223(Pt)中的Pt在优化相应氢结合能方面发挥的积极作用。PCN - 223(Pt)表现出优异的可回收性,在五个循环中保持其催化性能且无明显降解。这些结果为设计基于MOF的高效可见光活性催化剂提供了一种新方法。

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