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Solar‐Driven Hydrogen Generation Catalyzed by g‐C3N4 with Poly(platinaynes) as Efficient Electron Donor at Low Platinum Content
Advanced Science ( IF 15.1 ) Pub Date : 2021-01-04 , DOI: 10.1002/advs.202002465
Xuan Zhou 1, 2, 3 , Yurong Liu 2, 3 , Zhengyuan Jin 1 , Meina Huang 1 , Feifan Zhou 1 , Jun Song 1 , Junle Qu 1 , Yu-Jia Zeng 1 , Peng-Cheng Qian 4 , Wai-Yeung Wong 2, 3
Affiliation  

A metal‐complex‐modified graphitic carbon nitride (g‐C3N4) bulk heterostructure is presented here as a promising alternative to high‐cost noble metals as artificial photocatalysts. Theoretical and experimental studies of the spectral and physicochemical properties of three structurally similar molecules Fo–D, Pt–D, and Pt–P confirm that the Pt(II) acetylide group effectively expands the electron delocalization and adjusts the molecular orbital levels to form a relatively narrow bandgap. Using these molecules, the donor–acceptor assemblies Fo–D@CN, Pt–D@CN, and Pt–P@CN are formed with g‐C3N4. Among these assemblies, the Pt(II) acetylide‐based composite materials Pt–D@CN and Pt–P@CN with bulk heterojunction morphologies and extremely low Pt weight ratios of 0.19% and 0.24%, respectively, exhibit the fastest charge transfer and best light‐harvesting efficiencies. Among the tested assemblies, 10 mg Pt–P@CN without any Pt metal additives exhibits a significantly improved photocatalytic H2 generation rate of 1.38 µmol h−1 under simulated sunlight irradiation (AM1.5G, filter), which is sixfold higher than that of the pristine g‐C3N4.

中文翻译:

低铂含量下以聚铂炔为有效电子供体的 g-C3N4 催化太阳能制氢

本文提出了一种金属络合物改性的石墨碳氮化物(g-C 3 N 4)体异质结构,作为高成本贵金属作为人造光催化剂的有前景的替代品。对三种结构相似分子Fo–DPt–DPt–P的光谱和物理化学性质的理论和实验研究证实,Pt(II) 乙炔基有效地扩大了电子离域并调整分子轨道能级,形成带隙相对较窄。使用这些分子,用g-C 3 N 4形成供体-受体组件Fo–D @ CNPt–D @ CNPt–P @ CN。在这些组件中,基于 Pt(II) 乙炔化物的复合材料Pt–D @ CNPt–P @ CN具有本体异质结形态和极低的 Pt 重量比,分别为 0.19% 和 0.24%,表现出最快的电荷转移和最佳的光收集效率。在测试的组件中,在模拟太阳光照射下(AM1.5G,滤光片) ,不含任何Pt金属添加剂的10 mg Pt–P @ CN表现出显着提高的光催化H 2生成率为1.38 µmol h -1,是其六倍原始的g-C 3 N 4
更新日期:2021-02-17
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