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用于析氢的金纳米颗粒控制在石墨相氮化碳纳米片上形成金属和氧化态铂纳米颗粒。

Au nanoparticle-controlled formation of metallic and oxidized Pt nanoparticles on graphitic carbon nitride nanosheets for H evolution.

作者信息

Guo Xin, Kong Lina, Xu Jianping, Chen Jing, Li Lan

机构信息

School of Materials Science and Engineering, Institute of Material Physics, Key Laboratory of Display Materials and Photoelectric Devices, Ministry of Education, and Tianjin Key Laboratory for Photoelectric Materials and Devices, and National Demonstration Center for Experimental Function Materials Education, Tianjin University of Technology, Tianjin 300384, China.

出版信息

Dalton Trans. 2021 Jul 13;50(27):9529-9539. doi: 10.1039/d1dt00910a.

Abstract

Surface decoration of noble-metal cocatalysts on graphitic phase carbon nitride (g-C3N4) with high efficiency and trace content for water splitting is exciting but difficult to achieve. Herein, we report the anchoring of Au and metallic/oxidized Pt nanoparticles (NPs) on g-C3N4 as cocatalysts via a photoreduction process for enhancing photocatalytic H2 production. Au NPs are preferentially decorated on g-C3N4, which can control the formation of metallic/oxidized Pt complex species. The well dispersed Au and metallic/oxidized Pt NPs improved the light-harvesting and the photo-generated carrier separation of g-C3N4. G-C3N4 sequentially decorated with Au (0.3 wt%) and metallic/oxidized Pt (0.3 wt%) cocatalysts, exhibited the highest and stable H2 evolution rates of 2560 and 139 μmol h-1 g-1 under simulated sunlight and visible light (λ ≥ 420 nm) irradiation, respectively, compared to the samples that are simultaneously and sequentially decorated with the same content of Pt and Au on g-C3N4. The enhanced photocatalytic activity is attributed to the synergistic effect of Au and metallic/oxidized Pt cocatalysts, i.e., the effective localized surface plasma resonance coupling between Pt and Au NPs, as well as electron-sink function of metallic Pt, which promote the generation and transfer of more carriers from g-C3N4 to the Pt species, in addition to the superior hydrogen evolution capacity of metallic and oxidized Pt. This work maximizes the performance of noble-metal cocatalysts with minimized content and provides the possibility of realizing efficient solar-to-fuel conversion.

摘要

在石墨相氮化碳(g-C₃N₄)上进行高效且痕量的贵金属助催化剂表面修饰以用于水分解,这令人兴奋但难以实现。在此,我们报道了通过光还原过程将金和金属/氧化态铂纳米颗粒(NPs)锚定在g-C₃N₄上作为助催化剂,以增强光催化产氢性能。金纳米颗粒优先修饰在g-C₃N₄上,这可以控制金属/氧化态铂复合物种的形成。分散良好的金和金属/氧化态铂纳米颗粒改善了g-C₃N₄的光捕获和光生载流子分离。与在g-C₃N₄上同时和依次修饰相同含量的铂和金的样品相比,依次用0.3 wt%的金和0.3 wt%的金属/氧化态铂助催化剂修饰的g-C₃N₄,在模拟太阳光和可见光(λ≥420 nm)照射下,分别表现出最高且稳定的产氢速率,即2560和139 μmol h⁻¹ g⁻¹。增强的光催化活性归因于金和金属/氧化态铂助催化剂的协同效应,即铂和金纳米颗粒之间有效的局域表面等离子体共振耦合,以及金属铂的电子汇集功能,除了金属和氧化态铂优异的析氢能力外,这些促进了更多载流子从g-C₃N₄向铂物种的产生和转移。这项工作以最小化的含量最大化了贵金属助催化剂的性能,并为实现高效的太阳能到燃料转化提供了可能性。

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