Z 型 MIL-125-NH2(Ti)/PdTCPP异质结通过金氧化物电子桥加速载流子分离,实现高效光催化脱氮和氢气进化

IF 5.8 2区 材料科学 Q2 CHEMISTRY, PHYSICAL Journal of Alloys and Compounds Pub Date : 2024-07-02 DOI:10.1016/j.jallcom.2024.175428
Yue Li, Junhao Zhou, Xiaoping He, Youzhou He, Jiajia Jing, Xingyan Liu, Siqi Li, Siping Wei
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引用次数: 0

摘要

在全球双碳目标的推动下,光催化技术作为一种绿色技术,正被用于去除氮氧化物和制氢。然而,由于光催化剂对可见光的响应较弱以及光生载流子的分离效率较低,其应用往往受到限制。本文设计了一种简单高效的光催化剂 Au@NM-125/PdTCPP,用于去除 NO 和氢气进化。通过在 MIL-125-NH(Ti)中加入具有优异光吸收能力的 PdTCPP 分子,PdTCPP 的引入扩大了可见光的吸收范围。另一方面,具有表面等离子共振效应的 Au NPs 的引入促进了 PdTCPP 与 MIL-125-NH(Ti) 之间的电子传输,从而大大提高了光催化性能。与原始 NM-125 的氮氧化物去除率(22.06%)相比,NM-125/PdTCPP 的氮氧化物去除率为 63.72%,而 Au@NM-125/PdTCPP 的氮氧化物去除率最高,达到 73.23%。此外,Au@NM-125/PdTCPP 还表现出优异的氢进化性能(4 小时内 12.659 mmol/g),氢进化效果是 NM-125/PdTCPP 的 2.14 倍(4 小时内 5.911 mmol/g)和初始 NM-125 的 6.85 倍(4 小时内 1.848 mmol/g)。根据紫外可见光谱、Mott-Schottky 和 XPS 光谱的结果,我们提出了一种可能的光催化机理:MIL-125-NH(Ti) 和 PdTCPP 的合适带隙值使它们形成了一个 Z 型异质结,电子从 PdTCPP 流向 MIL-125-NH(Ti),而金纳米粒子作为电子桥促进了更多的电子转移,从而提高了光催化性能。将金属卟啉分子作为半导体直接与 MOFs 结合形成异质结,并加入 Au NPs 作为电子桥,是实现优异光催化性能的可行策略,在环境修复和能源生产方面也具有重要价值。
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Z-scheme MIL-125-NH2(Ti)/PdTCPP heterojunction accelerates carrier separation via Au NPs electron bridge for efficient photocatalytic NO removal and hydrogen evolution
Under the global dual-carbon goal, photocatalysis technology is being employed as a green technology for NO removal and hydrogen production. However, the application of photocatalysts is often limited by the weak response to visible light and the low separation efficiency of photogenerated carriers. In this paper, we designed a simple and efficient photocatalyst Au@NM-125/PdTCPP for NO removal and hydrogen evolution. By adding PdTCPP molecule with excellent light absorption ability combine with MIL-125-NH(Ti), the introduction of PdTCPP expands the absorption range of visible light. On the other hand, the introduction of Au NPs with surface plasmon resonance effect promotes electron transport between PdTCPP and MIL-125-NH(Ti), thus greatly improving the photocatalytic performance. Compared with the NO removal efficiency of the original NM-125 (22.06 %), the NO removal rate of NM-125/PdTCPP was 63.72 %, while the NO removal rate of Au@NM-125/PdTCPP was the highest, reaching 73.23 %. What’s more, Au@NM-125/PdTCPP also demonstrated excellent hydrogen evolution performance (12.659 mmol/g, in 4 h), with a hydrogen evolution effect 2.14 times that of NM-125/PdTCPP (5.911 mmol/g, in 4 h) and 6.85 times that of the initial NM-125 (1.848 mmol/g, in 4 h). Based on the results of UV-Vis spectroscopy, Mott-Schottky and XPS spectrum, we proposed a possible photocatalytic mechanism, the suitable band gap value of MIL-125-NH(Ti) and PdTCPP makes them form a Z-scheme heterojunction, where electrons flow from PdTCPP to MIL-125-NH(Ti), and Au NPs acts as an electron bridge to promote more electron transfer, thus improving the photocatalytic performance. It is a practicable strategy to achieve excellent photocatalytic performance by combining metalloporphyrin molecules as semiconductors directly with MOFs to form heterojunctions and adding Au NPs as electronic bridges, which is also valuable for environmental remediation and energy production.
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来源期刊
Journal of Alloys and Compounds
Journal of Alloys and Compounds 工程技术-材料科学:综合
CiteScore
11.10
自引率
14.50%
发文量
5146
审稿时长
67 days
期刊介绍: The Journal of Alloys and Compounds is intended to serve as an international medium for the publication of work on solid materials comprising compounds as well as alloys. Its great strength lies in the diversity of discipline which it encompasses, drawing together results from materials science, solid-state chemistry and physics.
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