通过锚定 Pt 位点的 2D/2D 异质结构催化剂促进可见光驱动的氢气进化:Cd-TCPP(Pt)@CdS

IF 9.1 Q1 ENGINEERING, CHEMICAL Green Chemical Engineering Pub Date : 2024-03-15 DOI:10.1016/j.gce.2024.03.002
Guo-Wei Guan, Yi-Tao Li, Li-Ping Zhang, Su-Tao Zheng, Si-Chao Liu, Hao-Ling Lan, Qing-Yuan Yang
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引用次数: 0

摘要

太阳能水分离是一种新兴的制氢方法。然而,它仍然面临着一些挑战,包括提高光响应速度、最大限度地利用光催化剂活性位点以及有效利用光诱导载流子以防止氢气产量过低。在本研究中,我们提出了一种设计二维/二维异质结构催化剂 Cd-TCPP(Pt)@CdS 的方法,该催化剂由二维 CdS 纳米片(NSs)和具有铂活性位点的二维金属有机框架(MOF)(Cd-TCPP(Pt))组成,旨在实现可见光驱动的高效氢气进化。首先,CdS NSs 对可见光具有极佳的响应性,确保了光诱导载流子的稳健生成。其次,二维 MOF 提供了丰富的铂活性位点,提高了电子利用率,降低了质子还原的能量障碍。与纯 CdS NSs(其制氢活性为 1220 μmol/g/h)相比,新设计的二维/二维复合催化剂 Cd-TCPP(Pt)@CdS 的活性为 13,434 μmol/g/h,提高了 11 倍。令人印象深刻的是,即使在阳光下,Cd-TCPP(Pt)@CdS 也能保持 3062 μmol/g/h 的高活性。密度泛函理论(DFT)计算用于研究质子还原原理。CdS 的合适带隙和二维 Cd-TCPP(Pt)的能隙有助于它们的强相互作用,从而提高氢气进化的效率。铂单原子(Pt-SA)也为质子还原提供了自由能较低的位点,从而提高了活性。Cd-TCPP(Pt)@CdS NSs 复合材料的光催化性能表明,二维无机半导体与含有铂位点的二维 MOF 之间存在协同效应,从而提高了光诱导载流子和原子的利用率。
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Boosting visible-light-driven hydrogen evolution through Pt site anchored 2D/2D heterostructure catalyst: Cd-TCPP(Pt)@CdS
Solar-powered water splitting is an up-and-coming method for hydrogen production. Still, it faces several challenges, including improving light responsiveness, maximizing utilization of photocatalyst active sites, and effectively utilizing photo-induced carriers to prevent low hydrogen production. In this research, we propose an approach for designing a 2D/2D heterostructure catalyst, the Cd-TCPP(Pt)@CdS, which consists of 2D CdS nanosheets (NSs) and a 2D metal-organic framework (MOF) with Pt active sites (Cd-TCPP(Pt)), aiming to achieve highly efficient visible-light-driven hydrogen evolution. Firstly, CdS NSs exhibit excellent responsiveness to visible light, ensuring robust generation of photo-induced carriers. Secondly, the 2D MOF provides abundant Pt active sites, enhancing electron utilization and reducing the energy barrier for proton reduction. Compared to pure CdS NSs (which demonstrate a hydrogen production activity of 1220 μmol/g/h), the newly designed 2D/2D composite catalyst Cd-TCPP(Pt)@CdS exhibits an activity of 13,434 μmol/g/h, representing an 11-fold increase. Impressively, Cd-TCPP(Pt)@CdS maintains a high activity of 3062 μmol/g/h even under sunlight. Density functional theory (DFT) calculations were employed to investigate the principle of proton reduction. The suitable bandgap of CdS and energy gap of 2D Cd-TCPP(Pt) contribute to their strong interaction and consequently higher efficiency in hydrogen evolution. The Pt-single atom (Pt-SA) also provides sites with low free energy for proton reduction, contributing to improved activity. The photocatalytic performance of Cd-TCPP(Pt)@CdS NSs composites demonstrates a synergistic effect between the 2D inorganic semiconductor and the 2D MOF containing the Pt-site, resulting in enhanced utilization of photo-induced carriers and atoms.
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来源期刊
Green Chemical Engineering
Green Chemical Engineering Process Chemistry and Technology, Catalysis, Filtration and Separation
CiteScore
11.60
自引率
0.00%
发文量
58
审稿时长
51 days
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