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具有外延异质界面和空间分离的光氧化还原位点的一维CdS@CdZnS@ZnS-Ni(OH)纳米杂化物,可实现高效可见光驱动的析氢反应。

One-dimensional CdS@CdZnS@ZnS-Ni(OH) nano-hybrids with epitaxial heterointerfaces and spatially separated photo-redox sites enabling highly-efficient visible-light-driven H evolution.

作者信息

Ruan Qinqin, Ma Xiaowei, Li Yanyan, Wu Jiakun, Wang Zhiyang, Geng Yanling, Wang Wenjing, Lin Haifeng, Wang Lei

机构信息

Taishan Scholar Advantage and Characteristic Discipline Team of Eco Chemical Process and Technology, Key Laboratory of Eco-chemical Engineering, College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao 266042, P. R. China.

Key Laboratory of Design and Assembly of Functional Nanostructures, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fujian 350002, P. R. China.

出版信息

Nanoscale. 2020 Oct 15;12(39):20522-20535. doi: 10.1039/d0nr04007j.

Abstract

Photocatalytic solar-to-fuel conversion has been of great interest in recent years. Nevertheless, the rational structural manipulation of photocatalysts toward an efficient H2 evolution reaction (HER) is still under-developed. In this work, by employing CdS nanowires as the growth substrate, unique one-dimensional (1D) CdS@Cd0.5Zn0.5S@ZnS-Ni(OH)2 heterostructures were first synthesized through the ultrasonic water-bath reaction combined with subsequent hydrothermal and in situ photo-deposition processes. Under the optimized conditions, CS@30CZ0.5S@40ZS-3N with 30 wt% Cd0.5Zn0.5S, 40 wt% ZnS, and 3 wt% Ni(OH)2 achieves a visible-light-driven HER activity as high as 86.79 mmol h-1 g-1 (corresponding to an apparent quantum yield of 22.8% at 420 nm), which is 4 and 119 times higher than that of Pt-decorated CS@30CZ0.5S@40ZS and CdS, respectively. In addition, CdS@Cd0.5Zn0.5S@ZnS-Ni(OH)2 is also endowed with a good stability for H2 production under long-term irradiation. The spatial separation of photo-redox sites and epitaxial heterointerfaces in CdS@Cd0.5Zn0.5S@ZnS-Ni(OH)2 nanowires facilitate the charge transfer and separation effectively, accounting well for their superior photocatalytic capability. The results indicated in this work could benefit the exploitation of high-performance nanostructures for promising photocatalytic applications.

摘要

近年来,光催化太阳能到燃料的转化备受关注。然而,针对高效析氢反应(HER)对光催化剂进行合理的结构调控仍不够成熟。在这项工作中,以硫化镉(CdS)纳米线作为生长基底,通过超声水浴反应结合后续水热和原位光沉积过程,首次合成了独特的一维(1D)CdS@Cd0.5Zn0.5S@ZnS-Ni(OH)2异质结构。在优化条件下,含有30 wt% Cd0.5Zn0.5S、40 wt% ZnS和3 wt% Ni(OH)2的CS@30CZ0.5S@40ZS-3N实现了高达86.79 mmol h-1 g-1的可见光驱动HER活性(对应于420 nm处22.8%的表观量子产率),分别是Pt修饰的CS@30CZ0.5S@40ZS和CdS的4倍和119倍。此外,CdS@Cd0.5Zn0.5S@ZnS-Ni(OH)2在长期辐照下制氢也具有良好的稳定性。CdS@Cd0.5Zn0.5S@ZnS-Ni(OH)2纳米线中光氧化还原位点的空间分离和外延异质界面有效地促进了电荷转移和分离,很好地解释了它们优异的光催化能力。这项工作所得结果有助于开发用于有前景的光催化应用的高性能纳米结构。

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