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Unique Cd1−xZnxS@WO3−x and Cd1−xZnxS@WO3−x/CoOx/NiOx Z-scheme photocatalysts for efficient visible-light-induced H2 evolution

Z-机制光催化剂Cd1−xZnxS@WO3−x和Cd1−xZnx S@WO3−x/CoOx/NiOx及其高效可见光解水产氢活 性研究

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Abstract

Artificial Z-scheme photocatalytic systems have received considerable attention in recent years because they can achieve wide light-absorption, high charge-separation efficiency, and strong redox ability simultaneously. Nevertheless, it is still challenging to exploit low-cost and stable Z-scheme photocatalysts with highly-efficient H2 evolution from solar water-splitting so far. Herein, we report a novel all-solid-state Z-scheme photocatalyst Cd1−xZnxS@WO3−x consisting of Cd1−xZnxS nanorods coated with oxygen-deficient WO3−x amorphous layers. The Cd1−xZnxS@WO3−x exhibits an outstanding H2 evolution reaction (HER) activity as compared with Pt-loaded Cd1−xZnxS and most \({\bf{W}}{{\bf{O}}_{{3^{-}}}}\) and CdS-based photocatalysts, due to the generation of stronger reducing electrons through the appropriate Zn-do** in Cd1−xZnxS and the enhanced charge transfer by introducing oxygen vacancies (W5+/OVs) into the ultrathin WO3−x amorphous coatings. The optimal HER rate of Cd1−xZnxS@WO3−x is determined to be 21.68 mmol h−1 g−1, which is further raised up to 28.25 mmol h−1 g−1 (about 12 times more than that of Pt/Cd1−xZnxS) when Cd1−xZnxS@WO3−x is hybridized by CoOx and NiOx dual cocatalysts (Cd1−xZnxS@WO3−x/CoOx/NiOx) through in-situ photo-deposition. Moreover, the corresponding apparent quantum yield (AQY) at 420 nm is significantly increased from 34.6% for Cd1−xZnxS@WO3−x to 60.8% for Cd1−xZnxS@WO3−x/CoOx/NiOx. In addition, both Cd1−xZn−-S@WO3−x and Cd1−xZnxS@WO3−x/CoOx/NiOx demonstrate good stability towards HER. The results displayed in this work will inspire the rational design and synthesis of high-performance nanostructures for photocatalytic applications.

摘要

人工Z-机制光催化剂因其同时具有光吸收范围宽、电荷分离效率高以及载流子氧化还原能力**等优势受到了研究者们的广泛关注. 然而, 设计和制备能够利用太阳能进行高效光解水产氢的低成本、高稳定性非贵金属Z-机制光催化剂仍具有挑战性. 本文报道了一种新颖的全固态Z-机制光催化剂Cd1−xZnxS@WO3−x, 该催化剂纳米结构是由氧缺陷WO3−x非晶层包覆Cd1−xZnxS纳米棒组成. 研究结果表明, 由于适量的Zn掺杂使得Cd1−xZnxS具有更**的产生还原性电子能力, 同时, WO3−x超薄非晶层中引入的氧空位(W5 +/OVs)有效地促进了电荷的分离, 使得该Z-机制Cd1−x-ZnxS@WO3−x光催化材料具有优异的光催化产氢反应(HER)活性, 且显著高于贵金属Pt负载的Cd1−xZnxS纳米棒(Pt/Cd1−xZnxS)及绝大多数WO3和CdS基光催化剂. 优化后的Cd1−xZnxS@WO3−x复合光催化剂的HER速率可达21.68 mmol h−1 g−1. 进一步通过原位光沉积负载CoOx和NiOx双共催化剂, Cd1−xZnxS@WO3−x/CoOx/NiOx复合材料的活性高达28.25 mmol h−1 g−1, 约为Pt/Cd1−xZnxS的12倍. 计算结果表明, Cd1−xZnxS@WO3−x在420 nm激发光下的HER表观量子产率(AQY)为34.6%, 而负载CoOx和NiOx双共催化剂后的Cd1−x-ZnxS@WO3−x/CoOx/NiOx的AQY提高到了60.8%. 此外, Cd1−xZnxS@WO3−x和Cd1−xZnxS@WO3−x/CoOx/NiOx均表现出了良好的长时间HER稳定性. 该工作将为理性设计和制备高效光解水产氢催化剂提供新视角.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (51572136, 51772162, 21571112, 51802170 and 21801150), the Natural Science Foundation of Shandong Province (ZR2018BEM014, ZR2018LB008 and ZR2019MB001), Taishan Scholar Foundation of Shandong Province (H. W., ts201712047), the Special Fund Project to Guide Development of Local Science and Technology by Central Government (H.W.), and Taishan Scholar Program of Advantage and Characteristic Discipline Team of Eco Chemical Process and Technology.

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  1. Key Laboratory of Eco-Chemical Engineering, Taishan Scholar Advantage and Characteristic Discipline Team of Eco-Chemical Process and Technology, Key Laboratory of Rubber-Plastics of Ministry of Education, Shandong Provincial Key Laboratory of Rubber-Plastics, College of Chemistry and Molecular Engineering, School of Polymer Science and Engineering, Qingdao University of Science and Technology, Qingdao, 266042, China

    Yanyan Li  (黎艳艳), Qinqin Ruan  (阮芹芹), Haifeng Lin  (林海峰), Yanling Geng  (耿延玲), Jiefei Wang  (王婕菲), Hui Wang  (王辉), Yu Yang  (杨宇) & Lei Wang  (王磊)

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  1. Yanyan Li  (黎艳艳)
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  2. Qinqin Ruan  (阮芹芹)
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  3. Haifeng Lin  (林海峰)
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  7. Yu Yang  (杨宇)
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Contributions

Lin H designed and engineered the experiments; Li Y, Ruan Q, Geng Y, Wang J, and Wang H performed the experiments, analyzed the data and wrote the paper with support from Yang Y and Wang L. All authors contributed to the general discussion.

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Correspondence to Haifeng Lin  (林海峰) or Lei Wang  (王磊).

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The authors declare no conflict of interest.

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Supporting data are available in the online version of the paper.

Yanyan Li is currently an associate professor in the College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology. She received her PhD degree in material physics and chemistry from Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences in 2015. Her current research mainly focuses on the design, synthesis and photocatalytic applications of semiconductor nanocrystals.

Haifeng Lin received his PhD degree from Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences in 2014. Then, he worked as a postdoctoral scholar at Tsinghua University (2014–2017). In 2017, he joined Qingdao University of Science and Technology as an associate professor. His current research interest concentrates on the design and controlled synthesis of semiconducting nanohybrids and their applications in efficient solar-to-fuel conversion.

Lei Wang obtained his PhD degree in inorganic chemistry from Jilin University in 2006. He is now a professor in inorganic chemistry in the College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology. The current research of his group focuses on the synthesis of nano-sized functional materials for applications in photocatalysis, electrocatalysis, and batteries.

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Unique Cd1−xZnxS@WO3−x and Cd1−xZnxS@WO3−x/ CoOx/NiOx Z-scheme photocatalysts for efficient visible-light-induced H2 evolution

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Li, Y., Ruan, Q., Lin, H. et al. Unique Cd1−xZnxS@WO3−x and Cd1−xZnxS@WO3−x/CoOx/NiOx Z-scheme photocatalysts for efficient visible-light-induced H2 evolution. Sci. China Mater. 63, 75–90 (2020). https://doi.org/10.1007/s40843-019-1179-4

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