期刊
CHEMISTRY OF MATERIALS
卷 30, 期 3, 页码 799-806出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.7b04313
关键词
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资金
- Foundation for National Natural Science Foundation of China [51425203, 51772191]
- Foundation for the Author of National Excellent Doctoral Dissertation of PR China [201434]
- Innovation Program of Shanghai Municipal Education Commission [15ZZ008]
- Program of Shanghai Subject Chief Scientist [15XD1501900]
- Shanghai Rising-Star Program [15QA1402700]
- Natural Science Foundation of Shanghai [17ZR1441100]
- International Science & Technology Cooperation Program of China [2015DFE52870]
The development of new pathways for 3D artificial photosynthetic systems (APS) with controllable architectures and tunable hierarchical porosity on a large scale is significant. Herein, we demonstrate a 3D printing approach for fabricating artificial microleaves with 3D architectures spanning orders of magnitude from nanometers to centimeters in a rapid, programmable, and scalable manner. TiO2-based inks served as a preliminary prototype, with surfactants and silica nanospheres incorporated for porosity modification. Thus, a TiO2-based ink is developed to allow for the fabrication of porosity-tunable hierarchical 3D architectures with high surface area (up to similar to 259 m(2)g(-1)) and structural integrity with well-designed patterns. The artificial microleaves have macropore architectures comparable to those of natural leaves, indicating their efficient mass transfer ability. Artificial photosynthesis via CO, reduction enhances CO and CH4 evolution on the 3D printed APS by up to 2-fold and 6-fold, respectively, compared with the levels observed for the corresponding powder counterparts. Furthermore, gas diffusion behaviors, closely related to the gas-phase reaction, are investigated by theoretical simulation to reveal the hierarchical structural effects on catalytic efficiency. The strategy is proven to be critical and demonstrates obvious advantages in the potential scale-up of 3D APS device manufacturing.
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