The development of new pathways for 3D solar energy conversion and utilization systems with controllable architectures and tunable hierarchical porosity on a large scale is significant. Herein, we demonstrate a 3D printing approach for fabricating artificial micro-leaves 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 ~259 m2g-1) and structural integrity with well-designed patterns. The artificial micro-leaves have macropore architectures comparable to those of natural leaves, indicating their efficient mass transfer ability. Artificial photosynthesis via CO2 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. Furthermore, We propose a 3D printing methodology to enable the programmable construction of carbon nitride-based hybrid aerogel membranes with patterned macroscopic architectures. g-C3N4 nanosheets (CNNS) are used as the building block, and sodium alginate (SA) increases the viscosity of the ink to obtain the desired rheological properties. Three printing routes, including printing directly in air and in the supporting reservoirs composed of CaCl2/glycerol solution or Pluronic F127, are demonstrated for printing versatility. The printed Au nanobipyramids-CNNS-SA hybrid aerogels exhibit broadband visible-light absorption and superior solar wastewater remediation performances with excellent cyclic stability and easy manipulation features. This approach could be extended to the macroscopic assembly of other 2D materials for myriad applications.

Solar energy conversion and utilization systems via 3D printing technique

256th National Meeting (2018)

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