Solar energy-driven organic synthesis performance control principle diagram based on atomic precision shell

Recently, Professor Xiong Yujie of the University of Science and Technology of China, based on the inorganic solid-precision preparation chemistry, designed a class of bimetallic nanostructures with an atomic-accuracy shell that has broad-spectrum solar energy utilization characteristics. By cooperating with the research group of China National University of Science and Technology Professor Zhang Qun, the effect of plasmon properties in the catalytic reaction was interpreted on the ultra-rapid time scale of picoseconds, and the performance of solar-driven organic synthesis was controlled. The work was published on the May 13th issue of the American Chemical Society. The co-first authors are doctoral students Huang Hao and Zhang Lei.

Metallic palladium is a highly efficient catalyst for many organic reactions. However, compared with common gold and silver, conventional metal palladium nanomaterials have poor absorption of sunlight, and the absorption range is limited to the ultraviolet wavelength, which brings enormous difficulties to solar energy capture and utilization. . On the other hand, the plasmon effect after light absorption of metal nanomaterials is very complicated, generally by generating hot electrons with high energy to be transferred to catalytic reaction molecules or by photothermal conversion to provide a heat source for catalytic reaction. How to control and optimize these two processes for the needs of organic synthesis is a difficult problem in the field.

Xiong Yujie's research group designed a series of gold-palladium core-shell nanostructures with atomic-accuracy shells for this series of challenges. In this design, the one-dimensional rod-like structure of the gold core greatly improves its light-absorbing performance. It not only absorbs light in a wide spectrum of visible light and near-infrared light, but also has a strong light-absorbing ability. At the same time, the metal palladium shell with controlled thickness at the atom precision provides convenience for the regulation of hot electron life and light-to-heat conversion rate. Based on systematic catalytic tests and combined with ultrafast absorption spectroscopy characterization by Zhang Qun's group, the researchers established the intrinsic link between the two plasmon processes and catalytic organic synthesis performance. Based on this understanding, researchers were able to regulate the performance of solar-driven organic synthesis through shell thickness control.

So far, the metal plasmon driven catalytic reaction is still a new research direction, and the mechanism of the photothermal effect and the thermoelectron effect in the process is still unclear in the industry. This progress provides the possibility of using solar energy as a substitute for heat source to drive organic synthesis, and it also plays an important role in the rational design of plasmon catalytic materials.

The above research work has been supported by the National Natural Science Foundation of China, the National Youth 1000 Program, the Chinese Academy of Sciences 100 Persons Program, the Hefei University Science Center, the Chinese Academy of Sciences pilot project, and the school's important project development fund.

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