Dalian Dye Institute realizes the photo-generated charges of different crystal faces of a single photocatalyst particle

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Photoelectric Imaging of Photogenerated Charges in Different Crystal Surfaces of Individual Photocatalyst Particles by DAL

Recently, the Chinese Academy of Sciences Dalian Institute of Chemical Physics, State Key Laboratory of Catalysis and the Clean Energy National Laboratory of the Department of Solar Energy Research Li Can, 100-person plan scholar Fan Fengji and Ph.D. Zhu Jian, etc., have independently developed a nanometer surface photovoltage imaging system. For the first time, photoelectric imaging of the photogenerated charge of different crystal faces of a single photocatalyst particle was realized. It was found that there are different space charge layer built-in electric fields between the semiconductor particles. The built-in electric field can promote highly anisotropic separation of photogenerated charge. The results were published online in the journal German Applied Chemistry.

Photocatalytic water decomposition is generally considered as one of the ideal approaches to solve the energy crisis and environmental pollution in the future, and photoelectron-hole effective separation is the key to achieving efficient photo-chemical conversion of solar energy. The establishment of an effective photovoltaic system for the separation and transmission of photogenerated charge has become an important measure for the development of a highly efficient artificial light synthesis catalyst system and is an important direction for scientists in this field. In recent years, Li Can's research team has made unremitting efforts to solve this core scientific problem: by constructing a CdS/MoS2 heterojunction, better photocatalytic activity for hydrogen production than Pt/CdS photocatalyst supported by a traditional noble metal Pt (J. Am. Chem. Soc., 2008, 130, 7176-7177); It is reported for the first time in the world that the use of ultraviolet Raman spectroscopy is sensitive to the surface phase and can significantly increase the “heterojunction” between the different phases of TiO2. Enhancing the photocatalytic activity of hydrogen production; based on this, it was found that the “heterojunction” constructed with semiconductor photocatalysts based on α, β-Ga 2 O 3 can promote the photocatalytic decomposition of pure water to hydrogen production, and the use of ultrafast spectroscopy is preliminary. The nature of its photocatalytic activity was revealed (Angew. Chem. Int. Ed., 2012, 51, 13089-13092); subsequently, the research group found that BiVO4 semiconductor photocatalytic materials with regular crystal surface exposure existed between different crystal planes. Photogenerated Charge Separation Effects (Nature Comm., 2013, 4, 1432).

In order to further reveal the key scientific issues of the above-mentioned system—the spatial characteristics of photogenerated charge separation and migration, the team developed a nano-photoelectricity imaging system for the study of the spatial distribution of photogenerated charge on the surface of micro-nanoscale and single semiconductor catalyst grains— Spatially resolved surface photovoltage spectra. The researchers used this instrument to observe the difference in surface potential of different crystal planes on the BiVO4 particles. Under light excitation, spatial resolution surface photovoltage spectroscopy reveals that there are different space charge layer built-in electric fields on different crystal planes of semiconductor particles. The presence of such an electric field can enable single-crystal semiconductor photocatalysts to exhibit more than 70-fold differential hole transport anisotropy, and further use of fluorescence imaging corroborates this result. This intrinsic physical property may be the main reason for the separation of photogenerated charges between different crystal planes. This work reveals the nature of photocatalyst's photo-induced charge separation from the micro-nano scale, and provides a scientific basis for the further development of high-efficiency solar photocatalytic hydrogen production and carbon dioxide reduction and other artificial photosynthetic systems.

This work was supported by the National Natural Science Fund, the "973" Project of the Ministry of Science and Technology and the Collaborative Innovation Center for Energy Materials Chemistry (2011 · iChEM) of the Ministry of Education.

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