Great research progress in photocatalytic organic synthesis has been made recently by Professor Zhang Zehui’s research team of the School of Chemistry and Materials Science. On December 14, the research paper High Nitrile Yields of Aerobic Ammoxidation of Alcohols Achieved by Generating •O2- and Br• Radicals over Iron-Modified TiO2Photocatalysts was published in the Journal of the American Chemical Society, one of the top international journals in chemistry (link to article: https://doi.org/10.1021/jacs.2c07061). Xian Chensheng and He Jie are the co-first authors of the article, respectively a postgraduate and a doctor from SCMZU, with Prof. Ze-Hui Zhang and Prof. Huaiyong Zhu from Queensland University of Technology as the corresponding authors and SCMZU as the first signatory.
The article reports on stable photocatalysts composed of iron-modified titanium dioxide (Fe/TiO2) for efficient ammonia oxidation reactions at room temperature that used oxygen and ammonia at atmospheric pressure as nitrogen source, and ammonium bromide as an additive. The modification of titanium dioxide by iron promoted the formation of reactive •O2- radicals, increased the adsorption of ammonia and amino intermediates on the catalyst, and accelerated the oxidation of ammonia to nitrile. The additive ammonium bromide acted as a hydrogen atom transfer agent to oxidize bromine ions to form bromine radicals (Br•), which significantly improved the catalytic efficiency. It synergizes with •O2- to capture H• from Cα-H, which in turn generates radicals centered on activated carbon. The reaction system can be obtained in ideal yield (80.3%) under solar irradiation and the catalyst possesses good stability with no significant chemical physical property changes for several weeks of light exposure. The combination of the photovoltaic properties of iron-modified titanium dioxide and the synergistic effect of bromine radicals (Br•) and superoxide radicals (•O2-) provides new opportunities for the development of semiconductor-based photocatalytic systems for fine chemical synthesis.
It is reported that the Green Synthetic Catalysis school-level team, led by Prof. Zehui Zhang, relying on the School of Chemical Materials, is mainly engaged in the catalytic conversion of biomass, photocatalytic organic synthesis and related research. The team has published a series of important researches in international top journals such as Nature Communications, Science Advances, Chem, Angewandte Chemie International Edition, Journal of the American Chemical Society, Chemical Society Reviews, etc., making considerable contributions to the development of the research field.
Edited by Liu Hong Reviewed by Pan Wenjun