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Interfacial Hydroxyl Promotes the Reduction of 4 Nitrophenol by Ag-Based Catalysts Confined in Dendritic Mesoporous Silica Nanospheres
preprintsubmitted on 26.11.2020, 05:22 and posted on 27.11.2020, 04:56 by Xiao-Dan Hu, Bingqian Shan, Ran Tao, Taiqun Yang, Kun Zhang
Surface states—the electronic states emerging as a solid material terminates at a surface—are usually vulnerable to contaminations and defects. This fundamental limitation has prohibited systematic studies of the potential role of surface states in surface reactions and catalysis, especially in more realistic environments. We use the selective reduction of 4-Nitrophenol on silver-covered dendritic mesoporous silica nanospheres (DMSNs) as a prototype example, and show that the dynamic intermediate surface states (DISS) spatially formed by spin orbital coupling (SOC) in singly hydrated hydroxyl complex can significantly enhance the adsorption energy of both 4-Nitrophenol and BH4- anions, by promoting different directions of static electron transfer. The concept of DISS as an electron bath may lead to new design principles beyond the conventional d-band theory of heterogeneous catalysis.