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- W4280490875 abstract "Formation and evolution of active hydrogen species from H2 on a metal oxide is of great importance in many hydrogenation reactions, while understanding the nature of surface hydrogen species remains a great challenge. Herein, high-vacuum-based transmission infrared spectroscopy coupled with temperature-programmed desorption has been applied to study surface hydrogen species over ZnO and ZnCrOx catalysts. We show that D2 dissociates readily to form Zn–D and O–D on ZnO at 153 K, and simultaneous Zn–D and O–D desorption in the form of D2 occurs at 223 K. This corroborates reversible dissociation and recombination of D2 on ZnO. (Cr−)Zn–D and (Cr−)O–D species appear on ZnCr2O4 in D2 at 273 K, indicating a higher barrier for D2 activation than that on ZnO. (Cr−)Zn–D can diffuse to form (Cr−)O–D at 573 K, and then desorption of surface O-D groups requires a higher temperature of 943 K. Theoretical studies demonstrate that surface geometry plays a crucial role in the evolution of the surface hydrogen species. The polar ZnCr2O4(111) surface can stabilize metal-H species due to the high barrier for its surface diffusion and the thermodynamic obstruction for its association with O–H, in contrast with the nonpolar ZnO(101̅0) surface. These results provide insights into the tuning of the stability of surface metal-H species on metal oxide catalysts, which will contribute to tailoring the hydrogenation processes in the H-involved catalytic reactions." @default.
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- W4280490875 date "2022-05-11" @default.
- W4280490875 modified "2023-10-13" @default.
- W4280490875 title "Modulating the Formation and Evolution of Surface Hydrogen Species on ZnO through Cr Addition" @default.
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- W4280490875 doi "https://doi.org/10.1021/acscatal.2c00978" @default.
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