Low Temperature Ammonia Synthesis from Atomic N and Water on Rutile TiO2(110)

Yuemiao Lai Qing Guo Xiao Chen

Yuemiao Lai, Qing Guo, Xiao Chen. Low Temperature Ammonia Synthesis from Atomic N and Water on Rutile TiO2(110)†[J]. Chinese Journal of Chemical Physics . doi: 10.1063/1674-0068/cjcp2210152
Citation: Yuemiao Lai, Qing Guo, Xiao Chen. Low Temperature Ammonia Synthesis from Atomic N and Water on Rutile TiO2(110)[J]. Chinese Journal of Chemical Physics . doi: 10.1063/1674-0068/cjcp2210152

doi: 10.1063/1674-0068/cjcp2210152

Low Temperature Ammonia Synthesis from Atomic N and Water on Rutile TiO2(110)

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  • Figure  1.  Typical TPD spectra acquired at (a) m/z=17 (NH3+, OH+) and (b) m/z=18 (H2O+) after surfaces of R-TiO2(110) were exposed to activated N for different sputtering times, followed by the dosing of 1 ML H2O at 120 K. The contribution of H2O in the TPD signal of m/z = 17 has been subtracted.

    Figure  2.  The decay of H2O (red circles) and the yield of NH3 (blue squares) as a function of sputtering time, derived from FIG. 1. All the plotted lines are only drawn to guide the eye.

    Figure  3.  Typical TPD spectra collected at (a) m/z = 18 (ND2+, NDH2+, OD+, H2O+), (b) m/z = 19 (NHD2+, HDO+) and (c) m/z = 20 (ND3+, D2O+) after surfaces of R-TiO2(110) were exposed to activated N for 5 min, followed by the dosing of 1 ML D2O at 120 K.

    Figure  4.  Typical TPD spectra collected at (a) m/z = 30 (NO+) and (b) m/z = 44 (CO2+, N2O+) after the surface was exposed to activated N for 5 min, followed by dosing with different coverages of H2O.

    Figure  5.  Typical TPD spectra collected at (a) m/z = 17 (NH3+, OH+) and (b) m/z = 18 (H2O+) as a function of H2O coverage. Before H2O adsorption, R-TiO2(110) surfaces were exposed to activated N for 5 min. The dash line in (b) represents the TPD spectrum collected after the clean R-TiO2(110) surface was dosed with 1 ML H2O.

    Figure  6.  Schematic model of hydrogen atom diffusion in NH3 formation. (a) Hydrogen diffusion along the Ob rows toward atomic N without the assistance of H2O; (b) H2O diffusion along the Ti5c rows toward atomic N; (c) H2O-assisted hydrogen diffusion across the Ob rows. Atoms are labeled as follows: Ti5c3+ sites (open black circles), Ti6c4+ sites (filled yellow circles), Ti5c4+ sites (filled purple circles), bridge-bonded oxygen atoms (BBO, filled pink circles), atomic N (Nads, filled green circles), H atoms (filled blue circles).

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  • 收稿日期:  2022-10-21
  • 录用日期:  2022-12-06
  • 网络出版日期:  2022-12-08

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