N2 emission-channel change in NO reduction over stepped Pd(211) by angle-resolved desorption |
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| Authors: | Tatsuo Matsushima Anton Kokalj Hideo Orita Toshitaka Kubo Masataka Sakurai Takahiro Kondo Junji Nakamura |
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| Institution: | 1. Catalysis Research Center, Hokkaido University, Sapporo, 001-0021, Japan;2. Jozef Stefan Institute, Jamova 39, 1000 Ljubljana, Slovenia;3. Nanosystem Research Institute (NRI), National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba Central 2, 1-1-1 Umezono, Tsukuba, Ibaraki 305-8568, Japan;4. Nanosystem Research Institute (NRI), National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba Central 5, 1-1-1 Higashi, Tsukuba, Ibaraki 305-8565, Japan;5. Faculty of Pure and Applied Sciences, University of Tsukuba, Tennodai 1-1-1,Tsukuba, Ibaraki 305-8573, Japan |
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| Abstract: | A sharp change in the N2 emission channel from N2O(a) → N2(g) + O(a) to N(a) + N(a) → N2(g) has been found at around 500 K in a steady-state NO + D2 reaction over stepped Pd(211) = (S)3(111) × (100)] by means of angle-resolved desorption. The desorbing N2 is highly collimated at around 30° off normal toward the step-down direction below about 500 K due to the intermediate N2O decomposition, whereas, above 500 K, the near normally directed desorption due to the recombination of N(a) is relatively enhanced. The N2O decomposition channel is promoted when the reaction is carried out with hydrogen (deuterium) and the channel change is accelerated by quick changes of the amounts of surface hydrogen and oxygen (or NO(a)) into the opposite directions, and enhanced nitrogen removal as ammonia on the resultant hydrogen-rich surface. In the steady-state NO + CO reaction, the N2 emission channel gradually changes above 500 K toward recombination. A model for the off-normal N2 emission is briefly described. |
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