Ammonia Decomposition over CaNH-Supported Ni Catalysts via an NH2–-Vacancy-Mediated Mars–van Krevelen Mechanism

催化作用 分解 脱氢 空位缺陷 化学 密度泛函理论 无机化学 材料科学 计算化学 结晶学 有机化学
作者
Kiya Ogasawara,Takuya Nakao,Kazuhisa Kishida,Tian‐Nan Ye,Yangfan Lu,Hitoshi Abe,Y. Niwa,Masato Sasase,Masaaki Kitano,Hideo Hosono
出处
期刊:ACS Catalysis [American Chemical Society]
卷期号:11 (17): 11005-11015 被引量:71
标识
DOI:10.1021/acscatal.1c01934
摘要

Nickel has been studied as an alternative catalyst to ruthenium for ammonia decomposition. However, high reaction temperatures are generally required to achieve good ammonia conversion because the weak interactions between nitrogen and the Ni surface reduce the frequency of the dehydrogenation reaction of ammonia. Here, we report Ni-supported CaNH as a highly efficient catalyst for ammonia decomposition through an NH2– vacancy-mediated Mars–van Krevelen mechanism. Ni/CaNH exhibited much greater ammonia decomposition activity than state-of-the-art Ni-based catalysts, and the operating temperature was 100 °C lower than those of the other Ni-based catalysts. Isotope-labeling experiments, NH3-pulse measurements, and density functional theory calculations suggested that two anionic electrons at the NH2– vacancy on the Ni/CaNH surface activated ammonia molecules to form intermediate NHx (x = 1, 2) species, even at 50 °C, and the supported Ni metal promoted the regeneration of NH2– vacancies on CaNH. These results demonstrate that NH2– vacancy sites on CaNH play an important role in overcoming the drawbacks of Ni-based catalysts in ammonia decomposition.
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