Effect of Pore Confinement of NaNH2 and KNH2 on Hydrogen Generation from Ammonia

被引:37
作者
Chang, Fei [1 ]
Wu, Han [2 ]
van der Pluijm, Robby [1 ]
Guo, Jianping [2 ]
Ngene, Peter [1 ]
de Jongh, Petra E. [1 ]
机构
[1] Univ Utrecht, Debye Inst Nanomat Sci, Inorgan Chem & Catalysis, Univ Weg 99, NL-3584 CG Utrecht, Netherlands
[2] Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
基金
中国国家自然科学基金; 欧洲研究理事会;
关键词
COX-FREE HYDROGEN; DECOMPOSITION CATALYSTS; CARBON NANOTUBES; NANOPARTICLES; STORAGE; NH3; POTASSIUM; HYDRIDES; NITRIDE; CARBIDE;
D O I
10.1021/acs.jpcc.9b03878
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The development of efficient catalysts for hydrogen generation via ammonia decomposition is crucial for the use of ammonia as an energy carrier. Here, we report the effect of pore confinement of NaNH2 and KNH2 on ammonia decomposition catalysis. For the first time, Ni- or Ru-doped NaNH2 and KNH(2 )were confined in carbon nanopores using a combination method of solution impregnation and melt infiltration. Structure characterization indicates the nanoscale intimacy between transition metals and alkali metal amides inside the pores of the carbon support. As a result, 8 wt % Ni-doped NaNH2 and KNH2 nanocomposites give NH3 conversions of 79 and 60%, respectively at 425 degrees C, close to the performance of a 5 wt % Ru/C reference catalyst. 0.8 wt % Rudoped nanocomposites exhibit even better catalytic performance, with about 95% NH3 conversion at a moderate temperature of 375 degrees C. The hydrogen production rates of these Ni- and Ru-doped nanocomposites in a pure NH3 flow are about 3-4 times higher than for the recently reported novel catalysts such as Ni-Li2NH and Ru-Li2NH/MgO. Interestingly, the apparent activation energies of the Ru- or Ni-based catalysts decrease 20-30 kJ mol(-1) alkali metal amides. The strategy of nanoconfinement of alkali metal amides in porous hosts may effectively generating H-2 from NH3 at low temperatures.
引用
收藏
页码:21487 / 21496
页数:10
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