Experimental and Theoretical Investigation of Molybdenum Carbide and Nitride as Catalysts for Ammonia Decomposition

IMR OpenIR

	Experimental and Theoretical Investigation of Molybdenum Carbide and Nitride as Catalysts for Ammonia Decomposition
	W. Q. Zheng; T. P. Cotter; P. Kaghazchi; T. Jacob; B. Frank; K. Schlichte; W. Zhang; D. S. Su; F. Schuth; R. Schlogl
	2013
发表期刊	Journal of the American Chemical Society
ISSN	0002-7863
卷号	135 期号:9 页码:3458-3464
摘要	Constant COx-free H-2 production from the catalytic decomposition of ammonia could be achieved over a high-surface-area molybdenum carbide catalyst prepared by a temperature-programmed reduction carburization method. The fresh and used catalyst was characterized by N-2 adsorption/desorption, powder X-ray diffraction, scanning and transmission electron microscopy, and electron energy-loss spectroscopy at different stages. Observed deactivation (in the first 15 h) of the high-surface-area carbide during the reaction was ascribed to considerable reduction of the specific surface area due to nitridation of the carbide under the reaction conditions. Theoretical calculations confirm that the N atoms tend to occupy subsurface sites, leading to the formation of nitride under an NH3 atmosphere. The relatively high rate of reaction (30 mmol/((g of cat.) min)) observed for the catalytic decomposition of NH3 is ascribed to highly energetic sites (twin boundaries, stacking faults, steps, and defects) which are observed in both the molybdenum carbide and nitride samples. The prevalence of such sites in the as-synthesized material results in a much higher H-2 production rate in comparison with that for previously reported Mo-based catalysts.
部门归属	[zheng, weiqing ; cotter, thomas p. ; frank, benjamin ; zhang, wei ; su, dang sheng ; schloegl, robert] max planck gesell, fritz haber inst, dept inorgan chem, d-14195 berlin, germany. [kaghazchi, payam ; jacob, timo] univ ulm, inst elektrochem, d-89069 ulm, germany. [schlichte, klaus ; schueth, ferdi] max planck inst coal res, dept heterogeneous catalysis, d-45470 mulheim, germany. [su, dang sheng] chinese acad sci, inst met res, shenyang natl lab mat sci, shenyang 110016, peoples r china. ; su, ds (reprint author), chinese acad sci, inst met res, shenyang natl lab mat sci, 72 wenhua rd, shenyang 110016, peoples r china. ; dangsheng@fhi-berlin.mpg.de
关键词	Transition-metal Carbides Tungsten Carbide Isomerization Conversion
URL	查看原文
语种	英语
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/71731
专题	中国科学院金属研究所
推荐引用方式 GB/T 7714	W. Q. Zheng,T. P. Cotter,P. Kaghazchi,et al. Experimental and Theoretical Investigation of Molybdenum Carbide and Nitride as Catalysts for Ammonia Decomposition[J]. Journal of the American Chemical Society,2013,135(9):3458-3464.
APA	W. Q. Zheng.,T. P. Cotter.,P. Kaghazchi.,T. Jacob.,B. Frank.,...&R. Schlogl.(2013).Experimental and Theoretical Investigation of Molybdenum Carbide and Nitride as Catalysts for Ammonia Decomposition.Journal of the American Chemical Society,135(9),3458-3464.
MLA	W. Q. Zheng,et al."Experimental and Theoretical Investigation of Molybdenum Carbide and Nitride as Catalysts for Ammonia Decomposition".Journal of the American Chemical Society 135.9(2013):3458-3464.