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题名: Highly Active MnN-Li2NH Composite Catalyst for Producing COx-Free Hydrogen
作者: Guo, Jianping1, 2;  Chang, Fei1, 2;  Wang, Peikun1, 2;  Hu, Daqiang1;  Yu, Pei1, 2;  Wu, Guotao1;  Xiong, Zhitao1;  Chen, Ping1, 3
关键词: manganese nitride ;  lithium imide ;  ternary lithium nitride ;  ammonia decomposition ;  heterogeneous catalysis
刊名: ACS CATALYSIS
发表日期: 2015-05-01
DOI: 10.1021/acscatal.5b00278
卷: 5, 期:5, 页:2708-2713
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Physical
研究领域[WOS]: Chemistry
英文摘要: We report on the significant synergistic effect of Li2NH on MnN in catalyzing NH3 decomposition to produce COx-free hydrogen. The MnNLi2NH exhibits catalytic activity below 623 K and reaches a hydrogen production rate of 37.5 mmolH(2) g(cat)(-1) min(-1) at 773 K, which is similar to 40 times the MnN and even superior to the highly active Ru-based catalysts under the same conditions. The apparent activation energy of MnN-Li2NH is similar to that of Ru/CNTs. The stability of the MnN-Li2NH composite catalyst depends on the molar ratio of MnN and Li2NH, and the catalyst with higher Mn content shows better stability. Our experimental results reveal that Li2NH reacts with MnN, giving rise to H-2 and Li7MnN4; Li7MnN4, on the other hand, can be easily ammoniated to give off N-2, which suggests that the catalysis is fulfilled via a redox cycle comprising (I) Li2NH + MnN -> Li7MnN4 + H-2 and (II) Li7MnN4 + NH3 -> MnN + Li2NH + N-2. The presence of Li2NH favors the formation of N-rich intermediate Li7MnN4, where Li+ executes a positive inductive effect to enhance the covalent Mn-N bonding and, therefore, leads to an altered reaction pathway and energetics. Our kinetic analyses indicate that the H-2 release step encounters a relatively higher barrier than the N-2 release step.
关键词[WOS]: FUEL-CELL APPLICATIONS ;  X-RAY-DIFFRACTION ;  AMMONIA DECOMPOSITION ;  1ST PRINCIPLES ;  HETEROGENEOUS CATALYSIS ;  BIMETALLIC CATALYSTS ;  CRYSTAL-STRUCTURE ;  METAL NITRIDES ;  NANOPARTICLES ;  GENERATION
语种: 英语
WOS记录号: WOS:000354012200003
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/146249
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian 116023, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
3.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China

Recommended Citation:
Guo, Jianping,Chang, Fei,Wang, Peikun,et al. Highly Active MnN-Li2NH Composite Catalyst for Producing COx-Free Hydrogen[J]. ACS CATALYSIS,2015,5(5):2708-2713.
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