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COx-free hydrogen production via ammonia decomposition over molybdenum nitride-based catalysts

机译：通过氨COx-free制氢在钼氮分解催化剂

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摘要

COx-free hydrogen generation via ammonia decomposition has received much attention as an important process for fuel cell applications. In the present study, non-precious Mo nitride-based catalysts with Co, Ni, and Fe additives were synthesized by temperature-programmed reaction of the corresponding oxide precursors with NH3. N-2 adsorption, X-ray diffraction (XRD), NH3-temperature programmed surface reaction (NH3-TPSR), NH3 pulse reaction, transmission electron microscopy (TEM), and scanning electron microscopy (SEM) were carried out to gain better insight into the chemical and textural properties of the catalysts. The XRD analysis confirmed the formation of the Mo2N, Co3Mo3N, Ni3Mo3N, and Fe3Mo3N phases, which act as active species for ammonia decomposition reaction. The Co3Mo3N, Ni3Mo3N, and Fe3Mo3N catalysts were more active for ammonia decomposition than the Mo2N catalysts, indicating that the Co, Ni, and Fe species promoted the reaction. The increase in particle size and the decrease in surface area by the Co, Ni, and Fe addition did not negatively affect the ammonia decomposition activity. Interestingly, the Co, Ni, and Fe addition facilitated the recombinative desorption of N atoms from the active components, resulting in the enhancement in the activity. In addition, kinetic analysis was also conducted in detail to investigate the effects of the NH3 and H-2 partial pressures. The Co, Ni, and Fe addition alleviated the negative effect of the H-2 poisoning on the active sites.
机译：通过氨COx-free氢生成分解为已获得了高度的关注燃料电池应用的重要过程。目前的研究中,non-precious莫氮催化剂对Co、镍和铁添加剂通过程序升温反应合成相应的氧化物与NH3前兆。吸附、x射线衍射(XRD),NH3-temperature编程表面反应(NH3-TPSR)、NH3脉冲反应,传播电子显微镜(TEM)、扫描电子显微镜(SEM)进行了获得更好了解化学和结构属性的催化剂。形成的Mo2N Co3Mo3N Ni3Mo3N,Fe3Mo3N阶段,作为活跃的物种氨分解反应。Ni3Mo3N, Fe3Mo3N催化剂更活跃比Mo2N对氨分解催化剂,表明有限公司镍和铁促进了物种的反应。粒子大小和面积的减少Co、Ni和菲没有负面影响影响氨分解活性。有趣的是,公司、镍和铁促进了recombinative解吸的N原子的活性成分,导致增强的活动。动能也进行了详细分析调查的影响NH3和2部分压力。缓解2的负面影响中毒在活动网站。

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