In Situ Electrochemical Promotion by Sodium of the Platinum-Catalyzed Reduction of NO by Propene

In Situ Electrochemical Promotion by Sodium of the Platinum-Catalyzed Reduction of NO by Propene
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钠对铂催化丙烯还原 NO 的原位电化学促进

DOI:
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发表时间:
1997
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通讯作者:
R. M. Lambert
R. M. Lambert
中科院分区:
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文献类型:
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作者:
I. Yentekakis;A. Palermo;Neil C. Filkin;A. S. Tikhov;R. M. Lambert

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丙烯在pt催化下对NO的还原表现出β " -氧化铝固体电解质提供的外溢Na的强烈电化学促进作用。在推广的制度下,利率提高一个数量级是可以实现的。在足够高的Na负荷下,系统表现出中毒,并且在促进和中毒状态之间的偏移是完全可逆的。作为催化剂电位、温度和气体组成函数的反应动力学数据表明,相对于丙烯,Na增加了NO的化学吸附强度。这伴随着N - O键的减弱,从而促进NO解离,这被认为是引发反应的关键步骤。N2/N2O选择性对催化剂电位的依赖性与这一观点一致:向Pt催化剂泵送Na有利于生成N2,而牺牲N2O。x射线光电子能谱(XPS)数据证实,Pt薄膜的电化学促进确实涉及到Na向…
The Pt-catalyzed reduction of NO by propene exhibits strong electrochemical promotion by spillover Na supplied from a β‘‘-alumina solid electrolyte. In the promoted regime, rate increases by an order of magnitude are achievable. At sufficiently high loadings of Na the system exhibits poisoning, and excursions between the promoted and poisoned regimes are fully reversible. Reaction kinetic data obtained as a function of catalyst potential, temperature, and gas composition indicate that Na increases the strength of NO chemisorption relative to propene. This is accompanied by weakening of the N−O bond, thus facilitating NO dissociation, which is proposed as the critical reaction-initiating step. The dependence of N2/N2O selectivity on catalyst potential is in accord with this view:  Na pumping to the Pt catalyst favors N2 production at the expense of N2O. X-ray photoelectron spectroscopic (XPS) data confirm that electrochemical promotion of the Pt film does indeed involve reversible pumping of Na to or from ...