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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Ce_(0.95)Cr_(0.05)O_2 and Ce_(0.97)Cu_(0.03)O_2: active, selective and stable catalysts for selective hydrogen combustion
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Ce_(0.95)Cr_(0.05)O_2 and Ce_(0.97)Cu_(0.03)O_2: active, selective and stable catalysts for selective hydrogen combustion

机译：Ce_（0.95）Cr_（0.05）O_2和Ce_（0.97）Cu_（0.03）O_2：选择性氢燃烧的活性，选择性和稳定催化剂

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摘要

Ceria-based materials are promising solid "oxygen reservoirs" for propane oxidative dehydrogenation. The ceria lattice oxygen can selectively combust hydrogen from the dehydrogenation mixture at 550 °C. This shifts the dehydrogenation equilibrium to the desired products side, generates heat aiding the endothermic dehydrogenation, and simplifies product separation. The process is also safer, since it avoids mixing O_2, and H_2 at high temperatures. While ceria itself is unselective, its catalytic properties can be tuned by doping. We study the effects of dopant type, concentration and the crystallite size on the catalytic properties. Doping with Cr or Cu increases both the selectivity and activity of the ceria, albeit that propane combustion also increases linearly with the Cu-concentration. The Cu-doped catalysts give selectivities up to 95% and combust up to 8% of the hydrogen feed. The best results are obtained with Cr-doped ceria, with selectivities up to 98%, and combustion of up to 15% of the hydrogen feed. The Cr-doped catalysts are stable in the reductive gas feed, and no extra coke is formed when the catalyst is subjected to an extra 10 min in the dehydrogenation mixture, after the hydrogen combustion reaction has stopped. This robustness is essential for industrial dehydrogenation applications.
机译：基于二氧化铈的材料是用于丙烷氧化脱氢的有希望的固体“储氧器”。所述二氧化铈晶格氧可以在550℃下选择性地燃烧来自所述脱氢混合物的氢。这将脱氢平衡转移到所需的产物侧，产生有助于吸热脱氢的热量，并简化了产物分离。该方法也更安全，因为它避免了在高温下混合O_2和H_2。尽管二氧化铈本身是非选择性的，但是其催化性能可以通过掺杂来调节。我们研究了掺杂剂类型，浓度和微晶尺寸对催化性能的影响。 Cr或Cu掺杂既可以提高二氧化铈的选择性，又可以提高二氧化铈的活性，尽管丙烷燃烧也随Cu浓度线性增加。掺杂铜的催化剂的选择性高达95％，燃烧的氢气进料高达8％。用Cr掺杂的二氧化铈可获得最佳结果，选择性高达98％，燃烧的氢气进料高达15％。 Cr掺杂的催化剂在还原性气体进料中是稳定的，并且在氢气燃烧反应停止后，如果催化剂在脱氢混合物中经过额外的10分钟，则不会形成多余的焦炭。这种坚固性对于工业脱氢应用至关重要。

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