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Selective catalytic oxidation of ammonia over LaMAl11O19−δ (M = Fe, Cu, Co, and Mn) hexaaluminates catalysts at high temperatures in the Claus process
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2020/01/15 , DOI: 10.1039/c9cy02512j Guoxia Jiang 1, 2, 3, 4, 5 , Fenglian Zhang 4, 5, 6, 7, 8 , Zheng Wei 4, 5, 6, 7, 8 , Zhuo Wang 9, 10, 11 , Yu Sun 1, 2, 3, 4, 5 , Yumeng Zhang 1, 2, 3, 4, 5 , Caihong Lin 4, 12, 13, 14 , Xin Zhang 4, 5, 6, 7, 8 , Zhengping Hao 1, 2, 3, 4, 5
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2020/01/15 , DOI: 10.1039/c9cy02512j Guoxia Jiang 1, 2, 3, 4, 5 , Fenglian Zhang 4, 5, 6, 7, 8 , Zheng Wei 4, 5, 6, 7, 8 , Zhuo Wang 9, 10, 11 , Yu Sun 1, 2, 3, 4, 5 , Yumeng Zhang 1, 2, 3, 4, 5 , Caihong Lin 4, 12, 13, 14 , Xin Zhang 4, 5, 6, 7, 8 , Zhengping Hao 1, 2, 3, 4, 5
Affiliation
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A method for the selective catalytic oxidation of ammonia at high temperature was innovatively proposed to substitute the traditional combustion method to remove the ammonia impurity in the Claus process. In the present work, transition metal (Fe, Cu Co, and Mn)-substituted La-hexaaluminate catalysts were synthesized and investigated for the selective catalytic oxidation of ammonia (NH3-SCO) at high temperature. It was observed that Cu-substituted catalysts could achieve the highest N2 yield at around 520 °C. It was confirmed that the conversion of NH3 was closely related to the reducibility of the prepared catalyst. In particular, it was observed that the molecular O2 could not be dissociatively adsorbed on the prepared catalyst surface. However, both lattice oxygen and gas-phase O2 could participate in NH3-SCO, with gas-phase O2 being the most favorable under the experimental conditions. It was evidenced that the NH3-SCO reaction over the prepared catalysts followed the i-SCR mechanism. Moreover, monodentate nitrates were the main reactive intermediates toward forming N2. Therefore, the development of high-temperature SCO technology and an efficient catalyst are beneficial for the sustainable development of the chemical industry.
中文翻译：
在克劳斯工艺中，在LaMAl11O19-δ（M = Fe，Cu，Co和Mn）六铝酸盐催化剂上对氨进行选择性催化氧化
创新地提出了一种在高温下选择性催化氧化氨的方法，以代替传统的燃烧方法在克劳斯工艺中去除氨中的杂质。在本工作中，合成了过渡金属（Fe，Cu Co和Mn）取代的La-六铝酸盐催化剂，并研究了其在高温下对氨（NH 3 -SCO）的选择性催化氧化的作用。观察到，在约520℃下，Cu-取代的催化剂可以达到最高的N 2产率。证实了NH 3的转化与所制备的催化剂的还原性密切相关。特别地，观察到分子O 2不能解离地吸附在制备的催化剂表面上。然而，晶格氧和气相O 2均可参与NH 3 -SCO，在实验条件下气相O 2是最有利的。证明了在制备的催化剂上的NH 3 -SCO反应遵循i-SCR机理。而且，单齿硝酸盐是形成N 2的主要反应中间体。因此，高温SCO技术和高效催化剂的发展有利于化学工业的可持续发展。
更新日期：2020-03-09
中文翻译：
在克劳斯工艺中，在LaMAl11O19-δ（M = Fe，Cu，Co和Mn）六铝酸盐催化剂上对氨进行选择性催化氧化
创新地提出了一种在高温下选择性催化氧化氨的方法，以代替传统的燃烧方法在克劳斯工艺中去除氨中的杂质。在本工作中，合成了过渡金属（Fe，Cu Co和Mn）取代的La-六铝酸盐催化剂，并研究了其在高温下对氨（NH 3 -SCO）的选择性催化氧化的作用。观察到，在约520℃下，Cu-取代的催化剂可以达到最高的N 2产率。证实了NH 3的转化与所制备的催化剂的还原性密切相关。特别地，观察到分子O 2不能解离地吸附在制备的催化剂表面上。然而，晶格氧和气相O 2均可参与NH 3 -SCO，在实验条件下气相O 2是最有利的。证明了在制备的催化剂上的NH 3 -SCO反应遵循i-SCR机理。而且，单齿硝酸盐是形成N 2的主要反应中间体。因此，高温SCO技术和高效催化剂的发展有利于化学工业的可持续发展。
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