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Ce–Si Mixed Oxide: A High Sulfur Resistant Catalyst in the NH3–SCR Reaction through the Mechanism-Enhanced Process
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2021-03-03 , DOI: 10.1021/acs.est.0c08410 Wei Tan 1 , Annai Liu , Shaohua Xie 1 , Yong Yan 2 , Thomas E. Shaw 3 , Yu Pu , Kai Guo , Lulu Li 4 , Shuohan Yu , Fei Gao , Fudong Liu 1 , Lin Dong
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2021-03-03 , DOI: 10.1021/acs.est.0c08410 Wei Tan 1 , Annai Liu , Shaohua Xie 1 , Yong Yan 2 , Thomas E. Shaw 3 , Yu Pu , Kai Guo , Lulu Li 4 , Shuohan Yu , Fei Gao , Fudong Liu 1 , Lin Dong
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Investigating catalytic reaction mechanisms could help guide the design of catalysts. Here, aimed at improving both the catalytic performance and SO2 resistance ability of catalysts in the selective reduction of NO by NH3 (NH3–SCR), an innovative CeO2–SiO2 mixed oxide catalyst (CeSi2) was developed based on our understanding of both the sulfur poisoning and reaction mechanisms, which exhibited excellent SO2/H2O resistance ability even in the harsh working conditions (containing 500 ppm of SO2 and 5% H2O). The strong interaction between Ce and Si (Ce–O–Si) and the abundant surface hydroxyl groups on CeSi2 not only provided fruitful surface acid sites but also significantly inhibited SO2 adsorption. The NH3–SCR performance of CeSi2 was promoted by an enhanced Eley–Rideal (E–R) mechanism in which more active acid sites were preserved under the reaction conditions and gaseous NO could directly react with adsorbed NH3. This mechanism-enhanced process was even further promoted on sulfated CeSi2. This work provides a reaction mechanism-enhanced strategy to develop an environmentally friendly NH3–SCR catalyst with superior SO2 resistance.
中文翻译：
Ce-Si混合氧化物：通过机理增强过程在NH 3 -SCR反应中的高抗硫催化剂
研究催化反应机理可以帮助指导催化剂的设计。在此，为了同时提高通过NH 3（NH 3 -SCR）选择性还原NO的催化剂的催化性能和抗SO 2的能力，在我们的基础上开发了创新的CeO 2 -SiO 2混合氧化物催化剂（CeSi2）了解硫中毒和反应机理，即使在苛刻的工作条件下（包含500 ppm的SO 2和5％的H 2）也表现出出色的SO 2 / H 2 O抵抗能力O）。Ce和Si（Ce–O–Si）之间的强相互作用以及CeSi2上大量的表面羟基基团不仅提供了丰富的表面酸位，而且显着抑制了SO 2的吸附。CeSi2的NH 3 -SCR性能通过增强的Eley-Rideal（E-R）机理得到了提高，该机理在反应条件下保留了更多的活性酸位，并且气态NO可以直接与吸附的NH 3反应。硫酸化的CeSi2甚至进一步促进了这种机理增强的过程。这项工作提供了一种增强反应机理的策略，以开发一种具有出色的SO 2耐受性的环保NH 3 -SCR催化剂。
更新日期：2021-03-16
中文翻译：
Ce-Si混合氧化物：通过机理增强过程在NH 3 -SCR反应中的高抗硫催化剂
研究催化反应机理可以帮助指导催化剂的设计。在此，为了同时提高通过NH 3（NH 3 -SCR）选择性还原NO的催化剂的催化性能和抗SO 2的能力，在我们的基础上开发了创新的CeO 2 -SiO 2混合氧化物催化剂（CeSi2）了解硫中毒和反应机理，即使在苛刻的工作条件下（包含500 ppm的SO 2和5％的H 2）也表现出出色的SO 2 / H 2 O抵抗能力O）。Ce和Si（Ce–O–Si）之间的强相互作用以及CeSi2上大量的表面羟基基团不仅提供了丰富的表面酸位，而且显着抑制了SO 2的吸附。CeSi2的NH 3 -SCR性能通过增强的Eley-Rideal（E-R）机理得到了提高，该机理在反应条件下保留了更多的活性酸位，并且气态NO可以直接与吸附的NH 3反应。硫酸化的CeSi2甚至进一步促进了这种机理增强的过程。这项工作提供了一种增强反应机理的策略，以开发一种具有出色的SO 2耐受性的环保NH 3 -SCR催化剂。
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