College of Chemistry, Sichuan University, Chengdu, 610064, China.
Institute of New Energy and Low-Carbon Technology, Sichuan University, Chengdu, 610064, Sichuan, China.
Environ Sci Pollut Res Int. 2019 Sep;26(25):26071-26081. doi: 10.1007/s11356-019-05834-3. Epub 2019 Jul 5.
Pd-only three-way catalysts with improved catalytic activity for NO elimination were prepared. In order to explore the catalytic reaction rules of NO reduction under a three-way catalytic system, a series of single reactions related to NO reduction were evaluated. It was found that the reaction temperatures of NO + H or NO + CO or NO + CH reactions were below 250 °C, while that of NO + CH was up to 350 °C. Thus, the reaction NO + CH served as the key reaction in determining the purification efficiency of NO at the high-temperature stage. By in situ FTIR, we proposed that three possible steps were involved in NO + CH reaction. The first step was the oxidation of CH and NO to acetone and nitrate species by active oxygen species, respectively (CH + O* → CHO, NO + O* → NO). XPS results revealed that the amount of active oxygen species in Pd/CeO-ZrO-AlO (Pd/CZA, 73.7%) was much higher than that in Pd/CeZrO+AlO (Pd/CZ+A, 64.1%). This was in line with the higher reaction efficiency of the first step over Pd/CZA. Then the NO + CH reaction was accelerated by the first step, which consequently contributed to the higher NO elimination efficiency of Pd/CZA.
研究了具有改善的 NO 消除催化活性的 Pd 单原子催化剂。为了探索三效催化体系下 NO 还原的催化反应规律,评估了一系列与 NO 还原相关的单反应。发现 NO+H 或 NO+CO 或 NO+CH 反应的反应温度低于 250°C,而 NO+CH 反应的反应温度高达 350°C。因此,NO+CH 反应成为决定高温阶段 NO 净化效率的关键反应。通过原位 FTIR,我们提出了 NO+CH 反应涉及三个可能的步骤。第一步是活性氧分别将 CH 和 NO 氧化为丙酮和硝酸盐物种(CH+O*→CHO,NO+O*→NO)。XPS 结果表明,Pd/CeO-ZrO-AlO(Pd/CZA,73.7%)中活性氧物种的数量远高于 Pd/CeZrO+AlO(Pd/CZ+A,64.1%)。这与 Pd/CZA 中第一步的更高反应效率一致。然后,第一步加速了 NO+CH 反应,从而导致 Pd/CZA 具有更高的 NO 消除效率。