Khivantsev Konstantin, Jaegers Nicholas R, Kovarik Libor, Hanson Jonathan C, Tao Franklin Feng, Tang Yu, Zhang Xiaoyan, Koleva Iskra Z, Aleksandrov Hristiyan A, Vayssilov Georgi N, Wang Yong, Gao Feng, Szanyi János
Institute for Integrated Catalysis, Pacific Northwest National Laboratory, Richland, WA, 99352, USA.
Voiland School of Chemical Engineering and Bioengineering, Washington State University, Pullman, WA, 99163, USA.
Angew Chem Int Ed Engl. 2018 Dec 17;57(51):16672-16677. doi: 10.1002/anie.201809343. Epub 2018 Nov 12.
The majority of harmful atmospheric CO and NO emissions are from vehicle exhausts. Although there has been success addressing NO emissions at temperatures above 250 °C with selective catalytic reduction technology, emissions during vehicle cold start (when the temperature is below 150 °C), are a major challenge. Herein, we show we can completely eliminate both CO and NO emissions simultaneously under realistic exhaust flow, using a highly loaded (2 wt %) atomically dispersed palladium in the extra-framework positions of the small-pore chabazite material as a CO and passive NO adsorber. Until now, atomically dispersed highly loaded (>0.3 wt %) transition-metal/SSZ-13 materials have not been known. We devised a general, simple, and scalable route to prepare such materials for Pt and Pd . Through spectroscopy and materials testing we show that both CO and NO can be simultaneously completely abated with 100 % efficiency by the formation of mixed carbonyl-nitrosyl palladium complex in chabazite micropore.
大气中大部分有害的一氧化碳和氮氧化物排放来自汽车尾气。尽管利用选择性催化还原技术在温度高于250°C时处理氮氧化物排放已取得成功，但车辆冷启动期间（温度低于150°C）的排放仍是一项重大挑战。在此，我们展示了，通过使用在小孔菱沸石材料的骨架外位置高度负载（2 wt%）的原子分散钯作为一氧化碳和被动氮氧化物吸附剂，我们能够在实际排气流量下同时完全消除一氧化碳和氮氧化物排放。到目前为止，尚未知晓原子分散的高负载（>0.3 wt%）过渡金属/SSZ-13材料。我们设计了一种通用、简单且可扩展的路线来制备用于铂和钯的此类材料。通过光谱学和材料测试，我们表明，通过在菱沸石微孔中形成混合羰基 - 亚硝酰钯配合物，一氧化碳和氮氧化物均可同时以100%的效率完全消除。
