Beijing Key Laboratory for Green Catalysis and Separation, Key Laboratory of Beijing on Regional Air Pollution Control, Key Laboratory of Advanced Functional Materials, Education Ministry of China, College of Materials Science and Engineering, Beijing University of Technology, Beijing 100124, China.
School of Environmental Science and Engineering, Hebei University of Science and Technology, Shijiazhuang,Hebei 050018, China.
Environ Sci Technol. 2024 Oct 1;58(39):17475-17484. doi: 10.1021/acs.est.4c03049. Epub 2024 Sep 16.
Synergistic catalytic removal of multipollutants (e.g., volatile organic compound (VOC) oxidation and nitrogen oxide (NO) reduction) is highly demanded due to the increasingly strict emission standards. The prevention of the key reactive intermediate species nitrite excessive oxidation over the supported noble-metal catalysts, rather than the traditional low-efficiency transition metal oxide catalysts, remains a great challenge. Herein, a sound strategy of Pd single atoms saturated with acidic transition element ligands is proposed. The coexistence of Pd and V dual single atoms strengthens the adsorption of reactants, while synergistic interaction between dual atoms and surface oxygen weakens activation of lattice oxygen, thus significantly reducing the overoxidation of nitrite. Meanwhile, the neutralization of the active Pd and inert V sites results in a rational decrease in the redox property of Pd and an obvious increase in that of V. The PdV/CeO dual single-atom catalyst achieves 90% conversion of NO and toluene at 238 and 230 °C and has a large temperature window (>150 °C) for NO reduction. This research makes a breakthrough in the development of efficient supported noble-/transition-metal dual single-atom catalysts for VOC and NO simultaneous purification.
由于日益严格的排放标准，需要协同催化去除多种污染物（例如，挥发性有机化合物（VOC）氧化和氮氧化物（NO）还原）。在负载型贵金属催化剂上防止关键反应中间体亚硝酸盐过度氧化，而不是传统的低效过渡金属氧化物催化剂，仍然是一个巨大的挑战。在此，提出了一种负载型贵金属催化剂的酸性过渡元素配体饱和 Pd 单原子的合理策略。Pd 和 V 双单原子的共存增强了反应物的吸附，而双原子之间的协同相互作用与表面氧减弱了晶格氧的活化，从而显著减少了亚硝酸盐的过度氧化。同时，活性 Pd 和惰性 V 位的中和导致 Pd 的氧化还原性能合理降低，V 的氧化还原性能明显增加。PdV/CeO 双单原子催化剂在 238 和 230°C 下实现了 90%的 NO 和甲苯转化率，并且具有较大的 NO 还原温度窗口（>150°C）。这项研究在开发用于 VOC 和 NO 同时净化的高效负载型贵金属/过渡金属双单原子催化剂方面取得了突破。
