Synergistic catalytic removal of multipollutants (e.g., volatile organic compound (VOC) oxidation and nitrogen oxide (NO_x) 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 Pd₁V₁/CeO₂ dual single-atom catalyst achieves 90% conversion of NO_x and toluene at 238 and 230 °C and has a large temperature window (>150 °C) for NO_x reduction. This research makes a breakthrough in the development of efficient supported noble-/transition-metal dual single-atom catalysts for VOC and NO_x simultaneous purification.

中文翻译：

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通过双单原子调节晶格氧迁移率，同时增强 VOC 氧化和 NOx 还原


由于排放标准日益严格，对多污染物（例如挥发性有机化合物 （VOC） 氧化和氮氧化物 （NO_x） 还原）的协同催化去除要求很高。防止关键反应性中间物种亚硝酸盐在负载型贵金属催化剂上过度氧化，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，提出了一种用酸性过渡元素配体饱和的 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，而双原子与表面氧之间的协同作用削弱了晶格氧的活化，从而显着降低了亚硝酸盐的过氧化。同时，活性 Pd 和惰性 V 位点的中和导致 Pd 的氧化还原性能合理降低，V 的氧化还原性能明显增加。Pd₁V₁/CeO₂ 双单原子催化剂在 238 °C 和 230 °C 下可实现 90% 的 NO_x 和甲苯转化率，并具有用于 NO_x 还原的大温度窗口 （>150 °C）。本研究在开发用于 VOC 和 NO_x 同时净化的高效负载贵金属/过渡金属双单原子催化剂方面取得了突破。