Balancing the NH₃ selective catalytic reduction (NH₃-SCR) and catalytic oxidation performance is difficult but necessary for the synergistic elimination of NO_x and chlorine-containing volatile organic compounds (CVOCs). We herein unveiled that electronic structure tailoring of the applied catalyst was an efficient pathway for balancing the catalytic behaviors in the NH₃-SCR of NO and chlorobenzene catalytic oxidation (CBCO). Specifically, environmentally friendly CeO₂ substituted by low valent Al³⁺ exhibited better NH₃-SCR of NO and CBCO activity in comparison with the CeO₂ sample without doping. Detailed characterizations and theoretical simulations revealed that the strong dopant-oxide pairs in the CeO₂ with Al³⁺ doping significantly tailored the electronic structure of O 2p states, enhancing the amount of Lewis acid sites and promoting the ability of lattice oxygen to act as an oxidizing agent, thereby leading to superior performance for the synergistic elimination of NO/CB. The counterpart with substitution of high valent Ta⁵⁺ showed an opposite trend, due to that Ta⁵⁺ donated more electrons to the coordination oxygen than Ce⁴⁺ inhibiting lattice oxygen separating from the surface of the catalyst, and Lewis base sites were formed.

平衡 NH ₃选择性催化还原 (NH ₃ -SCR) 和催化氧化性能是困难的，但对于协同消除 NO _x和含氯挥发性有机化合物 (CVOC) 是必要的。我们在此揭示了所应用催化剂的电子结构定制是平衡NO 和氯苯催化氧化 (CBCO)的 NH ₃ -SCR 中的催化行为的有效途径。具体而言，环境友好的CeO ₂由低化合价的Al取代³⁺显示出更好的NH ₃ NO和CBCO活性-SCR与比较的CeO ₂没有掺杂的样品。详细的表征和理论模拟表明，掺杂了 Al ³⁺的 CeO ₂中的强掺杂剂-氧化物对显着调整了 O 2p 态的电子结构，增加了路易斯酸位点的数量并促进了晶格氧作为氧化剂，从而导致协同消除 NO/CB 的优异性能。取代高价Ta ⁵⁺的对应物表现出相反的趋势，因为Ta ⁵⁺比Ce ⁴⁺向配位氧提供了更多的电子，抑制了晶格氧从催化剂表面分离，并形成了路易斯碱位。