Key Laboratory for Advanced Materials, Research Institute of Industrial Catalysis, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai 200237, P. R. China.
Erdos Electric Power and Metallurgy Group Co. Ltd., Ordos 016064, Inner Mongolia, P. R. China.
Environ Sci Technol. 2022 Jun 21;56(12):8854-8863. doi: 10.1021/acs.est.2c00942. Epub 2022 May 10.
Understanding the formation and inhibition of more toxic polychlorinated byproducts from the catalytic oxidation elimination of chlorinated volatile organic compounds (Cl-VOCs) and unveiling efficient strategies have been essential and challenging. Here, RuO supported on CePO-doped CeO nanosheets (Ru/Pi-CeO) is designed for boosting catalytic oxidation for the removal of dichloromethane (DCM) as a representative Cl-VOC. The promoted acid strength/number and sintering resistance due to the doping of electron-rich and thermally stable CePO are observed along with the undescended redox ability and the exposed multi-active sites, which demonstrates a high activity and durability of DCM oxidation (4000 mg/m and 15,000 mL/g·h, stable complete-oxidation at 300 °C), exceptional versatility for different Cl-VOCs, alkanes, aromatics, N-containing VOCs, CO and their multicomponent VOCs, and enhanced thermal stability. The suppression of polychlorinated byproducts is determined over Ru/Pi-CeO and oxy-anionic S, V, Mo, Nb, or W doping CeO, thus the oxy-anionic doping strategy is proposed based on the quenching of the electron-rich oxy-anions on chlorine radicals. Moreover, the simple mechanical mixing with these oxy-anionic salts is also workable even for other catalysts such as Co, Sn, Mn, and noble metal-based catalysts. This work offers further insights into the inhibition of polychlorinated byproducts and contributes to the convenient manufacture of monolithic catalysts with superior chlorine-poisoning resistance for the catalytic oxidation of Cl-VOCs.
理解氯化挥发性有机化合物 (Cl-VOC) 催化氧化消除过程中更具毒性的多氯副产物的形成和抑制，并揭示有效的策略一直是至关重要且具有挑战性的。在这里，设计了负载在 CePO 掺杂的 CeO 纳米片上的 RuO（Ru/Pi-CeO）来促进二氯甲烷 (DCM) 作为代表性 Cl-VOC 的催化氧化去除。观察到由于富电子和热稳定的 CePO 的掺杂而促进的酸强度/数量和抗烧结性，以及未下降的氧化还原能力和暴露的多活性位，这证明了 DCM 氧化（4000mg/m 和 15000mL/g·h，在 300°C 下稳定完全氧化）具有高活性和耐久性，对不同的 Cl-VOC、烷烃、芳烃、含 N 的 VOC、CO 和它们的多组分 VOC 具有出色的多功能性，以及增强的热稳定性。在 Ru/Pi-CeO 和氧阴离子 S、V、Mo、Nb 或 W 掺杂的 CeO 上确定了多氯副产物的抑制作用，因此提出了氧阴离子掺杂策略，基于富电子氧阴离子对氯自由基的猝灭。此外，即使对于其他催化剂（如 Co、Sn、Mn 和贵金属基催化剂），这些氧阴离子盐的简单机械混合也是可行的。这项工作为多氯副产物的抑制提供了进一步的见解，并为具有优异抗氯中毒性能的 Cl-VOC 催化氧化用整体式催化剂的方便制造做出了贡献。
