Department of Chemical & Environmental Engineering, University of California, Riverside, California 92521, United States.
Department of Civil, Environmental, and Construction Engineering, Catalysis Cluster for Renewable Energy and Chemical Transformations (REACT), NanoScience Technology Center (NSTC), University of Central Florida, Orlando, Florida 32816, United States.
Environ Sci Technol. 2023 Mar 7;57(9):3962-3970. doi: 10.1021/acs.est.3c00415. Epub 2023 Feb 21.
Chlorate (ClO) is a common water pollutant due to its gigantic scale of production, wide applications in agriculture and industry, and formation as a toxic byproduct in various water treatment processes. This work reports on the facile preparation, mechanistic elucidation, and kinetic evaluation of a bimetallic catalyst for highly active ClO reduction into Cl. Under 1 atm H and 20 °C, Pd and Ru were sequentially adsorbed and reduced on a powdered activated carbon support, affording Ru-Pd/C from scratch within only 20 min. The Pd particles significantly accelerated the reductive immobilization of Ru as >55% dispersed Ru outside Pd. At pH 7, Ru-Pd/C shows a substantially higher activity of ClO reduction (initial turnover frequency >13.9 min on Ru; rate constant at 4050 L h g) than reported catalysts (e.g., Rh/C, Ir/C, Mo-Pd/C) and the monometallic Ru/C. In particular, Ru-Pd/C accomplished the reduction of concentrated 100 mM ClO (turnover number > 11,970), whereas Ru/C was quickly deactivated. In the bimetallic synergy, Ru rapidly reduces ClO while Pd scavenges the Ru-passivating ClO and restores Ru. This work demonstrates a simple and effective design for heterogeneous catalysts tailored for emerging water treatment needs.
氯酸盐(ClO)是一种常见的水污染物,因为其大规模的生产、广泛应用于农业和工业,以及在各种水处理过程中形成有毒副产物。本工作报道了一种用于高效还原 ClO 为 Cl 的双金属催化剂的简便制备、机理阐明和动力学评价。在 1 个大气压 H 和 20°C 下,Pd 和 Ru 依次被吸附和还原在粉末活性炭载体上,仅在 20 分钟内即可从起始物制备出 Ru-Pd/C。Pd 颗粒显著加速了 Ru 的还原固定化,使超过 55%的 Ru 分散在 Pd 之外。在 pH 7 下,Ru-Pd/C 表现出比报道的催化剂(如 Rh/C、Ir/C、Mo-Pd/C 和单金属 Ru/C)更高的 ClO 还原活性(Ru 的初始周转频率 >13.9 min;在 4050 L h g 下的速率常数)。特别是 Ru-Pd/C 能够还原浓度为 100 mM 的 ClO(周转数 >11970),而 Ru/C 很快失活。在双金属协同作用中,Ru 快速还原 ClO,而 Pd 清除 Ru 钝化的 ClO 并恢复 Ru。本工作展示了一种针对新兴水处理需求定制的高效异相催化剂的简单而有效的设计。