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Preparation and Synergy of Supported Ru⁰ and Pd⁰ for Rapid Chlorate Reduction at pH 7.

ABSTRACT: Chlorate (ClO₃^-) 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 ClO₃^- reduction into Cl^-. Under 1 atm H₂ and 20 °C, Pd^II and Ru^III were sequentially adsorbed and reduced on a powdered activated carbon support, affording Ru⁰-Pd⁰/C from scratch within only 20 min. The Pd⁰ particles significantly accelerated the reductive immobilization of Ru^III as >55% dispersed Ru⁰ outside Pd⁰. At pH 7, Ru-Pd/C shows a substantially higher activity of ClO₃^- reduction (initial turnover frequency >13.9 min^-1 on Ru⁰; rate constant at 4050 L h^-1 g_metal^-1) 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 ClO₃^- (turnover number > 11,970), whereas Ru/C was quickly deactivated. In the bimetallic synergy, Ru⁰ rapidly reduces ClO₃^- while Pd⁰ scavenges the Ru-passivating ClO₂^- and restores Ru⁰. This work demonstrates a simple and effective design for heterogeneous catalysts tailored for emerging water treatment needs.

SUBMITTER: Gao J

PROVIDER: S-EPMC9996829 | biostudies-literature | 2023 Mar

REPOSITORIES: biostudies-literature

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Preparation and Synergy of Supported Ru0 and Pd0 for Rapid Chlorate Reduction at pH 7.

Gao Jinyu J Xie Shaohua S Liu Fudong F Liu Jinyong J

Environmental science & technology 20230221 9

Chlorate (ClO3-) 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 ClO3- reduction into Cl-. Under 1 atm H2 and 20 °C, PdII and RuIII wer ...[more]

PMID: 36808945

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Project description:Seedless, surfactantless and support-free unprotected, metallic, interconnected nano-chain networks of ruthenium nanoparticles (NPs) were successfully synthesized via the reduction of ruthenium(iii) chloride (RuCl3) with sodium borohydride (NaBH4) at three different temperatures, viz. 30 °C, 45 °C and 60 °C. The molar ratio of RuCl3 solution and borohydride was optimized to be 1 : 1.5 to produce stable colloids with the optimum final solution pH of 9.7 ± 0.2. Average diameters of the interconnected nano-chain networks prepared at 30 °C (Ru-30), 45 °C (Ru-45) and 60 °C (Ru-60) were 3.5 ± 0.5 nm, 3.0 ± 0.2 nm and 2.6 ± 0.2 nm respectively. The morphology and composition dependent catalytic and electrocatalytic activities of these unprotected Ru nano-chain networks (Ru-30, Ru-45 and Ru-60) were studied in detail. The catalysis study was performed by investigating the transfer hydrogenation of several substituted aromatic nitro compounds. It was observed that Ru-60 was relatively more active compared to Ru-30 and Ru-45, which was reflected in their rate constant values. The electrocatalytic activities of Ru-30, Ru-45 and Ru-60 were screened for anodic water splitting in alkaline medium (0.1 M NaOH) and it was found that all of them showed almost the same activity which required an over-voltage of 308 ± 2 mV to obtain an anodic current density of 10 mA cm-2. The catalytic and electrocatalytic performances of these unprotected Ru0 networks were compared with Ru0 nanomaterials prepared under similar conditions with three different surfactants, viz. CTAB, SDS and TX-100, which revealed that unprotected Ru0 networks are better catalysts than those stabilized with surfactants. The superior catalytic and electrocatalytic performance is due to the availability of unprotected Ru0 surfaces. The present route may provide a new possibility of synthesizing other surfactant-free, unprotected metal colloids for enhanced catalytic and electrocatalytic applications.

Dataset Information

Preparation and Synergy of Supported Ru⁰ and Pd⁰ for Rapid Chlorate Reduction at pH 7.

Publications

Preparation and Synergy of Supported Ru<sup>0</sup> and Pd<sup>0</sup> for Rapid Chlorate Reduction at pH 7.

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