CAS Key Laboratory of Urban Pollutant Conversion, Department of Chemistry, University of Science & Technology of China, Hefei 230026, China.
CAS Key Laboratory of Urban Pollutant Conversion, Department of Chemistry, University of Science & Technology of China, Hefei 230026, China.
Chemosphere. 2015 Apr;125:57-63. doi: 10.1016/j.chemosphere.2015.01.052. Epub 2015 Feb 16.
Electrocatalytic hydrodehalogenation is a cost-effective approach to degrade halogenated organic pollutants in groundwater, and Pd-based catalysts have been found to be an efficient cathode material for this purpose. In this work, a novel Cu@Pd bimetallic catalyst loaded on Ti plate was prepared via combined electrodeposition and galvanic replacement for electrocatalytic hydrodehalogenation of atrazine, a typical halogenated pollutant. The obtained bimetallic catalyst with uniformly dispersed Pd nanoparticles possessed a large electrochemically active surface area of 572 cm2. The Cu@Pd/Ti cathode exhibited a higher electrocatalytic efficiency towards atrazine reduction than the individual Pd/Ti or Cu/Ti cathodes, and achieved up to 91.5% within 120 min under a current density of 1 mA cm(-2). Such an electrocatalytic reduction followed pseudo-first-order kinetics with a rate constant of 0.0214 min(-1). Atrazine was selectively transformed to dechlorinated atrazine, and its degradation pathway was identified. Current density was found to have a critical influence on the atrazine reduction due to the competitive hydrogen evolution reaction at a higher current density. The fabricated bimetallic catalyst also exhibited a good stability. This work provides an efficient and stable electrocatalyst for chlorinated contaminate removal and groundwater remediation.
电催化加氢脱卤是一种经济有效的方法,可以降解地下水中的卤代有机污染物,而基于 Pd 的催化剂已被发现是一种有效的阴极材料。在这项工作中,通过联合电沉积和电置换法,在 Ti 板上制备了一种新型的负载在 Ti 板上的 Cu@Pd 双金属催化剂,用于电催化加氢脱卤阿特拉津,这是一种典型的卤代污染物。所获得的具有均匀分散的 Pd 纳米粒子的双金属催化剂具有 572 cm2 的大电化学活性表面积。与单独的 Pd/Ti 或 Cu/Ti 阴极相比,Cu@Pd/Ti 阴极对阿特拉津还原具有更高的电催化效率,在 1 mA cm(-2)的电流密度下,在 120 min 内达到 91.5%。这种电催化还原遵循准一级动力学,速率常数为 0.0214 min(-1)。阿特拉津被选择性地转化为脱氯阿特拉津,并确定了其降解途径。由于在较高电流密度下竞争的析氢反应,电流密度被发现对阿特拉津还原有重要影响。所制备的双金属催化剂也表现出良好的稳定性。这项工作为去除氯化污染物和地下水修复提供了一种高效稳定的电催化剂。