State Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China), Qingdao 266580, China.
State Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China), Qingdao 266580, China; Key Laboratory of Biofuels, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, China.
J Environ Sci (China). 2025 Mar;149:288-300. doi: 10.1016/j.jes.2024.01.053. Epub 2024 Feb 10.
Structural regulation of Pd-based electrocatalytic hydrodechlorination (EHDC) catalyst for constructing high-efficient cathode materials with low noble metal content and high atom utilization is crucial but still challenging. Herein, a support electron inductive effect of Pd-Mn/Ni foam catalyst was proposed via in-situ Mn doping to optimize the electronic structure of the Ni foam (NF), which can inductive regulation of Pd for improving the EHDC performance. The mass activity and current efficiency of Pd-Mn/NF catalyst are 2.91 and 1.34 times superior to that of Pd/NF with 2,4-dichlorophenol as model compound, respectively. The Mn-doped interlayer optimized the electronic structure of Pd by bringing the d-state closer to the Fermi level than Pd on the NF surface, which optimizied the binding of EHDC intermediates. Additionally, the Mn-doped interlayer acted as a promoter for generating H* and accelerating the EHDC reaction. This work presents a simple and effective regulation strategy for constructing high-efficient cathode catalyst for the EHDC of chlorinated organic compounds.
构建贵金属含量低、原子利用率高的高效阴极材料，对 Pd 基电催化加氢脱氯（EHDC）催化剂的结构进行调控至关重要，但极具挑战性。在此，通过原位 Mn 掺杂提出了 Pd-Mn/Ni 泡沫催化剂的支撑电子诱导效应，以优化 Ni 泡沫（NF）的电子结构，从而对 Pd 进行感应调节，以提高 EHDC 性能。以 2,4-二氯苯酚为模型化合物，Pd-Mn/NF 催化剂的质量活性和电流效率分别是 Pd/NF 的 2.91 倍和 1.34 倍。掺杂中间层优化了 Pd 的电子结构，使 d 态比 NF 表面上的 Pd 更接近费米能级，从而优化了 EHDC 中间体的结合。此外，掺杂中间层作为生成 H*的促进剂，并加速 EHDC 反应。这项工作提出了一种简单有效的调控策略，用于构建高效的 EHDC 氯代有机化合物阴极催化剂。
