Magnetically separable Pd-iron-oxides composites as highly efficient and recyclable catalysts for ultra-rapid degradation and debromination of polybrominated diphenyl ethers

Cuicui Wang; Nan Wang; Guihua Zhang; Dongxiao Wen; Fangfang Song; Lihua Zhu; Ming Lei; Shuangshuang Huang; Heqing Tang

doi:10.1016/j.scitotenv.2023.169717

Magnetically separable Pd-iron-oxides composites as highly efficient and recyclable catalysts for ultra-rapid degradation and debromination of polybrominated diphenyl ethers

Sci Total Environ. 2024 Mar 1:914:169717. doi: 10.1016/j.scitotenv.2023.169717. Epub 2023 Dec 30.

Authors

Cuicui Wang¹, Nan Wang¹, Guihua Zhang¹, Dongxiao Wen¹, Fangfang Song¹, Lihua Zhu², Ming Lei³, Shuangshuang Huang⁴, Heqing Tang⁵

Affiliations

¹ School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan 430074, PR China.
² School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan 430074, PR China. Electronic address: lhzhu63@hust.edu.cn.
³ College of Resources and Environmental Science, South-Central Minzu University, Wuhan 430074, PR China. Electronic address: leiming@mail.scuec.edu.cn.
⁴ School of Physics and Technology, Center for Electron Microscopy, MOE Key Laboratory of Artificial Micro- and Nano-structures, and Institute for Advanced Studies, Wuhan University, Wuhan 430072, PR China.
⁵ College of Resources and Environmental Science, South-Central Minzu University, Wuhan 430074, PR China.

PMID: 38163606
DOI: 10.1016/j.scitotenv.2023.169717

Abstract

When precious nano-metals are used as environmental catalysts, it is important to tune the particle sizes and the reusability of the nano-metals for achieving their highly efficient catalytic performance at a low cost. In the present work, magnetic iron oxides (FeO_x-Y) nanoparticles were pre-prepared as supports of nano-metals, where Y represented the mole percentage of Fe(III) in the total iron (Y ≥ 50 %). FeO_x-Y (support), PdCl₄^2- (Pd source) and NaBH₄ (reducing agent) were added into the organic pollutant solution containing 2,2',4,4'-tetrabromodiphenyl ether (BDE47). After the NaBH₄ was added, the followed reaction realized not only the rapid in-situ preparation of a Pd-loaded FeO_x-Y composite catalyst (Pd-FeO_x-Y), but also the ultra-fast and complete debromination of BDE47 within 30 s. Comparing the case without adding FeO_x-Y, the debromination efficiency of BDE47 was much promoted in the presence of FeO_x-Y. The support-induced enhancing effect on the catalytic ability of Pd nanoparticles was improved by increasing the Fe(III) content in the support, being attributed to the much more hydroxyl groups on the support surface. Considering both the catalytic and recovery abilities of Pd-FeO_x-Y, Pd-FeO_x-75 was the optimal choice because it could be magnetically recovered and re-used for multiple cycles with high catalytic activities. The presently developed "catalyst preparation-pollutant degradation" one-pot system could be applied to conduct complete debromination of all the PBDEs.

Keywords: Iron oxides support; Pd catalyst; Polybrominated diphenyl ethers; Reductive debromination; Surface hydroxyl species.