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TiO@PDA无机-有机核壳骨架负载钯纳米点用于增强电催化加氢脱氯反应

TiO@PDA inorganic-organic core-shell skeleton supported Pd nanodots for enhanced electrocatalytic hydrodechlorination.

作者信息

Zhao Zhefei, Yu Li, Zheng Lingxia, Guo Tianyang, Lv Zhuoqing, Song Shuang, Zheng Huajun

机构信息

Department of Applied Chemistry, Zhejiang University of Technology, Hangzhou 310032, PR China.

Department of Applied Chemistry, Zhejiang University of Technology, Hangzhou 310032, PR China; State Key Laboratory Breeding Base of Green Chemistry Synthesis Technology, Zhejiang University of Technology, Hangzhou 310032, PR China.

出版信息

J Hazard Mater. 2022 Aug 5;435:128998. doi: 10.1016/j.jhazmat.2022.128998. Epub 2022 Apr 22.

Abstract

The development of catalysts with high atom utilization and activity is the biggest challenge for electrocatalytic hydrodechlorination (EHDC) technology. Herein, a design strategy of TiO@PDA inorganic-organic core-shell skeleton for loading lower dosage of noble palladium (Pd) with robust activity is reported. The self-supported TiO@PDA nanorod arrays provides exposed surface area for anchoring Pd and PDA as interlayer controls the Pd nucleation to form nanodots with high dispersion, realizing high atom utilization. Moreover, the strong interaction between PDA and Pd realizes the coexistence of electron-rich and deficient Pd species with suitable proportion, which facilitate the H* formation and the C-Cl bond activation, respectively, resulting in the promoted activity. The optimal TiO@PDA/Pd electrode exhibits a low dosage of Pd (0.093 mg cm) and excellent activity for 4-chlorophenol reduction with a mass activity (MA) of 23.96 ming, which is 3.31 times as high as that of TiO/Pd. The design scheme with inorganic-organic core-shell skeleton as support is benefit for developing highly efficient and lower price elctrocatalysts for EHDC.

摘要

开发具有高原子利用率和活性的催化剂是电催化加氢脱氯(EHDC)技术面临的最大挑战。在此,报道了一种用于负载较低剂量且具有强大活性的贵金属钯(Pd)的TiO@PDA无机-有机核壳骨架的设计策略。自支撑的TiO@PDA纳米棒阵列提供了用于锚定Pd的暴露表面积,并且作为中间层的PDA控制Pd成核以形成高分散的纳米点,从而实现高原子利用率。此外,PDA与Pd之间的强相互作用实现了具有适当比例的富电子和缺电子Pd物种的共存,这分别促进了H*的形成和C-Cl键的活化,从而提高了活性。最佳的TiO@PDA/Pd电极显示出低剂量的Pd(0.093 mg/cm)以及对4-氯苯酚还原具有优异的活性,其质量活性(MA)为23.96 mA/mg,是TiO/Pd的3.31倍。以无机-有机核壳骨架为载体的设计方案有利于开发用于EHDC的高效且低价的电催化剂。

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