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Strong Pyrrolic-N-Pd Interactions Boost the Electrocatalytic Hydrodechlorination Reaction on Palladium Nanoparticles

Abstract

We demonstrated the heteroatomic nitrogen (N) doping on graphene can significantly enhance the performance of the graphene-palladium nanoparticles composite catalyst (N/G-Pd) in electrocatalytic hydrodechlorination reaction (EHDC). Specifically at -0.80 V (vs. Ag/AgCl), the N/G-430-Pd (prepared at 430 oC, pyridinic/pyrrolic-N-rich) and N/G-900-Pd (prepared at 900 oC, pyridinic/graphitic-N-rich) with equivalent total N content delivered the apparent rate constant (kobs) of 0.28 and 0.20 min-1 molPd-1 in removing 2,4-dichlorophenol, much higher than 0.13 min-1 molPd-1 of the C-Pd. Additionally, we identified the determinant role of pyrrolic-N in boosting EHDC from the linear relationship between kobs-N and the pyrrolic-N content in catalyst. A combined experimental and DFT analyses revealed the positive effect of N doping originated from the strong N-Pd interactions, which modulated the Pd electronic structure and its interactions with the reactant and EHDC products (phenol and Cl-). Pyrrolic N-Pd bond was favored as it could balance the reactant adsorption and the product desorption.

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Publication details

The article was received on 31 Aug 2019, accepted on 30 Nov 2019 and first published on 02 Dec 2019


Article type: Paper
DOI: 10.1039/C9NR07528C
Nanoscale, 2019, Accepted Manuscript

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    Strong Pyrrolic-N-Pd Interactions Boost the Electrocatalytic Hydrodechlorination Reaction on Palladium Nanoparticles

    W. Peng, X. Shi, C. Fu, J. X. Li, J. Li, X. Lv, Y. chu, F. Dong and G. Jiang, Nanoscale, 2019, Accepted Manuscript , DOI: 10.1039/C9NR07528C

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