Issue 14, 2023

Alloying promotion of Pd-based metallenes in electrocatalytic hydrogenation of functionalized nitroarenes

Abstract

Electrocatalytic hydrogenation (ECH) provides a controllable and sustainable reduction of organic compounds via multi-electron-transfer processes under ambient conditions, which urgently demands high-performance electrocatalysts with satisfactory activity and selectivity. Here, two-dimensional Pd-based metallenes are for the first time introduced as efficient electrocatalysts for the ECH of nitroarenes, showing the intrinsic promotion of active sites by alloying effects. Thereinto, a Pd–Mo metallene with a highly exposed active surface and strong electronic interactions between Pd and Mo atoms affords the chemoselective hydrogenation of 4-nitrostyrene (4-NS) toward value-added 4-vinylaniline (4-VA). At −0.25 V vs. RHE, it reaches a high selectivity (>90.0%) and faradaic efficiency (78.3%) of 4-VA, outperforming the counterparts of a home-made Pd metallene and commercial Pd/C. The consistent alloying promotion is further verified on a series of Pd–M (M = Cr, Mo, and W) metallenes, with the specific activity sequence (Pd–Mo > Pd–W > Pd–Cr > Pd) that can be theoretically interpreted by the gradually strengthened chemisorption of 4-NS after alloying Pd with M. Moreover, the good efficiency within a broad substrate scope highlights the promise of Pd-based metallenes in electrochemical refinery.

Graphical abstract: Alloying promotion of Pd-based metallenes in electrocatalytic hydrogenation of functionalized nitroarenes

Supplementary files

Article information

Article type
Paper
Submitted
27 Dez 2022
Accepted
01 Mrz 2023
First published
01 Mrz 2023

J. Mater. Chem. A, 2023,11, 7505-7512

Alloying promotion of Pd-based metallenes in electrocatalytic hydrogenation of functionalized nitroarenes

W. Zhang, W. Zhang, J. Tan, D. Pan, Y. Tang and Q. Gao, J. Mater. Chem. A, 2023, 11, 7505 DOI: 10.1039/D2TA10021E

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