A Pt1/(Co,Ni)(OH)2/C single-atom electro-catalyst efficiently splits water for H2generation,viabalanced water-dissociation and H2-formation steps from the synergistic effect of surface-defective (Co,Ni)(OH)2and electronically tuned Pt sites.
13 January 2025 in Journal of the American Chemical Society
Methanol (ME) is a liquid hydrogen carrier, ideal for on-site-on-demand H2 generation, avoiding its costly and risky distribution issues, but this "ME-to-H2" electric conversion suffers from high voltage (energy consumption) and competitive oxygen evolution reaction. Herein, we demonstrate that a synergistic cofunctional Pt1Pdn/(Ni,Co)(OH)x catalyst with Pt single atoms (Pt1) and Pd nanoclusters (Pdn) anchored on OH-vacancy(VOH)-rich (Ni,Co)(OH)x nanoparticles create synergistic triadic active sites, allowing for methanol-enhanced low-voltage H2 generation. For MOR, OH* is preferentially adsorbed on Pdn and then interacts with the intermediates (such as *CHO or *CHOOH) adsorbed favorably on neighboring Pt1 with the assistance of hydrogen bonding from the surface hydrogen of (Ni,Co)(OH)x. The enhanced selectivity of the *CHOOH pathway, instead of *CO, sustains the MOR activity to a practically high current density. For HER, triadic Pt1, Pdn, and OH-vacancy sites on (Ni,Co)(OH)x create an "acid-base" microenvironment to facilitate water adsorption and splitting, forming H* species on Pt1 and Pdn, and *OH at the vacancy, to promote efficient H2 evolution from the asymmetric Pt1 and Pdn sites via the Tafel mechanism. The triadic-site synergy opens new avenues for the design and synthesis of highly efficient and stable cofunctional catalysts for "on-site-on-demand" H2 production, here facilitated by liquid methanol.
Ru nanoclusters on Ni/Ni(OH)2 nanoparticles supported on carbon (Ru/Ni/Ni(OH)2/C) were successfully prepared and characterized. Ru/Ni/Ni(OH)2/C exhibited an unprecedented catalytic activity for naphthalene hydrogenation at room temperature due to synergetic catalysis.
Pd/CuO-Ni(OH) 2 /C showed superior electrocatalytic performance for EOR in comparison with PdCuNi alloy/C and Pd/C. In-situ FTIR studies have shown that CuO and Ni(OH) 2 effectively inhibited the adsorption of CO and increased the breaking rate of C-C.
This work illustrates that the synergistic effect of tiny Nics and PtNPs provides a novel strategy for designing highly active and durable electrocatalysts (Pt10/Ni-ZrO2-NC) for the MOR, HER and the coupling reaction of MOR∥HER.
Pt/rGNP exhibits much higher catalytic properties than other transition metal/rGNP catalysts for hydrogen evolution; its overpotential at 100 mA cm−2 in 0.5 M H2SO4 is only 10.6 mV, and its Tafel slope is 14.53 mV dec−1.