Advanced Science (Sep 2020)
Charge Redistribution Caused by S,P Synergistically Active Ru Endows an Ultrahigh Hydrogen Evolution Activity of S‐Doped RuP Embedded in N,P,S‐Doped Carbon
Abstract
Abstract Water splitting for production of hydrogen as a clean energy alternative to fossil fuel has received much attention, but it is still a tough challenge to synthesize electrocatalysts with controllable bonding and charge distribution. In this work, ultrafine S‐doped RuP nanoparticles homogeneously embedded in a N, P, and S‐codoped carbon sheet (S‐RuP@NPSC) is synthesized by pyrolysis of poly(cyclotriphosphazene‐co‐4,4′‐sulfonyldiphenol) (PZS) as the source of C/N/S/P. The bondings between Ru and N, P, S in PZS are regulated to synthesize RuS2 (800 °C) and S‐RuP (900 °C) by different calcination temperatures. The S‐RuP@NPSC with low Ru loading of 0.8 wt% with abundant active catalytic sites possesses high utilization of Ru, the mass catalytic activity is 22.88 times than 20 wt% Pt/C with the overpotential of 250 mV. Density functional theory calculation confirms that the surface Ru (−0.18 eV) and P (0.05 eV) are catalytic active sites for the hydrogen evolution reaction (HER), and the according charge redistribution of Ru is regulated by S and P with reverse electronegativity and electron–donor property to induce a synergistically enhanced reactivity toward the HER. This work provides a rational method to regulate the bonding and charge distribution of Ru‐based electrocatalysts by reacting macromolecules with multielement of C/N/S/P with Ru.
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