Exploring highly efficient Pt-free catalysts for hydrogen evolution reaction(HER)is of great importance for hydrogen(H2)production.Herein,a novel HER electrocatalyst having abundant ultra-small(2–3 nm)Ru electronical...Exploring highly efficient Pt-free catalysts for hydrogen evolution reaction(HER)is of great importance for hydrogen(H2)production.Herein,a novel HER electrocatalyst having abundant ultra-small(2–3 nm)Ru electronically confined by a B,N codoped polar carbon surface(Ru/(B-N)-PC)was constructed.The Ru/(B-N)-PC catalyst exhibits a low overpotential of 15 mV at the current density of 10 mA·cm^(−2),a low Tafel slope of 22.6 mV·dec^(−1),superior durability,which outperforms the benchmark Pt/C catalyst.Both experimental characterizations and theory calculations suggest that an electron communication established between B,N co-doped carbon surface and ultra-small Ru nanoparticles with electrons transferred from N atoms to Ru and backtransferred from Ru to B atoms,which exerts a moderate electronic modification of Ru.This,in turn,affords a modest H adsorption energy and a lower H2O dissociation barrier,leading to the high-performance hydrogen evolution reaction.The work provides meaningful insight into the size control and electronic modulation of Ru catalyst for intrinsic HER activity improvement.展开更多
基金the National Natural Science Foundation of China(No.22072069)the Research Fund Program of Guangdong Provincial Key Lab of Green Chemical Product Technology(No.GC202101)+3 种基金the Hubei Key Laboratory of Processing and Application of Catalytic materials(No.202121904)the State Key Laboratory of Structural Chemistry,Fujian Institute of Research on the Structure of Matter(No.20210012)the JST-ERATO Yamauchi Materials Space-Tectonics Project(No.JPMJER2003)the Researchers Supporting Project(No.RSP-2021/243),King Saud University,Riyadh,Saudi Arabia.
文摘Exploring highly efficient Pt-free catalysts for hydrogen evolution reaction(HER)is of great importance for hydrogen(H2)production.Herein,a novel HER electrocatalyst having abundant ultra-small(2–3 nm)Ru electronically confined by a B,N codoped polar carbon surface(Ru/(B-N)-PC)was constructed.The Ru/(B-N)-PC catalyst exhibits a low overpotential of 15 mV at the current density of 10 mA·cm^(−2),a low Tafel slope of 22.6 mV·dec^(−1),superior durability,which outperforms the benchmark Pt/C catalyst.Both experimental characterizations and theory calculations suggest that an electron communication established between B,N co-doped carbon surface and ultra-small Ru nanoparticles with electrons transferred from N atoms to Ru and backtransferred from Ru to B atoms,which exerts a moderate electronic modification of Ru.This,in turn,affords a modest H adsorption energy and a lower H2O dissociation barrier,leading to the high-performance hydrogen evolution reaction.The work provides meaningful insight into the size control and electronic modulation of Ru catalyst for intrinsic HER activity improvement.
