am8b10845_si_001.pdf (2.58 MB)
Pt–C Interfaces Based on Electronegativity-Functionalized Hollow Carbon Spheres for Highly Efficient Hydrogen Evolution
journal contribution
posted on 2018-12-06, 20:49 authored by Xiao Shang, Zi-Zhang Liu, Shan-Shan Lu, Bin Dong, Jing-Qi Chi, Jun-Feng Qin, Xien Liu, Yong-Ming Chai, Chen-Guang LiuThe
hydrogen evolution reaction activity of carbon-supported Pt
catalyst is highly dependent on Pt–C interfaces. Herein, we
focus on the relationships between Pt activity and N/O-functionalized
hollow carbon sphere (HCS) substrate in acidic media. The electrochemical
dissolution of Pt counter electrode is performed to prepare Pt nanoparticles
in low loading. The N groups are beneficial for homogeneously sized
Pt nanoparticles, whereas the O groups lead to aggregated nanoparticles.
Moreover, the proper electronegativity of the N groups may enable
capturing of protons to create proton-rich Pt–C interfaces
and transfer them onto the Pt sites. The O groups may also capture
protons by hydrogen bonding, but the subsequent release of protons
is more difficult due to a stronger electronegativity and result in
an inferior Pt activity. Consequently, the N-doped HCS with a low
Pt loading (1.7 μg cm–2 and 0.05 wt %) possesses
a higher intrinsic activity compared with Pt on O-doped HCS. Moreover,
it outperforms the commercial 20% Pt/C with a stable operation for
12 h. This work may provide suggestions for constructing the advantageous
Pt–C interfaces by proper functional groups for high catalytic
efficiencies.