TY - JOUR
T1 - Revealing The Role of Electronic Asymmetricity on Supported Ru Nanoclusters for Alkaline Hydrogen Evolution Reaction
AU - Zhu, Shenglin
AU - Li, Zijian
AU - Hou, Liqiang
AU - Kim, Min Gyu
AU - Jang, Haeseong
AU - Liu, Shangguo
AU - Liu, Xien
PY - 2024/4/25
Y1 - 2024/4/25
N2 - Modulating the electronic asymmetricity of catalysts is an effective method for optimizating the elementary steps of water dissociation and hydrogen adsorption/desorption process for the alkaline hydrogen evolution reaction (HER). Herein, uniform Ru nanoclusters anchored on N doped ultrathin carbon nanosheets (Ru/NC) are synthesized to optimize the asymmetricity electronic properties of supported Ru for efficient HER. It is found that Ru and NC with a large work function difference (ΔΦ) leading to the formation of stronger asymmetrical charge distributions of Ru that electron-deficient high-valence Ru (Run+) coupling with low-valence Ru (Ru0). Experimental and theoretical studies indicate the Run+ sites lowered the energy barrier for water dissociation and provided enough hydrogen proton to promote the hydrogen spillover from the Run+ to Ru0 sites, and Ru0 sites can enhance H desorption process, thus synergistically enhancing the hydrogen evolution activity. Notably, the Ru/NC catalyst exhibits a high alkaline HER activity (21.9 mV@10 mA cm−2, 29.03 mV dec−1). The role of electronic asymmetricity on supported Ru nanoclusters for the alkaline HER are demonstrated, which will provide guidelines for the rational design of high-efficiency alkaline HER catalysts. © 2023 Wiley-VCH GmbH.
AB - Modulating the electronic asymmetricity of catalysts is an effective method for optimizating the elementary steps of water dissociation and hydrogen adsorption/desorption process for the alkaline hydrogen evolution reaction (HER). Herein, uniform Ru nanoclusters anchored on N doped ultrathin carbon nanosheets (Ru/NC) are synthesized to optimize the asymmetricity electronic properties of supported Ru for efficient HER. It is found that Ru and NC with a large work function difference (ΔΦ) leading to the formation of stronger asymmetrical charge distributions of Ru that electron-deficient high-valence Ru (Run+) coupling with low-valence Ru (Ru0). Experimental and theoretical studies indicate the Run+ sites lowered the energy barrier for water dissociation and provided enough hydrogen proton to promote the hydrogen spillover from the Run+ to Ru0 sites, and Ru0 sites can enhance H desorption process, thus synergistically enhancing the hydrogen evolution activity. Notably, the Ru/NC catalyst exhibits a high alkaline HER activity (21.9 mV@10 mA cm−2, 29.03 mV dec−1). The role of electronic asymmetricity on supported Ru nanoclusters for the alkaline HER are demonstrated, which will provide guidelines for the rational design of high-efficiency alkaline HER catalysts. © 2023 Wiley-VCH GmbH.
KW - density functional theory
KW - electronic asymmetricity
KW - hydrogen evolution reaction
KW - Ru nanoclusters
UR - http://www.scopus.com/inward/record.url?scp=85180702520&partnerID=8YFLogxK
UR - https://www.scopus.com/record/pubmetrics.uri?eid=2-s2.0-85180702520&origin=recordpage
U2 - 10.1002/adfm.202314899
DO - 10.1002/adfm.202314899
M3 - RGC 21 - Publication in refereed journal
SN - 1616-301X
VL - 34
JO - Advanced Functional Materials
JF - Advanced Functional Materials
IS - 17
M1 - 2314899
ER -
