Unraveling the Function of Metal–Amorphous Support Interactions in Single-Atom Electrocatalytic Hydrogen Evolution

Yang Liu; Xinghui Liu; Amol R. Jadhav; Taehun Yang; Yosep Hwang; Hongdan Wang; Lingling Wang; Yongguang Luo; Ashwani Kumar; Jinsun Lee; Huong T.D. Bui; Min Gyu Kim; Hyoyoung Lee

doi:10.1002/anie.202114160

Unraveling the Function of Metal–Amorphous Support Interactions in Single-Atom Electrocatalytic Hydrogen Evolution

Yang Liu
, Xinghui Liu
, Amol R. Jadhav
, Taehun Yang
, Yosep Hwang
, Hongdan Wang
, Lingling Wang
, Yongguang Luo
, Ashwani Kumar
, Jinsun Lee
, Huong T.D. Bui
, Min Gyu Kim
, Hyoyoung Lee

Department of Chemistry

Research output: Contribution to journal › Article › peer-review

148 Scopus citations

Abstract

Amorphization of the support in single-atom catalysts is a less researched concept for promoting catalytic kinetics through modulating the metal–support interaction (MSI). We modeled single-atom ruthenium (Ru_SAs) supported on amorphous cobalt/nickel (oxy)hydroxide (Ru-a-CoNi) to explore the favorable MSI between Ru_SAs and the amorphous skeleton for the alkaline hydrogen evolution reaction (HER). Differing from the usual crystal counterpart (Ru-c-CoNi), the electrons on Ru_SAs are facilitated to exchange among local configurations (Ru-O-Co/Ni) of Ru-a-CoNi since the flexibly amorphous configuration induces the possible d–d electron transfer and medium-to-long range p–π orbital coupling, further intensifying the MSI. This embodies Ru-a-CoNi with enhanced water dissociation, alleviated oxophilicity, and rapid hydrogen migration, which results in superior durability and HER activity of Ru-a-CoNi, wherein only 15 mV can deliver 10 mA cm⁻², significantly lower than the 58 mV required by Ru-c-CoNi.

Original language	English
Article number	e202114160
Journal	Angewandte Chemie - International Edition
Volume	61
Issue number	9
DOIs	https://doi.org/10.1002/anie.202114160
State	Published - 21 Feb 2022

Keywords

Amorphous Support
Hydrogen Evolution Reaction
Metal–Support Interaction
Orbital Coupling
Single-Atom Catalysts

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.1002/anie.202114160

Cite this

Liu, Y., Liu, X., Jadhav, A. R., Yang, T., Hwang, Y., Wang, H., Wang, L., Luo, Y., Kumar, A., Lee, J., Bui, H. T. D., Gyu Kim, M., & Lee, H. (2022). Unraveling the Function of Metal–Amorphous Support Interactions in Single-Atom Electrocatalytic Hydrogen Evolution. Angewandte Chemie - International Edition, 61(9), Article e202114160. https://doi.org/10.1002/anie.202114160

@article{ba7b4d2f61434ec6baeaee38c8f4aaf2,

title = "Unraveling the Function of Metal–Amorphous Support Interactions in Single-Atom Electrocatalytic Hydrogen Evolution",

abstract = "Amorphization of the support in single-atom catalysts is a less researched concept for promoting catalytic kinetics through modulating the metal–support interaction (MSI). We modeled single-atom ruthenium (RuSAs) supported on amorphous cobalt/nickel (oxy)hydroxide (Ru-a-CoNi) to explore the favorable MSI between RuSAs and the amorphous skeleton for the alkaline hydrogen evolution reaction (HER). Differing from the usual crystal counterpart (Ru-c-CoNi), the electrons on RuSAs are facilitated to exchange among local configurations (Ru-O-Co/Ni) of Ru-a-CoNi since the flexibly amorphous configuration induces the possible d–d electron transfer and medium-to-long range p–π orbital coupling, further intensifying the MSI. This embodies Ru-a-CoNi with enhanced water dissociation, alleviated oxophilicity, and rapid hydrogen migration, which results in superior durability and HER activity of Ru-a-CoNi, wherein only 15 mV can deliver 10 mA cm−2, significantly lower than the 58 mV required by Ru-c-CoNi.",

keywords = "Amorphous Support, Hydrogen Evolution Reaction, Metal–Support Interaction, Orbital Coupling, Single-Atom Catalysts",

author = "Yang Liu and Xinghui Liu and Jadhav, \{Amol R.\} and Taehun Yang and Yosep Hwang and Hongdan Wang and Lingling Wang and Yongguang Luo and Ashwani Kumar and Jinsun Lee and Bui, \{Huong T.D.\} and \{Gyu Kim\}, Min and Hyoyoung Lee",

note = "Publisher Copyright: {\textcopyright} 2021 Wiley-VCH GmbH",

year = "2022",

month = feb,

day = "21",

doi = "10.1002/anie.202114160",

language = "English",

volume = "61",

journal = "Angewandte Chemie - International Edition",

issn = "1433-7851",

publisher = "John Wiley and Sons Ltd",

number = "9",

}

TY - JOUR

T1 - Unraveling the Function of Metal–Amorphous Support Interactions in Single-Atom Electrocatalytic Hydrogen Evolution

AU - Liu, Yang

AU - Liu, Xinghui

AU - Jadhav, Amol R.

AU - Yang, Taehun

AU - Hwang, Yosep

AU - Wang, Hongdan

AU - Wang, Lingling

AU - Luo, Yongguang

AU - Kumar, Ashwani

AU - Lee, Jinsun

AU - Bui, Huong T.D.

AU - Gyu Kim, Min

AU - Lee, Hyoyoung

PY - 2022/2/21

Y1 - 2022/2/21

N2 - Amorphization of the support in single-atom catalysts is a less researched concept for promoting catalytic kinetics through modulating the metal–support interaction (MSI). We modeled single-atom ruthenium (RuSAs) supported on amorphous cobalt/nickel (oxy)hydroxide (Ru-a-CoNi) to explore the favorable MSI between RuSAs and the amorphous skeleton for the alkaline hydrogen evolution reaction (HER). Differing from the usual crystal counterpart (Ru-c-CoNi), the electrons on RuSAs are facilitated to exchange among local configurations (Ru-O-Co/Ni) of Ru-a-CoNi since the flexibly amorphous configuration induces the possible d–d electron transfer and medium-to-long range p–π orbital coupling, further intensifying the MSI. This embodies Ru-a-CoNi with enhanced water dissociation, alleviated oxophilicity, and rapid hydrogen migration, which results in superior durability and HER activity of Ru-a-CoNi, wherein only 15 mV can deliver 10 mA cm−2, significantly lower than the 58 mV required by Ru-c-CoNi.

AB - Amorphization of the support in single-atom catalysts is a less researched concept for promoting catalytic kinetics through modulating the metal–support interaction (MSI). We modeled single-atom ruthenium (RuSAs) supported on amorphous cobalt/nickel (oxy)hydroxide (Ru-a-CoNi) to explore the favorable MSI between RuSAs and the amorphous skeleton for the alkaline hydrogen evolution reaction (HER). Differing from the usual crystal counterpart (Ru-c-CoNi), the electrons on RuSAs are facilitated to exchange among local configurations (Ru-O-Co/Ni) of Ru-a-CoNi since the flexibly amorphous configuration induces the possible d–d electron transfer and medium-to-long range p–π orbital coupling, further intensifying the MSI. This embodies Ru-a-CoNi with enhanced water dissociation, alleviated oxophilicity, and rapid hydrogen migration, which results in superior durability and HER activity of Ru-a-CoNi, wherein only 15 mV can deliver 10 mA cm−2, significantly lower than the 58 mV required by Ru-c-CoNi.

KW - Amorphous Support

KW - Hydrogen Evolution Reaction

KW - Metal–Support Interaction

KW - Orbital Coupling

KW - Single-Atom Catalysts

UR - https://www.scopus.com/pages/publications/85122760402

U2 - 10.1002/anie.202114160

DO - 10.1002/anie.202114160

M3 - Article

C2 - 34964231

AN - SCOPUS:85122760402

SN - 1433-7851

VL - 61

JO - Angewandte Chemie - International Edition

JF - Angewandte Chemie - International Edition

IS - 9

M1 - e202114160

ER -

Unraveling the Function of Metal–Amorphous Support Interactions in Single-Atom Electrocatalytic Hydrogen Evolution

Abstract

Keywords

UN SDGs

Access to Document

Other files and links

Fingerprint

Cite this