Structural and Electronic Engineering of Ir-Doped Ni-(Oxy)hydroxide Nanosheets for Enhanced Oxygen Evolution Activity

Liu，Jinlong1,2,6; Xiao，Juanxiu3; Wang，Zhenyu4; Yuan，Huimin4; Lu，Zhouguang4; Luo，Bingcheng5; Tian，Enke5; Waterhouse，Geoffrey I.N.2,6

2021

10.1021/acscatal.1c00110

ACS Catalysis   影响因子和分区

2155-5435

Discovering highly active and stable electrocatalysts for the oxygen evolution reaction (OER) is critical to the commercial development of many next-generation energy conversion and storage devices, with Fe-doped nickel (oxy)hydroxide representing one of the most promising OER catalysts developed to date. However, the active sites and mechanism of OER on Fe-doped nickel (oxy)hydroxide catalysts remain unclear. To gain deeper insights into the role of metal dopants in enhancing OER activity, we explored here the role of Ir-doping in the OER performance of nickel (oxy)hydroxide catalysts, placing particular emphasis on the nature of the active site. Density functional theory calculations with Hubbard U correction revealed that Ir-doping of a β-NiOOH(001) surface enhanced the electric conductivity while also activating an oxygen site involving three Ni atoms (Ni3 site) to realize a remarkably low OER overpotential of only η = 0.46 V, much lower than the overpotential on the oxygen site involving Ir + two Ni atoms (IrNi2 site, η = 0.77 V) or the oxygen site involving three Ni atoms in pristine β-NiOOH (η = 0.66 V). Guided by the computational results, ultrathin Ir-doped Ni(OH)2 nanosheets were then fabricated through a combination of hydrothermal assembly and liquid exfoliation, with the nanosheets transforming to Ir-doped NiOOH during OER and offering superior activity relative to pristine Ni(OH)2 nanosheets or a commercial IrO2 catalyst, thereby validating the theoretical predictions. The computational and experimental results thus conclusively demonstrate that Ir-doping and nanosheet engineering are synergistic strategies for tuning the electronic and structural properties of nickel (oxy)hydroxides for improved oxygen evolution electrocatalysis.

active site electrocatalyst iridium doping nickel oxyhydroxide oxygen evolution reaction

SCI ; EI

英语

其他

WOS:000649106200040

20212210424162

Atoms ; Binary alloys ; Catalyst activity ; Computation theory ; Density functional theory ; Electrocatalysis ; Electrocatalysts ; Energy conversion ; Nanocatalysts ; Nanosheets ; Oxygen ; Oxygen evolution reaction ; Virtual storage

Energy Conversion Issues:525.5 ; Computer Theory, Includes Formal Logic, Automata Theory, Switching Theory, Programming Theory:721.1 ; Data Storage, Equipment and Techniques:722.1 ; Nanotechnology:761 ; Electrochemistry:801.4.1 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Atomic and Molecular Physics:931.3 ; Solid State Physics:933

2-s2.0-85105555063

Scopus

1.College of Chemistry and Chemical Engineering,Central South University,Changsha,410083,China
2.School of Chemical Sciences,University of Auckland,Auckland,1142,New Zealand
3.State Laboratory of Marine Resource Utilization in South China Sea,Hainan University,Haikou,570228,China
4.Department of Materials Science and Engineering,Southern University of Science and Technology,Shenzhen,518055,China
5.School of Science,China University of Geosciences,Beijing,100083,China
6.MacDiarmid Institute for Advanced Materials and Nanotechnology,Wellington,6140,New Zealand

Liu，Jinlong,Xiao，Juanxiu,Wang，Zhenyu,et al. Structural and Electronic Engineering of Ir-Doped Ni-(Oxy)hydroxide Nanosheets for Enhanced Oxygen Evolution Activity[J]. ACS Catalysis,2021,11:5386-5395.

Liu，Jinlong.,Xiao，Juanxiu.,Wang，Zhenyu.,Yuan，Huimin.,Lu，Zhouguang.,...&Waterhouse，Geoffrey I.N..(2021).Structural and Electronic Engineering of Ir-Doped Ni-(Oxy)hydroxide Nanosheets for Enhanced Oxygen Evolution Activity.ACS Catalysis,11,5386-5395.

Liu，Jinlong,et al."Structural and Electronic Engineering of Ir-Doped Ni-(Oxy)hydroxide Nanosheets for Enhanced Oxygen Evolution Activity".ACS Catalysis 11(2021):5386-5395.