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Title: Single-Crystalline Ultrathin Co3O4 Nanosheets with Massive Vacancy Defects for Enhanced Electrocatalysis

Journal Article · · Advanced Energy Materials
 [1];  [2];  [3];  [1];  [4];  [2];  [4];  [2];  [2];  [3];  [4];  [2]
  1. Beijing Univ. of Chemical Technology (China); Yale Univ., West Haven, CT (United States)
  2. Beijing Univ. of Chemical Technology (China)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States)
  4. Yale Univ., West Haven, CT (United States)

Abstract The role of vacancy defects is demonstrated to be positive in various energy‐related processes. However, introducing vacancy defects into single‐crystalline nanostructures with given facets and studying their defect effect on electrocatalytic properties remains a great challenge. Here this study deliberately introduces oxygen defects into single‐crystalline ultrathin Co 3 O 4 nanosheets with O‐terminated {111} facets by mild solvothermal reduction using ethylene glycol under alkaline condition. As‐prepared defect‐rich Co 3 O 4 nanosheets show a low overpotential of 220 mV with a small Tafel slope of 49.1 mV dec −1 for the oxygen evolution reaction (OER), which is among the best Co‐based OER catalysts to date and even more active than the state‐of‐the‐art IrO 2 catalyst. Such vacancy defects are formed by balancing with reducing environments under solvothermal conditions, but are surprisingly stable even after 1000 cycles of scanning under OER working conditions. Density functional theory plus U calculation attributes the enhanced performance to the oxygen vacancies and consequently exposed second‐layered Co metal sites, which leads to the lowered OER activation energy of 2.26 eV and improved electrical conductivity. This mild solvothermal reduction concept opens a new door for the understanding and future designing of advanced defect‐based electrocatalysts.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States); Beijing University of Chemical Technology (China); Yale Univ., West Haven, CT (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC); National Natural Science Foundation of China (NSFC)
Grant/Contract Number:
SC0012704; 2016YFC0801302; 2016YFF0204402; DE‐SC0012704
OSTI ID:
1395946
Alternate ID(s):
OSTI ID: 1392682
Report Number(s):
BNL-114373-2017-JA; R&D Project: MA453MAEA; VT1201000
Journal Information:
Advanced Energy Materials, Vol. 8, Issue 3; ISSN 1614-6832
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 385 works
Citation information provided by
Web of Science

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Defect-Induced Pt-Co-Se Coordinated Sites with Highly Asymmetrical Electronic Distribution for Boosting Oxygen-Involving Electrocatalysis journal November 2018
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Structural Engineering of Low‐Dimensional Metal–Organic Frameworks: Synthesis, Properties, and Applications journal April 2019
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Insights into Correlation among Surface‐Structure‐Activity of Cobalt‐Derived Pre‐Catalyst for Oxygen Evolution Reaction journal January 2020
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