Journal
ACS CATALYSIS
Volume 9, Issue 3, Pages 2134-2157Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.8b02901
Keywords
proton exchange membrane (PEM) based water electrolysis; acidic oxygen evolution reaction (OER); electrocatalyst; one-dimensional nanorods; density functional theory (DFT)
Categories
Funding
- National Science Foundation, CBET [0933141, 1511390]
- U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering [DE-SC0001531]
- National Science Foundation [ACI-1053575]
- Edward R. Weidlein Chair Professorship funds
- Directorate For Engineering
- Div Of Chem, Bioeng, Env, & Transp Sys [0933141] Funding Source: National Science Foundation
- Div Of Chem, Bioeng, Env, & Transp Sys
- Directorate For Engineering [1511390] Funding Source: National Science Foundation
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Development of highly efficient, earth-abundant, and cost-effective electrocatalysts for the kinetically sluggish and energy intensive anodic oxygen evolution reaction (OER) is crucial for realizing the large-scale commercialization of proton exchange membrane based water electrolysis (PEMWE). Herein, we report the results of one-dimensional (1D) nanorods (NRs) containing an ultralow amount of noble metal (iridium, Ir) and 10 wt % fluorine (F) doped (Mn0.8Ir0.2)O-2:10F as an efficient anode electrocatalyst, synthesized via a simple hydrothermal and wet chemical approach for the acidic OER. The as-synthesized (Mn0.8Ir0.2)O-2:10F NRs demonstrate promising electrocatalytic performance for the OER with significantly lower overpotential (eta) and higher current density than state of the art IrO2 and many other electrocatalysts containing noble metal/reduced noble metal. Owing to the presence of 1D channels of the nanorod architecture and the unique electronic structure obtained upon formation of an F-containing solid solution, the (Mn0.8Ir0.2)O-2:10F NRs exhibit low charge transfer resistance (similar to 2.5 Omega cm(2)), low Tafel slope (similar to 38 mV dec(-1)), low water contact angle (similar to 18 degrees), high electrochemical active surface area (ECSA approximate to 704.76 m(2) g(-1)), high roughness factor (similar to 2114), and notable OER performance with similar to 6-, similar to 2.1-, and similar to 2.2-fold higher electrocatalytic activity in comparison to IrO2, (Mn0.8Ir0.2)O-2 NRs and a 2D thin film of (Mn0.8Ir0.2)O-2:10F, respectively. The significantly higher ECSA and BET specific activity (0.11 mA cm(BET)(-2)), mass activity (40 Ag-1), and TOF (0.01 s(-1)) at an overpotential (eta) of 220 mV suggest the intrinsically higher catalytic activity of (Mn0.8Ir0.2)O-2:10F NRs in comparison to other as-synthesized electrocatalysts. In addition, (Mn0.8Ir0.2)O-2:10F NRs function as robust electrocatalysts by delivering a current density of 10 mA cm(-2) at eta approximate to 200 mV and displaying long-term durability, devoid of any degradation of the catalytic activity, suggesting the structural robustness for displaying prolonged OER activity. Herein, on the basis of the synergistic effects of tailoring of 2D material length scales into a 1D nanorod framework and the corresponding formation of an F-substituted unique solid solution structure (as validated by density functional theory), (Mn0.8Ir0.2)O-2:10F NRs offer promise for an efficient OER in PEMWE.
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