Leveraging Commercial Silver Inks as Oxidation Reduction Reaction Catalysts in Alkaline Medium

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1 Supporting Information Leveraging Commercial Silver Inks as Oxidation Reduction Reaction Catalysts in Alkaline Medium Shlomi Polani, Naftali Kanovsky and David Zitoun, *, Bar Ilan University, Department of Chemistry and Bar Ilan Institute of Nanotechnology and Advanced Materials (BINA), Ramat Gan , Israel Materials Ethylene glycol (EG) was purchased from Fisher Bioreagents. Potassium tetrachloroplatinate (K 2 PtCl 4 ) (99.9% Pt) and palladium chloride (PdCl 2 ) (99.9% Pd) were acquired from Strem Chemicals, and Sicrys I50T-11 (batch number P67) Ag ink from PV Nano Cell Ltd. Synthesis of AgM (M = Pt or Pd) hollow nanoparticles via galvanic replacement reaction The silver colloidal solution was prepared by mixing 100 μl silver ink and 2.4 ml EG in a glass vial. A 10 mm solution of M II was prepared by dissolving K 2 PtCl 4 or PdCl 2 in 2.5 ml EG and was stirred until a homogenous solution was formed. The M II solution was added dropwise to the silver colloidal solution at a rate of 1 ml/min via a syringe pump under vigorous stirring. The solution was stirred overnight until the completion of the reaction, signified by the solution turning black for Pt and blue for Pd. The dissolution of AgCl(s) was achieved as follows: three cycles of washing with 5 ml NaCl saturated water solution in the centrifuge (9000 RPM 4 C) and three cycles of 5 ml deionized water in the centrifuge (9000 RPM 4 C). Characterization The morphology of the NPs was investigated using the following electron microscopes: Transmission electron microscope (TEM) JEOL 1400 at 120 kv and high resolution TEM (HRTEM) analyses were S-1

2 performed using a JEOL JEM-2100F with accelerating voltage of 200 kv equipped with a JEOL JED-2300T energy dispersive X-ray spectrometer (EDS) for elemental analysis. Scanning TEM (STEM) images were taken using a high-angle annular dark-field (HAADF) JEOL detector (EM 24560). Probe tracking (drift correction) was used for chemical analysis at the nm scale. The high resolution scanning electron microscope (HRSEM) was an FEI model Magellan 400L. X-Ray diffractions (XRD) were collected on a Rigaku Smartlab X-ray diffractometer. The nanocrystals were drop-casted on a glass slide. Electrochemical measurements Electrochemical measurements were performed in a polypropylene cell in a three-electrode configuration using a polished cm 2 glassy carbon disk as working electrode, a glassy carbon rod as a counter electrode and RHE as a reference electrode. The thin-film electrode was prepared by dropcasting 10 μl of the catalyst modified ink on the glassy carbon. The alkaline solution was prepared from KOH (Sigma-Aldrich, %) and ultrapure water. The glassy carbon was mounted on a rotating electrode (Pine instruments) and all data were collected using a VMP3 potentiostat (Bio-Logic) impendance channel. Potentials were corrected for ohmic losses, measured by impedance spectroscopy before each polarization curve. All the gases used were of the highest purity available (99.999%). After purging in Ar for 15 min, the voltammograms were collected at 50 mv/s after stabilization for 50 cycles from 0.05 to 1.35 V vs RHE. For the oxidation reduction reaction (ORR), the electrolyte was bubbled for 30 min with oxygen gas. Linear sweep voltammograms were done at 225, 400, 625, 900, 1225, and 1600 RPM with a scan rate of 10 mv/s. S-2

3 500 nm Figure S1. Pristine Ag polyhedral sacrificial template S-3

4 Figure S2. High resolution scanning electron microscopy (HRSEM) micrographs (A & B) and transmission electron microscopy (TEM) micrographs (C & D) of hollow Ag 0.9 Pt 0.1 nanoparticles S-4

5 Figure S3. High resolution scanning electron microscopy (HRSEM) micrographs (A & B) and transmission electron microscopy (TEM) micrographs (C & D) of hollow Ag 0.9 Pd 0.1 nanoparticles S-5

6 AgPd Frequency Mean size: 90 ± 30 Diameter (nm) Figure S5. PSD of AgPd nanoshell AgPt Mean size: 80 ± 20 Frequency Diameter (nm) Figure S6. PSD of AgPt nanoshell S-6

7 A B AgPd AgPd after cleaning Intensity θ Figure S7. XRD of the Ag sacrificial template and the resulting nanoshells from the ink (A); XRD after cleaning the ink by washing with saturated NaCl aqueous solution (B). S-7

8 Figure S8: Cyclic voltammetry in 0.1 M KOH saturated with argon at 50 mv/s scan rate after 50, 150 and 250 cycles for (A) AgPt) and (B) AgPd S-8

9 Figure S9. Left Column- ORR curves at different RPMs (A, C and E) Right Column Koutecky Levich plots (B, D and F). S-9

10 Figure S10. Prices of different metals per year S-10

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