TY - JOUR
T1 - Electrolysis on a Chip with Tunable Thin Film Nanostructured PGM Electrocatalysts Generated from Self-Assembled Block Copolymer Templates
AU - Bhattacharya, Deepra
AU - Kole, Subarna
AU - Kizilkaya, Orhan
AU - Strzalka, Joseph
AU - Angelopoulou, Polyxeni P.
AU - Sakellariou, Georgios
AU - Cao, Dongmei
AU - Arges, Christopher G.
N1 - Funding Information:
This material is based upon work supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences Separation Science program under Award No. DE‐SC0018989. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE‐AC02‐06CH11357 (Beamline 8‐ID‐E for GI‐SAXS experiments). LSU Shared Instrumentation Facilities, Nanofabrication Facility and Center for Advanced Microstructures and Devices (CAMD) were used for this work. D.B., S.K., and C.G.A. acknowledge Prof. Kevin McPeak's help with cleanroom operation. D.B. and C.G.A. acknowledge Prof. Bhuvnesh Bharti's assistance with tensiometry.
Publisher Copyright:
© 2021 Wiley-VCH GmbH
PY - 2021/6/24
Y1 - 2021/6/24
N2 - Self-assembled block copolymers are promising templates for fabricating thin film materials with tuned periodic feature sizes and geometry at the nanoscale. Here, a series of nanostructured platinum and iridium oxide electrocatalysts templated from poly(styrene)-block-poly(vinyl pyridine) (PSbPVP) block copolymers via an incipient wetness impregnation (IWI) pathway is reported. Both nanowire and nanocylinder electrocatalysts of varying feature sizes are assessed and higher catalyst loadings are achieved by the alkylation of the pyridine moieties in the PVP block prior to IWI. Electrocatalyst evaluations featuring hydrogen pump and water electrolysis demonstrations are carried out on interdigitated electrode (IDE) chips flexible with liquid supporting electrolytes and thin film polymer electrolytes. Notably, the mass activities of the nanostructured electrocatalysts from alkylated block copolymer templates are 35%–94% higher than electrocatalysts from non-alkylated block copolymer templates. Standing cylinder nanostructures lead to higher mass activities than lamellar variants despite their not having the largest surface area per unit catalyst loading demonstrating that mesostructure architectures have a profound impact on reactivity. Overall, IDE chips with model thin film electrocatalysts prepared from self-assembled block copolymers offer a high-throughput experimental method for correlating electrocatalyst nanostructure and composition to electrochemical reactivity.
AB - Self-assembled block copolymers are promising templates for fabricating thin film materials with tuned periodic feature sizes and geometry at the nanoscale. Here, a series of nanostructured platinum and iridium oxide electrocatalysts templated from poly(styrene)-block-poly(vinyl pyridine) (PSbPVP) block copolymers via an incipient wetness impregnation (IWI) pathway is reported. Both nanowire and nanocylinder electrocatalysts of varying feature sizes are assessed and higher catalyst loadings are achieved by the alkylation of the pyridine moieties in the PVP block prior to IWI. Electrocatalyst evaluations featuring hydrogen pump and water electrolysis demonstrations are carried out on interdigitated electrode (IDE) chips flexible with liquid supporting electrolytes and thin film polymer electrolytes. Notably, the mass activities of the nanostructured electrocatalysts from alkylated block copolymer templates are 35%–94% higher than electrocatalysts from non-alkylated block copolymer templates. Standing cylinder nanostructures lead to higher mass activities than lamellar variants despite their not having the largest surface area per unit catalyst loading demonstrating that mesostructure architectures have a profound impact on reactivity. Overall, IDE chips with model thin film electrocatalysts prepared from self-assembled block copolymers offer a high-throughput experimental method for correlating electrocatalyst nanostructure and composition to electrochemical reactivity.
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U2 - 10.1002/smll.202100437
DO - 10.1002/smll.202100437
M3 - Article
C2 - 33991064
AN - SCOPUS:85105780386
SN - 1613-6810
VL - 17
JO - Small
JF - Small
IS - 25
M1 - 2100437
ER -