Electrolysis on a Chip with Tunable Thin Film Nanostructured PGM Electrocatalysts Generated from Self-Assembled Block Copolymer Templates

Deepra Bhattacharya; Subarna Kole; Orhan Kizilkaya; Joseph Strzalka; Polyxeni P. Angelopoulou; Georgios Sakellariou; Dongmei Cao; Christopher G. Arges

doi:10.1002/smll.202100437

Electrolysis on a Chip with Tunable Thin Film Nanostructured PGM Electrocatalysts Generated from Self-Assembled Block Copolymer Templates

Deepra Bhattacharya, Subarna Kole, Orhan Kizilkaya, Joseph Strzalka, Polyxeni P. Angelopoulou, Georgios Sakellariou, Dongmei Cao, Christopher G. Arges

Research output: Contribution to journal › Article › peer-review

15 Scopus citations

Abstract

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.

Original language	English
Article number	2100437
Journal	Small
Volume	17
Issue number	25
DOIs	https://doi.org/10.1002/smll.202100437
State	Published - Jun 24 2021
Externally published	Yes

Funding

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.

Keywords

block copolymers
electrocatalysts
hydrogen pumps
platinum group metals
water electrolysis

Access to Document

10.1002/smll.202100437

Cite this

@article{0b1d398ee3bb4c03b3d7ddfd60cc7392,

title = "Electrolysis on a Chip with Tunable Thin Film Nanostructured PGM Electrocatalysts Generated from Self-Assembled Block Copolymer Templates",

abstract = "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.",

keywords = "block copolymers, electrocatalysts, hydrogen pumps, platinum group metals, water electrolysis",

author = "Deepra Bhattacharya and Subarna Kole and Orhan Kizilkaya and Joseph Strzalka and Angelopoulou, \{Polyxeni P.\} and Georgios Sakellariou and Dongmei Cao and Arges, \{Christopher G.\}",

note = "Publisher Copyright: {\textcopyright} 2021 Wiley-VCH GmbH",

year = "2021",

month = jun,

day = "24",

doi = "10.1002/smll.202100437",

language = "English",

volume = "17",

journal = "Small",

issn = "1613-6810",

publisher = "wiley",

number = "25",

}

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.

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.

KW - block copolymers

KW - electrocatalysts

KW - hydrogen pumps

KW - platinum group metals

KW - water electrolysis

UR - https://www.scopus.com/pages/publications/85105780386

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 -

Electrolysis on a Chip with Tunable Thin Film Nanostructured PGM Electrocatalysts Generated from Self-Assembled Block Copolymer Templates

Abstract

Funding

Keywords

Access to Document

Other files and links

Fingerprint

Cite this