Unveiling Key Descriptors of Ionomer Materials for Enhanced Electrochemical CO₂ Reduction

Wonsang Jung; Sang-Hun Shin; Sejin Park; Younghyun Chae; Ung Lee; Hye Jin Cho; Sungjun Kim; Yun Jeong Hwang; Jang Yong Lee; Da Hye Won

doi:10.1021/acsenergylett.4c03009

journal article·2025-01-10

Unveiling Key Descriptors of Ionomer Materials for Enhanced Electrochemical CO₂ Reduction

Wonsang Jung, Sang-Hun Shin, Sejin Park, Younghyun Chae, Ung Lee, Hye Jin Cho, Sungjun Kim, Yun Jeong Hwang, Jang Yong Lee, Da Hye Won

ACS Energy Letters· Volume 10· Issue 1

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Source abstract

Abstract

Polymeric ionomers near the catalyst surface of CO 2 reduction reaction (CO 2 RR) electrodes affect their efficiency; however, their multifaceted properties complicate structure–activity relationship elucidation. Here, we synthesized polycarbazole-based anion-exchange (QPC) ionomers bearing varying functionalized side chains to explore this relationship. Comprehensive analysis in physicochemical properties, electrochemical activity, and operando ATR-SEIRAS revealed that functional group modification significantly influenced the intrinsic ionomer properties, thereby affecting the Ag catalyst properties, microenvironments of interfacial water structures, and reaction kinetics of the protonation step for CO 2 RR and the hydrogen evolution reaction (HER). Notably, the QPC-trimethyl phosphonium (TMP) ionomer induced favorable interfacial water structures, having a high proportion of strong H-bonded water with low Stark tuning slopes, which inhibit HER and promote CO 2 RR. A high CO Faradaic efficiency (>90%) was maintained using QPC-TMP in a membrane electrode assembly, even under varying CO 2 concentrations (100–15%) and elevated temperatures (28–72 °C). These findings suggest that the catalytic environment can be optimized by fine-tuning the ionomer structure, contributing to the advancement of high-performance CO 2 RR ionomers.

Source: openalex_inverted_index · Quality: baseline

Research context

Polymers Catalysis & surfaces

OpenAlex topics: Fuel Cells and Related Materials · CO2 Reduction Techniques and Catalysts · Advanced battery technologies research

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Clean Energy Research Center, Korea Institute of Science and Technology (KIST), Seoul 02792, Republic of Korea

Division of Energy and Environmental Technology, KIST School, Korea University of Science and Technology (UST), Seoul 02792, Republic of Korea

Industrial Gas Research Cell, Research Institute of Industrial Science & Technology (RIST), 187-12, Geumho-ro, Gwangyang-si, Jeollanam-do 57801, Republic of Korea

Hydrogen Energy Research Center, Korea Research Institute of Chemical Technology (KRICT), Daejeon 34114, Republic of Korea

Department of Chemistry, Seoul National University, Seoul 08826, Republic of Korea

Graduate School of Energy and Environment (Green School), Korea University, Seoul 02841, Republic of Korea

Center for Nanoparticle Research, Institute for Basic Science (IBS), Seoul 08826, Republic of Korea

Department of Chemical Engineering, Konkuk University, Seoul 05029, Republic of Korea

KHU-KIST Department of Converging Science and Technology, Kyung Hee University, Seoul 02477, Republic of Korea

Funding

National Research Foundation of Korea · Seoul National University · Korea Institute of Science and Technology (KIST)

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