Operando Magnetic Resonance Imaging for Visualizing Electrochemical Triple‐Phase Boundary
Abstract
Abstract The triple‐phase boundary (TPB) is a complex interface where gas, liquid, and solid phases converge, crucially regulating the efficiency and performance of many electrochemical devices including fuel cells and batteries. However, conventional characterization techniques struggle to capture the dynamic processes and flooding at TPB. To address this, we develop operando electrochemical magnetic resonance imaging (EC‐MRI), an inherently non‐invasive technique sensitive to 1 H, which probes both bulk and boundary regions, enabling real‐time visualization of TPB evolution and a deeper understanding of its function at the device level under operational conditions. In a study of proton exchange membrane fuel cell (PEMFC), with a focus on the kinetically sluggish O 2 reduction reaction in the cathode, operando EC‐MRI quantitatively illustrates the interplay between power output, water content, and TPB evolution. It reveals that the TPB maps undergo significant spatial and dynamic variations, with TPB deterioration, rather than apparent water accumulation, directly triggering flooding, as proved using catalysts with different water generation and adsorption capabilities. Our finding opens new perspectives on water management and TPB design, with potential applications in other critical electrochemical processes such as H 2 oxidation, CO 2 reduction, and N 2 reduction, underscoring the value of operando EC‐MRI for real‐time diagnostics of electrochemical devices.
Article Details
Authors (16)
Wen‐Long Jiang
State Key Laboratory of Physical Chemistry of Solid Surfaces MOE Key Laboratory of Spectrochemical Analysis & Instrumentation Fujian Provincial Key Laboratory of Plasma and Magnetic Resonance School of Electronic Science and Engineering College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 P.R. China
Shuo‐Hui Cao
State Key Laboratory of Physical Chemistry of Solid Surfaces MOE Key Laboratory of Spectrochemical Analysis & Instrumentation Fujian Provincial Key Laboratory of Plasma and Magnetic Resonance School of Electronic Science and Engineering College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 P.R. China
Chun‐Yu Qiu
State Key Laboratory of Physical Chemistry of Solid Surfaces MOE Key Laboratory of Spectrochemical Analysis & Instrumentation Fujian Provincial Key Laboratory of Plasma and Magnetic Resonance School of Electronic Science and Engineering College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 P.R. China
Hui‐Jun Sun
State Key Laboratory of Physical Chemistry of Solid Surfaces MOE Key Laboratory of Spectrochemical Analysis & Instrumentation Fujian Provincial Key Laboratory of Plasma and Magnetic Resonance School of Electronic Science and Engineering College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 P.R. China
Li‐Na Wang
State Key Laboratory of Physical Chemistry of Solid Surfaces MOE Key Laboratory of Spectrochemical Analysis & Instrumentation Fujian Provincial Key Laboratory of Plasma and Magnetic Resonance School of Electronic Science and Engineering College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 P.R. China
Jun‐Bo Sheng
State Key Laboratory of Physical Chemistry of Solid Surfaces MOE Key Laboratory of Spectrochemical Analysis & Instrumentation Fujian Provincial Key Laboratory of Plasma and Magnetic Resonance School of Electronic Science and Engineering College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 P.R. China
Li‐Fei Ji
State Key Laboratory of Physical Chemistry of Solid Surfaces MOE Key Laboratory of Spectrochemical Analysis & Instrumentation Fujian Provincial Key Laboratory of Plasma and Magnetic Resonance School of Electronic Science and Engineering College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 P.R. China
Shuo Liu
Zu‐Rong Ni
State Key Laboratory of Physical Chemistry of Solid Surfaces MOE Key Laboratory of Spectrochemical Analysis & Instrumentation Fujian Provincial Key Laboratory of Plasma and Magnetic Resonance School of Electronic Science and Engineering College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 P.R. China
Shu‐Hu Yin
School of Microelectronics and School of Integrated Circuits Nantong University Nantong 226019 P.R. China
Xiao‐Ping Zhang
State Key Laboratory of Physical Chemistry of Solid Surfaces MOE Key Laboratory of Spectrochemical Analysis & Instrumentation Fujian Provincial Key Laboratory of Plasma and Magnetic Resonance School of Electronic Science and Engineering College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 P.R. China
Yan‐Xia Jiang
State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical Engineering Xiamen University Xiamen P. R. China
Yu‐Cheng Wang
State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical Engineering Xiamen University Xiamen China
Zhi‐You Zhou
State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical Engineering Xiamen University Xiamen China
Zhong Chen
Shi‐Gang Sun
State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical Engineering Xiamen University Xiamen P. R. China