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DOE OSTI · 3408250

Rigor and Reproducibility in Electrocatalysis: Best Practices for Operando Studies

Tackett, Brian M. [Purdue University, West Lafayette, IN (United States)] (ORCID:0000000259965339)·Schreier, Marcel [University of Wisconsin−Madison, WI (United States)] (ORCID:0000000236745667)·Clark, Ezra L. [Pennsylvania State University, University Park, PA (United States)] (ORCID:0000000204351276)·Jahrman, Evan P. [National Institute of Standards and Technology, Gaithersburg, MD (United States)] (ORCID:0000000295900057)·Seitz, Linsey C. [Northwestern University, Evanston, IL (United States)] (ORCID:0000000168316747)·Hoffman, Adam S. [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000276824108)·Chang, Qiaowan [Washington State University, Pullman, WA (United States)] (ORCID:0000000317652331)·Bare, Simon R. [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000249320342)·Chen, Jingguang G. [Columbia University, New York, NY (United States)] (ORCID:0000000295922635)·Waegele, Matthias M. [Boston College, Chestnut Hill, MA (United States)] (ORCID:0000000211867545)·Corson, Elizabeth R. [University of Kansas, Lawrence, KS (United States)] (ORCID:000000032722674X)·Hall, Anthony Shoji [University of Pennsylvania, Philadelphia, PA (United States)] (ORCID:0000000341344160)·Kim, Sungin [Cornell University, Ithaca, NY (United States)] (ORCID:0000000191070781)·Jiang, Jiahong [Cornell University, Ithaca, NY (United States)] (ORCID:0009000487502560)·Yang, Yao [Cornell University, Ithaca, NY (United States)] (ORCID:0000000303213792)·Raciti, David [National Institute of Standards and Technology, Gaithersburg, MD (United States)] (ORCID:0000000295804524)
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Abstract

Operando measurements have rapidly expanded the scope of electrocatalysis by enabling direct observation of catalytic interfaces under working conditions and by linking structural, compositional, and spectroscopic observables to activity and selectivity. However, the growth of operando methods has outpaced the adoption of broadly shared experimental standards, creating persistent challenges in reproducibility, interpretation, and comparison across laboratories and platforms. This perspective synthesizes discussions from the 2025 National Science Foundation Workshop on Rigor and Reproducibility in Electrocatalysis and outlines a practical framework for the rigorous use of operando measurements in electrocatalysis. We highlight three recurring needs: careful implementation of complex methods to avoid overinterpretation; recognition that (subtle) differences in reactor architecture, hydrodynamics, and electrical boundary conditions can alter apparent kinetics and selectivity; and transparent reporting standards that enable meaningful cross-comparison without constraining measurement-specific cell innovation. Focusing on widely used techniques (including X-ray and vibrational spectroscopies, mass spectrometry, and electron microscopy), we discuss technique-specific pitfalls, cross-validation strategies, and recurring platform-agnostic considerations such as mass transport, current distribution, temporal-resolution mismatches, and catalyst evolution. This Perspective aims to strengthen the mechanistic inference and improve the reproducibility, comparability, and predictive value of operando electrocatalysis research.

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X-ray absorption spectroscopyelectrocatalysiselectrochemical mass spectrometryin situ characterizationoperando electrocatalysisoperando spectroscopyreproducibilityvibrational spectroscopy

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Tackett, Brian M. [Purdue University, West Lafayette, IN (United States)] (ORCID:0000000259965339), Schreier, Marcel [University of Wisconsin−Madison, WI (United States)] (ORCID:0000000236745667), Clark, Ezra L. [Pennsylvania State University, University Park, PA (United States)] (ORCID:0000000204351276), Jahrman, Evan P. [National Institute of Standards and Technology, Gaithersburg, MD (United States)] (ORCID:0000000295900057), Seitz, Linsey C. [Northwestern University, Evanston, IL (United States)] (ORCID:0000000168316747), Hoffman, Adam S. [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000276824108), Chang, Qiaowan [Washington State University, Pullman, WA (United States)] (ORCID:0000000317652331), Bare, Simon R. [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000249320342), Chen, Jingguang G. [Columbia University, New York, NY (United States)] (ORCID:0000000295922635), Waegele, Matthias M. [Boston College, Chestnut Hill, MA (United States)] (ORCID:0000000211867545), Corson, Elizabeth R. [University of Kansas, Lawrence, KS (United States)] (ORCID:000000032722674X), Hall, Anthony Shoji [University of Pennsylvania, Philadelphia, PA (United States)] (ORCID:0000000341344160), Kim, Sungin [Cornell University, Ithaca, NY (United States)] (ORCID:0000000191070781), Jiang, Jiahong [Cornell University, Ithaca, NY (United States)] (ORCID:0009000487502560), Yang, Yao [Cornell University, Ithaca, NY (United States)] (ORCID:0000000303213792), Raciti, David [National Institute of Standards and Technology, Gaithersburg, MD (United States)] (ORCID:0000000295804524). 2026-07-09. Rigor and Reproducibility in Electrocatalysis: Best Practices for Operando Studies. https://doi.org/10.1021/acscatal.6c01946

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