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Metal\u2010free carbon catalysts, featuring tunable structures, readily available precursors, and excellent stability, have garnered significant attention for sustainable H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    production. However, despite extensive investigations, the precise mechanisms underlying catalytic selectivity on these carbon materials remain unclear and highly debated. Previous mechanistic interpretations frequently attribute catalytic activity to specific oxygen functional groups or heteroatom dopants through correlation\u2010driven hypotheses and simplified theoretical models. Such approaches often overlook the intrinsic complexity of carbon surfaces, where multiple variables, including dopant types, defect structures, surface groups, and hybridization states, coexist and interact simultaneously, leading to contradictory conclusions. This review critically examines\u00a0the limitations of these traditional approaches and emphasize the need of systematic experimental designs that independently vary structural parameters, along with advanced analytical methods capable of resolving active\u2010site ambiguity, are critically reviewed. Recent developments employing orthogonal material libraries, rigorous experimental controls, catalyst passport metadata, and advanced multivariate and meta\u2010analytical tools have emerged as robust frameworks for bias\u2010resistant catalyst design. Integrating explainable and generative machine learning models with operando spectroscopy provides a robust, end\u2010to\u2010end approach for identifying and validating accurate catalytic descriptors.\n                  <\/jats:p>","DOI":"10.1002\/adma.70122","type":"journal-article","created":{"date-parts":[[2025,10,17]],"date-time":"2025-10-17T07:19:07Z","timestamp":1760685547000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":17,"title":["Beyond Presumptions: Toward Mechanistic Clarity in Metal\u2010Free Carbon Catalysts for Electrochemical H\n                    <sub>2<\/sub>\n                    O\n                    <sub>2<\/sub>\n                    Production via Data Science"],"prefix":"10.1002","volume":"37","author":[{"given":"Dayu","family":"Zhu","sequence":"first","affiliation":[{"name":"School of Chemistry Monash University  Clayton Melbourne VIC 3800 Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hsi\u2010wen","family":"Wu","sequence":"additional","affiliation":[{"name":"School of Chemistry Monash University  Clayton Melbourne VIC 3800 Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiao","family":"Wang","sequence":"additional","affiliation":[{"name":"School of Chemistry Monash University  Clayton Melbourne VIC 3800 Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2493-5209","authenticated-orcid":false,"given":"Jie","family":"Zhang","sequence":"additional","affiliation":[{"name":"School of Chemistry Monash University  Clayton Melbourne VIC 3800 Australia"},{"name":"ARC Research Hub for Carbon Utilisation and Recycling Monash University  Clayton VIC 3800 Australia"},{"name":"ARC Centre of Excellence for Green Electrochemical Transformation of Carbon Dioxide Monash University  Clayton VIC 3800 Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,10,17]]},"reference":[{"key":"e_1_2_8_1_1","doi-asserted-by":"crossref","DOI":"10.5040\/9798400605284","volume-title":"The 100 Most Important Chemical Compounds: A Reference Guide","author":"Myers R. 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