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However, high-current-density operation relies on catalysts that sustain fast kinetics and high selectivity under strong interfacial gradients. Electro-oxidized lignin is employed to construct a lignin-metal supramolecular framework composite, which upon carbonization yields RuNi@NOLC, a Ni-enriched RuNi alloy confined within an oxygen-enriched, nitrogen-doped lignin-derived carbon (NOLC) microenvironment. In a membrane-free flow electrolyzer using RuNi@NOLC as both cathode and anode catalysts, the coupled process achieves a specific energy consumption of 0.76 kWh Nm\u20133 H2, a formate Faradaic efficiency of 99.5%, and an apparent hydrogen Faradaic efficiency of 199.6% arising from dual-compartment hydrogen generation and collection. The NOLC microenvironment provides Donnan hydration with a hydration-funnel effect, enabling directional enrichment of H2O together with OH\u2013 at N-containing sites and stabilization of the transition configuration for water splitting, thereby markedly accelerating the Ni-centered Volmer step as the rate-determining process and establishing a 3-fold synergy of Ni-centered water activation, Ru-mediated hydrogen release, and NOLC-directed transport of water and hydroxide. Under formaldehyde oxidation bias, Ru\u2013OH and RuOxH species dominate low-potential initiation. Assisted by neighboring Ni\u2013OHads, these Ru-centered oxygenated species drive intermediates toward OCHO formation and formate production, while alloy electronic effects mitigate poisoning by strongly adsorbed intermediates before transport limitations prevail at higher potentials. This work converts the coordination-chemistry programmability of lignin into quantifiable interfacial-solvation advantages, providing a clear paradigm for understanding and designing microenvironment-dominated mechanisms in paired electrolysis.<\/jats:p>","DOI":"10.1021\/jacs.6c07813","type":"journal-article","created":{"date-parts":[[2026,7,27]],"date-time":"2026-07-27T12:35:48Z","timestamp":1785155748000},"page":"32219-32231","source":"Crossref","is-referenced-by-count":8,"title":["Interfacial\nDonnan Hydration Funnels in Lignin-Derived\nCarbon Orchestrate RuNi Synergy for Aldehyde-Assisted Dual-Hydrogen\nElectrosynthesis"],"prefix":"10.1021","volume":"148","author":[{"given":"Jianglin","family":"Liu","sequence":"first","affiliation":[{"name":"Guangdong University of Technology , , ,","place":["Guangzhou, China, 510006"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dalang","family":"Chen","sequence":"additional","affiliation":[{"name":"Guangdong University of Technology , , ,","place":["Guangzhou, China, 510006"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chongyi","family":"Dong","sequence":"additional","affiliation":[{"name":"Guangdong University of Technology , , ,","place":["Guangzhou, China, 510006"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fangbao","family":"Fu","sequence":"additional","affiliation":[{"name":"Guangdong University of Technology , , ,","place":["Guangzhou, China, 510006"]},{"name":"Guangdong Provincial Laboratory of Chemistry and Fine Chemical Engineering Jieyang Center , ,","place":["Jieyang, China, 515200"]},{"name":"Guangdong University of Technology , , ,","place":["Guangzhou, China, 510006"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3043-0821","authenticated-orcid":true,"given":"Yanlin","family":"Qin","sequence":"additional","affiliation":[{"name":"Guangdong University of Technology , , ,","place":["Guangzhou, China, 510006"]},{"name":"Guangdong Provincial Laboratory of Chemistry and Fine Chemical Engineering Jieyang Center , ,","place":["Jieyang, China, 515200"]},{"name":"Guangdong University of Technology , , ,","place":["Guangzhou, China, 510006"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2170-5985","authenticated-orcid":true,"given":"Xuliang","family":"Lin","sequence":"additional","affiliation":[{"name":"Guangdong University of Technology , , ,","place":["Guangzhou, China, 510006"]},{"name":"Guangdong Provincial Laboratory of Chemistry and Fine Chemical Engineering Jieyang Center , ,","place":["Jieyang, China, 515200"]},{"name":"Guangdong University of Technology , , ,","place":["Guangzhou, China, 510006"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8765-7061","authenticated-orcid":true,"given":"Xueqing","family":"Qiu","sequence":"additional","affiliation":[{"name":"Guangdong University of Technology , , ,","place":["Guangzhou, China, 510006"]},{"name":"Guangdong Provincial Laboratory of Chemistry and Fine Chemical Engineering Jieyang Center , ,","place":["Jieyang, China, 515200"]},{"name":"Guangdong University of Technology , , ,","place":["Guangzhou, China, 510006"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,7,27]]},"reference":[{"key":"2026080511143005600_cit1a","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-022-28260-5","article-title":"Electrode reconstruction strategy\nfor oxygen evolution reaction: maintaining Fe-CoOOH phase with intermediate-spin\nstate during electrolysis","volume":"13","author":"Lee","year":"2022","journal-title":"Nat. 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