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Here, we propose an electric double layer (EDL)-programmable nucleic-acid interfacial switch on metal\u2013organic framework (MOF) interfaces. In this system, EDL-mediated interfacial stabilization, andcoordination anchoring at coordinatively unsaturated metal sites retain probes and posthybridization duplexes within a near-surface quenching region, producing a stable signal-off state. Increasing ionic strength and introducing competitive polyphosphate anions (PPi\/STPP) weaken interfacial anchoring and trigger release of the complexes into the surrounding solution, thereby generating a signal-on response. Based on this mechanism, we developed two complementary miRNA assays: a MIL-101(Cr)-based multiplex fluorescence platform with quencher strands to suppress background, and a Zn2Ph2Da-enabled duplex-release strategy that generates DNA templates for extraction-free, reverse-transcription-free one-step qPCR with a detection limit of 10\u201318 M. Both readouts discriminated liver cancer patients from healthy controls in plasma, demonstrating the potential of EDL-programmable interfacial chemistry for miRNA analysis.<\/jats:p>","DOI":"10.1021\/acs.analchem.6c03060","type":"journal-article","created":{"date-parts":[[2026,8,18]],"date-time":"2026-08-18T15:16:39Z","timestamp":1787066199000},"page":"25133-25145","source":"Crossref","is-referenced-by-count":0,"title":["Programmable\nElectric Double Layer at Metal\u2013Organic\nFramework Interfaces for miRNA Resolution"],"prefix":"10.1021","volume":"98","author":[{"given":"Zhen","family":"Song","sequence":"first","affiliation":[{"name":"China Pharmaceutical University , , ,","place":["Nanjing, China, 210009"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yi-Hui","family":"Wang","sequence":"additional","affiliation":[{"name":"China Pharmaceutical University , , ,","place":["Nanjing, China, 210009"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jing-Yi","family":"Wang","sequence":"additional","affiliation":[{"name":"China Pharmaceutical University , , ,","place":["Nanjing, China, 210009"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yue","family":"Lin","sequence":"additional","affiliation":[{"name":"China Pharmaceutical University , , ,","place":["Nanjing, China, 210009"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3802-5698","authenticated-orcid":true,"given":"Jin-Long","family":"Chen","sequence":"additional","affiliation":[{"name":"China Pharmaceutical University , , ,","place":["Nanjing, China, 210009"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7892-018X","authenticated-orcid":true,"given":"Huai-Song","family":"Wang","sequence":"additional","affiliation":[{"name":"China Pharmaceutical University , , ,","place":["Nanjing, China, 210009"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,18]]},"reference":[{"issue":"48","key":"2026090306472819200_cit1","doi-asserted-by":"publisher","first-page":"17834","DOI":"10.1021\/acs.analchem.3c03914","article-title":"Integrating reliable\nPt\u2013S bond-mediated 3D DNA nanomachine\nwith magnetic separation in a homogeneous electrochemical strategy\nfor exosomal microRNA detection with low background and high sensitivity","volume":"95","author":"Yang","year":"2023","journal-title":"Anal. 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Bioelectron."},{"key":"2026090306472819200_cit28","doi-asserted-by":"publisher","DOI":"10.1016\/j.bios.2020.112832","article-title":"Nucleic acid-functionalized\nmetal-organic\nframework for ultrasensitive immobilization-free photoelectrochemical\nbiosensing","volume":"173","author":"Liu","year":"2021","journal-title":"Biosens. Bioelectron."},{"key":"2026090306472819200_cit29","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2022.135296","article-title":"Fluorescent oligonucleotide\nindicators for ratiometric microRNA sensing on metal-organic frameworks","volume":"437","author":"Wang","year":"2022","journal-title":"Chem. Eng. J."},{"issue":"11","key":"2026090306472819200_cit30","doi-asserted-by":"publisher","first-page":"7605","DOI":"10.1021\/acs.jmedchem.3c00499","article-title":"Visual and electrochemical\ndetection\nof let-7a: a tumor suppressor and biomarker","volume":"66","author":"Song","year":"2023","journal-title":"J. Med. 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