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However, a systematic understanding of the HBN and the establishment of predictive descriptors remain lacking, which hinders the rational design of effective electrochemical systems. In this work, two descriptors, hydrogen bond (HB) strength and HB number, are introduced to characterize the flexibility and connectivity of the HBN, respectively. By adding a series of urea derivatives to the electrolyte, both HB strength and HB number can be continuously tuned, enabling precise modulation of HBN flexibility and connectivity. By only varying the HBN properties, the current density, Faradaic efficiency for multicarbon products (FEC2+), and the FEC2H4\/FEC2H5OH ratio can be modulated from 0.38 to 0.81 A cm\u20132, 48.2% to 90.5%, and 1.04 to 2.45, respectively. A direct and predictive link between HBN properties and CO2RR performance is established. An optimal HBN stabilizes the key *CO intermediate through water-mediated hydrogen bonding, thereby enhancing C\u2013C coupling. A highly connected network favors ethylene production, while a flexible HBN promotes ethanol formation. Consequently, the reactivity, FEC2+, and the ethylene\/ethanol ratio can all be tuned by adjusting the properties of the HBN.<\/jats:p>","DOI":"10.1021\/jacs.6c14000","type":"journal-article","created":{"date-parts":[[2026,10,9]],"date-time":"2026-10-09T04:01:54Z","timestamp":1791518514000},"page":"44679-44687","source":"Crossref","is-referenced-by-count":0,"title":["Hydrogen\nBond Network Descriptors Dictate Reactivity\nand Selectivity of CO2 Electroreduction"],"prefix":"10.1021","volume":"148","author":[{"given":"Jiahao","family":"Yang","sequence":"first","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]},{"name":"University of Chinese Academy of Sciences , , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shiju","family":"Yu","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]},{"name":"University of Chinese Academy of Sciences , , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiapeng","family":"Jiao","sequence":"additional","affiliation":[{"name":"Xi\u2019an Polytechnic University , , ,","place":["Xi\u2019an, China, 710048"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shiqiang","family":"Liu","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Lanzhou, China, 730000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Meng","family":"Zhou","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]},{"name":"University of Chinese Academy of Sciences , , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yiyong","family":"Wang","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]},{"name":"University 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100190"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Huisheng","family":"Qin","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]},{"name":"University of Chinese Academy of Sciences , , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ke","family":"Li","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]},{"name":"University of Chinese Academy of Sciences , , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yanjia","family":"Wang","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]},{"name":"University of Chinese Academy of Sciences , , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Rongjuan","family":"Feng","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8730-8486","authenticated-orcid":true,"given":"Qinggong","family":"Zhu","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]},{"name":"University of Chinese Academy of Sciences , , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8108-0975","authenticated-orcid":true,"given":"Yi","family":"Xu","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]},{"name":"University of Chinese Academy of Sciences , , ,","place":["Beijing, China, 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U.S.A."},{"issue":"42","key":"2026102111091981600_cit32","doi-asserted-by":"publisher","first-page":"13291","DOI":"10.1021\/jp4037217","article-title":"Structure\nand Dynamics of Urea\/Water Mixtures Investigated by Vibrational Spectroscopy\nand Molecular Dynamics Simulation","volume":"117","author":"Carr","year":"2013","journal-title":"J. Phys.\nChem. B"},{"issue":"22","key":"2026102111091981600_cit33","doi-asserted-by":"publisher","first-page":"6220","DOI":"10.1021\/jp066474n","article-title":"Aqueous Urea\nSolutions: Structure, Energetics, and\nUrea Aggregation","volume":"111","author":"Stumpe","year":"2007","journal-title":"J. Phys. Chem. B"},{"issue":"6","key":"2026102111091981600_cit34","doi-asserted-by":"publisher","first-page":"689","DOI":"10.1038\/s41929-024-01162-z","article-title":"Modulating\nWater Hydrogen Bonding within a Non-Aqueous\nEnvironment Controls its Reactivity in Electrochemical Transformations","volume":"7","author":"Gomes","year":"2024","journal-title":"Nat. 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