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oai:riubu.ubu.es:10259/119932026-09-04T00:05:27Zcom_10259_4323com_10259_5086com_10259_2604col_10259_4330

Huerta Sainz, Sergio de la 845 600 0000-0002-6843-1419 Santamaría, Sara 8bff5459-1fc0-4f40-a32d-72450ce58f7f 500 Escobedo Monge, María Antonieta 20eb83ad-5b66-4ddb-867c-f559b00ebda7 600 Trenzado, José L. 96a154ce-8edf-4ac8-9b59-2a3061ab858c 500 Diez Cabanes, Valentin de6f08a3-922f-4441-b35a-ae2da8240e5c 600 Gutiérrez Vega, Alberto 271 600 0000-0003-2000-7413 Marcos Villa, Pedro A. 336 600 0000-0002-6890-8088 Bol Arreba, Alfredo 70 600 0000-0003-4641-4826 Atilhan, Mert 51023856-6e72-4667-b27a-fe52e5115d61 600 Aparicio Martínez, Santiago 30 600 0000-0001-9996-2426 2026-09-03T10:07:52Z 2026-09-03T10:07:52Z 2026-07 2470-1343 https://hdl.handle.net/10259/11993 10.1021/ACSOMEGA.6C02376 2470-1343 Deep eutectic solvents (DESs) owe their remarkable melting-point depression, high viscosity, and tunable solvation to a hydrogen-bond network far richer than the binary donor–acceptor picture suggests. This study advances the framework of competitive hydrogen-bond partitioning: ionic Cl–···H–X interactions, neutral donor–donor self-association, cation-mediated contacts, and water-competitive motifs coexist and continuously redistribute as a function of composition, temperature, and interfacial confinement. Evidence is synthesized from vibrational spectroscopy, multinuclear NMR, neutron and X-ray scattering, dielectric relaxation, classical and ab initio molecular dynamics, DFT cluster calculations, and machine-learning potentials, establishing that no single technique can fully characterize the network─a triangulation criterion requiring at least two independent method categories is essential. A quantitative structure–property framework is developed linking six hydrogen-bond descriptors─motif population, persistence distribution, network connectivity, competitive hydration index, dynamic heterogeneity, and interfacial partitioning─to viscosity, conductivity, diffusion, and glass transition across Type III, Type V, Natural DES (NADES), and hydrophobic DES. A central finding is the cooperativity–mobility tradeoff: cooperative charge spreading at Cl– simultaneously drives eutectic depression and network rigidity, defining a design axis along which DES can be rationally positioned. Water is analyzed as both competitive and cooperative partner across four hydration regimes, and interfacial hydrogen-bond reorganization at electrodes─largely neglected in prior studies─is critically examined. An integrated characterization workflow with standardized reporting criteria, validated force-field benchmarks, and data-driven descriptors for predictive screening is proposed. This work has been funded by Agencia Estatal de Investigación (Project NADESforPFAS, ref.: PID2022-142405OB-I00) and Junta de Castilla y León (Project NADES4NATURE, ref.: BU047P23). application/pdf eng ACS Publications ACS Omega. 2026, V. 11, n. 26, p. 38868–38891 https://doi.org/10.1021/acsomega.6c02376?urlappend=%3Fref%3DPDF&jav=VoR&rel=cite-as Atribución 4.0 Internacional http://creativecommons.org/licenses/by/4.0/ info:eu-repo/semantics/openAccess Mathematical methods Viscosity Solvents Physical and chemical properties Noncovalent interactions Hidrógeno Disolventes Hydrogen Solvents Competitive Hydrogen-Bond Partitioning in Deep Eutectic Solvents: From Cooperative Charge Spreading to Structure–Property Design Rules info:eu-repo/semantics/article info:eu-repo/semantics/publishedVersion ACS Omega 11 26 38868 38891 THUMBNAIL Huerta-ACSO_2026.pdf.jpg Huerta-ACSO_2026.pdf.jpg IM Thumbnail image/jpeg 5436 https://riubu.ubu.es/bitstream/10259/11993/4/Huerta-ACSO_2026.pdf.jpg 64d942e11cf695b685b9facc7bdb1e39 MD5 4 LICENSE license.txt license.txt text/plain; charset=utf-8 998 https://riubu.ubu.es/bitstream/10259/11993/3/license.txt aa90105e1c90a1b4fe810649aa967b7d MD5 3 CC-LICENSE license_rdf license_rdf application/rdf+xml; charset=utf-8 908 https://riubu.ubu.es/bitstream/10259/11993/2/license_rdf 0175ea4a2d4caec4bbcc37e300941108 MD5 2 ORIGINAL Huerta-ACSO_2026.pdf Huerta-ACSO_2026.pdf application/pdf 5838260 https://riubu.ubu.es/bitstream/10259/11993/1/Huerta-ACSO_2026.pdf c3450b78672c53ab00fbff77e8f84982 MD5 1 10259/11993 oai:riubu.ubu.es:10259/11993 2026-09-04 02:05:27.643 Repositorio Institucional de la Universidad de Burgos bubrep@ubu.es RWwgYXV0b3IgY29tbyDDum5pY28gdGl0dWxhciBkZSBsb3MgZGVyZWNob3MgZGUgcHJvcGllZGFkIGludGVsZWN0dWFsIGRlIGxhIG9icmEsIG8gZGlzcG9uaWVuZG8gZGUgbG9zIGRlYmlkb3MgcGVybWlzb3MgZGUgbG9zIG90cm9zIHRpdHVsYXJlcywgc2kgbG9zIGh1YmllcmEsIHkgZW4gdmlydHVkIGRlIGxvcyBkZXJlY2hvcyBxdWUgbGUgY29uZmllcmUgbGEgbGVnaXNsYWNpw7NuIHZpZ2VudGUgc29icmUgcHJvcGllZGFkIGludGVsZWN0dWFsIHkgZGVyZWNob3MgZGUgYXV0b3IsIA0KQVVUT1JJWkEgYSBsYSBVbml2ZXJzaWRhZCBkZSBCdXJnb3MgYSBkaWZ1bmRpciwgZGUgbWFuZXJhIGdyYXR1aXRhLCBlbCBjb250ZW5pZG8gZGUgbG9zIGFyY2hpdm9zIGRpZ2l0YWxlcyBxdWUgY29ycmVzcG9uZGVuIGFsIGRvY3VtZW50byBkZXNjcml0byBhbnRlcmlvcm1lbnRlLCBjb24gY2Fyw6FjdGVyIG5vIGV4Y2x1c2l2byB5IGRlIG1hbmVyYSBww7pibGljYSBlbiBhY2Nlc28gYWJpZXJ0byBhIHRyYXbDqXMgZGUgSW50ZXJuZXQsIHBhcmEgbG8gcXVlIGxhIEJpYmxpb3RlY2EgcHJvY2VkZXLDoSBhIGFyY2hpdmFybG9zIGVuIGVsIFJlcG9zaXRvcmlvIEluc3RpdHVjaW9uYWwuIEFzaW1pc21vIGF1dG9yaXphIGEgbGEgVW5pdmVyc2lkYWQgZGUgQnVyZ29zIGEgcmVhbGl6YXIgbGFzIHRyYW5zZm9ybWFjaW9uZXMgbmVjZXNhcmlhcyBkZSBmb3JtYXRvLCBubyBkZSBjb250ZW5pZG8sIHBhcmEgZ2FyYW50aXphciBsYSBwcmVzZXJ2YWNpw7NuIHkgZWwgYWNjZXNvIGVuIGVsIGZ1dHVyby4NCg0KRWwgYXV0b3IgZGlzcG9uZSwgZW4gdG9kbyBjYXNvLCBkZWwgZGVyZWNobyBhIHJldm9jYXIgZXN0YSBhdXRvcml6YWNpw7NuLg0KDQpMYSBjZXNpw7NuIGRlIGRlcmVjaG9zIGRlIGVzdGEgb2JyYSBzZSBlbmN1ZW50cmEgc3VqZXRhIGEgbGEgbGVnaXNsYWNpw7NuIHZpZ2VudGUgc29icmUgcHJvcGllZGFkIGludGVsZWN0dWFsIHkgZGVyZWNob3MgZGUgYXV0b3I=