{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,9,23]],"date-time":"2026-09-23T16:05:15Z","timestamp":1790179515272,"version":"4.1.0"},"reference-count":59,"publisher":"American Chemical Society (ACS)","issue":"37","license":[{"start":{"date-parts":[[2026,9,9]],"date-time":"2026-09-09T00:00:00Z","timestamp":1788912000000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-029"},{"start":{"date-parts":[[2026,9,9]],"date-time":"2026-09-09T00:00:00Z","timestamp":1788912000000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-037"},{"start":{"date-parts":[[2026,9,9]],"date-time":"2026-09-09T00:00:00Z","timestamp":1788912000000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-045"}],"funder":[{"name":"National Key R&D Program of China","award":["2023YFA1507400"],"award-info":[{"award-number":["2023YFA1507400"]}]},{"name":"Center of High Performance Computing in Tsinghua University","id":[{"id":"https:\/\/ror.org\/03cve4549","id-type":"ROR","asserted-by":"crossref"}]},{"name":"Haihe Laboratory of Sustainable Chemical Transformations","award":["25HHWCSS00009"],"award-info":[{"award-number":["25HHWCSS00009"]}]},{"name":"Energy Revolution S&T Program of Yulin Innovation Institute of Clean Energy","award":["E511010817"],"award-info":[{"award-number":["E511010817"]}]},{"name":"National Natural Science Foundation of China (NSFC)","award":["22325805"],"award-info":[{"award-number":["22325805"]}],"id":[{"id":"https:\/\/ror.org\/01h0zpd94","id-type":"ROR","asserted-by":"crossref"}]},{"name":"National Natural Science Foundation of China (NSFC)","award":["22441010"],"award-info":[{"award-number":["22441010"]}],"id":[{"id":"https:\/\/ror.org\/01h0zpd94","id-type":"ROR","asserted-by":"crossref"}]},{"name":"National Natural Science Foundation of China (NSFC)","award":["22521202"],"award-info":[{"award-number":["22521202"]}],"id":[{"id":"https:\/\/ror.org\/01h0zpd94","id-type":"ROR","asserted-by":"crossref"}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":[],"published-print":{"date-parts":[[2026,9,23]]},"abstract":"<jats:title>Abstract<\/jats:title>\n                  <jats:p>Heterolytic hydrogenation via hydride species transfer represents a fundamental transformation in industry for chemical synthesis, but H2 or organic hydride donors are often utilized as the hydrogen source. An electrochemical palladium (Pd) membrane reactor shows the ability to catalyze heterolytic reactions by using water as the hydrogen source, but quantitative descriptions of this reactivity remain absent, and the reaction often relies on external polarization of the chemical compartment. Herein, we report thermochemical polarization-driven heterolytic hydrogenation in an electrochemical Pd-membrane reactor. By employing Hantzsch ester (HEH) regeneration as a model reaction, we first established a quantitative thermodynamic framework by showing basicity-dependent activity, and then provided experimental evidence supporting the kinetics by observing an interfacial charge transfer process, together demonstrating a heterolytic hydrogenation mechanism. Moreover, the origin of the electrons that generate hydride species was supported by experimental evidence using mixed potential theory (MPT)\u2500a theory widely applied in metal corrosion and thermal catalysis but rarely applied to electrochemical systems. As a proof of concept, by employing the regenerated HEH as a mediator, we achieved asymmetric hydrogenation of imines with high yield (up to 99.1%) and enantioselectivity (up to 98.1% e.e.), thus demonstrating the integration of electrochemical hydrogen generation with homogeneous asymmetric catalysis. This work provides a mechanistic foundation for heterolytic hydrogenation in a Pd-membrane reactor and inspires the rational design of catalyst modifications.<\/jats:p>","DOI":"10.1021\/jacs.6c08382","type":"journal-article","created":{"date-parts":[[2026,9,10]],"date-time":"2026-09-10T02:02:05Z","timestamp":1789005725000},"page":"39623-39637","source":"Crossref","is-referenced-by-count":0,"title":["Thermochemical Polarization-Driven\nHeterolytic Hydrogenation\nin an Electrochemical Palladium-Membrane Reactor"],"prefix":"10.1021","volume":"148","author":[{"given":"Kejian","family":"Kong","sequence":"first","affiliation":[{"name":"Tsinghua University , , ,","place":["Beijing, China, 100084"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Huilin","family":"Zheng","sequence":"additional","affiliation":[{"name":"Tsinghua University , , ,","place":["Beijing, China, 100084"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hedan","family":"Liu","sequence":"additional","affiliation":[{"name":"Tsinghua University , , ,","place":["Beijing, China, 100084"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0003-2233-7499","authenticated-orcid":true,"given":"Xiang","family":"Liu","sequence":"additional","affiliation":[{"name":"Tsinghua University , , ,","place":["Beijing, China, 100084"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yu-Wen","family":"Sun","sequence":"additional","affiliation":[{"name":"Tsinghua University , , ,","place":["Beijing, China, 100084"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8528-8514","authenticated-orcid":true,"given":"Bi-Jie","family":"Li","sequence":"additional","affiliation":[{"name":"Tsinghua University , , ,","place":["Beijing, China, 100084"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9241-0984","authenticated-orcid":true,"given":"Haohong","family":"Duan","sequence":"additional","affiliation":[{"name":"Tsinghua University , , ,","place":["Beijing, China, 100084"]},{"name":"Haihe Laboratory of Sustainable Chemical Transformations , ,","place":["Tianjin, China, 300192"]},{"name":"Tsinghua University , , ,","place":["Beijing, China, 100084"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,9,9]]},"reference":[{"issue":"3","key":"2026092311084690500_cit1","doi-asserted-by":"publisher","first-page":"1103","DOI":"10.1021\/acs.chemrev.2c00550","article-title":"Hydrogenation of Carboxylic Acids,\nEsters, and Related Compounds over Heterogeneous Catalysts: A Step\ntoward Sustainable and Carbon-Neutral Processes","volume":"123","author":"Qu","year":"2023","journal-title":"Chem. 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Application to\nan Oxygen Evolution Catalyst","volume":"10","author":"Costentin","year":"2020","journal-title":"ACS Catal."},{"issue":"9","key":"2026092311084690500_cit3","doi-asserted-by":"publisher","first-page":"8594","DOI":"10.1021\/acs.chemrev.1c00905","article-title":"Designing\nSites in Heterogeneous Catalysis: Are We Reaching Selectivities Competitive\nWith Those of Homogeneous Catalysts?","volume":"122","author":"Zaera","year":"2022","journal-title":"Chem.\nRev."},{"issue":"20","key":"2026092311084690500_cit4","doi-asserted-by":"publisher","first-page":"10921","DOI":"10.1021\/jp502309r","article-title":"Homolytic\nProducts from Heterolytic Paths in H2 Dissociation on Metal\nOxides: The Example of CeO2","volume":"118","author":"Garci\u0301a-Melchor","year":"2014","journal-title":"J. Phys.\nChem. 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