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Here we report a thermodynamically coupled strategy that integrates endothermic cyclohexane dehydrogenation with exothermic CO2 hydrogenation, enabling thermodynamically compensated aromatization under mild conditions. Using a tandem Pd@S-1 and ZnZrOx\/ZSM-5 catalyst, cyclohexane dehydrogenation, CO2 activation, and methanol-mediated alkylation are synergistically coupled within a hydrogen-shuttling network. Under continuous-flow conditions (370 \u00b0C, 3 MPa), the system achieves 99% cyclohexane conversion and 99% aromatics selectivity with 38% CO2 conversion. Operando X-ray absorption spectroscopy (XAS) reveals dynamic Pd0\/PdO interconversion, while Zn\u2013O\u2013Zr sites remain structurally stable to facilitate CO2 activation. 13CO2 isotopic tracing confirms direct incorporation of CO2-derived carbon into aromatic products. This work establishes a hydrogen shuttle-enabled thermochemical paradigm for coupling endothermic and exothermic reactions, offering an energy-efficient route for naphthene upgrading and CO2 valorization.<\/jats:p>","DOI":"10.1021\/jacs.6c13315","type":"journal-article","created":{"date-parts":[[2026,8,22]],"date-time":"2026-08-22T09:57:10Z","timestamp":1787392630000},"page":"37466-37476","source":"Crossref","is-referenced-by-count":0,"title":["Self-Sustained Hydrogen\nRelay Enables Thermodynamically\nCoupled Cyclohexane-CO2 Conversion to Aromatics over Tandem\nCatalysts"],"prefix":"10.1021","volume":"148","author":[{"given":"Haohao","family":"Feng","sequence":"first","affiliation":[{"name":"Dalian Institute of Chemical Physics, Chinese Academy of Sciences , , ,","place":["Dalian, China, 116023"]},{"name":"University of Chinese Academy of Sciences, Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jingyi","family":"Zhu","sequence":"additional","affiliation":[{"name":"Dalian Institute of Chemical Physics, Chinese Academy of Sciences , , ,","place":["Dalian, China, 116023"]},{"name":"University of Chinese Academy of Sciences, Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhong-Pan","family":"Hu","sequence":"additional","affiliation":[{"name":"Dalian Institute of Chemical Physics, Chinese Academy of Sciences , , ,","place":["Dalian, China, 116023"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Enze","family":"Chen","sequence":"additional","affiliation":[{"name":"Dalian Institute of Chemical Physics, Chinese Academy of Sciences , , ,","place":["Dalian, China, 116023"]},{"name":"University of Chinese Academy of Sciences, Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7775-4183","authenticated-orcid":true,"given":"Jingfeng","family":"Han","sequence":"additional","affiliation":[{"name":"Dalian Institute of Chemical Physics, Chinese Academy of Sciences , , ,","place":["Dalian, China, 116023"]},{"name":"Dalian Institute of Chemical Physics, Chinese Academy of Sciences , , ,","place":["Dalian, China, 116023"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0412-1980","authenticated-orcid":true,"given":"Yingxu","family":"Wei","sequence":"additional","affiliation":[{"name":"Dalian Institute of Chemical Physics, Chinese Academy of Sciences , , ,","place":["Dalian, China, 116023"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7999-2940","authenticated-orcid":true,"given":"Zhongmin","family":"Liu","sequence":"additional","affiliation":[{"name":"Dalian Institute of Chemical Physics, Chinese Academy of Sciences , , ,","place":["Dalian, China, 116023"]},{"name":"University of Chinese Academy of Sciences, Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]},{"name":"Dalian Institute of Chemical Physics, Chinese Academy of Sciences , , ,","place":["Dalian, China, 116023"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,21]]},"reference":[{"issue":"1","key":"2026090312090939600_cit1","doi-asserted-by":"publisher","first-page":"67","DOI":"10.1080\/01614947208076866","article-title":"Catalytic Naphtha Reforming","volume":"5","author":"Ciapetta","year":"1972","journal-title":"Catal. 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