000121222 001__ 121222
000121222 005__ 20241125101128.0
000121222 0247_ $$2doi$$a10.1002/anie.202214048
000121222 0248_ $$2sideral$$a131636
000121222 037__ $$aART-2023-131636
000121222 041__ $$aeng
000121222 100__ $$aFarpón, Marcos G.
000121222 245__ $$aRhodium single-atom catalyst design through oxide support modulation for selective gas-phase ethylene hydroformylation
000121222 260__ $$c2023
000121222 5060_ $$aAccess copy available to the general public$$fUnrestricted
000121222 5203_ $$aA frontier challenge in single-atom (SA) catalysis is the design of fully inorganic sites capable of emulating the high reaction selectivity traditionally exclusive of organometallic counterparts in homogeneous catalysis. Modulating the direct coordination environment in SA sites, via the exploitation of the oxide support's surface chemistry, stands as a powerful albeit underexplored strategy. We report that isolated Rh atoms stabilized on oxygen-defective SnO2 uniquely unite excellent TOF with essentially full selectivity in the gas-phase hydroformylation of ethylene, inhibiting the thermodynamically favored olefin hydrogenation. Density Functional Theory calculations and surface characterization suggest that substantial depletion of the catalyst surface in lattice oxygen, energetically facile on SnO2, is key to unlock a high coordination pliability at the mononuclear Rh centers, leading to an exceptional performance which is on par with that of molecular catalysts in liquid media.
000121222 536__ $$9info:eu-repo/grantAgreement/ES/MICINN/FPU17-04751$$9info:eu-repo/grantAgreement/ES/MICINN/FPU17-04701$$9info:eu-repo/grantAgreement/ES/MICINN-AEI/PID2019-104739GB-I00/AEI-10.13039-501100011033$$9This project has received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement No H2020 823717-ESTEEM3$$9info:eu-repo/grantAgreement/EC/H2020/823717/EU/Enabling Science and Technology through European Electron Microscopy/ESTEEM3$$9info:eu-repo/grantAgreement/EC/ERC/2019/CoG/864195$$9info:eu-repo/grantAgreement/ES/DGA/E13-20R$$9info:eu-repo/grantAgreement/ES/AEI/PRE2019-087571$$9info:eu-repo/grantAgreement/ES/MICINN/RTI2018-096399-A-I00
000121222 540__ $$9info:eu-repo/semantics/openAccess$$aby-nc-nd$$uhttp://creativecommons.org/licenses/by-nc-nd/3.0/es/
000121222 590__ $$a16.1$$b2023
000121222 592__ $$a5.3$$b2023
000121222 591__ $$aCHEMISTRY, MULTIDISCIPLINARY$$b14 / 231 = 0.061$$c2023$$dQ1$$eT1
000121222 593__ $$aChemistry (miscellaneous)$$c2023$$dQ1
000121222 593__ $$aCatalysis$$c2023$$dQ1
000121222 594__ $$a26.6$$b2023
000121222 655_4 $$ainfo:eu-repo/semantics/article$$vinfo:eu-repo/semantics/publishedVersion
000121222 700__ $$aHenao, Wilson
000121222 700__ $$aPlessow, Philipp N.
000121222 700__ $$aAndrés, Eva
000121222 700__ $$0(orcid)0000-0002-2071-9093$$aArenal, Raúl
000121222 700__ $$aMarini, Carlo
000121222 700__ $$aAgostini, Giovanni
000121222 700__ $$aStudt, Félix
000121222 700__ $$aPrieto, Gonzalo
000121222 773__ $$g62, 1 (2023), e202214048 [9 pp.]$$pAngew. Chem. (Int. ed.)$$tAngewandte Chemie (International ed.)$$x1433-7851
000121222 8564_ $$s1281652$$uhttps://zaguan.unizar.es/record/121222/files/texto_completo.pdf$$yVersión publicada
000121222 8564_ $$s2956055$$uhttps://zaguan.unizar.es/record/121222/files/texto_completo.jpg?subformat=icon$$xicon$$yVersión publicada
000121222 909CO $$ooai:zaguan.unizar.es:121222$$particulos$$pdriver
000121222 951__ $$a2024-11-22-11:58:06
000121222 980__ $$aARTICLE