Isolated Co-Ti-Y Trimetallic Synergistic Catalysis Based on Apparent Anti-Electronegative Polarization

Yu Qiu; Chongchong Wu; Ian Donald GatesYuanxi YangShuhai GuoZhuowu MenBin LouXiujie YangNan ShiFushan WenChanglong YinJiashun ZhouBen LiWeichao ChouDong Liu

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Isolated Co-Ti-Y Trimetallic Synergistic Catalysis Based on Apparent Anti-Electronegative Polarization

机译：Isolated Co-Ti-Y Trimetallic Synergistic Catalysis Based on Apparent Anti-Electronegative Polarization

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Rational design of multimetallic synergistic catalysis is a grand challenge inthe field of green catalysis because synergistic mechanisms are poorly understood.Here, by exploiting a unique apparent anti-electronegativity polarizationin cobalt-titanium-yttrium trimetallic synergy, a unified methodology isdemonstrated to activate oxygen and nitrogen. The new trimetallic synergisticcatalyst achieves direct solvent-free aerobic oxidation of cyclohexaneto adipic acid and direct nitrogen oxidation of acetonitrile to guanidine. Thedelocalization of d-orbitals and activation of inner electrons are the linchpinsof catalytic performance, contributing to 90.87% selectivity for ketone-alcoholoil and adipic-acid and 89.30% selectivity for guanidine, respectively. Theexperiments and calculations demonstrate that the prodigious electrophilicityof the yttrium site overcomes the homeostasis of valence shell structures inthe isolated cobalt and titanium sites. The valence electrons of this synergisticsystem become enriched with anti-electronegative polarization andconcomitant high charge transfer efficiency. In response to urging sustainablechemistry, the results corroborate that the activation strategies and mechanismsof molecular oxygen and nitrogen can be moderated and unified whenmultimetallic synergy is considered.

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《Advanced functional materials》 |2022年第43期|2207482.1-2207482.13|共13页
作者
Yu Qiu; Chongchong Wu; Ian Donald GatesYuanxi YangShuhai GuoZhuowu MenBin LouXiujie YangNan ShiFushan WenChanglong YinJiashun ZhouBen LiWeichao ChouDong Liu;
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作者单位

CenerTech Tianjin Chemical Research and Design Institute Co. LtdTianjin 300131, China;

State Key Laboratory of Heavy Oil Processing, Department of Chemistryand Chemical EngineeringChina University of Petroleum (East China)Qingdao 266580, China;

Department of Chemical and Petroleum EngineeringUniversity of CalgaryAlberta T2N1N4, Canada CNOOC Research Institute of Refining and PetrochemicalsBeijing 102200, ChinaDepartment of Chemical and Petroleum EngineeringUniversity of CalgaryAlberta T2N1N4, CanadaDepartment of Chemical EngineeringUniversity College LondonTorrington Place, London WC1E7JE, UKInstitute of Applied EcologyChinese Academy of SciencesShenyang 110016, ChinaNational Institute of Clean and Low-Carbon EnergyBeijing 102211, China;

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正文语种英语
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adipic acid; anti-electronegativity; nitrogen activation; synergistic catalysis; trimetallic catalysts;

Isolated Co-Ti-Y Trimetallic Synergistic Catalysis Based on Apparent Anti-Electronegative Polarization

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