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Four unprecedented V_(14)clusters as highly efficient heterogeneous catalyst for CO_(2)fixation with epoxides and oxidation of sulfides

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Science China Chemistry 2023年第1期66卷 107-116页

作者： Ji-Lei Wang Jia-Peng Cao Yin-Hua Zhu Qin Wang Ning-Fang Li Xin-Rong Fan Hua Mei Yan Xu State Key Laboratory of Materials-Oriented Chemical Engineering College of Chemical EngineeringNanjing Tech UniversityNanjing210009China State Key Laboratory of Coordination Chemistry Coordination Chemistry InstituteNanjing UniversityNanjing 210093China

Chemical fixation of carbon dioxide(CO_(2))is an energy-saving method for alleviating the greenhouse gas emissions,whereas it persists a challenge posed by the demand for efficient ***,four unprecedented examples of tetradecanuclear vanadium clusters,namely,[(C_(2)H_(8)N_(2))6(CH_(3)O)8(CH_(3)OH)_(2)V_(10)^(Ⅳ)V_(4)ⅤO_(26)](V_(14)-1),[(C_(3)H_(10)N_(2))_(6)(CH_(3)O)_(8)(CH_(3)OH)_(2)V_(10)^(Ⅳ)V_(4)ⅤO_(26)](V14^(-2)),[(C_(6)H_(14)N_(2))6(CH_(3)O)8(CH_(3)OH)_(2)V_(10)^(Ⅳ)V_(4)ⅤO_(26)]·5H_(2)O(V14^(-3))and[(C_(4)H_(12)N_(2)O)_(4)(C_(4)H_(11)N_(2)O)_(2)(CH_(3)O)_(2)V_(10)^(Ⅳ)V_(4)ⅤO_(28)]·6H_(2)O(V_(14)-4),have been triumphantly designed and constructed under solvothermal *** them,compounds V_(14)-1–4 are the first cases of tetradecanuclear vanadium clusters without the introduction of inorganic acid radical *** main units[V_(10)^(Ⅳ)V_(4)ⅤO_(26)]8+and[V10ⅣV4ⅤO28]4+represent brand-new configurations of tetradecanuclear vanadium *** the fact that the presence of V^(Ⅳ)/V^(Ⅴ)can potentially facilitate electron transfer and consequently expedite catalytic reactions,we explored the catalytic activities of these ***,V_(14)-1 was further used as a heterogeneous catalyst in the CO_(2)fixation into cyclic carbonates under milder conditions(60℃,0.5 MPa)and exhibited higher catalytic ***,the experimental results indicated that V_(14)-1 could efficiently catalyze the sulfoxidation,which could fully convert most sulfides within 40 min at room ***,as a stable heterogeneous catalyst employed in CO_(2)fixation with epoxides and oxidation of sulfides,V_(14)-1 could be consecutively used multiple cycles without losing its catalytic activity.

关键词： V_(14)clusters heterogeneous catalyst CO_(2)fixation oxidation of sulfides

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Extending aromatic acids on TiO_(2)for cooperative photocatalysis with triethylamine:Violet light-induced selective aerobic oxidation of sulfides

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Chinese Chemical Letters 2022年第8期33卷 3733-3738页

作者： Hui Li Xia Li Jun Zhou Wenlong Sheng Xianjun Lang Sauvage Center for Molecular Sciences College of Chemistry and Molecular SciencesWuhan UniversityWuhan 430072China

Designing visible light photocatalysts with a metal oxide semiconductor as the starting material could expand a new horizon for the conversion and storage of solar ***,the benchmark photocatalyst TiO_(2) was used to pursue this goal by anchoring aromatic *** the aromatic acid was strategically deployed to design TiO_(2) complexes with violet light-induced selective aerobic oxidation of sulfide as the probe *** benzoic acid(BA)as the initial molecule,horizontally extending one or two benzene rings furnishes 2-naphthoic acid(2-NA)and 2-anthracene acid(2-AA).Moreover,triethylamine(TEA),an electron transfer mediator,was introduced to maintain the integrity of the anchored aromatic ***,there was a direct correlation between theπ-conjugation of aromatic acid ligand and the selective aerobic oxidation of *** the three aromatic acids,2-AA delivered the best result over TiO_(2) due to the most extensiveπ-conjugated ***,violet light-induced selective aerobic oxidation of sulfides into corresponding sulfoxides was conveniently realized by cooperative photocatalysis of 2-AA-TiO_(2) with 10 mol%of *** work affords an extending strategy for designing the next-generation ligands for semiconductors to expand visible light-induced selective reactions.

关键词： Aromatic acid Extendingπ-conjugation Complex photocatalyst oxidation of sulfides Cooperative photocatalysis

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Decavanadate-based Transition Metal Hybrids as Bifunctional Catalysts for Sulfide oxidation and C-C Bond Construction

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Chinese Journal of Chemistry 2021年第9期39卷 2495-2503页

作者： Xianqiang Huang Xiaoyu Gu Yuquan Qi Yanru Zhang Guodong Shen Bingchuan Yang Wenzeng Duan Shuwen Gong Zechun Xue Yifa Chen Shandong Provincial Key Laboratory of Chemical Energy Storage and Novel Cell Technology School of Chemistry&Chemical EngineeringLiaocheng UniversityLiaochengShandong 252059China Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials Jiangsu Key Laboratory of New Power BatteriesSchool of Chemistry and Materials ScienceNanjing Normal UniversityNanjingJiangsu 210023China

The development of bifunctional catalysts has drawn much attention in realizing efficient and feasible catalytic systems to meet the diverse dema nd of pote ntial industrial *** n of stable and powerful bifun ctional catalysts for various catalysis systems is highly desirable yet largely ***,three kinds of decavanadate-based transition metal hybrids(DTMH)(i.e.,Co-DTMH,Ni-DTMH and Ag-DTMH)have been successfully synthesized through a pH tuning strategy and further ***,the rare M05N six-coordinated transition metal coordination modes have been detected in Co-DTMH and Ni-DTMH,while Ag atoms in Ag-DTMH exhibited three-and five-coordinated geometries with the tuning of specially selected imidazole ***-obtained clusters can serve as powerful bifunctional catalysts for both sulfide oxidation and C-C bond ***,Ag-DTMH dem on st rated excellent heteroge ne ous bifunctional catalytic properties in the selective oxidati on of sulfides and construction of C-C bond(yields up to 99%),which enable successful recycling for three cycles with remained catalytic activities and structure *** newly designed decavanadate-based transition metal hybrids with bifunctional property hold high promise in the practical applications like continuous catalysis or flow bed reactions.

关键词： Polyoxometalates Crystal engineering Bifunctional catalysts oxidation of sulfides Heterogeneous catalysis

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