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Cu_(1)-B dual-active sites catalysts for the efficient dehydrogenative coupling and CO_(2)electroreduction

Nano Research 2023年第4期16卷 4582-4588页

作者： Konglin Wu Zhaobin Fang Cheng Peng Yining Zhang Binbin Jiang Yanshang Kang Zhiming Chen Mingfu Ye Yuxi Wu Xianwen Wei Shoujie Liu Sha Li Jian Zhang Key Laboratory of Metallurgical Emission Reduction&Resources Recycling of Ministry of Education Anhui University of TechnologyMaanshan 243002China Anhui Laboratory of Clean Catalytic Engineering School of Chemical and Environmental EngineeringAnhui Polytechnic UniversityWuhu 241000China Institute of Clean Energy and Advanced Nanocatalysis(iClean) School of Chemistry and Chemical EngineeringAnhui University of TechnologyMaanshan 243002China Chemistry and Chemical Engineering Guangdong Laboratory Shantou 515063China Institute of Molecular Plus Tianjin UniversityTianjin 300072China School of Chemistry and Chemical Engineering Anqing Normal UniversityAnqing 246001China Jiangxi Province Engineering Research Center of Ecological Chemical Industry Jiujiang UniversityJiujiang 332005China College of Chemistry and Materials Engineering Wenzhou UniversityWenzhou 325035China

Dual-active sites(DASs)catalysts have positive potential applications in broad fields because of their specific active sites and synergistic catalytic effects.Therefore,the controllable synthesis and finely regulating the activity of such catalysts has become a hot research area for now.In this work,we developed a pyrolysis-etching-hydrogen activation strategy to prepare the DASs catalysts involving single-atom Cu and B on N-doped porous carbon material(Cu_(1)-B/NPC).Numerous systematic characterization and density functional theoretical(DFT)calculation results showed that the Cu and B existed as Cu-N4 porphyrinlike unit and B-N_(3)unit in the obtained catalyst.DFT calculations further revealed that single-atom Cu and B sites were linked by bridging N atoms to form the Cu_(1)-B-N6 dual-sites.The Cu_(1)-B/NPC catalyst was more effective than the single-active site catalysts with B-N_(3)sites in NPC(B/NPC)and Cu-N4 porphyrin-like sites in NPC(Cu_(1)/NPC),respectively,for the dehydrogenative coupling of dimethylphenylsilane(DiMPSH)with various alcohols,performing the great activity(>99%)and selectivity(>99%).The catalytic performances of the Cu_(1)-B/NPC catalyst remained nearly unchanged after five cycles,also indicating its outstanding recyclability.DFT calculations showed that the Cu_(1)-B-N6 dual-sites exhibited the lowest energy profile on the potential energy surface than that of sole B-N_(3)and Cu-N4 porphyrin-like sites.Furthermore,the rate-limiting step of dehydrogenation of DiMPSH on Cu_(1)-B-N6 dual-sites also showed a much lower activation energy than the other two single sites.Benefitting from the superiority of the Cu_(1)-B-N6 dual-sites,the Cu_(1)-B/NPC catalyst can also be used for CO_(2)electroreduction to produce syngas.Thus,DASs catalysts are promising to achieve multifunctional catalytic properties and have aroused positive attention in the field of catalysis.

关键词： dual-active sites single-atom catalysis porous carbon dehydrogenative coupling

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Electrode material promoted dehydrogenative homo-/cross-coupling of weakly activated naphthalenes

绿色合成与催化(英文)

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绿色合成与催化(英文) 2023年第1期4卷 71-75页

作者： Siyuan Liu Yi Lua Siying Sun Hong Wang Wei Gao Yuying Wang Xiaofei Jia Jianbin Chen Shandong Provincial Key Laboratory of Molecular Engineering State Key Laboratory of Biobased Material and Green PapermakingSchool of Chemistry and Chemical EngineeringQilu University of Technology(Shandong Academy of Sciences)Jinan 250353China Key Laboratory of Optic-electric Sensing and Analytical Chemistry for Life Science MOECollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China

Herein,we reported an electrochemical dehydrogenative homo-/cross-coupling of weakly activated naphthalene in the exogenous transition metal-and oxidants-free manner.Benefiting from the microscopic interaction between the reactants and the carbon plate anode,the electropolymerization of aromatic rings was suppressed.And a series of binaphthyl and naphthalene-aryl privileged scaffolds were obtained in 28%–90%yields by homo-or cross-coupling.This C(sp2)-H activation strategy featured atom and step economy as well as the ready scalability.

关键词： Electrosynthesis dehydrogenative coupling Weakly activated naphthalene Anode material tuning High efficiency

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Metal-Free 12-Catalyzed Highly Selective dehydrogenative coupling of Alcohols and Cyclohexenones

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Chinese Journal of Chemistry 2018年第3期36卷 233-240页

作者： Yu-Feng Liang Yizhi Yuan Tao Shen Song Song Ning Jiao State Key Laboratory of Natural and Biomimetic Drugs School of Pharmaceutical Sciences Peking University Xue Yuan Rd. 38 Beijing 100191 China State Key Laboratory of Elemento-Organic Chemistry Nankai University Weijin Road 94 Tianjin 300071 China

The l2 catalyzed highly selective oxidatve condensation of cydohexenones and alcohols for the synthesis of aryl atkyl ethers has been described. DMSO is employed as the mild terminal oxidant. This novel methodology offers a metal-free reaction condition, operational simplicity and broad substrate scope to afford valuable products from inexpensive reagents. Various meta-substituted aromatic ethers which are hardly synthesized from the reported methods requiring meta-substituted phenols, are efficiently prepared by the present protocol.

关键词： metal-free dehydrogenative coupling oxidation selectivity alcohols

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Thermocatalytic Dehydrogenation-Enabled Arene-Alkane couplings

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Chinese Journal of Chemistry 2023年第16期41卷 1905-1914页

作者： Feng Yu Renqing Tao Lan Gan Hao Ni Qi-Kai Kang Guixia Liu Zheng Huang Chang-Kung Chuang Institute East China Normal UniversityShanghai 200062China The State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of Sciences345 Lingling RoadShanghai 200032China School of Chemistry and Material Sciences Hangzhou Institute of Advanced StudyUniversity of Chinese Academy of Sciences1 Sub-lane XiangshanHangzhouZhejiang 310024China

Comprehensive Summary The direct use of non-prefunctionalized arene and alkane as the starting materials to construct Caryl−Calkyl bond is an unfulfilled target and approaches to this challenge rarely surface in methodology studies.Current methods for thermocatalytic arene-alkane couplings(AAC)occur with specific substrates and/or inconvenient reagents.Herein,we report a one-pot relay bicatalysis system for AAC involving(pincer)Ir-catalyzed alkane transfer dehydrogenation and Fe(OTf)3-catalyzed olefin hydroarylation.This system exhibits broad scope and is particularly effective for alkylation of arenes with arylalkanes to form 1,1-diarylalkanes with high chemo-and regioselectivity,making it potentially useful for late-stage alkylation of complex molecules.Experimental mechanistic data provide a view into the factors controlling the regioselectivity.Finally,the strategy of dehydrogenation-enabled arene-alkane couplings has been successfully extended to a tandem catalysis by using a heterogeneous olefin hydroarylation catalyst.

关键词： Alkanes Arenes dehydrogenative coupling Hydroarylation lridium

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Reoxidation of Transition-metal Catalysts with O2

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Chinese Journal of Chemistry 2017年第9期35卷 1349-1365页

作者： Xinyao Li Ning Jiao State Key Laboratory of Natural and Biomimetic Drugs School of Pharmaceutical Sciences Peking University Xue Yuan Rd. 38 Beijing 100191 China State Key Laboratory of Organometallic Chemistry Chinese Academy of Sciences Shanghai 200032 China

Transition-metal catalyzed oxidation reactions are central components of organic chemistry. On behalf of green and sustainable chemistry, molecular oxygen （02） has been considered as an ideal oxidant due to its natu... 详细信息

关键词： transition-metal catalysts molecular oxygen aerobic oxidation oxygenation dehydrogenative coupling

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