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Selenium vacancies regulate d-band centers in Ni_(3)Se_(4)toward paired electrolysis in anion-exchange membrane electrolyzers for upgrading N-containing compounds

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Science China Chemistry 2023年第7期66卷 2109-2120页

作者： Feng Yue Chuantao Wang Wen Duan Huijuan Pang Tingting Wei Kaixin Xue Danjun Wang Feng Fu Chunming Yang Research Institute of Comprehensive Energy Industry Technology College of Chemistry&Chemical EngineeringYan’an UniversityYan’an 716000China

paired electrolysis in anion-exchange membrane(AEM)electrolyzers toward the cathodic nitrate reduction reaction(NO_(3)RR)and anodic benzylamine oxidation reaction(BOR)could generate high value-added N-containing compounds *** key challenge is to develop bifunctional electrocatalysts with a wide potential window,which can achieve highly efficient conversion of anode and cathode ***,Ni_(3)Se_(4)with Se vacancies was prepared and employed as the cathode and anode of AEM electrolyzers for NO_(3)RR and BOR.^(15)N isotope-labeling online differential electrochemical mass spectrometry(DEMS)proved that ammonium was reduced from nitrates and revealed the reaction pathway of NO_(3)*** density functional theory calculation clarified that Se vacancies regulate d-band centers,and then further modulate the adsorption energy of adsorbed hydrogen,NO_(3)^(-)and intermediates on the Ni_(3)Se_(4)-60s surface in NO_(3)RR,so as to optimize the hydrogenation of NO_(3)^(-)into ***,during the BOR,the Se vacancy can promote the adsorption of OH^(-),which is easier to form the active species of Ni *** technical and economic evaluation exhibited that the cost of paired electrolysis is 1.21 times lower and the profit is 1.42 times higher than that of the unpaired electrolysis,which shows the economic attraction of paired *** work delivers the guidance for the design of efficient catalysts for paired electrolysis in AEM electrolyzer toward the sustainable synthesis of value-added chemicals.

关键词： Ni_(3)Se_(4) controllable selenium vacancy paired electrolysis AEM electrolyzer upgrading N-containing compounds

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Catalyst-Dependent Direct and Deoxygenative Coupling of Alcohols by Convergent paired electrolysis

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CCS Chemistry 2022年第6期4卷 1938-1948页

作者： Sheng Zhang Jianxue Shi Jingjing Li Man-Bo Li Guigen Li Michael Findlater Institute of Physical Science and Information Technology Anhui UniversityHefeiAnhui 230601 College of Chemistry and Pharmaceutical Engineering Nanyang Normal UniversityNanyang Institute of Chemistry and Biomedical Sciences School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210093 Department of Chemistry and Biochemistry Texas Tech UniversityLubbockTX 79423 Department of Chemistry and Biochemistry University of CaliforniaMercedCA 95343

Developing a general and mild approach to upgrade alcohols into high value products is a hot topic in synthetic chemistry because alcohol is one of the most abundant raw ***,direct coupling and deoxygenative coupling of alcohols are the two main approaches for the functionalization of alcohols to afford structurally diverse products,and it receives considerable *** significant advances in the field,there still remains a great challenge to develop a general approach accommodating both coupling reactions,as they commonly involve distinct ***,we report an electrochemical approach for the direct coupling and deoxygenative coupling of alcohols with *** paired electrolysis,this catalyst-dependent protocol gives divergent access to diols and tertiary ***,the synthetic utility of 9H-fluoren-9-ol products has been demonstrated in the synthesis of organic luminophores,phenanthrol,phenanthridine,and amino *** present approach exhibits some impressive features:(a)catalystdependent selectivity;(b)excellentfunctional-group tolerance(156 examples);(c)mild conditions;and(d)good scalability(∼20 gram scale).

关键词： paired electrolysis deoxygenative coupling direct coupling catalyst-dependent selectivity

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基于成对电解和光催化协同作用的镍催化环烷醇的芳基化反应

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Science Bulletin 2024年第12期69卷 1866-1874页

作者：刘昭然朱萧谕郭剑峰马聪左智伟梅天胜 State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of SciencesShanghai 200032China

The merging of transition metal catalysis with electrochemistry has become a powerful tool for organic synthesis because catalysts can govern the reactivity and ***,coupling catalysts with alkyl radical species generated by anodic oxidation remains challenging because of electrode passivation,dimerization,and *** this study,we developed convergent paired electrolysis for the coupling of nickel catalysts with alkyl radicals derived from photoinduced ligand-to-metal charge-transfer of cyclic alcohols and iron catalysts,providing a practical method for site-specific and remote arylation of *** synergistic use of photocatalysis with convergent paired electrolysis can provide alternative avenues for metal-catalyzed radical coupling reactions.

关键词： Organic electrochemistry Electrophotocatalysis paired electrolysis Ni catalysis Remote arylation

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The synergism of sequential paired electrosynthesis with halogen bonding activation for the cyclization of organochlorides with olefins

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Science China Chemistry 2023年第2期66卷 540-547页

作者： Fei Lian Kun Xu Chengchu Zeng Faculty of Environment and Life Beijing University of TechnologyBeijing100124China

Reported herein is the design of a new catalytic paradigm by synergistically combining sequential paired electrosynthesis with halogen-bonding(XB)activation for the cyclization of organochlorides with *** dual activation strategy enables rapid access to densely functionalized 2-alkylidene-tetrahydrofurans with exclusive Z-selectivities,which are challenging to be synthesized by other methods.4,4′-Di-tert-butyl-2,2′-bipyridine(dtbbpy)showed an unprecedented reactivity as a XB acceptor to activate C-Cl bond by shifting its reduction potential positively by 220 m *** different from previous electroreductions of C-Cl bonds relying upon high electrode potentials or matched redox properties between mediators and organochlorides,the XB activator employed herein has no limit on the abovementioned redox property matching but can lower the applied electrode *** decreased operating potential allows broad functional group tolerance,which was highlighted by the late-stage functionalization of 11 examples of drugs and natural products-derived alkenes.

关键词： electrochemistry cross-electrophile coupling electrocatalysis paired electrolysis

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Molecularly Dispersed Heterogenized Metallomacrocycles:Molecular Structure Sensitivity of CO_(2) electrolysis

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CCS Chemistry 2023年第8期5卷 1827-1840页

作者： Dong-Dong Ma Shu-Guo Han Sheng-Hua Zhou Wen-Bo Wei Xiaofang Li Bo Chen Xin-Tao Wu Qi-Long Zhu State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of Sciences(CAS)Fuzhou 350002Fujian Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108Fujian University of Chinese Academy of Sciences Beijing 100049 Department of Chemistry City University of Hong KongHong Kong 999077

Revealing the structure-performance relationships of the molecularly dispersed heterogenized metallomacrocycles(MDHMs)withπ-conjugated heterojunctions is of great,yet largely unmet,significance for realizing the rational regulation of selectivity,Faradaic efficiency,and durability in the electrochemical CO_(2) reduction reaction(CO_(2)RR).Herein,we describe new insights into the molecularstructure sensitivity of the electrochemical CO_(2)RR over the MDHMs through peripherally functionalizing the heterogenized nickel phthalocyanines with diverse methylimidazole *** studied experimentally and theoretically,the heterointerfacial effect and self-built microenvironment of the MDHMs are significantly modulated by accurate structural clipping at the molecular level,predominately steering their electrocatalytic performance for CO_(2)-to-CO conversion in both H-type and flow electrolytic ***,the optimized MDHM,2MIMCβNiPc/CNT,displays a significantly improved electrocatalytic performance for CO_(2)RR with near-unity Faradaic efficiency and large current ***,the paired electrolysis systems with the MDHMs as the multifunctional electrocatalysts was developed for making full use of the anodic and cathodic reactions,which shows a new and profitable prospect for energy optimization,pollutant regeneration,and green electrosynthesis in a modular form,and also provides guidance for the design and synthesis of novel effi-cient yet economical electrocatalysts.

关键词： metallomacrocycles π-conjugated heterojunctions carbon nanotubes CO_(2)electroreduction molecular structure sensitivity paired electrolysis

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Electrochemical Umpolung Enabled Radical-Radical Cross-Coupling Between Electron-Deficient Methylarenes and Aldehydes

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CCS Chemistry 2023年第9期5卷 1973-1981页

作者： Fei Lian Kun Xu Chengchu Zeng Faculty of Environment and Life Beijing University of TechnologyBeijing 100124

The electrochemical utilization of electron-deficient methylarenes for radical-radical cross-couplings remains very *** by an umpolung strategy,the unprecedented electrochemical cross-coupling of electron-deficient methylarenes with aldehydes was *** paired electrolysis simultaneously generated electron-deficient benzylic radicals and ketyl radicals at both electrodes,which then underwent radical recombination,governed by polarity matching and persistent-radical effect(PRE)to afford functionalized alcohols that are not easily accessible by other *** protocol features catalystand external redox agent-free conditions and a formal 100%atom *** studies support the radical-radical cross-coupling pathway.

关键词： paired electrolysis ketyl radical umpolung radical-radical cross-coupling methylarene aldehyde

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Merging electrolysis and Nickel Catalysis in Redox Neutral Cross-Coupling Reactions:Experiment and Computation for Electrochemically Induced C–P and C–Se Bonds Formation

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CCS Chemistry 2020年第2期2卷 179-190页

作者： Chen Zhu Huifeng Yue Pavlo Nikolaienko Magnus Rueping KAUST Catalysis Center(KCC) King Abdullah University of Science and Technology(KAUST)Thuwal 23955-6900Saudi Arabia

We have achieved a nickel-catalyzed cross-coupling reaction via concerted paired electrolysis under mild reaction *** this electrochemical transformation,the anodic oxidation of NiII to NiIII and cathodic reduction of NiI to Ni0 occurred simultaneously,resulting in an economical and sustainable cross-coupling ***,weperformed mechanistic investigations,achieved by experiments and density functional theory(DFT)calculations for different C–heteroatom bond formations to reveal the catalytic cycle in more detail.

关键词： nickel catalysis paired electrolysis redox neutral cross-coupling C–P bond formation C–Se bond formation aryl halides DFT calculations

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