Education2002-2006 B.S. Xiamen University 2006-2010 Ph.D. Washington University in St. Louis (Supervisor: Prof. Kevin D, Moeller)Experience2011-2013 Postdoctoral Researcher, Department of Chemistry, Yale University...Education2002-2006 B.S. Xiamen University 2006-2010 Ph.D. Washington University in St. Louis (Supervisor: Prof. Kevin D, Moeller)Experience2011-2013 Postdoctoral Researcher, Department of Chemistry, Yale University, USA (with Prof. ]onathan A. Ellman) 2013-2014 Associate Professor, Department of Chemistry, Xiamen University 2014-present Professor, Department of Chemistry, Xiamen University展开更多
Implementing a new energy-saving electrochemical synthesis system with high commercial value is a strategy of the sustainable development for upgrading the bulk chemicals preparation technology in the future.Here,we r...Implementing a new energy-saving electrochemical synthesis system with high commercial value is a strategy of the sustainable development for upgrading the bulk chemicals preparation technology in the future.Here,we report a multiple redox-mediated linear paired electrolysis system,combining the hydrogen peroxide mediated cathode process with the I2 mediated anode process,and realize the conversion of furfural to furoic acid in both side of the dividedflow cell simultaneously.By reasonably controlling the cathode potential,the undesired water splitting reaction and furfural reduction side reactions are avoided.Under the galvanostatic electrolysis,the two-mediated electrode processes have good compatibility,which reduce the energy consumption by about 22%while improving the electronic efficiency by about 125%.This system provides a green electrochemical synthesis route with commercial prospects.展开更多
An electrochemical synthesis of functionalized (aza)indolines through dehydrogenative [3+2] annulation of arylamines with tethered alkenes has been developed. Previous reported syntheses through similar inter- and ...An electrochemical synthesis of functionalized (aza)indolines through dehydrogenative [3+2] annulation of arylamines with tethered alkenes has been developed. Previous reported syntheses through similar inter- and intramolecular annulation reactions required noble-metal catalysts and are mostly limited to terminal alkenes or 1,3-dienes. The electrosynthesis employs the easily available and inexpensive ferrocene as the molecular catalyst and is compatible with di-, tri- and even tetrasubstituted alkenes to construct indolines as well as the more challenging azaindolines. Employing the newly developed electrosynthesis as a key step, the total synthesis of marine alkaloid (+)-hinckdentine A has been achieved in 12 steps (longest linear sequence) from commercially available materials.展开更多
Organic electrosynthesis has been widely used as an environmentally conscious alternative to conventional methods for redox reactions because it utilizes electric current as a traceless redox agent instead of chemical...Organic electrosynthesis has been widely used as an environmentally conscious alternative to conventional methods for redox reactions because it utilizes electric current as a traceless redox agent instead of chemical redox agents. Indirect electrolysis employing a redox catalyst has received tremendous attention, since it provides various advantages compared to direct electrolysis. With indirect electrolysis, overpotential of electron transfer can be avoided, which is inherently milder, thus wide functional group tolerance can be achieved. Additionally, chemoselectivity, regioselectivity, and stereoselectivity can be tuned by the redox catalysts used in indirect electrolysis. Furthermore, electrode passivation can be avoided by preventing the formation of polymer films on the electrode surface. Common redox catalysts include N-oxyl radicals, hypervalent iodine species, halides, amines, benzoquinones(such as DDQ and tetrachlorobenzoquinone), and transition metals. In recent years, great progress has been made in the field of indirect organic electrosynthesis using transition metals as redox catalysts for reaction classes including C–H functionalization, radical cyclization, and cross-coupling of aryl halides-each owing to the diverse reactivity and accessible oxidation states of transition metals. Although various reviews of organic electrosynthesis are available, there is a lack of articles that focus on recent research progress in the area of indirect electrolysis using transition metals, which is the impetus for this review.展开更多
Although the combination of electrochemistry and homogeneous catalysis has proven to be a powerful strategy for achieving a diverse array of novel transformations,some challenges such as controlling the diffusion of c...Although the combination of electrochemistry and homogeneous catalysis has proven to be a powerful strategy for achieving a diverse array of novel transformations,some challenges such as controlling the diffusion of catalyst-related species and the instability of catalysts at electrodes remain to be overcome.Herein,we review recent advances in electrochemical homogeneous catalysis,focusing on electrochemical noble-transition-metal catalysis,photoelectrochemical catalysis,and electrochemical enantioselective catalysis.The topics discussed include:(1)how the noblemetal catalystworks in the presence of cathodic hydrogen evolution,(2)how the photocatalyst gets enhanced redox property,and(3)how the enantioselectivity is regulated in a catalytic electrochemical reaction.展开更多
Summary of main observation and conclusion An electrochemical synthesis of oxazol-2-ones and imidazol-2-ones has been developed via 5-exo-dig cyclization of propargylic carbamates-and ureas-derived amidyl radicals.The...Summary of main observation and conclusion An electrochemical synthesis of oxazol-2-ones and imidazol-2-ones has been developed via 5-exo-dig cyclization of propargylic carbamates-and ureas-derived amidyl radicals.The electrosynthesis relies on the dual function of 2,2,66-tetramethylpiperidin-1-y oxyl(TEMPO)as a redox mediator for amidyl radical formation and an oxygen atom donor.The reactions are conducted under mild conditions using a simple setup and provide convenient access to functionalized oxazol-2-ones and imidazol-2-ones from readily available materials.展开更多
Dehydrogenative cyclization of thioamides is an attractive approach for the synthesis of S-heterocycles.Reported herein is an electrochemical dehydrogenative cyclization reaction of N-benzyl thioamides in a flow elect...Dehydrogenative cyclization of thioamides is an attractive approach for the synthesis of S-heterocycles.Reported herein is an electrochemical dehydrogenative cyclization reaction of N-benzyl thioamides in a flow electrolysis cell.The continuous-flow electrosynthesis has addressed the limitations associated with previously reported methods for the cyclization of alkylthioamides and provide a transition metal-and oxidizing reagent-free access to various functionalized 1,3-benzothiazines in good yields.展开更多
Acridinium dyes have been broadly used as photocatalysts,but it remains synthetically challenging to fine-tune their catalytic performance by functionalization of their structural cores.Acridinium photocatalysts are u...Acridinium dyes have been broadly used as photocatalysts,but it remains synthetically challenging to fine-tune their catalytic performance by functionalization of their structural cores.Acridinium photocatalysts are usually prepared through de novo synthesis,which involves difficult steps and requires sensitive organometallic reagents.展开更多
文摘Education2002-2006 B.S. Xiamen University 2006-2010 Ph.D. Washington University in St. Louis (Supervisor: Prof. Kevin D, Moeller)Experience2011-2013 Postdoctoral Researcher, Department of Chemistry, Yale University, USA (with Prof. ]onathan A. Ellman) 2013-2014 Associate Professor, Department of Chemistry, Xiamen University 2014-present Professor, Department of Chemistry, Xiamen University
基金This study is supported by the National Key Research and Development Program of China(2017YFB0307500).
文摘Implementing a new energy-saving electrochemical synthesis system with high commercial value is a strategy of the sustainable development for upgrading the bulk chemicals preparation technology in the future.Here,we report a multiple redox-mediated linear paired electrolysis system,combining the hydrogen peroxide mediated cathode process with the I2 mediated anode process,and realize the conversion of furfural to furoic acid in both side of the dividedflow cell simultaneously.By reasonably controlling the cathode potential,the undesired water splitting reaction and furfural reduction side reactions are avoided.Under the galvanostatic electrolysis,the two-mediated electrode processes have good compatibility,which reduce the energy consumption by about 22%while improving the electronic efficiency by about 125%.This system provides a green electrochemical synthesis route with commercial prospects.
文摘An electrochemical synthesis of functionalized (aza)indolines through dehydrogenative [3+2] annulation of arylamines with tethered alkenes has been developed. Previous reported syntheses through similar inter- and intramolecular annulation reactions required noble-metal catalysts and are mostly limited to terminal alkenes or 1,3-dienes. The electrosynthesis employs the easily available and inexpensive ferrocene as the molecular catalyst and is compatible with di-, tri- and even tetrasubstituted alkenes to construct indolines as well as the more challenging azaindolines. Employing the newly developed electrosynthesis as a key step, the total synthesis of marine alkaloid (+)-hinckdentine A has been achieved in 12 steps (longest linear sequence) from commercially available materials.
基金supported by the National Natural Science Foundation of China (21821002, 21772222, and 91956112)Chinese Academy of Sciences (XDB20000000)Science and Technology Commission of Shanghai Municipality (18JC1415600 and 20JC1417100)。
文摘Organic electrosynthesis has been widely used as an environmentally conscious alternative to conventional methods for redox reactions because it utilizes electric current as a traceless redox agent instead of chemical redox agents. Indirect electrolysis employing a redox catalyst has received tremendous attention, since it provides various advantages compared to direct electrolysis. With indirect electrolysis, overpotential of electron transfer can be avoided, which is inherently milder, thus wide functional group tolerance can be achieved. Additionally, chemoselectivity, regioselectivity, and stereoselectivity can be tuned by the redox catalysts used in indirect electrolysis. Furthermore, electrode passivation can be avoided by preventing the formation of polymer films on the electrode surface. Common redox catalysts include N-oxyl radicals, hypervalent iodine species, halides, amines, benzoquinones(such as DDQ and tetrachlorobenzoquinone), and transition metals. In recent years, great progress has been made in the field of indirect organic electrosynthesis using transition metals as redox catalysts for reaction classes including C–H functionalization, radical cyclization, and cross-coupling of aryl halides-each owing to the diverse reactivity and accessible oxidation states of transition metals. Although various reviews of organic electrosynthesis are available, there is a lack of articles that focus on recent research progress in the area of indirect electrolysis using transition metals, which is the impetus for this review.
基金supported by the National Science Foundation of China(nos.22071105 and 22031008)the Qinglan Project of Jiangsu Education Department.
文摘Although the combination of electrochemistry and homogeneous catalysis has proven to be a powerful strategy for achieving a diverse array of novel transformations,some challenges such as controlling the diffusion of catalyst-related species and the instability of catalysts at electrodes remain to be overcome.Herein,we review recent advances in electrochemical homogeneous catalysis,focusing on electrochemical noble-transition-metal catalysis,photoelectrochemical catalysis,and electrochemical enantioselective catalysis.The topics discussed include:(1)how the noblemetal catalystworks in the presence of cathodic hydrogen evolution,(2)how the photocatalyst gets enhanced redox property,and(3)how the enantioselectivity is regulated in a catalytic electrochemical reaction.
基金The authors acknowledge the financial support of this re-search from the Ministry of Science and Technology of China(No.2016YFA0204100)the National Natural Science Foundation of China(No.21672178)the Fundamental Research Funds for the Central Universities.
文摘Summary of main observation and conclusion An electrochemical synthesis of oxazol-2-ones and imidazol-2-ones has been developed via 5-exo-dig cyclization of propargylic carbamates-and ureas-derived amidyl radicals.The electrosynthesis relies on the dual function of 2,2,66-tetramethylpiperidin-1-y oxyl(TEMPO)as a redox mediator for amidyl radical formation and an oxygen atom donor.The reactions are conducted under mild conditions using a simple setup and provide convenient access to functionalized oxazol-2-ones and imidazol-2-ones from readily available materials.
基金supported by the National Natural Science Foundation of China(21672178)Fundamental Research Funds for the Central Universities
文摘Dehydrogenative cyclization of thioamides is an attractive approach for the synthesis of S-heterocycles.Reported herein is an electrochemical dehydrogenative cyclization reaction of N-benzyl thioamides in a flow electrolysis cell.The continuous-flow electrosynthesis has addressed the limitations associated with previously reported methods for the cyclization of alkylthioamides and provide a transition metal-and oxidizing reagent-free access to various functionalized 1,3-benzothiazines in good yields.
基金The authors acknowledge the financial support of this research from NSFC(no.21672178,21971213)MOST(no.2016YFA0204100)+2 种基金the National Postdoctoral Program for Innovative Talents(no.BX201700141)China Postdoctoral Science Foundation(no.2018M630730)Fundamental Research Funds for the Central Universities.
文摘Acridinium dyes have been broadly used as photocatalysts,but it remains synthetically challenging to fine-tune their catalytic performance by functionalization of their structural cores.Acridinium photocatalysts are usually prepared through de novo synthesis,which involves difficult steps and requires sensitive organometallic reagents.