The complex reaction system of the coal gasification coupling C1 reaction was analyzed based on the principles of thermodynamics. The results show that an increase in the temperature is beneficial to the generation of...The complex reaction system of the coal gasification coupling C1 reaction was analyzed based on the principles of thermodynamics. The results show that an increase in the temperature is beneficial to the generation of hydrocarbons with high carbon-atom contents, in which the alkane yield is higher than the alkene yield. The complex reaction system consisting of C, H20, CO, CO2, H2, C2H4, C3H6 and C4Hs was studied, and the obtained results indicated that when the maximum mole fraction content of C2-C4 olefins was regarded as the optimized objective function, the optimum temperature was approximately 648 K, the pressure was 0.1 MPa, the feed ratio was approximately 0.6, and the maximum mole fraction content of C2-C4 olefins was approximately 28.24%. The thermodynamic simulation and calculation of the complex reaction system can provide a basis for the determination and optimization of actual process conditions and are therefore of great theoretical and practical significance.展开更多
An efficient route to synthesize the heteroaryl-substituted 1,8-naphthyridine derivatives was described. Eight 2-heteroaryl- and 2,7-diheteroaryl-1,8-naphthyridine derivatives were obtained through palladium-catalyzed...An efficient route to synthesize the heteroaryl-substituted 1,8-naphthyridine derivatives was described. Eight 2-heteroaryl- and 2,7-diheteroaryl-1,8-naphthyridine derivatives were obtained through palladium-catalyzed C-N-coupling reactions of chloronaphthyridines with imidazole, benzimidazole, morpholine, 3,5-dimethylpyrazole, and phthalimide in moderate to good yields.展开更多
Development of transition metal-based photocatalysts with low cost, strong visible light absorption, and high efficiency is a longstand pursuit for advanced organic synthesis, yet remains highly challenging. In this a...Development of transition metal-based photocatalysts with low cost, strong visible light absorption, and high efficiency is a longstand pursuit for advanced organic synthesis, yet remains highly challenging. In this article, an anthraquinone-based copper(I)cyclic trinuclear complex(1) was designed and it featured strong visible light absorption, high charge separation efficiency and photochemical properties. Complex 1 as a heterogeneous photocatalyst can efficiently catalyze homo-coupling of terminal alkynes and denitrification-oxidative coupling reaction between hydrazinopyridine and terminal alkynes with excellent yield(up to 99%), broad substrate tolerance(27 examples) and superior reusability(up to 10 cycles without loss of performance) under mild conditions.展开更多
A fast and convenient C―S bond formation reaction was achieved catalyzed by CuI/L-proline in aqueous two-phase system providing a simple method for synthesis of aryl sulfides in good yields in short time.
Catalytic hydrogenation of CO_(2) using renewable hydrogen not only reduces greenhouse gas emissions,but also provides industrial chemicals.Herein,a Co-Fe bimetallic catalyst was developed by a facile reactive ball-mi...Catalytic hydrogenation of CO_(2) using renewable hydrogen not only reduces greenhouse gas emissions,but also provides industrial chemicals.Herein,a Co-Fe bimetallic catalyst was developed by a facile reactive ball-milling method for highly active and selective hydrogenation of CO_(2) to value-added hydrocarbons.When reacted at 320℃,1.0 MPa and 9600 mL h^(-1) g_(cat)^(-1),the selectivity to light olefin(C_(2)^(=)-C_(4)^(=)) and C_(5)+ species achieves 57.3% and 22.3%,respectively,at a CO_(2) co nversion of 31.4%,which is superior to previous Fe-based catalysts.The CO_(2) activation can be promoted by the CoFe phase formed by reactive ball milling of the Fe-Co_(3)O_(4) mixture,and the in-situ Co_(2)C and Fe_(5)C_(2) formed during hydrogenation are beneficial for the C-C coupling reaction.The initial C-C coupling is related to the combination of CO species with the surface carbon of Fe/Co carbides,and the sustained C-C coupling is maintained by self-recovery of defective carbides.This new strategy contributes to the development of efficient catalysts for the hydrogenation of CO_(2) to value-added hydrocarbons.展开更多
Graphene is of great interest because of its exciting properties and potential applications,but its production on a large-scale still presents considerable challenges.Herein,we report the synthesis of predominately fe...Graphene is of great interest because of its exciting properties and potential applications,but its production on a large-scale still presents considerable challenges.Herein,we report the synthesis of predominately few-layer graphene,due toπ–πstacking,and single-layer graphene from reaction between hexabromobenzene and Na metal,followed by annealing to improve crystallinity.The reaction proceeds via a free-radical C(sp^(2))–C(sp^(2))coupling mechanism,which is supported by theoretical calculations.The graphene can host unpaired spin electrons,leading to a short acquisition time for a solidstate nuclear magnetic resonance 13C spectrum from unlabeled graphene,which is ascribed to the very short spin-lattice relaxation time.High catalytic activity for transforming amine to imine with a conversion of>99%and a yield of∼97%is demonstrated,and high electronic conductivity of∼105 S·m^(−1) is found by terahertz spectroscopy.The reaction delivers a method for synthesizing graphene with a high spin concentration from perbrominated benzene molecules by using an active metallic agent,such as Na,Li,or Mg.展开更多
基金supported by the National Natural Science Foundation of China(NSFC Grant No. 51706168)
文摘The complex reaction system of the coal gasification coupling C1 reaction was analyzed based on the principles of thermodynamics. The results show that an increase in the temperature is beneficial to the generation of hydrocarbons with high carbon-atom contents, in which the alkane yield is higher than the alkene yield. The complex reaction system consisting of C, H20, CO, CO2, H2, C2H4, C3H6 and C4Hs was studied, and the obtained results indicated that when the maximum mole fraction content of C2-C4 olefins was regarded as the optimized objective function, the optimum temperature was approximately 648 K, the pressure was 0.1 MPa, the feed ratio was approximately 0.6, and the maximum mole fraction content of C2-C4 olefins was approximately 28.24%. The thermodynamic simulation and calculation of the complex reaction system can provide a basis for the determination and optimization of actual process conditions and are therefore of great theoretical and practical significance.
基金the National Natural Science Foundation of China （no. 20572096） the Zhejiang Provincial Science Foundation （Grant R405066）.
文摘An efficient route to synthesize the heteroaryl-substituted 1,8-naphthyridine derivatives was described. Eight 2-heteroaryl- and 2,7-diheteroaryl-1,8-naphthyridine derivatives were obtained through palladium-catalyzed C-N-coupling reactions of chloronaphthyridines with imidazole, benzimidazole, morpholine, 3,5-dimethylpyrazole, and phthalimide in moderate to good yields.
基金Guo-Hong Ning is thankful for the support from the Guangdong Basic and Applied Basic Research Foundation (2019B151502024)the Guangzhou Science and Technology Project (202201020038)+1 种基金supported by the National Natural Science Foundation of China (22371091, 21975104, 22150004, 22101099)the Guangdong Major Project of Basic and Applied Research (2019B030302009)。
文摘Development of transition metal-based photocatalysts with low cost, strong visible light absorption, and high efficiency is a longstand pursuit for advanced organic synthesis, yet remains highly challenging. In this article, an anthraquinone-based copper(I)cyclic trinuclear complex(1) was designed and it featured strong visible light absorption, high charge separation efficiency and photochemical properties. Complex 1 as a heterogeneous photocatalyst can efficiently catalyze homo-coupling of terminal alkynes and denitrification-oxidative coupling reaction between hydrazinopyridine and terminal alkynes with excellent yield(up to 99%), broad substrate tolerance(27 examples) and superior reusability(up to 10 cycles without loss of performance) under mild conditions.
基金Supported by the Zhejiang Province Natural Science Foundation, China(No.407240)
文摘A fast and convenient C―S bond formation reaction was achieved catalyzed by CuI/L-proline in aqueous two-phase system providing a simple method for synthesis of aryl sulfides in good yields in short time.
基金supported by the National Natural Science Foundation of China (22008098, 21978156, 42002040)the Program for Innovative Research Team (in Science and Technology) in University of Henan Province (21IRTSTHN004)+1 种基金the Program for Science & Technology Innovation Talents in Universities of Henan Province (22HASTIT008)the Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering (2022-K34)。
文摘Catalytic hydrogenation of CO_(2) using renewable hydrogen not only reduces greenhouse gas emissions,but also provides industrial chemicals.Herein,a Co-Fe bimetallic catalyst was developed by a facile reactive ball-milling method for highly active and selective hydrogenation of CO_(2) to value-added hydrocarbons.When reacted at 320℃,1.0 MPa and 9600 mL h^(-1) g_(cat)^(-1),the selectivity to light olefin(C_(2)^(=)-C_(4)^(=)) and C_(5)+ species achieves 57.3% and 22.3%,respectively,at a CO_(2) co nversion of 31.4%,which is superior to previous Fe-based catalysts.The CO_(2) activation can be promoted by the CoFe phase formed by reactive ball milling of the Fe-Co_(3)O_(4) mixture,and the in-situ Co_(2)C and Fe_(5)C_(2) formed during hydrogenation are beneficial for the C-C coupling reaction.The initial C-C coupling is related to the combination of CO species with the surface carbon of Fe/Co carbides,and the sustained C-C coupling is maintained by self-recovery of defective carbides.This new strategy contributes to the development of efficient catalysts for the hydrogenation of CO_(2) to value-added hydrocarbons.
基金This work was financially support from the National Key R&D Program of China(no.2016YFA0200200)the National Program on Key Basic Research Project(973 program,no.2013CB933804)+1 种基金the National Natural Science Foundation of China(no.21271112)the Tribology Science Fund of State Key Laboratory of Tribology(SKLTKF20B18).
文摘Graphene is of great interest because of its exciting properties and potential applications,but its production on a large-scale still presents considerable challenges.Herein,we report the synthesis of predominately few-layer graphene,due toπ–πstacking,and single-layer graphene from reaction between hexabromobenzene and Na metal,followed by annealing to improve crystallinity.The reaction proceeds via a free-radical C(sp^(2))–C(sp^(2))coupling mechanism,which is supported by theoretical calculations.The graphene can host unpaired spin electrons,leading to a short acquisition time for a solidstate nuclear magnetic resonance 13C spectrum from unlabeled graphene,which is ascribed to the very short spin-lattice relaxation time.High catalytic activity for transforming amine to imine with a conversion of>99%and a yield of∼97%is demonstrated,and high electronic conductivity of∼105 S·m^(−1) is found by terahertz spectroscopy.The reaction delivers a method for synthesizing graphene with a high spin concentration from perbrominated benzene molecules by using an active metallic agent,such as Na,Li,or Mg.
