Catalytic oxidation of benzene with N_(2)O to phenol over the hierarchical and microporous Fe/ZSM-5-based catalysts in a continuous fixedbed reactor was investigated.The spent catalyst was in-situ regenerated by an ox...Catalytic oxidation of benzene with N_(2)O to phenol over the hierarchical and microporous Fe/ZSM-5-based catalysts in a continuous fixedbed reactor was investigated.The spent catalyst was in-situ regenerated by an oxidative treatment using N_(2)O and in total 10 reaction-regeneration cycles were performed.A 100% N_(2)O conversion,93.3% phenol selectivity,and high initial phenol formation rate of 16.49±0.06mmol_(phenol gcatalyst)^(-1)h^(-1)at time on stream(TOS) of 5 min,and a good phenol productivity of 147.06 mmol_(phenol gcatalyst)^(-1)during catalyst lifetime of 1800 min were obtained on a fresh hierarchical Fe/ZSM-5-Hi2.8 catalyst.With the reaction-regeneration cycle,N_(2)O conversion is fully recovered within TOS of 3 h,moreover,the phenol productivity was decreased ca.2.2±0.8% after each cycle,leading to a total phenol productivity of ca.0.44 ton_(pheol kg_(catalyst)^(-1)estimated for 300 cycles.Catalyst characterizations imply that the coke is rapidly deposited on catalyst surface in the initial TOS of 3 h(0.28 mgc_(gcatalyst)^(-1)min^(-1)) and gradually becomes graphitic during the TOS of 30 h with a slow formation rate of 0.06 mgc g_(catalyst)^(-1)min^(-1).Among others(e.g.,the decrease of textural property and acidity),the nearly complete coverage of the active Fe-O-Al sites by coke accounts for the main catalyst deactivation.Besides these reversible deactivation characteristics related to coking,the irreversible catalyst deactivation is also observed with the reaction-regeneration cycle.The latter is reflected by a further decreased amount of the active Fe-O-Al sites,which agglomerate on catalyst surface with the cycle,likely associated with the hard coke residue that is not completely removed by the regeneration.展开更多
Certain phenols and naphthols were nitrated regioselectively with Zn(NO)·6HO/TCT in acetonitrile as solvent at room temperature and short reaction time in good yields.The reaction condition was mild.TCT is a chea...Certain phenols and naphthols were nitrated regioselectively with Zn(NO)·6HO/TCT in acetonitrile as solvent at room temperature and short reaction time in good yields.The reaction condition was mild.TCT is a cheap and commercially available reagent.It performed as an acid catalyst in this transformation.展开更多
The title compound (E)-2-[(4-tert-butyl-5-(4-methoxybenzyl)thiazol-2-ylimino)methyl]phenol was synthesized by the reaction of 5-(4-methoxybenzyl)-4-tert- butylthiazol-2-amine with salicylaldehyde, and its crys...The title compound (E)-2-[(4-tert-butyl-5-(4-methoxybenzyl)thiazol-2-ylimino)methyl]phenol was synthesized by the reaction of 5-(4-methoxybenzyl)-4-tert- butylthiazol-2-amine with salicylaldehyde, and its crystal structure was determined by single-crystal X-ray diffraction. The crystal belongs to the monoclinic system, space group P21/c with a = 5.9362(8), b = 11.5070(15), c = 29.460(4)A, β= 97.326(3)°, V = 1995.9(5) A^3, Z = 4, F(000) = 808, C22H24N2O2S, Mr= 380.49, De= 1.266 g/cm^3, S = 1.031,μ = 0.181 mm^-1, the final R = 0.0474 and wR = 0.1441 for 4327 observed reflections (I 〉 2σ(I)). Intramolecular O-H…N hydrogen bond is observed in the crystal. The preliminary bioassay showed that the title compound exhibits 95% inhibition rate against Rhizoctonia solani at the test concentration of 500 mg/L.展开更多
Phenol hydrogenation is a green route to prepare cyclohexanone,an intermediate for the production of nylon 66 and nylon 6.The development of high-performance catalysts still keeps a great challenge.Herein,the activate...Phenol hydrogenation is a green route to prepare cyclohexanone,an intermediate for the production of nylon 66 and nylon 6.The development of high-performance catalysts still keeps a great challenge.Herein,the activated carbon(AC)was modified with an acidic material Nb_(2)O_(5)to adjust the microstructure and surface properties of AC,and the influences of the calcination temperature and Nb_(2)O_(5)content on the catalytic performance of the Pd/AC-Nb_(2)O_(5)catalysts for the phenol hydrogenation to cyclohexanone were investigated.The Nb_(2)O_(5)with proper content can be highly uniformly distributed on the AC surface,enhancing the acidity of the Pd/AC-Nb_(2)O_(5)catalysts with comparable specific surface area and Pd dispersion,thereby improving the catalytic activity.The hybrid Pd/AC-10 Nb_(2)O_(5)-500 catalyst exhibits the synergistic effect between the Pd nanoparticles and AC-10 Nb_(2)O_(5),which enhances the catalytic activity for the hydrogenation of phenol.Furthermore,the as-prepared Pd/AC-10 Nb_(2)O_(5)-500 catalyst shows good reusability during 7 reaction cycles.展开更多
The title compound N1-(2-(4-bromo-2-nitrophenoxy)-2-dimethyl acyloxymethyl)-5-fluorouracil(C15H13BrFN3O7, Mr = 446.19) was synthesized and structurally characterized by ^1H-NMR, -(13)C-NMR, ESI-MS and single-c...The title compound N1-(2-(4-bromo-2-nitrophenoxy)-2-dimethyl acyloxymethyl)-5-fluorouracil(C15H13BrFN3O7, Mr = 446.19) was synthesized and structurally characterized by ^1H-NMR, -(13)C-NMR, ESI-MS and single-crystal X-ray diffraction. The compound crystallizes in triclinic, space group P1, with a = 8.3325(6), b = 10.1808(13), c = 11.8194(16) A, α = 73.194(12), β= 72.351(9), γ = 89.509(8)o, V = 911.2(2) A^3, Z = 2, T = 300.79(10) K, μ(Cu Kα) = 3.578 mm^-1, Dc = 1.626 g/cm3, F(000) = 448.0, GOF = 1.060, 5723 reflections measured(8.232≤2θ≤139.592°), 3339 unique(Rint = 0.0184, Rsigma = 0.0254) which were used in all calculations. The final R = 0.0517(I 〉 2s(I)) and wR = 0.1494(all data). Hydrogen bonds and π-π interactions together stabilize the structure of the molecule. The preliminary biological test shows that the title compound has good antitumor activity against A549 in vitro and lower toxicity to normal cells.展开更多
基金Financial support by the Specialized Research Fund for Doctoral Program of Higher Education,China (No.20120010110003)。
文摘Catalytic oxidation of benzene with N_(2)O to phenol over the hierarchical and microporous Fe/ZSM-5-based catalysts in a continuous fixedbed reactor was investigated.The spent catalyst was in-situ regenerated by an oxidative treatment using N_(2)O and in total 10 reaction-regeneration cycles were performed.A 100% N_(2)O conversion,93.3% phenol selectivity,and high initial phenol formation rate of 16.49±0.06mmol_(phenol gcatalyst)^(-1)h^(-1)at time on stream(TOS) of 5 min,and a good phenol productivity of 147.06 mmol_(phenol gcatalyst)^(-1)during catalyst lifetime of 1800 min were obtained on a fresh hierarchical Fe/ZSM-5-Hi2.8 catalyst.With the reaction-regeneration cycle,N_(2)O conversion is fully recovered within TOS of 3 h,moreover,the phenol productivity was decreased ca.2.2±0.8% after each cycle,leading to a total phenol productivity of ca.0.44 ton_(pheol kg_(catalyst)^(-1)estimated for 300 cycles.Catalyst characterizations imply that the coke is rapidly deposited on catalyst surface in the initial TOS of 3 h(0.28 mgc_(gcatalyst)^(-1)min^(-1)) and gradually becomes graphitic during the TOS of 30 h with a slow formation rate of 0.06 mgc g_(catalyst)^(-1)min^(-1).Among others(e.g.,the decrease of textural property and acidity),the nearly complete coverage of the active Fe-O-Al sites by coke accounts for the main catalyst deactivation.Besides these reversible deactivation characteristics related to coking,the irreversible catalyst deactivation is also observed with the reaction-regeneration cycle.The latter is reflected by a further decreased amount of the active Fe-O-Al sites,which agglomerate on catalyst surface with the cycle,likely associated with the hard coke residue that is not completely removed by the regeneration.
文摘Certain phenols and naphthols were nitrated regioselectively with Zn(NO)·6HO/TCT in acetonitrile as solvent at room temperature and short reaction time in good yields.The reaction condition was mild.TCT is a cheap and commercially available reagent.It performed as an acid catalyst in this transformation.
基金the National Project of Scientific and Technical Supporting Programs and Ministry of Science & Technology of China (No.2006BAE01A01-4)
文摘The title compound (E)-2-[(4-tert-butyl-5-(4-methoxybenzyl)thiazol-2-ylimino)methyl]phenol was synthesized by the reaction of 5-(4-methoxybenzyl)-4-tert- butylthiazol-2-amine with salicylaldehyde, and its crystal structure was determined by single-crystal X-ray diffraction. The crystal belongs to the monoclinic system, space group P21/c with a = 5.9362(8), b = 11.5070(15), c = 29.460(4)A, β= 97.326(3)°, V = 1995.9(5) A^3, Z = 4, F(000) = 808, C22H24N2O2S, Mr= 380.49, De= 1.266 g/cm^3, S = 1.031,μ = 0.181 mm^-1, the final R = 0.0474 and wR = 0.1441 for 4327 observed reflections (I 〉 2σ(I)). Intramolecular O-H…N hydrogen bond is observed in the crystal. The preliminary bioassay showed that the title compound exhibits 95% inhibition rate against Rhizoctonia solani at the test concentration of 500 mg/L.
基金The financial supports from the National Natural Science Foundation(21776127,21921006)the Jiangsu Province Key R&D Program(BE2018009-2)+3 种基金the Jiangsu Province natural science research of College and university general project(20KJB540003)a project funded by the priority academic program development of Jiangsu higher education institutions(PAPD)the State Key Laboratory of Materials-Oriented Chemical Engineering(ZK201902)the outstanding young teacher’s project of Changzhou Vocational Institute of Textile and Garment of China。
文摘Phenol hydrogenation is a green route to prepare cyclohexanone,an intermediate for the production of nylon 66 and nylon 6.The development of high-performance catalysts still keeps a great challenge.Herein,the activated carbon(AC)was modified with an acidic material Nb_(2)O_(5)to adjust the microstructure and surface properties of AC,and the influences of the calcination temperature and Nb_(2)O_(5)content on the catalytic performance of the Pd/AC-Nb_(2)O_(5)catalysts for the phenol hydrogenation to cyclohexanone were investigated.The Nb_(2)O_(5)with proper content can be highly uniformly distributed on the AC surface,enhancing the acidity of the Pd/AC-Nb_(2)O_(5)catalysts with comparable specific surface area and Pd dispersion,thereby improving the catalytic activity.The hybrid Pd/AC-10 Nb_(2)O_(5)-500 catalyst exhibits the synergistic effect between the Pd nanoparticles and AC-10 Nb_(2)O_(5),which enhances the catalytic activity for the hydrogenation of phenol.Furthermore,the as-prepared Pd/AC-10 Nb_(2)O_(5)-500 catalyst shows good reusability during 7 reaction cycles.
基金Gansu Province Science and Technology Bureau Program Funds(144FKCA065)
文摘The title compound N1-(2-(4-bromo-2-nitrophenoxy)-2-dimethyl acyloxymethyl)-5-fluorouracil(C15H13BrFN3O7, Mr = 446.19) was synthesized and structurally characterized by ^1H-NMR, -(13)C-NMR, ESI-MS and single-crystal X-ray diffraction. The compound crystallizes in triclinic, space group P1, with a = 8.3325(6), b = 10.1808(13), c = 11.8194(16) A, α = 73.194(12), β= 72.351(9), γ = 89.509(8)o, V = 911.2(2) A^3, Z = 2, T = 300.79(10) K, μ(Cu Kα) = 3.578 mm^-1, Dc = 1.626 g/cm3, F(000) = 448.0, GOF = 1.060, 5723 reflections measured(8.232≤2θ≤139.592°), 3339 unique(Rint = 0.0184, Rsigma = 0.0254) which were used in all calculations. The final R = 0.0517(I 〉 2s(I)) and wR = 0.1494(all data). Hydrogen bonds and π-π interactions together stabilize the structure of the molecule. The preliminary biological test shows that the title compound has good antitumor activity against A549 in vitro and lower toxicity to normal cells.