Introduction The compounds that can take up and release molecular oxygen reversibly is of significance because they can be used as model compounds for the study of the reversible oxygenation mechanisms involved in the...Introduction The compounds that can take up and release molecular oxygen reversibly is of significance because they can be used as model compounds for the study of the reversible oxygenation mechanisms involved in the very complex natural oxygen carriers, e.g., the hemoglobins and hemocyanins, and as the means of separating molecular oxygen from the air. The dioxygen carriers extensively studied are the Cobalt展开更多
Oxygenation constants and thermodynamic parameters DeltaH degrees and DeltaS degrees of cobalt (II) complexes with bis-(furaldehyde) Schiff bases (1, 2, 3, 4)were obtained by mearsuring saturated dioxygen uptake of th...Oxygenation constants and thermodynamic parameters DeltaH degrees and DeltaS degrees of cobalt (II) complexes with bis-(furaldehyde) Schiff bases (1, 2, 3, 4)were obtained by mearsuring saturated dioxygen uptake of these complexes in pyridine at different temperature. These complexes could activate molecular oxygen and were used as catalysts in cyclohexene oxidation. The influence of ligand structure on the dioxygen affinity and catalytic activity of the complexes were discussed.展开更多
The chemical looping concept provided a novel way to achieve carbon separation during the production of energy or substances. In this work, hydrogen generation with inherent CO2 capture in single packed bed reactor vi...The chemical looping concept provided a novel way to achieve carbon separation during the production of energy or substances. In this work, hydrogen generation with inherent CO2 capture in single packed bed reactor via this concept was discussed. Two oxygen carriers, Fe203 60 wt.% and Fe2O3 55 wt.%/CuO 5 wt.% supported by Al2O3, were made by ball milling method. First, according to the characteristics of the reduction breakthrough curve, a strict fuel supply strategy was selected to achieve simultaneous CO2 capture and HE production. Then, in the long term tests using CO as fuel, it was proved that CuO addition improved hydrogen generation with the maximum intensity of 3700 μmol H2·g^-1 Fe2O3 compared with Fe-Al of 2300 μmol HE.g^-1 Fe2O3. The overall CO2 capture efficiency remained 98%- 98.8% over 100 cycles. Moreover, the reactivity of deactivated materials was recovered nearly like that of fresh ones by sintering treatment. Finally, two kinds of complex gases consist of CO, HE, CH4 and CO2 were utilized as fuels to test the feasibility. The results showed all components could be completely converted by Fe-Cu- Al in the reduction stage. The intensity of hydrogen production and the overall CO2 capture efficiency were in the range of 2000-2400 μnol H2^g^-1 Fe2O3 and 89%, 95%, respectively.展开更多
The Schiff base containing pendant monoaza crown ether HL 1, HL 2, HL 3 and HL 4 have been synthesized by condensation of salicylaldehyde with N (4 aminoaryl)monoaza crown ethers, which were prepared conven...The Schiff base containing pendant monoaza crown ether HL 1, HL 2, HL 3 and HL 4 have been synthesized by condensation of salicylaldehyde with N (4 aminoaryl)monoaza crown ethers, which were prepared conveniently from 4 nitro N,N di(hydroxyethyl)aniline or 4 nitrobenzyl chloride via cyclization or condensation and reduction. The structures of HL 1—HL 4 were verified by 1H NMR, IR spectra, MS and elemental analysis. Moreover, the oxygenation constants ( K O 2 ) and thermodynamic parameters (Δ H 0 and Δ S 0) of their cobalt(II) complexes were determined in the range of -5 ℃ to 25 ℃, and the effect of crown ring bonded to a Schiff base on the dioxygen affinities of cobalt(II) complexes was also observed as compared to the uncrowned analogue (CoL 5 2).展开更多
In this paper, the stability constants of the o Phdn Co complexes and oxygenated complexes were determined by pH potentiometry for the first time. The determined method was verified with the known o Phdn Cu system by ...In this paper, the stability constants of the o Phdn Co complexes and oxygenated complexes were determined by pH potentiometry for the first time. The determined method was verified with the known o Phdn Cu system by comprising the stability constants obtained from experiment results with those in literatures. The calculated results of oxygenated complexes were confirmed by spectrophotometry. All the results are agreed very well, which show the correctness of the determination.展开更多
基金Supported by Shandong University Youth Scientific Foundation
文摘Introduction The compounds that can take up and release molecular oxygen reversibly is of significance because they can be used as model compounds for the study of the reversible oxygenation mechanisms involved in the very complex natural oxygen carriers, e.g., the hemoglobins and hemocyanins, and as the means of separating molecular oxygen from the air. The dioxygen carriers extensively studied are the Cobalt
文摘Oxygenation constants and thermodynamic parameters DeltaH degrees and DeltaS degrees of cobalt (II) complexes with bis-(furaldehyde) Schiff bases (1, 2, 3, 4)were obtained by mearsuring saturated dioxygen uptake of these complexes in pyridine at different temperature. These complexes could activate molecular oxygen and were used as catalysts in cyclohexene oxidation. The influence of ligand structure on the dioxygen affinity and catalytic activity of the complexes were discussed.
文摘The chemical looping concept provided a novel way to achieve carbon separation during the production of energy or substances. In this work, hydrogen generation with inherent CO2 capture in single packed bed reactor via this concept was discussed. Two oxygen carriers, Fe203 60 wt.% and Fe2O3 55 wt.%/CuO 5 wt.% supported by Al2O3, were made by ball milling method. First, according to the characteristics of the reduction breakthrough curve, a strict fuel supply strategy was selected to achieve simultaneous CO2 capture and HE production. Then, in the long term tests using CO as fuel, it was proved that CuO addition improved hydrogen generation with the maximum intensity of 3700 μmol H2·g^-1 Fe2O3 compared with Fe-Al of 2300 μmol HE.g^-1 Fe2O3. The overall CO2 capture efficiency remained 98%- 98.8% over 100 cycles. Moreover, the reactivity of deactivated materials was recovered nearly like that of fresh ones by sintering treatment. Finally, two kinds of complex gases consist of CO, HE, CH4 and CO2 were utilized as fuels to test the feasibility. The results showed all components could be completely converted by Fe-Cu- Al in the reduction stage. The intensity of hydrogen production and the overall CO2 capture efficiency were in the range of 2000-2400 μnol H2^g^-1 Fe2O3 and 89%, 95%, respectively.
基金ProjectsupportedbytheNationalNaturalScienceFoundationofChina (No .2 95 72 0 5 9)
文摘The Schiff base containing pendant monoaza crown ether HL 1, HL 2, HL 3 and HL 4 have been synthesized by condensation of salicylaldehyde with N (4 aminoaryl)monoaza crown ethers, which were prepared conveniently from 4 nitro N,N di(hydroxyethyl)aniline or 4 nitrobenzyl chloride via cyclization or condensation and reduction. The structures of HL 1—HL 4 were verified by 1H NMR, IR spectra, MS and elemental analysis. Moreover, the oxygenation constants ( K O 2 ) and thermodynamic parameters (Δ H 0 and Δ S 0) of their cobalt(II) complexes were determined in the range of -5 ℃ to 25 ℃, and the effect of crown ring bonded to a Schiff base on the dioxygen affinities of cobalt(II) complexes was also observed as compared to the uncrowned analogue (CoL 5 2).
文摘In this paper, the stability constants of the o Phdn Co complexes and oxygenated complexes were determined by pH potentiometry for the first time. The determined method was verified with the known o Phdn Cu system by comprising the stability constants obtained from experiment results with those in literatures. The calculated results of oxygenated complexes were confirmed by spectrophotometry. All the results are agreed very well, which show the correctness of the determination.
