In this study,the effects of low temperature on aluminum(Ⅲ)(Al)hydrolysis were examined both theoretically and experimentally by constructing a solubility diagram for amorphous aluminum hydroxide(Al(OH)_3(am))and a d...In this study,the effects of low temperature on aluminum(Ⅲ)(Al)hydrolysis were examined both theoretically and experimentally by constructing a solubility diagram for amorphous aluminum hydroxide(Al(OH)_3(am))and a distribution diagram of hydrolyzed Al species.First,thermodynamic data of Al species at 4℃were calculated from that at 25℃.A well confirmed polymeric Al species, AlO_4Al_(12)(OH)_(24)^(7+)(Al_(13)),was involved in building the diagrams and,correspondingly,the non-linear simultaneous equations wit...展开更多
The elegant 2D multiquantum (MQ) MAS NMR has been applied to investigate the coordination of Al atoms in SAPO-34. The results show that the effects of the template and/or water on the coordination of Al atoms are sig...The elegant 2D multiquantum (MQ) MAS NMR has been applied to investigate the coordination of Al atoms in SAPO-34. The results show that the effects of the template and/or water on the coordination of Al atoms are significant, which lead to the formation of various Al species. Up to four kinds of Al species are distinctly resolved.展开更多
The IR spectrum and 11B and 27Al MAS NMR spectra of Al18B4O33 are presented and discussed in relation to the possible existence of boron atoms substituting for aluminum atoms. The IR spectrum shows that the strong vi...The IR spectrum and 11B and 27Al MAS NMR spectra of Al18B4O33 are presented and discussed in relation to the possible existence of boron atoms substituting for aluminum atoms. The IR spectrum shows that the strong vibrations of the BO3 groups are present in the 1 500-1 200 cm-1 region, and very weak bands of BO4 units are present in the region from 1 000 to 1 100 cm-1. 11B MAS NMR spectrum indicates that the strong signal for BO3 units appears in the region from δ+5 to δ+20, and the very weak signal for BO4 units is at about δ- 1, while 27Al MAS NMR spectrum shows five peaks at about δ+62, +42. 1, +14, -4. 7 and -6. 4, originating from AlO4, AlO4, AlO5, AlO6 and AlO6, respectively. These results reveal that there are minor BO4 units in Al18B4O33, indicating that a small amount of B atoms substitute for Al atoms in the 4-fold coordination.展开更多
Aluminum is the primary structural material in nuclear engineering,and its cross section induced by 14-MeV neutrons is of great significance.To address the issue of insufficient accuracy for the^(27)Al(n,2n)^(26)Al re...Aluminum is the primary structural material in nuclear engineering,and its cross section induced by 14-MeV neutrons is of great significance.To address the issue of insufficient accuracy for the^(27)Al(n,2n)^(26)Al reaction cross section,the activation method and accelerator mass spectrometry(AMS)technique were used to determine the^(27)Al(n,2n)^(26)Al cross section,which could be used as a D-T plasma ion temperature monitor in fusion reactors.At the China Academy of Engineering Physics,neutron activation was performed using a K-400 neutron generator produced by the T(d,n)4He reaction.The^(26)Al∕^(27)Al isotope ratios were measured using the newly installed GYIG 1 MV AMS at the Institute of Geochemistry,Chinese Academy of Sciences.The neutron flux was monitored by measuring the activity of 92mNb produced by the 93Nb(n,2n)92mNb reaction.The measured results were compared with available data in the experimental nuclear reaction database,and the measured values showed a reasonable degree of consistency with partially available literature data.The newly acquired cross-sectional data at 12 neutron energy points through systematic measurements clarified the divergence,which has two different growth trends from the existing experimental values.The obtained results are also compared with the corresponding evaluated database,and the newly calculated excitation functions with TALYS−1.95 and EMPIRE−3.2 codes,the agreement with CENDL−3.2,TENDL-2021 and EMPIRE−3.2 results are generally acceptable.A substantial improvement in the knowledge of the^(27)Al(n,2n)^(26)Al reaction excitation function was obtained in the present work,which will lay the foundation for the diagnosis of the fusion ion temperature,testing of the nuclear physics model,evaluation of nuclear data,etc.展开更多
Pentacoordinated Al(Al~Ⅴ)species in silica-alumina are promising to promote the formation of acid sites or act as surface defects for tailoring single-atom catalysts.However,pentahedral coordination(Al~Ⅴ)is rarely o...Pentacoordinated Al(Al~Ⅴ)species in silica-alumina are promising to promote the formation of acid sites or act as surface defects for tailoring single-atom catalysts.However,pentahedral coordination(Al~Ⅴ)is rarely observed in conventionally prepared silica-alumina.Here,we show that high population and dispersion of Al~Ⅴ species on the surface of amorphous silica-alumina(ASA)can be achieved by means of flame spray pyrolysis.High resolution TEM/EDX,high magnetic-field NMR and DFT calculations are employed to characterize the structure of as-prepared ASAs.Solid-state ^(27)Al multi-quantum MAS NMR experiments show that most of the Al~Ⅴspecies are formed independently from the alumina phase and are accessible for guest molecules on the surface.Upon water adsorption,these Al~Ⅴ species are transformed to Al~Ⅵ species,structurally similar to surface Al~Ⅳ species,as confirmed by DFT calculations.The outstanding catalytic activity of as-synthesized ASA is demonstrated using the in situ H/D exchange reaction with deuterated benzene as an example.The Al~Ⅴ-rich ASA provides a much lower activation energy(～30 kJ/mol)than that reported for zeolite H-ZSM-5(～60 kJ/mol).The superior catalytic performance is attributed to the high Al~Ⅴcontent promoting the surface active sites in ASA.The knowledge gained on the synthesis of Al~Ⅴ-rich ASAs and the nature of aluminum coordination in these materials could pave the way to more efficient silica-alumina based catalysts.展开更多
Poly(aluminum chloride)(PAC) solutions of different basicity were prepared from pure aluminum foil and hydrochloric acid. Aluminum species were investigated by 27Al NMR spectroscopy and the tridecameric polycation Al ...Poly(aluminum chloride)(PAC) solutions of different basicity were prepared from pure aluminum foil and hydrochloric acid. Aluminum species were investigated by 27Al NMR spectroscopy and the tridecameric polycation Al 13 was detected. With the increase of PAC′s basicity, the molar ratio of Al 13 to Al m in PAC increases. The jar tests with kaolin water and water from Huangpu River at the same PACs dosage showed that the more basicity and content of Al 13, the more effective the coagulation effect on water with middle-high turbidity, while only less effect of the basicity was observed on water with low turbidity.展开更多
文摘In this study,the effects of low temperature on aluminum(Ⅲ)(Al)hydrolysis were examined both theoretically and experimentally by constructing a solubility diagram for amorphous aluminum hydroxide(Al(OH)_3(am))and a distribution diagram of hydrolyzed Al species.First,thermodynamic data of Al species at 4℃were calculated from that at 25℃.A well confirmed polymeric Al species, AlO_4Al_(12)(OH)_(24)^(7+)(Al_(13)),was involved in building the diagrams and,correspondingly,the non-linear simultaneous equations wit...
基金We are grateful to the support of the National Natural Science Foundation of China and the Ministry of Science and Technology of China. We appreciate Dr. R. Fu (NHMFL Tallahassee) for his kind help regarding the MQ MAS NMR experiments.
文摘The elegant 2D multiquantum (MQ) MAS NMR has been applied to investigate the coordination of Al atoms in SAPO-34. The results show that the effects of the template and/or water on the coordination of Al atoms are significant, which lead to the formation of various Al species. Up to four kinds of Al species are distinctly resolved.
基金Supported by the National Natural Science Foundation of China.
文摘The IR spectrum and 11B and 27Al MAS NMR spectra of Al18B4O33 are presented and discussed in relation to the possible existence of boron atoms substituting for aluminum atoms. The IR spectrum shows that the strong vibrations of the BO3 groups are present in the 1 500-1 200 cm-1 region, and very weak bands of BO4 units are present in the region from 1 000 to 1 100 cm-1. 11B MAS NMR spectrum indicates that the strong signal for BO3 units appears in the region from δ+5 to δ+20, and the very weak signal for BO4 units is at about δ- 1, while 27Al MAS NMR spectrum shows five peaks at about δ+62, +42. 1, +14, -4. 7 and -6. 4, originating from AlO4, AlO4, AlO5, AlO6 and AlO6, respectively. These results reveal that there are minor BO4 units in Al18B4O33, indicating that a small amount of B atoms substitute for Al atoms in the 4-fold coordination.
基金the Open Project of Guangxi Key Laboratory of Nuclear Physics and Nuclear Technology(NLK 2022-04)the Central Government Guidance Funds for Local Scientific and Technological Development,China(No.Guike,ZY22096024)+1 种基金the National Natural Science Foundation of China(12065003)Guangxi Key R&D Project(2023AB07029).
文摘Aluminum is the primary structural material in nuclear engineering,and its cross section induced by 14-MeV neutrons is of great significance.To address the issue of insufficient accuracy for the^(27)Al(n,2n)^(26)Al reaction cross section,the activation method and accelerator mass spectrometry(AMS)technique were used to determine the^(27)Al(n,2n)^(26)Al cross section,which could be used as a D-T plasma ion temperature monitor in fusion reactors.At the China Academy of Engineering Physics,neutron activation was performed using a K-400 neutron generator produced by the T(d,n)4He reaction.The^(26)Al∕^(27)Al isotope ratios were measured using the newly installed GYIG 1 MV AMS at the Institute of Geochemistry,Chinese Academy of Sciences.The neutron flux was monitored by measuring the activity of 92mNb produced by the 93Nb(n,2n)92mNb reaction.The measured results were compared with available data in the experimental nuclear reaction database,and the measured values showed a reasonable degree of consistency with partially available literature data.The newly acquired cross-sectional data at 12 neutron energy points through systematic measurements clarified the divergence,which has two different growth trends from the existing experimental values.The obtained results are also compared with the corresponding evaluated database,and the newly calculated excitation functions with TALYS−1.95 and EMPIRE−3.2 codes,the agreement with CENDL−3.2,TENDL-2021 and EMPIRE−3.2 results are generally acceptable.A substantial improvement in the knowledge of the^(27)Al(n,2n)^(26)Al reaction excitation function was obtained in the present work,which will lay the foundation for the diagnosis of the fusion ion temperature,testing of the nuclear physics model,evaluation of nuclear data,etc.
基金the financial supports by Australian Research Council Discovery Projects (DP150103842)Discovery Earlier Career Research Project (DE190101618)+1 种基金the Faculty's MCR Scheme, Energy and Materials Clusters at the University of Sydneythe support by the National Natural Science Foundation of China (21522310, 21473244 and 21210005)
文摘Pentacoordinated Al(Al~Ⅴ)species in silica-alumina are promising to promote the formation of acid sites or act as surface defects for tailoring single-atom catalysts.However,pentahedral coordination(Al~Ⅴ)is rarely observed in conventionally prepared silica-alumina.Here,we show that high population and dispersion of Al~Ⅴ species on the surface of amorphous silica-alumina(ASA)can be achieved by means of flame spray pyrolysis.High resolution TEM/EDX,high magnetic-field NMR and DFT calculations are employed to characterize the structure of as-prepared ASAs.Solid-state ^(27)Al multi-quantum MAS NMR experiments show that most of the Al~Ⅴspecies are formed independently from the alumina phase and are accessible for guest molecules on the surface.Upon water adsorption,these Al~Ⅴ species are transformed to Al~Ⅵ species,structurally similar to surface Al~Ⅳ species,as confirmed by DFT calculations.The outstanding catalytic activity of as-synthesized ASA is demonstrated using the in situ H/D exchange reaction with deuterated benzene as an example.The Al~Ⅴ-rich ASA provides a much lower activation energy(～30 kJ/mol)than that reported for zeolite H-ZSM-5(～60 kJ/mol).The superior catalytic performance is attributed to the high Al~Ⅴcontent promoting the surface active sites in ASA.The knowledge gained on the synthesis of Al~Ⅴ-rich ASAs and the nature of aluminum coordination in these materials could pave the way to more efficient silica-alumina based catalysts.
文摘Poly(aluminum chloride)(PAC) solutions of different basicity were prepared from pure aluminum foil and hydrochloric acid. Aluminum species were investigated by 27Al NMR spectroscopy and the tridecameric polycation Al 13 was detected. With the increase of PAC′s basicity, the molar ratio of Al 13 to Al m in PAC increases. The jar tests with kaolin water and water from Huangpu River at the same PACs dosage showed that the more basicity and content of Al 13, the more effective the coagulation effect on water with middle-high turbidity, while only less effect of the basicity was observed on water with low turbidity.
