Engineering transition metal compounds(TMCs)catalysts with excellent adsorption-catalytic ability has been one of the most effec-tive strategies to accelerate the redox kinetics of sulfur cathodes.Herein,this review f...Engineering transition metal compounds(TMCs)catalysts with excellent adsorption-catalytic ability has been one of the most effec-tive strategies to accelerate the redox kinetics of sulfur cathodes.Herein,this review focuses on engineering TMCs catalysts by cation doping/anion doping/dual doping,bimetallic/bi-anionic TMCs,and TMCs-based heterostructure composites.It is obvious that introducing cations/anions to TMCs or constructing heterostructure can boost adsorption-catalytic capacity by regulating the electronic structure including energy band,d/p-band center,electron filling,and valence state.Moreover,the elec-tronic structure of doped/dual-ionic TMCs are adjusted by inducing ions with different electronegativity,electron filling,and ion radius,resulting in electron redistribution,bonds reconstruction,induced vacancies due to the electronic interaction and changed crystal structure such as lat-tice spacing and lattice distortion.Different from the aforementioned two strategies,heterostructures are constructed by two types of TMCs with different Fermi energy levels,which causes built-in electric field and electrons transfer through the interface,and induces electron redistribution and arranged local atoms to regulate the electronic structure.Additionally,the lacking studies of the three strategies to comprehensively regulate electronic structure for improving catalytic performance are pointed out.It is believed that this review can guide the design of advanced TMCs catalysts for boosting redox of lithium sulfur batteries.展开更多
TiCl4/MgCl2/clay compound catalyst was prepared by chemical reaction. Exfoliated polypropylene (PP)/clay nanocomposites were synthesized by in situ polymerization with this compound catalyst. Effects of polymerizati...TiCl4/MgCl2/clay compound catalyst was prepared by chemical reaction. Exfoliated polypropylene (PP)/clay nanocomposites were synthesized by in situ polymerization with this compound catalyst. Effects of polymerization temperature, polymerization time, propylene pressure, solvent consumption and pre-treat time of catalyst on catalyst activity and catalytic stereospecificity were studied. Under optimal conditions, activity of the nano-compound catalyst is about 88.3 kg/(mol Ti-h). Isotacticity of PP obtained in the nanocomposites is in the range of 89%-99%, and its melting temperature is about 159℃. The weight-average molecular weight of PP can reach 6.7 × 10^5 - 7.8 × 10^5, and the molecular weight distribution is between 7.7 and 7.9.展开更多
The steam reforming of four bio-oil model compounds(acetic acid,ethanol,acetone and phenol) was investigated over Ni-based catalysts supported on Al2O3 modified by Mg,Ce or Co in this paper.The activation process ca...The steam reforming of four bio-oil model compounds(acetic acid,ethanol,acetone and phenol) was investigated over Ni-based catalysts supported on Al2O3 modified by Mg,Ce or Co in this paper.The activation process can improve the catalytic activity with the change of high-valence Ni(Ni2O3,NiO) to low-valence Ni(Ni,NiO).Among these catalysts after activation,the Ce-Ni/Co catalyst showed the best catalytic activity for the steam reforming of all the four model compounds.After long-term experiment at 700°C and the S/C ratio of 9,the Ce-Ni/Co catalyst still maintained excellent stability for the steam reforming of the simulated bio-oil(mixed by the four compounds with the equal masses).With CaO calcinated from calcium acetate as CO2 sorbent,the catalytic steam reforming experiment combined with continuous in situ CO2 adsorption was performed.With the comparison of the case without the adding of CO2 sorbent,the hydrogen concentration was dramatically improved from 74.8% to 92.3%,with the CO2 concentration obviously decreased from 19.90% to 1.88%.展开更多
Allantoin was synthesized with the yield as high as 68.5% using H3PW12O40. xH(2)O as catalyst. Optimum conditions for the synthesis were determined. It. was found that the heteropoly compound has higher catalytic acti...Allantoin was synthesized with the yield as high as 68.5% using H3PW12O40. xH(2)O as catalyst. Optimum conditions for the synthesis were determined. It. was found that the heteropoly compound has higher catalytic activity than conventional inorganic acid catalysts (such as hydrochloric acid, etc.)展开更多
Ni-Co bimetallic catalysts with different Ni/Co content were derived from cold plasma jet decomposition and reduction of hydrotalcite-like compounds containing Ni,Co,Mg and Al,and their catalytic performance was inves...Ni-Co bimetallic catalysts with different Ni/Co content were derived from cold plasma jet decomposition and reduction of hydrotalcite-like compounds containing Ni,Co,Mg and Al,and their catalytic performance was investigated with dry reforming of methane.Experimental results showed that the hydrotalcite-like precursors could be completely decomposed and partly reduced by cold plasma jet,and the Nicontained catalysts exhibited much higher activity than the catalyst without Ni.Especially,the catalyst with Ni/Co ratio of 8/2 achieved not only the highest conversions of 80.3%and 69.3%for CH4 and CO2,respectively,but also the best stability in 100 h testing.The catalysts were characterized by XRD,XPS,TEM and N2 adsorption techniques,and the results showed that the better performance of the 8Ni2Co bimetallic catalyst was attributed to its higher metal dispersion,smaller metal particle size,as well as the interaction effect between Ni and Co,which were brought by the special catalyst preparation method.展开更多
Sulphur-containing aromatic amines were prepared efficiently in good to excellent yields by reduction of the corresponding sulphur-containing aromatic nitro compounds with hydrazine hydrate in the presence of iron(Ⅲ...Sulphur-containing aromatic amines were prepared efficiently in good to excellent yields by reduction of the corresponding sulphur-containing aromatic nitro compounds with hydrazine hydrate in the presence of iron(Ⅲ) oxide-MgO catalyst. The catalyst exhibited high activity and stability for the reduction of sulphur-containing aromatic nitro compounds. The yields of sulphur-containing aromatic amines were up to 91-99 % at 355 K after reduction for 1-4 h over this catalyst.展开更多
Graphite intercalation compounds(GIC) were tested as an experimental model for studying the electronic effect of carbon support on the catalytic activity and poisoning tolerance of Pt catalyst for direct methanol fu...Graphite intercalation compounds(GIC) were tested as an experimental model for studying the electronic effect of carbon support on the catalytic activity and poisoning tolerance of Pt catalyst for direct methanol fuel cells. The GIC samples with different intercalation degrees were prepared by electrolyzing graphite flake in H2SO4 for varying the periods of time. The GIC-supported Pt catalyst was deposited electrochemically. The catalytic activity and poisoning tolerance of the GIC-supported Pt catalysts were evaluated. It was found that GIC with sulfate anion as intercalate was able to catalyze methanol electrooxidation, which could be related to the positive charges generated on the graphite layer upon intercalation. As intercalation degree increased, the catalytic activity of the GIC-supported Pt catalyst decreased while the poisoning tolerance improved. This suggests that electron donation from support to catalyst had great effect on both catalytic activity and poisoning tolerance of Pt catalyst. And intercalation can be adopted as another important way to make modification on carboneous catalyst support.展开更多
A new solvent free method for protection of carbonyl compounds as their thioacetals has been accomplished through the use of iodine supported on nanostructured pyrophosphate. Advantages of the methodology include very...A new solvent free method for protection of carbonyl compounds as their thioacetals has been accomplished through the use of iodine supported on nanostructured pyrophosphate. Advantages of the methodology include very short reaction time, the requirement for minimum amounts of catalyst, the remarkably simple experimental procedure, and no necessity for solvents or inert atmospheres, excellent yields and recyclability of the catalyst used. An efficient method for the chemoselective thioacetalization of ketones in the presence of aldehydes using I2/nanostructured pyrophosphate is also reported in this article. The nanostructured pyrophosphate was characterized by scanning electron microscopy, X-ray diffraction, infrared spectroscopy, Transmission electron microscopy and thermal gravimetric analysis, respectively.展开更多
基金The authors acknowledge funding from National Natural Science Foundation of China(52302307)Shaanxi Province(2023-ZDLGY-24,2023-JC-QN-0473)+2 种基金project funded by China Postdoctoral Science Foundation(2023MD734210)the Open Foundation of State Key Laboratory for Advanced Metals and Materials(2022-Z01)Shaanxi Provincial Department of Education industrialization project(21JC018).
文摘Engineering transition metal compounds(TMCs)catalysts with excellent adsorption-catalytic ability has been one of the most effec-tive strategies to accelerate the redox kinetics of sulfur cathodes.Herein,this review focuses on engineering TMCs catalysts by cation doping/anion doping/dual doping,bimetallic/bi-anionic TMCs,and TMCs-based heterostructure composites.It is obvious that introducing cations/anions to TMCs or constructing heterostructure can boost adsorption-catalytic capacity by regulating the electronic structure including energy band,d/p-band center,electron filling,and valence state.Moreover,the elec-tronic structure of doped/dual-ionic TMCs are adjusted by inducing ions with different electronegativity,electron filling,and ion radius,resulting in electron redistribution,bonds reconstruction,induced vacancies due to the electronic interaction and changed crystal structure such as lat-tice spacing and lattice distortion.Different from the aforementioned two strategies,heterostructures are constructed by two types of TMCs with different Fermi energy levels,which causes built-in electric field and electrons transfer through the interface,and induces electron redistribution and arranged local atoms to regulate the electronic structure.Additionally,the lacking studies of the three strategies to comprehensively regulate electronic structure for improving catalytic performance are pointed out.It is believed that this review can guide the design of advanced TMCs catalysts for boosting redox of lithium sulfur batteries.
基金financially supported by the National Natural Science Foundation of China(Nos.20774098,50973123, 50503023)the Scientific Research Startup Foundation of Qingdao University of Science and Technology
文摘TiCl4/MgCl2/clay compound catalyst was prepared by chemical reaction. Exfoliated polypropylene (PP)/clay nanocomposites were synthesized by in situ polymerization with this compound catalyst. Effects of polymerization temperature, polymerization time, propylene pressure, solvent consumption and pre-treat time of catalyst on catalyst activity and catalytic stereospecificity were studied. Under optimal conditions, activity of the nano-compound catalyst is about 88.3 kg/(mol Ti-h). Isotacticity of PP obtained in the nanocomposites is in the range of 89%-99%, and its melting temperature is about 159℃. The weight-average molecular weight of PP can reach 6.7 × 10^5 - 7.8 × 10^5, and the molecular weight distribution is between 7.7 and 7.9.
基金supported by the National Natural Science Foundation of China(No.51274066,51304048)the National Key Technology R&D Program of China(No.2013BAA03B03)the National Science Foundation for Post-doctoral Scientists of China(No.2013M541240)
文摘The steam reforming of four bio-oil model compounds(acetic acid,ethanol,acetone and phenol) was investigated over Ni-based catalysts supported on Al2O3 modified by Mg,Ce or Co in this paper.The activation process can improve the catalytic activity with the change of high-valence Ni(Ni2O3,NiO) to low-valence Ni(Ni,NiO).Among these catalysts after activation,the Ce-Ni/Co catalyst showed the best catalytic activity for the steam reforming of all the four model compounds.After long-term experiment at 700°C and the S/C ratio of 9,the Ce-Ni/Co catalyst still maintained excellent stability for the steam reforming of the simulated bio-oil(mixed by the four compounds with the equal masses).With CaO calcinated from calcium acetate as CO2 sorbent,the catalytic steam reforming experiment combined with continuous in situ CO2 adsorption was performed.With the comparison of the case without the adding of CO2 sorbent,the hydrogen concentration was dramatically improved from 74.8% to 92.3%,with the CO2 concentration obviously decreased from 19.90% to 1.88%.
文摘Allantoin was synthesized with the yield as high as 68.5% using H3PW12O40. xH(2)O as catalyst. Optimum conditions for the synthesis were determined. It. was found that the heteropoly compound has higher catalytic activity than conventional inorganic acid catalysts (such as hydrochloric acid, etc.)
基金supported by the National Natural Science Foundation of China(11075113)
文摘Ni-Co bimetallic catalysts with different Ni/Co content were derived from cold plasma jet decomposition and reduction of hydrotalcite-like compounds containing Ni,Co,Mg and Al,and their catalytic performance was investigated with dry reforming of methane.Experimental results showed that the hydrotalcite-like precursors could be completely decomposed and partly reduced by cold plasma jet,and the Nicontained catalysts exhibited much higher activity than the catalyst without Ni.Especially,the catalyst with Ni/Co ratio of 8/2 achieved not only the highest conversions of 80.3%and 69.3%for CH4 and CO2,respectively,but also the best stability in 100 h testing.The catalysts were characterized by XRD,XPS,TEM and N2 adsorption techniques,and the results showed that the better performance of the 8Ni2Co bimetallic catalyst was attributed to its higher metal dispersion,smaller metal particle size,as well as the interaction effect between Ni and Co,which were brought by the special catalyst preparation method.
文摘Sulphur-containing aromatic amines were prepared efficiently in good to excellent yields by reduction of the corresponding sulphur-containing aromatic nitro compounds with hydrazine hydrate in the presence of iron(Ⅲ) oxide-MgO catalyst. The catalyst exhibited high activity and stability for the reduction of sulphur-containing aromatic nitro compounds. The yields of sulphur-containing aromatic amines were up to 91-99 % at 355 K after reduction for 1-4 h over this catalyst.
基金Supported by the National Natural Science Foundation of China(No.20673068)
文摘Graphite intercalation compounds(GIC) were tested as an experimental model for studying the electronic effect of carbon support on the catalytic activity and poisoning tolerance of Pt catalyst for direct methanol fuel cells. The GIC samples with different intercalation degrees were prepared by electrolyzing graphite flake in H2SO4 for varying the periods of time. The GIC-supported Pt catalyst was deposited electrochemically. The catalytic activity and poisoning tolerance of the GIC-supported Pt catalysts were evaluated. It was found that GIC with sulfate anion as intercalate was able to catalyze methanol electrooxidation, which could be related to the positive charges generated on the graphite layer upon intercalation. As intercalation degree increased, the catalytic activity of the GIC-supported Pt catalyst decreased while the poisoning tolerance improved. This suggests that electron donation from support to catalyst had great effect on both catalytic activity and poisoning tolerance of Pt catalyst. And intercalation can be adopted as another important way to make modification on carboneous catalyst support.
文摘A new solvent free method for protection of carbonyl compounds as their thioacetals has been accomplished through the use of iodine supported on nanostructured pyrophosphate. Advantages of the methodology include very short reaction time, the requirement for minimum amounts of catalyst, the remarkably simple experimental procedure, and no necessity for solvents or inert atmospheres, excellent yields and recyclability of the catalyst used. An efficient method for the chemoselective thioacetalization of ketones in the presence of aldehydes using I2/nanostructured pyrophosphate is also reported in this article. The nanostructured pyrophosphate was characterized by scanning electron microscopy, X-ray diffraction, infrared spectroscopy, Transmission electron microscopy and thermal gravimetric analysis, respectively.