Energetic molecular perovskites have attracted widespread attention in the fields of energy materials due to their high detonation performance.In this work,we reported the effect of MgCo_(2)O_(4) nanosheets on the the...Energetic molecular perovskites have attracted widespread attention in the fields of energy materials due to their high detonation performance.In this work,we reported the effect of MgCo_(2)O_(4) nanosheets on the thermal decomposition of ammonium perchlorate(NH_(4)ClO_(4),AP)-based energetic molecular perovskites(AP-based energetic molecular perovskites).The morphology and structure of the MgCo_(2)O_(4) nanosheets were characterized.And their catalytic effect on the thermal decomposition of AP-based energetic molecular perovskites(H_2pz)[NH_(4)(ClO_(4))_(3)](PAP-4),(H_2dabco)[NH_(4)(ClO_(4))_(3)](DAP-4),(H_2mpz)[NH_(4)(ClO_(4))_(3)](PAP-M_(4)),and (H_2hpz)[NH_(4)(ClO_(4))_(3)](PAP-H_(4)) was analyzed.The results showed that MgCo_(2)O_(4) nanosheets had excellent intrinsically catalytic performance towards enhancing the thermal decomposition of AP-based energetic molecular perovskites.After adding MgCo_(2)O_(4) nanosheets,the thermal decomposition peak temperatures of PAP-4,DAP-4,PAP-M_(4),and PAP-H_(4) had been reduced by35.7℃,48.4℃,37.9℃,and 43.6℃,respectively.And the activation energy(Ea)of the thermal decomposition of AP-based energetic molecular perovskites had been reduced,the Eaof PAP-H_(4) decreased by 46.4 kJ/mol at most among them.The catalytic mechanism of MgCo_(2)O_(4) nanosheets for AP-based energetic molecular perovskites is analyzed.This work provides a reference for the future application of AP-based energetic molecular perovskites.展开更多
A series of single-phase T-structured NdSrCu 1-x Co x O 4-δ with oxygen vacancies and T -structured Sm 1.8 Ce 0.2 Cu 1-x Co x O 4-δ (x: 0–0.4) with oxygen excess were prepared using ultrasound-assisted citric ac...A series of single-phase T-structured NdSrCu 1-x Co x O 4-δ with oxygen vacancies and T -structured Sm 1.8 Ce 0.2 Cu 1-x Co x O 4-δ (x: 0–0.4) with oxygen excess were prepared using ultrasound-assisted citric acid complexing method, and characterized by means of techniques such as thermogravimetric analysis and NO temperature-programmed desorption (NO-TPD). The catalytic activities of these materials were evaluated for the decomposition of NO. It was found that the NdSrCu 1-x Co x O 4-δ catalysts were of oxygen vacancies whereas the Sm 1.8 Ce 0.2 Cu 1?x Co x O 4-δ ones possessed excessive oxygen (i.e., over-stoichiometric oxygen); with a rise in Co doping level, the oxygen vacancy density of NdSrCu 1-x Co x O 4-δ decreased while the over-stoichiometric oxygen amount of Sm 1.8 Ce 0.2 Cu 1-x Co x O 4-δ increased. The NO-TPD results revealed that NO could be activated much easier over the oxygen-deficient perovskite-like oxides than over the oxygen-excessive perovskite-like oxides, with the NdSrCuO 3.702 catalyst showing the best efficiency in activating NO molecules. Under the conditions of 1.0% NO/helium, 2800 hr -1 , and 600–900°C, the catalytic activity of NO decomposition followed the order of NdSrCuO 3.702 〉 NdSrCu 0.8 Co 0.2 O 3.736 〉 NdSrCu 0.6 Co 0.4 O 3.789 〉 Sm 1.8 Ce 0.2 Cu 0.6 Co 0.4 O 4.187 〉 Sm 1.8 Ce 0.2 Cu 0.8 Co 0.2 O 4.104 〉 Sm 1.8 Ce 0.2 CuO 4.045 , in concord with the sequence of decreasing oxygen vacancy or oxygen excess density. Based on the results, we concluded that the higher oxygen vacancy density and the stronger Cu 3+ /Cu 2+ redox ability of NdSrCu 1-x Co x O 4-δ account for the easier activation of NO and consequently improve the catalytic activity of NO decomposition over the catalysts.展开更多
Hairong Wang, Yaoqiang Chen, Qiulin Zhang, Qingchao Zhu, Maochu Gong, Ming Zhao( Key Laboratory of Green Chemistry & Technology of Ministry Education, College of Chemistry, Sichuan University, Chengdu 610064, Sichua...Hairong Wang, Yaoqiang Chen, Qiulin Zhang, Qingchao Zhu, Maochu Gong, Ming Zhao( Key Laboratory of Green Chemistry & Technology of Ministry Education, College of Chemistry, Sichuan University, Chengdu 610064, Sichuan, China展开更多
A series of monometallic nitrides and bimetallic nitrides were prepared by temperature-programmed reaction with NH3. The effects of Co, Ni and Fe additives and the synergic action between Fe, Co, Ni and Mo on the amm...A series of monometallic nitrides and bimetallic nitrides were prepared by temperature-programmed reaction with NH3. The effects of Co, Ni and Fe additives and the synergic action between Fe, Co, Ni and Mo on the ammonia decomposition activity were investigated. TPR-MS, XRD were also carried out to obtain better insight into the structure of the bimetallic nitride. The results of ammonia decomposition activity show that bimetallic nitrides are more active than monometallic nitrides or bimetallic oxides.展开更多
Pd/Ce0.8Zro.202 catalysts modified by cobalt were prepared by a sequential impregnation method and characterized by X-ray powder diffraction (XRD), N2 adsorption/desorption (Brunauer-Emmet-Teller), oxygen storage ...Pd/Ce0.8Zro.202 catalysts modified by cobalt were prepared by a sequential impregnation method and characterized by X-ray powder diffraction (XRD), N2 adsorption/desorption (Brunauer-Emmet-Teller), oxygen storage capacity (OSC), CO-chemisorption, H2-temperature-programmed reduction (H2-TPR) and X-ray photoelectron spectroscopy (XPS). The effect of Co on the performance of methanol decomposition was eval- uated at a fixed-bed microreactor. The results showed that the addition of Co can improve the oxygen storage capacity of the catalyst and the dispersion of Pd. XPS results indicated that Pd was in a partly oxidized (Pd6+, 1〈8〈2) state and Co2+ was present in Pd catalysts modified by Co. A 90% conversion of methanol was achieved at around 280 ℃ over Pd-Co/Ceo.8Zro.202 catalyst which was 20 ℃ lower than that over Pd/Ceo.sZro.202, indicating that both pd6+and Co2+ play an important role in improving the catalytic activity of methanol decomposition.展开更多
Li-O_(2) batteries provide an attractive and potential strategy for energy conversion and storage with high specific energy densities.However,large over-potential in oxygen evolution reactions (OER) caused by the deco...Li-O_(2) batteries provide an attractive and potential strategy for energy conversion and storage with high specific energy densities.However,large over-potential in oxygen evolution reactions (OER) caused by the decomposition obstacles of Li_(2)O_(2) seriously impedes its electrochemical performances.Herein,a novel N,O,S and F co-doping vesicular carbon was prepared by self-template pyrolysis method and used in LiO_(2) battery to tune the nucleation and decomposition of Li_(2)O_(2).The introduction of F in the carbon matrix with suitable content can regulate the adsorption of intermediates,through which the morphology of Li_(2)O_(2) can be controlled to film,favorable to its decomposition in charge process.The cathode based on the optimized F doped carbon vesicle exhibits improved electrochemical performances including a low over-potential,large capacity and a long-term stability.Density functional theory (DFT) results show that F and C in C–F bond hasve a strong interaction to Li and O in Li_(2)O_(2),respectively,which can enhance the transfer of electrons from Li_(2)O_(2) to the carbon matrix to generate hole polaron and thus accelerate the delithiation and decomposition of Li_(2)O_(2).This work provides a new sight into understanding the mechanism of nucleation and decomposition of Li_(2)O_(2) for the development of high-performance Li-O_(2) batteries.展开更多
Nanometer α-Fe2O3 catalysts were prepared by hydrolyzation in high temperature. Three kinds of precipitators, NaOH, (NH4)2CO3 and urea were used to compare the effect in the process of hydrolyzation. Nanometer size...Nanometer α-Fe2O3 catalysts were prepared by hydrolyzation in high temperature. Three kinds of precipitators, NaOH, (NH4)2CO3 and urea were used to compare the effect in the process of hydrolyzation. Nanometer sizer, transmission electron microscopy (TEM) and X-ray diffraction (XRD) were employed to test the profiles and diameters of the product particles. The test results indicate that the production is nanometer α-Fe2O3 with narrow particle size distribution (PSD) and good dispersibility. The catalysts are mixed with ammonia perchlorate (AP) in 1.0 wt.%. And the composite particles of catalysts with AP are prepared using a new solvent-nonsolvent method. Differential thermal analyzer (DTA) is employed to analysis the thermal decomposition of the composite particles and pure AP sample. The results imply that the thermal decomposition curve peaks of the samples in which nanometer α-Fe2O3 catalysts are added appear comparatively more ahead than that of pure AP sample. Among these mixtures added nanometer material, the smaller the particle diameter of catalyst is, the more ahead the thermal decomposition curve peaks of AP appear. The high and low temperature thermal decomposition curve peaks of AP mixed with the catalyst deposed by urea are more ahead of 77.8?℃ and 9.7?℃ than that of pure AP, respectively. The mechanism of the catalyst deposed by urea with smaller diameter and the distinct catalysis of the particles on the thermal decomposition of AP are discussed.展开更多
CO2 is a major component of the greenhouse gases, which causes the global warming. To reduce CO2 gas, high activity nanosized Ni+2 substituted Fe2TiO5 samples were synthesized by conventional ceramic method. The effe...CO2 is a major component of the greenhouse gases, which causes the global warming. To reduce CO2 gas, high activity nanosized Ni+2 substituted Fe2TiO5 samples were synthesized by conventional ceramic method. The effect of the composition of the synthesized ferrite on the H2-reduction and CO2-catalytic decomposition was investigated. Fe2TiO5 (iron titanate) phase that has a nanocrystallite size of -80 nm is formed as a result of heating Fe2O3 and TiO2 while the addition of NiO leads to the formation of new phases (-80 nm) NiTiO3 and NiFe2O4, but the mixed solid of NiO and Fe2O3 results in the formation of NiFe2O4 only. Samples with Ni^+2=0 shows the lowest reduction extent (20%); as the extent of Ni+2 increases, the extent of reduction increases. The increase in the reduction percent is attributed to the presence of NiTiO3 and NiFe2O4 phases, which are more reducible phases than Fe2TiO5. The CO2 decomposition reactions were monitored by thermogravimetric analysis (TGA) experiments. The oxidation of the H2-reduced Ni+2 substituted Fe2TiO5 at 500℃ was investigated. As Ni^+2 increases, the rate of reoxidation increases. Samples with the highest reduction extents gave the highest reoxidation extent, which is attributed to the highly porous nature and deficiency in oxygen due to the presence of metallic Fe, Ni and/or FeNi alloy. X-ray diffraction (XRD) and transmission electron microscopy (TEM) of oxidized samples show also the presence of carbon in the sample containing Ni+2〉0, which appears in the form of nanotubes (25 nm).展开更多
Characteristics of carbon deposition of CH 4 and C 2H 4 decomposition over supported Ni and Ni Ce catalysts were studied by using a pulse reaction as well as BET, TPR, XPS and hydrogen chemisorption techniques. It...Characteristics of carbon deposition of CH 4 and C 2H 4 decomposition over supported Ni and Ni Ce catalysts were studied by using a pulse reaction as well as BET, TPR, XPS and hydrogen chemisorption techniques. It is found that there is a metal semiconductor interaction (MScI) in the Ni Ce catalyst, and the effect of MScI on the carbon deposition of CH 4 decomposition is opposite to that of C 2H 4. A novel model of carbon deposition of CH 4 or C 2H 4 decomposition was proposed.展开更多
To study the thermal decomposition of Al/Zr H_(2)/PTFE with different Al particle size as well as mechanical strength and impact sensitivity under medium and low strain rates,molding-vacuum sintering was adopted to pr...To study the thermal decomposition of Al/Zr H_(2)/PTFE with different Al particle size as well as mechanical strength and impact sensitivity under medium and low strain rates,molding-vacuum sintering was adopted to prepare four groups of power materials and cylindrical specimens with different Al particle size.The active decomposition temperature of Zr H_(2) was obtained by TG-DSC,and the quasi-static mechanics/reaction characteristics as well as the impact sensitivity of the specimen were studied respectively by quasi-static compression and drop-hammer test.The results show that the yield strength of the material decreased with the increase of the Al particle size,while the compressive strength,failure strain and toughness increased first and then decreased,which reached the maximum values of 116.61 MPa,191%,and 119.9 MJ/m respectively when the Al particle size is 12-14 mm because of particle size grading.The specimens with the highest strength and toughness formed circumferential open cracks and reacted partly when pressed.Those with developmental cracks formed inside did not react.It is considered that fracture of specimens first triggered initial reaction between Al and PTFE to release an amount of heat.Then ZrH_(2) was activated and decomposed,and participated in subsequent reaction to generate Zr C.The impact sensitivity of the specimens decreased with the increase of Al particle size.展开更多
Nd-Co 3O 4 catalysts were prepared by hydrothermal and co-precipitation methods to catalyze the decomposition of N 2O. The catalysts prepared by hydrothermal method showed higher activity. Among the hydrothermal Nd-Co...Nd-Co 3O 4 catalysts were prepared by hydrothermal and co-precipitation methods to catalyze the decomposition of N 2O. The catalysts prepared by hydrothermal method showed higher activity. Among the hydrothermal Nd-Co 3O 4 catalysts, the catalyst with Nd/Co molar ratio of 0.01 had higher activity. 0.01Nd-Co 3O 4 catalyst was then impregnated by K 2CO 3 solution to prepare K-modified catalyst. The catalysts were characterized by means of X-ray diffraction (XRD), nitrogen physisorption, scanning electrons microscopy (SEM), X-ray photoelectron spectroscopy (XPS), hydrogen temperature-programmed reduction (H 2-TPR), and oxygen temperature-programmed desorption (O 2-TPD). The results show that Nd-Co 3O 4 and K-modified catalysts exhibit spinel structure. In contrast to bare Nd-Co 3O 4, the K-modified catalyst with higher activity is due to its weaker strength of Co-O bond and easier desorption of surface oxygen species. In addition, over 90% conversion of N 2O can be reached over 0.02K/0.01Nd-Co 3O 4 at 350 ℃ for 40 h under the co-presence of oxygen and steam in feed gases.展开更多
Hydrotalcite precursors of La modified Ni-Al2O3 and Ni-SiO2 catalysts prepared by co-precipitation method and the catalytic activities were examined for the production of COx-free H2 by CH4 decomposition. Physico-chem...Hydrotalcite precursors of La modified Ni-Al2O3 and Ni-SiO2 catalysts prepared by co-precipitation method and the catalytic activities were examined for the production of COx-free H2 by CH4 decomposition. Physico-chemical characteristics of fresh, reduced and used catalysts were evaluated by XRD, TPR and O2 pulse chemisorptions, TEM and BET-SA techniques. XRD studies showed phases due to hydrotalcite-like precursors in oven dried form produced dispersed NiO species upon calcination in static air above 450 C. Raman spectra of deactivated samples revealed the presence of both ordered and disordered forms of carbon. Ni-La-Al2O3catalyst with a mole ratio of Ni : La : Al = 2 : 0.1 : 0.9 exhibited tremendously high longevity with a hydrogen production rate of 1300 molH2 mol 1 Ni. A direct relationship between Ni metal surface area and hydrogen yields was established.展开更多
Methanol synthesis from hydrogenation of CO2 is investigated over Cu/ZnO/Al2O3 catalysts prepared by decomposition of M(Cu,Zn)-ammonia complexes (DMAC) at various temperatures.The catalysts were characterized in d...Methanol synthesis from hydrogenation of CO2 is investigated over Cu/ZnO/Al2O3 catalysts prepared by decomposition of M(Cu,Zn)-ammonia complexes (DMAC) at various temperatures.The catalysts were characterized in detail,including X-ray diffraction,N2 adsorption-desorption,N2O chemisorption,temperature-programmed reduction and evolved gas analyses.The influences of DMAC temperature,reaction temperature and specific Cu surface area on catalytic performance are investigated.It is considered that the aurichalcite phase in the precursor plays a key role in improving the physiochemical properties and activities of the final catalysts.The catalyst from rich-aurichalcite precursor exhibits large specific Cu surface area and high space time yield of methanol (212 g/(Lcat·h);T=513 K,p=3MPa,SV=12000 h-1).展开更多
Nanosized ZrO2 powder was prepared by evaporative decomposition of solution(EDS). The particle size is from 50 nm to 200 nm. This process has such advantages as high purity, precise compositional control, simple pro...Nanosized ZrO2 powder was prepared by evaporative decomposition of solution(EDS). The particle size is from 50 nm to 200 nm. This process has such advantages as high purity, precise compositional control, simple procedure and successive auto-operating. In this process, mixed solution of zirconium acetate and yttrium nitrate was atomized to from a fine mist and blown into the hot zone from the bottom of furnace. The solution was rapidly decomposed at 900℃ and the powder was collected by a filter system. The powder characteristics can be controlled by adjusting the concentration, droplet volume and decomposition temperature of the solution.展开更多
The thermal decomposition of 2, 2'-azobis (isobutyronitrile) (AIBN) in supercritical CO2 with cosolvent methanol or cyclohexane has been studied by using UV/Vis spectroscopic method at 335.15 K and at 12.0 MPa and...The thermal decomposition of 2, 2'-azobis (isobutyronitrile) (AIBN) in supercritical CO2 with cosolvent methanol or cyclohexane has been studied by using UV/Vis spectroscopic method at 335.15 K and at 12.0 MPa and 14.0 MPa. Both of the cosolvents can accelerate the decomposition rate, and the effect of methanol is more significant than that of the cyclohexane.展开更多
The paper presented the results regarding the decomposition of gaseous CF_2ClB_r by cold plasma method.After two minutes discharge,the maximum decomposition rate of 2660 Pa CF_2ClB_r pure and 2660 Pa CF_2ClBr plus 798...The paper presented the results regarding the decomposition of gaseous CF_2ClB_r by cold plasma method.After two minutes discharge,the maximum decomposition rate of 2660 Pa CF_2ClB_r pure and 2660 Pa CF_2ClBr plus 7980 Pa O_2 reached 60% and 80%,respectively.The pa- per also studied the cold plasma gas phase chemistry reaction mechanism of CF_2ClBr at low pres- sure,and the pressure effects of CF_2ClBr and added gas(He,N_2,O_2 and dry air)on the CF_2ClBr decomposition respectively by cold plasma method.These studies will be helpful to application of cold plasma method in the treatment of hazardous gaseous wastes.展开更多
基金the National Natural Science Foundation of China(Grant No.21975227)the Found of National defence Sci&Tech Laboratory(Grant No.6142602210306)。
文摘Energetic molecular perovskites have attracted widespread attention in the fields of energy materials due to their high detonation performance.In this work,we reported the effect of MgCo_(2)O_(4) nanosheets on the thermal decomposition of ammonium perchlorate(NH_(4)ClO_(4),AP)-based energetic molecular perovskites(AP-based energetic molecular perovskites).The morphology and structure of the MgCo_(2)O_(4) nanosheets were characterized.And their catalytic effect on the thermal decomposition of AP-based energetic molecular perovskites(H_2pz)[NH_(4)(ClO_(4))_(3)](PAP-4),(H_2dabco)[NH_(4)(ClO_(4))_(3)](DAP-4),(H_2mpz)[NH_(4)(ClO_(4))_(3)](PAP-M_(4)),and (H_2hpz)[NH_(4)(ClO_(4))_(3)](PAP-H_(4)) was analyzed.The results showed that MgCo_(2)O_(4) nanosheets had excellent intrinsically catalytic performance towards enhancing the thermal decomposition of AP-based energetic molecular perovskites.After adding MgCo_(2)O_(4) nanosheets,the thermal decomposition peak temperatures of PAP-4,DAP-4,PAP-M_(4),and PAP-H_(4) had been reduced by35.7℃,48.4℃,37.9℃,and 43.6℃,respectively.And the activation energy(Ea)of the thermal decomposition of AP-based energetic molecular perovskites had been reduced,the Eaof PAP-H_(4) decreased by 46.4 kJ/mol at most among them.The catalytic mechanism of MgCo_(2)O_(4) nanosheets for AP-based energetic molecular perovskites is analyzed.This work provides a reference for the future application of AP-based energetic molecular perovskites.
基金supported by the Natural Science Foundation of Beijing Municipality Key Class B Project (No.KZ200610005004)the Beijing Municipal Commission of Education (No. PHR200907105)the Academic Human Resources Development in Institutions of Higher Learning under the Jurisdiction of Beijing Municipality(PHR (IHLB))
文摘A series of single-phase T-structured NdSrCu 1-x Co x O 4-δ with oxygen vacancies and T -structured Sm 1.8 Ce 0.2 Cu 1-x Co x O 4-δ (x: 0–0.4) with oxygen excess were prepared using ultrasound-assisted citric acid complexing method, and characterized by means of techniques such as thermogravimetric analysis and NO temperature-programmed desorption (NO-TPD). The catalytic activities of these materials were evaluated for the decomposition of NO. It was found that the NdSrCu 1-x Co x O 4-δ catalysts were of oxygen vacancies whereas the Sm 1.8 Ce 0.2 Cu 1?x Co x O 4-δ ones possessed excessive oxygen (i.e., over-stoichiometric oxygen); with a rise in Co doping level, the oxygen vacancy density of NdSrCu 1-x Co x O 4-δ decreased while the over-stoichiometric oxygen amount of Sm 1.8 Ce 0.2 Cu 1-x Co x O 4-δ increased. The NO-TPD results revealed that NO could be activated much easier over the oxygen-deficient perovskite-like oxides than over the oxygen-excessive perovskite-like oxides, with the NdSrCuO 3.702 catalyst showing the best efficiency in activating NO molecules. Under the conditions of 1.0% NO/helium, 2800 hr -1 , and 600–900°C, the catalytic activity of NO decomposition followed the order of NdSrCuO 3.702 〉 NdSrCu 0.8 Co 0.2 O 3.736 〉 NdSrCu 0.6 Co 0.4 O 3.789 〉 Sm 1.8 Ce 0.2 Cu 0.6 Co 0.4 O 4.187 〉 Sm 1.8 Ce 0.2 Cu 0.8 Co 0.2 O 4.104 〉 Sm 1.8 Ce 0.2 CuO 4.045 , in concord with the sequence of decreasing oxygen vacancy or oxygen excess density. Based on the results, we concluded that the higher oxygen vacancy density and the stronger Cu 3+ /Cu 2+ redox ability of NdSrCu 1-x Co x O 4-δ account for the easier activation of NO and consequently improve the catalytic activity of NO decomposition over the catalysts.
基金the National Natural Science Foundation of China (20773090)the Specialized Research Fund for the Doctoral Program of Higher Education of China (20070610026, 200806100009)
文摘Hairong Wang, Yaoqiang Chen, Qiulin Zhang, Qingchao Zhu, Maochu Gong, Ming Zhao( Key Laboratory of Green Chemistry & Technology of Ministry Education, College of Chemistry, Sichuan University, Chengdu 610064, Sichuan, China
文摘A series of monometallic nitrides and bimetallic nitrides were prepared by temperature-programmed reaction with NH3. The effects of Co, Ni and Fe additives and the synergic action between Fe, Co, Ni and Mo on the ammonia decomposition activity were investigated. TPR-MS, XRD were also carried out to obtain better insight into the structure of the bimetallic nitride. The results of ammonia decomposition activity show that bimetallic nitrides are more active than monometallic nitrides or bimetallic oxides.
基金supported by the National Natural Science Foundation of China(No.21173153)Sichuan Province Science and Technology Support Projects(2012FZ0008)
文摘Pd/Ce0.8Zro.202 catalysts modified by cobalt were prepared by a sequential impregnation method and characterized by X-ray powder diffraction (XRD), N2 adsorption/desorption (Brunauer-Emmet-Teller), oxygen storage capacity (OSC), CO-chemisorption, H2-temperature-programmed reduction (H2-TPR) and X-ray photoelectron spectroscopy (XPS). The effect of Co on the performance of methanol decomposition was eval- uated at a fixed-bed microreactor. The results showed that the addition of Co can improve the oxygen storage capacity of the catalyst and the dispersion of Pd. XPS results indicated that Pd was in a partly oxidized (Pd6+, 1〈8〈2) state and Co2+ was present in Pd catalysts modified by Co. A 90% conversion of methanol was achieved at around 280 ℃ over Pd-Co/Ceo.8Zro.202 catalyst which was 20 ℃ lower than that over Pd/Ceo.sZro.202, indicating that both pd6+and Co2+ play an important role in improving the catalytic activity of methanol decomposition.
基金financially supported by the National Natural Science Foundation of China(Grant No.21701145)the China Postdoctoral Science Foundation(Grant Nos.2017M610459,2018T110739)。
文摘Li-O_(2) batteries provide an attractive and potential strategy for energy conversion and storage with high specific energy densities.However,large over-potential in oxygen evolution reactions (OER) caused by the decomposition obstacles of Li_(2)O_(2) seriously impedes its electrochemical performances.Herein,a novel N,O,S and F co-doping vesicular carbon was prepared by self-template pyrolysis method and used in LiO_(2) battery to tune the nucleation and decomposition of Li_(2)O_(2).The introduction of F in the carbon matrix with suitable content can regulate the adsorption of intermediates,through which the morphology of Li_(2)O_(2) can be controlled to film,favorable to its decomposition in charge process.The cathode based on the optimized F doped carbon vesicle exhibits improved electrochemical performances including a low over-potential,large capacity and a long-term stability.Density functional theory (DFT) results show that F and C in C–F bond hasve a strong interaction to Li and O in Li_(2)O_(2),respectively,which can enhance the transfer of electrons from Li_(2)O_(2) to the carbon matrix to generate hole polaron and thus accelerate the delithiation and decomposition of Li_(2)O_(2).This work provides a new sight into understanding the mechanism of nucleation and decomposition of Li_(2)O_(2) for the development of high-performance Li-O_(2) batteries.
文摘Nanometer α-Fe2O3 catalysts were prepared by hydrolyzation in high temperature. Three kinds of precipitators, NaOH, (NH4)2CO3 and urea were used to compare the effect in the process of hydrolyzation. Nanometer sizer, transmission electron microscopy (TEM) and X-ray diffraction (XRD) were employed to test the profiles and diameters of the product particles. The test results indicate that the production is nanometer α-Fe2O3 with narrow particle size distribution (PSD) and good dispersibility. The catalysts are mixed with ammonia perchlorate (AP) in 1.0 wt.%. And the composite particles of catalysts with AP are prepared using a new solvent-nonsolvent method. Differential thermal analyzer (DTA) is employed to analysis the thermal decomposition of the composite particles and pure AP sample. The results imply that the thermal decomposition curve peaks of the samples in which nanometer α-Fe2O3 catalysts are added appear comparatively more ahead than that of pure AP sample. Among these mixtures added nanometer material, the smaller the particle diameter of catalyst is, the more ahead the thermal decomposition curve peaks of AP appear. The high and low temperature thermal decomposition curve peaks of AP mixed with the catalyst deposed by urea are more ahead of 77.8?℃ and 9.7?℃ than that of pure AP, respectively. The mechanism of the catalyst deposed by urea with smaller diameter and the distinct catalysis of the particles on the thermal decomposition of AP are discussed.
文摘CO2 is a major component of the greenhouse gases, which causes the global warming. To reduce CO2 gas, high activity nanosized Ni+2 substituted Fe2TiO5 samples were synthesized by conventional ceramic method. The effect of the composition of the synthesized ferrite on the H2-reduction and CO2-catalytic decomposition was investigated. Fe2TiO5 (iron titanate) phase that has a nanocrystallite size of -80 nm is formed as a result of heating Fe2O3 and TiO2 while the addition of NiO leads to the formation of new phases (-80 nm) NiTiO3 and NiFe2O4, but the mixed solid of NiO and Fe2O3 results in the formation of NiFe2O4 only. Samples with Ni^+2=0 shows the lowest reduction extent (20%); as the extent of Ni+2 increases, the extent of reduction increases. The increase in the reduction percent is attributed to the presence of NiTiO3 and NiFe2O4 phases, which are more reducible phases than Fe2TiO5. The CO2 decomposition reactions were monitored by thermogravimetric analysis (TGA) experiments. The oxidation of the H2-reduced Ni+2 substituted Fe2TiO5 at 500℃ was investigated. As Ni^+2 increases, the rate of reoxidation increases. Samples with the highest reduction extents gave the highest reoxidation extent, which is attributed to the highly porous nature and deficiency in oxygen due to the presence of metallic Fe, Ni and/or FeNi alloy. X-ray diffraction (XRD) and transmission electron microscopy (TEM) of oxidized samples show also the presence of carbon in the sample containing Ni+2〉0, which appears in the form of nanotubes (25 nm).
文摘Characteristics of carbon deposition of CH 4 and C 2H 4 decomposition over supported Ni and Ni Ce catalysts were studied by using a pulse reaction as well as BET, TPR, XPS and hydrogen chemisorption techniques. It is found that there is a metal semiconductor interaction (MScI) in the Ni Ce catalyst, and the effect of MScI on the carbon deposition of CH 4 decomposition is opposite to that of C 2H 4. A novel model of carbon deposition of CH 4 or C 2H 4 decomposition was proposed.
基金financial support from the National Natural Science Foundation of China(General Program.Grant No.51673213)the National Natural Science Foundation of China(Youth Science Foundation.Grant No.51803235)。
文摘To study the thermal decomposition of Al/Zr H_(2)/PTFE with different Al particle size as well as mechanical strength and impact sensitivity under medium and low strain rates,molding-vacuum sintering was adopted to prepare four groups of power materials and cylindrical specimens with different Al particle size.The active decomposition temperature of Zr H_(2) was obtained by TG-DSC,and the quasi-static mechanics/reaction characteristics as well as the impact sensitivity of the specimen were studied respectively by quasi-static compression and drop-hammer test.The results show that the yield strength of the material decreased with the increase of the Al particle size,while the compressive strength,failure strain and toughness increased first and then decreased,which reached the maximum values of 116.61 MPa,191%,and 119.9 MJ/m respectively when the Al particle size is 12-14 mm because of particle size grading.The specimens with the highest strength and toughness formed circumferential open cracks and reacted partly when pressed.Those with developmental cracks formed inside did not react.It is considered that fracture of specimens first triggered initial reaction between Al and PTFE to release an amount of heat.Then ZrH_(2) was activated and decomposed,and participated in subsequent reaction to generate Zr C.The impact sensitivity of the specimens decreased with the increase of Al particle size.
基金The project was supported by the Shandong Natural Science Foundation (ZR2017MB020)Graduate Innovation Foundation of Yantai University (YDYB1909).
文摘Nd-Co 3O 4 catalysts were prepared by hydrothermal and co-precipitation methods to catalyze the decomposition of N 2O. The catalysts prepared by hydrothermal method showed higher activity. Among the hydrothermal Nd-Co 3O 4 catalysts, the catalyst with Nd/Co molar ratio of 0.01 had higher activity. 0.01Nd-Co 3O 4 catalyst was then impregnated by K 2CO 3 solution to prepare K-modified catalyst. The catalysts were characterized by means of X-ray diffraction (XRD), nitrogen physisorption, scanning electrons microscopy (SEM), X-ray photoelectron spectroscopy (XPS), hydrogen temperature-programmed reduction (H 2-TPR), and oxygen temperature-programmed desorption (O 2-TPD). The results show that Nd-Co 3O 4 and K-modified catalysts exhibit spinel structure. In contrast to bare Nd-Co 3O 4, the K-modified catalyst with higher activity is due to its weaker strength of Co-O bond and easier desorption of surface oxygen species. In addition, over 90% conversion of N 2O can be reached over 0.02K/0.01Nd-Co 3O 4 at 350 ℃ for 40 h under the co-presence of oxygen and steam in feed gases.
文摘Hydrotalcite precursors of La modified Ni-Al2O3 and Ni-SiO2 catalysts prepared by co-precipitation method and the catalytic activities were examined for the production of COx-free H2 by CH4 decomposition. Physico-chemical characteristics of fresh, reduced and used catalysts were evaluated by XRD, TPR and O2 pulse chemisorptions, TEM and BET-SA techniques. XRD studies showed phases due to hydrotalcite-like precursors in oven dried form produced dispersed NiO species upon calcination in static air above 450 C. Raman spectra of deactivated samples revealed the presence of both ordered and disordered forms of carbon. Ni-La-Al2O3catalyst with a mole ratio of Ni : La : Al = 2 : 0.1 : 0.9 exhibited tremendously high longevity with a hydrogen production rate of 1300 molH2 mol 1 Ni. A direct relationship between Ni metal surface area and hydrogen yields was established.
基金supported by the National Basic Research Program of China (No. 2011CB201404)the financial support of the State Key Laboratory for Oxo Synthesis and Selective Oxidation (OSSO) of China
文摘Methanol synthesis from hydrogenation of CO2 is investigated over Cu/ZnO/Al2O3 catalysts prepared by decomposition of M(Cu,Zn)-ammonia complexes (DMAC) at various temperatures.The catalysts were characterized in detail,including X-ray diffraction,N2 adsorption-desorption,N2O chemisorption,temperature-programmed reduction and evolved gas analyses.The influences of DMAC temperature,reaction temperature and specific Cu surface area on catalytic performance are investigated.It is considered that the aurichalcite phase in the precursor plays a key role in improving the physiochemical properties and activities of the final catalysts.The catalyst from rich-aurichalcite precursor exhibits large specific Cu surface area and high space time yield of methanol (212 g/(Lcat·h);T=513 K,p=3MPa,SV=12000 h-1).
文摘Nanosized ZrO2 powder was prepared by evaporative decomposition of solution(EDS). The particle size is from 50 nm to 200 nm. This process has such advantages as high purity, precise compositional control, simple procedure and successive auto-operating. In this process, mixed solution of zirconium acetate and yttrium nitrate was atomized to from a fine mist and blown into the hot zone from the bottom of furnace. The solution was rapidly decomposed at 900℃ and the powder was collected by a filter system. The powder characteristics can be controlled by adjusting the concentration, droplet volume and decomposition temperature of the solution.
文摘The thermal decomposition of 2, 2'-azobis (isobutyronitrile) (AIBN) in supercritical CO2 with cosolvent methanol or cyclohexane has been studied by using UV/Vis spectroscopic method at 335.15 K and at 12.0 MPa and 14.0 MPa. Both of the cosolvents can accelerate the decomposition rate, and the effect of methanol is more significant than that of the cyclohexane.
文摘The paper presented the results regarding the decomposition of gaseous CF_2ClB_r by cold plasma method.After two minutes discharge,the maximum decomposition rate of 2660 Pa CF_2ClB_r pure and 2660 Pa CF_2ClBr plus 7980 Pa O_2 reached 60% and 80%,respectively.The pa- per also studied the cold plasma gas phase chemistry reaction mechanism of CF_2ClBr at low pres- sure,and the pressure effects of CF_2ClBr and added gas(He,N_2,O_2 and dry air)on the CF_2ClBr decomposition respectively by cold plasma method.These studies will be helpful to application of cold plasma method in the treatment of hazardous gaseous wastes.