The effect of adding Co, Ni or La on the methanation activity of a Mo-based sulfur-resistant catalyst was investigated. As promoters, Co, Ni and La all improved the methanation activity of a 15% MOO3/ A1203 catalyst b...The effect of adding Co, Ni or La on the methanation activity of a Mo-based sulfur-resistant catalyst was investigated. As promoters, Co, Ni and La all improved the methanation activity of a 15% MOO3/ A1203 catalyst but to different extents. Similar improvements were also found when Co, Ni or La was added to a 15% MoO3/25%-CeO2-A1203 catalyst. The promotion effects of Co and Ni were better than that of La. However, the catalytic methanation activity deteriorated the most with time for the Ni-promoted catalyst. The used catalysts were analyzed by nitrogen adsorption measurement, X-ray diffraction and X-ray photoelectron spectroscopy.展开更多
The effect of promoter cobalt and the sequences of adding cobalt and molybdenum precursors on the performance of sulfur-resistant methanation were investigated. All these samples were prepared by impregnation method a...The effect of promoter cobalt and the sequences of adding cobalt and molybdenum precursors on the performance of sulfur-resistant methanation were investigated. All these samples were prepared by impregnation method and characterized by N2-adsorption, X-ray diffraction(XRD), temperature-programmed reduction(TPR) and laser Raman spectroscopy(LRS). The conversions of CO for Mo-Co/Al, Co-Mo/Al and CoMo/Al catalysts were 59.7%, 54.3% and 53.9%, respectively. Among these catalysts, the Mo-Co/Al catalyst prepared stepwisely by impregnating Mo precursor firstly showed the best catalytic performance. Meanwhile, the conversions of CO were 48.9% for Mo/Al catalyst and 10.5% for Co/Al catalyst. The addition of cobalt species could improve the catalytic activity of Mo/Al catalyst. The N2-adsorption results showed that Co-Mo/Al catalyst had the smallest specific surface area among these catalysts. CoMoO4species in CoMo/Al catalyst were detected with XRD, TPR and LRS. Moreover, crystal MoS2which was reported to be less active than amorphous MoS2was found in both Co-Mo/Al and CoMo/Al catalysts. Mo-Co/Al catalyst showed the best catalytic performance as it had an appropriate surface structure, i.e., no crystal MoS2and very little CoMoO4species.展开更多
In this paper, Ce_(0.2)Zr_(0.8)O_2 composite supports were prepared by different Ce-addition methods including impregnation of cerium(CeZr-imp), impregnation of citric acid and cerium(CeZr-CA) simultaneously and depos...In this paper, Ce_(0.2)Zr_(0.8)O_2 composite supports were prepared by different Ce-addition methods including impregnation of cerium(CeZr-imp), impregnation of citric acid and cerium(CeZr-CA) simultaneously and deposition precipitation method(CeZr-DP), respectively. The as-prepared supports were applied to prepare 10 wt% MoO_3/Ce_(0.2)Zr_(0.8)O_2 catalysts for sulfur-resistant methanation. The N_2 adsorption/desorption,X-ray diffraction(XRD), Raman spectroscopy(RS), X-ray photoelectron(XPS), temperature-programmed reduction by hydrogen(H_2-TPR) were undertaken to get textural properties, morphological information and structures of the catalysts. The results showed that Mo O_3 was highly dispersed on the surface of these three supports and Ce was mostly of coexisted in Ce^(4+)/Ce^(3+) redox pairs. Compared with Mo/CeZrimp, the CO conversion increased by 10% and 15% for Mo/CeZr-CA and Mo/CeZr-DP, respectively. This was mainly attributed to the larger specific surface area, Ce^(3+) concentration and content of active MoS_2 on the surface of catalysts.展开更多
CeOsupports were prepared by calcination or precipitation method and 5% MoO/CeOcatalysts were prepared by incipient-wetness impregnation method. The catalytic performance of the 5% MoO/CeOcatalysts toward sulfur-resis...CeOsupports were prepared by calcination or precipitation method and 5% MoO/CeOcatalysts were prepared by incipient-wetness impregnation method. The catalytic performance of the 5% MoO/CeOcatalysts toward sulfur-resistant methanation was investigated. The results showed that the Mo/Ce-1 catalysts with CeOsupport prepared by calcination method exhibited the best sulfur-resistant methanation activity and stability with CO conversion as high as 75% while the Mo/Ce-3 catalysts the poorest. The supports and catalysts were characterized by N-adsorption–desorption, temperature-programmed reduction（TPR）, X-ray diffraction（XRD）, Raman spectroscopy（RS） and scanning electron microscope（SEM）. The results indicated that the saturated monolayer loading MoOon Ce-3 support was lower than 5% and there were some crystalline MoOparticles on the surface of the Mo/Ce-3. The preparation method of CeOhad a big influence on the specific surface area, the crystalline of CeO, and the catalytic performance of the corresponding Mo-based catalyst for sulfur-resistant methanation.展开更多
The effect of boron on the performance of MoO_3/CeO_2–Al_2O_3 catalysts, which were prepared with impregnation method, was investigated. The catalysts were characterized with N_2 adsorption–desorption, XRD, H_2-TPR,...The effect of boron on the performance of MoO_3/CeO_2–Al_2O_3 catalysts, which were prepared with impregnation method, was investigated. The catalysts were characterized with N_2 adsorption–desorption, XRD, H_2-TPR, and NH_3-TPD, and were tested in sulfur-resistant methanation. The results indicated that the MoO_3/CeO_2–Al_2O_3 catalysts modified by boron showed higher catalytic performance in sulfur-resistant methanation. The CO conversion increased from 47% to 62% with 0.5 wt% boron content. When the content of boron was under 0.5 wt%, the results suggested there was an increase in the amorphous form of MoO_3 caused by the generation of weak and intermediate acid sites, which had weakened the interaction between the active components and supports. While, the catalyst added 2.0 wt% boron showed the strong acid sites and the largest crystalline size resulting in the uneven distribution of ceria.展开更多
In this study, the e ects of ZrO 2 carrier precursors, MoO 3 loading, and washing treatment on the catalytic performance of M o O 3 /ZrO 2 toward sulfur-resistant methanation were investigated. All the catalysts were ...In this study, the e ects of ZrO 2 carrier precursors, MoO 3 loading, and washing treatment on the catalytic performance of M o O 3 /ZrO 2 toward sulfur-resistant methanation were investigated. All the catalysts were prepared by co-precipitation method and further characterized by N 2 adsorption desorption, H 2 -temperature-programmed reduction, X-ray di raction, Raman spectroscopy and transmission electron microscopy. The prepared MoO 3 /ZrO 2 catalysts were tested in a continuous- ow pressurized xed bed reactor for CO methanation. The results revealed that the carrier precursors, MoO3 loading, and wash- ing treatment a ected not only the crystalline phase of Mo species but also the grain size of ZrO 2 carrier and consequently in uenced the MoO 3 /ZrO 2 activity toward sulfur-resistant methanation. The 25 wt% M oO 3 /ZrO 2 catalyst prepared using Zr(NO 3 ) 4 5H 2 O as the precursor and treated by water washing displayed the best activity for sulfur-resistant methanation due to its greater number of octahedral Mo species and smaller ZrO 2 grain size.展开更多
文摘The effect of adding Co, Ni or La on the methanation activity of a Mo-based sulfur-resistant catalyst was investigated. As promoters, Co, Ni and La all improved the methanation activity of a 15% MOO3/ A1203 catalyst but to different extents. Similar improvements were also found when Co, Ni or La was added to a 15% MoO3/25%-CeO2-A1203 catalyst. The promotion effects of Co and Ni were better than that of La. However, the catalytic methanation activity deteriorated the most with time for the Ni-promoted catalyst. The used catalysts were analyzed by nitrogen adsorption measurement, X-ray diffraction and X-ray photoelectron spectroscopy.
文摘The effect of promoter cobalt and the sequences of adding cobalt and molybdenum precursors on the performance of sulfur-resistant methanation were investigated. All these samples were prepared by impregnation method and characterized by N2-adsorption, X-ray diffraction(XRD), temperature-programmed reduction(TPR) and laser Raman spectroscopy(LRS). The conversions of CO for Mo-Co/Al, Co-Mo/Al and CoMo/Al catalysts were 59.7%, 54.3% and 53.9%, respectively. Among these catalysts, the Mo-Co/Al catalyst prepared stepwisely by impregnating Mo precursor firstly showed the best catalytic performance. Meanwhile, the conversions of CO were 48.9% for Mo/Al catalyst and 10.5% for Co/Al catalyst. The addition of cobalt species could improve the catalytic activity of Mo/Al catalyst. The N2-adsorption results showed that Co-Mo/Al catalyst had the smallest specific surface area among these catalysts. CoMoO4species in CoMo/Al catalyst were detected with XRD, TPR and LRS. Moreover, crystal MoS2which was reported to be less active than amorphous MoS2was found in both Co-Mo/Al and CoMo/Al catalysts. Mo-Co/Al catalyst showed the best catalytic performance as it had an appropriate surface structure, i.e., no crystal MoS2and very little CoMoO4species.
基金Financial supports from the National High Technology Research and Development Program of China (863 Project) (2015AA050504)the National Natural Science Foundation of China (21576203)
文摘In this paper, Ce_(0.2)Zr_(0.8)O_2 composite supports were prepared by different Ce-addition methods including impregnation of cerium(CeZr-imp), impregnation of citric acid and cerium(CeZr-CA) simultaneously and deposition precipitation method(CeZr-DP), respectively. The as-prepared supports were applied to prepare 10 wt% MoO_3/Ce_(0.2)Zr_(0.8)O_2 catalysts for sulfur-resistant methanation. The N_2 adsorption/desorption,X-ray diffraction(XRD), Raman spectroscopy(RS), X-ray photoelectron(XPS), temperature-programmed reduction by hydrogen(H_2-TPR) were undertaken to get textural properties, morphological information and structures of the catalysts. The results showed that Mo O_3 was highly dispersed on the surface of these three supports and Ce was mostly of coexisted in Ce^(4+)/Ce^(3+) redox pairs. Compared with Mo/CeZrimp, the CO conversion increased by 10% and 15% for Mo/CeZr-CA and Mo/CeZr-DP, respectively. This was mainly attributed to the larger specific surface area, Ce^(3+) concentration and content of active MoS_2 on the surface of catalysts.
基金Financial supports from the National High Technology Research and Development Program of China(863 Project)(2015AA050504)the National Natural Science Foundation of China(21576203)
文摘CeOsupports were prepared by calcination or precipitation method and 5% MoO/CeOcatalysts were prepared by incipient-wetness impregnation method. The catalytic performance of the 5% MoO/CeOcatalysts toward sulfur-resistant methanation was investigated. The results showed that the Mo/Ce-1 catalysts with CeOsupport prepared by calcination method exhibited the best sulfur-resistant methanation activity and stability with CO conversion as high as 75% while the Mo/Ce-3 catalysts the poorest. The supports and catalysts were characterized by N-adsorption–desorption, temperature-programmed reduction（TPR）, X-ray diffraction（XRD）, Raman spectroscopy（RS） and scanning electron microscope（SEM）. The results indicated that the saturated monolayer loading MoOon Ce-3 support was lower than 5% and there were some crystalline MoOparticles on the surface of the Mo/Ce-3. The preparation method of CeOhad a big influence on the specific surface area, the crystalline of CeO, and the catalytic performance of the corresponding Mo-based catalyst for sulfur-resistant methanation.
基金Supported by the National High Technology Research and Development Program of China(863 Project)(2015AA050504)the National Natural Science Foundation of China(21576203)
文摘The effect of boron on the performance of MoO_3/CeO_2–Al_2O_3 catalysts, which were prepared with impregnation method, was investigated. The catalysts were characterized with N_2 adsorption–desorption, XRD, H_2-TPR, and NH_3-TPD, and were tested in sulfur-resistant methanation. The results indicated that the MoO_3/CeO_2–Al_2O_3 catalysts modified by boron showed higher catalytic performance in sulfur-resistant methanation. The CO conversion increased from 47% to 62% with 0.5 wt% boron content. When the content of boron was under 0.5 wt%, the results suggested there was an increase in the amorphous form of MoO_3 caused by the generation of weak and intermediate acid sites, which had weakened the interaction between the active components and supports. While, the catalyst added 2.0 wt% boron showed the strong acid sites and the largest crystalline size resulting in the uneven distribution of ceria.
基金supported by the National Natural Science Foundation of China (No. 21576203)
文摘In this study, the e ects of ZrO 2 carrier precursors, MoO 3 loading, and washing treatment on the catalytic performance of M o O 3 /ZrO 2 toward sulfur-resistant methanation were investigated. All the catalysts were prepared by co-precipitation method and further characterized by N 2 adsorption desorption, H 2 -temperature-programmed reduction, X-ray di raction, Raman spectroscopy and transmission electron microscopy. The prepared MoO 3 /ZrO 2 catalysts were tested in a continuous- ow pressurized xed bed reactor for CO methanation. The results revealed that the carrier precursors, MoO3 loading, and wash- ing treatment a ected not only the crystalline phase of Mo species but also the grain size of ZrO 2 carrier and consequently in uenced the MoO 3 /ZrO 2 activity toward sulfur-resistant methanation. The 25 wt% M oO 3 /ZrO 2 catalyst prepared using Zr(NO 3 ) 4 5H 2 O as the precursor and treated by water washing displayed the best activity for sulfur-resistant methanation due to its greater number of octahedral Mo species and smaller ZrO 2 grain size.
