A support(denoted AM) was prepared using pseudo-boehmite and mordenite.Ni-B and NiPtB amorphous catalysts were prepared on the support by the impregnation method followed by chemical reduction with a KBH4 solution.And...A support(denoted AM) was prepared using pseudo-boehmite and mordenite.Ni-B and NiPtB amorphous catalysts were prepared on the support by the impregnation method followed by chemical reduction with a KBH4 solution.And the catalysts were characterized by X-ray diffraction(XRD),environment scanning electron microscope(ESEM),inductively coupled plasma(ICP),H2-temperature programmed reduction(H2-TPR),differential thermal analysis(DTA),and BET.Benzene hydrogenation was used as a probe reaction to evaluate the effect of addition of small quantities of Pt on the NiB/AM catalyst.The results show that Pt can promote the reduction of NiO and the formation of active sites,leading to smaller catalyst particles and better dispersion of active metal particles on the support.The catalytic activity,sulfur resistance and thermal stability were remarkably improved by Pt doping of the NiB/AM catalyst.展开更多
Pd/oxide/cordierite monolithic catalysts(oxide = Al_2O_3, SiO_2 and SiO_2\\Al_2O_3) were prepared by the impregnation method. The results of ICP, XRD, SEM–EDX, XPS and N_2 adsorption–desorption measurements revealed...Pd/oxide/cordierite monolithic catalysts(oxide = Al_2O_3, SiO_2 and SiO_2\\Al_2O_3) were prepared by the impregnation method. The results of ICP, XRD, SEM–EDX, XPS and N_2 adsorption–desorption measurements revealed that the Pd penetration depth increased with increasing the thickness of oxide layer, and the catalysts with Al_2O_3 layers had the larger pore size than those with SiO_2 and SiO_2\\Al_2O_3 layers. Catalytic hydrogenation of 2-ethylanthraquinone(eA Q), a key step of the H_2O_2 production by the anthraquinone process, over the various monolithic catalysts(60 °C, atmosphere pressure) showed that the monolithic catalyst with the moderate thickness of Al_2O_3 layer(about 6 μm) exhibited the highest conversion of e AQ(99.1%) and hydrogenation efficiency(10.0 g·L^(-1)). This could be ascribed to the suitable Pd penetration depth and the larger pore size, which provides a balance between the distribution of Pd and accessibility of active sites by the reactants.展开更多
The effect of ammonia on the catalytic performance for 1-methylnaphthalene(1-MN) selective hydrogenation saturation was studied with Co-Mo/γ-Al_2O_3, Ni-W/γ-Al_2O_3, Ni-Mo/γ-Al_2O_3, and Ni-Mo-W/γ-Al_2O_3 catalyst...The effect of ammonia on the catalytic performance for 1-methylnaphthalene(1-MN) selective hydrogenation saturation was studied with Co-Mo/γ-Al_2O_3, Ni-W/γ-Al_2O_3, Ni-Mo/γ-Al_2O_3, and Ni-Mo-W/γ-Al_2O_3 catalysts. The results indicated that Ni-Mo-W/γ-Al_2O_3 catalyst exhibited the best performance for saturation of 1-MN. The introduction of NH3 remarkably inhibited the hydrogenation of 1-MN in the dynamic control area, but it had no effect in the thermodynamic control area. Besides, the mono-aromatics selectivity on the Ni-Mo-W and Ni-Mo catalysts was enhanced. However, it had little effect on the Ni-W and Co-Mo catalysts.展开更多
The effect of catalyst properties on residue oil hydroconversion was studied at moderate operating conditions(at a temperature of 400 ℃, an initial hydrogen pressure of 10 MPa, and a reaction time of 4 h) in a batch ...The effect of catalyst properties on residue oil hydroconversion was studied at moderate operating conditions(at a temperature of 400 ℃, an initial hydrogen pressure of 10 MPa, and a reaction time of 4 h) in a batch mode slurry phase with different catalyst samples. The results showed that the catalyst acidity had a good effect on residue conversion and MCR(micro carbon residue) conversion but brought about higher coke yield. Residue conversion was thermally induced but the catalyst acidity changed its conversion route. A catalyst with higher metal loading, higher hydrogenation activity and appropriate pore size had higher sulfur and metal removal rate, higher MCR conversion and also a lower coke formation. The activity of spent commercial catalyst AS1 and DS1 was slightly lower than the corresponding fresh ones but was still high enough for residue oil hydroconversion. It assumes that the role of the catalyst is to activate hydrogen species toward reaction with an aromatic carbon radical to yield a cyclohexadienyl type intermediate which will turn into liquid and also to absorb the mesophase which can easily aggregate to form coke.展开更多
The design of non-noble metal heterogeneous catalyst with superior performance for selective hydrogenation or transfer hydrogenation of nitroarenes to amines is significant but challenging.Herein,a single-atom Fe supp...The design of non-noble metal heterogeneous catalyst with superior performance for selective hydrogenation or transfer hydrogenation of nitroarenes to amines is significant but challenging.Herein,a single-atom Fe supported by nitrogen-doped carbon(Fe_(1)/N-C)catalyst is reported.The Fe_(1)/N-C sample shows superior performances for the selective hydrogenation and transfer hydrogenation of nitrobenzene to aniline at different temperatures.Density functional theory(DFT)calculations show that the superior catalytic activity for the selective hydrogenation at lower temperatures could be attributed to the effective activation of the reactant and intermediates by the Fe_(1)/N-C.Moreover,the excellent performance of Fe_(1)/N-C for the selective transfer hydrogenation could be attributed to that the reaction energy barrier for dehydrogenation of isopropanol can be overcome by elevated temperatures.展开更多
基金Supported by the Overseas Scholars of Heilongjiang Province of China (1151hq006)
文摘A support(denoted AM) was prepared using pseudo-boehmite and mordenite.Ni-B and NiPtB amorphous catalysts were prepared on the support by the impregnation method followed by chemical reduction with a KBH4 solution.And the catalysts were characterized by X-ray diffraction(XRD),environment scanning electron microscope(ESEM),inductively coupled plasma(ICP),H2-temperature programmed reduction(H2-TPR),differential thermal analysis(DTA),and BET.Benzene hydrogenation was used as a probe reaction to evaluate the effect of addition of small quantities of Pt on the NiB/AM catalyst.The results show that Pt can promote the reduction of NiO and the formation of active sites,leading to smaller catalyst particles and better dispersion of active metal particles on the support.The catalytic activity,sulfur resistance and thermal stability were remarkably improved by Pt doping of the NiB/AM catalyst.
基金Supported by the Sinopec Corp.Scientific Research Projects(414076)
文摘Pd/oxide/cordierite monolithic catalysts(oxide = Al_2O_3, SiO_2 and SiO_2\\Al_2O_3) were prepared by the impregnation method. The results of ICP, XRD, SEM–EDX, XPS and N_2 adsorption–desorption measurements revealed that the Pd penetration depth increased with increasing the thickness of oxide layer, and the catalysts with Al_2O_3 layers had the larger pore size than those with SiO_2 and SiO_2\\Al_2O_3 layers. Catalytic hydrogenation of 2-ethylanthraquinone(eA Q), a key step of the H_2O_2 production by the anthraquinone process, over the various monolithic catalysts(60 °C, atmosphere pressure) showed that the monolithic catalyst with the moderate thickness of Al_2O_3 layer(about 6 μm) exhibited the highest conversion of e AQ(99.1%) and hydrogenation efficiency(10.0 g·L^(-1)). This could be ascribed to the suitable Pd penetration depth and the larger pore size, which provides a balance between the distribution of Pd and accessibility of active sites by the reactants.
文摘The effect of ammonia on the catalytic performance for 1-methylnaphthalene(1-MN) selective hydrogenation saturation was studied with Co-Mo/γ-Al_2O_3, Ni-W/γ-Al_2O_3, Ni-Mo/γ-Al_2O_3, and Ni-Mo-W/γ-Al_2O_3 catalysts. The results indicated that Ni-Mo-W/γ-Al_2O_3 catalyst exhibited the best performance for saturation of 1-MN. The introduction of NH3 remarkably inhibited the hydrogenation of 1-MN in the dynamic control area, but it had no effect in the thermodynamic control area. Besides, the mono-aromatics selectivity on the Ni-Mo-W and Ni-Mo catalysts was enhanced. However, it had little effect on the Ni-W and Co-Mo catalysts.
文摘The effect of catalyst properties on residue oil hydroconversion was studied at moderate operating conditions(at a temperature of 400 ℃, an initial hydrogen pressure of 10 MPa, and a reaction time of 4 h) in a batch mode slurry phase with different catalyst samples. The results showed that the catalyst acidity had a good effect on residue conversion and MCR(micro carbon residue) conversion but brought about higher coke yield. Residue conversion was thermally induced but the catalyst acidity changed its conversion route. A catalyst with higher metal loading, higher hydrogenation activity and appropriate pore size had higher sulfur and metal removal rate, higher MCR conversion and also a lower coke formation. The activity of spent commercial catalyst AS1 and DS1 was slightly lower than the corresponding fresh ones but was still high enough for residue oil hydroconversion. It assumes that the role of the catalyst is to activate hydrogen species toward reaction with an aromatic carbon radical to yield a cyclohexadienyl type intermediate which will turn into liquid and also to absorb the mesophase which can easily aggregate to form coke.
基金the National Key R&D Program of China(2018YFA0702003)the National Natural Science Foundation of China(21890383,21671117,21871159 and21901135)the Science and Technology Key Project of Guangdong Province of China(2020B010188002)。
文摘The design of non-noble metal heterogeneous catalyst with superior performance for selective hydrogenation or transfer hydrogenation of nitroarenes to amines is significant but challenging.Herein,a single-atom Fe supported by nitrogen-doped carbon(Fe_(1)/N-C)catalyst is reported.The Fe_(1)/N-C sample shows superior performances for the selective hydrogenation and transfer hydrogenation of nitrobenzene to aniline at different temperatures.Density functional theory(DFT)calculations show that the superior catalytic activity for the selective hydrogenation at lower temperatures could be attributed to the effective activation of the reactant and intermediates by the Fe_(1)/N-C.Moreover,the excellent performance of Fe_(1)/N-C for the selective transfer hydrogenation could be attributed to that the reaction energy barrier for dehydrogenation of isopropanol can be overcome by elevated temperatures.
