Ga_2O_3改性Cu/SiO_2催化剂降低水蒸气催化重整产物中CO选择性
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摘要
采用蒸氨法制备的xGa-Cu/SiO_2催化剂可以同时产生Cu~0和Cu~+物种,加入Ga后催化剂的二甲醚水蒸气重整反应活性和选择性都有很大程度的提高,其中5Ga-Cu/SiO_2催化剂在380°C时的二甲醚转化率为99.8%,CO选择性为4.8%。通过透射电子显微镜(TEM),氢气-程序升温还原(H_2-TPR),N_2O滴定和X射线光电子能谱(XPS)结果发现,Ga与Cu物种之间的相互作用,一方面可以提高Cu物种的分散度,另一方面可以促进Cu~+的形成。通过改变Ga负载量可以调变Cu~+/(Cu~0+Cu~+)的比例,氢气的时空收率结果表明,Ga通过调变Cu~+/(Cu~0+Cu~+)影响催化活性,并且当Cu~+/(Cu~0+Cu~+)=0.5时,氢气时空收率达到最大值为5.02mol·g~(-1)·h~(-1)。程序升温表面反应(TPSR)结果表明,Ga通过促进水气变换反应提高反应产物CO_2选择性。
Dimethyl ether(DME) is considered a promising energy source and clean fuel for the next generation, with its high hydrogen content, and non-toxicity compared with methanol. In addition, it is easy to store and transport. DME steam reforming(SR) has received considerable attention for its applicability in the production of hydrogen for fuel cell applications. Generally, DME SR consists of two steps: DME hydrolysis and methanol SR. DME hydrolysis often occurs on an acidic catalyst, such as γ-Al_2O_3. Methanol SR in Cu-based catalysts requires both Cu~0 and Cu~+ as the active sites; moreover, the relative ratios of Cu~0 and Cu~+ can influence the catalytic performance. In addition, the byproduct of CO also commonly exists in DME SR, and a small amount of CO can poison Pt electrodes of fuel cells. Therefore, it is necessary to reduce the concentration of the generated CO in DME SR. Herein, using an ammonia-evaporation method, we synthesized a Cu/SiO_2 catalyst, which can simultaneously generate the dual copper species of Cu~0 and Cu~+ by reduction. After modification with Ga_2O_3, the xG a-Cu/SiO_2 catalysts show much improved catalytic activity and decreased CO selectivity. The Cu/SiO_2 catalyst shows a DME conversion of 90.7% and CO selectivity of 11.5% at 380 °C. The 5 Ga-Cu/SiO_2 catalyst, with a loading amount of Ga_2O_3 of 5%(w, based on the weight of Cu), shows the best performance, with a DME conversion of 99.8% and CO selectivity of 4.8% under the same conditions. The measurement of apparent activation energies shows that the addition of Ga_2O_3 cannot change the reaction path. By multiple characterization methods, we demonstrated that the improved performance can be ascribed to the following two aspects. First, our characterization results show that the loaded Ga_2O_3 is highly dispersed on the Cu/SiO_2 catalyst, which can increase the interaction between Ga and Cu species. This can not only improve the dispersion of copper species(Cu~0 and Cu~+) on the catalysts, but can also adjust the ratios of Cu~+/(Cu~0 + Cu~+). The H_2 production rate shows a typical volcano curve owing to the ratio of Cu~+/(Cu~0 + Cu~+), and reaches a maximum of 5.02 mol·g~(-1)·h~(-1) at Cu~+/(Cu~0 + Cu~+) = 0.5 for the 5 Ga-Cu/SiO_2 catalyst. We conclude that the interaction between Ga and Cu species and the synergistic effect between Cu~0 and Cu~+ result in the promoted catalytic activity for DME SR. Second, by using a temperature-programmed surface reaction(TPSR), we showed that the addition of Ga_2O_3 can efficiently promote the water–gas shift reaction, thereby reducing the CO selectivity in DME SR. Thus, Ga_2O_3 suppresses the generation of CO, leading to the low CO selectivity and high CO_2 selectivity. In summary, the Ga_2O_3-modified Cu/SiO_2 catalyst yields reformates with low CO selectivity and high catalytic activity for DME SR. Our work provides a novel approach to designing a highly efficient Cu-based catalyst for catalytic SR systems.
Dimethyl ether(DME) is considered a promising energy source and clean fuel for the next generation, with its high hydrogen content, and non-toxicity compared with methanol. In addition, it is easy to store and transport. DME steam reforming(SR) has received considerable attention for its applicability in the production of hydrogen for fuel cell applications. Generally, DME SR consists of two steps: DME hydrolysis and methanol SR. DME hydrolysis often occurs on an acidic catalyst, such as γ-Al_2O_3. Methanol SR in Cu-based catalysts requires both Cu~0 and Cu~+ as the active sites; moreover, the relative ratios of Cu~0 and Cu~+ can influence the catalytic performance. In addition, the byproduct of CO also commonly exists in DME SR, and a small amount of CO can poison Pt electrodes of fuel cells. Therefore, it is necessary to reduce the concentration of the generated CO in DME SR. Herein, using an ammonia-evaporation method, we synthesized a Cu/SiO_2 catalyst, which can simultaneously generate the dual copper species of Cu~0 and Cu~+ by reduction. After modification with Ga_2O_3, the xG a-Cu/SiO_2 catalysts show much improved catalytic activity and decreased CO selectivity. The Cu/SiO_2 catalyst shows a DME conversion of 90.7% and CO selectivity of 11.5% at 380 °C. The 5 Ga-Cu/SiO_2 catalyst, with a loading amount of Ga_2O_3 of 5%(w, based on the weight of Cu), shows the best performance, with a DME conversion of 99.8% and CO selectivity of 4.8% under the same conditions. The measurement of apparent activation energies shows that the addition of Ga_2O_3 cannot change the reaction path. By multiple characterization methods, we demonstrated that the improved performance can be ascribed to the following two aspects. First, our characterization results show that the loaded Ga_2O_3 is highly dispersed on the Cu/SiO_2 catalyst, which can increase the interaction between Ga and Cu species. This can not only improve the dispersion of copper species(Cu~0 and Cu~+) on the catalysts, but can also adjust the ratios of Cu~+/(Cu~0 + Cu~+). The H_2 production rate shows a typical volcano curve owing to the ratio of Cu~+/(Cu~0 + Cu~+), and reaches a maximum of 5.02 mol·g~(-1)·h~(-1) at Cu~+/(Cu~0 + Cu~+) = 0.5 for the 5 Ga-Cu/SiO_2 catalyst. We conclude that the interaction between Ga and Cu species and the synergistic effect between Cu~0 and Cu~+ result in the promoted catalytic activity for DME SR. Second, by using a temperature-programmed surface reaction(TPSR), we showed that the addition of Ga_2O_3 can efficiently promote the water–gas shift reaction, thereby reducing the CO selectivity in DME SR. Thus, Ga_2O_3 suppresses the generation of CO, leading to the low CO selectivity and high CO_2 selectivity. In summary, the Ga_2O_3-modified Cu/SiO_2 catalyst yields reformates with low CO selectivity and high catalytic activity for DME SR. Our work provides a novel approach to designing a highly efficient Cu-based catalyst for catalytic SR systems.
引文
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