Research progresses in the hydrogenation of carbon dioxide to certain hydrocarbon products
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摘要: 化石资源的大量使用导致CO2的大量排放,带来了严重的环境问题。与此同时,CO2又是一种清洁、无毒的含碳资源。将CO2作为原料,直接转化制备重要化学品,不仅可以减缓温室效应,同时也是一条有效利用含碳资源制备清洁燃料和化学品的新路线。本文概述了近年来关于CO2加氢制备一些烃类化合物(主要包括甲烷、烯烃和芳烃)的相关研究进展;重点分析了CO2加氢制烃类化合物相关过程催化剂的研发状态和对催化反应机理的认识,并对CO2加氢转化利用的未来发展进行了展望。Abstract: Accompanying with the rapid consumption of fossil fuel resources, a huge amount of CO2 has being released into the atmosphere, which brings serious environmental concerns. However, CO2 can also be considered as a clean and non-toxic carbon resource; the utilization of CO2 by converting it into various hydrocarbons can not only alleviate the greenhouse effect, but also provide a new sustainable route to produce clean fuel and chemical products. In this paper, we attempt to make a review on the recent research progresses in the hydrogenation of CO2 to certain hydrocarbons (including methane, olefins and aromatics) in recent years; in particular, the advance in the development of efficient catalysts for the hydrogenation of CO2 to methane, light olefins and aromatics as well as in the exploration of catalytic reaction mechanisms were retrospectively summarized. Lastly, we would like to have an outlook on the possible trends in the utilization of CO2 as a carbon resource through hydrogenation.
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Key words:
- carbon dioxide hydrogenation /
- methane /
- light olefins /
- aromatics /
- reaction mechanism
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图 3 Rh/TiO2催化剂上CO2甲烷化反应,各温度下甲烷生成速率随Rh粒径的变化(a)以及生成甲烷的TOF值随Rh粒径的变化(b)[18]
Figure 3 CO2 methanation over the Rh/TiO2 catalyst: (a) relationship between the methane formation rate and Rh particle size at different temperatures; (b) relationship between the TOF value of methane formation and Rh particle size at different temperatures[18](with permission from Elsevier)
图 5 Na作助剂Fe基催化剂上的CO2加氢制烯烃反应
Figure 5 Hydrogenation of CO2 to light olefins over Na-promoted Fe-based catalysts
(a): variance of chain growth probability (FTY) and olefins-to-paraffins (O/P) ratio with the content of Na; (b): CH4, $ {\rm{C}}^{0}_{2-7} $ alkanes and $ {\rm{C}}^{=}_{2-7} $ olefins yields with the Na content[31](with permission from Elsevier)
表 1 CO2加氢制烃类化合物的基础热力学数据
Table 1 Thermodynamic data for the hydrogenation of CO2 to certain hydrocarbons
Entry Reaction ΔrH0298 K/(kJ·mol−1) ΔrG0298 K/(kJ·mol−1) n(H2)/n(CO2) ΔrH0298 K/n(CO2)/(kJ·mol−1) 1 CO2 + 4H2 = CH4 + 2H2O −164.94 −113.51 4 −164.94 2 2CO2 + 6H2 = C2H4 + 4H2O −127.99 −57.42 3 −64.00 3 3CO2 + 9H2 = C3H6 + 6H2O −249.96 −125.57 3 −83.32 4 4CO2 + 12H2 = C4H8 + 8H2O −360.64 −179.74 3 −90.16 5 6CO2 + 15H2 = C6H6 + 12H2O −457.83 −246.98 2.5 −76.31 6 7CO2 + 18H2 = C7H8 + 14H2O −580.89 −317.39 2.6 −82.98 7 8CO2 + 21H2 = p-C8H10 + 16H2O −703.07 −381.02 2.6 −87.88 表 2 Fe基催化剂上K掺杂量对于其CO2加氢活性的影响[30]
Table 2 Effect of K doping amount on the activity of Fe-based catalyst in the hydrogenation of CO2 to light olefins[30](with permission from Elsevier)
K loading w/% CO2 conversion/% Selectivity/% Hydrocarbon distribution/% ${\rm{C} }^{=}_{{2-4}}$ yield/% CO C−H C-oxy CH4 ${\rm{C} }^{=}_{{2-4}}$ ${\rm{C} }^{0}_{{2-4}}$ ${\rm{C} }^{=}_{{5+}}$ ${\rm{C} }^{0}_{{5+}}$ 0 5.6 12 88 0.0 62 0.0 38 0.0 0.9 0.0 1 5.0 10 89 1.3 45 2.1 48 0.1 5.2 0.1 2 37 5.8 86 7.8 28 25 34 6.8 3.4 7.9 5 38 7.3 78 15 21 34 14 19 11 10 10 27 7.2 89 4.3 22 39 13 18 7.2 9.3 16 25 8.3 79 13 23 37 18 21 6.7 7.3 32 25 20 71 9.6 24 36 11 22 6.5 6.3 表 3 部分金属氧化物与SAPO-34复合的双功能催化剂对CO2加氢制烯烃反应性能
Table 3 Performance of certain bifunctional catalysts composed of metal oxides and SAPO-34 in the hydrogenation of CO2 to light olefins
表 4 用于CO2加氢制芳烃反应的部分双功能催化剂性能对比
Table 4 Performances of certain bifunctional catalysts in the hydrogenation of CO2 to aromatics
Catalyst t/℃ p/MPa GHSV/(mL·g−1·h−1) CO2 conv./% Aromatic sel./% CO sel./% Ref. ZnCrOx/Zn-ZSM-5 320 5 2000 19.9 81.1 (in C5+) 70.0 [68] ZnCr2O4/H-ZSM-5 350 4 1200 23.1 85.3 27.8 [70] ZnO-ZrO2/H-ZSM-5 340 4 7200 16.0 76.0 34.3 [45] ZnO-ZrO2/H-ZSM-5 340 3 4800 9.0 70.0 40.0 [67] ZnZrOx/H-ZSM-5 315 3 1020 15.5 74.7 35.3 [71] ZnZrOx/H-ZSM-5 320 4 1200 14.0 73.0 44.0 [57] ZnAlOx/H-ZSM-5 320 3 2000 9.1 73.9 57.4 [66] nNa-ZnFeOx/H-ZSM-5 320 3 4000 41.2 75.6 < 20.0 [65] Na-Fe/H-ZSM-5 320 1 2400 29.4 54.3 23.1 [60] Na-Fe@C/H-ZSM-5 320 3 9000 33.3 50.2 13.3 [61] Na-Fe3O4/H-ZSM-5 340 3 4000 45.3 23.5(yield) 11.3 [62] Na-Fe3O4/H-ZSM-5 320 3 4000 34.0 44.0 < 15.0 [63] Cu-Fe2O3/H-ZSM-5 320 3 1000 57.3 56.6 3.2 [64] In2O3/H-ZSM-5 340 3 9000 13.1 14.6 45.0 [69] Cr2O3/H-ZSM-5 350 4 1200 14.6 85.5 35.8 [70] 15Fe-10K-Al2O3/0.8%P-HZSM-5 400 3 3000 36.4 35.5 (incl. CO) 10.2 [72] -
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