化工进展 ›› 2024, Vol. 43 ›› Issue (5): 2723-2738.DOI: 10.16085/j.issn.1000-6613.2023-2207
• 二氧化碳捕集与资源化利用 • 上一篇
周运桃1,2(), 王洪星1,2, 李新刚1(
), 崔丽凤2(
)
收稿日期:
2023-12-15
修回日期:
2024-03-01
出版日期:
2024-05-15
发布日期:
2024-06-15
通讯作者:
李新刚,崔丽凤
作者简介:
周运桃(1988—),男,博士,研究方向为催化反应。E-mail:zhouyuntao1005@163.com。
基金资助:
ZHOU Yuntao1,2(), WANG Hongxing1,2, LI Xingang1(
), CUI Lifeng2(
)
Received:
2023-12-15
Revised:
2024-03-01
Online:
2024-05-15
Published:
2024-06-15
Contact:
LI Xingang, CUI Lifeng
摘要:
随着经济的快速发展,CO2排放导致的温室效应日益严峻,通过与绿氢反应将其转化为甲醇等有价值的化工产品是减少CO2排放、缓解全球气候变暖的有效途径。近年来,CeO2负载金属催化剂在CO2加氢制甲醇反应中得到了广泛关注。本文主要综述了CeO2表面氧空位和碱性位点、Ce3+/Ce4+可逆氧化还原能力、几何形貌等特性在CO2/H2吸附活化和甲醇形成过程中所起到的重要作用,比较了CeO2与ZrO2、ZnO以及复合金属氧化物等载体在反应中的差异,提出了CeO2载体催化剂在确认活性关键中间体、兼顾CO2转化率和甲醇选择性、提高催化活性与稳定性等方面的不足和挑战,以期为新型CO2加氢制甲醇催化剂的设计提供有益参考。
中图分类号:
周运桃, 王洪星, 李新刚, 崔丽凤. CeO2载体在CO2加氢制甲醇中的应用和研究进展[J]. 化工进展, 2024, 43(5): 2723-2738.
ZHOU Yuntao, WANG Hongxing, LI Xingang, CUI Lifeng. Application and research progress of CeO2 support in CO2 hydrogenation to methanol[J]. Chemical Industry and Engineering Progress, 2024, 43(5): 2723-2738.
催化剂 | H2/CO2 | 温度/℃,压力/MPa | GHSV/WHSV | CO2转化率/% | 甲醇选择性/% | STY/g·kgcat-1·h-1 |
---|---|---|---|---|---|---|
2Pd/CeO2-R[ | 3 | 240,3.0 | 2.0L/(gcat·h) | 约6.2① | 约30① | 12.0 |
2Pd/CeO2-P[ | 3 | 240,3.0 | 2.0L/(gcat·h) | — | 约29① | 9.5 |
2Pd/CeO2-C[ | 3 | 240,3.0 | 2.0L/(gcat·h) | — | 约25① | 5.0 |
2Pd/CeO2-O[ | 3 | 240,3.0 | 2.0L/(gcat·h) | 约6.3① | 约26① | 2.5 |
Cu/CeO2-R[ | 3 | 240,2.0 | 3.0L/(gcat·h) | 约2.2① | 89.5 | 21.1 |
Cu/CeO2-C[ | 3 | 240,2.0 | 3.0L/(gcat·h) | 约1.5① | 84 | 13.5 |
Cu/CeO2-S[ | 3 | 240,2.0 | 3.0L/(gcat·h) | 约0.6① | 89 | 5.7 |
1Cu2Ni/CeO2-R[ | 3 | 260,3.0 | 6.0L/h | 18.3 | 73.3 | 230.2 |
1Cu2Ni/CeO2-S[ | 3 | 260,3.0 | 6.0L/h | 约17.5① | 约69.5① | 208.8 |
1Cu2Ni/CeO2-P[ | 3 | 260,3.0 | 6.0L/h | 约14.0① | 约68.5① | 164.6 |
Cu/CeO2-SG[ | 3 | 240,3.0 | 2.4L/(gcat·h) | 6.4 | 89.1 | 48.9 |
Cu/CeO2-SCP[ | 3 | 240,3.0 | 2.4L/(gcat·h) | 5.9 | 84.6 | 42.8 |
Cu/CeO2-CP[ | 3 | 240,3.0 | 2.4L/(gcat·h) | 3.8 | 80.5 | 26.2 |
Cu-CF[ | 3 | 260,3.0 | 18.0L/(gcat·h) | 约9.8① | 约41.0① | 249.0 |
Cu-CP[ | 3 | 260,3.0 | 18.0L·/(gcat·h) | 约9.0① | 约35.0① | 197.0 |
Cu-IM[ | 3 | 260,3.0 | 18.0L/(gcat·h) | 约5.1① | 约42.5① | 143.0 |
5Ag/ZrCeO x-IM[ | 3 | 250,2.0 | 1.8L/h | 7 | 70 | 31.9 |
5Ag/ZrCeO x-CH[ | 3 | 250,2.0 | 1.8L/h | 8 | 60 | 30.9 |
表1 CeO2形貌对催化活性的影响
催化剂 | H2/CO2 | 温度/℃,压力/MPa | GHSV/WHSV | CO2转化率/% | 甲醇选择性/% | STY/g·kgcat-1·h-1 |
---|---|---|---|---|---|---|
2Pd/CeO2-R[ | 3 | 240,3.0 | 2.0L/(gcat·h) | 约6.2① | 约30① | 12.0 |
2Pd/CeO2-P[ | 3 | 240,3.0 | 2.0L/(gcat·h) | — | 约29① | 9.5 |
2Pd/CeO2-C[ | 3 | 240,3.0 | 2.0L/(gcat·h) | — | 约25① | 5.0 |
2Pd/CeO2-O[ | 3 | 240,3.0 | 2.0L/(gcat·h) | 约6.3① | 约26① | 2.5 |
Cu/CeO2-R[ | 3 | 240,2.0 | 3.0L/(gcat·h) | 约2.2① | 89.5 | 21.1 |
Cu/CeO2-C[ | 3 | 240,2.0 | 3.0L/(gcat·h) | 约1.5① | 84 | 13.5 |
Cu/CeO2-S[ | 3 | 240,2.0 | 3.0L/(gcat·h) | 约0.6① | 89 | 5.7 |
1Cu2Ni/CeO2-R[ | 3 | 260,3.0 | 6.0L/h | 18.3 | 73.3 | 230.2 |
1Cu2Ni/CeO2-S[ | 3 | 260,3.0 | 6.0L/h | 约17.5① | 约69.5① | 208.8 |
1Cu2Ni/CeO2-P[ | 3 | 260,3.0 | 6.0L/h | 约14.0① | 约68.5① | 164.6 |
Cu/CeO2-SG[ | 3 | 240,3.0 | 2.4L/(gcat·h) | 6.4 | 89.1 | 48.9 |
Cu/CeO2-SCP[ | 3 | 240,3.0 | 2.4L/(gcat·h) | 5.9 | 84.6 | 42.8 |
Cu/CeO2-CP[ | 3 | 240,3.0 | 2.4L/(gcat·h) | 3.8 | 80.5 | 26.2 |
Cu-CF[ | 3 | 260,3.0 | 18.0L/(gcat·h) | 约9.8① | 约41.0① | 249.0 |
Cu-CP[ | 3 | 260,3.0 | 18.0L·/(gcat·h) | 约9.0① | 约35.0① | 197.0 |
Cu-IM[ | 3 | 260,3.0 | 18.0L/(gcat·h) | 约5.1① | 约42.5① | 143.0 |
5Ag/ZrCeO x-IM[ | 3 | 250,2.0 | 1.8L/h | 7 | 70 | 31.9 |
5Ag/ZrCeO x-CH[ | 3 | 250,2.0 | 1.8L/h | 8 | 60 | 30.9 |
催化剂 | H2/CO2 | 温度/℃,压力/MPa | GHSV/WHSV | CO2转化率/% | 甲醇选择性/% | STY/g·kgcat-1·h-1 |
---|---|---|---|---|---|---|
1Pd-10Cu/CeO2[ | 3 | 250,3.0 | 3.0L/(gcat·h) | 16.1 | 26.7 | 28.3 |
5Pd5Zn/CeO2[ | 3 | 220,3.0 | 2.4L/(gcat·h) | 6.3 | 100 | 54.1 |
0.5Ca5Pd5Zn/CeO2[ | 3 | 220,3.0 | 2.4L/(gcat·h) | 7.7 | 100 | 66.1 |
PdZn/CeO2[ | 3 | 220,2.0 | 2.4L/(gcat·h) | 14.1 | 94.5 | 114.3 |
CuNi2/CeO2-NT[ | 3 | 260,3.0 | 6.0L/h | 17.8 | 78.8 | 579.9 |
表2 CeO2负载双金属催化剂
催化剂 | H2/CO2 | 温度/℃,压力/MPa | GHSV/WHSV | CO2转化率/% | 甲醇选择性/% | STY/g·kgcat-1·h-1 |
---|---|---|---|---|---|---|
1Pd-10Cu/CeO2[ | 3 | 250,3.0 | 3.0L/(gcat·h) | 16.1 | 26.7 | 28.3 |
5Pd5Zn/CeO2[ | 3 | 220,3.0 | 2.4L/(gcat·h) | 6.3 | 100 | 54.1 |
0.5Ca5Pd5Zn/CeO2[ | 3 | 220,3.0 | 2.4L/(gcat·h) | 7.7 | 100 | 66.1 |
PdZn/CeO2[ | 3 | 220,2.0 | 2.4L/(gcat·h) | 14.1 | 94.5 | 114.3 |
CuNi2/CeO2-NT[ | 3 | 260,3.0 | 6.0L/h | 17.8 | 78.8 | 579.9 |
催化剂 | H2/CO2 | 温度/℃,压力/MPa | GHSV/WHSV | CO2转化率/% | 甲醇选择性/% | STY/g·kgcat-1·h-1 |
---|---|---|---|---|---|---|
Cu/CeO2[ | 3 | 220,3.0 | 2.4L/(gcat·h) | 约2.5① | 91 | 19.5 |
Cu/ZrO2[ | 3 | 220,3.0 | 2.4L/(gcat·h) | 约3.0① | 80 | 20.6 |
Cu/ZnO[ | 3 | 220,3.0 | 2.4L/(gcat·h) | 约3.5① | 74 | 22.2 |
Cu/CeO2[ | 3 | 220,3.0 | 10L/h | 4.5 | 约85① | 136.8 |
Cu/ZrO2[ | 3 | 220,3.0 | 10L/h | 6.5 | 约77① | 179.0 |
Cu/CeO2[ | 3 | 250,3.0 | 30L/(gcat·h) | 1.0 | 53 | 45.5 |
Cu/SiO2[ | 3 | 250,3.0 | 60L/(gcat·h) | 1.1 | 16 | 30.2 |
Au/CeO2[ | 9 | 225,0.1 | 20L/h | — | 62.2 | — |
Au/ZnO[ | 9 | 225,0.1 | 20L/h | — | 88.9 | — |
Ni5Ga3/SiO2[ | 3 | 270,1.0 | 8.0L/(gcat·h) | 1.5 | 12.5 | 50.0 |
Ni5Ga3/ZrO2[ | 3 | 270,1.0 | 8.0L/(gcat·h) | 3.5 | 18.0 | 160.0 |
Ni5Ga3/CeO2[ | 3 | 270,1.0 | 8.0L/(gcat·h) | 6.1 | 3.4 | 54.0 |
表3 CO2加氢制甲醇催化剂载体效应
催化剂 | H2/CO2 | 温度/℃,压力/MPa | GHSV/WHSV | CO2转化率/% | 甲醇选择性/% | STY/g·kgcat-1·h-1 |
---|---|---|---|---|---|---|
Cu/CeO2[ | 3 | 220,3.0 | 2.4L/(gcat·h) | 约2.5① | 91 | 19.5 |
Cu/ZrO2[ | 3 | 220,3.0 | 2.4L/(gcat·h) | 约3.0① | 80 | 20.6 |
Cu/ZnO[ | 3 | 220,3.0 | 2.4L/(gcat·h) | 约3.5① | 74 | 22.2 |
Cu/CeO2[ | 3 | 220,3.0 | 10L/h | 4.5 | 约85① | 136.8 |
Cu/ZrO2[ | 3 | 220,3.0 | 10L/h | 6.5 | 约77① | 179.0 |
Cu/CeO2[ | 3 | 250,3.0 | 30L/(gcat·h) | 1.0 | 53 | 45.5 |
Cu/SiO2[ | 3 | 250,3.0 | 60L/(gcat·h) | 1.1 | 16 | 30.2 |
Au/CeO2[ | 9 | 225,0.1 | 20L/h | — | 62.2 | — |
Au/ZnO[ | 9 | 225,0.1 | 20L/h | — | 88.9 | — |
Ni5Ga3/SiO2[ | 3 | 270,1.0 | 8.0L/(gcat·h) | 1.5 | 12.5 | 50.0 |
Ni5Ga3/ZrO2[ | 3 | 270,1.0 | 8.0L/(gcat·h) | 3.5 | 18.0 | 160.0 |
Ni5Ga3/CeO2[ | 3 | 270,1.0 | 8.0L/(gcat·h) | 6.1 | 3.4 | 54.0 |
催化剂 | H2/CO2 | 温度/℃,压力/MPa | GHSV/WHSV | CO2转化率/% | 甲醇选择性/% | STY/g·kgcat-1·h-1 |
---|---|---|---|---|---|---|
Cu/ZnO-CeO2[ | 3 | 280,3.0 | 12.0L/h | 15.6 | 64.5 | 431.7 |
Cu/AlCeO-7[ | 3 | 260,3.0 | 14.4L/(gcat·h) | 约17① | 约45① | 381.3 |
Cu0.3Zr0.3Ce0.7[ | 3 | 240,3.0 | 30.0L/(gcat·h) | 4.1 | 55.3 | 192.0 |
Cu30Ce35Zr35O[ | 3 | 250,3.0 | 7.5L/(gcat·h) | 14.3 | 53.8 | 165.0 |
5-Cu-CeO2/ZrO2[ | 3 | 260,5.0 | 60.0L/(gcat·h) | 1.7 | 42 | 147.1 |
CuO/Ce0.4Zr0.6O2[ | 3 | 280,3.0 | 10.0L/h | 13.2 | 71.8 | 338.9 |
CuO/Mn0.2CeO x[ | 3 | 260,1.5 | 6.0L/(gcat·h) | 14.2 | 82.3 | 250.0 |
CuO/La0.25CeO x[ | 3 | 260,1.5 | 6.0L/(gcat·h) | 15.7 | 83.3 | 281.0 |
Cu/CeO2[ | 3 | 250,3.5 | 15.0L/(gcat·h) | 1.3 | 51 | 40.4 |
Cu/CeW0.25O x[ | 3 | 250,3.5 | 15.0L/(gcat·h) | 13 | 87 | 394.7 |
表4 含CeO2复合氧化物催化剂活性
催化剂 | H2/CO2 | 温度/℃,压力/MPa | GHSV/WHSV | CO2转化率/% | 甲醇选择性/% | STY/g·kgcat-1·h-1 |
---|---|---|---|---|---|---|
Cu/ZnO-CeO2[ | 3 | 280,3.0 | 12.0L/h | 15.6 | 64.5 | 431.7 |
Cu/AlCeO-7[ | 3 | 260,3.0 | 14.4L/(gcat·h) | 约17① | 约45① | 381.3 |
Cu0.3Zr0.3Ce0.7[ | 3 | 240,3.0 | 30.0L/(gcat·h) | 4.1 | 55.3 | 192.0 |
Cu30Ce35Zr35O[ | 3 | 250,3.0 | 7.5L/(gcat·h) | 14.3 | 53.8 | 165.0 |
5-Cu-CeO2/ZrO2[ | 3 | 260,5.0 | 60.0L/(gcat·h) | 1.7 | 42 | 147.1 |
CuO/Ce0.4Zr0.6O2[ | 3 | 280,3.0 | 10.0L/h | 13.2 | 71.8 | 338.9 |
CuO/Mn0.2CeO x[ | 3 | 260,1.5 | 6.0L/(gcat·h) | 14.2 | 82.3 | 250.0 |
CuO/La0.25CeO x[ | 3 | 260,1.5 | 6.0L/(gcat·h) | 15.7 | 83.3 | 281.0 |
Cu/CeO2[ | 3 | 250,3.5 | 15.0L/(gcat·h) | 1.3 | 51 | 40.4 |
Cu/CeW0.25O x[ | 3 | 250,3.5 | 15.0L/(gcat·h) | 13 | 87 | 394.7 |
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