化工进展 ›› 2024, Vol. 43 ›› Issue (5): 2776-2785.DOI: 10.16085/j.issn.1000-6613.2024-0341
• 二氧化碳捕集与资源化利用 • 上一篇
周秋明(), 牛丛丛(
), 吕帅帅, 李红伟, 文富利, 徐润, 李明丰(
)
收稿日期:
2024-03-01
修回日期:
2024-04-26
出版日期:
2024-05-15
发布日期:
2024-06-15
通讯作者:
李明丰
作者简介:
周秋明(1993—),女,博士,研究方向为C1化学。E-mail:zhouqiuming.ripp@sinopec.com基金资助:
ZHOU Qiuming(), NIU Congcong(
), LYU Shuaishuai, LI Hongwei, WEN Fuli, XU Run, LI Mingfeng(
)
Received:
2024-03-01
Revised:
2024-04-26
Online:
2024-05-15
Published:
2024-06-15
Contact:
LI Mingfeng
摘要:
将过量排放的CO2加氢合成高附加值甲醇的过程因受热力学限制使其原料转化利用率较低,通过产物转化分离的方式能够打破热力学平衡,从而推动反应正向进行,提高CO2转化率。本文以将甲醇作为中间体耦合其他反应继续转化成低碳烯烃、芳烃等化工原料,以及利用膜反应器将副产水原位脱除等两种典型的产物转化分离方式为中心,分别展开论述其在促进CO2加氢反应过程中,耦合反应条件优化、催化剂筛选制备以及分子筛膜反应器设计与改性等方面的研究现状。重点讨论了耦合反应的双功能型催化剂中分子筛载体的酸性与孔道结构对反应性能的影响,并分析了膜反应器未来的研发重点与难点在于进一步提高其制备可重复性。
中图分类号:
周秋明, 牛丛丛, 吕帅帅, 李红伟, 文富利, 徐润, 李明丰. 通过产物转化分离推动CO2加氢制甲醇过程的研究进展[J]. 化工进展, 2024, 43(5): 2776-2785.
ZHOU Qiuming, NIU Congcong, LYU Shuaishuai, LI Hongwei, WEN Fuli, XU Run, LI Mingfeng. Promoting CO2 hydrogenation to methanol through product transformation and separation[J]. Chemical Industry and Engineering Progress, 2024, 43(5): 2776-2785.
催化剂 | 温度/℃ | 压力/MPa | CO2转化率/% | 低碳烯烃选择性/% | 参考文献 |
---|---|---|---|---|---|
In2O3-ZrO2/SAPO-34 | 400 | 3.0 | 35.0 | 80.0 | [ |
ZnO-ZrO2/SAPO-34 | 380 | 2.0 | 12.6 | 80.0 | [ |
ZnGa2O4/SAPO-34 | 370 | 3.0 | 13.0 | 86.0 | [ |
ZnAl2O4/SAPO-34 | 370 | 3.0 | 15.0 | 87.0 | [ |
In2O3/SAPO-34 | 360 | 2.5 | 34.6 | 70.0 | [ |
CZZ@SAPO-34 | 400 | 2.0 | 19.6 | 60.5 | [ |
CuO-ZnO/SAPO-34 | 400 | 3.0 | 43.5 | 63.9 | [ |
ZnZrO x /bio-SAPO-34 | 380 | 3.0 | 13.8 | 83.0 | [ |
ZZ/4%MnSAPO-34 | 380 | 2.0 | 17.3 | 83.2 | [ |
表1 不同催化剂上CO2加氢制低碳烯烃的反应性能
催化剂 | 温度/℃ | 压力/MPa | CO2转化率/% | 低碳烯烃选择性/% | 参考文献 |
---|---|---|---|---|---|
In2O3-ZrO2/SAPO-34 | 400 | 3.0 | 35.0 | 80.0 | [ |
ZnO-ZrO2/SAPO-34 | 380 | 2.0 | 12.6 | 80.0 | [ |
ZnGa2O4/SAPO-34 | 370 | 3.0 | 13.0 | 86.0 | [ |
ZnAl2O4/SAPO-34 | 370 | 3.0 | 15.0 | 87.0 | [ |
In2O3/SAPO-34 | 360 | 2.5 | 34.6 | 70.0 | [ |
CZZ@SAPO-34 | 400 | 2.0 | 19.6 | 60.5 | [ |
CuO-ZnO/SAPO-34 | 400 | 3.0 | 43.5 | 63.9 | [ |
ZnZrO x /bio-SAPO-34 | 380 | 3.0 | 13.8 | 83.0 | [ |
ZZ/4%MnSAPO-34 | 380 | 2.0 | 17.3 | 83.2 | [ |
催化剂 | 温度/℃ | 压力/MPa | CO2转化率/% | C5+中芳烃选择性/% | 参考文献 |
---|---|---|---|---|---|
ZnZrO/ZSM-5 | 320 | 4.0 | 14.1 | 73.0 | [ |
ZnZrO x /HZSM-5 | 315 | 3.0 | 17.5 | 60.3 | [ |
ZnO-ZrO2/ZSM-5 | 340 | 4.0 | 14.0 | 74.0 | [ |
ZnO/ZrO2-Z5-300 | 340 | 3.0 | 9.0 | 70.0 | [ |
ZnCrO x -ZnZSM-5 | 320 | 5.0 | 19.9 | 81.1 | [ |
ZnCr2O4-ZSM-5 | 350 | 4.0 | 23.4 | 66.1 | [ |
ZnAlO x /HZSM-5 | 320 | 3.0 | 5.8 | 73.9 | [ |
Cr2O3/H-ZSM-5 | 350 | 3.0 | 34.5 | 76.0 | [ |
Cr2O3/Zn-ZSM-5@SiO2 | 350 | 3.0 | 22.1 | 58.4 | [ |
In2O3/HZSM-5 | 320 | 3.0 | 23.2 | 34.1 | [ |
ZnFeO x -4.25Na/S-HZSM-5 | 320 | 3.0 | 41.2 | 75.6 | [ |
表2 不同催化剂上CO2加氢制芳烃的反应性能
催化剂 | 温度/℃ | 压力/MPa | CO2转化率/% | C5+中芳烃选择性/% | 参考文献 |
---|---|---|---|---|---|
ZnZrO/ZSM-5 | 320 | 4.0 | 14.1 | 73.0 | [ |
ZnZrO x /HZSM-5 | 315 | 3.0 | 17.5 | 60.3 | [ |
ZnO-ZrO2/ZSM-5 | 340 | 4.0 | 14.0 | 74.0 | [ |
ZnO/ZrO2-Z5-300 | 340 | 3.0 | 9.0 | 70.0 | [ |
ZnCrO x -ZnZSM-5 | 320 | 5.0 | 19.9 | 81.1 | [ |
ZnCr2O4-ZSM-5 | 350 | 4.0 | 23.4 | 66.1 | [ |
ZnAlO x /HZSM-5 | 320 | 3.0 | 5.8 | 73.9 | [ |
Cr2O3/H-ZSM-5 | 350 | 3.0 | 34.5 | 76.0 | [ |
Cr2O3/Zn-ZSM-5@SiO2 | 350 | 3.0 | 22.1 | 58.4 | [ |
In2O3/HZSM-5 | 320 | 3.0 | 23.2 | 34.1 | [ |
ZnFeO x -4.25Na/S-HZSM-5 | 320 | 3.0 | 41.2 | 75.6 | [ |
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