双金属负载<italic style="font-style: italic">γ</italic>-Al2O3固体酸催化CO2有机胺富液解吸性能

邱微; 宁一睿; 赵澍; 张毅然; 李珂; 黄震; 林赫

doi:10.12434/j.issn.2097-2547.20240407

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双金属负载γ-Al₂O₃固体酸催化CO₂有机胺富液解吸性能

二氧化碳捕集与利用 | 更新时间：2025-07-30

- 双金属负载γ-Al₂O₃固体酸催化CO₂有机胺富液解吸性能
- Catalytic performances of bimetal-loaded γ-Al₂O₃ solid acids for CO₂ desorption from rich amine solution
- 低碳化学与化工 2025, 50(7): 99-108.
- 作者机构：
  
  1.上海交通大学智慧能源创新学院，上海 200240
  2.中国船舶集团有限公司第七一一研究所，上海 201108
  3.上海交通大学机械与动力工程学院，上海 200240
- 作者简介：
  
  邱微（2000—），硕士研究生，研究方向为碳捕集催化解吸技术，E-mail：qw2339149409@sjtu.edu.cn。
  张毅然（1992—），博士，副教授，研究方向为碳捕集与利用，E-mail：zhangyiran@sjtu.edu.cn。
- 基金信息：
  
  国家重点研发计划(2022YFE0208900)
- DOI：10.12434/j.issn.2097-2547.20240407
  中图分类号： TQ426
- 收稿日期：2024-10-05，
  
  修回日期：2024-10-26，
  
  纸质出版日期：2025-07-25
- 稿件说明：
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邱微,宁一睿,赵澍等.双金属负载γ-Al₂O₃固体酸催化CO₂有机胺富液解吸性能[J].低碳化学与化工,2025,50(07):99-108.

QIU Wei,NING Yirui,ZHAO Shu,et al.Catalytic performances of bimetal-loaded γ-Al₂O₃ solid acids for CO₂ desorption from rich amine solution[J].Low-Carbon Chemistry and Chemical Engineering,2025,50(07):99-108.
邱微,宁一睿,赵澍等.双金属负载γ-Al₂O₃固体酸催化CO₂有机胺富液解吸性能[J].低碳化学与化工,2025,50(07):99-108. DOI： 10.12434/j.issn.2097-2547.20240407.

QIU Wei,NING Yirui,ZHAO Shu,et al.Catalytic performances of bimetal-loaded γ-Al₂O₃ solid acids for CO₂ desorption from rich amine solution[J].Low-Carbon Chemistry and Chemical Engineering,2025,50(07):99-108. DOI： 10.12434/j.issn.2097-2547.20240407.

摘要

有机胺溶液吸收法是一种前景广阔的CO

捕集技术，但高再生能耗导致该方法的成本较高。开发高催化活性和稳定性的固体酸催化剂是降低有机胺溶液再生能耗的重要途径。以

-Al

为载体，采用浸渍法制备了一系列双金属负载氧化铝固体酸催化剂ZrM/

-Al

（M = Ni、Fe、Ce或Cu，Zr和M质量分数均为10%），并对其在富CO

单乙醇胺溶液（MEA富液）中的催化解吸性能和作用机理等进行了研究。结果表明，在解吸温度为91 ℃、搅拌速率为500 r/min和MEA富液CO

负载量为0.5 mol/mol的条件下，ZrNi/

-Al

具有最优的催化解吸性能，其CO

解吸速率峰值、CO

解吸量和相对能耗（与未加入催化剂的空白组相比）分别为1.92 mmol/min、46.53 mmol和55.04%。在吸收温度为40 °C、解吸温度为92 °C下经历8次吸收-解吸循环后，ZrNi/

-Al

仍具有较好的催化解吸性能，其作用下MEA富液的再生能耗较空白组仍降低了23%左右，因此ZrNi/

-Al

循环稳定性良好。N

吸/脱附、NH

-TPD和Py-IR等表征结果显示，ZrM/

-Al

具有适宜的织构性质和酸性，其丰富的B酸和L酸位点在MEA富液的催化解吸过程中发挥了关键作用。

Abstract

The amine-based absorption method is a promising technology for CO

capture

but the high regeneration energy consumption increases its costs. Developing solid acid catalysts with high catalytic activity and stability is a key approach to reducing the regeneration energy consumption of amine solutions. A series of bimetal-loaded

-Al

solid acid catalysts ZrM/

-Al

(M = Ni

Ce or Cu

mass fractions of Zr and M both are 10%) were prepared by loading two types of metals on the support

-Al

using the impregnation method. And the catalytic desorption performances and mechanisms of the catalysts in monoethanolamine rich solution with CO

(MEA rich solution) were investigated. The results show that under the conditions of desorption temperature of 91 ℃

stirring rate of 500 r/min and CO

loading of 0.5 mol/mol

ZrNi/

-Al

exhibits the most favorable catalytic desorption performance. Specifically

the peak CO

desorption rate

total desorption amount and relative energy consumption (compared to the blank group without catalyst) catalyzed by ZrNi/

-Al

are 1.92 mmol/min

46.53 mmol and 55.04%

respectively. After eight absorption-desorption cycles at 40 ℃ for absorption and 92 ℃ for desorption

ZrNi/

-Al

maintains good catalytic desorption performance with reducing the regeneration energy consumption of MEA rich solution by approximately 23% compared to the blank group. This indicates that ZrNi/

-Al

possesses good cyclic stability. The characterization results of N

adsorption/desorption

-TPD and Py-IR show that ZrM/

-Al

catalysts demonstrate suitable textural properties and acidity. The abundant Brønsted and Lewis acid sites play critical role in the catalytic desorption process of MEA rich solutions.

关键词

Keywords

references

IPCC . Climate Change 2023 [R ] . Geneva : Intergovernmental Panel on Climate Change , 2023 .

TAN Z , ZHANG S S , ZHAO F F , et al . SnO 2 /ATP catalyst enabling energy-efficient and green amine-based CO 2 capture [J ] . Chemical Engineering Journal , 2023 , 453 : 139801 .

申长俊 , 陆诗建 , 刘玲 , 等 . 船舶尾气净化技术研究进展 [J ] . 低碳化学与化工 , 2024 , 49 ( 4 ): 98 - 106 .

SHEN C J , LU S J , LIU L , et al . Research progress of ship exhaust purification technologies [J ] . Low-Carbon Chemistry and Chemical Engineering , 2024 , 49 ( 4 ): 98 - 106 .

陈家伟 , 杨柳 , 李新令 , 等 . MAP-DMSO-PMDETA三元相变吸收剂的CO 2 捕集性能 [J ] . 化工环保 , 2024 , 44 ( 2 ): 213 - 220 .

CHEN J W , YANG L , LI X L , et al . CO 2 capture capability of MAP-DMSO-PMDETA ternary phase-change absorbent [J ] . Environmental Protection of Chemical Industry , 2024 , 44 ( 2 ): 213 - 220 .

陆诗建 , 方梦祥 , 陈浮 , 等 . AEP-DPA-CuO相变纳米流体捕集烟气中CO 2 [J ] . 化工环保 , 2021 , 41 ( 6 ): 724 - 730 .

LU S J , FANG M X , CHEN F , et al . Capture of CO 2 in flue gas by AEP-DPA-CuO phase change nanofluid [J ] . Environmental Protection of Chemical Industry , 2021 , 41 ( 6 ): 724 - 730 .

李亚清 , 宋沆 , 张玉涛 , 等 . 醇胺法吸收烟道气中二氧化碳的研究进展 [J ] . 低碳化学与化工 , 2024 , 49 ( 10 ): 81 - 91 .

LI Y Q , SONG H , ZHANG Y T , et al . Research progress on absorption of carbon dioxide in flue gas by alcohol amine method [J ] . Low-Carbon Chemistry and Chemical Engineering , 2024 , 49 ( 10 ): 81 - 91 .

XING L , LI M , LI M Y , et al . MOF-derived robust and synergetic acid sites inducing C—N bond disruption for energy-efficient CO 2 desorption [J ] . Environmental Science & Technology , 2022 , 56 ( 24 ): 17936 - 17945 .

XING L , WEI K X , LI Y C , et al . TiO 2 coating strategy for robust catalysis of the metal-organic framework toward energy-efficient CO 2 capture [J ] . Environmental Science & Technology , 2021 , 55 : 11216 - 11224 .

刘竞文 , 孙乐乐 , 刘健 , 等 . 有机胺CO 2 吸收液催化解吸研究进展 [J ] . 低碳化学与化工 , 2025 , 50 ( 1 ): 120 - 131 .

LIU J W , SUN L L , LIU J , et al . Research progress on catalytic desorption of organic amine CO 2 absorption liquids [J ] . Low-Carbon Chemistry and Chemical Engineering , 2025 , 50 ( 1 ): 120 - 131 .

SHI H , NAAMI A , IDEM R , et al . Catalytic and non catalytic solvent regeneration during absorption-based CO 2 capture with single and blended reactive amine solvents [J ] . International Journal of Greenhouse Gas Control , 2014 , 26 : 39 - 50 .

ZHANG X W , ZHANG X , LIU H L , et al . Reduction of energy requirement of CO 2 desorption from a rich CO 2 -loaded MEA solution by using solid acid catalysts [J ] . Applied Energy , 2017 , 202 : 673 - 684 .

BHATTI U H , KAZMI W W , MIN G H , et al . Facilely synthesized M-montmorillonite (M = Cr , Fe, and Co) as efficient catalysts for enhancing CO 2 desorption from amine solution [J ] . Industrial & Engineering Chemistry Research , 2021 , 60 ( 36 ): 13318 - 13325 .

GAO H X , HUANG Y F , ZHANG X W , et al . Catalytic performance and mechanism of SO <math id="M35"><msubsup><mrow/><mrow><mn mathvariant="normal">4</mn></mrow><mrow><mn mathvariant="normal">2</mn><mo>-</mo></mrow></msubsup></math> https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=86357162&type= 3.64066648 https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=86357173&type= 2.37066650 /ZrO 2 /SBA-15 catalyst for CO 2 desorption in CO 2 -loaded monoethanolamine solution [J ] . Applied Energy , 2020 , 259 : 114179 .

WEI K X , XING L , LI Y C , et al . Heteropolyacid modified cerium-based MOFs catalyst for amine solution regeneration in CO 2 capture [J ] . Separation and Purification Technology , 2022 , 293 : 121144 .

ZHANG X W , HUANG Y F , GAO H X , et al . Zeolite catalyst-aided tri-solvent blend amine regeneration: An alternative pathway to reduce the energy consumption in amine-based CO 2 capture process [J ] . Applied Energy , 2019 , 240 : 827 - 841 .

LIU S H , MAO X D , CHEN H , et al . Catalytic-CO 2 -desorption studies of BZA-AEP mixed absorbent by the Lewis acid catalyst CeO 2 - γ -Al 2 O 3 [J ] . Molecules , 2023 , 28 ( 11 ): 4438 .

IDEM R , SH H , GELOWITZ D , et al . Catalytic method and apparatus for separating a gaseous component from an incoming gas stream : PCT/CA2011/000328 [P ] . 2011-03-29 .

XING L , WEI K X , LI Q W , et al . One-step synthesized SO <math id="M36"><msubsup><mrow/><mrow><mn mathvariant="normal">4</mn></mrow><mrow><mn mathvariant="normal">2</mn><mo>-</mo></mrow></msubsup></math> https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=86357162&type= 3.64066648 https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=86357173&type= 2.37066650 /ZrO 2 -HZSM-5 solid acid catalyst for carbamate decomposition in CO 2 capture [J ] . Environmental Science & Technology , 2020 , 54 ( 21 ): 13944 - 13952 .

ZHANG X W , HONG J L , LIU H L , et al . SO <math id="M37"><msubsup><mrow/><mrow><mn mathvariant="normal">4</mn></mrow><mrow><mn mathvariant="normal">2</mn><mo>-</mo></mrow></msubsup></math> https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=86357162&type= 3.64066648 https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=86357173&type= 2.37066650 /ZrO 2 supported on γ -Al 2 O 3 as a catalyst for CO 2 desorption from CO 2 -loaded monoethanolamine solutions [J ] . AIChE Journal , 2018 , 64 ( 11 ): 3988 - 4001 .

ZHANG R , LI Y F , ZHANG Y M , et al . Energy-saving effect of low-cost and environmentally friendly sepiolite as an efficient catalyst carrier for CO 2 capture [J ] . ACS Sustainable Chemistry & Engineering , 2023 , 11 ( 11 ): 4353 - 4363 .

BHATTI A H , WARIS M , KAZMI W W , et al . Metal impregnated activated carbon as cost-effective and scalable catalysts for amine-based CO 2 capture [J ] . Journal of Environmental Chemical Engineering , 2023 , 11 ( 1 ): 109231 .

GENG Z B , YANG Y , WANG Y X , et al . Catalytic regeneration of amine-based absorbents for CO 2 capture: The effect of acidic sites and accessibility [J ] . Separation and Purification Technology , 2023 , 327 : 124889 .

HUANG Y F , ZHANG X W , LUO X , et al . Catalytic performance and mechanism of meso-microporous material β -SBA-15-supported FeZr catalysts for CO 2 desorption in CO 2 -loaded aqueous amine solution [J ] . Industrial & Engineering Chemistry Research , 2021 , 60 ( 6 ): 2698 - 2709 .

ZHANG X W , ZHU Z Q , SUN X Y , et al . Reducing energy penalty of CO 2 capture using Fe promoted SO <math id="M38"><msubsup><mrow/><mrow><mn mathvariant="normal">4</mn></mrow><mrow><mn mathvariant="normal">2</mn><mo>-</mo></mrow></msubsup></math> https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=86357155&type= 3.64066648 https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=86357175&type= 2.37066650 /ZrO 2 /MCM-41 catalyst [J ] . Environmental Science & Technology , 2019 , 53 ( 10 ): 6094 - 6102 .

任永旺 , 王一泽 , 常飞祥 , 等 . 氮掺杂碳改性Ni/Al 2 O 3 催化剂的甲烷干重整反应性能研究 [J ] . 低碳化学与化工 , 2023 , 48 ( 3 ): 49 - 55 .

REN Y W , WANG Y Z , CHANG F X , et al . Performance study of nitrogen-doped carbon-modified Ni/Al 2 O 3 catalysts for methane dry reforming reaction [J ] . Low-Carbon Chemistry and Chemical Engineering , 2023 , 48 ( 3 ): 49 - 55 .

丁传敏 , 马自立 , 李宇峰 , 等 . Ni@ZSM-5催化剂的制备及其甲烷部分氧化反应性能的研究 [J ] . 天然气化工—C1化学与化工 , 2020 , 45 ( 6 ): 1 - 6 .

DING C M , MA Z L , LI Y F , et al . Preparation of Ni@ZSM-5 catalyst and its reaction performance for partial oxidation of methane [J ] . Natural Gas Chemical Industry , 2020 , 45 ( 6 ): 1 - 6 .

RIVERO-MENDOZA D , STANLEY J , SCOTT J , et al . An Alumina-supported Ni-La-based catalyst for producing synthetic natural gas [J ] . Catalysts , 2016 , 6 ( 11 ): 170 .

ALOTHMAN Z . A review: Fundamental aspects of silicate mesoporous materials [J ] . Materials , 2012 , 5 ( 12 ): 2874 - 2902 .

BHATTI U H , NAM S , PARK S , et al . Performance and mechanism of metal oxide catalyst-aided amine solvent regeneration [J ] . ACS Sustainable Chemistry & Engineering , 2018 , 6 ( 9 ): 12079 - 12087 .

王宁 , 陆诗建 , 刘玲 , 等 . 胺吸收体系中CO 2 催化解吸再生技术的研究进展 [J ] . 化工进展 , 2025 , 44 ( 1 ): 445 - 464 .

WANG N , LU S J , LIU L , et al . Research progress of catalytic regeneration for energy-efficient CO 2 capture in amine absorption system [J ] . Chemical Industry and Engineering Progress , 2025 , 44 ( 1 ): 445 - 464 .

ZHANG R , LI T , ZHANG Y M , et al . CuO modified KIT-6 as a high-efficiency catalyst for energy-efficient amine solvent regeneration [J ] . Separation and Purification Technology , 2022 , 300 : 121702 .

AN S L , XU T , XING L . Recent progress and prospects in solid acid-catalyzed CO 2 desorption from amine-rich liquid [J ] . Gas Science and Engineering , 2023 , 120 : 205152 .

LI T , YU Q , BARZAGLI F , et al . Energy efficient catalytic CO 2 desorption: Mechanism, technological progress and perspective [J ] . Carbon Capture Science & Technology , 2023 , 6 : 100099 .

ALIVAND M S , MAZAHERI O , WU Y , et al . Catalytic solvent regeneration for energy-efficient CO 2 capture [J ] . ACS Sustainable Chemistry & Engineering , 2020 , 8 ( 51 ): 18755 - 18788 .

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有机胺CO₂吸收液催化解吸研究进展

共轭聚合物在CO₂捕集中的作用机制及研究进展

高效低能耗氨基酸盐水溶液固-液相变吸收剂捕集CO₂性能探究

双金属负载γ-Al2O3固体酸催化CO2有机胺富液解吸性能

Catalytic performances of bimetal-loaded γ-Al2O3 solid acids for CO2 desorption from rich amine solution

DOI：10.12434/j.issn.2097-2547.20240407

摘要

Abstract

关键词

Keywords

references

双金属负载γ-Al₂O₃固体酸催化CO₂有机胺富液解吸性能

Catalytic performances of bimetal-loaded γ-Al₂O₃ solid acids for CO₂ desorption from rich amine solution