SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Xing Li,Lei Xing,Chunyu Zhang,Shudan He,Fanghua Liu,Zhen Chen,Huazhen Chang,Junhua Li
Catalytic solvent regeneration is widely considered a promising solution for addressing the intensive heat duty of amine-based carbon dioxide (CO 2 ) capture. This highly challenging application has motivated researchers to develop excellent catalysts with high activity and durability. In this study, we engineered active and durable Fe − N − C catalyst coated with high-graphitization carbon layers (labeled Phen − Fe − N − C) through a secondary thermal pyrolysis treatment. The multiple graphite layers and atomic metal sties were verified by experimental characterization and coordination structure analysis. The improved graphite layers further enhanced the activity of Fe − N − C sites, providing more acid sites for proton-electron transfer and C − N breaking during solvent regeneration (or CO 2 desorption). Thus, the maximal CO 2 desorption rate increased by 50 % when Fe − N − C was used compared with that of the blank case, and the rate further increased by 27 % when Phen − Fe − N − C was used. After 15 days of hydrothermal testing, the single Fe atom over the spent catalysts presented no significant aggregation or dissolution in the solvent, validating the durability of Phen − Fe − N − C. This work demonstrates a feasible and novel strategy to improve M − N − C materials for efficient and robust CO 2 desorption from amine solvents toward energy-saving CO 2 capture.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED ENERGY
·
2017
·
IF 7.182
Xiaowen Zhang,Xin Zhang,Helei Liu,Wensheng Li,Min Xiao,Hongxia Gao,Zhiwu Liang
In this work, the regeneration of rich CO 2 -loaded monoethanolamine (MEA) solvent with two catalysts (e.g. SAPO-34 and SO 4 2− /TiO 2 ) was investigated in order to reduce the energy requirement for solvent regeneration. The regeneration behavior with and without catalyst of a 5M MEA solution with an initial CO 2 loading of 0.5 mol CO 2 /mol amine at 96 °C was studied to compare their CO 2 desorption rate and heat duties. The results show that the two solid acid catalysts can reduce the heat duty for solvent regeneration and increase the CO 2 desorption rate in comparison with blank test. The mechanism of CO 2 desorption with catalyst in 5M MEA was proposed based on the result of catalyst characterization (e.g. N 2 absorption/desorption experiment, Py-IR, NH 3 -TPD, FT-IR and XRD) to better understand the desorption process. The results indicate that SAPO-34 with the higher joint value of Brϕnsted/Lewis acid sites ratio (B/L) and mesopore surface area (MSA) shows the faster CO 2 desorption rate and lower heat duty than SO 4 2− /TiO 2 . Based on the experimental results, the addition of solid acid catalysts into amine solution could be considered as one of choices to reduce the heat duty for CO 2 desorption from CO 2 -loaded amine solvent.
研究领域:
化学工程
·
环境科学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2025
·
IF 7.5
Wenqian Song,Yuxin Wen,Guojun Kang,Wenqing Lv,Dekang Li,Haoquan Hu,Lijun Jin,Shijian Lu,Zhong Yan,Pengfei Liu
Amine-based solution absorption as the most promising and commercialized CO 2 capture method, attracted the increasing attention. However, its key lies in improving the CO 2 desorption performance while reducing the energy consumption in desorption. In this paper, HZSM-5 was dealuminated by sulfuric acid, further loaded by Fe 2 O 3 , Co 3 O 4 , NiO and ZnO via impregnation method and used in catalytic desorption of the blended amine solution of N-methyl-diethanolamine and piperazine. Results indicated that sulfuric acid leaching increased the number of acid sites and mesoporous surface area. When sulfuric acid reached 0.8 mol/L, the resultant catalyst (0.8H 2 SO 4 -HZ) improved the amount of the desorbed CO 2 by 10.26% and decreased the heat duty to 2128 kJ/mol CO 2 , with a reduction of 17.01% compared to non-catalytic system. The loading of metal oxides on 0.8H 2 SO 4 -HZ decreased surface area and changed acidity of catalysts. CO 2 desorption amount under catalysis of metal oxide modified M /0.8H 2 SO 4 -HZ followed the order of Fe/0.8H 2 SO 4 -HZ > Zn/0.8H 2 SO 4 -HZ > Ni/0.8H 2 SO 4 -HZ > Co/0.8H 2 SO 4 -HZ, whereas the relative heat duty was in order of Zn/0.8H 2 SO 4 -HZ > Co/0.8H 2 SO 4 -HZ > Ni/0.8H 2 SO 4 -HZ > Fe/0.8H 2 SO 4 -HZ. Fe/0.8H 2 SO 4 -HZ exhibited excellent catalytic performance, along with 12.82% increase in amount of CO 2 desorbed and reduction in heat duty to 2039 kJ/mol CO 2 , with a 20.49% decrease. Meanwhile, Fe/0.8H 2 SO 4 -HZ showed good stability after ten cycles and the addition of Fe/0.8H 2 SO 4 -HZ promoted CO 2 absorption. Suitable pore structure and abundant acid sites of the modified catalyst contributed to proton transfer and decomposition of carbamate. A possible mechanism for catalytic desorption over modified HZSM-5 was proposed. The work indicates that catalytic desorption by modified HZSM-5 catalyst is a promising way to decrease the energy consumption of amine solution regeneration.
研究领域:
化学工程
·
环境科学
·
能源化学
·
催化化学
·
气体分离
·
材料科学
·
工业催化
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Liju Bai,Shijian Lu,Qizheng Zhao,Linlin Chen,Yingjie Jiang,Chunxiao Jia,Siming Chen
Non-aqueous biphasic solvents, which combine the advantages of a non-aqueous absorbent and biphasic absorbent, have attracted increasing attention for CO 2 capture because of their great potential to reduce the energy consumption. This study proposed a non-aqueous N -ethylethanolamine (EMEA)/ N , N -diethylethanolamine (DEEA)-based liquid–liquid biphasic absorbent with p -xylene (PX) to replace 45–65 % of DEEA. The biphasic absorbent comprising 30 wt% EMEA + 5 wt% DEEA + 65 wt% PX (30E5D65P) had the best phase-change behaviour. In this absorbent, 98.8 % of the absorbed CO 2 was in the lower phase of the solvent, with a volume percentage of 35.1 %. This absorbent also showed the best CO 2 -desorption performance, with almost double the CO 2 -desorption amount and maximum CO 2 -desorption rate compared with those achieved using the 30 wt% EMEA + 70 wt% DEEA (30E70D) non-aqueous absorbent. The regeneration energy of 30E5D65P was 1.71 GJ∙t −1 CO 2 , which was reduced by 31 % and 55 % compared with that of the non-aqueous 30E70D absorbent and the aqueous 30 wt% monoethanolamine absorbent, respectively. 13 C NMR analysis and quantum chemical calculations showed that carbamate and PX have a better separation effect than that of EMEA and DEEA, owing to the presence of both polarity and hydrogen bonding. PX with low polarity was beneficial for the separation of carbamate. The carbamate interacted with (protonated) EMEA, (protonated) DEEA and carbamic acid through hydrogen bonds, resulting in the appearance of these components in the lower phase. The carbamate had no hydrogen bond self-aggregation, which may be the reason why there was no crystal precipitation.
研究领域:
化学工程
·
环境科学
·
能源技术
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yingjie Niu,Shiying Zou,Haonan Liu,Minyue Hu,Jinjun Cai,Chao'en Li,Kathryn A. Mumford,Masood S. Alivand,Francesco Barzagli,Rui Zhang
Improving the energy efficiency of CO 2 desorption remains a key challenge in post-combustion carbon capture using amine solvents. In this work, a series of solid acid catalysts based on sulfonated mesoporous SBA-15 and functionalized with phosphotungstic acid (HPW) were synthesized via post-synthetic modification and applied to the catalytic regeneration of monoethanolamine (MEA). The catalysts, featuring both Brønsted and Lewis acid sites, were thoroughly characterized and tested in desorption experiments using CO 2 -loaded MEA solutions. Among the synthesized materials, HPW-SBA-15-SO 3 H-1 exhibited the best performance, achieving significantly higher CO 2 desorption rate and cyclic capacity compared to the uncatalyzed system, while reducing the relative heat duty by up to 37.7 %. This catalyst also demonstrated good stability over 20 absorption–desorption cycles, maintaining its structural integrity. In addition, machine learning was employed to correlate the catalysts' physicochemical features with their desorption performance, highlighting the role of acidity and porosity and supporting the proposed mechanism by which acidic sites promote carbamate decomposition and MEAH + deprotonation. These findings underscore the potential of functionalized mesoporous silica as efficient solid catalysts for lowering the regeneration energy penalty in MEA-based carbon capture systems.
研究领域:
化学工程
·
材料科学
·
环境科学
·
催化
·
机器学习
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）