FLUID PHASE EQUILIBRIA
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2024
·
IF 2.8
Nan He,Yukun Zhang,Fenhong Song,Jing Fan,Xiwu Zhang
Deep eutectic solvents (DESs) have appealed increasing research interest across various scientific and industrial applications, notably in relation to efforts in CO 2 capture. This study presents a novel series of DESs were synthesized on the basis of monoethanolamine (MEA) and N-methyldiethanolamine (MDEA) as hydrogen bond donors with tetrabutylammonium bromide (TBAB) and tetrabutylphosphine bromide (TBPB) salt as hydrogen bond acceptors. A gas solubility measurement experimental system based on pressure drop method has been established to evaluate the solubility of CO 2 in amine-based deep eutectic solvents. The evaluation was performed over a temperature range of 303.15 to 323.15 K and a pressure range of 100 to 1000 kPa. The results indicated that as the molar ratio of hydrogen bond donors increases, the solubility of CO 2 in DESs increases, while it was found to be less affected by the hydrogen bond acceptor. Of these, the solubility of CO 2 is strongest at a 1:10 molar ratio of TBAB and MEA. The nuclear magnetic resonance spectroscopy spectra (NMR) and FTIR spectroscopy revealed that the MEA-based DES mixture primarily exhibited chemical absorption of CO 2 , while the MDEA-based DES predominantly showed physical dissolution of CO 2 . In addition, it was observed that both temperature and pressure significantly influenced the CO 2 solubility, and a successful correlation was developed using different semi-empirical models.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Dan Gao,Yuanyuan Cao,Zhaohao Li,Niankun Guo,Hongyuan Zhang
The waste heat utilization in the coal-fired plant has always been one of important ways of the energy saving. In this paper, a novel device is constructed by the combination of the ceramic membrane desorption and the flue gas waste heat utilization. In the device, the absorption solution is the “double-cationic” ionic liquid ([TEPA][1-MIm]). Furthermore, experimental results show that the contact angle of the hydrophobic ceramic membrane is 130°. Under ambient temperature conditions, it is observed that at a concentration of 25 % [TEPA][1-MIm] in an ethylene glycol solution, the maximum absorption amount of CO 2 reaches approximately 1.605 mol CO 2 /mol amine. The saturation time of the absorption is about 20 min. As the concentration of ionic liquids increases, the saturation time gradually extends due to an increase in [TEPA][1-MIm] and consequently higher total CO 2 absorption mass. Subsequently, effects of the operating parameters on the desorption rates are analyzed. The contribution of this work is to put forward the idea of utilizing ceramic membranes to recover the waste heat from the flue gas to reduce the CO 2 desorption energy consumption. According to experiments, the overall heat transfer coefficient can reach 20.33 W/(m 2 ·K), and the amount of the recovered waste heat can reach 29.97 W.
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RSC Advances
·
2024
·Vol. 14
·期 5
·3146-3157
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IF 3.9
Yanlong Hu,Qiang Wang,Dingkai Hu,Yingshuang Zhang,Muhammad Furqan,Shijian Lu
Monoethanolamines (MEAs) are widely used for CO2 capture, but their regeneration energy consumption is very high. CO2 Phase change absorbents (CPCAs) can be converted into CO2-rich and CO2-lean phases after absorbing CO2, and the regeneration energy consumption can be reduced because only the CO2-rich phase is thermally desorbed. In this paper, a novel CPCA with the composition “MEA/n-butanol/H2O (MNBH)” is proposed. Compared with the reported MEA phase change absorbent, the MNBH absorbent has higher CO2 absorption capacity, smaller absorbent viscosity and CO2-rich phase volume. The MNBH absorbent has the highest CO2 absorption capacity of 2.5227 mol CO2 per mol amine at a mass ratio of 3 : 4 : 3. The CO2 desorption efficiency reaches 89.96% at 120 °C, and the CO2 regeneration energy consumption is 2.6 GJ tCO2−1, which is about 35% lower than that of the 30 wt% MEA absorbent. When the mass ratio of MNBH absorbent was 3 : 6 : 1, the CO2 recycling capacity was 4.1918 mol CO2 L−1, which is 76% higher than that of the conventional 30 wt% MEA absorbent. The phase change absorbent developed in this paper can reduce the desorbent volume by about 50% and has good absorption performance for CO2 in flue gas.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Yunpeng Liu,Lei Gong,Jianglong Liu,Peng Xiao,Baotong Chen,Fei Xie,Caoyu Yang,Zhonghua Wu
The production of formic acid/formate from electrochemical CO 2 reduction reaction (CO 2 RR) is fascinating but challenging due to the lack of highly active electrocatalysts. Herein, uniform PVP-capped bismuth nanospheres (PVP@Bi-NSs) with a capping-bonding synergy were optimally fabricated to enhance the CO 2 RR to formate. This study unveils the reaction process in Bi-based solution. It was found that the formation of PVP@Bi-NSs experienced five stages of Bi-O 8 (I), Bi-O 3 (II), Bi-O 4 (III), Bi-Bi 6 (IV), and PVP@Bi-NSs (V), corresponding to the nucleation in precursor solution, Bi(OH) 3 precipitate, decomposition to KBiO 2 , reduction to metallic Bi, and PVP coating, respectively. By solvothermal treatment and simply modulating the KOH concentration in the precursor, the hydrophilic ends of PVP molecules can be well bonded to the Bi nanoparticles (Bi-NPs) to form a PVP-capping layer. Compared with the Bi-NPs without PVP coating, this uniform PVP@Bi-NSs displays a higher activity with a maximal Faradaic efficiency (FE) of 92.5 % and part current density ( J formate ) of 158.2 mA cm −2 at −0.9 V vs. RHE in the flow cell as well as excellent stability, which is comparable to the state-of-the-art Bi-based catalysts. The maximum J formate can reach 280 mA cm −2 with an FE of 87.3 % at −1.2 V vs. RHE, meeting the needs of industrial current density. Further characterizations show that the capping effect of PVP contributed to the uniform distribution of nanosized PVP@Bi-NSs, increasing the electrochemical surface areas (ECSAs) and the numbers of CO 2 RR active sites. The bonding effect of PVP to Bi-NPs enhanced the hydrophobic property of PVP@Bi-NPs, boosting the CO 2 absorption and suppressing the hydrogen evolution reaction (HER). DFT calculations reveal that this fabricated structure facilitates the generation of *OCHO intermediate and benefits formate yield. This work provides a fascinating strategy for the design of Bi-based catalysts, enabling interface engineering toward high-efficiency CO 2 RR.
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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
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2024
·Vol. 121
·期 25
·e2400546121
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IF 9.4
Yu-Cai Zhang,Xiao-Long Zhang,Zhi-Zheng Wu,Zhuang-Zhuang Niu,Li-Ping Chi,Fei-Yue Gao,Peng-Peng Yang,Ye-Hua Wang,Peng-Cheng Yu,Jing-Wen Duanmu,Shu-Ping Sun,Min-Rui Gao
Reduction of carbon dioxide (CO2) by renewable electricity to produce multicarbon chemicals, such as ethylene (C2H4), continues to be a challenge because of insufficient Faradaic efficiency, low production rates, and complex mechanistic pathways. Here, we report that the rate-determining steps (RDS) on common copper (Cu) surfaces diverge in CO2 electroreduction, leading to distinct catalytic performances. Through a combination of experimental and computational studies, we reveal that C─C bond-making is the RDS on Cu(100), whereas the protonation of *CO with adsorbed water becomes rate-limiting on Cu(111) with a higher energy barrier. On an oxide-derived Cu(100)-dominant Cu catalyst, we reach a high C2H4 Faradaic efficiency of 72%, partial current density of 359 mA cm−2, and long-term stability exceeding 100 h at 500 mA cm−2, greatly outperforming its Cu(111)-rich counterpart. We further demonstrate constant C2H4 selectivity of >60% over 70 h in a membrane electrode assembly electrolyzer with a full-cell energy efficiency of 23.4%.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Linbo Yang,Yichao Lin,Yayun Zhao,Jiejie Li,Ziqi Tian,Yaqi Wu,Haitao Hu,Hao Wang,Liang Chen
Zeolites are promising materials for CO2 adsorption, yet they still face the challenges of low adsorption capacity and selectivity. Herein, we report a strategy of grafting ethylenediamine to a Co-exchanged Y zeolite to improve the CO2 adsorption capacity of Y zeolite via strong interactions between Co2+ and amine groups. Functionalization of zeolite Y with amines (Co-Y-EN) enables significant improvement in the CO2 adsorption capacity (4.36 mmol/g at 1 bar and 298 K), which is 1.73 times higher than that of pristine Na-Y zeolite. Moreover, Co-Y-EN demonstrates enhanced CO2 selectivity, as confirmed by both single-component gas adsorption experiments and breakthrough tests. The superior selectivity is attributed to the strong affinity between the amine sites and CO2 molecules, as well as the optimized pore sizes for CO2 adsorption. Overall, this study presents a straightforward approach to enhancing the CO2 adsorption performance of zeolite materials.
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JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Yunqi Zhou,Ye Yuan,Xinlei Liu,Zhi Wang
Metal-organic framework (MOF) membranes with proper pore size distribution and functional groups are generally more suitable for separation. Most MOFs are characterized by a hierarchical pore structure, which possesses large cavities surrounded by small windows. Fabrication of MOF membranes only retaining microporous fragment structure is a workable method to narrow pore size distribution. In this study, well-grown NH 2 -MIL-101(Cr) fragment membranes were fabricated for CO 2 separation by adjusting acetic acid – ligand – metal ratio to balance the nucleation and growth. NH 2 -MIL-101(Cr) fragment has a similar chemical structure to NH 2 -MIL-101(Cr) as expected, but only small pores with size around 0.56 nm is retained. The NH 2 -MIL-101(Cr) fragment membranes exhibited CO 2 /N 2 selectivity of about 37 with CO 2 permeance up to 6104 GPU.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Chen Xue,Libin Liu,Yuxi Si,Yangqiang Huang,Shengdong Yang,Kuanrong Xue,Jun Xi,Youwei Cheng
The direct esterification reaction of CO2 with methanol to produce dimethyl carbonate (DMC) provides a sustainable pathway for the resourceful utilization of CO2. However, the chemical stability of CO2 makes the reaction kinetically difficult with low methanol conversion and DMC yields. In this study, a series of catalysts (denoted as M-CeO2, M = Fe, Cu, Co, La, Zr, Ni, and Al) with oxygen vacancy defects were constructed by a doping strategy, which provided critical sites for the adsorption and activation of methanol and CO2. Additionally, 2-cyanopyridine (2-CP) was employed as a dehydrating agent to facilitate the esterification reaction through dehydration. Under the optimized experimental conditions, the conversion of methanol was 61.9% and the DMC yield was 61.6%. The experimental and characterization results show that the extensive oxygen vacancies and base sites on the surface of the 5% Co-CeO2 catalyst are crucial for activating methanol and CO2, which is the main reason for the high catalytic activity of the catalyst. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) effectively demonstrated the efficient activation of methanol and CO2 on the catalyst and further confirmed the formation of monomethyl carbonate species during the reaction process. The high catalytic performance was also demonstrated in the direct esterification of other monohydric alcohols, thus confirming the broad applicability of the catalyst. This study presents a viable approach for the efficient utilization of CO2 resources, offering a promising solution for the sustainable management of greenhouse gas.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Manman Zhang,Raphael Semiat,Xuezhong He
Design and synthesis of novel poly(ionic liquids) (PILs) containing amino groups hold great promise in CO 2 separation fields owing to the tunability of the cation and anion, as well as the high CO 2 affinity of the amino groups. Herein, two novel amino-functionalized PILs were designed for the preparation of composite membranes by casting the synthesized PIL-based solutions on the top of polysulfone ultrafiltration membranes to explore the effect of different chemical structures on the separation performances of the NH 2 -carrier-based membranes. Highly CO 2 -selective membranes with a CO 2 /N 2 selectivity of 173.5 were obtained by introducing the mobile carrier of 2-(1-piperazinyl) ethylamine sarcosine (PZEA-Sar) into the amino-functionalized PIL-based membranes, which provides the synergistic effect from both fixed-site and mobile carriers for promoting CO 2 -facilitated transport. Thus, the developed membranes may offer a high energy-efficiency process for industrial CO 2 capture.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Maijun Li,Yubo Long,Zhibo Zheng,Xu Hu,Siwei Liu,Zhenguo Chi,Nanwen Li,Jiarui Xu,Yi Zhang
Chemical modification of polyimide membranes is employed to achieve “trade-off” breakthrough or improve the plasticization resistance in CO2 separation. However, harsh reaction conditions restrict the application of traditional chemical modifications. In this work, a simple chemical modification method─the coordination cross-linking between hydroxyl groups on polyimide (6FSPI) and Zn(II)─was investigated. Because of the reversible complexation of Zn(II) in the modified membrane as a transport carrier with CO2, and the addition of Zn(II) disrupts coiled chain of spiro moiety or intrachain cross-linking to induce more quantities of ultrafine micropores, the CO2 permeability coefficient of the modified membrane is 2.97 times that of the pristine 6FSPI. Simultaneously, there is improvement in diffusion selectivity of the modified membrane, resulting in the CO2/CH4 selectivity improvement. The overall CO2/CH4 separation performance of the modified membrane reaches up to the 2008 Robeson limit. In addition to serving as facilitated transport carriers, Zn(II) can also be used as cross-linking points. The modified membrane maintains a stable CO2 permeability coefficient beyond 4000 kPa. Our work suggests that the Zn(II) coordination cross-linking is a facile chemical modification method that can enhance long-term performance and separation performance of polyimide membranes simultaneously.
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FUEL
·
2024
·
IF 6.7
Wenxia Wang,Yuliang Zhu,Yingchao Hu
High-temperature CO 2 capture based on Li 4 SiO 4 sorbents has been well recognized as an effective approach to mitigate the global warming issues. However, the relatively low sorption performance is one of the biggest challenges for the practical application. In the current investigation, Na- and Y-based dopants have been employed to enhance cyclic CO 2 sorption performance of Li 4 SiO 4 sorbents. Various physicochemical properties and cyclic CO 2 sorption performance of the prepared sorbents have been systematically studied. The results indicated that Na 2 CO 3 and Y 2 O 3 codoped Li 4 SiO 4 sorbent (Li 4 SiO 4 -10Na-15Y) exhibited excellent cyclic CO 2 capture performance with stable capacity of >0.27 g CO 2 /g sorbent (corresponding to the carbonation conversion of ∼96 %) during 15 sorption/desorption cycles. Even under lower CO 2 concentration and longer cycles, satisfying conversions of 85 % could be kept in the cyclic tests for the codoped Li 4 SiO 4 sorbent. In addition, the materials also showed high heat storage density of 557.8 kJ/kg and the performance was stabilized in the multicycle energy storage/release tests. The characterization results showed that the introduction of Y-based dopants induced triple positive effects for Li 4 SiO 4 including porosity creation, sintering-resistant ability, and producing Li 4 SiO 4 lattice defects. As a result, the enhanced specific surface area and reduced diffusion resistance were achieved and, thus, the CO 2 sorption performance including sorption capacity (heat storage density) and cyclic stability was obviously improved.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Pengchao Zang,Jiyun Tang,Yihui Tao,Hao Zhang,Xiaozhe Wang,Lin Cui,Shouyan Chen,Pei Zhao,Yong Dong
Calcium looping (CaL) represents a promising technology for CO 2 capture from flue gas. Nevertheless, CaO-based sorbents, characterized by high theoretical absorption capacities and low costs, experience significant degradation in CO 2 capture capacity during continuous cycling. In the present study, a novel K 2 CO 3 -doped CaO sorbent was synthesized through a concurrent hydrophilic impregnation process, and the performance of consecutive cyclic CO 2 capture was evaluated. The optimal 0.05 K-CaO demonstrated the highest CO 2 sorption (12.4 mmol/g), maintaining about 64 % of the initial sorption after 20 repetitive cycles under N 2 calcination atmosphere, which is 6.6 times greater than that of CaO. These findings indicated that K 2 CO 3 can regulate the particle size and the state of surface oxygen species in CaO-based sorbents while simultaneously enhancing CO 2 diffusivity on the sorbent surface. The DFT calculations indicated that the incorporation of K 2 CO 3 improved the mechanism of CaO chemisorption of CO 2 . Additionally, the vacancies and CO 3 2– generated by K 2 CO 3 doping can enhance the CO 2 sorption energy and reduce the system’s energy level. Notably, the net charge transfer for CO 2 sorption from K 2 CO 3 doping is greater than that from pure CaO, and the O atoms on the surface of K 2 CO 3 -CaO (001) exhibit strong covalent interactions with the C atoms in CO 2 , both of which facilitate CO 2 chemisorption. This study offers a comprehensive theoretical mechanism for the incorporation of K-based alkali metals to enhance the CO 2 capture performance of CaO sorbents.
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