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JOURNAL OF MEMBRANE SCIENCE · 2021 · IF 8.742

Fabrication of highly (110)-Oriented ZIF-8 membrane at low temperature using nanosheet seed layer

Chenhan Zhang,Jiahui Yan,Taotao Ji,Dongying Du,Yanwei Sun,Liangliang Liu,Xiongfu Zhang,Yi Liu

Preferred orientation represents a main concern for microstructure control and performance optimization of MOF membranes. To date, it remains a challenging task to precisely control preferred orientation of ZIF-8 membrane. Herein, we prepared highly (110)-oriented ZIF-8 membrane by oriented secondary growth. Among various elements, preparation of uniform ZIF-8 nanosheet seeds through thermal conversion of identically shaped ZIF-L precursors, spin-coating-assisted oriented deposition of (110)-oriented ZIF-8 seed layer, and controlled in-plane secondary growth at low temperature were found crucial for obtaining well-intergrown (110)-oriented ZIF-8 membrane whose H 2 /CO 2 ideal selectivity exceeded H 2 /N 2 and H 2 /CH 4 under ambient conditions, owing to preferential CO 2 adsorption capacity of not only PEI but also ZIF-8 nanosheets compared with their bulk counterparts. Our research highlighted the significance of preferred orientation regulation in tailoring the gas permeation behavior of MOF membranes.

研究领域: 材料科学 · 化学工程 · 膜技术
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FLUID PHASE EQUILIBRIA · 2026 · IF 2.7

High-temperature solubility and thermodynamic correlation of CO2, H2, and CH4 in 1-Ethyl-2-pyrrolidone: Implications for catalytic CO2 hydrogenation to ethanol

Yufan Ma,Cong Liu,Hongxing Wang,Jie Li,Qingli Qian

The solubilities of CO 2 , H 2 , and CH 4 in 1-ethyl-2-pyrrolidone (NEP) were measured using the isochoric saturation method at 413.15–453.15 K under pressures of 0.45–3.89 MPa (CO 2 ), 4.42–7.64 MPa (H 2 ), and 0.59–3.49 MPa (CH 4 ). The reliability of the apparatus was verified by measuring CO 2 solubility in N-methyl-2-pyrrolidone (NMP) at 323.15–353.15 K. The solubility order in NEP was found to be CO 2 > CH 4 > H 2 . Temperature-dependent Henry’s constants were obtained, and the experimental data were correlated using the Krichevsky–Kasarnovsky equation and the generic Redlich–Kwong (RK) cubic equation of state, with the RK model providing better accuracy. These results offer essential thermodynamic data for describing gas–liquid equilibrium in NEP and support solvent selection and process design in high-temperature CO 2 conversion systems.

CAS / MDL: 872-50-4
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RSC Advances · 2016 ·Vol. 6 ·期 38 ·32400-32404 · IF 3.289

Propylene oxide as a dehydrating agent: potassium carbonate-catalyzed carboxylative cyclization of propylene glycol with CO2 in a polyethylene glycol/CO2 biphasic system

Zhen-Feng Diao,Zhi-Hua Zhou,Chun-Xiang Guo,Bing Yu,Liang-Nian He

The synthesis of propylene carbonate (PC) from 1,2-propylene glycol (PG) and CO2 was smoothly performed in a PEG800 (polyethylene glycol)/CO2 biphasic system with K2CO3 as a catalyst and propylene oxide (PO) as a dehydrating agent. In the reaction of PG with CO2, PO presumably removes the water produced, and simultaneously generates more PG, both of which shift the thermodynamic control process and thus accelerate the PC synthesis. The PC yield directly from PG and CO2 reached 78% under relatively mild reaction conditions (4 MPa, 120 °C, 10 h). Notably, no additional by-product was detected in this process, resulting in economic benefits and the ease of workup procedure.

研究领域: 绿色化学 · 二氧化碳利用 · 催化化学 · 有机合成 · 可持续化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2021 · IF 8.128

Taming structure and modulating carbon dioxide (CO2) adsorption isosteric heat of nickel-based metal organic framework (MOF-74(Ni)) for remarkable CO2 capture

Lei Lei,Yan Cheng,Changwei Chen,Mohammadreza Kosari,Zeyu Jiang,Chi He

Though the highest CO 2 capture capacity belongs to liquid amine-solutions, solid matters capable of CO 2 capture are also highly sought, providing that, they offer at least analogous CO 2 adsorption capacity and CO 2 /N 2 selectivity. Herein, a surprisingly high-performance Ni-based metal–organic framework for CO 2 adsorption, namely MOF-74(Ni), was synthesized by a facile condensation reflux approach. It was found that the structure and CO 2 adsorption isosteric heat of MOF-74(Ni) could tune upon varying the synthesis duration under various temperatures. The optimized MOF-74(Ni)-24-140 (synthesized at 140 °C for 24 h) displays outstanding CO 2 adsorption capacity of 8.29/6.61 mmol/g at 273/298 K under normal pressure of 1.0 bar, several times higher than previously reported MOF-74-Ni (2.0/2.1 times), UTSA-16 (1.5/1.6 times), and DA-CMP-1 (3.6/4.9 times) under similar conditions. The excellent CO 2 capture capacity is associated to the abundant adsorption sites (mainly arising from the cationic Ni 2+ ions) and narrow micropore channels (mainly arising from the cage structure of Ni 2+ ions coordinated with organic linkers). Offering a high CO 2 selectivity (CO 2 /N 2  = 49) and a well-tuned isosteric heat of CO 2 adsorption (27–52 kJ/mol) besides its decent CO 2 capture capacity, MOF-74(Ni) strongly stands out as an efficient and strong CO 2 capturing material with industrial scale applicability.

CAS / MDL: 64-17-5 68-12-2 610-92-4
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2021 · IF 3.764

Catalytic Performance and Mechanism of Meso–Microporous Material β-SBA-15-Supported FeZr Catalysts for CO2 Desorption in CO2-Loaded Aqueous Amine Solution

Yufei Huang,Xiaowen Zhang,Xiao Luo,Hongxia Gao,Zain Ali Saleh Bairq,Paitoon Tontiwachwuthikul,Zhiwu Liang

The huge energy consumption of rich amine solution regeneration severely restricts the large-scale application and promotion of the CO2 capture process by the amine method. In order to reduce the operating energy consumption during the CO2 capture process using amines, especially the energy consumption of absorbent regeneration, zeolite β/SBA-15 (BS) has been synthesized in this work using the hydrothermal method with zeolite beta (β) as the silicon source; β was used to prepare the novel Zr@BS and Fe–Zr@BS catalysts for amine regeneration. Experiments for CO2 stripping were performed at 370.15 K using amine solvent [monoethanolamine (MEA)] with an initial CO2 loading of 0.50 mol CO2/mol amine. Additionally, all the materials were characterized by X-ray diffraction, Fourier transform infrared spectroscopy, N2 adsorption–desorption experiment, ammonia temperature-programmed desorption, and pyridine adsorption infrared spectroscopy. Also, the catalytic CO2 desorption performances of seven different catalysts (β, SBA-15, three BS catalysts, Zr@BS, and Fe–Zr@BS) were investigated and assessed from the aspects of the cyclic capacity, desorption rate, and energy consumption. Experimental results indicated that the Fe–Zr@BS catalysts exhibited superior catalytic behaviors than other catalysts studied in this work, improving the desorption factor of MEA solution by 212% and bringing down the energy heat by 33% compared with 5 M MEA solution without catalysts. Furthermore, the Fe–Zr@BS catalysts show good stability and easy regeneration and do not influence absorption performance of the amine solution. Moreover, the possible catalytic mechanism for amine regeneration was proposed, and the stability of the material in terms of the structure of the material and the regeneration heat duty were also studied.

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ANALYST · 2020 ·Vol. 145 ·期 10 ·3528-3534 · IF 3.978

Synergy of CO2-response and aggregation induced emission in a small molecule: renewable liquid and solid CO2 chemosensors with high sensitivity and visibility

Zhijian Mai,Hao Li,Yixun Gao,Yue Niu,Yongrui Li,Nicolaas Frans de Rooij,Ahmad Umar,M. S. Al-Assiri,Yao Wang,Guofu Zhou

A tetraphenylethylene (TPE) derivative (N,N-dimethyl-N′-(4-(1,2,2-triphenylvinyl)phenyl)acetimidamide, TPE-amidine) was designed and synthesized, and used to prepare visible CO2 chemosensors, TPE-amidine-L (liquid) and TPE-amidine-S (solid). The hydrophilicity of TPE-amidine thoroughly changed because of the unique reversible reaction between the amidine group and CO2, which controlled the molecular aggregation extent in water by CO2. Combining with the well-known aggregate-induced emission effect, the highly selective CO2 chemosensor TPE-amidine-L was developed, which has the lowest CO2 detection limit of 24.6 ppm compared with other reported CO2 chemosensors, and can be regenerated within 10 s by adding triethylamine. With the aim of being safer and more convenient to use, a polyacrylamide hydrogel containing TPE-amidine was prepared as a renewable CO2 sensing “tape” (TPE-amidine-S). The flexibility, adhesivity, CO2 sensitivity and reversibility of the “tape” is systematically investigated, showing great potential for “on-site” and “real-time” CO2 detection in practical applications.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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JOURNAL OF MEMBRANE SCIENCE · 2015 · IF 5.056

Incorporating one-dimensional aminated titania nanotubes into sulfonated poly(ether ether ketone) membrane to construct CO2-facilitated transport pathways for enhanced CO2 separation

Qingping Xin,Yuying Gao,Xingyu Wu,Congdi Li,Tianyu Liu,Yue Shi,Yifan Li,Zhongyi Jiang,Hong Wu,Xingzhong Cao

One-dimensional aminated titania nanotubes were prepared by a facile distillation-precipitation polymerization method and were incorporated into sulfonated poly(ether ether ketone) (SPEEK) to fabricate mixed matrix membranes (MMMs). The aminated titania nanotubes (TNT-IM) with abundant amine groups increased the CO 2 -facilitated transport sites in MMMs. Moreover, the CO 2 -facilitated transport pathways (CO 2 -FTP) were constructed from aminated titania nanotubes in polymer matrix , and acted as the fast CO 2 transport channels to transfer CO 2 molecules continuously and smoothly. Water uptake and water state in MMMs also played an important role in the gas separation performance. The relationship between the water content and CO 2 separation performance was investigated. Nanotubes as fillers showed water retention properties during water evaporation from the MMMs at low humidity. The highest ideal selectivities of the SPEEK/TNT-IM MMMs for CO 2 /CH 4 and CO 2 /N 2 were 56.8 and 62.0, respectively, with a CO 2 permeability of 2090   Barrer.

CAS / MDL: 1072-63-5
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GREEN CHEMISTRY · 2016 ·Vol. 18 ·期 11 ·3370-3377 · IF 8.506

Hydrogenation of levulinic acid by RuCl2(PPh3)3 in supercritical CO2: the significance of structural changes of Ru complexes via interaction with CO2

Wenjing Yang,Haiyang Cheng,Bin Zhang,Yan Li,Tong Liu,Mingli Lan,Yancun Yu,Chao Zhang,Weiwei Lin,Shin-ichiro Fujita,Masahiko Arai,Fengyu Zhao

The hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL) was studied with a homogeneous RuCl2(PPh3)3 catalyst in supercritical CO2 (scCO2). The conversion of LA was observed to increase with CO2 pressure and the possible reasons for this rate acceleration were discussed, including the molecular interactions of CO2 with the reacting and catalytic species as well as the acidity and phase behavior of the reaction mixture. The interaction between CO2 and RuCl2(PPh3)3 was significant, which resulted in the production of an active RuHCl(CO)(PPh3)3 complex and thus enhanced the rate of hydrogenation in the presence of CO2.

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APPLIED ENERGY · 2017 · IF 7.182

Preferential enclathration of CO2 into tetra-n-butyl phosphonium bromide semiclathrate hydrate in moderate operating conditions: Application for CO2 capture from shale gas

Zheng Li,Dong-Liang Zhong,Yi-Yu Lu,Jin Yan,Zhen-Lin Zou

This work presents an investigation of using tetra- n -butyl phosphonium bromide (TBPB) semiclathrate hydrate for CO 2 capture from simulated shale gas that is composed of 40% CO 2 and 60% CH 4 in mole fraction. The experiments were performed in a stirred tank reactor with the mass fraction of TBPB ( w TBPB ) varying from 5.0% to 33.2%. The phase equilibrium data of TBPB semiclathrate hydrate formed in the presence of the 40% CO 2 /CH 4 gas mixture were measured and reported. The effects of TBPB concentration on gas solubility, hydrate formation kinetics, and CO 2 separation efficiency were investigated in the temperature range of 278.1–284.2   K with the initial pressure fixed at 2.8   MPa. The results indicated that at a fixed driving force (overpressure), the gas uptake obtained at the induction time was nearly constant, despite the variation in TBPB concentration, while the rate of hydrate formation increased with the increase in TBPB concentration. Compared to the results obtained at a mole fraction of 1% THF, it was found that enhanced hydrate formation kinetics, a higher CO 2 separation factor (31.7   ±   3.3), and a higher operating temperature (284.2   K) were obtained at the stoichiometric TBPB concentration ( w TBPB   =   33.2%). Therefore, TBPB may be used as a promising promoter for hydrate-based CO 2 capture from the simulated shale gas (CO 2 /CH 4 gas mixture).

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Journal of Environmental Chemical Engineering · 2024 · IF 7.4

Theoretical and experimental insights into the effects of CO2 on the heterogeneous NO reduction over char surface: Gasification and CO2-mediated oxygen rearrangement

Ji Liu,Yuan-gu Xia,Meng-fan Liu,Bin Hu,Hong-jin Zhang,Ji-hong Li,Zhen-xi Zhang,Qiang Lu

Nitrogen oxides are the major pollutants in solid fuel/waste combustion processes, which can be reduced by unburned or additive chars. The surface char–NO reaction is significantly influenced by CO 2 , whereas the impact mechanism is far from conclusive. Herein, fixed-bed experiments and computational methods were adopted to elucidate the role of CO 2 on char–NO reaction. Experimentally, CO 2 exhibited an inhibitive impact on NO reduction at 873 K but a promotive influence at 1023 K and 1173 K. According to the detection of outlet CO, characterization of char, and density function theory (DFT) calculations, CO and gasified char derived from char–CO 2 gasification are both responsible for the promotive effect at 1173 K, which offers a clear image of the gasification mechanism conjectured in previous work. More importantly, a CO 2 -mediated oxygen rearrangement (CO 2 -MOR) mechanism has been found and confirmed for the first time, which can well explain the experimental results observed at 873 K and 1023 K. The adsorbed CO 2 can intervene in the oxygen rearrangement on the char surface to alter the NO reduction behaviors. The present study offers a comprehensive insight into the roles of CO 2 in the heterogeneous reduction of NO on char surface.

CAS / MDL: 7440-44-0
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JOURNAL OF MEMBRANE SCIENCE · 2024 · IF 8.4

Tartaric acid anion intercalated layered double hydroxides constructed a CO2-favorable transport channel in PIM-1 mixed matrix membranes for CO2/N2 separation

Caifeng Xia,Qikang Yin,Xinle Sun,Qinglong Liu,Sen Liu,Shuxian Wei,Siyuan Liu,Weifeng Lv,Zhaojie Wang,Xiaoqing Lu

As a unique polymer of intrinsic microporosity, PIM-1 has great potential in mixed matrix membranes (MMMs) for gas separation with ultra-high permeability. However, the separation performance, e.g. CO 2 /N 2 separation, is still limited by its poor selectivity. In this work, PIM-1-based MMMs containing tartaric acid anion intercalated layered double hydroxides (TA-LDH) nanofillers are successfully prepared. The uniformly dispersed TA-LDH in the PIM-1 matrix contributes to optimizing the stacking of polymer chains for accessible pores, which is conducive to CO 2 diffusion. In addition, the assistant experiment and theoretical calculation point out that the -COO - , –OH between the TA-LDH layers had an affinity for CO 2 , creating a two-dimensional fast transport channel between the enlarged interlayer space. Compared with the pristine PIM-1 membrane, the CO 2 permeability and CO 2 /N 2 selectivity of 0.7 % TA-LDH/PIM-1 membrane is increased by 43.19 % and 105.48 %. The excellent gas separation performance with CO 2 permeability of 8343.18 Barrer and CO 2 /N 2 selectivity of 39.02 exceeds the 2019 Robson upper limit. This paves a new way to improve the gas separation performance of PIM-1-based MMMs and suggests high perspectives for real applications.

CAS / MDL: 6381-59-5
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ENERGY · 2025 · IF 9.4

Dual-objective enhancement of CO2 injection and hydrate conversion for CO2 solid sequestration in submarine sediments via penicillin G sodium solution pre-injection

Ming-Long Wang,Yi-Fei Sun,Hong-Nan Chen,Jin-Rong Zhong,Dan Rao,Yu Liu,De-Jun Xuan,Bei Liu,Chang-Yu Sun,Guang-Jin Chen

CO 2 hydrate provides an important way for the long-term stable CO 2 geological sequestration considering CO 2 has potential self-sealing ability in submarine hydrate stable zone. However, the insufficient displacement efficiency of pore water and hydrate conversion rate pose significant challenges to ensuring long term CO 2 injection and hydrate sequestration under shallow burial sediments. Here, to enhance CO 2 injection into water-saturated sediments and hydrate conversion, we report a novel self-emulsification injection approach via penicillin G sodium solution pre-injection, which enables the rapid dispersion of injected CO 2 into the pore water as micro- and nano-sized CO 2 droplets in submarine sediments. The effects of liquid CO 2 injection rate, flow distance, sediment particle size, and reagent dosage on droplet dispersion were quantitatively analyzed. On this basis, we further tested its complex behaviors of displacement flow and hydrate formation. The results indicate that compared to conventional liquid CO 2 injection, self-emulsification injection effectively reduces injection pressure by 25 %–49 % and achieves the CO 2 storage density up to 181 kg/m 3 , indicating that this method is more suitable for rapid and large-scale CO 2 injection on the seabed. Moreover, the sufficiently small CO 2 microdroplets generated by self-emulsification flow almost eliminate the interphase hydrate membrane effect, thereby increasing the CO 2 hydration rate to over 70 %. This provides a guarantee for the effective establishment of CO 2 hydrate sealing cap in shallow seabed sediments. Given its comprehensive excellent performance, the self-emulsification injection technology is expected to significantly advance the hydrated CO 2 sequestration.

CAS / MDL: 7647-14-5 7732-18-5
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