JOURNAL OF MEMBRANE SCIENCE
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2017
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IF 6.035
Ning Zhang,Dongdong Peng,Hong Wu,Yanxiong Ren,Leixin Yang,Xingyu Wu,Yingzhen Wu,Zihan Qu,Zhongyi Jiang,Xingzhong Cao
For high-performance hybrid membranes, it is crucial to design multi-functional filler to rationally manipulate the structure-property relationship. In this study, a novel kind of hybrid membrane was fabricated by incorporating zinc ion loaded sulfonated pitch (SP-Zn 2+ ) nanofillers into poly (ether-block-amide) (Pebax) matrix for CO 2 /CH 4 separation. Sulfonated pitch (SP) with high sulfonate content was functionalized by zinc ion (Zn 2+ ) via complexation reaction to synthesize SP-Zn 2+ nanofillers with high Zn 2+ loading. Mixed gas separation performances of membranes with different SP-Zn 2+ loading were conducted. Meanwhile, the effect of operating pressure on separation performance and long-term operation stability were investigated. The hybrid membranes displayed significantly enhanced permeability and CO 2 /CH 4 selectivity. First, the hydrophilic sulfonate group in SP had good compatibility with Pebax matrix and effectively suppressed interfacial defects. Second, zinc ions and sulfonate group could form zinc-sulfonate complex network. The sulfonated moiety afforded strong affinity toward CO 2 due to multiple interactions whereas the Zn 2+ moiety afforded a transport highway for CO 2 . Third, the incorporation of SP-Zn 2+ nanofillers could disturb the Pebax chain packing and optimize the free volume characteristics. Particularly, Pebax/SP-Zn 2+ (2) membrane exhibited an increment of 104% and 70.2% in CO 2 permeability and CO 2 /CH 4 selectivity respectively, much higher than that of Pebax membrane.
研究领域:
材料科学
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化学工程
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环境科学
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产品关联
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2023
·Vol. 10
·期 15
·4519-4525
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IF 7
Chaoran Wang,Xiao Li,Shiyue Liu,Tingting Wang,Puxu Liu,Xiaowei Song,Zhiqiang Liang
Silicoaluminophosphate (SAPO) zeolites with small pores (8-ring window), such as SAPO-34, SAPO-17, and SAPO-RHO, have attracted a lot of attention due to their unique structural features, and their applications in the field of small-molecule gas adsorption and separation. However, the fast, efficient and green synthesis of SAPO zeolites remains a great challenge. In this work, SAPO-17 zeolites were synthesized within 1 min for the first time by a seed-assisted microwave method, and the resulting samples possessed excellent performance in the application of CO2 adsorption and separation for flue gas and natural gas. The microwave-assisted route can shorten the crystallization time of traditional hydrothermal methods from a few hours to 30 min. Furthermore, the crystallization time could be drastically shortened to 1 min with the addition of seeds, which represents the shortest time for the preparation of a SAPO-17 zeolite up to now. SAPO-17 synthesized within 1 min (SAPO-17-S-1) possessed the smallest crystal size, and the largest micropore volume and specific surface area among all the samples, which enhanced mass transfer and exposed more active sites, and thus it possessed prominent performance for CO2 adsorption (3.47 mmol g−1 at 273 K and 1 bar) and gas separation. At 298 K and 100 kPa, SAPO-17-S-1 exhibited the highest gas selectivity for CO2/N2 (276) and CO2/CH4 (63) over the other samples, which were synthesized in a relatively long time. Transient binary breakthrough experiments on SAPO-17-S-1 further verified the highly-efficient gas separation performance. This work proposes a green and ultrafast strategy for the synthesis of SAPO-17 zeolites with highly selective CO2 adsorption over N2 and CH4.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2024
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IF 3.8
Zhilin Ma,Yongda Cao,Xiujun Peng,Qiulin Yang,Chao Wang,Chang-An Zhou,Lei Song,Kui Ma,Hairong Yue
The chemical absorption method using MEA has been one of the most effective CO2 capture technologies, but the problems of low process efficiency and poor economics limit its application. In this work, the rapid phase change absorbent composed of alcohol ether solvent and potassium amino acid salt (AaK) solution was investigated, and the effects of different AaKs and ethers on the phase change behavior, phase separation mechanism, and CO2 absorption performance of the absorbent were analyzed. The results showed that when the carbon chain of the linear AaK was longer, the solubility in water was larger, and the lower liquid phase (LP) volume, phase separation time, AaK enrichment in the LP, and CO2 molar loading were larger. When the alkyl group of the branched-chain AaK was larger, the solubility in water was smaller, and the gas–liquid mass transfer, enrichment effect, and absorption rate were smaller. When the ether bonds of ether solvent were greater, the solubility of organic salts and competition for water were stronger; thus, the LP volume was smaller. Moreover, the absorption rate and CO2 loading of AaK systems were affected by the spatial structure effect of amino and carboxyl groups and the viscosity effect of solvent before absorption.
研究领域:
化学工程
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环境科学
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能源技术
✓ 已验证
产品关联
DOI
高影响因子
Sustainable Chemistry for Climate Action
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2023
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IF 0
Ya-Qi Ba,Yong-Sheng Wang,Tian-Yi Li,Zhe Zheng,Guang-Ping Hao,An-Hui Lu
CO 2 capture from flue gas is one of the global urgent tasks. Adsorption separation of CO 2 is an energy-efficient way as compared to the absorption method. The central issue is to devise efficient adsorbents that work well under flue gas conditions with temperatures of 323–348 K and low CO 2 concentrations of 15%. In this work, we targeted this issue and proposed a well-controlled diffusion strategy, which is achieved over a series of poly(furfuryl alcohol)-derived carbons (PFCs) with dense and abundant ultra-micropores. As the adsorption temperature increased from 298 to 348 K, the CO 2 capture capacity is 54% kept for PFC-800, which is 1.2 times higher than that for samples without diffusion limitation. The capture of CO 2 is kinetics control at ambient temperature, however, at 348 K CO 2 with higher kinetic energy can overcome the restriction of the narrow pore entrance and the CO 2 /N 2 selectivity for simulated flue gas composition increases from 20 to 40. Furthermore, the PFCs exhibit a high CO 2 volumetric adsorption capacity of 97 cm 3 cm −3 at 298 K and 1 bar, benefiting the practical application deployed with an integrated adsorption column. The diffusion kinetics can be further tuned when altering the bulk phase into nanocoating, which would inspire their application in different scenarios.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
DOI
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Kaifang Wang,Danlin Chen,Jiali Tang,Zihao Hong,Zhongtai Zhu,Ziyi Yuan,Zhihong Lin,Yuqi Liu,Raphael Semiat,Xuezhong He
Membrane gas separation technologies have emerged as highly prospective avenues for the selective separation of CO 2 . In this research, a novel array of mixed-matrix membranes (MMMs) was engineered, integrating two-dimensional nanosheets of MXene, specifically Ti 3 C 2 T x , into polymers of intrinsic microporosity (PIMs) to selectively separate CO 2 from N 2 . The inclusion of Ti 3 C 2 T x nanosheets, rich in polar functional groups, significantly increases the affinity between CO 2 molecules and the fabricated MMMs. Additionally, the precise modulation of the molecular diffusion channels for CO 2 and N 2 is achievable due to the interlayer spacing between MXene layers (∼0.35 nm) within the PIM-1 matrix. This innovation is predicated on the synergistic effect of solution-diffusion and molecular sieving mechanisms that underpin the gas separation process, leading to a marked improvement in both selectivity for CO 2 over N 2 and the permeability of CO 2 . Among the series, the MMMs with a 0.5 wt% MXene display exceptional separation efficiency, achieving a CO 2 permeability of 12475.3 barrer and a CO 2 /N 2 selectivity of 32.7. Notably, all the PIM-1/MXene membranes prepared with different compositions in this study exceed the Robeson upper bound defined in 2019, indicating their substantial promise for CO 2 separation and capture in industrial applications.
研究领域:
材料科学
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环境工程
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
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2021
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IF 9.229
Changyang Liu,Shuting Li,Jianquan Gao,Liuzhen Bian,Yunting Hou,Lijun Wang,Jun Peng,Jinxiao Bao,Xiwen Song,Shengli An
The development of cathode materials with high catalytic activity and low cost is a challenge for CO2 electrolysis based on solid oxide electrolysis cells. Herein, we report a low-cost and highly active metallic Fe nanoparticle-decorated Ruddlesden-Popper (La, Sr)FeO4+δ cathode catalyst (Fe-RPLSF), which shows a high oxygen vacancy concentration and robust CO2 reduction rate. At 850 °C, the current density of the electrolysis cell with the Fe-RPLSF cathode reaches −1920 mA cm–2 at a voltage of 1.5 V, and the Faraday efficiency is as high as 100%. The polarization resistance at low frequency (0.1–10 Hz), which is the rate-limit step for CO2 electrolysis, significantly decreases with the exsolved Fe nanoparticles because of improved CO2 dissociative adsorption. Moreover, our electrolysis cell demonstrates acceptable short-term stability for direct CO2 electrolysis.
研究领域:
材料科学
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能源化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL
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2021
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IF 6.609
Hao Shen,Zihao Yang,Xiaochen Li,Ying Peng,Meiqin Lin,Juan Zhang,Zhaoxia Dong
Hydraulic fracturing and CO 2 flooding are extensively used in low-permeability reservoirs to enhance oil recovery (EOR). However, due to the serious heterogeneity of the formation, CO 2 is prone to break through the oil-bearing zone prematurely, which leads to the decrease of the swept volume. Conventional blocking agents have some defects such as difficult injection, poor stability and weak sealing strength. Therefore, it is critical to developing a new type of channeling blocking agent for low-permeability fractured reservoirs. In this study, ten kinds of chemicals with tertiary amino groups are filtered for the most effective CO 2 -responsive agent, which turns out to be N, N-Dimethyl erucamide tertiary amine (DMETA). Subsequently, rheological properties, response performance, and microstructure of the optimum agent are researched systematically through rheological experiments, CO 2 -response processes and Cryo-TEM. The results show that the viscosity of the DMETA solution can increase to nearly 605,700 mPa·s by self-assembly into wormlike micelles (WLMs). And it can be reversibly circulated between low viscosity and high viscosity by alternately introducing and removing CO 2 , which endows it with the ability to healing its viscoelasticity under an environment full of CO 2 . A new method based on optical microrheology is proposed to study the viscoelastic properties of WLMs under no external force. The experiments prove that the network structure is not stable after formation, but remains in a continuous process of separation and reconstruction as “a living polymer.” Furthermore, the plugging performance and EOR capacity are evaluated using fractured tight cores. The experiments demonstrate that the optimum agent can effectively restrain gas channeling and enhance recovery factor by 21.7%. We expect our work can provide insights for the synthesis of CO 2 -responsive WLMs and guidance for retarding gas channeling during CO 2 flooding in low permeability reservoirs.
研究领域:
石油工程
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化学工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
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2023
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IF 8.4
Xuejian Liu,Yan Li,Guang-Jin Chen,Dao-Yi Chen,Bo Sun,Zhenyuan Yin
CO2 capture and sequestration are broadly recognized as the most effective technology for reducing CO2 emissions and mitigating global climate change. In this regard, hydrate-based CO2 sequestration (HBCS) has been proposed as an effective method for long-term safe and stable CO2 sequestration. It is a promising technology for reducing the concentration of CO2 in the atmosphere and achieving carbon neutrality. However, one major challenge related to HBCS technology is the lack of understanding of how to improve the formation kinetics of CO2 hydrate effectively. Herein, in this study, we identified the synergistic promotion effect on CO2 hydrate formation when a low-dose thermodynamic promoter (tetrahydrofuran, THF) is coupled with an environment-friendly kinetic promoter (l-methionine, l-Met). Based on the kinetic experiments and the morphological observation, 0.6 mol % THF coupled with 0.1 wt %l-Met yields the optimal CO2 gas uptake. In situ Raman spectra reveal the mechanism of the observed two-step growth behavior at the molecular level, where low-dose THF promotes the initial CO2-THF sII hydrate nucleation and growth in the solution and l-Met promotes the subsequent CO2 sI hydrate growth along the surface of the reactor. Our study unveils the underlying synergistic mechanism when thermodynamic and kinetic promoters are coupled for CO2 hydrate formation. The results provide guidance for the identification and use of novel bio-friendly thermodynamic and kinetic promoters and are beneficial to a series of sustainable hydrate-based technologies when fast CO2 formation is required.
研究领域:
化学工程
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环境科学
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材料科学
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可持续能源
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2019
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IF 3.372
Zihan Qu,Hong Wu,Yue Zhou,Leixin Yang,Xingyu Wu,Yingzhen Wu,Yanxiong Ren,Ning Zhang,Yutao Liu,Zhongyi Jiang
Membranes with fast CO 2 transport pathways have attracted intense attention due to their outstanding CO 2 permeability, showing potential for industrial application. Regulating the spatial distribution of CO 2 -philic groups in polymer-based membranes is expected to be a promising strategy to achieve the fast CO 2 transport pathways. In membrane matrix, the interconnected network of concentrated domains of CO 2 facilitated transport groups provides membranes with specific CO 2 transport pathways and finally leads to their high separation performance. In this study, a novel kind of polyelectrolyte membrane, quaternary ammonium polysulfone with interconnected ionic clusters, is prepared to enhance the CO 2 permeability. The hydrophilic quaternary ammonium groups tend to aggregate spontaneously to create ionic clusters. Furthermore, under humidified conditions, these ionic clusters are connected by water to form an ionic cluster network in the membrane matrix. The ionic cluster network plays the crucial role in accelerating the selective transport for CO 2 molecules over CH 4 by the reversible interaction between CO 2 and ion pairs. By tuning the quaternization degree of polysulfone, a series of polyelectrolyte membranes with different size of ionic clusters were developed. Membranes with hydrated ionic clusters (5–9 nm) show dramatic enhancement in CO 2 separation performance, especially in CO 2 permeability. The as-prepared quaternary ammonium polysulfone membrane with 8.98 nm ionic clusters exhibited the high CO 2 permeability of 1109.44 Barrer and a high CO 2 /CH 4 selectivity of 29.70, which exceeds 2008 Robeson upper bound limit. The optimized separation performance of QA-PSf membranes is attractive for potential application such as CO 2 capture from flue gas and natural gas.
研究领域:
材料科学
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化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
CRYSTENGCOMM
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2025
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IF 2.6
Bolin Ma,Guanghui Chen,Lingling Zhou,Chengyang Ni,Xinyu Sun,Lei Zhang,Xinguo Xi,Lanqin Tang,Yong Zhou
The development of highly efficient photocatalysts for CO2 reduction remains a critical challenge in achieving sustainable energy conversion. In this study, we report the synthesis of a UiO66-NH2@In2O3, integrating UiO66-NH2 metal organic frameworks (MOFs) with indium oxide (In2O3) nanoparticles, forming a robust heterostructure. Characterization results demonstrated that calcination at 250 °C for 4 hours yielded a heterostructure with indium uniformly incorporated, as confirmed by XRD, SEM, TEM and ICP-OES analyses. XPS studies revealed significant electronic interactions between UiO66-NH2 and In2O3, including shifts in binding energies of indium and zirconium, indicative of chemical bonding. This heterostructure facilitated enhanced charge separation and transfer, as evidenced by photocurrent measurements, leading to superior photocatalytic CO2 reduction performance. Under light irradiation, UiO66-NH2@In2O3 achieved a CO production rate of 83.68 μmol g−1 during the first hour and a cumulative yield of 485.08 μmol g−1 after 7 hours, significantly outperforming pristine UiO66-NH2 and In2O3. The superior activity is attributed to the large surface area of UiO66-NH2, facilitating CO2 adsorption, and the heterojunction formation with In2O3, enhancing charge carrier dynamics. These findings highlight the synergistic effects of UiO66-NH2 and In2O3, providing insights into the design of advanced photocatalysts for environmental and energy applications.
研究领域:
材料科学
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环境科学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
AICHE JOURNAL
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2018
·Vol. 64
·期 11
·3988-4001
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IF 3.326
Xiaowen Zhang,Jieling Hong,Helei Liu,Xiao Luo,Wilfred Olson,Paitoon Tontiwachwuthikul,Zhiwu Liang
In this work, the composite catalysts, SO 4 2 /ZrO 2 /γ-Al 2 O 3 (SZA), with different ZrO 2 and γ-Al 2 O 3 mass ratios were prepared and used for the first time for the carbon dioxide (CO 2 )-loaded monoethanolamine (MEA) solvent regeneration process to reduce the heat duty. The regeneration characteristics with five catalysts (three SZA catalysts and two parent catalysts) of a 5 M MEA solution with an initial CO 2 loading of 0.5 mol CO 2 /mol amine at 98°C were investigated in terms of CO 2 desorption performance and compared with those of a blank test. All the catalysts were characterized using X-ray diffraction, Fourier transform infrared spectroscopy, N 2 adsorption–desorption experiment, ammonia temperature programmed desorption, and pyridine-adsorption infrared spectroscopy. The results indicate that the SZA catalysts exhibited superior catalytic activity to the parent catalysts. A possible catalytic mechanism for the CO 2 desorption process over SZA catalyst was proposed. The results reveal that SZA1/1, which possesses the highest joint value of Brφnsted acid sites (BASs) and mesopore surface area (MSA), presented the highest catalytic performance, decreasing the heat duty by 36.9% as compared to the catalyst-free run. The SZA1/1 catalyst shows the best catalytic performance as compared with the reported catalyst for this purpose. Moreover, the SZA catalyst has advantages of low cost, good cyclic stability, easy regeneration and has no effect on the CO 2 absorption performance of MEA. © 2018 American Institute of Chemical Engineers AIChE J , 64: 3988–4001, 2018
研究领域:
化学工程
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催化材料
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环境科学
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
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2017
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IF 3.387
Leiqing Hu,Jun Cheng,Yannan Li,Jianzhong Liu,Li Zhang,Junhu Zhou,Kefa Cen
Mixed matrix membranes with ionic liquids and molecular sieve particles had high CO 2 permeabilities, but CO 2 separation from small gas molecules such as H 2 was dissatisfied because of bad interfacial interaction between ionic liquid and molecular sieve particles. To solve that, amine groups were introduced to modify surface of molecular sieve particles before loading with ionic liquid. SAPO 34 was adopted as the original filler, and four mixed matrix membranes with different fillers were prepared on the outer surface of ceramic hollow fibers. Both surface voids and hard agglomerations disappeared, and the surface became smooth after SAPO 34 was modified by amine groups and ionic liquid [P 66614 ][2-Op]. Mixed matrix membranes with composites of amine-modified SAPO 34 and ionic liquid exhibited excellent CO 2 permeability (408.9 Barrers) and CO 2 /H 2 selectivity (22.1).
研究领域:
材料科学
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环境工程
✓ 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）