APPLIED SURFACE SCIENCE
·
2017
·
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).
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
·
IF 9
Chengzhong Xiong,Runzhang Tao,Jian Lu,Shilong Li,Dong Zou,Yuqing Sun,Wenheng Jing
Efficient recovery of Li + from lithium-ion batteries (LiBs), which also include Co 2+ , Ni 2+ , or Mn 2+ in the cathode material, remains a formidable challenge because the sizes and physicochemical properties of these ions. Composite lamellar membranes are emerging as highly ion-selective nanochannels with controllable interlayers. Herein, Li + /Co 2+ was precisely separated through two-dimensional MXene/δ-MnO 2 composite nanochannels under an electric field. The nanochannels were constructed on tubular ceramic membranes via hydroxyl crosslinking. The membrane layer spacing can be extended to 5.7 Å by electrostatic repulsion between MXene and δ-MnO 2 nanosheets, which is suitable for Li + /Co 2+ separation. Under an electric field of 2 mA cm −2 , Li + /Co 2+ was nearly completely separated, with a high Li + flux of 0.0094 mol m -2 h −1 , and the energy consumption was ∼0.315 kW h (mol Li + ) -1 . Similarly, near-complete separation of Li + /Ni 2+ and Li + /Mn 2+ can be achieved at a current density of 2 mA cm −2 . The transport of Li + in solution was accelerated under a positive electric field and by partial dehydration in the nanopores. Meanwhile, the zeta potential was distinctly more negative in the composite membranes than in individual MXene or δ-MnO 2 . Consequently, Co 2+ was rapidly adsorbed on the negatively charged membrane surface through electrostatic interactions and complexation, forming a positively charged Co 2+ layer that electrostatically repelled further Co 2+ adsorption, ultimately achieving near-complete separation of Co 2+ . Owing to their stable and robust structure, the MXene/δ-MnO 2 membranes maintained high separation efficiency in acidic solutions containing Li + and Co 2+ and remained stable over eight cycles (up to 14 h) of ion separation under an electric field. This approach can potentially realize 2D membrane composites for efficient ion separation in practical applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Yan-Mei Zhang,Wen-Wen Xie,Xiao-Xue Hu,Xin-Ru Chen,Heng Mao,Li-Hao Xu,Xin-Yu Shi,Tao Wang,Ying-Nan Feng,Zhi-Ping Zhao
Bioethanol has garnered widespread attention as a potential substitute for traditional fossil fuels. Focusing on the treatment of bioethanol fermentation exhaust is crucial for optimizing bioethanol recovery and achieving carbon dioxide (CO 2 ) purification. This study successfully achieved the large-scale synthesis of zeolitic imidazolate framework-8 (LSZIF-8), which was then incorporated into polydimethylsiloxane (PDMS) to fabricate large-area ZIF-8/PDMS/PVDF mixed matrix membranes (MMMs) for bioethanol recovery from fermentation exhaust via vapor permeation (VP) processes. The ZIF-8/PDMS/PVDF MMMs exhibited a 1.5-time increase in ethanol permeability and selectivity improved by 1.7 times compared to the PDMS/PVDF membrane. The mass transport behavior of ethanol and CO 2 molecules within the membrane, as well as examining the interactions between different components was systematically explored. It delves into the disparities in separation performance between PDMS/PVDF membrane and ZIF-8/PDMS/PVDF MMMs with nitrogen (N 2 ), water vapor as the third component. Notably, high-quality LSZIF-8 crystals serves as a crucial source of raw materials for the continuous preparation of high-performance MMMs, addressing the limitation of traditional nanoparticle fillers in terms of scalability for production. This study paving new avenues for purifying fermentation exhaust and recovering bioethanol, while simultaneously present significant potential for industrial applications.
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CHEMICAL ENGINEERING JOURNAL
·
2024
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IF 13.3
Ming-Long Wang,Yi-Fei Sun,Hong-Nan Chen,Jin-Rong Zhong,Liang-Liang Ren,Ming Wang,Dan Rao,Yong-Quan Liu,Yi-Bo Hao,Bei Liu,Chang-Yu Sun,Guang-Jin Chen
Hydrate-based CO 2 storage is a highly promising technology for long-term stable CO 2 storage in sediments. However, the unclear displacement and hydration mechanisms, along with the low conversion rate of CO 2 hydrates, have hindered the field application. Here, we report a method of the injection of CO 2 /water emulsion to replace liquid CO 2 to regulate the ratio of CO 2 to water in the sediment pores and to enhance their contact ability, which can significantly improve the CO 2 hydrate conversion rate. Compared to liquid CO 2 injection, emulsion injection can flow through more sediment pores with an increase in displacement efficiency by 45 %-62 %, which leaves a CO 2 -to-water ratio within the pores that is more suitable for hydrate formation, ultimately tripling the hydrate conversion rate. We have outlined the hydrate growth mechanisms for both injection forms, where the micron-sized CO 2 droplets within the emulsion can greatly reduce the barrier effect of hydrate film. Under the combined influences, the CO 2 storage density in hydrates up to 91.2 kg/m 3 for CO 2 /water emulsion injection is 47.8 % higher than that of 61.7 kg/m 3 for liquid CO 2 injection. Our work provides a new approach to high conversion CO 2 hydrate sequestration in submarine sediments.
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ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Yan Wang,Wanxiang Zhang,Shuhang Ren,Yucui Hou,Weize Wu
Due to low cost and high efficiency, amino-based functionalized deep eutectic solvents (DESs) have been widely investigated in CO2 capture. The amino group reacted with CO2 in a quantized ratio of 2:1 to form a carbamate and quaternary ammonium cation, which not only limited the absorption capacity of the amino group but also led to a dramatic increase in viscosity. In this work, we proposed a new strategy to improve the absorption capacity of amino-based functionalized DESs and inhibit viscosity increase by changing the proton transfer site from –NH2 to –N═ to prevent the formation of –NH–COO– and –NH3+ using aromatic amines and ethylene glycol (EG). EG exhibited significant activation effect on 4-aminopyridine (AP). The absorption capacity of AP was enhanced from 0.10 mol of CO2/mol of DES to 0.60 mol of CO2/mol of DES at 303.15 K and 101.3 kPa after forming DES with EG. In addition, the saturated DES could be rapidly regenerated within 20 min at 353.15 K, and the absorption performance was maintained after six cycles. Results of proton nuclear magnetic resonance and carbon nuclear magnetic resonance spectra revealed the formation of carbamate and the protonation of pyridine nitrogen. The new reaction path effectively reduced the increase in viscosity. The viscosity of AP/EG (1:3) DES increased slightly from 29.17 to 68.40 mPa·s after absorption.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-8
·
IF 15.7
Zhang Zhewei,Yao Jun,Shen Chenyang,Li Fengfeng,Deng Changshun,Zhao Taotao,Guo Xuefeng,Zhu Yan,Guo Xiangke,Xue Nianhua,Peng Luming,Ding Weiping
In typical heterogeneous catalytic reactions, catalysts, whether fixed or flowing, maintained their bulk and surface structures as stable as possible. We report here dynamic activation catalysts having continuously generate highly active sites in working, which enables a usually low active Cu/Al 2 O 3 catalyst for CO 2 hydrogenation, showing extraordinary catalytic performances. Using reaction streams in unusually high linear speed to blow and carry the Cu/Al 2 O 3 particulates to collide cyclically with a rigid target, the CO 2 conversion rate is more than three times enhanced at methanol selectivity promoted to 95% from less than 40% and the methanol space-time-yield is six times increased. By experimental and theoretical investigation, the dynamic activation of Cu/Al 2 O 3 is defined as a discrete condensed state with a distorted and elongated lattice, reduced coordination, and abnormal catalytic properties. We envision that continuous research on the dynamical activation catalysts will advance novel methods for promoting catalytic performance and discovering new catalytic reactions.
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ENERGY
·
2020
·
IF 6.082
Hongwei Li,Zhigang Tang,Zhimin He,Xia Gui,Longpeng Cui,Xian-zhong Mao
In order to show the structure-activity relationship for CO 2 absorbent, and identify or screen novel and efficient physical solvents of CO 2 , the constant-volume method, the Peng-Robinson equation of state , and a molecular simulation were used to investigate the impacts of type of functional groups, carbon chain length and number of functional groups for nine physical solvents. The three methods produced highly consistent results. Comparison of the CO 2 solubility in solvents with the same carbon numbers but different functional groups suggested that the ester group could promote CO 2 absorption. Investigation of the CO 2 solubility in solvents with one ester group but different carbon chain lengths revealed that longer carbon chains could enhance CO 2 absorption. Analyses of the CO 2 solubility of solvents with one and two ester groups demonstrated that more ester groups could further increase the CO 2 absorption. Therefore, the presence and number of ester groups and increased carbon chain length could promote CO 2 absorption. It provides direction and method for screening of highly efficient CO 2 absorbents and for the design and synthesis of new solvents.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-13
·
IF 14.7
Liu Tao,Wang Yunpeng,Wu Yifan,Jiang Wenchuan,Deng Yuchao,Li Qing,Lan Cheng,Zhao Zhiyu,Zhu Liangyu,Yang Dongsheng,Noël Timothy,Xie Heping
Electrochemical CO 2 capture driven by renewable electricity holds significant potential for efficient decarbonization. However, the widespread adoption of this approach is currently limited by issues such as instability, discontinuity, high energy demand, and challenges in scaling up. In this study, we propose a scalable strategy that addresses these limitations by transforming the conventional single-step electrochemical redox reaction into a stepwise electrochemical-chemical redox process. Specifically, the hydrogen evolution reaction (HER) at the cathode and the oxidation of a redox carrier at the anode are employed to modulate the pH of the electrolyte, thereby facilitating effective CO 2 capture. By decoupling the electrochemical swing for CO 2 capture from redox carrier regeneration in both temporal and spatial domains, this approach mitigates unwanted side reactions and enhances system stability. Our results demonstrate a stable CO 2 capture process sustained for over 200 h, with a electrical work of 49.16 kJ e mol -1 CO 2 at a current density of 10 mA cm -2 . Furthermore, a scaled-up system capable of producing approximately 0.4 kg of pure CO 2 per day maintained stable operation for 72 h, highlighting the potential feasibility of this method for large-scale decarbonization applications.
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ADVANCED MATERIALS
·
2020
·Vol. 32
·期 22
·1907701
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IF 27.398
Bo Wang,Zhihua Qiao,Jiayou Xu,Jixiao Wang,Xinlei Liu,Song Zhao,Zhi Wang,Michael D. Guiver
Ultrathin unobstructed gas transport channels through the membrane selective layer are constructed in mixed matrix membranes (MMMs) by using gravity-induced interface self-assembly of poly(vinylamine) and polymer-modified MIL-101(Cr). For CO 2 /N 2 (15/85 by volume) mixed gas, the MMMs achieve a high CO 2 permeance of 823 gas permeation units and CO 2 /N 2 selectivity of 242 at 0.5 MPa. Based on economic analyses, a two-stage membrane process can achieve gas separation and economic targets.
研究领域:
材料科学
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化学工程
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JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Xi Chen,Nana Wang,Guining Chen,Zhenggang Wang,Gongping Liu,Rongfei Zhou,Wanqin Jin
Mixed-matrix formulation is a promising method to overcome permeability-selectivity trade-off of polymers with incorporation of fillers with well-defined nanopores . The filler properties play a key role in determining the performance of mixed-matrix membrane (MMM). In this work, for the first time, we explored the critical effect of filler structural integrity on separation performance of MMM. Typically, micron as-synthesized, submicron as-synthesized and submicron ground SAPO-34 zeolites were incorporated into 6FDA-DAM polyimide , respectively. The interface compatibility between two phases was ensured by (3-aminopropyl) trimethoxysilane (APTMS) modification on SAPO-34 fillers. It was found that the directly synthesized micron and submicron fillers contributed to enhance the CO 2 /CH 4 separation performance whereas the submicron ground filler lowered the CO 2 permeability. Notably, incorporating 30 wt% micron as-synthesized SAPO-34 into 6FDA-DAM enhanced the CO 2 permeability by 68% and CO 2 /CH 4 by 37%, surpassing the performance upper-bound. Moreover, the hydrogen bonding between the filler and polymer matrix endowed the membrane with outstanding plasticization resistance with CO 2 partial pressure up to 20 bar. Adsorption isotherms and Maxwell model prediction revealed that the filler transport properties could be significantly affected by commonly-used methods of reducing the filler size. A decreased structural integrity was identified in the sequence of micron as-synthesized, submicron as-synthesized and submicron ground fillers. This work highlights the importance of a careful balance between structural integrity and crystal size of filler, and reliable routes to obtain nanofillers with desirable structural integrity as pursuing high-performing MMM toward practical application.
研究领域:
材料科学
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化学工程
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RSC Advances
·
2023
·Vol. 13
·期 20
·13902-13910
·
IF 3.9
Jing Tian,Weixin Qian,Haitao Zhang,Hongfang Ma,Weiyong Ying
In this paper, catalysts with different aluminum contents were prepared by a co-precipitation method using LDHs (layered double hydroxides) as the precursors through the adjustment of Cu2+ : Fe2+, and the catalysts were named LDO catalysts. The effect of aluminum on CO2 hydrogenation to methanol was investigated by evaluating the characterization. With the addition of Al, Ar physisorption results showed an increase in BET-specific surface area, TEM demonstrated a decrease in catalyst particle diameter, XRD showed that Cu and Fe existed in the catalyst mainly in the form of CuFe2O4 and CuO, XPS demonstrated a decrease in electron cloud density and an increase in base sites and oxygen vacancies, and CO2-TPD and H2-TPD results indicated that Al promoted the dissociation and adsorption of CO2 and H2. When the reaction temperature was 230 °C, the pressure was 4 MPa, H2/CO2 = 2.5 and the space velocity was 2000 ml (h gcat)−1, the best conversion (14.87%) and the highest methanol selectivity (39.53%) of the catalyst were obtained at 30% aluminum content.
研究领域:
催化
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化学工程
·
材料科学
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FUEL
·
2025
·
IF 7.5
Liangliang Ren,Lixia Zhang,Tie Geng,Xuejian Liu,Jiayu Sun,Dnyaneshwar R. Bhawangirkar,Botao Xu,Huaike Li,Lei Guo,Zhenyuan Yin
Hydrate-based CO 2 storage (HBCS) in subsea sediments has emerged as a promising climate mitigation method due to its high CO 2 storage capacity and long-term stability. However, practical application encounters significant challenges due to sluggish CO 2 hydrate formation kinetics, primarily resulting from limited liquid CO 2 -water interfacial contact after CO 2 hydrate film formation and blockage. Generating CO 2 microdroplets in continuous aqueous phase forms CO 2 (L) in H 2 O (C/W) emulsion, which enhances CO 2 dispersion and expands the liquid–liquid interfacial area. However, effective methods to synthesize stable C/W emulsion under high pressures and their role in enhancing CO 2 hydrate formation kinetics is less understood and warrant systematic investigation. In this study, we formulate C/W emulsion using an environmentally benign non-ionic surfactant alkyl polyglucoside (APG), and systematically examine the effects of APG concentrations and stirring rates on C/W emulsion stability in a fully-visual reactor. Under optimal 3.0 wt% APG, C/W emulsion forms under 1800 rpm in 13 s and maintains stability for ∼ 7 hrs with average CO 2 micro-droplet size of ∼ 14 μm. The dispersion of liquid CO 2 microdroplets promotes ultra-rapid CO 2 hydrate formation, achieving a CO 2 uptake of 187.8 v CO2 / v H2O (water conversion of 94.8%) with t 90 of 40 min, representing a ten-fold increase compared to the conventional CO 2 (L)–H 2 O mixing system by stirring. Findings of this study will guide effective methods for synthesizing and improving the stability of C/W emulsion under high pressure. Moreover, enhanced CO 2 hydrate formation kinetics enabled by emulsion-based method can be applied in a series of CO 2 hydrate-based applications. The study offers both mechanistic insights and practical guidance for future field-scale HBCS deployment.
研究领域:
环境科学
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化学工程
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物理化学
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能源存储
·
气候缓解技术
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危险品化学品经营许可证（带存储）