JOURNAL OF POLYMER RESEARCH
·
2021
·Vol. 28
·期 7
·1-10
·
IF 3.097
Xian Wenqi,Yuan Jie,Xie Zhengbin,Ou Wei,Liu Xiaoxuan,Liu Baohua
A series of CO 2 copolymer-based waterborne polyurethanes with high solid content were successfully prepared by using CO 2 copolymer diol, isophorone diisocyanate, and dimethylol propionic acid as the donors of hydrophilic groups. In order to obtain of the emulsion with high solid content and good physical property, the synthesis conditions of CO 2 copolymer-based waterborne polyurethane were studied. The influence of dimethylol propionic acid content and synthesis process on the physical property of the emulsion was also investigated. Results show that CO 2 copolymer-based waterborne polyurethane with high solid content can be synthesized by chain expansion at relatively low temperature. The waterborne polyurethane emulsion particle size distribution was wide. As the content of hydrophilic groups in prepolymer increased, the viscosity and water absorption increased obviously, this is difficult to synthesize waterborne polyurethane with high solid content and low water absorption. Thermal gravimetric analysis shows that the higher the chain extending temperature of CO 2 copolymer-based waterborne polyurethane, the higher the thermal decomposition temperature. When the CO 2 molar content of CO 2 copolymer diol is about 30%, the CO 2 copolymer-based waterborne polyurethane has high strength and better water resistance.
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Chemical Science
·
2018
·Vol. 9
·期 14
·3426-3437
·
IF 9.063
Xinyu Li,Zhi-Jian Zhao,Liang Zeng,Jiubing Zhao,Hao Tian,Sai Chen,Kang Li,Sier Sang,Jinlong Gong
La2O3 exhibits good performance for various catalytic applications, such as oxidative coupling of methane (OCM) and dry reforming of methane (DRM), during which coke formation may lead to the deactivation of catalysts. Typically, the reaction between CO2 adsorbed on La2O3 and coke is the rate-determining step of the coke elimination process. This paper describes the influence of Ce addition on the CO2 adsorption and activation over La2O3. Combined with in situ and ex situ characterization and density functional theory (DFT) calculation, we show that Ce addition promotes the formation of bidentate carbonate on La2O3via tuning CO2 adsorption energy. In addition, Ce addition adjusts the ratio of bidentate/monodentate carbonate, and affects the ratio of hexagonal/monoclinic La2O2CO3 on the binary oxides. DRM is used as a probe reaction to examine the coke elimination performance of Ce–La binary oxide. It is found that when the Ce/La ratio reaches the optimal value (0.15), Ce–La binary oxide has the highest CO2 adsorption energy and predominantly promotes the formation of bidentate carbonate, and hence possesses the highest basicity above 700 °C and finally exhibits the best coke elimination performance.
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Journal of Environmental Chemical Engineering
·
2025
·Vol. 14
·期 1
·120640
·
IF 7.2
Yifan Wang,Zeliang Xiong,Shilin Xu,Yuan Gao,Haoli Zhou,Wanqin Jin
Polyimides with intrinsic microporosity are promising materials for gas separation, but their industrial application is hindered by poor long-term stability. This study proposes diamine modification of a polyimide membrane with diamines, such as p-phenylenediamine (p-PD), to enhance both membrane stability and selectivity for separating gas pairs such as CO 2 /CH 4 . Various characterization techniques confirmed the crosslinking reaction between the diamine and imide groups, which restricted the movement or rearrangement of polymer chains, resulting in improved membrane anti-plasticization performance and stability. Meanwhile, CO 2 -philic emeraldine base and quinone structures were formed due to the in-situ oxidation of p-PD during the crosslinking process, which significantly boosted CO 2 /CH 4 selectivity. The maximum selectivity (44.5), which is 66.0 % higher than that of the pristine membrane, was achieved using a p-PD-modified polyimide membrane for the separation of pure single CO 2 /CH 4 . Additionally, the separation of other gas pairs (such as CO 2 /N 2 ) and the effect of pressure on the separation of a CO 2 /CH 4 mixture were investigated using the p-PD-modified polyimide membrane, which demonstrated improved performance. Thus, this study provides a reference for enhancing the selectivity and stability of polyimide membranes through diamine modification using p-PD and its analogues.
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Nature Communications
·
2025
·
IF 15.7
Qian Zhengyi,Han Guokang,Tan Yingjun,Ye Na,Wang Shuguang,Lin Zheng,Huang Qizheng,Gu Yu,Guo Hongyu,Liu Fei,Wang Kai,Li Lu,Shang Changshuai,Luo Mingchuan,Guo Shaojun
Copper-based catalysts are the premier choice for electrochemical reduction of CO 2 (CO 2 RR) into hydrocarbons or oxygenates. However, the facilely structural reconstruction of copper sites during electrolysis poses significant challenges to the long-life electrolytic efficiency. Herein, we leverage the strong σ-π dative bonding between Cu δ+ and alkyne-based ligands to stabilize copper sites for the prolonged CO 2 RR. We demonstrate the feasibility of taming the electronic structures of copper sites through the tug of war between σ and π backbonding interactions. The optimal copper organic polymer with methoxy group functionalization (OMe-PhCu) exhibits a moderate charge density of copper sites and an intensified local asymmetric charge distribution of coordinative carbon, enhancing the selectivity of methane with a Faradaic efficiency of 68.8% and a partial current density of 324.5 mA cm −2 in acidic electrolyte. In situ spectra and density functional theory calculations reveal enhanced *CO adsorption and lowered energy barrier for CO 2 RR into methane over OMe-PhCu. Building upon such stable Cu δ+ sites, we further construct Cu δ+ /Cu 0 catalytic interfaces for the generally enhanced electrosynthesis of multi-carbons and ammonias. This synthetic chemistry paves the pathway for the design of stable catalytic active sites for renewable conversions.
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CHEMICAL ENGINEERING RESEARCH & DESIGN
·
2025
·
IF 3.9
Pengchao Zang,Daokuan Liang,Jiyun Tang,Xiaozhe Wang,Lin Cui,Pei Zhao,Ning Qin,Zeyad Ammar Almutairi,Yong Dong
Adsorbents prepared by impregnating tetraethylenepentamine (TEPA) into porous materials represent promising candidates for CO 2 capture from coal-fired flue gas. This study impregnated TEPA into four types of resins to investigate the influence of different resins on the CO 2 adsorption performance of TEPA-resin adsorbents. Experimental data indicate that the CO 2 adsorption performance of TEPA-resin composites follows the order: DA201D > XAD-2 > ADS-17 > AB-8, where TEPA@DA201D exhibited the highest adsorption capacity of 3.46 mmol/g under 35℃ and 15 vol% CO 2 conditions. TEPA@DA201D possesses a hierarchical mesoporous structure with a high pore volume (1.084 cm 3 /g) and large average pore diameter (20.0 nm), which synergistically enhances CO 2 adsorption by promoting CO 2 diffusion and improving the dispersion of active sites. Simultaneously, SEM images reveal that DA201D exhibits the least aggregation of surface amine groups compared to other adsorbents. Different adsorption kinetic models reveal that its adsorption behavior conforms to the Avrami model, primarily governed by the synergistic effects of physical and chemical adsorption. The rate-limiting steps for CO 2 adsorption by the TEPA@DA201D adsorbent are mainly membrane diffusion and intra-particle diffusion at different temperatures. Furthermore, multifactorial interaction analysis indicates that adsorption temperature, gas flow rate, and CO 2 concentration independently regulate the adsorption capacity of TEPA@DA201D. This work provides theoretical guidance and design strategies for improving the design and performance of organic amine-modified resin-based adsorbents.
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Nature Communications
·
2025
·Vol. 16
·期 1
·10389
·
IF 15.7
Zhai Yanjie,Gong Shanhe,Li Weisong,Xia Qing,Li Tingting,Guan Jianyu,Leu Shao-Yuan,Wu Zhen-Yu,Lau Shu Ping,Zhang Xiao
Electrochemical carbon capture offers a sustainable pathway for carbon management, yet current systems are hindered by low concentration of atmospheric carbon dioxide (CO 2 ), resulting in inefficiencies and limited stability. Here, we develop an electrochemical system employing a modular porous solid electrolyte (PSE) reactor for continuous, scalable carbon capture from diverse sources, including ambient air and flue gas, while regenerating high-purity CO 2 ( >99%) without additional chemical input through a recirculation mode. By leveraging oxygen evolution and reduction reactions (OER/ORR) and employing sodium (bi)carbonate as a reversible cyclic mediator, the system achieves continuous CO 2 capture from flue gas, delivering high Faradaic efficiencies for Na⁺ transport (~85%), and high carbon capture rates (3060 ml h − 1 at 10 A, 100 cm 2 ). Notably, direct air capture is demonstrated using ambient air, showing a long-term stability of over 2000 hours while maintaining high carbon removal efficiency (>93%) at 30 mA cm -2 and a large air treatment capacity (approximately 8820 kg air day -1 m -2 ), thus contributing to the goal of achieving net-zero emissions.
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Science Advances
·
2025
·Vol. 11
·期 48
·
IF 12.5
Kaifang Wang,Zhongtai Zhu,Yuqi Liu,Weiran Zheng,Ziyi Yuan,Zhihong Lin,Raphael Semiat,Lu Shao,Xuezhong He
Carbon membranes are emerging as a versatile platform for the selective separation of gas mixtures with similar molecular sizes. Here, a high-performance carbon membrane is developed from an asymmetric, rigid copolyimide precursor via a precisely controlled carbonization process. Membranes carbonized at 800°C exhibit exceptional CO 2 separation performance, with CO 2 permeabilities up to 15,700 barrer and CO 2 /N 2 and CO 2 /CH 4 selectivities of 63 and 52, respectively—surpassing the 2019 upper bounds. Molecular dynamic simulations, in conjunction with in situ thermogravimetric analysis-mass spectroscopy and thermogravimetric analysis-Fourier transform infrared spectroscopy, reveal the evolution of a bimodal carbon matrix with micropores (7 to 20 angstroms) and ultramicropores (4 to 7 angstroms). Gas transport is dominated by synergistic adsorption-selective and molecular sieving mechanisms, enabling subangstrom discrimination between CO 2 and larger gases. This work demonstrates a facile, tunable strategy to engineer carbon membranes with outstanding CO 2 separation capabilities, offering previously unexplored opportunities for energy-efficient gas separation processes in industrial applications.
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CATALYSIS COMMUNICATIONS
·
2024
·
IF 3.4
Yan Kong,Long Tian,Guiming Xie,Xiaorui Wang,Yi Man,Zhou-jun Wang
Molybdenum phosphide (MoP) has attracted increasing attention as a novel catalytic material for CO 2 reforming of methane in virtue of superior coke resistance, but its catalytic reactivity is still relatively low. This work for the first time improved the reforming activity of MoP via ZrO 2 modification. The Zr 0.01 MoP catalyst with Zr/Mo molar ratio of 0.01 possessed much higher activity than bare MoP at 800–900 °C. Structural characterizations revealed that the introduction of ZrO 2 would decrease the particle size, modify the electronic structure and change the reducibility property of MoP, which may function together to deliver the higher activity.
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ENERGY & FUELS
·
2021
·
IF 3.605
Shuanshi Fan,Hong Huang,Chi Yu,Yanhong Wang,Xuemei Lang,Shenglong Wang,Gang Li,Wangyang Yu
The product gas of natural gas hydrate production by CO2 replacement is the lean-CH4/CO2 binary gas which contains 85–95% CO2. In this work, the lean-CH4/CO2 (10 mol % CH4/90 mol % CO2) binary mixture was used to simulate the product gas of natural gas hydrate production via CO2 replacement, and a promising and mild (low pressure) hydrate-based gas separation (HBGS) technology was employed. This work innovatively proposes to inject the reaction liquid to maintain the constant pressure of the whole process, which makes hydrates form continuously to increase the gas consumption. First, the hydrate phase equilibrium of 10 mol % CH4/90 mol % CO2 + 5 wt % tetrabutylammonium bromide (TBAB, aq) was measured in the range of 280–287 K and 0.5–4 MPa. After that, hydrate-based mild separation of the lean-CH4/CO2 binary gas was conducted with the help of TBAB at a constant pressure in the range of 1–4 MPa. The results show that after HBGS in addition with 5 wt % TBAB(aq) at 1 MPa and 278 K, the CH4 concentration could be increased from 17.2 to 66.2 mol % under constant pressure operation, while it was just slightly increased to 17.2 mol % under nonconstant pressure operation. HBGS with 5 wt % TBAB under constant pressure had the best separation performance. Subcooling has a greater effect on the separation kinetics. HBGS of 10 mol % CH4/90 mol % CO2 under a constant pressure operation of 2 MPa, subcooling of 6 K, and 5 wt % TBAB has the highest separation factor above 37. It is suggested that hydrate-based lean-CH4/CO2 separation experiments are carried out at a mild pressure with low G/L and, more importantly, in a short time. This work proposed a mild HBGS of lean-CH4/CO2 separation, which could benefit the separation of gas produced by natural gas hydrate replacement exploitation. This work also simultaneously provides insights into other HBGS for other gas mixtures (flue gas, coalbed methane, biogas, and shift gas) to achieve low energy consumption, high gas consumption, and high efficiency.
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Frontiers of Environmental Science & Engineering
·
2013
·Vol. 8
·期 2
·162-168
·
IF 0.886
Xie Jiangkun,Yan Naiqiang,Liu Fei,Qu Zan,Yang Shijian,Liu Ping
Porous ZIF-7 with the sodalite (SOD) cage structure (ZIF, Zeolitic imidazolate framework) were synthesized by the solvothermal method. Synthesized material was characterized by powder X-ray diffraction (PXRD), thermal gravity (TG), scanning electron microscopy (SEM) and N 2 adsorption analysis. ZIF-8 with the SOD structure and a little larger pore window was synthesized in a similar way and was characterized for comparisons. Thermal stability and structural stability of ZIF-7 were tested through PXRD analysis, and the capability of the material for CO 2 capture from simulated flue gas was investigated through physical adsorption method. The results showed that CO 2 adsorption capacity on ZIF-7 was about 48 mL·g −1 while the capacity on ZIF-8 was about 18 mg·g −1 (at 12°C and 0.98 P / P
0 relative pressure). Furthermore, the impact of flue gas components on adsorption capacity of ZIF-7 and the selectivity of CO 2 against N 2 on ZIF-7 was also investigated in this work.
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ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Guanhua Liu,Huaxun Chen,Hao Zhao,Ran Chen,Minghui Yang,Jing Gao,Fengshou Yu,Yanjun Jiang
Enzymatic conversion of CO2 to high value-added chemicals is in line with green chemistry. However, low solubility of CO2 under mild conditions and high cost of cofactor limit the efficiency of CO2 enzymatic conversion. Therefore, we designed a system for enzymatic electrocatalysis of CO2 by the combination of polyethylenimine (PEI)-enhanced enzyme immobilization and CO2 adsorption, and electrocatalytic nicotinamide adenine dinucleotide (NADH) regeneration. Furthermore, the PEI dendritic structure and SiO2 channel skeleton can effectively protect the enzyme structure from external damage. To be specific, PEI was first modified on mesoporous silica SBA-15 by glutaraldehyde, and then the enzyme was immobilized by electrostatic adsorption. The modified amount of PEI, the amount of enzyme for immobilization, and the amount of immobilized enzyme were optimized. The initial reaction rate increased from 1.3 to 1.9 times as the amount of PEI modification increased from 10 to 60 wt %. The optimized catalysis system could produce 1.118 mM formate after a 3 h reaction, with a productivity of 5323.8 μmol gcat–1h–1, which was 3.7 times more than that of the free enzyme system. Furthermore, the immobilized enzyme still retained over 80% activity after 12 cycles reuse with improved thermal stability.
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AICHE JOURNAL
·
2025
·
IF 4
Xinrui Liu,De Ao,Mao Ye,Zhi Wang,Zhihua Qiao,Song Zhao
Metal–organic framework (MOF) glass holds great promise for gas separation applications. However, the inherent low porosity of MOF glass poses a considerable challenge in improving membrane permeability. In this work, a self-supporting MOF crystal-glass composite (CGC) membrane was synthesized via an innovative blending and melting approach, in which ZIF-62 powder was converted into an amorphous glassy phase and ZIF-9 powder was partially flux-melted, effectively preventing the reorganization of Zn─N bonds within ZIF-62. Consequently, the composite component structure significantly enhances the porosity and permeability of the MOF glass membrane. Furthermore, the incorporation of cobalt into the membrane matrix has notably enhanced its adsorption affinity for CO 2 , thereby boosting CO 2 /CH 4 selectivity. The resultant a g [(ZIF-9) 0.2 /(ZIF-62) 0.8 ] membrane has demonstrated exceptional CO 2 permeability of 20,324 barrer and superior CO 2 /CH 4 selectivity, both surpassing the 2018 upper bound. Thus, the innovative strategy for the design of MOF CGC membranes offers effective solutions to the challenges inherent in gas separation processes.
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