SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Meigui He,Jiangquan Chen,Xiaodong Zhang,Chang Chen,Mengfan Ren,Jing Zhao,Wanqin Jin
Ultrathin mixed-matrix membranes (MMMs) have emerged as promising candidates for efficient membrane-based carbon capture, owing to the combination of the high performance of mixed-matrix materials, and the low mass-transfer resistance of ultrathin membranes. However, incorporating fillers into ultrathin separation layers remains challenging due to the strict requirements on filler dimension and dispersion. Herein, we report a Pebax-based ultrathin MMM incorporating ZIF-8@COF composite porous nanosheets for efficient CO 2 /N 2 separation. Ultrasmall ZIF-8 nanoparticles (∼4 nm) were grown in situ on COF nanosheets, yielding a composite porous filler (∼11 nm thick) that combines the high aspect ratio of COFs with the superior interfacial compatibility and CO 2 affinity of ZIF-8. The resulting ZIF-8@COF/Pebax membrane exhibits 63% and 41% enhancements in CO 2 permeability and CO 2 /N 2 selectivity, respectively, over the pristine Pebax membrane, which can be attributed to abundant CO 2 adsorption sites from ultrasmall ZIF-8, well-defined molecular transport pathways from the porous nanosheets, and hydrogen-bond-mediated interfacial chain rigidification. Remarkably, the separation layer remains defect-free even when thinned to ∼100 nm, owing to the ultrathin architecture of the ZIF-8@COF nanosheets and their excellent interfacial compatibility. The resulting ultrathin mixed matrix membrane delivers an attractive CO 2 permeance of 1365 GPU and a CO 2 /N 2 selectivity of 38.4 under mixed-gas conditions, along with robust operational stability and pressure resistance. This work demonstrates that two-dimensional porous composites hold great promise as fillers for fabricating high-performance ultrathin MMMs toward practical carbon capture applications.
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Membranes
·
2026
·Vol. 16
·期 6
·189
·
IF 4.2
Huimin Ma,Xiaoxue Jiang,Nianwei Man,Jing Zhao
The urgent demand for energy-efficient CO2separation technologies has propelled significant advancements in polymer-based CO2separation membranes over the past decade. This review systematically examines three primary classes of these membrane materials: conventional dense polymer membranes, microporous polymer membranes, and mixed matrix membranes (MMMs). We analyze their distinct transport mechanisms, advantages, and the persistent challenges of permeability-selectivity trade-offs, physical aging, and scalability that have hindered widespread industrial adoption despite significant laboratory advances. Furthermore, we offer a forward-looking perspective on critical research directions, including the molecular design of stable microporous polymers, the evolution of MMMs towards continuous hybrid architectures, and the development of scalable ultrathin membrane fabrication techniques. By integrating materials innovation with engineering practicality, polymer-based membranes are poised to play a transformative role in sustainable carbon management.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Jing Zhang,Yutong Dai,Songyao Liu,Can Fang,Jingru Yang,Xianyi Ma,Linjie Ye,Jiqing Lu,Yubing Xiong,Zhifeng Dai
To address the challenges associated with global carbon emissions, this study developed a novel class of porous ionic polymer catalysts. Using a bipyridine-based porous organic polymer (POP-Bpy) as the framework, two Ionic liquid-functionalized materials, POP-Bpy-Et and POP-Bpy-OH, were successfully synthesized via quaternization with 1,2-dibromoethane and 2,3-dibromopropanol, respectively. Comprehensive structural characterization (including 13 C NMR, FTIR, and XPS) confirmed the successful quaternization and formation of the desired ionic polymer architectures. Catalytic evaluation revealed that POP-Bpy-OH exhibits outstanding performance in the cycloaddition of CO 2 with epoxides. Under mild conditions (60 °C, 1 atm CO 2 , 48 h), POP-Bpy-OH achieved 94.3% conversion of epichlorohydrin with 99% selectivity toward the corresponding cyclic carbonate, significantly outperforming the hydroxyl-free counterpart POP-Bpy-Et (78.4% conversion). Moreover, under industrially relevant low-CO 2 conditions (15 %CO 2 , 96 h), POP-Bpy-OH maintained a high conversion of 83.3%, far exceeding that of POP-Bpy-Et (64.2%). This enhanced activity is attributed to a pronounced synergistic effect between the hydroxyl groups (acting as hydrogen-bond donors) and the bromide anions (Br − ) in POP-Bpy-OH, which not only boosts reaction efficiency but also affords good substrate compatibility for epoxides with low to moderate steric hindrance. These results underscore that incorporating hydroxyl functionalities into the polymer backbone is a key strategy for improving CO 2 cycloaddition catalysis. In addition to high activity, POP-Bpy-OH demonstrated excellent structural stability and recyclability. After five consecutive reaction cycles, its catalytic activity decreased by only about 3%, highlighting its potential for practical industrial application. To elucidate the origin of its superior performance, density functional theory (DFT) calculations were employed to probe the reaction mechanism. The simulations show that the hydroxyl groups lower the ring-opening energy barrier of the epoxide via hydrogen-bonding interactions, while the adjacent Br − facilitates the nucleophilic attack. This cooperative action efficiently drives the cycloaddition reaction forward, providing an atomic-level understanding of the catalyst's high activity and selectivity.
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Petroleum Exploration and Development
·
2023
·
IF 7.5
Chunming XIONG,Falin WEI,Haiyang YANG,Song ZHANG,Bin DING,Zhengdong LEI,Deping ZHANG,Qiang ZHOU
A smart response fluid was designed and developed to overcome the challenges of gas channeling during CO 2 flooding in low-permeability, tight oil reservoirs. The fluid is based on Gemini surfactant with self-assembly capabilities, and the tertiary amine group serves as the response component. The responsive characteristics and corresponding mechanism of the smart fluid during the interaction with CO 2 /oil were studied, followed by the shear characteristics of the thickened aggregates obtained by the smart fluid responding to CO 2 . The temperature and salt resistance of the smart fluid and the aggregates were evaluated, and their feasibility and effectiveness in sweep-controlling during the CO 2 flooding were confirmed. This research reveals: (1) Thickened aggregates could be assembled since the smart fluid interacted with CO 2 . When the mass fraction of the smart fluid ranged from 0.05% to 2.50%, the thickening ratio changed from 9 to 246, with viscosity reaching 13 to 3100 mPa·s. As a result, the sweep efficiency in low-permeability core models could be increased in our experiments. (2) When the smart fluid (0.5% to 1.0%) was exposed to simulated oil, the oil/fluid interfacial tension decreased to the level of 1×10 −2 mN/m. Furthermore, the vesicle-like micelles in the smart fluid completely transformed into spherical micelles when the fluid was exposed to simulated oil with the saturation greater than 10%. As a result, the smart fluid could maintain low oil/fluid interfacial tension, and would not be thickened after oil exposure. (3) When the smart fluid interacted with CO 2 , the aggregates showed self-healing properties in terms of shear-thinning, static-thickening, and structural integrity after several shear-static cycles. Therefore, this fluid is safe to be placed in deep reservoirs. (4) The long-term temperature and salt resistance of the smart fluid and thickened aggregates have been confirmed.
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Advanced Materials Interfaces
·
2018
·Vol. 6
·期 2
·1801200
·
IF 4.834
Yutian Wang,Hanjun Hu,Yufan Sun,Yang Tang,Liming Dai,Qing Hu,Adrian Fisher,Xiao Jin Yang
Nanostructure and crystallinity of transition metals play an important role in catalyzing carbon dioxide electroreduction (CO 2 ER) where Cu is a typical electrocatalyst with a wide variety of products and Pb has a high overpotential for H 2 evolution and is selective toward formic acid. In this study, 3D hierarchical nanostructures of Cu–Pb catalyst are prepared by a two-step electrodepositing–annealing–electroreduction approach (EAE). Cu nanowires (Cu NWs) of 200–400 nm diameter are built on the surface of commercial nickel foam substrates through an EAE step. Then, Pb nanoparticles with diameter of 5–10 nm are uniformly created on the surface of Cu NWs by a second EAE step. The nanostructural Cu–Pb electrodes catalyze CO 2 ER at a current density of −9.35 mA cm −2 (at −0.93 V vs reversible hydrogen electrode (RHE)). The H 2 evolution is suppressed by 35.6% and CO and HCOOH are enhanced by 29.6% and 9.2%, respectively, as compared with Cu NWs. The protocol proposed in this study provides a simple and straightforward approach for preparing high-performance, hierarchical nanostructures of Cu–Pb bimetal catalyst for CO 2 ER.
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Journal of Energy Chemistry
·
2026
·
IF 15.6
Zhongliang Dong,Wenfa Chen,Ruixi Qiao,Yuyang Long,Meipeng Jian,Mingkai Xu,Zheng Tang,Xuchen Nie,Jun Yin,Yanpeng Liu,Zhiwei Hu,Yinlong Zhu
To realize an ideal photocatalyst for CO 2 photoreduction to CH 4 , developing an “all-in-one” optimization system that targets every elementary step in the photocatalytic CO 2 methanation is highly desirable but remains a great challenge. Here, we present a unique rare-earth modulation strategy to collectively regulate the behaviors of light adsorption, charge separation, reactant supply, and active sites in the photocatalysis process for achieving highly active, selective, stable, and economic CO 2 methanation photocatalysts. Particularly, the proof-of-concept CuPr alloy quantum dots-decorated TiO 2 photocatalysts optimized with rare-earth elements and compositions (denoted as TiO 2 -Cu 7 Pr 1 AQDs) exhibit outstanding photocatalytic activity with a CH 4 production rate of 792.6 μmol g −1 h −1 and electron selectivity of 96.6%, surpassing various state-of-the-art photocatalysts ever reported. Comprehensive experiments and theoretical analysis demonstrate that rare-earth regulation can create multiple advantageous conditions targeting different steps, which enable TiO 2 -Cu 7 Pr 1 to fulfill the essential criteria for an ideal high-efficiency non-noble-metal photocatalyst for CO 2 methanation, including favorable light absorption, enriched reactant supply of CO 2 /H + , rapid carrier separation and transfer, as well as highly active methanation site. The proposed all-in-one design concept in this work not only develops a noble-metal-free photocatalyst with ultrahigh performance toward photocatalytic CO 2 methanation but also provides significant inspiration in various photocatalysis applications.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Junpeng Huang,Wenbo Wang,Hongyang Zhou,Yujie Tao,Bin Liu,Guoxing Zhu,Xiaomeng Lv
Electrocatalytic CO 2 -to-methanol (MeOH) is hindered by the low efficiency of single-site catalysts, primarily due to insufficient local concentration of the key ⁎ CO intermediate. This work aims to construct a dual-site catalyst to synergistically boost ⁎ CO generation and its subsequent hydrogenation, thereby enhancing methanol production. Herein, a cooperative interface was designed by integrating single atoms Ni (SAs Ni) for CO 2 -to-CO conversion and amino-functionalized cobalt phthalocyanine (CoPc-NH 2 ) for methanol formation on N-doped carbon nanotubes ((SAs Ni + CoPc-NH 2 )/N-CNT). The dual-site catalyst achieves a remarkable methanol Faradaic efficiency (FE MeOH ) of 48.7% and a total current density of 45.6 mA cm −2 at −1.05 V vs. RHE, outperforming single-component CoPc-NH 2 /N-CNT (FE max = 28.4%) and physically mixed SAs Ni/N-CNT + CoPc-NH 2 /N-CNT (FE max = 30.6%) in an H-cell. A peak FE MeOH of 51.9% and a methanol partial current density of 103.8 mA cm −2 are achieved in a flow cell. When tested in a membrane electrode assembly (MEA) electrolyzer fed with simulated flue gas (10% CO 2 ), the catalyst delivers a current density of 500 mA cm −2 , while maintaining a FE MeOH of 67.1%. In situ attenuated total reflectance–surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) confirms the enhanced surface coverage of ⁎ CO and the emergence of the ⁎ CHO intermediate exclusively on the dual-site interface, revealing a synergistic mechanism wherein SAs Ni sites enrich the local ⁎ CO concentration and adjacent CoPc-NH 2 sites facilitate its selective hydrogenation to methanol. This work provides a catalyst design paradigm for efficient CO 2 -to-methanol conversion and offers fundamental insights into constructing cooperative interfaces for multistep electrocatalytic reactions. Download: Download high-res image (185KB) Download: Download full-size image
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Tengfei Zhang,Feng He,Jianling Zhang,Fangna Gu
It is challenging to fabricate supported Ni catalysts with more active sites to improve their low-temperature catalytic performance in CO 2 methanation . Herein, firstly, ultrathin (∼4 nm) NiZrAl layered double hydroxide (LDH) nanosheets were synthesized by co-precipitation method, followed by aqueous miscible organic solvent treatment (AMOST), and applied as catalyst precursors for CO 2 methanation. After H 2 reduction, the surface area of Ni particles in NiZrAl-LDH-AMO-R was significantly higher than that of NiZrAl-LDH-R without AMOST. As a result, the NiZrAl-LDH-AMO-R showed higher catalytic activity than NiZrAl-LDH-R owing to its higher H 2 and CO 2 chemisorption capacity and lower activation energy . During the 100 h-lifetime test, NiZrAl-LDH-AMO-R maintained a steady CO 2 conversion of about 92.3%. Moreover, NiZrAl-LDH-AMO-R maintained its catalytic activity after a 600 °C-hydrothermal treatment, suggesting its high stability. In situ DRIFTS results reveal that CO 2 methanation on both NiZrAl-LDH-R and NiZrAl-LDH-AMO-R followed the HCOO∗ route. Interestingly, more active sites obtained after AMOST strongly promoted the generation and decomposition of HCOO∗, and thus significantly improved the activity of NiZrAl-LDH-AMO-R at low temperatures.
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RSC Advances
·
2022
·Vol. 12
·期 40
·26307-26318
·
IF 4.036
Juan Bai,Ziwei Song,Lijuan Liu,Xu Zhu,Faming Gao,Raghunath V. Chaudhari
Metal–organic frameworks (MOF) have been studied extensively for the adsorption and catalytic conversion of CO2. However, previous studies mainly focused on the adsorption capabilities of partially or totally Ce substituted UiO-66, there are few studies focusing on transformation of the structure and catalytic activity of these materials. In this work, a series of Zr/Ce-based MOFs with UiO-66 architecture catalysts were prepared for the conversion of CO2 into value-added dimethyl carbonate (DMC). Owing to the different addition order of the two metals, significantly varied shapes and sizes were observed. Accordingly, the catalytic activity is greatly varied by adding a second metal. The different catalytic activities may arise from the different acid–base properties after Ce doping as well as the morphology and shape changes. Besides, the formation of terminal methoxy (t-OCH3) was found to be the rate limiting step. Finally, the reaction mechanism of CO2 transformation in the presence of a dehydrating agent was proposed.
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ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Chao Miao,Kaixuan Shang,Lixing Liang,Shumei Chen,Jing Ouyang
In this work, a Ni-based catalyst supported on a core–shell structure catalytic carrier material (Ni/ZSM-5@MCM-41) based on kaolinite tailings is reported, which exhibits excellent CO2 methanation performance at atmospheric pressure. At 400 °C, CO2 conversion and CH4 selectivity reach 80 and 97% with the space velocity of 12,000 mL gcat–1 h–1, respectively, and it can maintain good stability during the 80 h stability test. Compared with traditional Ni/ZSM-5 and Ni/MCM-41 catalysts, Ni/ZSM-5@MCM-41 has more substantial confinement effects on the active components, and the active components are more evenly dispersed on surface of the carrier. In addition, it is confirmed by the in situ diffuse reflectance infrared Fourier transform spectroscopy technique that CO2 methanation over the Ni/ZSM-5@MCM-41 catalyst follows the path of formate and CO as intermediates.
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ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Guanzhang Liu,Hang Yuan,Xiaobo Li,Ke Li,Lei Mao,Guangya Zhang
Carbon dioxide capture, conversion, and utilization with carbonic anhydrase (CA) as a green and sustainable method still faces the challenges of complex and costly purification, relatively low yield, and poor catalytic performances and reusability. Herein, we proposed an all-in-one strategy to solve these problems by self-assembling nanosized CA oligomeric particles (nCAOPs) into micrometer-sized CA supraparticles (mCASPs) with well-designed tags. The preparation of the purified mCASPs was simple and effective by an easy scalable low-speed centrifugation method with 78% activity recovery. The obtained mCASPs with a yield of 870 mg/L was the reported highest yield of CAs. Interestingly, mCASPs could serve as carrier-free immobilized CAs and retain over 90% original activity after 15 reuse cycles. More encouragingly, mCASPs could redissolve and form nCAOPs, which had excellent catalytic performances. The hydrated activity of nCAOPs was 1.05 times that of free CAs. Also, the kcat/Km value was 1.74 times that of free CAs, and the half-life at 40 °C was 3.83 times that of free CAs. Due to the simplicity of purification and immobilization, high yield, and excellent enzymatic properties, mCASPs and nCAOPs are considered novel bioactive materials, which offer the feasibility of CAs for sustainable CO2 capture to achieve the target of carbon neutrality.
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HIGH PERFORMANCE POLYMERS
·
2022
·
IF 1.73
Yihao Nie,Xibin Yi,Xinfu Zhao,Shimo Yu,Jing Zhang,Xiaochan Liu,Sijia Liu,Zhipeng Yuan,Minna Zhang
The cost of CO2 separation and energy consumption can be decreased through the use of CO2 adsorption. Due to the electron-rich heteroatoms in its network, polyimide (PI) has a remarkable affinity for CO2. Polyethylene glycol (PEG) can increase the layer spacing of polymers, so as to change the mass transfer of CO2 in it. Furthermore, the ether bond (-O-) in PEG has good affinity for CO2. In this study, PEG-1000 was introduced into PI aerogel by mild sol-gel method at low temperature, and freeze-drying was used to produce PI/PEG composite aerogels with directional pore structure. The effect of PEG-1000 content and directional pore structure of the PI/PEG composite aerogels on CO2 adsorption performance were further studied. The L-PI/PEG-4 composite aerogel, which contains 4 g PEG and is directionally frozen in liquid nitrogen, has a CO2 adsorption capacity of 16.76 cm3/g at 25°C and 1 bar. L-PI/PEG-4 aerogel also exhibits high CO2/N2 selectivity and adsorption cycle stability.
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