SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Yanan Jiang,Yanbin Yun,Lihua Wang,Min He,Zhi Qiu,ZuYu Li
Polybenzimidazole (PBI) membranes have attracted considerable attention in the energy sector for their outstanding performance. Nevertheless, their development is often restricted by low ionic conductivity. Coordinating metal ions (Fe 3+ ) with PBI can expand the spacing between polymer chains, creating nano-scale ion channels that enhance OH - transport within the membranes. In this study, we fabricated mPBI@Fe coordination membranes using the solution casting method. By varying the iron content, the ionic conductivity of these membranes was regulated. The findings revealed that the conductivity of OH - in these membranes was approximately 61.81 % higher than that of the original mPBI membranes, and they demonstrated excellent mechanical and thermal stability. Furthermore, compared to the commercial FAA-3–50 membrane, the [email protected] membrane demonstrates higher carbon monoxide (CO) fraction current density at a voltage of 3.0 V in the membrane-electrode assembly (MEA). Notably, at 50 mA cm -2 , the Faraday efficiency (FE CO ) of the [email protected] membrane electrodes remained above 95 %. Even after 870 min of electrolysis at 100 mA cm -2 , the FE CO decreased by only 1.57 %. These findings suggest promising prospects for advancing high-performance PBI-based membranes in electrochemical carbon dioxide reduction applications.
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高影响因子
LANGMUIR
·
2025
·
IF 3.9
Yuchen Zhou,Zezhi Chen,Huijuan Gong,Donglin Jiang,Huiqiang Yu,Lu Chen
Zinc porphyrin is a promising carbonic anhydrase (CA) mimic for promoting CO2 absorption, but its application is hindered by poor dispersibility in absorption solutions. To address these challenges, we developed a strategy to impregnate zinc porphyrin on an γ-Al2O3 carrier. The hydrophilic surface groups and porous structure of γ-Al2O3 were expected to enhance both the hydrophilicity and stability of zinc porphyrin. To verify its feasibility, zinc tetraphenylporphyrin (ZnTPP) was chosen as the representative to synthesize ZnTPP/Al2O3. Characterizations showed that ZnTPP could be loaded into the pores of γ-Al2O3 in a highly dispersed state. Also, ZnTPP/Al2O3 could be uniformly dispersed in the absorption liquid, effectively exposing the Zn2+ active sites and reducing diffusion resistance. CO2 absorption experiments revealed that ZnTPP/Al2O3 significantly enhanced CO2 absorption in water, 20 wt % K2CO3, and 20 wt % monoethanolamine (MEA) solutions, far outperforming original ZnTPP. Density functional theory (DFT) calculations further elucidated the interaction mechanisms, showing that oxygen atoms on γ-Al2O3 stabilize ZnTPP by forming van der Waals and coordination bonds with Zn2+ active sites. Additionally, these oxygen atoms donate electrons to Zn2+, enhancing its catalytic activity. These findings highlight the effectiveness of this strategy and provide a promising pathway for optimizing other CA-mimics for CO2 capture applications.
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CHEMICAL ENGINEERING SCIENCE
·
2024
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IF 4.1
Wenxing Ye,Yizhen Tang,Xiaoru Liang,Qingyuan Luo,Weihai Liang,Chao Chen,Ke Zhang
Porous silicas have been extensively investigated as amine carriers for the production of CO 2 adsorbents, while few studies demonstrated that as-synthesized silicas (without template removal) can also serve as good amine carriers for efficient CO 2 capture. This raises a fundamental question of whether the time-consuming and energy-intensive process of removing the template from as-synthesized silicas is still necessary. More importantly, a reasonable mechanism is quite needed to explain the as-synthesized silicas as effective amine carriers. To this end, in this study, four types of as-synthesized silicas were compared together with their corresponding porous silicas as amine carriers for CO 2 capture. Experimental results show that as-synthesized silicas exhibit comparable or even better performance at medium amine loadings (50 ∼ 60 wt%), including larger CO 2 adsorption capacities and better cyclic stability, while porous silicas predominate at high amine loadings (70 wt%). Molecular simulation results indicate that the amine species are located in the interparticle cavities in the silicas rather than in the structural pores. This work provides important guidance for the future design of practical solid-amine CO 2 adsorbents.
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JOURNAL OF MOLECULAR LIQUIDS
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2024
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IF 5.3
Kunpeng Hou,Hairong Wu,Guorui Xu,Genglin Li,Tianfang Luan,Jiawei Chang,Tong Cheng,Zhaojie Song,Jirui Hou
Aiming to address the issues of limited suitability of conventional chemical oil displacement materials for formation conditions and the serious emulsification of oil and water in the produced liquid, the innovative nano oil-displacing system with CO 2 -responsive behavior has been developed. This system integrates oil displacement and emulsion breaking. The efficacy of the CO 2 -response system in creating stable emulsions with a high capacity to decrease interfacial tension has been demonstrated. The interfacial responsive behavior of all active components, including Janus nanoparticles, sodium oleate, gums, and asphaltenes, in the emulsion system was analyzed in terms of interfacial rheology and adsorption. Additionally, the prepared system demonstrated a rapid response to CO 2 , effectively breaking the emulsion within 5 min. Furthermore, the oil recovery enhancing mechanism of the CO 2 -response system was investigated using a microscopic visualization model. The system was proved to be efficient in initiating the residual oil within pore channels. Considering the combined effectiveness of the CO 2 -response system in terms of efficient oil displacement and rapid response, it offers valuable insights for advancing the chemical flooding technology of in enhanced oil recovery.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Lihang Yan,Guanhua Liu,Jianqiao Liu,Jing Bai,Yaoxuan Li,Huaxun Chen,Liya Zhou,Jing Gao,Yanjun Jiang
The utilization of CO 2 has become an important issue aiming to the achievement of carbon neutrality. The enzyme electrocatalytic CO 2 reduction to produce carbonaceous fuels has been increasingly appealing. While the low CO 2 aqueous solubility severely limits the CO 2 reduction efficiency, and the expensive cofactor restricts the application potential. In this study, microporous UiO-66-NH 2 was firstly converted into hierarchically porous structure (HP-UiO-66-NH 2 ) containing both micropores and mesopores to simultaneously enhance the enrichment of CO 2 and the immobilization of formate dehydrogenase by optimizing the pore structure. The relative contents of the protein secondary structures were similar after immobilization. The mechanism of enzyme electrocatalytic CO 2 reduction was proposed. The enzyme stability was highly enhanced after immobilization and the CO 2 reduction was enhanced by the enzyme electrocatalytic system through the combination of CO 2 enrichment and electrocatalytic NADH regeneration. The optimized catalytic system can obtain formate yield of 1.826 mM in 3 h (5.57 times higher than the free enzyme system) with a generation rate of 6086.7 μmol g cat ‑1 h ‑1 .
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Zheng Lian,Youcai Lu,Shiyu Ma,Liqin Wang,Zhongjun Li,Qingchao Liu
In Li-CO 2 battery, redox mediators (RMs) are considered to have bright prospects due to their advantages of optimizing the mediated reaction pathway and reducing over-potential. However, some inherent defects caused by RMs, such as induced Li anode degradation and electron shuttle, limit its application in Li-CO 2 battery. In this work, ruthenium acetylacetonate (Ru(acac) 3 ) was innovatively applied as an efficient RM to boost the performance of Li-CO 2 battery, and the “shuttle effect” of Ru(acac) 3 to Li anode was also confirmed. To avoid the anode degradation caused by “shuttle effect” of RM, a novel Zn-MOF nanoplate modified glass fiber (M-GF) separator is skillfully prepared and used as a dual-function separator for Li-CO 2 battery. Experiments coupled with density functional theory simulations verifies that M-GF can protect Li anode by preventing Ru(acac) 3 from entering Li anode by physical and chemical interactions. Moreover, the highly ordered micropores in Zn-MOF also induce uniform deposition of Li + on the Li anode to delay the degradation process of anode, and thus prolonged the cycle life of the battery. Thanks to the bidirectional support of Ru(acac) 3 and M-GF strategy, the electrochemical performances of the Li-CO 2 battery, especially the round-trip efficiency and cycle life, has been greatly improved.
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Journal of Energy Chemistry
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2024
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IF 14
Liangping Xiao,Qizheng Zheng,Rusen Zhou,Sifan Liu,Yifan Zhao,Yadong Zhao,Renwu Zhou,Kostya Ken Ostrikov
The electrochemical carbon dioxide reduction (eCO 2 RR) to formate, driven by clean energy, is a promising approach for producing renewable chemicals and high-value fuels. Despite its potential, further development faces challenges due to limitations in electrocatalytic activity and durability, especially for non-noble metal-based catalysts. Here, naturally abundant bismuth-based nanosheets that can effectively drive CO 2 -to-formate electrocatalytic reduction are prepared using the plasma-activated Bi 2 Se 3 followed by a reduction process. Thus-obtained plasma-activated Bi nanosheets (P-BiNS) feature ultrathin structures and high surface areas. Such nanostructures ensure the P-BiNS with outstanding eCO 2 RR catalytic performance, highlighted by the current density of over 80 mA cm −2 and a formate Faradic efficiency of >90%. Furthermore, P-BiNS catalysts demonstrate excellent durability and stability without deactivation following over 50 h of operation. The selectivity for formate production is also studied by density functional theory (DFT) calculations, validating the importance and efficacy of the stabilization of intermediates (*OCHO) on the P-BiNS surfaces. This study provides a facile plasma-assisted approach for developing high-performance and low-cost electrocatalysts.
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DYES AND PIGMENTS
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2024
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IF 4.1
Ji Xiong,Ming-Hui Chen,Xiang-Yu Li,Quan Shi,Yun-Hao Xu,Ya-Qing Feng,Bao Zhang
The sunlight-driven CO 2 fixation into high value-added industrial products constitutes a promising approach to mitigating global warming, offering an alternative to traditional thermally-driven fixation requiring high temperature and/or high pressure. Herein, we design and synthesize four isostructural porphyrinic covalent triazine frameworks ( Por-CTFs ) including metal-free Por-CTF ( H2Por-CTF ) and metallized Por-CTFs ( MPor-CTFs , M = Co, Zn, Cu) and their photocatalytic activity in CO 2 cycloaddition. All Por-CTFs exhibit wide light adsorption range in visible region via introducing porphyrins into the covalent triazine frameworks (CTFs) skeleton. Different metal ions which are well anchored in the MPor-CTFs skeleton not only offer Lewis acidic sites for substrate interaction but also apparently endow photocatalysts with longer photogenerated carrier lifetimes and higher electron-hole separation efficiency. Encouragingly, under visible light-assisted and mild conditions, the CoPor-CTF exhibits excellent photocatalytic performance achieving a reaction rate of 62.22 mmol g −1 h −1 , which is among the state-of-the-art cases for photocatalytic CO 2 cycloaddition and outperforms two other MPor-CTFs . This work demonstrates that the photophysical and electronic properties of Por-CTFs can be rationally tuned by incorporating various metal ions into porphyrin units to achieve effective photocatalysts for CO 2 cycloaddition.
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JOURNAL OF DISPERSION SCIENCE AND TECHNOLOGY
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2025
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IF 1.9
M. L. Shao,M. J. Cheng,J. Gong,A. L. Chang,L. P. Fu,K. L. Liao,X. Q. Liu
Carbon dioxide (CO2) flooding is one of the efficacious channels to enhance oil recovery efficiency of low permeability reservoirs. However, CO2 gas channeling has seriously affected the development effect due to severe formation heterogeneity. Nanomaterials have good application prospects in plugging gas channeling, but the dispersibility in water limits the plugging effect. In this paper, a nanoparticle plugging agent with a core-shell architecture was synthesized via emulsion polymerization. The impacts of different elements such as grain diameter, temperature and salinity on the swelling characteristic of nanoparticles were studied respectively. Subsequently, the CO2 response property of nanoparticles was tested by uniformly injecting CO2. Finally, based on the calculation of molecular dynamics, the interaction between nanoparticles and water molecules was analyzed. The results showed that the CO2-responsive nanoparticles exhibit a lower swelling ratio (<5), and the residual resistance coefficient is 2.47, demonstrating a limited expansion property and superior plugging performance. The interaction between protonated nanoparticles and water molecules was stronger, resulting in enhanced hydrophilicity and responsive inflation of nanoparticles. The system has great potential application prospects for in-depth CO2 conformance control.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-18
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IF 15.7
Shen Yan,Fang Nan,Liu Xinru,Ling Yu,Su Yuming,Tan Tian,Chen Feng,Lin He,Zhao Boxuan,Wang Jin,Si Duanhui,Xie Shunji,Wang Ye,Zhou Da,Zhang Teng,Cao Rong,Wang Cheng
Interphases are critical in electrochemical systems, influencing performance by controlling ion transport and stability. This study explores a metal-organic interphase in the electrocatalytic reduction of CO 2 (CO 2 RR) on Cu, extending the concept of interphases to CO 2 conversion. Investigating organic modifications on CuO x , we discover metal-organic interphases over 10 nm thick in highly ethanol-selective systems, contrary to the expected monolayer adsorption. Using an automated platform, 1080 CO 2 RR experiments with 180 molecular modifiers identify functional groups affecting selectivity for ethanol and multi-carbon (C 2+ ) products. We find that these modifiers consistently produce metal-organic interphases on the Cu or CuO x surface. These interphases modulate Cu coordination, CO 2 RR intermediates, and interfacial water configuration, significantly improving electrocatalytic performance. Testing across 11 CuO x -based catalysts validates this approach, culminating in the development of two electrocatalysts that achieve ~80% faradaic efficiency for C 2+ products with ethanol partial current densities up to 328 and 507 mA cm −2 . This study highlights the pivotal role of interphases in CO 2 RR, advancing CO 2 conversion technologies.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Yajing Hu,Yong Men,Shuyi Xu,Yuanfen Feng,Jinguo Wang,Kaijie Liu,Yibo Zhang
Constructing the interface of Ni/Y 2 O 3 heterogeneous catalyst is a feasible strategy for efficient catalyst design in CO 2 methanation, which can create the active Y–O–Ni interfacial sites by utilizing the interaction between Ni and Y 2 O 3 . In this work, the strategy of using different nickel precursors (nickel nitrate, nickel acetate, basic nickel carbonate and nickel citrate) was used to prepare various Ni-based catalysts supported on Y 2 O 3 , which were estimated for their catalytic performance on CO 2 methanation. The catalysts were characterized based on BET, XRD, TEM, H 2 -TPR, XPS and CO 2 -TPD, etc. The results indicated a close correlation between the metal dispersion and particle size of Ni/Y 2 O 3 catalysts and the nickel precursor employed. The Y–O–Ni interface structure in Ni/Y 2 O 3 catalysts, associated with basic sites, provides a richer source of basic sites, offering more active sites for CO 2 adsorption and activation. Ni/Y 2 O 3 catalyst prepared with nickel nitrate as the precursor exhibited characteristics such as a highly enhanced nickel dispersion, a smaller nickel particle size, and more abundant metallic Ni 0 sites. Moreover, nickel nitrate-derived Ni/Y 2 O 3 catalyst exhibited optimal catalytic activity, achieving a CO 2 conversion rate of up to 92 % at 300 °C, with 100 % selectivity to CH 4 , and displaying good stability over 30 h. Therefore, the dispersion of Ni and the size of Ni particles could be controlled by adjusting the precursor, which is closely associated with the catalytic activity of Ni/Y 2 O 3 catalyst. This work unveils the interface-property relationship of Ni/Y 2 O 3 catalysts and provides a new insight into strategy of constructing more effective Ni-based catalyst for CO 2 methanation through the controlled nickel precursor.
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FUEL
·
2025
·
IF 7.5
Cuncun Qian,Ming-Jia Li,Ruilong Wang
Solar-powered photocatalytic CO 2 reduction offers great potential for carbon fixation. Conventional wide-bandgap semiconductors absorb little visible light. Dye sensitization improves absorption but reduces photoelectron transfer efficiency, limiting photocatalytic performance. This work reports a self-sensitized anatase brown titanium dioxide (B-TiO 2 ) catalyst developed through an optimized two-step method. Comprehensive experimental and computational analyses reveal that B-TiO 2 extends its spectral absorption edge to 601.94 nm, over 43.69 % compared to P25, significantly enhancing visible light absorbance. The surface of B-TiO 2 characterized by oxygen vacancies, Ti 3+ species, and lattice defects, which are crucial for its markedly improved photocatalytic activity. Under irradiation from a 300 W Xe-lamp, the self-sensitized B-TiO 2 catalyst achieves an impressive total charge-transferred electron number of 570.84 μmol·g −1 ·h −1 and a CO 2 conversion rate of 142.05 μmol·g −1 ·h −1 . Furthermore, the photocatalytic mechanism was investigated in detail. This innovative self-sensitized catalyst offers a promising strategy for developing high-efficiency photocatalysts, potentially advancing the field of photocatalytic CO 2 reduction.
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