CHEMICAL ENGINEERING JOURNAL
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2016
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IF 5.31
Feng Xu,Ying Yu,Jian Yan,Qibin Xia,Haihui Wang,Jing Li,Zhong Li
An ultrafast synthesis method is developed for the preparation of composites of graphite oxide and HKUST-1, GrO@HKUST-1. Fast synthesis of GrO@HKUST-1 composites can be quickly achieved at room temperature within 1 min. The synthesized composites were characterized by XRD, SEM, N 2 adsorption, FTIR and TGA. The isotherms of CO 2 and N 2 on the as-synthesized materials were measured and the isosteric heats of CO 2 adsorption were estimated. The CO 2 /N 2 adsorption selectivities were predicted by means of ideal adsorbed solution theory (IAST). Results show that the GrO@HKUST-1 composites have higher BET surface area and pore volume than the parent HKUST-1. The CO 2 adsorption capacity of 2GrO@HKUST-1 (2% of GrO) is up to 9.02 mmol/g at 1 bar and 273 K, giving an increase of 32% in comparison of the parent HKUST-1. The isosteric heat of CO 2 adsorption on 2GrO@HKUST-1 is slightly higher than that of HKUST-1, suggesting the stronger interaction between CO 2 molecules and 2GrO@HKUST-1. The CO 2 /N 2 adsorption selectivity of 2GrO@HKUST-1 is significantly enhanced over pristine HKUST-1. At 1 bar, the CO 2 /N 2 adsorption selectivity of 2GrO@HKUST-1 is up to 186, while that of parent HKUST-1 is only 103. This rapid room temperature synthesis route is promising for new MOF-based composites.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2017
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IF 2.843
Ke Mei,Xi He,Kaihong Chen,Xiuyuan Zhou,Haoran Li,Congmin Wang
A strategy for improving CO2 capture by imidazolium ionic liquids (ILs) through a reduction in the formation of carbene–CO2 complex was reported. The carbene–CO2 complex content in CO2 capture by imidazolium ILs was determined by a quantitative NMR method, and the carbene–CO2 complex formation was decreased through a reduction in the basicity of the anion and an enlargement in the steric hindrance of the cation. Thus, both enhanced absorption capacity and improved desorption were achieved, where an ideal IL, [Ipmim][Triz], exhibited a very high capacity of 0.21 g of CO2/g of IL and excellent reversibility.
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Energy Technology
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2017
·Vol. 5
·期 8
·1195-1199
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IF 2.789
Yuanhao Cai,Yulong Chen,Qijie Li,Liang Li,Haoxin Huang,Suying Wang,Weixing Wang
We demonstrate that l -methionine, a natural amino acid, can be used to dramatically enhance CO 2 uptake kinetics in the formation of CO 2 hydrate without the use of energy-intensive mixing technologies or environmentally harmful chemicals. To the best of our knowledge, l -methionine is the most effective promoter to enhance CO 2 hydrate formation (at a concentration of 0.2 wt %, the gravimetric capacity reached up to 356 mg g −1 in 1000 min, and t 90 (the time to achieve 90 % of this capacity) was only 15 min). We also present a tentative explanation for the promotion mechanism of l -methionine in the formation of CO 2 hydrate from the point of view of structure–property relationship that will help search for more effective promoters. Our results may offer the possibility of practical application of hydrate-based CO 2 capture and storage technology.
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APPLIED ENERGY
·
2017
·
IF 7.182
Xiaowen Zhang,Xin Zhang,Helei Liu,Wensheng Li,Min Xiao,Hongxia Gao,Zhiwu Liang
In this work, the regeneration of rich CO 2 -loaded monoethanolamine (MEA) solvent with two catalysts (e.g. SAPO-34 and SO 4 2− /TiO 2 ) was investigated in order to reduce the energy requirement for solvent regeneration. The regeneration behavior with and without catalyst of a 5M MEA solution with an initial CO 2 loading of 0.5 mol CO 2 /mol amine at 96 °C was studied to compare their CO 2 desorption rate and heat duties. The results show that the two solid acid catalysts can reduce the heat duty for solvent regeneration and increase the CO 2 desorption rate in comparison with blank test. The mechanism of CO 2 desorption with catalyst in 5M MEA was proposed based on the result of catalyst characterization (e.g. N 2 absorption/desorption experiment, Py-IR, NH 3 -TPD, FT-IR and XRD) to better understand the desorption process. The results indicate that SAPO-34 with the higher joint value of Brϕnsted/Lewis acid sites ratio (B/L) and mesopore surface area (MSA) shows the faster CO 2 desorption rate and lower heat duty than SO 4 2− /TiO 2 . Based on the experimental results, the addition of solid acid catalysts into amine solution could be considered as one of choices to reduce the heat duty for CO 2 desorption from CO 2 -loaded amine solvent.
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CHEMICAL ENGINEERING RESEARCH & DESIGN
·
2025
·
IF 3.9
Xingyu Lin,Hongsheng Lu,Ruoxin Zhang,Yingjiang Chen,Baiwen Huang
Gas channeling during CO 2 flooding presents a significant challenge to the effective underground storage of CO 2 . This study introduces a novel gas channel blocking strategy using the phase transition properties of fatty acid based CO 2 -responsive ionic liquids (ILs). The ILs were synthesized from choline hydroxide (Ch) and high-melting-point fatty acids (FA), including myristic acid (C14) and palmitic acid (C16), named FA-Ch ILs. These ILs demonstrate phase transformation behavior after CO 2 injection, leading to the precipitation of FA as solid particles. The FA-Ch ILs aqueous solution exhibits low viscosity, ensuring excellent injectivity for oilfield applications. After CO 2 injection, the precipitated FA particles act as gas channeling plugging agents, while the protonated Ch ions effectively inhibit clay swelling to enhance oil recovery with a synergistic effect. Structural properties and interaction mechanisms of the FA-Ch system were characterized by FT-IR, 1 H NMR, and molecular dynamics simulations. The particle size of the FA precipitates was regulated by adjusting FA-Ch concentration and CO 2 injection rate to make it suitable as a profile control agent. Furthermore, Ch + ions demonstrate clay swelling inhibition comparable to traditional inhibitors like KCl. This dual-functionality positions FA-Ch ILs as an innovative solution for addressing gas channeling and clay swelling in CO 2 flooding, offering a cost-effective and environmentally friendly alternative to conventional methods.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Yan Xin,Binfei Li,Zhaomin Li,Zongyang Li,Bo Wang,Xiaopu Wang,Mengyuan Zhang,Weitao Li
During the CO 2 flooding process in fractured low-permeability oil reservoirs, the injected CO 2 is prone to channeling along fractures due to severe reservoir heterogeneity, resulting in poor development effect. The CO 2 -responsive gel system shows dual advantages in achieving CO 2 capture and plugging gas channeling to enhance oil recovery. This paper constructed a system with good CO 2 sensitivity based on long-chain alkyl amide propyl dimethyl tertiary amine first. Subsequently, the properties of the system before and after the response were evaluated through rheological test, and its microstructure was characterized by Cryo-TEM. The system exhibited good CO 2 responsiveness, transitioning from low-viscosity solution system to high-viscosity CO 2 -responsive gel system upon contact with CO 2 , with its viscosity increasing by nearly five orders of magnitude. The CO 2 -responsive gel demonstrated excellent shear resistance, viscoelasticity and shear self-repairing ability. The change of microstructure further verified the mechanism of molecules self-assembly in the system under the action of CO 2 . Then, a series of core physical simulation experiments were carried out to comprehensively evaluate the effects of different factors on the injection capacity, plugging characteristics, dynamic filtration damage performance and EOR effect of CO 2 -responsive gel. The gel maintained injectability while achieving an exceptional deep plugging effect, and the plugging rate reached 98.77%. It showed good characteristics of low filtration and permeability damage in low permeability reservoirs, effectively ensuring the fracture plugging effect. After the fracture was plugged by gel, the sweep range of CO 2 to the matrix significantly expanded, and the gas flooding recovery increased by 18.19–21.7%. Finally, the matrix-fracture dual-media chip model was used to conduct microfluidic experiment, the oil displacement characteristics in different displacement stages were visually clarified, and the synergistic plugging and oil displacement mechanism between the CO 2 -responsive gel and CO 2 was summarized. The research results can provide important insights for the green and efficient application of CO 2 -responsive gel in fractured low-permeability reservoirs.
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Small
·
2024
·
IF 13
Rou-Yu Li,Wenyu Yuan,Shuo Wang,Peng Zhang,Heng Wu,Yi-Min Su,En-Lei Wen,Xiaolin Zhu,Quan-Guo Zhai
The synthesis of value-added products via CO 2 electroreduction (CO 2 ER) is of great significance, but the development of efficient and versatile strategies for the controllable selectivity tuning is extremely challenging. Herein, the tuning of CO 2 ER selectivity through the modulation of CO 2 adsorption behavior is proposed. Using the constructed zeolitic MOF (SNNU-339), CO 2 adsorption behavior is controllably changed from *CO 2 to CO 2 * via the precise ligand-to-metal charge donation (LTMCD) regulation. It is confirmed that the high electronegativity of the coordinate ligand directly restricts the LTMCD, reduces the charge density on the metal sites, lowers the Gibbs free energy for CO 2 * adsorption, and leads to the transformation of CO 2 adsorption mode from *CO 2 to CO 2 *. Owing to the modulated CO 2 adsorption behavior and regulated kinetics, SNNU-339 exhibits superior HCOOH selectivity (≈330% promotion, 85.6% Faradaic efficiency) and high CO 2 ER activity. The wide applicability of the proposed approach sheds light on the efficient CO 2 ER. This study provides a competitive strategy for rational catalyst design and underscores the significance of adsorption behavior tuning in electrocatalysis.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Mingjie Cheng,Bo Gao,Xiaoli Zheng,Wenzhuo Wu,Weiqian Kong,Pengfei Yan,Zubin Wang,Bin An,Yunpeng Zhang,Qingchao Li,Qun Xu
Exploring a facile, rapid and efficient route to produce metal-organic frameworks (MOFs) with highly accessible active sites is of great importance for catalysis. Here we demonstrate the CO 2 coordination can drive low temperature rapid synthesis of porphyrin-based bismuth-MOFs (Bi-PMOFs) by utilizing synergistic physical and chemical properties of supercritical CO 2 (SC-Bi-PMOFs). The molecular-level role of scCO 2 in the synthesis of SC-Bi-PMOFs have been investigated through a series of characterizations including in-situ time-dependent infrared spectroscopy, wherein chemical coordination of CO 2 promotes to fabricate 2D SC-Bi-PMOFs nanosheets. Moreover, the formation of Cu-PMOFs and Fe-PMOFs proves the universal scCO 2 strategy for synthesizing PMOFs. Density functional theory (DFT) calculations together with experiments results confirm the SC-Bi-PMOFs with abundant active sites guarantee efficient ligand-to-metal charge transfer and reduction efficiency of CO 2 . The high-efficiency utilization of CO 2 for synthesizing a series of MOFs and subsequent catalysis on photocatalytic CO 2 reduction for valuable chemicals realize the carbon recycle.
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GREEN CHEMISTRY
·
2025
·
IF 9.2
ZhiWei Dong,YaLing Jia,Zeyu Wang,Antony Rajendran,Wen-Ying Li
Electrocatalytic CO2 reduction to formic acid is a promising strategy to obtain value-added chemicals and achieve the carbon cycle. However, its practical application is generally impeded by the limited accessibility of CO2 to the catalyst's surface and the lack of efficient universal catalyst across different pH levels. Herein, we report a new catalyst, i.e., SnS2 decorated with hydrophobic polymer polyvinylidene fluoride (SnS2+PVDF), for the effective electrocatalytic CO2 reduction to formate/formic acid across a wide pH range in a flow cell. This catalytic system accomplishes a remarkable Faradaic efficiency for the formic acid production in alkaline (98%), neutral (86%), and acidic (93%) electrolytes. Also, the single-pass carbon efficiency reaches up to 72.77% in acidic electrolyte. Water contact angle measurements in association with the in-situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy results indicate that the inclusion of PVDF creates a hydrophobic microenvironment which increases the CO2/H2O ratio near the surface of SnS2 particles. As a consequence, SnS2 particles enjoy the enhanced CO2 concentration around their surface to form many three-phase (solid-liquid-gas) boundary. In-situ Raman spectra combined with electrocatalytic studies reveal that SnS2 undergoes reconstitution to form catalytically active Sn/SnS2 during the reaction. These findings ensure and expand the generality of hydrophobic microenvironment regulation strategy in promoting electrocatalytic CO2 reduction to formic acid.
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MATERIALS RESEARCH BULLETIN
·
2024
·
IF 5.3
Chuanyun Yang,Xingjian Zhang,Zhengdao Li,Zhishuai Wang,Jiping Shi,Haiquan Xie,Ting Li,Yong Zhou
A series of hybrid films were designed and fabricated by in situ growth of Ag 2 S nanoparticles with varying content on BiVO 4 nanosheets deposited on stainless steel mesh. The formation of a p-n heterojunction between Ag 2 S and BiVO 4 enabled an extended spectral response range and facilitated the separation of charge carriers through a single directional pathway for electron transport. Exploiting these advantages, Ag 2 S/BiVO 4 composites were employed in various photocatalytic applications under simulated solar irradiation. The results demonstrated, in terms of water purification, that the composite not only possessed photocatalytic ability to degrade RhB or Cr(VI) individually but also exhibited significantly enhanced photocatalytic efficiency in simultaneously removing mixed pollutants containing RhB and Cr(VI). In terms of CO 2 conversion, Ag 2 S/BiVO 4 also displayed a stronger photocatalysis capability compared to pure BiVO 4 film. Furthermore, the immobilized Ag 2 S/BiVO 4 film exhibited improved mechanical strength and long-term stability, making it highly suitable for practical applications.
研究领域:
材料科学
·
环境科学
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Advanced Energy Materials
·
2026
·
IF 25.5
Siyun Ren,Junnan Han,Jie Liang,Weixi Lu,Lin Zhou,Xing Zhang,Jun Xu,Jia Zhu
Solar-driven carbon dioxide (CO 2 ) hydrogenation represents a promising route for producing value-added chemicals/fuels with a negative carbon footprint. Plasmonic catalysis attracts significant attention as it synergistically employs thermochemistry and photochemistry, facilitated by multiple thermal and/or nonthermal effects, including efficient solar energy harvesting, localized heating, localized electric field, and hot carrier excitations. Herein, a metallic cobalt nanowire array is employed as the plasmonic catalyst to demonstrate that the reaction kinetics of CO 2 hydrogenation are effectively improved by light-excited plasmonic localized electric field through regulating the binding strength of reactive intermediates. Theoretical simulations and operando spectroscopic data further reveal that the catalytic durability is significantly enhanced compared to traditional thermocatalysis because of the localized electric field-assisted suppression of coking deactivation. This work presents the first demonstration of plasmonic-enhanced catalytic durability, delivering key mechanistic insights for the future design of efficient and stable plasmonic catalysts.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-10
·
IF 16.6
Lei Qinqin,Yuan Huiqing,Du Jiehao,Ming Mei,Yang Shuang,Chen Ya,Lei Jingxiang,Han Zhiji
The direct utilization of solar energy to convert CO 2 into renewable chemicals remains a challenge. One essential difficulty is the development of efficient and inexpensive light-absorbers. Here we show a series of aminoanthraquinone organic dyes to promote the efficiency for visible light-driven CO 2 reduction to CO when coupled with an Fe porphyrin catalyst. Importantly, high turnover numbers can be obtained for both the photosensitizer and the catalyst, which has not been achieved in current light-driven systems. Structure-function study performed with substituents having distinct electronic effects reveals that the built-in donor-acceptor property of the photosensitizer significantly promotes the photocatalytic activity. We anticipate this study gives insight into the continued development of advanced photocatalysts for solar energy conversion.
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