ENERGY & FUELS
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2018
·
IF 3.024
Yuning Meng,Xindian Wang,Feng Zhang,Zhibing Zhang,Youting Wu
Dual amino functionalized ionic liquid tetramethylammonium lysinate ([N1111][Lys]) was synthesized and mixed with 2-[2-(dimethylamino)ethoxy]ethanol (DMEE) to obtain a series of nonwater absorbents for CO2 capture. The density and viscosity of the IL hybrids were measured. Using dual-vessel absorption system, CO2 absorption capacity and rate were investigated over a wide range of IL mass fractions (5–100%) to evaluate the influence of DMEE content, and 20% was chosen for further studies including influences of temperature and regeneration performances. Mass transfer coefficients with constant absorption area were calculated from apparent absorption rate constant. Fourier transform infrared (FT-IR) and 13C NMR spectra were applied to indicate the absorption process and mechanism. This new nonwater mixed system was proved to have high absorption capacities and prominent regeneration efficiency under mild conditions (80 °C).
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POLYMER
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2018
·
IF 3.483
Shuangbin Fu,Yusheng Qin,Lijun Qiao,Xianhong Wang,Fosong Wang
In the past decade, poly(carbonate ether)polyols, or CO 2 -polyols, have been synthesized by the copolymerization of CO 2 and propylene oxide (PO) with a double metal cyanide (DMC) catalyst in the presence of various chain transfer agents. CO 2 -polyols show great potential use as substitutes for polyols derived from fossil feedstock in the polyurethane industry. Brookfield viscosity tests have revealed the importance of primary hydroxyl (1° OH) content in the reactivity of CO 2 -polyols; in particular, the low 1° OH content of CO 2 -polyols severely limits their application in foam materials . Incorporation of more carbonate linkages has proven to be only moderately efficient for preparing CO 2 -polyols with high 1° OH content, e.g., 19 F NMR spectroscopy indicates that the 1° OH content of a CO 2 -polyol can increase from 13% to 39% when the carbonate content in the CO 2 -polyol is increased from 26.1% to 80.0%. In this study, the PO end-capping route was developed using a strong Lewis acid, such as tris(pentafluorophenyl)borane (FAB) as a catalyst, and a CO 2 -polyol with 1° OH content of 60% was synthesized.
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高影响因子
GREEN CHEMISTRY
·
2018
·Vol. 20
·期 18
·4236-4244
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IF 8.586
Xiaoyan Pei,Dazhen Xiong,Yuanchao Pei,Huiyong Wang,Jianji Wang
Phase separation of microemulsions plays an important role in many applications such as oil recovery, nanomaterials synthesis, and chemical reactions. However, reversible switching from ionic liquid-based microemulsions to complete oil–water phase separation has not been reported so far. In this work, we developed a novel class of stimuli-responsive microemulsions composed of CO2-responsive ionic liquids, n-pentanol and water. The microstructures and phase behavior of the microemulsion systems before and after the bubbling of CO2 were investigated by electrical conductivity, dynamic light scattering, small-angle X-ray scattering, cryogenic transmission electron microscopy, and optical microscopy. It was found that these microemulsions could be reversibly switched from W/O monophase to complete oil–water phase separation upon alternate bubbling and removal of CO2 at atmospheric pressure. Furthermore, 13C NMR spectroscopy was used to understand the CO2-driven reversible phase separation of the microemulsions. The results suggest that the mechanism behind the reversible phase separation involved the reversible formation of bicarbonate and carbamate from the reaction between CO2 and the anions of the ionic liquids in the presence of water, which resulted in the increase of ionic strength (or vice versa) in the mixture. Using the microemulsions as microreactors, the phase separation protocol was applied in the Knoevenagel reaction for an efficient coupling of a chemical reaction, product separation, and recycling of the microemulsions.
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
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2019
·Vol. 94
·期 12
·3780-3786
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IF 2.659
Yujiang Wang,Yang Xu,Qiankun Liu,Jinwei Sun,Shengfu Ji,Zhou-jun Wang
Background Carbon dioxide (CO 2 ) methanation is an important reaction in energy and environmental fields, which aims to convert CO 2 into natural gas with hydrogen (H 2 ) from renewable sources. One of the technical bottlenecks for CO 2 methanation is the lack of feasible catalysts, especially the ones with satisfactory low-temperature activity. Results The NiMgAl/SiC composite catalyst that was derived from hydrotalcite precursor on the SiC substrate possessed enhanced low-temperature activity and excellent long-term stability in CO 2 methanation. For the low-temperature activity, CO 2 conversion reached 63.8% and 74.5% at 300 and 325 °C respectively. For the long-term stability, CO 2 conversion merely decreased from 78.4% to 76.9% after 50 h of reaction at 400 °C. Conclusion The NiMgAl/SiC composite catalyst was successfully synthesized by the co-precipitation method, which exhibited enhanced low-temperature methanation activity compared with the NiMgAl and Ni/SiC catalysts. The superior low-temperature activity was mainly ascribed to two structural parameters. One was the small nickel (Ni) nanoparticle size, which was endowed by the unique structure of the hydrotalcite precursor. The other one was the high reducibility of Ni species, which was rendered by the appropriate metal-support interactions. The present work provides guidelines for the synthesis of highly efficient composite catalysts for energy and environmental applications. © 2019 Society of Chemical Industry
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CHEMICAL ENGINEERING JOURNAL
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2019
·
IF 8.355
Yafei Guo,Chang Tan,Peng Wang,Jian Sun,Weiling Li,Chuanwen Zhao,Ping Lu
Magnesium-based adsorbents present great potential in separating CO 2 from flue gas stream. To satisfy the requirement of efficient CO 2 capture, it is imperative to select suitable methods for preparing MgO adsorbents with good physicochemical properties. In this study, MgO adsorbents were prepared with different methods using MgCl 2 ·6H 2 O as magnesium precursor, and the effect of synthesis method on their structure-performance relationships were investigated. It is found that MgO adsorbents prepared with different methods exhibited varied physicochemical properties, and these were associated with their diverse CO 2 adsorption capacities. Amongst the different MgO adsorbents, the sample prepared with the solid-state chemical reaction method (MgO-SR) featured good textural properties (high specific surface area and total pore volume of 100.03 m 2 /g and 0.67 cm 3 /g), preferable surface morphology (sheet-like structure with reduced layer diffusion resistance) and excellent CO 2 adsorption capacity (2.39 mmol CO 2 /g). The solid-state chemical reaction method endowed the adsorbent with abundant surface basic active sites, and CO 2 molecules interacted with the weak sites (OH group), medium sites (Mg-O pairs) and strong sites (O 2− ) to form stable bicarbonate, bidentate and unidentate carbonates. The experimental CO 2 uptakes were in good agreement with the values predicted by the Avrami fractional kinetic model. Physical adsorption and chemisorption coexisted in the CO 2 adsorption process and the chemisorption sites played a dominant role. The approach enlightens the facile fabrication of cost-effective MgO adsorbents from waste precursors for large-scale CO 2 capture applications.
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FUEL
·
2017
·
IF 4.601
Zhaohe Huang,Bin Jiang,Huawei Yang,Baoyu Wang,Na Zhang,Haozhen Dou,Guangsen Wei,Yongli Sun,Luhong Zhang
Glycerol, an abundant byproduct in biodiesel industry process, has received a lot of attention in recent years. In this work, a series of glycerol-derived binary and ternary CO 2 binding organic liquids (CO 2 BOLs), were proposed for carbon capture. Physical properties, 1 H NMR spectra and FT-IR spectra of these systems were studied to describe the multiple interactions between constituents. The CO 2 absorption performances were evaluated in details, and excellent CO 2 uptake capacity was achieved. In order to systematically clarify the role of glycerol in superbase environment for CO 2 capture process, binary systems were further explored to support the conclusions both theoretically and experimentally. The characteristic that glycerol could easily be deprotonated in superbase environment, was proved to be benefit to the efficient and homogeneous capture of CO 2 , and a corresponding absorption mechanism was put forward. In addition, the effects of superbase and ionic liquids on absorption were also investigated. The results in this work showed how green, economic and high performance absorbents could be designed for applications of carbon capture.
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RSC Advances
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2017
·Vol. 7
·期 78
·49777-49786
·
IF 3.108
Zanru Guo,Hongjian Gu,Wei Ma,Qiang Chen,Zhanfeng He,Jiali Zhang,Yongxin Liu,Longzhen Zheng,Yujun Feng
The design of controllable or “signal-triggered” metal nanoparticles is one of the emerging trends in nanotechnology and advanced materials. CO2-switchable polymer-hybrid silver nanoparticles (AgNPs) were prepared by a one-pot reaction reducing AgNO3 and trithioester terminated PDEAEMA with sodium borohydride (NaBH4). The hybrids showed a long-term stability, and their size and size distribution can be easily modulated by tuning the molar ratio of polymers to AgNO3. The hybrids not only exhibit hydrophobic–hydrophilic transitions in immiscible mixed solvents, but also undergo a switchable dispersion/aggregation states upon alternately treating with CO2 and N2. Moreover, this smart hybrid was preliminarily used as catalyst for the reduction of 4-nitrophenol. The catalytic activity of the hybrids can be switched and monotonously tuned by varying the flow rate of CO2 purged into the reaction system, which may open a new avenue for tailoring the catalytic activity of metal nanoparticles toward a given reaction.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2017
·
IF 4.421
Xuepeng Wu,Yongping Huang,Sisi Fang,Caili Dai,Hao Li,Zhongliang Xu,Mingwei Zhao
CO 2 -responsive wormlike micelles based on monomer erucic acid 3-(N,N-dimethylamino)propylamide (EADP) with or without sodium salicylate (NaSal) in aqueous solution were studied and compared with “pseudo” gemini system. The “pseudo” gemini system were formed by a mixture of EADP and maleic acid (MA) with molar ratio between 2:1–1:1. Different morphological transformations of microstructures in response to EADP concentrations, additives and CO 2 stimuli were further investigated in these systems, the wormlike micelle or vesicles can be obtained. The mechanism of these transitions were further investigated by rheology, cryo-TEM and DFT calculation, the results showed that the mechanism behind this transition involved reversible reaction of CO 2 with EADP. The mechanism in this research may give further evidence to the self-assembly of CO 2 -responsive surfactants.
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JOURNAL OF DISPERSION SCIENCE AND TECHNOLOGY
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2017
·
IF 1.591
Lei Liu,Cunchuan Zheng,Hongsheng Lu
We reported two simple and novel CO2-responsive surfactant wormlike micellar systems consisting of commercial anionic surfactant sodium oleate (NaOA) and common hydrophobic tertiary amine N,N-dimethylcyclohexylamine (DMCHA), N,N-dimethylbenzylamine (DMBA). The conductivity, pH, and rheological measurements demonstrated the CO2-sensitive flowing behavior and property, which were attributed to the spherical-wormlike micelles transition, verified by cryogenic transmission electron microscopy (Cryo-TEM) and dynamic laser light scattering (DLS) measurements. Moreover, the transition can be easily cycled more than three times without deterioration of viscosity. Combined with the species distribution curve and 1H NMR spectra, a mechanism of the intermolecular electrostatic interaction and hydrophobic effects was proposed.
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高影响因子
AICHE JOURNAL
·
2024
·
IF 3.5
Dongyu Jin,Wenyu Ge,Zhiyong Zhou,Yuming Tu,Chenchan Du,Zhongqi Ren
Porous liquids (PLs) with unique porous frameworks and good flow properties can achieve coupling enhancement for CO 2 capture and conversion. In this paper, a series of novel PLs were designed and synthesized using UiO-66 as the framework and novel bi-cationic ionic liquids (ILs) as an excluded solvent. The prepared PLs showed significant improvement in CO 2 uptake capacity over ILs at different pressures and exhibited excellent CO 2 catalytic conversion performance, exceeding the sum of the effects of ILs and UiO-66. Especially at low pressure, the PLs still showed excellent catalytic performance, but the catalytic performance of the corresponding ILs was significantly reduced, which was due to the rapid adsorption and conversion of CO 2 by the porous framework of UiO-66 to improve the CO 2 uptake and transfer efficiency within the ILs, thus achieving coupling enhancement. It can provide a new way to realize the efficient conversion of CO 2 under milder conditions.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
Ren Yuqi,Fu Yiwei,Li Naixu,You Changjun,Huang Jie,Huang Kai,Sun Zhenkun,Zhou Jiancheng,Si Yitao,Zhu Yuanhao,Chen Wenshuai,Duan Lunbo,Liu Maochang
H 2 O dissociation plays a crucial role in solar-driven catalytic CO 2 methanation, demanding high temperature even for solar-to-chemical conversion efficiencies <1% with modest product selectivity. Herein, we report an oxygen-vacancy (V o ) rich CeO 2 catalyst with single-atom Ni anchored around its surface V o sites by replacing Ce atoms to promote H 2 O dissociation and achieve effective photothermal CO 2 reduction under concentrated light irradiation. The high photon flux reduces the apparent activation energy for CH 4 production and prevents V o from depletion. The defects coordinated with single-atom Ni, significantly promote the capture of charges and local phonons at the Ni d -impurity orbitals, thereby inducing more effective H 2 O activation. The catalyst presents a CH 4 yield of 192.75 µmol/cm 2 /h, with a solar-to-chemical efficiency of 1.14% and a selectivity ~100%. The mechanistic insights uncovered in this study should help further the development of H 2 O-activating catalysts for CO 2 reduction and thereby expedite the practical utilization of solar-to-chemical technologies.
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PubMed
高影响因子
Science Advances
·
2024
·Vol. 10
·期 47
·
IF 11.7
Rongrong Pan,Qi Wang,Yan Zhao,Zhendong Feng,Yanjun Xu,Zhuan Wang,Yapeng Li,Xiuming Zhang,Haoqing Zhang,Jia Liu,Xiang-Kui Gu,Jiangwei Zhang,Yuxiang Weng,Jiatao Zhang
Sluggish surface reaction is a critical factor that strongly governs the efficiency of photocatalytic solar fuel production, particularly in CO2-to-ethanol photoconversion. Here, inspired by the principles underlying enzyme catalytic proficiency and specificity, we report a biomimetic photocatalyst that affords superior CO2-to-ethanol photoreduction efficiency (5.5 millimoles gram−1 hour−1 in average with 98.2% selectivity) distinctly surpassing the state of the art. The key is to create a class of catalytic pocket, which contains spatially organized NH2…Cu-Se(-Zn) multiple functionalities at close range, over ZnSe colloidal quantum wells. Such structure offers a platform to mimic the concerted cooperation between the active site and surrounding secondary/outer coordination spheres in enzyme catalysis. This is manifested by the chemical adsorption and activation of CO2 via a bent geometry, favorable stabilization toward a variety of important intermediates, promotion of multielectron/proton transfer processes, etc. These results highlight the potential of incorporating enzyme-like features into the design of photocatalysts to overcome the challenges in CO2 reduction.
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高影响因子
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