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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

MgO promoted by Fe2O3 and nitrate molten salt for fast and enhanced CO2 capture: Experimental and DFT investigation

Fengchun Gong,Zhen Huang,Xiaolan Wei,Shule Liu,Jianfeng Lu,Jing Ding,Weilong Wang

Rapid and strong CO 2 capture is critical in CO 2 capture and utilization (CCU) techniques to mitigate global warming. Alkali molten salt (AMS) promoted-MgO sorbents with high capacity attracted attention, but their applications suffer from various limitations of low adsorption kinetics and poor stability. Here, AMS-promoted MgO sorbents corporation with Fe 2 O 3 (Mg 100-x Fe x -AMS 10 ) were fabricated via modified methanol evaporation-induced surface precipitation for use in rapid and stable CO 2 capture. Based on characterization of the sorbents, Mg 98 Fe 2 -AMS 10 showed a loose flake structure, with a large surface area and numerous exposed active sites. Therefore, Mg 98 Fe 2 -AMS 10 exhibited a strong CO 2 capacity (14.86 mmol CO2 /g sorbent at 300 °C) and good cyclic durability. Three kinetic models were explored, and the Avrami model provided a good prediction of the CO 2 adsorption behavior, with Mg 98 Fe 2 -AMS 10 exhibiting rapid adsorption kinetics. The adsorption mechanism was investigated using density functional theory (DFT) calculations. The charge transfer and bonding strengths of the surface O atoms on MgO increased, and these atoms preferentially bonded with activated CO 2 (CO 2 ∙− ) under Fe catalysis. This study may provide insights into enhancing the CO 2 capture and kinetics of MgO via combination with 3d transition metals.

研究领域: 化学工程 · 环境科学 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Preparation of molten salt promoted MgO for efficient CO2 capture by microwave method: Performance evaluation and mechanism exploration

Junshen Zhang,Juan Luo,Jiashan Chen,Ziyan Xu,Yuyu Chen,Han Yan,Rui Ma,Shichang Sun

MgO’s great potential for capturing CO 2 has drawn a lot of attention, but the limited O 2– sites prevents its further development. This work proposed a microwave-induced method (microwave hydrothermal and microwave sintering) to produce high-performance MgO CO 2 adsorbent and was further modified using carbonates (K 2 CO 3 ) and nitrates of alkali metals (NaNO 3 , KNO 3 ). The outcomes demonstrated that the small particle size MgO nanocrystals (6.20 nm) with a CO 2 uptake of 1.8 mmol·g −1 could be produced by a unique method of microwave heating from the inside out. Among the modified samples, addition of 20 mol% NaNO 3 on the surface of MgO exhibited the highest CO 2 uptake (11.91 mmol·g −1 ), and the uptake was still 7.9 mmol·g −1 after 10 cycles. The addition of molten salt changed the adsorbent’s active sites, resulting in an increase in O 2– alkaline sites and the activation of MgO lattice defects, both of which improved the sample’s CO 2 adsorption performance. This work could offer a new idea for creating affordable and effective CO 2 solid adsorbents to capture CO 2 .

CAS / MDL: 57-09-0
研究领域: 材料科学 · 环境科学
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ACS Omega · 2023 · IF 4.1

CuCl2-Activated Sustainable Microporous Carbons with Tailorable Multiscale Pores for Effective CO2 Capture

Shunyang Yao,Zhi Li,Zhen Liu,Xiaodong Geng,Li Dai,Yanmei Wang

Porosity is the key factor in determining the CO2 capture capacity for porous carbon-based adsorbents, especially narrow micropores of less than 1.0 nm. Unfortunately, this desired feature is still a great challenge to tailor micropores by an effective, low-corrosion, and environmentally friendly activating agent. Herein, we reported a suitable dynamic porogen of CuCl2 to engineer microporous carbons rich in narrow micropores of <1.0 nm for solving the above problem. The porosity can be easily tuned by varying the concentration of the CuCl2 porogen. The resultant porous carbons exhibited a multiscale micropore size, high micropore volume, and suitable surface nitrogen doping content, especially high-proportioned ultromicropores of <0.7 nm. As adsorbents for capturing CO2, the obtained microporous carbons possess satisfactory CO2 uptake, moderate heat of CO2 adsorption, reasonable CO2/N2 selectivity, and easy regeneration. Our work proposes an alternative way to design porous carbon-based adsorbents for efficiently capturing CO2 from the postcombustion flue gases. More importantly, this work opens up an almost-zero cost and industrially friendly route to convert biowaste into high-added-value adsorbents for CO2 capture in an industrial practical application.

CAS / MDL: 7447-39-4 7647-01-0
研究领域: 材料科学 · 环境科学 · 化学工程
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Frontiers of Chemical Science and Engineering · 2013 ·Vol. 7 ·期 3 ·297-302 · IF 0

Comparison study on strategies to prepare nanocrystalline Li2ZrO3-based absorbents for CO2 capture at high temperatures

Xiao Qiang,Tang Xiaodan,Liu Yefeng,Zhong Yijun,Zhu Weidong

A comparison study has been conducted on the strategies for synthesizing nanocrystalline Li 2 ZrO 3 and Kdoped Li 2 ZrO 3 absorbents for CO 2 capture at high temperatures, including solid-state and liquid-phase methods, citrate route, and starch-assisted sol-gel method combined with freeze-drying technique. The absorption properties, including uptake rate and absorption capacity, of synthesized absorbents were investigated by thermogravimetric analysis (TGA) at different CO 2 partial pressures. The nanosized Li 2 ZrO 3 crystals synthesized by the citrate route exhibit a faster uptake and a higher, nearly stoichiometric absorption capacity than those synthesized by the solid-state and liquid-phase methods. The doping of K into Li 2 ZrO 3 can significantly improve the uptake rate of CO 2 , especially at low CO 2 partial pressures. For the synthesis of K-doped Li 2 ZrO 3 , the citrate route has poor reproducibility and scalability, whereas the starch-assisted sol-gel method combined with freeze-drying technique is reproducible and easily scaled up, and the thus synthesized absorbents possess excellent CO 2 capture properties.

研究领域: 材料科学 · 环境科学
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RSC Advances · 2022 ·Vol. 12 ·期 51 ·33069-33078 · IF 4.036

The development of activated carbon from corncob for CO2 capture

Xia Wang,Wulan Zeng,Chunling Xin,Xiangjun Kong,Xiude Hu,Qingjie Guo

The accumulation and incineration of crop waste pollutes the environment and releases a large amount of CO2. In this study, corncob crop waste was directly activated using solid KOH in an inert atmosphere to prepare porous activated carbon (AC) to capture CO2, and to introduce N-containing functional groups that favour CO2 adsorption, urea was mixed with corncob and KOH to prepare N-doped AC. The physical and chemical properties of the AC were characterized, and the effects of the mass ratio of KOH and urea to corncob, the activation temperature and time as well as regeneration were investigated to explore the optimal preparation process. The pores in the AC are mainly micropores, with the specific surface area and pore volume reaching 926.07 m2 g−1 and 0.40 cm3 g−1 for KOH-activated corncob and 1096.70 m2 g−1 and 0.48 cm3 g−1 after N-doping; the C–O plus O–H ratio and the –NH– ratio, which favour CO2 adsorption in N-doped AC were 6.04 and 1.92%, respectively. The maximum adsorption capacities for KOH-activated corncob before and after N-doping were 3.49 and 4.58 mmol g−1, respectively, at 20 °C and remained at 3.44 and 4.52 mmol g−1 after ten regenerations. The prepared corncob-based AC showed good application prospects for CO2 capture.

CAS / MDL: 57-13-6 1310-58-3
研究领域: 环境科学 · 材料科学
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Sustainable Chemistry for Climate Action · 2023 · IF 0

Fine tuning CO2 adsorption and diffusion behaviors in ultra-microporous carbons for favorable CO2 capture at moderate temperature

Ya-Qi Ba,Yong-Sheng Wang,Tian-Yi Li,Zhe Zheng,Guang-Ping Hao,An-Hui Lu

CO 2 capture from flue gas is one of the global urgent tasks. Adsorption separation of CO 2 is an energy-efficient way as compared to the absorption method. The central issue is to devise efficient adsorbents that work well under flue gas conditions with temperatures of 323–348 K and low CO 2 concentrations of 15%. In this work, we targeted this issue and proposed a well-controlled diffusion strategy, which is achieved over a series of poly(furfuryl alcohol)-derived carbons (PFCs) with dense and abundant ultra-micropores. As the adsorption temperature increased from 298 to 348 K, the CO 2 capture capacity is 54% kept for PFC-800, which is 1.2 times higher than that for samples without diffusion limitation. The capture of CO 2 is kinetics control at ambient temperature, however, at 348 K CO 2 with higher kinetic energy can overcome the restriction of the narrow pore entrance and the CO 2 /N 2 selectivity for simulated flue gas composition increases from 20 to 40. Furthermore, the PFCs exhibit a high CO 2 volumetric adsorption capacity of 97 cm 3  cm −3 at 298 K and 1 bar, benefiting the practical application deployed with an integrated adsorption column. The diffusion kinetics can be further tuned when altering the bulk phase into nanocoating, which would inspire their application in different scenarios.

研究领域: 材料科学 · 环境科学 · 化学工程
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ACS Sustainable Chemistry & Engineering · 2024 · IF 7.1

Uncovering the Influence Mechanisms of H2O, O2, and NO2 on CeNiCa Dual-Function Material for Integrated CO2 Capture and In Situ Methanation

Linjia Li,Yiran Zhang,Jiaqi Feng,Shu Zhao,Wei Qiu,Ke Li,Zhen Huang,He Lin

Derived from carbon capture, utilization, and storage (CCUS), integrated carbon capture and utilization (ICCU) has been widely developed recently. Understanding the influences of H2O, O2, and NO2 on dual-function materials (DFMs) performance is crucial for their practical application. In this study, the influence mechanisms of O2, H2O, and NO2 on CeNiCa DFM for ICCU-methanation are investigated. The catalyst was oxidized by O2, H2O, and NO2. NO2 competes with CO2 for basic adsorption sites, inhibiting CO2 adsorption and methanation, but adsorbed NO2 is reduced mainly to N2 and NH3 during methanation. H2O induces agglomeration of the adsorbent and catalyst─the former due to the Ca(OH)2 mobility, and the latter attributed to OH-promoted migration and agglomeration of Ni. On this basis, it is proposed that the dominant roles of H2O, O2, and NO2 change in two- and multi-interference components, but the joint effects among them should not be neglected.

研究领域: 化学工程 · 环境科学
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AICHE JOURNAL · 2022 ·Vol. 68 ·期 8 ·e17706 · IF 4.167

Efficient nickel-based catalysts for amine regeneration of CO2 capture: From experimental to calculations verifications

Qiang Sun,Hongxia Gao,Yu Mao,Teerawat Sema,Sen Liu,Zhiwu Liang

High heat duty is an urgent challenge for industrial applications of amine-based CO 2 capture. The temperature (>110°C) of carbamate breakdown in amine regeneration requires large energy consumption. In this work, we report a novel, stable, efficient, and inexpensive Ni-HZSM-5 catalyst to improve the CO 2 desorption rate and reduce the heat duty. The impregnation method was applied for varying nickel content in the catalysts from 2.16 to 9.80 wt% in HZSM-5. The catalysts were characterized by scanning electron microscope, X-ray powder diffraction, N 2 adsorption–desorption, inductively coupled plasma-optical emission spectrometry, ultraviolet-visible diffuse reflectance spectroscopy, X-ray photoelectron spectroscopy, NH 3 -temperature programmed desorption (TPD), Infrared spectroscopy of pyridine adsorption, and Fourier transform infrared spectroscopy. The catalytic performance was evaluated by CO 2 desorption of rich amine solvent at 90°C. It was found that the introduction of nickel increased the acid sites of catalysts compared with parent HZSM-5. This phenomenon plays a key role on improving the CO 2 desorption rate. The density functional theory (DFT) calculations successfully explain the catalytic performance. The catalytic activity associates with the combined properties of MSA × B/L × Ni 2+ . The 7.85-Ni-HZ catalyst presents an excellent catalytic activity for the CO 2 desorption: it increases the amount of desorbed CO 2 up to 36%, reduces the relative heat duty by 27.07% with the same reaction time, and possesses high stability during five cyclic tests. A possible catalytic mechanism for the Ni-HZSM-5 catalysts through assisting carbamate breakdown and promoting CO 2 desorption is proposed based on experimental results and theoretical calculations. Therefore, the results present that the 7.85-Ni-HZ catalyst significantly accelerates the protons transfer in CO 2 desorption and can potentially apply in industrial CO 2 capture.

CAS / MDL: 142-58-5
研究领域: 化学工程 · 环境科学 · 催化材料
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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Nanostructured AlOOH – A promising catalyst to reduce energy consumption for amine-based CO2 capture

Cong Jiang,Maohong Fan,Ge Gao,Wufeng Jiang,Xiaoshan Li,Cong Luo,Liqi Zhang,Fan Wu

In order to alleviate the intensive energy demand of amine-based post-combustion carbon capture technology, metal oxyhydroxide AlOOH of nanoscale was synthesized through the hydrothermal method and applied to accelerate the CO 2 desorption rate and reduce the regeneration heat duty of aqueous monoethanolamine (MEA) solution for the first time. Results showed that the use of AlOOH could accelerate the desorption rate by up to 560% and increase the desorption amount by 251%. By comparing the performance between AlOOH and Al 2 O 3 , it can be found that the presence of extra hydroxyl groups is 20.6% more efficient in catalyzing CO 2 desorption. According to a simplified heat transfer model created in this work, AlOOH could reduce the heat duty by 17% with only 0.1 wt% loading, which exhibited the highest performance cost ratio among related literature. In addition, the cyclic stability of AlOOH was confirmed through various characterization methods, including XRD, FT-IR, SEM, and N 2 adsorption–desorption. More importantly, a possible catalytic mechanism of AlOOH was discussed and proved where it could change reaction pathways in different CO 2 loading regions. This work reveals a promising research direction towards cost-efficient and high-performance metal oxyhydroxide catalysts in the catalytic amine regeneration field to approach the net-zero carbon emission goal.

研究领域: 材料科学 · 环境工程 · 化学工程
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Journal of CO2 Utilization · 2020 · IF 5.993

Bimetal based inorganic-carbonic anhydrase hybrid hydrogel membrane for CO2 capture

Huan Wen,Lei Zhang,Yingjie Du,Ziyuan Wang,Yunhong Jiang,Hongjie Bian,Jiandong Cui,Shiru Jia

In this study, we synthesized for the first time a bimetal-based inorganic-carbonic anhydrase (CA) hybrid nanoflower to immobilize CA using Cu 2+ and Zn 2+ instead of single metal ion. Subsequently, the synthesized bimetallic hybrid nanoflowers (CANF) were embedded into the poly(vinyl alcohol) (PVA)-chitosan (CS) hydrogel networks to obtain PVA/CS@CANF hydrogel membrane. The CANF exhibited a significantly higher activity recovery of 70 % compared with 35 % with CA/Zn 3 (PO 4 ) 2 hybrid nanoflowers and 10 % with CA/Cu 3 (PO 4 ) 2 hybrid nanoflowers. The PVA/CS@CANF hydrogel membrane possessed excellent mechanical strength, high catalytic activity, and were easy to flow out without centrifugation or filtration. At the same time, the PVA/CS@CANF displayed higher thermostability, storage stability, and pH stability than free CA and CANF , and superior reusability and CO 2 capture capacity. The hydrogel membrane maintained more than 75 % of its original activity after 8 cycles. However, CANF only maintained 12 % of its original activity. Furthermore, the amount of CaCO 3 produced by PVA/CS@CANF membrane was 9.0-fold and 2.0-fold compared with free CA and CANF, respectively. Therefore, This approach to synthesizing bimetallic-based protein hybrid hydrogel membrane could have a bright future in CO 2 capture.

研究领域: 生物化学 · 材料科学 · 环境科学
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Advanced Composites and Hybrid Materials · 2021 ·Vol. 4 ·期 3 ·562-573 · IF 5.693

Poly(sodium-p-styrenesulfonate)-grafted UiO-66 composite membranes boosting highly efficient molecular separation for environmental remediation

Cheng Xi Quan,Li Songwei,Bao Hongfei,Yang Xiaobin,Li Zhixing,Zhang Yingjie,Wang Kai,Ma Jun,Ullah Asmat,Shao Lu

The lack of highly permeable and selective separation membranes hampers the application of the energy-efficient membrane separation process for water remediation and CO 2 capture in molecular scale. Nanoparticles have been widely applied for tailoring pore structures and surface properties of the molecular separation membranes, thereby enhancing separation performance. However, limited by non-ideal nanoparticle aggregation, it remains a big challenge to fabricate such membranes on a large scale. Herein, we designed a kind of highly dispersed nanoparticles through grafting poly(sodium-p-styrenesulfonate) (PSS) on metal organic frameworks UiO-66 and deployed them for tailoring structure of polyelectrolyte membrane (PEM) for water remediation and Pebax (PEBA) symmetrical membranes for CO 2 capture, respectively. Because of electrostatic interaction, the PSS-grafted-UiO-66 (UiO-66-PSS) demonstrated nearly 100% dispersion in water and had an average particle size around 200 nm. Most interestingly, the introduction of the UiO-66-PSS finely tailored the affinity between membranes and target molecules, and the molecular structure of both PEM and PEBA membranes, thereby tripling the permeances of the membranes and slightly improving the selectivity of the membranes meanwhile. The PEM/UiO-66-PSS membranes demonstrated pure water permeance as high as 27.3 L m −2  h −1  bar −1 with MgSO 4 rejection above 98.7%. For CO 2 capture, the PEBA/UiO-66-PSS membranes exhibited 414.5 barrer with selectivity about 53.8. Taken together, the highly dispersed UiO-66-PSS shows strong promise in constructing molecular separation membranes with high separation performance for environmental remediation. Graphical abstract The highly dispersed PSS-grafted-UiO-66 finely tailored membrane structures of PEM membranes and the PEBA membranes and enhanced affinity between the target molecules and the aforementioned membranes, thereby tripling membrane permeances and improving the membrane selectivity slightly. The obtained PEM/UiO-66-PSS membranes and PEBA/UiO-66-PSS membranes show strong promise in water remediation and CO 2 capture, respectively.

研究领域: 环境科学 · 材料科学
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LANGMUIR · 2023 · IF 3.9

Porous Polymer Supported Amino Functionalized Ionic Liquid for Effective CO2 Capture

Jianmeng Wu,Zeying Yang,Jiaqi Xie,Peng Zhu,Jiajiao Wei,Renzhe Jin,Hui Yang

A decrease in CO2 emissions is urgently required in the present situation due to the fast growth of carbon dioxide (CO2) in the atmosphere, which has caused a series of global climate issues. This study used an impregnation–evaporation method to immobilize an amino functionalized ionic liquid [C2OHmim][Lys] on a chromatographic column filler GDX-103 and create a novel supported ionic liquid. The results showed that the supported ionic liquid with 60 wt % ionic liquid content had the best adsorption performance at 40 °C, and the CO2 adsorption isotherm showed that the adsorption capacity at 0.1 MPa was 1.29 mmol CO2/g sorbent, which was 6 times greater than the adsorption capacity of the pure carrier. The sample with 60% ionic liquid content has an adsorption capacity of 1.02 mmol CO2/g sorbent under the condition of CO2/N2 mixed gas with 10% CO2 content. This is 43 times greater than the adsorption capacity of the pure carrier, and its adsorption performance is stable after three adsorption and desorption cycles. Through the rich porous structure of GDX-103, the ionic liquid is effectively supported and dispersed, which expands the contact area between CO2 and ionic liquid and enhances the mass transfer of CO2. At the same time, CO2 can be chemically bound to the groups on the anion of ionic liquid and be immobilized, so it has a high selective adsorption capacity of CO2, which makes it a great alternative to traditional CO2 adsorbents.

研究领域: 环境科学 · 化学工程
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