JOURNAL OF SOLID STATE CHEMISTRY
·
2022
·
IF 3.656
Lei Ma,Feifei Zhang,Kunjie Li,Yingying Zhang,Zhiqiang Song,Li Wang,Jiangfeng Yang,Jinping Li
The capture of N 2 O from CO 2 by an adsorption-based mechanism remains a significant challenge due to their similar molecular sizes and physical properties. Although substituent engineering has been widely employed for the selectivity regulation and improvement of gas mixtures in metal-organic frameworks, its effect on N 2 O/CO 2 separation has yet not been explored. Herein, four isoreticular MTN-type metal-organic frameworks (MOFs) with different substituents (-H, –NH 2 , -Br or –NO 2 ) are reported for the capture of N 2 O from a N 2 O/CO 2 mixture. As revealed by isothermal measurements, thermodynamic studies and ideal adsorbed solution theory computations, the N 2 O/CO 2 separation potential can be effectively improved by an electron-donating group (-NH 2 ), whereas electron-withdrawing groups (-NO 2 or -Br) exhibit the opposite effect. Notably, MIL-101(Cr)–NH 2 exhibits, by far, the highest ideal adsorbed solution theory equilibrium adsorption selectivity of 1.91 for 50/50 N 2 O/CO 2 . The N 2 O/N 2 separation ability of the modified materials is also studied and functionalization with a -Br group yields an improved separation potential compared to the parent MIL-101(Cr) material. The strategy of using substituents to enhance the N 2 O/CO 2 separation efficiency of MOFs could also be extended to other porous materials for chemical separation processes.
研究领域:
材料科学
·
化学工程
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DOI
高影响因子
Carbon Energy
·
2026
·
IF 21.4
Sheraz Ahmed,Byunggon Song,Mun Kyoung Kim,Yurim Sohn,Chirong Sun,Wooyul Kim,Hyung-Suk Oh,Jong Ho Won,Hyung Mo Jeong,Jaehoon Kim
Electrochemical reduction of CO 2 (CO 2 RR) offers a promising route to convert waste carbon into valuable chemical feedstocks while mitigating greenhouse emissions. However, achieving high activity and selectivity in CO 2 RR remains challenging due to the low solubility of CO 2 in aqueous electrolytes and competing hydrogen evolution reactions (HER) that limit efficiency under practical conditions. Here, we address these limitations by coupling high-pressure operation with atomic-scale catalyst design. A tin oxide (SnO x ) nanoparticle catalyst featuring sub-nanometer interplanar gaps (< 1 nm) was synthesized via an electrochemical cation implantation (ECI) process to create confined reaction environments. The resulting ECI(S)–SnO x achieved a Faradaic efficiency for CO (FE CO ) of 69.2% and a current density of –11.2 mA cm −2 at –3.0 V under 7.4 MPa. Additionally, the CO 2 RR reaction maintained stable performance for 40 h. The synergy between atomic-scale confinement and CO 2 pressurization enhances CO 2 availability, suppresses HER, and promotes CO formation through a *COOH-mediated pathway. This work establishes a general strategy for tuning CO 2 electroreduction pathways by integrating nanoscale structural confinement with controlled reaction environments.
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高影响因子
JOURNAL OF CHEMICAL THERMODYNAMICS
·
2018
·
IF 2.631
Hui Guo,Li Hui,Shufeng Shen
Non-aqueous amine-based absorbents are considered as a potential application for CO 2 removal from biogas to reduce energy consumption, due to lower heat capacity and evaporation enthalpy of organics than conventional water solvent. In this work, monoethanolamine (MEA) + 2-methoxyethanol (EGME) mixtures were proposed as a novel CO 2 carrier. The density and viscosity of CO 2 -free and CO 2 -loaded MEA + EGME solutions were measured at temperatures of (293–353) K, for 10–100 mass % MEA. CO 2 solubility in 31.0 mass% (5.0 M) MEA solutions was investigated at temperatures from 313 K to 393 K and CO 2 partial pressures up to 260 kPa. The excess molar volumes and the ratio of viscosity η · η EGME −1 were correlated by Redlich-Kister equation and Weiland’s model, respectively. The vapour-liquid equilibrium data were correlated by using a semi-empirical model, i.e. CO 2 partial pressure as a function of temperature and CO 2 loading. The predicted values and the measured data matched well each other, with AAD within 0.2% for density, 4.5% for viscosity and 19.5% for CO 2 solubility respectively.
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高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Zhen Wang,Li Deng,Xue-Rui Yang,Jin-Xia Lin,De-Quan Cao,Jun-Ke Liu,Zhen Tong,Jing Zhang,Gao-Yang Bai,Yu-Xi Luo,Zu-Wei Yin,Yao Zhou,Juntao Li
The production of Li 2 CO 3 /C through CO 2 reduction reaction in nonaqueous systems is a complex four-electron, multi-step process, and the short existence time of intermediate monomers is not conducive to observation, which causes great difficulties in clarifying and regulating the CO 2 reduction path. Herein, ferrocene (Fc) as a functional additive into the electrolyte can stabilize the discharge intermediates and favor the occurrence of the two-electron reaction path during CO 2 RR, which leads to more stable operation of the Li-CO 2 battery; with the assistance of Fc, the CO 2 reduction pathway in Li-CO 2 battery is also clarified. Theoretical calculation analysis combined with experimental characterization observation confirms that Fc can shorten the CO 2 reduction distance through interaction with CO 2 and affecting the solvent environment around Li + , stabilize intermediate products to clarify the discharge path. The existence time of intermediates and discharge depth of the battery are key factors affecting the CO 2 reduction pathway. The Li 2 C 2 O 4 formed by CO 2 reduction through the 2-electron pathway is more favorable for the reversible operation of the Li-CO 2 battery than Li 2 CO 3 /C through the 4-electron pathway. This work provides inspiration for clarifying the reaction mechanism and regulating the CO 2 reduction pathway to improve the electrochemical performance of Li-CO 2 battery in the future.
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高影响因子
Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 13
·7300-7313
·
IF 14.511
Zhao Sun,Junpeng Liu,Rongjun Zhang,Yu Wu,Hongwei Li,Sam Toan,Zhiqiang Sun
Sorption-enhanced steam reforming of methanol (SE-SRM) is a promising approach to creating a high-purity hydrogen supply. However, catalysts suffer from activity deactivation and low CO2 uptake capacity. In this study, we investigate the role of Ga doping of Cu–MgO in SE-SRM by synthesizing a series of MgO embedded xGaCuMg catalytic sorbents via a sol–gel method. The TEM-EDX mapping results indicate that MgO nanoparticles can be successfully embedded in the bulk-phase of the catalytic sorbent with a stabilized microstructure. The results from in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) reveal that the Ga-doped catalytic sorbent is conducive to promoting the conversion of C-containing intermediates in SE-SRM, and absorbing CO2 in the form of bidentate carbonate rather than monodentate carbonate. Experimental studies verify that the best uptake capacity of 18GaCuMg catalytic sorbent (36.25 mg CO2/g MgO) achieves almost complete conversion of methanol (99.70%) with 100% H2 selectivity at 200 °C. Specifically, no CO is formed during the kinetic-control stage of SE-SRM. Density functional theory (DFT) calculations based on the Cu(111)Ga2O3(202)MgO(200) model revealed that the Ga doping can enhance the adsorption energies of methanol and carbon dioxide, promoting methanol activation and increasing CO2 uptake capacity. These findings provide valid strategies for functionalized nanomaterial design, which will substantially promote the SE-SRMR performance with desired catalytic sorbent recyclability.
研究领域:
材料科学
·
催化化学
·
能源工程
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DOI
高影响因子
Catalysts
·
2026
·Vol. 16
·期 3
·245
·
IF 4.5
Yijun Wen,Yang Liu,Shuwei Wang,Junyi Liu,Haize Jin
A type of photothermal catalyst was prepared by photoreducing cobalt ions with geopolymer/Ag9(SiO4)2NO3(GA). The loading of Co0significantly expanded the visible-light response range. Due to the photoreduction effect, the loading of Ag0and Co0facilitated the transfer of photogenerated electrons and strong thermal excitation, significantly enhancing the photothermal synergy effect. The photothermal catalyst achieved a CO production rate of 70.20 mmol·gcat−1·h−1, and the selectivity of CO reached 97.67% at 400 °C. The CO product rate in the fifth cycle still reached 68.8 mmol·gcat−1·h−1, which provided a reference for extending the functionality of photocatalysts after the photoreduction of heavy metal ions.
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高影响因子
APPLIED ENERGY
·
2022
·
IF 11.446
Rukuan Chai,Yuetian Liu,Jingru Wang,Qianjun Liu,Zhenhua Rui
Owing to the harmful consequences of the greenhouse effect, mankind has reached a consensus to reduce CO 2 emissions. CO 2 utilization and sequestration is considered the most feasible solution for realizing an effective and economical sequestration of CO 2 . Herein, CO 2 -enhanced oil recovery (EOR) is a representative strategy owing to its tremendous sequestration capacity and reasonable economic viability. However, the low sequestration stability and the accompanying secondary disasters have hindered its wider application. Considering this, a novel CO 2 utilization and sequestration technology, i.e., CO 2 electrochemical reduction (CO 2 RR)-EOR technology was proposed and its effects and mechanisms were studied. First, a SnO 2 catalyst that can be used in the coreflooding experiments was synthesized and its efficiency on CO 2 RR was evaluated. Then, coreflooding experiments using the SnO 2 catalyst were conducted to study the influence of CO 2 RR on the CO 2 sequestration and oil recovery. Next, contact angle and interfacial tension were measured to analyze the effect of the CO 2 RR on the CO 2 -crude oil-brine-rock interaction. Finally, the CO 2 RR-EOR mechanism was proposed. Multiple experiments revealed that the low-cost and easy-synthesis SnO 2 catalyst, which was characterized by the 3-dimensioned hierarchical and porous structure, was in the high efficiency and strong stability. Coreflooding results illustrated that the CO 2 RR remarkably enhanced CO 2 sequestration and oil recovery. At the optimal cell potential of 3.75 V, the CO 2 sequestration efficiency and oil recovery were as high as 75.93% and 43.8%, respectively, which are much higher than those (50.56% and 37.9%, respectively) achieved in conventional CO 2 flooding. Contact angle and interfacial tension results indicated that the CO 2 RR has a significant impact on the CO 2 -crude oil-brine-rock interaction. At the optimal cell potential, the crude oil-contact angle and the interfacial tension were 36.2° and 8.9 mN/m, respectively, which are much lower than those (64.6° and 16.4 mN/m, respectively) achieved in conventional CO 2 flooding; the CO 2 -contact angle was 52.2°, which too is much larger than that (31.7°) achieved in conventional CO 2 flooding. In this technology, the CO 2 RR converts the injected CO 2 into formate to sequestrate itself, and meanwhile alters the CO 2 -crude oil-brine-rock interactions, resulting in enhanced CO 2 wettability and consequently increases CO 2 trapping and retention; causing the weakened oil wettability and the enhanced oil-brine interaction, and finally enhances oil recovery. CO 2 RR-EOR can be a novel, efficient, and economically-viable CO 2 utilization and sequestration technology, which provide a feasible option for the future industrial CO 2 emission reduction.
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高影响因子
ADSORPTION SCIENCE & TECHNOLOGY
·
2022
·
IF 4.373
Zhijuan Zhang,Pengwei Li,Ting Zhao,Yuanhan Xia
The ZIF-8 crystals were successfully postsynthetically modified using methylamine (MA), ethylenediamine (ED), and N, N-dimethylethylenediamine (MMEN) to improve their adsorption performance toward CO2. Results showed that, compared with the original ZIF-8, the BET specific surface area of MA-ZIF-8, MMEN-ZIF-8, and ED-ZIF-8 has increased by 118.2%, 92.0%, and 29.8%, respectively. In addition, their total pore volume increased separately by 130.8%, 100%, and 48.7%. The adsorption capacities of CO2 on the amine-modified ZIF-8 samples followed the order . The CO2 adsorption capacities at 298 K on MA-ZIF-8, MMEN-ZIF-8, and ED-ZIF-8 were increased by 118.2%, 90.2%, and 29.8%, respectively. What is more, the CO2/N2 selectivities calculated using an IAST model of the amine@ZIF-8 samples at 0.01 bar and 298 K were also significantly improved and followed the order , which increased by 173.0%, 121.4%, and 22.6%, respectively. The isosteric heat of CO2 adsorption () on the MA-ZIF-8, MMEN-ZIF-8, and ED-ZIF-8 all becomes higher, while of N2 on these samples was slightly lower in comparison with that on the ZIF-8. Furthermore, after six recycle runs of gravimetric CO2 adsorption-desorption on MA-ZIF-8, the adsorption performance of CO2 is still very good, indicating that the MA-ZIF-8 sample has good regeneration performance and can be applied into industrial CO2 adsorption and separation.
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DOI
高影响因子
ENERGY & FUELS
·
2023
·
IF 5.3
Chuanhong Wang,Xuefang Chen,Shimiao Yao,Fen Peng,Lian Xiong,Haijun Guo,Hairong Zhang,Xinde Chen
The morphology and regeneration ability of adsorbents are important for gas pressure swing adsorption and separation. Herein, HCP-1 (a hyper-crosslinked polymer) and HCP@MAO(Fe) (a hyper-crosslinked polymer modified by ferrocene) with a spherical morphology are synthesized by a post-crosslinking reaction of chloromethylated styrene-divinylbenzene (Cl-St-DVB) beads for the separation of CO2/CO and CO2/CH4. Both static adsorption and dynamic separation tests verified that HCP@MAO(Fe) has the best gas adsorption and separation performance. The highest adsorption capacity of CO2 reached 1.24 mmol/g. The IAST selectivity of CO2/CO is up to 20.6. Moreover, HCP@MAO(Fe) can be regenerated by simple vacuum operation, contributing to the low value of adsorption enthalpy (24.5 KJ/mol). The adsorption mechanism between CO2 and the resin framework was also studied by experiments and electrostatic potential map analysis. A stronger interaction can be found between CO2 and HCP@MAO(Fe) as a result of the higher Mulliken charge of the cyclopentadiene structure.
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高影响因子
JOURNAL OF NANOSCIENCE AND NANOTECHNOLOGY
·
2019
·Vol. 19
·期 6
·3232-3236
·
IF 1.093
Peng Mingyue,Ci Suqin,Shao Ping,Cai Pingwei,Wen Zhenhai
Exploiting effective electrocatalysts toward electrochemical conversion of CO2 into valued-added chemicals is highly desirable for achieving the global carbon cycle. In this work, we report the synthesis of Cu3P/C nanocomposites by phosphatizing the copper-based
metal organic framework precursor. Systematic electrochemical characterizations demonstrate the Cu3P/C nanocomposites hold high activity and favorable selectivity towards CO2 reduction reaction (CO2RR) into CO, as manifested by an onset potential is about −0.25
V versus reversible hydrogen electrode (RHE) and a faradic efficiency (FE) of 47% for CO production at a relatively low potential (−0.3 V). The attractive catalytic properties might be attributed to the synergistic effect of cooper and phosphorus elements, as well as the unique structure
of Cu3P. Furthermore, we propose an asymmetrical-electrolyte Zn–CO2 battery with the Cu3P/C as cathode catalyst, demonstrating a decent performance with an open-circuit voltage of 1.5 V and a power density of 2.6 mW cm−2 (at 10 mA cm−2).
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PubMed
高影响因子
ACS Applied Polymer Materials
·
2025
·
IF 4.7
Jinpeng Liu,Chengcheng Hao,Huili Zhang,Hongyu Chen,Ling Zhang,Xiaodong Chen,Jianye Wang,Maohuai Wang,Shuxian Wei,Xiaoqing Lu,Zhaojie Wang,Siyuan Liu
Covalent organic frameworks (COFs) have become potential candidates for gas purification technology, especially in carbon capture and storage applications. By utilizing strategies such as pore structure design and functional modification, COFs have been developed to exhibit high selectivity and superior adsorption capacity for the effective capture and separation of CO2 from industrial waste gases. Notably, alkali metals exhibit strong interactions with the backbone of the COFs, which can enhance the CO2/N2 adsorption separation performance of these porous materials. This study details the synthesis of two-dimensional COF materials modified with acidic groups (TpPa-COOH and TpPa-SO3H) via mechanical grinding. Alkali metals such as Na, Li, and K were introduced into these groups through simple ion exchange reactions, thereby creating metal-modified COF materials. The impact of various alkali metals on the CO2/N2 adsorption separation performance of COF materials was investigated. Among the resulting products, lithiated TpPa-COOH showed the highest CO2 capture capacity of 2.65 mmol/g at 273 K and 1 bar. This may be due to the smaller atomic size of Li that offers larger adsorption space. Under the same conditions, the K-modified TpPa-SO3H exhibited the highest selectivity of 548, which surpasses most COFs reported in the literature. The superior performance was caused by the high polarization of the COF backbone triggered by the alkali metals. The inference was further confirmed by computational simulations. This work provides a facile method for the modification of porous materials with alkali metals to achieve superior gas separation performance.
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高影响因子
Nanomaterials
·
2024
·Vol. 14
·期 15
·1269
·
IF 4.4
Haobin Wu,Xin Huang,Min Xiao,Shuanjin Wang,Dongmei Han,Sheng Huang
High-energy-density Li-CO2batteries are promising candidates for large-capacity energy storage systems. However, the development of Li-CO2batteries has been hindered by low cycle life and high overpotential. In this study, we propose a CO2-based thermoplastic polyurethane (CO2-based TPU) with CO2adsorption properties and excellent self-healing performance to replace traditional polyvinylidene fluoride (PVDF) as the cathode binder. The CO2-based TPU enhances the interfacial concentration of CO2at the cathode/electrolyte interfaces, effectively increasing the discharge voltage and lowering the charge voltage of Li-CO2batteries. Moreover, the CO2fixed by urethane groups (-NH-COO-) in the CO2-based TPU are difficult to shuttle to and corrode the Li anode, minimizing CO2side reactions with lithium metal and improving the cycling performance of Li-CO2batteries. In this work, Li-CO2batteries with CO2-based TPU as the multifunctional binders exhibit stable cycling performance for 52 cycles at a current density of 0.2 A g−1, with a distinctly lower polarization voltage than PVDF bound Li-CO2batteries.
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PubMed
高影响因子
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