Journal of Materials Chemistry A
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2025
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IF 9.5
Tao Zhang,Ruijia Wang,Wei Li,Shujun Li,Bing Tian,Shouxin Liu,Zhijun Chen
A simple carbon dots (CDs) catalyst prepared from lignin-derived syringic acid was used for catalytic fixation of CO2 with epoxides to synthesize cyclic carbonates. The catalysts exhibited high catalytic performance which can proceed the reaction under metal-, solvent-, halogen-, and additive-free conditions with 1 atm of CO2 and 80 °C reaction temperature. Various cyclic carbonates could be obtained in high yields and selectivities under the extremely mild catalytic conditions. Additionally, the CDs catalysts showed excellent recyclability with stable catalytic activity. Mechanistic study revealed that the hydroxyl groups on the surface of CDs are responsible for epoxides activation and nitrogen-containing sites (graphitic N and pyridinic N) are crucial for CO2 activation. The cheap precursors, easy and sustainable preparation of catalyst, mild and simple operation of CO2 fixation make the CDs catalyst a promising catalyst for the CO2 conversion.
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Catalysis Science & Technology
·
2024
·
IF 4.4
Zafar A. K. Khattak,Nazir Ahmad,Hussein A. Younus,Habib Ullah,Baoyi Yu,Khurram S. Munawar,Muhammad Ashfaq,Muhammad Yaseen,Muhammad Danish,Mohammed Al-Abri,Rashid AlHajri,Francis Verpoort
Metal(II)-carboxylate frameworks are an important class of MOF materials finding applications in gas storage, separation, sensing, catalysis, etc. Recently, their design, synthesis and characterization have been established at a very fast pace. Here two novel MOFs based on 5,5′-(([1,1′-biphenyl]-4,4′-dicarbonyl)bis(azanediyl))diisophthalic acid (H4L, an amide containing ligand) and transition metals (copper and zinc) are reported. Several characterization tools e.g., FT-IR, XRD, SEM, TGA, and XPS are used to characterize these MOFs. Single-crystal X-ray diffraction and Hirshfeld surface analyses are used to characterize the 3D structural framework. The void and cavity analysis revealed the strength of the crystal packing. Both MOFs followed multistage thermogravimetric disintegration profiles. The solvent molecules escaped around 200 °C and the structural changes due to decompositions in the frameworks continued till 500 °C. The morphological analysis for Zn-MOF and Cu-MOF showed uniform wedge-shaped rectangular blocks and spherical balls with dimensions around 100 and 50 μm, respectively. The amide functionalized Zn(II)-carboxylate framework exhibited high catalytic activity (85–>99%) towards the solvent-free cycloaddition of CO2 to different epoxides e.g., epichlorohydrin, propylene oxide, allyl glycidyl ether and glycidyl isopropyl ether with 100% selectivity under ambient conditions (i.e., 1 bar at 40 °C for 24 h) at very low catalyst loading. By adjusting the reaction conditions (T, P, and co-catalyst), the catalytic conversion reached 100% within only 2 hours. The results showed Zn-MOF as a superior and efficient catalyst compared to other reported MOFs. Additionally, the catalyst can be easily recovered and regenerated for repeated use without performance loss.
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Small
·
2025
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IF 12.1
Ruipeng Jin,Rui Li,Ming-Li Ma,Da-Yu Chen,Jian-Yu Zhang,Zheng-He Xie,Li-Feng Ding,Yabo Xie,Jian-Rong Li
Metal–organic frameworks (MOFs) are rigorously investigated as promising candidates for CO 2 capture and conversion. MOF-on-MOF heterostructures integrate bolstered charger carrier separation with the intrinsic advantages of MOF components, exhibiting immense potential to substantially escalate the efficiency of photocatalytic CO 2 reduction (CO 2 RR). However, the structural and compositional complexity poses significant challenges to the controllable development of these heterostructures. Herein, a conventional MOF-on-MOF nanocomposite is readily optimized from a type II heterojunction to a state-of-the-art cascade Z-scheme configuration via the encapsulation of Pt nanoparticles (Pt NPs), establishing synergistic MOF-MOF and metal-MOF heterojunctions with reinforced built-in electric field. A cascade electron flow is thus propelled, vigorously separating the photogenerated charge carriers and profoundly extending their lifetimes. Collectively, the photocatalytic activity of the cascade Z-scheme is drastically promoted, exhibiting a nearly quintuple enhancement in the CO production rate over the original type II heterostructure. Moreover, the anti-sintering capacity of the developed nanocomposite is unveiled, elucidating its simultaneously improved activity and stability. These findings present unprecedented regulation over the configuration of a MOF-on-MOF heterojunction, substantially enriching the fundamental understanding and rational design strategies of composite materials.
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PubMed
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MATERIALS LETTERS
·
2024
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IF 2.7
Hongmin Cui,Jianguo Xu,Nanfu Yan,Runhan Yan,Jinsong Shi
In the current work, we explored the direct synthesis of S-doped porous carbons employing cesium methanesulfonate as a novel bifunctional chemical activator. The obtained carbons showed high surface area (654–2264 m 2 /g) and high S content (6.56–15.13 wt%). Effects of activation temperature and cesium methanesulfonate amount on the carbons’ properties were also studied. The obtained carbons showed CO 2 uptake of 3.58–4.76 mmol/g at 0 °C and 1 bar. Effects of textural properties and S-doping on CO 2 adsorption performances were discussed.
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JOURNAL OF MOLECULAR LIQUIDS
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2024
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IF 5.3
Sen Qin,Shanshan Dai,Wei Fan,Mei Li,Zou He,Jie Qi,Yang Yang,Huan Yan
To achieve excellent absorptive loading and low viscosity, a novel amino-functionalized ionic liquid [G1.0 PAMAM] [2-MI] combined with water for CO 2 capture is proposed in this work. The concentration of [G1.0 PAMAM] [2-MI], absorption temperature, and aeration rate were optimized by using Response Surface Methodology based on Box-Behnken design, and the model predictions were in good agreement with the experimental data. The results illustrated that the absorption loading of 42.71 wt% [G1.0 PAMAM] [2-MI]/H 2 O was 6.81 mol CO 2 /mol ILs (38.5°C, 100 mL/min), which was much higher than that of MEA /H 2 O, and the regeneration efficiency was maintained at 89.5 % after the eighth regeneration cycle. With the combined effect of 2-MI and water, the viscosities of the solution before and after absorption at 40°C were 35.3 and 53.8 mPa·s, respectively, which were significantly lower than those of the majority of ionic liquid absorbents. The reaction mechanism of [G1.0 PAMAM] [2-MI] with CO 2 was demonstrated by 13 C NMR to be a synergistic combination of a zwitterionic mechanism and a base-catalyzed hydration mechanism to produce carbamate and carbonate/bicarbonate (CO 3 2– /HCO 3 – ).
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-15
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IF 15.7
Xu Ting,Yang Hao,Lu Tianrui,Zhong Rui,Lv Jing-Jing,Zhu Shaojun,Zhang Mingming,Wang Zheng-Jun,Yuan Yifei,Li Jun,Wang Jichang,Jin Huile,Pan Shuang,Wang Xin,Cheng Tao,Wang Shun
Creating and maintaining a favorable microenvironment for electrocatalytic CO 2 reduction reaction (eCO 2 RR) is challenging due to the vigorous interactions with both gas and electrolyte solution during the electrocatalysis. Herein, to boost the performance of eCO 2 RR, a unique synthetic method that deploys the in situ reduction of precoated precursors is developed to produce activated Ag nanoparticles (NPs) within the gas diffusion layer (GDL), where the thus-obtained Ag NPs-Skeleton can block direct contact between the active Ag sites and electrolyte. Specifically, compared to the conventional surface loading mode in the acidic media, our freestanding and binder free electrode can achieve obvious higher CO selectivity of 94%, CO production rate of 23.3 mol g −1 h −1 , single-pass CO 2 conversion of 58.6%, and enhanced long-term stability of 8 hours. Our study shows that delivering catalysts within the GDL does not only gain the desired physical protection from GDL skeleton to achieve a superior local microenvironment for more efficient pH-universal eCO 2 RR, but also manifests the pore structures to effectively address gas accumulation and flood issues.
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FUEL
·
2024
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IF 6.7
Wang Xiangyu,Liu Chenwei,Nie Jiacheng,Zhou Chenru,Huang Chenmei,Liu Long,Li Mingzhong
CO 2 foam (CF) flooding is a widely adopted enhanced oil recovery (EOR) technique for later stage water flooding reservoirs. However, inadequate mixing of CO 2 and foaming agents often results in uneven and unstable foam, limiting its efficiency. To address this limitation, a novel CO 2 aerosol foam system (CAFS) generated with a custom-designed aerosol foam generator was developed for systematically evaluating CAFS performance following water flooding, with a focus on gas–liquid ratio, pre-injection volume, and solution concentration through core flooding experiments and visualized microscopic flooding experiments. Core flooding experiments show that CAFS achieved an ultimate recovery factor of 62.43 % and reduced water cut by up to 32.51 %, representing improvements over conventional CF by 10.45 % and 20.57 %, respectively. This improvement is attributed to changing rock wettability of nanofluid addition and the high resistance coefficient of aerosol foam. The visualized microscopic flooding experiments further reveal that CAFS produces more uniform and stable foam, enhancing sweep efficiency through mechanisms such as trapping effects, Jamin effects, and pore-throat occupation. Moreover, the emulsification of SDS solution and dissolution viscosity-reducing of CO 2 further improve oil displacement efficiency. Collectively, these findings demonstrate that CAFS outperforms conventional CF flooding and has broad application potential in oilfield development.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Zikang Qin,Yulei Ma,Wentao Du,Jing Wei,Jia Song,Xinyue Fan,Lu Yao,Lin Yang,Yuanfa Zhuang,Wenju Jiang,Zhongde Dai
Amine-functionalized Metal-Organic Frameworks (MOFs) stand out as highly promising materials in membrane separation technology. Nevertheless, the incorporation of amine-functionalized additives may lead to uncontrollable alterations in MOF morphology. Two intact blade-like MOFs (PEI (Polyethylenimine)-ZIF-L and PAMAM (Polyamidoamine)-ZIF-L) were successfully synthesized by controlling the conditions and then introduced into Pebax 2533 to fabricate Mixed Matrix Membranes (MMMs). Hydrogen bonding and other interactions with Pebax can be formed by PEI-ZIF-L and PAMAM-ZIF-L to enhance interfacial compatibility. Simultaneously, a reversible reaction with CO 2 molecules can be undergone by the amine groups, resulting in facilitated transport in MMMs. The CO 2 separation performance of the MMMs is enhanced by this process, with the facilitation being more pronounced under humid conditions. Under humid conditions, the CO 2 permeabilities of Pebax-PEI-ZIF-L (2 wt%) and Pebax-PAMAM-ZIF-L (2 wt%) MMMs were 639.4 Barrer and 702.7 Barrer, respectively, while the CO 2 /N 2 selectivities were 26.68 and 24.35, respectively. Both permeability and selectivity exhibited a significant increase of 200% and 130%, respectively, compared to pure Pebax. Furthermore, the MMMs demonstrated excellent long-term stability during 72 h of continuous operation in a humid environment, showcasing significant potential for industrial applications, particularly in humid flue gas carbon capture.
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FUEL
·
2024
·
IF 6.7
Shaoliang Zhu,Bingtao Zhao,Yaxin Su
High-efficiency and cost-effective adsorbents are crucial to dry capture of carbon dioxide (CO 2 ). The polyethyleneimine (PEI) was co-impregnated with tetraethylenepentamine (TEPA) on γ-alumina (Al 2 O 3 ) to synthesize the adsorbent and enhance the capture process. The influence of amine loading and operating parameters on CO 2 adsorption was investigated, and the process parameters were modeled. The results depict that the optimal loading is 50 % when functionalized either PEI or TEPA individually, which is 3.7 and 4.6 times higher than γ–Al 2 O 3 . The CO 2 capacity of γ–Al 2 O 3 functionalized with multiple amines (30 %PEI+20 %TEPA) is 2.65 mmol/g, due to the synergies of the two amines to increase the chance of CO 2 binding to the sites. Regeneration performance illustrates that the adsorbent remains at 90.2 % of the initial capacity after seven tests. The maximal capacity of 2.70 mmol/g occurs at 70 °C. Modeling results indicate the kinetics can be evaluated by the Avrami model (R 2 > 0.990) with the activation energy of 5.65 kJ/mol. The process is controlled by physical–chemical adsorption, influenced by intraparticle diffusion, as described by the deactivation model. Finally, a comparison and assessment were conducted for their techno-economic performances, and the pathway to applications was also proposed in engineering practice.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Mingrui Wang,Guanghui Zhang,Jie Zhu,Wenhui Li,Jianyang Wang,Kai Bian,Yi Liu,Fanshu Ding,Chunshan Song,Xinwen Guo
Unraveling the correlation between the structure of the active sites and the reaction pathway is of utmost importance to designing selective catalysts for efficient conversion of greenhouse gas CO 2 . In this contribution, the tunable selectivity of CO 2 hydrogenation to CO or CH 4 is achieved in response to the regulation of valance state of active cobalt species. We combined multiple in situ spectroscopic characterizations to show that the small CoO particles highly dispersed in the mesopores and interacted with SBA-15 support prefer to keep the oxidized state (+2). These CoO species is stable in bulk and the surface is partially reduced under the reactive conditions. More CoO sites exposed in this catalyst lead to the higher performance of reverse water gas shift reaction, whereas more metallic cobalt sites derived from the large CoO particles on regular SiO 2 mainly promote CO 2 methanation. In situ FT-IR experiments demonstrated that adsorbed formate dominates on CoO and serves as the key intermediate for the formation of CO, while the adsorbed carboxylate intermediate observed on Co 0 site is dissociated into adsorbed CO and then further hydrogenated to CH 4 . Stronger CO and H 2 adsorption and activation on Co 0 sites lead to the high CH 4 selectivity, whereas weakly bonded CO prefers to desorb from CoO site, resulting in the high CO selectivity. This work discloses the tunable selectivity and offers an opportunity for rational design of efficient cobalt catalysts aiming for selective CO 2 hydrogenation.
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CHEMICAL ENGINEERING JOURNAL
·
2022
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IF 16.744
Jiadong Li,Feng Wei,Ziyuan Xiu,Xiaojun Han
InVO 4 possesses great potential in photocatalytic CO 2 conversion. It is still highly desired to develop efficient strategies of photocatalyst fabrication to prevent its attenuated activity caused by the rapid recombination of photogenerated electron-hole. Herein, a direct Z-scheme heterojunction of Bi 2 WO 6 /InVO 4 nanosheets is constructed via two-step hydrothermal synthesis. The Bi 2 WO 6 /InVO 4 composite exhibits a superior photocatalytic performance toward CO 2 reduction into CO and CH 4 under visible light irradiation. The CO evolution rate reaches up to 17.97 μmol g −1 h −1 , while the CH 4 production rate is 1.13 μmol g −1 h −1 , which are higher than those catalyzed by bare InVO 4 and bare Bi 2 WO 6 . Based on the photoelectrochemical results, hydroxyl radical test, Scanning Kelvin Probe (SKP) and electron spin resonance (ESR) investigation, the enhanced activity of CO 2 reduction can be attributed to a Z-scheme electron transfer at the interface to promote spatial charge separation, which effectively preserves the reduction ability of photoelectron on the conduction band of InVO 4 for CO 2 conversion.
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ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Haitao Shi,Rong Cao,Haijun Zhang,Jiajia Yang,Yanlin Fu,Jiping Chen
Solid amine adsorbents represent a promising class of CO 2 sorbents, but their amine efficiency is limited by the inaccessibility of peripheral amines. The surface of mesocellular silica foam (MCF) is functionalized with the mixture of short-chain 3-Glycidyloxypropyl) triethoxysilane (GPTES) and long-chain Octadecyltrimethoxysilane (OTMS), forming pocket structures on the support surface, thereby exposing more amine sites and enhancing the amine efficiency of polyethylenimine (PEI). The resulting adsorbent demonstrates a high CO 2 adsorption capacity (5.02 mmol g −1 at 50 °C, 10 vol.% CO 2 , and 50%RH), high amine efficiency (0.43 at the dry condition), outstanding cyclic stability (0.5% performance decline per cycle under the conditions of dry CO 2 regeneration), and fast adsorption kinetics (15 min for adsorption saturation at 50 °C). First-principles calculations and CO 2 temperature-programmed desorption (TPD) experiments demonstrate that the introduction of GPTES and OTMS is beneficial to decreasing adsorption energy and forming paired carbamic acid states and ammonium carbamate states.
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