ACS Applied Energy Materials
·
2024
·
IF 5.4
Yue Yang,Nanhui Li,Jianghao Wang,Wei Zhao,Hao Bin Wu
Gas diffusion electrodes (GDEs) show great potential to improve the current densities of the industrial electrochemical carbon dioxide reduction reaction (eCO2RR). The triple-phase boundary (TPB) in GDEs is the key for promoted reaction kinetics, yet such a reaction interface typically suffers from rapid degradation due to electrolyte flooding and salt precipitation. Herein, we demonstrate that a GDE modified with liquid perfluorocarbon (PFC) would notably prolong the lifespan of the GDE with a Bi catalyst in flow-cell electrolyzers. PFC with superhydrophobicity and high CO2 solubility would construct a liquid–solid–liquid reaction interface that prevents the intrusion of electrolytes into the microporous layer (MPL) without hampering the mass transport of CO2. Our work demonstrates an effective strategy to construct a robust and efficient electrochemical reaction interface for the eCO2RR with improved stability for potential industrial applications.
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DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 5
·1989-1998
·
IF 3.5
Yanshu Liu,Guanyun Zhang,Dexin Wang,Guanjie Chen,Fangfang Gao,Chen-Ho Tung,Yifeng Wang
A cryptand-like Ti-coordination compound, namely Ti12Cs, comprising two Ti6-salicylate cages and hosting two Cs+ ions, was synthesized by the solvothermal method. It exhibits strong visible-light absorption with an absorption band edge of 652 nm, attributed to the electron transition from salicylate ligands to Ti ions. Electrochemical impedance, visible-light transient photocurrent response, and photoluminescence spectra confirm that Ti12Cs has excellent visible-light response and charge-separation properties. Ti12Cs can be used as a heterogeneous and recyclable photocatalyst for CO2/epoxide cycloaddition, with high utilization efficiency of visible-light under mild conditions. The mechanism investigation points to a synergistic effect of photocatalysis and Lewis acid catalysis.
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JOURNAL OF MOLECULAR LIQUIDS
·
2024
·
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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SEPARATION AND PURIFICATION TECHNOLOGY
·
2017
·
IF 3.359
Yiming Zhang,Huixian Wang,Yatao Zhang,Xiaoxu Ding,Jindun Liu
Montmorillonite (MMT) and Mg-Al hydrotalcite (HT) nanosheets were prepared via vigorous agitation and ultrasonic, respectively. In order to increase the permeability of CO 2 , poly (PEA-MMT-TMC)/PS and poly (PEA-HT-TMC)/PS composite membranes were prepared via interfacial polymerization by adding the dimensional (2D) inorganic nanosheets (MMT and HT) into the aqueous phase of PEA. And in consequence, the poly (PEA-MMT-TMC)/PS composite membrane showed CO 2 permeability of 15.87 barrer and the CO 2 /N 2 selectivity of 37 at 1.0 bar when the MMT concentration was 0.068 wt%. The poly (PEA-HT-TMC)/PS composite membrane also showed CO 2 permeability of 15.3 barrer and the CO 2 /N 2 selectivity of 40 at 1.0 bar when the HT concentration was 0.25 wt%. Compared with the controlled membrane (CO 2 permeability: 6.9 barrer, CO 2 /N 2 selectivity: 103), the CO 2 permeability increased after incorporating the inorganic nanosheets into the membranes and maintained the pretty CO 2 /N 2 selectivity. The addition of exfoliated MMT and HT could facilitate the gas permeation to improve the gas separation performance of the composite membranes. Also, the combination of inorganic nanosheets with organic membrane has a great potential application in the gas separation.
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ISIJ INTERNATIONAL
·
2017
·Vol. 57
·期 1
·62-67
·
IF 1.11
Zijian Su,Yuanbo Zhang,Yingming Chen,Guanghui Li,Tao Jiang
A considerable amount of works were focused on the formation mechanism of calcium ferrite phases during the iron ore sintering process, especially under various O2 content atmospheres at temperatures higher than 1100°C. But little attention has been paid on reactions between CaO and iron oxides in CO–CO2 atmospheres at lower temperatures. In this study, the solid state reaction mechanisms between CaO and Fe3O4 under CO–CO2 atmospheres at 800°C–1100°C were revealed by using XRD, VSM, etc. The results indicated that Ca2Fe2O5 was easily formed under 5–50 vol% CO/(CO+CO2) atmosphere above 850°C via the reaction of 6CaO + 2Fe3O4 +CO2 = 3Ca2Fe2O5 + CO and the reaction would be promoted with increasing the roasting temperature. In the CO–CO2 atmosphere, Fe3O4 is easily oxidized to Fe2O3 in the presence of CaO because CO2 components act as oxidative medium for the oxidation of Fe2+ to Fe3+.
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ChemPlusChem
·
2024
·
IF 3
Hongguang Liang,Xiaoyun Li,Junwei Wang,Qifeng Li,Yuelan Feng,Maoqing Kang,Yingan Zhang
Graphical The efficient utilization of CO 2 into cyclic carbonate as electrolytes and medical intermediates with 100 % atom efficiency is interesting. Employed as catalyst, carbon nitride family with different polymerization degree and pore structure exhibits excellent potential in the cycloaddition reaction. The active amino and hydroxyl groups in the catalyst form interaction with CO 2 molecules and epoxy groups, respectively, generating the synergistic effect to promote the reaction. For the efficient utilization of CO 2 into valuable product, the attractive carbon nitride catalysts have been widely studied. In this work, heptazine-related materials with varying degree of polymerization were designed by an intrinsically modification strategy and employed in the cycloaddition of CO 2 with the bisepoxide 1, 4-butanediol diglycidyl ether (BDODGE). We initially figured out that the sample prepared at 450 °C contained more melem hydrate, exhibiting the best performance. The epoxides conversion and corresponding cyclic carbonates selectivity could achieve 93.1 % and 99.3 % at 140 °C for 20 h without any cocatalyst and solvent, respectively. Results of the catalytic tests suggested that the high catalytic activity was dependent on big size porous structure and the synergetic effect of active amino groups and −OH groups. The role of water in maintaining the specific structure and providing active site has been proved. Moreover, the CN-450-W catalyst exhibited outstanding recycling stability. And finally, a plausible reaction mechanism was proposed.
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Molecular Catalysis
·
2024
·
IF 3.9
Yi He,Peng Bai,Shibo Yuan,Jiafa Chen,Yicheng Zhao,Yongdan Li
N -formylation of amines with CO 2 is a promising approach to high-efficient utilization of CO 2 as C1 feedstock, while conventional thermocatalytic processes suffer from harsh reaction condition and intense energy consumption. In this work, photocatalytic N -formylation of amines with CO 2 is achieved at room temperature over Pt-Bi/CeO 2− x composite catalyst. The Pt-Bi bimetallic sites increase the concentration of surface oxygen vacancies. Furthermore, the synergistic effects of Pt and Bi improve the light absorption capacity, reduce the band gap energy of the photocatalyst and promote the separation of photoinduced charge carriers. Using PhSiH 3 as the reducing agent, the conversion of N -methylaniline reaches 100 % after 3 h irradiation in N, N -dimethylformamide solvent with a N- methylformanilide selectivity of 90.8 %. The composite photocatalyst shows promising cycling stability and universality.
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Catalysis Science & Technology
·
2024
·
IF 4.4
Sisi Lin,Xinkui Wang,Xiaoyu Liang,Xinxin Zhang,Min Wang
Photocatalytic reduction of CO2 to high value-added chemicals and fuels has received widespread attention. However, the higher thermodynamic stability of CO2 greatly limits its conversion efficiency. Frustrated Lewis pairs (FLPs) have been well-established to be very effective in CO2 activation. In this work, we prepared ZnIn2S4–AlOOH (ZIS–AlOOH) composites for visible-light-driven CO2 reduction. The Lewis basic OHv sites on the AlOOH surface (one H removed from OH) and an adjacent Lewis acidic unsaturated Al site (Al3+unsatur.) form the FLPs. The composite structure facilitated light absorption, CO2 adsorption activation, and separation of photogenerated carriers, thus improving the CO2 photoreduction activity (CO generation rate of 510.3 μmol g−1 h−1), and suppressing hydrogen evolution with the CO/H2 ratio increasing from 0.38 for ZnIn2S4 (ZIS) to 0.84 for ZIS–AlOOH. This work elucidates a rational strategy for the construction of efficient photocatalysts and provides insight into the mechanism of the photocatalytic CO2 reduction reaction.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Keming Zhang,Sihui Li,Xiaohe Tian,Rui Zhang,Xiaoting Feng,Qingnan Wang,Yanting Tang,Chenlu Liu,Hongxia Gao,Shaofei Wang
Metal-organic framework (MOF) membranes demonstrate significant potential for industrial gas separations, yet fabricating vertically aligned two-dimensional (2D) MOF membranes on polymer substrates remains a considerable challenge due to the weak adhesion and difficulty in achieving precise alignment. This study presents a one-step method for the rapid synthesis of vertically aligned ZIF-L membranes, using a polydopamine (PDA)-assisted approach. This method enables the rapid formation of homogenous, thin but defect-free membranes on polymer substrates within 5 min, drastically reducing the preparation time by over 200 times. The vertically aligned ZIF-L membranes, characterized by the interlayer galleries facing the gas mixtures, exhibit an excellent CO 2 permeance exceeding 1200 GPU and a CO 2 /N 2 selectivity of 14.5. The versatility of this approach allows for its application on various flat-sheet or even hollow fiber supports. Our findings highlight the potential of PDA-assisted synthesis for efficient, scalable preparation of high-performance MOF membranes for industrial gas separations.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Liwei Sun,Lipeng Wang,Meilin Yin,Shaokun Tang
Direct utilization of low-concentration CO 2 is of importance to mitigate the global warming and reduce energy consumption. Herein, a new bi-functional ionic liquid-grafted material was fabricated for CO 2 /N 2 selectivity and diluted CO 2 cycloaddition reaction. Following the preparation of 1-carboxymethyl-3-methoxy ethyl-imidazolium chloride ([CmMOEim]Cl) containing carboxyl and ether group, MIL-53(Al) was used for directly chemical grafting of the ionic liquid to obtain [CmMOEim]Cl@MIL-53(Al). CO 2 capture capacity of [CmMOEim]Cl@MIL-53(Al) reached up to 70 cm 3 CO 2 /g sorbent at 25 °C and 0.1 MPa, which was higher than that of two individual components. Cyclopropyl carbonate of 97 % yield was obtained at 110 °C, 3 MPa of initial 50 vol% CO 2 /N 2 pressure and 4 h with 2.4 wt% [CmMOEim]Cl@MIL-53(Al)-0.4 under solventless and co-catalyst-free condition. Various terminal cyclocarbonates were synthesized with above 90 % yield. In addition, the heterogeneous catalyst was separated from reaction system by simple centrifugation and the yield of cyclopropyl carbonate was higher than 90 % after 12 cycles owing to the chemical grafting of [CmMOEim]Cl on MIL-53(Al).
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-14
·
IF 14.7
Yang Haozhou,Guo Na,Xi Shibo,Wu Yao,Yao Bingqing,He Qian,Zhang Chun,Wang Lei
Cobalt phthalocyanine immobilized on carbon nanotube has demonstrated appreciable selectivity and activity for methanol synthesis in electrocatalytic CO 2 /CO reduction. However, discrepancies in methanol production selectivity and activity between CO 2 and CO reduction have been observed, leading to inconclusive mechanisms for methanol production in this system. Here, we discover that the interaction between cobalt phthalocyanine molecules and defects on carbon nanotube substrate plays a key role in methanol production during CO 2 /CO electroreduction. Through detailed operando X-ray absorption and infrared spectroscopies, we find that upon application of cathodic potential, this interaction induces the transformation of the planar CoN 4 center in cobalt phthalocyanine to an out-of-plane distorted configuration. Consequently, this potential induced structural change promotes the transformation of linearly bonded *CO at the CoN 4 center to bridge *CO, thereby facilitating methanol production. Overall, these comprehensive mechanistic investigations and the outstanding performance (methanol partial current density over 150 mA cm −2 ) provide valuable insights in guiding the activity and selectivity of immobilized cobalt phthalocyanine for methanol production in CO 2 /CO reduction.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2025
·
IF 5.4
Hao Yuan,Hanxiang Guo,Zhaosheng Huang,Ping Zhang,Zhe Wang,Chunde Jin
Traditional polyurethane coatings are typically synthesized from non-renewable petrochemical resources, which contradicts modern environmental principles. This paper aims to develop eco-friendly polyurethane wood coatings and enhance coating properties. CO 2 -based polyurethane (PU) was first synthesized by using CO 2 -based polyols instead of petroleum-based polyols and reacting them with isocyanates. The properties of PU coatings such as corrosion resistance, hardness, and adhesion were improved by introducing soybean oil-based polyols (P-ESO) from ring-opening reactions of epoxidized soybean oil (ESO) during the synthesis process. P-ESO-CO 2 -based PU (SPU) wood coatings demonstrated superior tensile strength and adhesion values of 0.77 MPa and 3.66 MPa, respectively, and exhibited a hydrophobicity with a water contact angle of 102°. Hence, SPU holds greater promise and potential for future development in the field of environmentally friendly wood coatings.
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