ACS Sustainable Chemistry & Engineering
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2022
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IF 9.224
Xiaoyan Pei,Zhiyong Li,Huiyong Wang,Qiuju Zhou,Zuodong Liu,Jianji Wang
Surfactant-free microemulsions (SFMEs) have shown great potential in many aspects such as chemical reactions and material preparation. Ionic liquid (IL)-based SFME is a promising member in this family. However, switchable phase separation of nonaqueous IL SFMEs has not been reported up to now although it is of great importance for the separation of products and recycling of the systems. Herein, a new kind of CO2-responsive SFMEs composed of quaternary ammonium IL, dimethyl sulfoxide, and ethyl acetate has been developed. It is worth noting that the microemulsion can be reversibly switched between emulsification and complete phase separation upon alternative CO2 and N2 bubbling at atmospheric pressure. The microstructures and phase behavior of the systems before and after CO2 bubbling have been systematically studied by phase diagrams, electrical conductivity, dynamic light scattering, optical microscopy, and atomic force microscopy, respectively. Mechanism studies verify that the reversible switching is attributed to the generation and restoration of more hydrophilic carbamate salts from the reaction of CO2 with IL anions, which results in poor solubility of ILs in the nonaqueous microemulsions and thus reversible breaking and rebuilding of the microemulsions. Based on this unique phase behavior, the CO2-switchable SFMEs are used as a microreactor for room temperature synthesis of Zn-based metal–organic frameworks, and effective reaction and microemulsion recycling have been achieved. This study may provide a new strategy for the integration of reaction, separation, and recycling procedures to obtain sustainable chemical processes.
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ACS Catalysis
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2022
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IF 13.7
Jianping Sheng,Ye He,Ming Huang,Chaowei Yuan,Shengyao Wang,Fan Dong
Lead (Pb) halide perovskite quantum dots (PQDs) are promising candidates for the photochemical reduction of CO2. However, the intrinsically weak adsorption and activation toward inert CO2 molecules have seriously hindered their practical application. This study reports alternative Cs2CuBr4 PQDs for gas–solid phase photocatalytic CO2 reduction under simulated solar irradiation. Cs2CuBr4 PQDs exhibited CO2 photoreduction performance with CH4 and CO yields of 74.81 and 148.98 μmol g–1, respectively. In situ diffuse reflectance infrared Fourier transform spectra and density functional theory calculations cooperatively revealed the synergistic strengthening of microelectronic polarization in Cs2CuBr4 PQDs induced by surface-frustrated Lewis pair-like properties and intrinsic Cu d-band properties facilitated robust CO2 adsorption and activation. This study demonstrated the potential of Cs2CuBr4 PQDs as a platform for highly efficient CO2 photoreduction and provided a distinct concept for CO2 adsorption and activation based on the catalytic mechanism of Cu-based PQDs.
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Coatings
·
2022
·Vol. 12
·期 2
·233
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IF 3.236
Shiyuan Liu,Botao Hu,Junkai Zhao,Wenjun Jiang,Deqiang Feng,Ce Zhang,Wei Yao
The electrocatalytic CO2reduction reaction (CO2RR) into hydrocarbon products is one of the most promising approaches for CO2utilization in modern society. However, the application of CO2RR requires optimizing state-of-the-art catalysts as well as elucidating the catalytic interface formation mechanism. In this study, a flower-like nano-structured Bi catalyst is prepared by a facile pulse current electrodeposition method wherein the morphologies could be accurately controlled. Interestingly, nano-structured Bi is inclined to generate Bi2O2CO3in the air and form a stable Bi2O2CO3@Bi interface, which could enhance the CO2adsorption and conversion. In-situ Raman spectroscopy analysis also proves the existence of Bi2O2CO3on the electrode surface. In a practical CO2reduction test by a flow-cell reactor, the Bi2O2CO3@Bi electrode delivers a high faradaic efficiency of the CO2to formate/formic acid (~90%) at −1.07 V vs. reversible hydrogen electrode (RHE) with no obvious decay during more than a 10 h continuous test. The introducing surface Bi2O2CO3in nano-structured Bi supports a promising strategy as well as facile access to prepare improved CO2RR electrocatalysts.Keywords:CO2reduction;bismuth;Bi2O2CO3;interface;formic acid
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ACS Sustainable Chemistry & Engineering
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2022
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IF 9.224
Meisi Chen,Mengjia Li,Lin Zhang,Xiemin Liu,Feng Zhang,Youting Wu
Amino acid ionic liquids (AAILs) exhibit prominent merits for CO2 capture including biocompatibility and good stability, but they still suffer from several demerits, such as high viscosity and low molecular utilization. Therefore, it is critical to construct proper systems that can address these problems to enhance CO2 absorption of AAILs. In this work, three types of AAIL absorbent systems, DMEE (2-[2-(dimethylamino) ethoxy] ethanol)–AAIL, H2O–AAIL, and EG (ethylene glycol)–AAIL, are prepared with six AAILs that have different amino acids. The absorption performance of these absorbents is characterized to investigate the reinforcing effects of the additives on the absorption properties of AAILs. With temperatures ranging from 293 to 313 K, the CO2 capture studies on the binary systems reveal that AAILs present better absorption efficiency when their concentrations are 40 or 50 wt %. Based on the zwitterion reaction mechanism model and a thermodynamic model, the interactions of AAILs with H2O, DMEE, and EG systems for absorbing CO2 are discussed, respectively. The results obtained in this work indicate that AAIL–DMEE systems are promising candidates for CO2 capture since the interaction between AAILs and DMEE increases the capacity of AAILs and promotes kinetics.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Wanfeng Yang,Conghui Si,Yong Zhao,Qingru Wei,Guixing Jia,Guanhua Cheng,Jingyu Qin,Zhonghua Zhang
Antimony (Sb) as a low-toxic and cost-effective metal is a promising material to catalyse CO 2 electroreduction to formate with practical viability. However, monometallic Sb suffers from intrinsically low catalytic activity and the competing hydrogen evolution. Here, we report nanoporous Sb-Bi alloys for substantially improving the catalytic activity of Sb and suppressing hydrogen evolution. The optimal Sb-Bi alloy exhibits a maximum Faradaic efficiency of 95.8 % toward formate production, surpassing the 11.6 % of monometallic Sb counterpart. Operating the catalyst in the flow cell demonstrates a formate partial current density of 734 mA cm −2 and cathodic energy efficiency of 59 % at a moderate overpotential of 800 mV, representing a record formate-production performance so far. Experimental and theoretical studies indicate that the Sb-Bi interactions activate Sb sites to selectively stabilize *OCHO intermediates, facilitating CO 2 -to-formate conversion. This work offers insights in manipulating bimetallic interactions to transform inert materials into active catalysts for efficient electrocatalysis.
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Nature Communications
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2022
·Vol. 13
·期 1
·1-8
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IF 17.694
Mu Shijia,Lu Honglei,Wu Qianbao,Li Lei,Zhao Ruijuan,Long Chang,Cui Chunhua
Cu δ+ sites on the surface of oxide-derived copper (OD-Cu) are of vital importance in electrochemical CO 2 reduction reaction (CO 2 RR). However, the underlying reason for the dynamically existing Cu δ+ species, although thermodynamically unstable under reductive CO 2 RR conditions, remains uncovered. Here, by using electron paramagnetic resonance, we identify the highly oxidative hydroxyl radicals (OH • ) formed at room temperature in HCO 3 - solutions. In combination with in situ Raman spectroscopy, secondary ion mass spectrometry, and isotope-labelling, we demonstrate a dynamic reduction/reoxidation behavior at the surface of OD-Cu and reveal that the fast oxygen exchange between HCO 3 - and H 2 O provides oxygen sources for the formation of OH • radicals. In addition, their continuous generations can cause spontaneous oxidation of Cu electrodes and produce surface CuO x species. Significantly, this work suggests that there is a “seesaw-effect” between the cathodic reduction and the OH • -induced reoxidation, determining the chemical state and content of Cu δ+ species in CO 2 RR. This insight is supposed to thrust an understanding of the crucial role of electrolytes in CO 2 RR.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2022
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IF 3.898
Ye Yuan,Yurui Pan,Menglong Sheng,Guangyu Xing,Ming Wang,Jixiao Wang,Zhi Wang
Membrane technology features inspiring excellence from numerous separation technologies for CO 2 capture from post-combustion gas. Polyvinylamine (PVAm)-based facilitated transport membranes show significantly high separation performance, which has been proven promising for industrial scale-up. However, commercialized PVAm with low molecular weight and excessive crystallinity is not available to prepare high-performance membranes. Herein, the synthesis process of PVAm was optimized by regulating polymerization and acidic hydrolytic conditions. The membranes based on PVAm with a molecular weight of 154 kDa and crystallinity of 11.37% display high CO 2 permeance of 726 GPU and CO 2 /N 2 selectivity of 55 at a feed gas pressure of 0.50 MPa. Furthermore, we established a PVAm synthesis reactor with an annual PVAm solution (1%(mass)) capacity of over 7000 kg and realized the scaled-up manufacture of both PVAm and composite membranes.
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Journal of CO2 Utilization
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2022
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IF 8.321
Jinsong Shi,Hongmin Cui,Jianguo Xu,Nanfu Yan,Shengyong You
Influences of porous carbon’s physicochemical properties on CO 2 adsorption vary with CO 2 pressure. The clarification of such complicated influences will undoubtedly be beneficial to the design and synthesis of carbonaceous adsorbents. To this end, in the current work we synthesized a series of N-doped hierarchically ordered micro-mesoporous carbons (NHOMCs). Ordered mesoporous polymer was synthesized with a solvent-free method using F127 as the soft template. After removing F127, the polymer was activated with KHCO 3 in the presence of urea at 700–800 °C. The obtained NHOMCs inherited the ordered structure of the polymer, and exhibited high surface area and nitrogen content. Synergistic effects of urea and KHCO 3 on nitrogen content and textural properties were discussed and revealed. At 25 °C, high CO 2 uptakes of 4.02 mmol/g (1 bar) and 15.42 mmol/g (20 bar) were achieved by the NHOMCs. We then systematically investigated the correlation between CO 2 uptake and physicochemical properties. The decisive factors of CO 2 uptakes at different pressures (1 bar, 5 bar, 10 bar, 20 bar) were analyzed. We believe the current work will provide helpful insights into the research of porous carbons for CO 2 adsorption.
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CARBOHYDRATE POLYMERS
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2022
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IF 10.723
Jinqiang Sun,Mengge Shang,Minna Zhang,Shimo Yu,Zhipeng Yuan,Xibin Yi,Serguei Filatov,Jing Zhang
Biomass aerogels are attractive in various applications owing to their inherent advantages of renewability, biodegradability and eco-friendly. Herein, a novel composite aerogel of konjac glucomannan (KGM)/TEMPO-oxidized cellulose nanofibers (TOCNF)@HKUST-1 (KTA@HKUST-1) is prepared through a facile vacuum impregnation method combined with the directional freeze-drying process, which using KGM and TOCNF as raw materials. The structural analyses disclose that the KTA@HKUST-1 has a hierarchical porosity, in which HKUST-1 can provide micropores for adsorption, while the meso -/macropores from KTA act as high-speed channels to improve diffusion and mass transfer rate to transport CO 2 components into the micropores of HKUST-1. The experiment results of KTA@HKUST-1-10 (KTA@H10) show that the CO 2 adsorption capacity can reach 3.50 mmol·g −1 at 1 bar and 298 K, and the adsorption capacity retention rate as high as 91.43% after 7 cycles. In addition, the CO 2 /N 2 adsorption selectivity of KTA@H10 can reach 18.42, which has an excellent potential for selective CO 2 adsorption.
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ENVIRONMENTAL RESEARCH
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2022
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IF 8.431
Jinchang Liu,Yaping Li,Xiaoya An,Chenyang Shen,Qiang Xie,Dingcheng Liang
Wasted coal liquefaction residual was used to synthesize activated carbon fibers (ACFs) for CO 2 capture, and the properties of the developed ACFs were optimized by adjusting the activation conditions, including the reaction temperature and soaking time. The yield, element distribution, pore structure, composition, functional group, morphology, and adsorption capacity of the as-synthesized ACFs were characterized by various apparatuses. In addition, static and dynamic adsorption experiments were conducted to investigate the adsorption capacity of CO 2 in flue gas . The results revealed that the synthesized ACFs are mainly composed of carbon, accounting for more than 90% of the total elements. The specific surface area, pore volume, and pore width distribution of the prepared ACFs were optimized by changing the activation conditions, and ACFs with a specific surface area higher than 1400 m 2 /g were successfully developed by activation at 950 for 3 h. The amount of micropores occupied more than 90% of the total pore volume. The pore width distribution dominated by micropores is beneficial for CO2 adsorption since the diameter of CO 2 is 0.33 nm. From FTIR and XPS analysis, it is found that the main structure of ACFs is a carbon skeleton composed of polycyclic aromatic hydrocarbons with a small number of oxygen-containing functional groups. The adsorption isotherm of ACFs for CO 2 conforms to the Langmuir model, indicating that the adsorption process of CO 2 by ACFs can be attributed to monolayer adsorption. Both the specific surface area and oxygen-containing functional groups have crucial effects on the adsorption capacity of CO 2 . The dynamic adsorption experiment determined that ACFs-920-3 had the highest adsorption capacity for CO 2 in flue gas, and adsorption equilibrium was achieved after 7 min of adsorption. The adsorption process of CO 2 in flue gas by the as-synthesized ACFs fits well with the pseudosecond kinetic model. The CO 2 adsorption capacity of the obtained ACFs remained unchanged after 10 cycles of adsorption. A high-value-added route for synthesizing ACFs for CO 2 capture using CLR as a raw material was developed.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Xiaoyi Gao,Xin Li,Siyi Cheng,Bihong Lv,Guohua Jing,Zuoming Zhou
The main issues in the application of biphasic amine absorbent include the inconvenient separation of the liquid–liquid biphase and the clogging that is associated with the solid–liquid mixture. A novel solid–liquid ‘phase controllable’ biphasic amine absorbent was therefore developed, in which the phase separation occurred only when the absorbent was near saturation. The absorbent, composed of triethylene tetramine (TETA), 2-amino-2-methyl-1-propanol (AMP), and N-methylformamide (NMF), turned into solid–liquid biphase under CO 2 loading of 0.85 mol mol −1 , which is close to saturation (0.92 mol mol −1 ). The solid phase comprised white powder that accounted for only 42 % of the total volume while absorbing 91 % of the total load. Turbidity and particle size tests showed that the phase separation was self-aggregating. The mechanisms of absorption and regulation were obtained using 13 C NMR and molecular simulation. During the absorption, CO 2 first combined with TETA to generate TETAH + CO 2 – /TETACO 2 – through the zwitterion mechanism, and then combined with AMP to generate AMPCO 2 – because of the lower reaction activity between CO 2 and AMP. The TETA-carbamate was found to greatly weakened the strength of the hydrogen bonds and the van der Waals forces between AMPH + and AMPCO 2 – , increasing the solubility of the intermediate products, and therefore achieved the purpose of controlling the phases separation inherent in the reaction.
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CHEMICAL ENGINEERING JOURNAL
·
2021
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IF 13.273
HaiyanYang,Xinzhong Wang,Jun Liu,Wanzhen Liu,Yue Gong,Yankun Sun
Solid amine materials are promising adsorbents for CO 2 capture from biogas , flue gas and other similar gas mixture. Here, tetraethylenepentamine (TEPA)-impregnated porous polymeric resin (ADS-17) with very high CO 2 adsorption capacity was successfully prepared. Its CO 2 separation performance from simulated biogas was investigated by breakthrough experiments. And the influence of parameters such as TEPA loading, adsorption temperature and flow rate on the adsorption behaviours were studied in detail. The optimal TEPA loading was 40 wt% (ADS-17–40%TEPA) and the CO 2 adsorption capacity of this adsorbent reached the optimal value (ca. 264.2 mg▪g −1 ) at the flow rate of 200 mL▪min −1 . The CO 2 adsorption capacity of ADS-17–40%TEPA had no pronounced change from 25 °C to 70 °C, but it decreased obviously when the adsorbent was heated to 90 °C. At 100 °C, the adsorption capacity became negligible. According to detailed characterization, it was inferred that the pores of ADS-17–40%TEPA in the range of 13–115 nm were probably responsible for CO 2 diffusion. In addition, ADS-17–40%TEPA possessed good reversibility and the CO 2 adsorption capacity was nearly stable after two adsorption–desorption cycles. ADS-17–40%TEPA with high and fast CO 2 adsorption exhibits a very promising application in CO 2 separation from biogas.
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