JOURNAL OF MOLECULAR LIQUIDS
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2024
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IF 5.3
Xupeng Fu,Yuting Wang,Xiaoyu Wang,Liming Chai,Enna Wang,Zhaojun Wu,Jianbin Zhang
Density ( ρ ) and viscosity ( η ) data of the polyethylene glycol 300 (PEG300) and hydroxyethyl ethylenediamine (AEEA) mixed solution were measured at P = 1005 hPa and T = (298.15–318.15) K. Following these data, Jouyban-Acree model exhibited superior correlation to density in the mixed system compared to nonlinear least square method, while the McAllister four-body equation yielded a better fitting for kinematic viscosity than other models. Utilizing ρ and η data, the Redlich-Kister equation was employed for the systematic computation and analysis of excess molar volume ( V m E ), excess activation Gibbs free energy ( Δ G *E ), partial molar volumes ( V 1 ¯ and V 2 ¯ ), and viscosity deviation ( Δη ) in the PEG300 (1) + AEEA (2) mixed solution. These excess properties indicated the advantageous nature of intermolecular binding in the PEG300 (1) + AEEA (2) mixed solution, further substantiated on the basis of various spectroscopic characterizations. Finally, under conditions of CO 2 flow rate at 150 mL/min, absorption experiments were conducted for 4 h in the PEG300 (1) + AEEA (2) mixed solution, pure AEEA, and pure PEG300, which indicated that the mixed solution exhibited the highest CO 2 absorption capacity of 0.95 mol CO 2 /mol AEEA, demonstrating superior absorption performance compared to the two pure substances.
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ACS Applied Polymer Materials
·
2024
·
IF 4.4
Ziru Yu,Zhenghua Guo,Liang Yu,Xiao Feng,Bo Wang
Various metal–organic framework (MOF)-based porous nanomaterials have been adopted to fabricate mixed matrix membranes (MMMs) aiming at breaking through the Robeson upper bound of individual polymer membranes for gas separation. However, the insufficient compatibility between the polymeric matrix and MOF nanofillers limits the further improvement of their gas separation performance. To overcome this challenge, we constructed relatively ideal Pebax/PEG/NH2–UiO-66 mixed matrix membranes inspired by θ solvent theory of polymer solutions. Polyethylene glycol (PEG) molecules were introduced to selectively swell the polar poly(tetramethylene oxide) (PTMO) domains of the Pebax matrix via hydrophobic–hydrophilic interactions and in turn furnished dispersed “nests” for NH2–UiO-66 nanofillers with polar nature to reduce the interparticle agglomeration (PEG nesting effect). MOF nanofillers tended to be relatively undisturbed, in which either the rigidity of polymer chains or the pore blocking of MOFs seen in unideal MMMs was restricted. The PEG “nesting effect” proposed herein could bring benefits to further improve the allowed maximum loading capacity of MOF nanofillers as well as adjust the interactions therein and therefore maximize the CO2 separation performance of Pebax/PEG/NH2–UiO-66 MMMs. Compared with individual Pebax membranes, Pebax/PEG/NH2–UiO-66 with a 15 wt % loading of NH2–UiO-66 showed a 73% higher CO2 permeability (210 barrer) and a 220% higher CO2/N2 selectivity (130), which demonstrated the most dramatical increases among Pebax-based MMMs until now and as well significantly exceeded the Robeson upper bound. Therefore, the proposed PEG “nesting effect” for the preparation of θ-type MMMs holds promising potential for membrane-based carbon capture and is possibly extended to the preparation of other MMMs.
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POLYMER BULLETIN
·
2024
·
IF 3.1
Zhang Beibei,Zhang Lihua,Li Jin,Qiang Qi
Carbon emission reduction has been accepted as a common concern all over the world. Currently, CO 2 emission is mainly derived from the consumption of fossil fuels. To solve this issue, there is an urgent need to develop technologies for CO 2 capture. The utilization of membrane technology to remove CO 2 from a mixture gas attracts great interest. In the present work, poly(2-hydroxyethyl methacrylate- co -vinylamine) was synthesized by polymerization ( n -vinyl formamide and 2-hydroxyethyl methacrylate), hydrolysis, and ion exchange. The surface function of graphene oxide was carried out by aerobic self-polymerization of dopamine. The mixed matrix membranes were fabricated by adding the nanofiller (before and after modification) into the polymeric matrix. The membrane properties and its structure were characterized by FTIR, TGA, XRD, and SEM. The effect of nanofiller content and operation conditions on membrane performance was investigated. Results showed that the additions of nanofiller could decrease the crystallization of these membranes and effectively improve gas permeance. Remarkably, for the addition of 2.0 wt% dopamine-modified graphene oxide, the CO 2 permeance of the membrane was increased by 30.9% while achieving a CO 2 /N 2 selectivity of 83.5. The CO 2 permeation for CO 2 /CH 4 was also increased by 16.77%. These were surpassed over the 2008 Robeson’s upper bound. These resultant membranes demonstrated attractive potential for low-pressure post-combustion CO 2 capture. Besides, the stability of longtime tests on membranes was studied, and it was observed that membranes exhibited excellent stabilization with continuously operated for 220 h. The excellent properties of these membranes provide new opportunities for gas separation applications.
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Materials Today Energy
·
2024
·
IF 9
Fei-Feng Mao,Yu-Hua Dong,Yan Zhou,Ming-Shuai Sun,Wei Hui,Duan-jian Tao
Global climate change has driven the scientific community to improve the utilization of a critical C1 resource carbon dioxide (CO 2 ) through carbon capture utilization (CCU) technology. The cycloaddition of CO 2 with epoxides provides perfect atom economy and economic feasibility to produce versatile cyclic carbonates used in various industries. However, the stable nature of CO 2 and epoxides requires highly active catalysts. In this work, the repurpose of nitrogenous waste melamine foams (MF) as high-performance catalysts for the cycloaddition of CO 2 were explored. The pyrolyzed MF were modified with Cu to prepare a series of acid-base bifunctional porous catalysts (MFC-X-Cu). The results demonstrate that the acid-base synergy of the MFC-X-Cu catalysts increases the efficiency of the cycloaddition of various epoxides, yielding target products at 96-99% under mild conditions. Moreover, the characterization results revealed that the superior performance of MFC-X-Cu stems from its hollow structure and acid-base synergy, which are derived from nitrogen species in the repurposed MF and the post-modified copper component. The catalyst maintained consistent catalytic efficiency over five cycles, highlighting its strong recyclability. This work presents an eco-friendly and sustainable approach towards carbon neutrality by utilizing modified waste materials for CO 2 conversion into high-value chemicals.
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LANGMUIR
·
2024
·
IF 3.7
Zhenghao Zhang,Bo Peng,Yupeng Zhang,Jiaxin Xiong,Jingwei Li,Jianwei Liu
A CO2/N2-responsive emulsion provides milder reaction conditions, nontoxicity, and economic feasibility compared to other switchable surfactants. In this study, CO2/N2-responsive pickering emulsions were fabricated by using a compounded dispersion containing SiO2 nanoparticles (NPs) and superamphiphiles as the emulsifying agents. The synergistic effects of the SiO2 NPs and superamphiphiles significantly stabilized the emulsion at all of the tested concentrations and prevented complete phase separation of oil and water. The electrostatic interaction between the SiO2 NPs and superamphiphiles was disrupted after bubbling with CO2 for 30 s, resulting in the breaking of the emulsion. However, the dispersion recovered its interfacial activity after the introduction of N2 and again emulsified the emulsion. This reversible switching behavior was validated through three consecutive cycles of bubbling CO2/N2. The protonation and deprotonation of the SiO2 NPs and superamphiphiles in response to CO2/N2 facilitated reversible assembly and disassembly, which enabled the switching of the emulsions between inactive and active forms. The novel highly stable Pickering emulsions demonstrated rapid demulsification and emulsification in response to CO2/N2 and are promising for a wide range of applications.
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PubMed
高影响因子
CARBON
·
2024
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IF 10.5
Shide Wu,Yifei Zhang,Dan Ping,Yapeng Li,Wan Li,Shuqing Liu,Di Wu,Shiwen Wang,Xuzhao Yang,Guanglu Han,Dongjie Guo,Shaoming Fang
Developing efficient electrocatalysts for CO 2 electroreduction to syngas with a specific H 2 /CO ratio over a wide potential window is desperately required but still challenging. In this work, a series of dual-site catalysts composed of iron phthalocyanine (FePc) and ∼18 nm Cobalt nanoparticles (Co NPs) anchored on N-doped carbon matrix has been constructed from zeolitic imidazolate framework-67 (ZIF-67). Benefiting from the synergistic effect of FePc and Co NPs, the derived FePc/Co@N–C catalyst shows impressive capability for CO 2 electrolysis to syngas. By varying the pyrolysis temperatures (600–800 °C) of ZIF-67 and the mass ratio of Co@N–C to FePc (1–3), an adjustable H 2 /CO ratio of 2–4 is obtained, and the value can be maintained stable within a potential window of −0.66 to −0.86 V vs . RHE in an H-type cell. Moreover, this electrocatalyst exhibits favorable stability without distinct performance decay. When conducted in a flow cell, an enhanced catalytic activity is demonstrated with an industrial current density (>100 mA cm −2 ) at −0.8 V vs . RHE and a steady H 2 /CO ratio of 2 from −0.4 to −0.6 V vs . RHE. This work provides a promising strategy of designing bifunctional electrocatalysts for syngas generation with stable H 2 /CO ratio across a wide potential range.
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Processes
·
2024
·Vol. 12
·期 9
·1912
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IF 2.8
Bowen Lu,Huiying Sang,Liang Liu,Zhijian Yu,Yaqin Guo,Yongqing Xu
The catalytic applications of micron Cu powder are limited due to its large particle size and small specific surface area. Modifying micro-Cu powder to achieve a high catalytic performance is a challenge in the application of micron copper. In this work, micro-Cu was used to synthesize a CeO2–Cu catalyst, and the phase composition and surface pore structure were analyzed using XRD, BET, etc. The CO2hydrogenation performance of the CeO2–Cu catalyst was analyzed in comparison with CeO2and Cu, and we found that the CeO2–Cu catalyst exhibited a synergistic effect between Cu and cerium, resulting in a much higher hydrogenation performance at 500 °C than CeO2or Cu alone. H2-TPR and TEM characterization revealed that the CeO2–Cu catalyst formed interfacial interactions with a relatively large Ce–Cu interface, where cerium oxide could promote the reduction of CuO and lower the reduction temperature. Additionally, cerium oxide formed a confinement structure for Cu, and the CeO2–Cu catalyst exhibited a higher oxygen vacancy concentration, thereby promoting the CO2hydrogenation performance. Cu–CeO2interaction provides valuable insights into the catalytic application of micron Cu powder.
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ACS Catalysis
·
2024
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IF 11.3
Wenhang Wang,Kaixuan Huo,Yang Wang,Jinghao Xie,Xu Sun,Yingluo He,Meng Li,Jie Liang,Xinhua Gao,Guohui Yang,Simin Lin,Fengliang Cao,Hu Jiang,Mingbo Wu,Noritatsu Tsubaki
Oxygen vacancies (Ov) in reducible metal oxides are the vital active sites for methanol synthesis via a CO2 hydrogenation technology. However, the relationship between the density of Ov and the methanol synthesis performance is still ambiguous, and it still shows a lack of a versatile strategy to precisely tailor the number of Ov. In this study, with In2O3 as a representatively catalytic component, the density functional theory computation confirms that the Ov property, especially Ov density, is pivotal to enhancing methanol selectivity of CO2 hydrogenation by suppressing the undesirable reverse water–gas shift reaction for CO formation, which is attributed to the unique electronic density of In atoms around Ov. To verify the theoretical results, we report a protocol to optimize the concentration of Ov on In2O3 by sequential carbonization and oxidation (SCO) treatments of In-based metal–organic frameworks, during which the consumption of carbon species and the structural reconstruction of the In2O3 crystal regulated the particle size and Ov concentration of In2O3 by varying the oxidation temperature. The In2O3-5 catalyst carbonized and oxidized at 500 °C exhibits good methanol selectivity (72.3%) at a CO2 conversion of 9.9% under 330 °C, 3 MPa, and high space velocity of 12,000 L–1 kgcat–1 h–1. Multiple in situ characterizations clarify that the proposed Ov property regulating the SCO strategy is convenient to boost methanol synthesis by altering the CO2 hydrogenation process to the HCOO* intermediate-dominated pathway. Our work provides the catalyst design strategy and will shed light on the rational design of reducible metal oxide-based catalysts with a controllable Ov density.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Feifei You,Tianhao Zhou,Jiaxin Li,Shihui Huang,Chuntao Chang,Xiaoyu Fan,Hao Zhang,Xiaohong Ma,Dawei Gao,Jian Qi,Danyang Li
Solar energy driving CO 2 reduction is a potential strategy that not only mitigates the greenhouse effect caused by high CO 2 level in atmosphere, but also yields carbon chemicals/fuels at the same time. Herein, a facile way to design the heterogeneous TiO 2 @In 2 S 3 hollow structures possessing robust light harvesting in both ultraviolet and visible regions is proposed and exhibits a higher generation rate of 25.35 and 1.24 μmol·g −1 ·h −1 for photocatalytic CO 2 reduction to CO and CH 4 , respectively. The excellent photocatalytic catalytic performance comes from i) the confined heterostructured TiO 2 @In 2 S 3 possesses a suitable band structure and a broadband-light absorbing capacity for CO 2 photoreduction, ii) the rich interfaces between nanosized TiO 2 and In 2 S 3 on the shell can significantly reduce the diffusion length of carriers and enhance the utilization efficiency of photogenerated electron-hole pairs, and iii) enriched surface oxygen vacancies can provide more active sites for CO 2 adsorption.
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ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Mengting Li,Huiying Mu,Ran Su,Ruihong Liu,Ying Liu,Yilei Li,Fa-tang Li
Although crystal facet engineering is extensively studied in energy and environmental technologies, the in-depth understanding of intrinsic mechanisms governing crystal facet heterojunctions in tuning band alignments is still limited. Here, novel Bi 5 O 7 NO 3 crystals exposing tailor {080} facets are synthesized via NH 4 + -assisted self-confined construction. It has been confirmed that NH 4 + ions selectively adsorb on the {141} facets, inversely inducing the growth of desired {080} crystal facets, while the tailored {080} facets facilitate the generation of oxygen vacancies. The controllable concentration of oxygen vacancies, influenced by different exposed facets, can optimize the relative positions of Fermi levels and shift the photoelectron transfer route between the {141} and {080}-OV facets from type-II to S-scheme, thus triggering rapid charge transport channels and effectively suppressing electron-hole recombination. DFT calculation verifies that the energy barrier for the *COOH formation on Bi 5 O 7 NO 3 -{080}-OV is the lowest, thereby promoting the generation of CO. The well-designed Bi 5 O 7 NO 3 crystals with the optimal {080}/{141} facet ratio exhibit a 3.8-fold enhancement in photocatalytic CO 2 reduction, compared to traditional Bi 5 O 7 NO 3 dominated by the {141} facets. This work offers new insights into the regulation of band alignments at heterointerfaces and the design of high-efficiency photocatalysts.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Xinyue Cheng,Xueyan Sun,Shiqiang Zheng,Wenjia Zhou,Zhen Yuan,Liangliang Zhu,Xi Chen
Direct air capture (DAC) of CO2 is emerging as an important technology to mitigate the environmental challenges posed by excessive carbon emissions. The development of reliable and affordable adsorbents has long been a topic of great interest in the DAC field. In this work, through a quaternization process, inexpensive and readily available plant-based biochars including walnut shell, cornstalk, rice husk, and long-stalked lentil shell were prepared as moisture-swing adsorbents to capture CO2 from ambient air. Among these biochar adsorbents, the most effective one was found to be the quaternized long-stalked lentil shell, whose CO2 adsorption capacity reached 0.88 mmol/g at 25 °C and 50% relative humidity, which is around five times that of previously reported biochar moisture-swing adsorbents (including bamboo cellulose and chitosan aerogel). Interestingly, different from the anion-exchange resin (the most studied moisture-swing adsorbent) whose adsorption capacity decreases progressively with increasing ambient humidity and the optimal adsorption requires a relative humidity below 5%, the adsorbents developed here obtained optimal adsorption performance at 50% relative humidity (at room temperature). This result greatly expands the suitable deployment area of moisture-swing DAC since the relative humidity of most land areas on earth is in the range of 40–80%.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Yu Nie,Yanfang Li,Chao An,Xin Tan,Zhuofeng Hu,Jinhua Ye,Tao Yu
Ethylene production by CO 2 reduction is sluggish because the repulsive dipole-dipole interaction and 12 proton-coupled electron-transfer steps consecutively. Amorphous structured photocatalysts possess few grain boundaries and abundant unsaturated sites, accelerating the reaction efficiency from the angle of dynamics and thermodynamics, which still not yet be used in PCR to C 2 products currently. Herein, an amorphous Cu x CoS y composed of the minority crystalline CuCo 2 S 4 is fabricated to realize an excellent C 2 H 4 selectivity in terms of R electron (94.9%). Unsaturated Co and S play the key roles in the improved efficiency of C 2 H 4 generation. C-C coupling is achieved via shortening Co-S bonds distance, and *CO-*CO coupling barrier is decreased by more electrons accumulated on unsaturated S. Water is adsorbed on Co adjacent to S and provide protons for *COCO to form *CH 2 = C. This work paves a new way for broadening the efficient of C 2 H 4 photocatalytic evolution using amorphous photocatalyst.
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