Nanomaterials
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2023
·Vol. 13
·期 24
·3153
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IF 5.3
Zhenteng Sheng,Hui Zhou,Yuhua Zhang,Jinlin Li,Li Wang
The selective hydrogenation of CO2into high-value chemicals is an effective approach to address environmental issues. Cobalt-based catalysts have significant potential in CO2hydrogenation reaction systems; however, there is a need to control their selectivity better. In this study, copper is introduced onto Co3O4nanosheets using the ion exchange reverse loading method. The unique interaction of these materials significantly alters the selectivity of the cobalt-based catalyst. Results from scanning transmission electron microscopy and scanning electron microscopy indicate that this catalyst enables a more even dispersion of copper species in the Co3O4nanosheets. Temperature-programmed reduction and X-ray photoelectron spectroscopy reveal that the catalyst facilitates the metal–metal interaction between Co and Cu. Temperature-programmed desorption experiments for CO2and H2demonstrate that the close interaction between Co and Cu modifies CO2adsorption, leading to differences in catalytic activity. Moreover, the catalyst effectively suppresses CO2methanation and promotes methanol formation by altering the alkalinity of the catalyst surface and weakening the hydrogen dissociation ability.Keywords:CO2hydrogenation;methanol;cobalt;copper
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FOOD CHEMISTRY
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2023
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IF 8.8
Shanshan Wang,Tian Lei,Leilei Liu,Zhijian Tan
Hesperidin, also known as vitamin P, is widely studied for its distinctive potential in food and pharmaceutical industries. This work focuses on the research of CO 2 -responsive deep eutectic solvents (DESs) used as recyclable extractants for efficient extraction of hesperidin from Fertile orange peel. Reversible phase transformation of DES solution was achieved by bubbling CO 2 /N 2 . The maximum extraction yield of 22.39 mg/g was obtained for hesperidin under the following conditions: DES-6 (triethanolamine: 4-methoxyphenol = 1:1) used as extractant, water content of 35 wt%, solid–liquid ratio of 1:60 g/mL, extraction temperature of 25 °C, and ultrasonic time of 25 min, which was much higher than that extracted by methanol. Hesperidin of 74.38% was recovered in top phase after CO 2 triggering. Density function theory (DFT) results indicated that hydrogen and π - π bonds were the main factors affecting hesperidin extraction. This study provides a new idea for extracting natural bioactive compounds using recyclable extractants.
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ENERGY
·
2023
·
IF 9
Xin Yin,Shufeng Shen
Water-lean amine absorbents have potential in reducing regeneration energy consumption for post-combustion CO 2 capture. In this work, dimethyl sulfoxide (DMSO) was proposed as a cosolvent to develop water-lean monophasic absorbents for capturing CO 2 in the simulated flue gas treatment. CO 2 absorption and desorption performance has been investigated for nonaqueous/water-lean systems involving three secondary alkanolamines and compared with the conventional monoethanolamine (MEA). Effect of water content in these absorbents on reaction products, regeneration energy consumption and capture performance was also discussed. Interestingly, the DMSO-based amine blends can maintain the monophasic state before and after CO 2 absorption at the investigated conditions. Water-lean absorbent of 2-(butylamino)ethanol (BAE)/DMSO/H 2 O was proposed for energy-efficient CO 2 capture, due to the observed high cyclic capacity and super-low energy consumption. Increasing water content in the absorbents can slightly improve the absorption capacity and cyclic capacity, but significantly increased the regeneration energy. Maintaining the water content not higher than 10 mass% can reduce the regeneration energy by 48–55% compared with the benchmark aqueous 30% MEA (4.05 MJ kg −1 CO 2 ), which makes the proposed absorbent as a compelling candidate in the conventional CO 2 capture process without major process modification.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Yuke Zhang,Yi Huang,Shangqing Chen,Lijuan Shi,Jiancheng Wang,Qun Yi,Feng Pei
The high-efficiency capture of CO 2 from biogas by adsorption is highly desirable, which, yet faces the challenges regards of the unsatisfactory adsorption efficiency, selectivity, and regeneration performance. Herein, ionic ultramicroporous metal organic frameworks (IUM-MOFs) with high CO 2 affinity are constructed by one-step in-situ coordination strategy and used for CO 2 /CH 4 separation. The phenoxylate anion-functionalized ionic liquid (FIL) serves as competitive ligands in the formation of IUM-MOFs. The oxyl group exhibits high affinity with CO 2 as the Lewis basic center, while the rigid counterion occupies the adsorption space of CH 4 in the cavities of IUM-MOFs, thus bringing about superior CO 2 adsorption capacity of 149 cm 3 g −1 (150% higher than that of Cu-BTC) and high IAST predicted selectivity with CH 4 of 22 under atmospheric condition. Mechanism analysis demonstrated that the formation of hydrogen bonds between CO 2 with coordinated IL and H 2 O and IL-enhanced polarity of MOFs benefit to the CO 2 adsorption. In addition, the IUM-MOFs could be facilely regenerated at 120 °C with favorable recycling stability. This work provides facile strategy for the rational design of IUM-MOFs and lays useful insights for structural tuning to promote their applications.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Qiang Wang,Yaru Li,Zichen Yu,Xuewen Li,Shouhua Yin,Wen Ji,Yonghua Hu,Weiping Cai,Xianbiao Wang
Highly porous carbon adsorbent is much desired to diminish greenhouse effect caused by CO 2 emission and benefit for subsequent carbon cycle . Herein, a low-cost and environment-friendly carbonization strategy was reported for preparation of highly porous carbon derived from biomass. Such carbonization is a synergistic process with hydrothermal treatment coupled with a subsequent pyrolysis using sugarcane as biomass. The obtained hydrothermal-pyrolysis derived porous carbon (HPC) has a BET surface area of 938 m 2 /g, which is much higher than that of carbon produced through direct pyrolysis (PC, 528 m 2 /g). During the hydrothermal carbonization pretreatment, highly thermostable aromatic skeletons are formed and converted to carbon skeletons in the post-pyrolysis process, leading to formation of highly stable micropores and higher surface area. Further, HPC shows remarkable adsorption ability of CO 2 (2.8 mmol/g, 25 °C, 1 bar), higher than that of PC (2.1 mmol/g). In addition, the HPC exhibits high CO 2 /N 2 adsorption selectivity and recyclability, demonstrating its potential application in CO 2 capture. This work not only gives new light for tailoring carbon materials with highly porous structure but also provides novel adsorbent for CO 2 adsorption.
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ACS Applied Materials & Interfaces
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2023
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IF 9.5
Shaoqi Zhang,Haiyang Yu,Yi Wang,Yuxiang Yan,Jun Dai,Dajun Shu,Xinglong Wu
CO2 possesses extraordinary thermodynamic stability, and its reduction reaction involves multiple electron-transfer processes. Thus, high-density electron occupation on a catalyst surface is an effective driving force for improving the photocatalytic activity. Here, we report on the fabrication of Fe-doped Bi2O3 catalysts (denoted as FexBi2-xO3) with different Fe contents using the solvothermal method. The self-assembled catalyst has a nanoflower-like morphology, and its performance of CO2 reduction to CO is improved largely dependent on the Fe content. In the sample with a 7.0% Fe content (Fe0.07Bi1.93O3), the CO evolution rate reaches 30.06 μmol g–1 h–1, which is about 6 times higher than the 4.95 μmol g–1 h–1 of pristine Bi2O3, and shows excellent photostability after three cycles, with each cycle lasting for 7 h. Theoretical calculation and spectral characterization reveal that such a good CO2 reduction reaction performance arises from effective surface occupation of Fe, which not only enhances sunlight absorption but also significantly increases the surface electron density on the double metal active sites. This work provides a new strategy for improving the photocatalytic performance by surface metal doping in some metal oxide photocatalysts.
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NEW JOURNAL OF CHEMISTRY
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2023
·Vol. 47
·期 20
·9842-9851
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IF 3.3
Li Luo,Jie Deng,Yingying Wang,Qiang Tang,Mengyue Hou,Ziyue Zhang,Shijian Lu,Yongdong Chen
Developing efficient catalysts is crucial for the chemical utilization of CO2, which would be conducive to solving both environmental issues and the resource crisis. In this work, a basalt fiber (BF)-supported CuNi catalyst was constructed for the conversion of CO2 and methanol to dimethyl carbonate (DMC). In order to optimize the surface properties of BF, the pristine BF (BF-U) was modified by HCl (BF-H) and NaOH (BF-N) solutions. The influence of the BF surface properties on the physicochemical state of CuNi and the catalytic performance of the supported CuNi/BF catalysts was systematically investigated. The results showed that the CuNi/BF-N monolithic catalyst had the best activity, and the yield of DMC reached 12.9%. SEM, XRD, and XPS characterizations exhibited that the CuNi nanoalloy particles were uniformly distributed on BF-N and possessed high Cu0/1+ and Ni0 contents. This contributed to the abundant CO2 adsorption sites, as evidenced by CO2-TPD, especially for the medium-strength CO2 adsorption sites, which was responsible for the superior catalytic activity. This study provides an efficient catalyst for the synthesis of DMC from CO2 and methanol and can serve as a reference for industrial catalyst design.
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JOURNAL OF MEMBRANE SCIENCE
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2023
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IF 9.5
Boyu Li,Jiaxiang Liu,Xuanting He,Rong Wang,Wenquan Tao,Zhuo Li
Facilitated transport mixed matrix membranes (FTMMMs) separation technology has shown advantages in improving CO 2 recycling efficiency and reducing the environmental impacts associated with carbon emission. The design of FTMMMs is highly dependent on the selection of a compatible combination of polymer and filler. Herein, a novel grafted nanoparticles (GNPs) filler UiO-66-NM@PEG with multiple groups prone to hydrogen bond was designed to alleviate the phase separation and performance degradation caused by filler/polymer poor compatibility. In the GNPs configuration, by employing the coexistence strategy of coupling reaction and covalent bonds , maleic anhydride (MAH) was coupled with the amino group on UiO-66-NH 2 without clogging or cracking, and the generated carboxyl groups can be cross-linked with the hydroxyl groups on the poly (ethylene glycol) (PEG) by covalent bonds. The UiO-66-NM@PEG demonstrated excellent interface compatibility between the filler and matrix phase of UiO-66-NM@PEG/PVDF, which was further convinced by molecular modelling. The resultant UiO-66-NM@PEG/PVDF achieved a simultaneous enhancement of gas permeability (537.6 Barrer) and ideal CO 2 /N 2 selectivity (47.8), which surpassed Robenson upper bound. Moreover, the UiO-66-NM@PEG/PVDF has a lasting sustainability over 960 h (40 days), and a valid anti-acid/alkali corrosion resistance in harsh environments. More importantly, UiO-66-NM@PEG can also be well mixed with other mixture matrices such as hydroxy-terminated polydimethylsiloxane (PDMS) and polyether-block-polyamide copolymer (PEBAX) to promote permeability/ideal selectivity up to (724.1 Barrer/21.1) and (307.4 Barrer/31.4). We thus concluded that this rational-design GNPs approach provides a general toolbox for controllable engineering in GNPs whereby enhanced favorable filler/matrix compatibility in FTMMMs with optimized CO 2 /N 2 separation properties.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Jiaying Yan,Yayu Guan,Barbara Marchetti,Yuyu Liu,Fanghua Ning,Jin Yi,Xiao-Dong Zhou
Electrochemical reduction of CO 2 (ERCO 2 ) is an effective way to convert CO 2 into useful chemical products. However, most catalysts used for ERCO 2 show poor selectivity and stability. Here, we design a Bi 8 Eu 1 bimetallic catalyst, which exhibits both excellent stability (>400 h) and Faradaic efficiency for formate production (∼100% at − 0.89 V RHE ). Moreover, high Faradaic efficiency (>97%) is observed over a wide potential window (from − 0.89 V RHE to − 1.19 V RHE ). In a flow-cell, the Bi 8 Eu 1 catalyst shows an ultra-high current density of 250 mA cm −2 at − 0.77 V RHE . Density functional theory calculations indicate that the Bi-Eu interactions activate the Bi sites for strongly stabilizing *OCHO intermediates, thus promoting the conversion of CO 2 to formate. This work provides insights into the design of excellent electrocatalysts for ERCO 2 with improved activity and durability.
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CHEMICAL ENGINEERING SCIENCE
·
2023
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IF 4.7
Wenji Zheng,Ziheng Li,Yan Dai,Xiangcun Li,Xuehua Ruan,Xiaobin Jiang,Xiujuan Zhang,Gaohong He
The regulation on cage size and CO 2 -philic environment of metal–organic frameworks (MOFs) is essential to improve CO 2 capture. In this work, [Bmim][Tf 2 N] was proposed to position into cages of ZIF-8 to achieve the selective permeation of CO 2 by pore screening and CO 2 adsorption. [Bmim][Tf 2 N] was introduced into cages of ZIF-8 by “adsorption-infiltration” strategy. Due to the strong interaction between [Tf 2 N] − and ZIF-8, the cages present a CO 2 -philic environment, which preferentially attracts CO 2 to enter these cages, ensuring the dissolution selectivity of CO 2 . Besides, the proper cage size tuned by [Bmim][Tf 2 N] provides CO 2 with a faster transport channel due to its smaller average kinetic diameter than N 2 , guaranteeing the diffusion selectivity of CO 2 . Consequently, the CO 2 separation in [Bmim][Tf 2 N]@ZIF-8/Pebax MMMs is intensified. With increasing the [Bmim][Tf 2 N] content in cages of ZIF-8, the pore volume by BET results decreases and the CO 2 adsorption from molecular simulation increases. In response, the CO 2 /N 2 selectivity of [Bmim][Tf 2 N]@ZIF-8/Pebax MMMs is enhanced constantly. Meanwhile, the CO 2 permeability is declined due to the narrowed cage size. All of these results demonstrate the significance of pore screening and CO 2 adsorption induced by [Bmim][Tf 2 N]. Specifically, [Bmim][Tf 2 N] 8 @ZIF-8/Pebax MMM at filler loading of 15 wt% exhibits the CO 2 permeability of 108.3 Barrer and the CO 2 /N 2 selectivity of 86.7, exceeding the 2008 Robeson upper bound. Especially the CO 2 /N 2 selectivity locates at a higher level than those of most reported works, indicating that appropriate tuning of the physicochemical properties within the nanocages of MOFs is significative to improve CO 2 capture.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Shujie Liang,Xiaohui Zhong,Zuqi Zhong,Hong Deng,Wai-Yeung Wong
Photoconversion of CO 2 into value-added fuels has aroused widespread interest; however, this process is significantly limited by the inefficient thermodynamics and sluggish reaction dynamics in the diluted CO 2 . To circumvent these obstacles, we design a bipyridine-based polyimide polymer for anchoring single Ni site for diluted CO 2 photoreduction. The desired Ni single atomic catalysts achieve high generation activity of ∼ 2262 μmol/h with apparent quantum efficiency (A.Q.E.) of 0.20% for CO 2 -to-CO in 0.1 atm CO 2 pressure. No measurable H 2 is produced in the catalytic process, affording nearly 100% CO selectivity over water splitting. This superior activity and selectivity outperform most previous atomical catalysts. Mechanistic analyses elucidate that the highly dispersed Ni atoms act as active sites for effective CO 2 binding and activation, and stabilize the rate-determining step of intermediates for CO generation. This work discloses the relationship between catalytic properties and single atoms for efficient solar-driven diluted CO 2 reduction.
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Journal of Energy Chemistry
·
2023
·
IF 13.1
Hua-Qing Yin,Zuo-Shu Sun,Qiu-Ping Zhao,Lu-Lu Yang,Tong-Bu Lu,Zhi-Ming Zhang
Traditional urea synthesis under harsh conditions is usually associated with high energy input and has aroused severe environmental concerns. Electrocatalytic C–N coupling by converting nitrate and CO 2 into urea under ambient conditions represents a promising alternative process. But it was still limited by the strong competition between nitrate electrochemical reduction (NO 3 ER) and CO 2 electrochemical reduction (CO 2 ER). Here, Fe II -Fe III OOH@BiVO 4 - n heterostructures are constructed through hydrothermal synthesis and exhibited superior performance toward urea electrosynthesis with NO 3 − and CO 2 as feedstocks. The optimized urea yield and Faradaic efficiency over Fe II -Fe III OOH@BiVO 4 -2 can reach 13.8 mmol h −1 g −1 and 11.5% at −0.8 V vs. reversible hydrogen electrode, which is much higher than that of bare FeOOH (3.2 mmol h −1 g −1 and 1.3%), pristine BiVO 4 (2.0 mmol h −1 g −1 and 5.4%), and the other Fe II -Fe III OOH@BiVO 4 - n ( n = 1, 3, 5) heterostructures. Systematic experiments have verified that BiVO 4 and FeOOH are subreaction active sites towards simultaneous CO 2 ER and NO 3 ER, respectively, achieving co-activation of CO 2 and NO 3 − on Fe II -Fe III OOH@BiVO 4 -2. Moreover, the urea synthesis via the *CO and NO* intermediates and C–N coupling was confirmed by the in situ Fourier transform infrared spectroscopy. This work not only alleviates the CO 2 emission and nitrate pollution but also presents an efficient catalyst for synergistic catalysis towards sustainable urea synthesis.
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