APPLIED SURFACE SCIENCE
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2022
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IF 7.392
Tianyou Chen,Jin Hu,Kaizhao Wang,Kaijun Wang,Weijun Zhang,Haijiao Xie,Guoyou Gan,Jin Shi
Electron transfer to CO 2 is commonly regarded as a critical step for activating CO 2 . Herein, we describe the development of a simple and effective strategy to facilitate electron transfer to CO 2 by introducing oxygen vacancies (O V ) in electrocatalysts. We discovered that stirring oxidized eutectic gallium indium is an important pretreatment step for introducing O V . In the subsequent CO 2 reduction process, the oxidized eutectic gallium indium (O-EGaIn) was reduced to the oxide-derived EGaIn (OD-EGaIn), which achieved 4 times higher Faradic efficiency for CO production than the eutectic gallium indium (EGaIn) in a tetrabutylammonium chloride/acetonitrile (Bu 4 NCl/AN) electrolytes. The XPS results showed that the O V concentration in the OD-EGaIn is much larger than that in the O-EGaIn and EGaIn samples. Electrokinetic studies indicated that the introduction of O V facilitates electron transfer to CO 2 . Density functional theory (DFT) calculations further revealed that the electrons tend to accumulate around the O V . These localized electrons then flow to the antibonding orbitals of CO 2 molecules, resulting in activating CO 2 and forming the key CO 2 •− radical.
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JOURNAL OF MOLECULAR LIQUIDS
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2023
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IF 6
Zhiyong Zhu,Guanyao Yu,Liangjing Duan,Xiao Liu,Li Wang,Jinglai Zhang
Developing a robust catalyst for CO 2 reduction reaction (CO 2 RR) is critical to achieving a closed carbon cycle. Yet, the process of CO 2 RR still faces enormous challenges, in part because of the lack of highly active, stable, as well as cost-effective electrocatalysts. In this work, we reported an effective and sample strategy to immobilize nickel phthalocyanine (Ni-Pc) molecules on the fruit-peel-derived carbon framework surface (denoted as Ni-Pc/CF and carbon framework denoted as CF) with exceptional CO production performances. Dispersed Ni-Pc molecules on the carbon materials are verified by transmission electron microscopy (TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and Raman measurements. The obtained Ni-Pc/CF catalyst shows that the high faradaic efficiency (FE) exceeds 95.0 % over a potential of −0.7 to −0.9 V ( vs reversible hydrogen electrode (RHE), V RHE ), the maximum FE (99.1 %) can close to 100 % at −0.8 V, and the excellent stability over a 10 h reaction period. This work offers valuable insights into the immobilization of stabilized, highly dispersed molecule catalysts on carbon materials surfaces for selective reduction of CO 2 to CO.
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 16
·2214215
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IF 19
Xiaosong Hu,Xinyu Liu,Xin Hu,Chaoyue Zhao,Qingxin Guan,Wei Li
Reverse water-gas shift (RWGS) reaction is the initial and necessary step of CO 2 hydrogenation to high value-added products, and regulating the selectivity of CO is still a fundamental challenge. In the present study, an efficient catalyst (CuZnN x @C-N) composed by Zn single atoms and Cu clusters stabilized by nitrogen sites is reported. It contains saturated four-coordinate Zn-N 4 sites and low valence CuN x clusters. Monodisperse Zn induces the aggregation of pyridinic N to form Zn-N 4 and N 4 structures, which show strong Lewis basicity and has strong adsorption for *CO 2 and *COOH intermediates, but weak adsorption for *CO, thus greatly improves the CO 2 conversion and CO selectivity. The catalyst calcined at 700 °C exhibits the highest CO 2 conversion of 43.6% under atmospheric pressure, which is 18.33 times of Cu-ZnO and close to the thermodynamic equilibrium conversion rate (49.9%) of CO 2 . In the catalytic process, CuN x not only adsorbs and activates H 2 , but also cooperates with the adjacent Zn-N 4 and N 4 structures to jointly activate CO 2 molecules and further promotes the hydrogenation of CO 2 . This synergistic mechanism will provide new insights for developing efficient hydrogenation catalysts.
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ChemistrySelect
·
2023
·Vol. 8
·期 5
·e202204303
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IF 2.1
Weishan Tang,Yunpeng Shen,Peng Yang,Caiyun Lin,Zhijun Ke,Xiaoping Rao
Graphical The single-walled carbon nanotubes dispersed by an extremely rigid CO 2 -responsive surfactant were used to fabricate highly conductive epoxy composites with ultra-strong mechanical properties. The emerging nanomaterials single-walled carbon nanotube (SWNTs) with large specific surface area, excellent electrical conductivity and high mechanical strength, has been used to fabricate electronic devices. However, the extremely strong π-π interactions make SWNTs easy to agglomerate, thus limiting their application. In this work, a novel method was applied to disperse SWNTs by using rigid rosin-based CO 2 responsive surfactant rosin acid dimaleimide choline (R-BMI-C). When pH 10.4, SWNTs can be uniformly and stably dispersed, and at pH 6.3, SWNTs aggregated. The dispersed SWNTs was then integrated into diglycidyl ether of bis phenol A (DGEBA) to fabricate high conductive epoxy composites. Their properties were characterized by SEM, TG, high resistivity meters, etc. . The results showed that the modified SWNTs/DGEBA composites obtained an ultra-low percolation threshold (0.025 wt.%). Compared with the original SWNTs/DGEBA composite, its tensile strength and elastic modulus were enhanced by 17 % and 96 %, respectively, when the SWNTs content was 0.5 wt.%.
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Membranes
·
2022
·Vol. 13
·期 1
·36
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IF 4.562
Yunwu Yu,Chunyang Xie,Yan Wu,Peng Liu,Ye Wan,Xiaowei Sun,Lihua Wang,Yinan Zhang
In this study, a novel composite membrane was developed by casting the mixed aqueous solution of chitosan (CS) and polyvinyl alcohol (PVA) on a glass fiber microporous membrane. The polymeric coating of a composite membrane containing amino groups and hydroxyl groups has a favorable CO2affinity and provides an enhanced CO2transport mechanism, thereby improving the permeance and selectivity of CO2. A series of tests for the composite membranes were taken to characterize the chemical structure, morphology, strength, and gas separation properties. ATR-FTIR spectra showed that the chemical structure and functional group of the polymer coating had no obvious change after the heat treatment under 180 °C, while SEM results showed that the composite membranes had a dense surface. The gas permeance and selectivity of the composite membrane were tested using single gases. The results showed that the addition of chitosan can increase the CO2permeance which could reach 233 GPU. After a wetting treatment, the CO2permeance (454 GPU) and gas selectivity (17.71) were higher than that of dry membranes because moisture promotes the composite membrane transmission. After a heat treatment, the permeance of N2decreased more significantly than that of CO2, which led to an increase in CO2/N2selectivity (10.0).Keywords:carbon dioxide;polyvinyl alcohol;chitosan;glass fiber microporous membrane;gas separation
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高影响因子
MOLECULES
·
2023
·Vol. 28
·期 3
·1074
·
IF 4.6
Xin Zhao,Jingjing Li,Hengxin Jian,Mengyu Lu,Mei Wang
One mononuclear Mn(III) complex [MnIIIL(H2O)(MeCN)](ClO4) (1) and one hetero-binuclear complex [(CuIILMnII(H2O)3)(CuIIL)2](ClO4)2·CH3OH (2) have been synthesized with the Schiff base ligand (H2L= N,N′-bis(3-methoxysalicylidene)-1,2-phenylenediamine). Single crystal X-ray structural analysis manifests that the Mn(III) ion in1has an octahedral coordination structure, whereas the Mn(II) ion in2possesses a trigonal bipyramidal configuration and the Cu(II) ion in2is four-coordinated with a square-planar geometry. Electrochimerical catalytic investigation demonstrates that the two complexes can electrochemically catalyze water oxidation and CO2reduction simultaneously. The coordination environments of the Mn(III), Mn(II), and Cu(II) ions in1and2were provided by the Schiff base ligand (L) and labile solvent molecules. The coordinately unsaturated environment of the Cu(II) center in2can perfectly facilitate the catalytic performance of2. Complexes1and2display that the over potentials for water oxidation are 728 mV and 216 mV, faradaic efficiencies (FEs) are 88% and 92%, respectively, as well as the turnover frequency (TOF) values for the catalytic reduction of CO2to CO are 0.38 s−1at −1.65 V and 15.97 s−1at −1.60 V, respectively. Complex2shows much better catalytic performance for both water oxidation and CO2reduction than that of complex1, which could be owing to a structural reason which is attributed to the synergistic catalytic action of the neighboring Mn(III) and Cu(II) active sites in2. Complexes1and2are the first two compounds coordinated with Schiff base ligand for both water oxidation and CO2reduction. The finding in this work can offer significant inspiration for the future development of electrocatalysis in this area.Keywords:electrocatalysis;carbon dioxide reduction;water oxidation;hetero-binuclear complex;cooperative catalytic effect
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Yun Li,Houfang Lu,Yingying Liu,Kejing Wu,Yingming Zhu,Bin Liang
Nano-SiO 2 was used to enhance the performance of CO 2 absorption and desorption in viscous DBU-glycerol solution with a viscosity of about 60 mPa·s. The effects of ultrasonic time in the preparation of nanofluids, solids loading and particle/cluster size of SiO 2 on absorbent properties and absorption performance were investigated. Meanwhile, the enhancements of heat transfer and mass transfer with nanoparticles in the desorption of CO 2 -loaded DBU-glycerol solutions were also analyzed. Proper ultrasonic vibration time and nano-SiO 2 loading can both decrease the average particle size in the system which can improve the absorption. The increase of interfacial area between gas and liquid with the addition of nano-SiO 2 dominates the enhancement of absorption and it has little effect on the enhancement factor when the nano-SiO 2 size is 102 nm or below. But when the particle size is higher than 102 nm, the enhancement factor decreases with the increase of particle/cluster size. The addition of 0.10 wt% SiO 2 nanoparticle with a particle size of 16 nm can increase the absorption rate by 31 % compared with base liquid. In desorption process, the desorption rate for CO 2 -loaded DBU-glycerol solutions can increase 18 % with the addition of 0.10 wt% nano-SiO 2 with a particle size of 32 nm. The main reason could be that nano-SiO 2 can improve the heating rate of the base fluid and supply plenty of nucleation sites for the formation of bubbles to improve the desorption rate. It shows that nano-SiO 2 can be used to enhance both the absorption and desorption processes in solutions with high viscosity.
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International Journal of Electrochemical Science
·
2023
·
IF 1.5
Lijuan Guo,Wen Chen,Cuiqiong Wang,Boran Dong
The CH 4 -CO 2 reforming reaction can realize the utilization of both CH 4 and CO 2 , which is important to control the greenhouse effect and protect the environment. The development of low-cost, high-activity and high-stability reforming catalysts is the focus of research. This work used electrochemical methods to synthesize Cu 3 (BTC) 2 in high yields. Cu 3 (BTC) 2 was subsequently used as a precursor and Cu 3 P was synthesized by direct phosphorylation at different temperatures. Both high and low phosphatization temperatures can reduce the hydrogen precipitation performance of the prepared catalyst. In the CH 4 -CO 2 reforming reaction, the Cu 3 P catalyst prepared at elevated temperature has more excellent activity and stability. However, the activity of the catalyst did not keep increasing with the increase of temperature. After the CH 4 -CO 2 reforming reaction at 700 ℃ for 6 h, the conversion of Cu 3 P-350 did not change significantly, and the stability was significantly higher than that of Cu 3 P-300 and Cu 3 P-325. At the same time, when the phosphating temperature is lower than 375 ℃ Cu 3 P carbon accumulation are less. The amount of carbon accumulation increases when the phosphating temperature reaches 400 °C.
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ULTRASONICS SONOCHEMISTRY
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2022
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IF 9.336
Jiabei Wang,Zhiqiang Jiang
A series of porous S-doped carbon nitride ribbons (PSCN) were prepared by one-pot hydrothermal and sonochemical synthesis techniques. The morphologies and nanostructures of the catalysts were characterized by SEM, XRD and IR, which confirmed the pristine graphitic structures of carbon nitrides retained in the products. Due to sonication treatment, PSCN has porous structures in the thin ribbon and larger specific surface areas (PSCN 43.5 m 2 /g, SCN 26.6 m 2 /g and GCN 6.5 m 2 /g). XPS and elemental mappings verified that sulfur atoms were successfully introduced into the carbon nitride framework. Diffuse reflectance spectroscopy (DRS) results showed S-doping in the carbon nitride reduced the bandgap energy and enhanced their capability of the utilization of visible light, which contributed to higher photo-generated current. Photoluminescence (PL) analysis indicates the recombination of photogenerated carriers was suppressed in PSCN. Moreover, the photocatalytic performance showed that S-doping and porous and thin ribbon nanostructures may effectively boost the CO 2 reduction rate (to as much as 5.8 times of GCN) when illuminated by visible light (>420 nm) without the need of sacrificial materials. The preliminary mechanisms of the formation of PSCN and its applications in photocatalytic CO 2 reduction are proposed. It highlights the potential of the current technique to produce effective, nonmetal-doped carbon nitride photocatalysts.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Rujing Hou,Shilong Wang,Lei Wang,Chang Li,Huan Wang,Yingtian Xu,Chongqing Wang,Yichang Pan,Weihong Xing
The trade-off relationship between permeability and selectivity as well as plasticization issues have largely impeded the advancement of membrane technology. Mixed-matrix-membranes (MMMs) with the incorporation of fillers into the polymer matrix is one promising method to deal with these challenges by carefully tuning their chemical properties. Compared with nanoparticles, the counterpart of nanosheet has a larger external surface area with a tendency to have closer contact with a polymer matrix to form a defect-free membrane at higher loading. This work successfully synthesized a high aspect ratio (30/1) of KAUST-8 nanosheets with high CO 2 uptake (60 cm 3 /g). This enables an optimal loading of 30 wt.% in the CO 2 -attractive crosslinked poly(ethylene oxide) (XLPEO) membrane and results in the simultaneously enhanced CO 2 permeability and CO 2 /N 2 selectivity with 280 % and 30 % up, respectively in the mixed gas permeation measurements (50/50 vol.). The resultant membrane performance surpassed the 2008 Robeson upper bound. Meanwhile, the stabilized MMM performance of up to 6 bar and high thermal stability of up to 350 °C bring extra benefits to the KAUST-8-based XLPEO membrane for post-combustion flue gas treatment.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Guiming Xie,Rongrong Jin,Pengju Ren,Yunming Fang,Runduo Zhang,Zhou-jun Wang
Boosted CO 2 hydrogenation to methanol was achieved by introducing appropriate amount of Au into conventional Cu-based catalysts. The Au x Cu/ZnO bimetallic catalysts with various Au/Cu molar ratio (x = 0.001, 0.005, 0.02 and 0.05) were prepared by the co-precipitation method, among which the Au 0.005 Cu/ZnO catalyst exhibited the highest methanol production rate. The formation of Au-Cu alloy was identified on the Au x Cu/ZnO bimetallic catalysts. Experimental characterizations and density functional theory (DFT) calculations suggested metal-oxide interfaces with oxygen vacancies as intrinsic active sties for both un-promoted and Au-promoted Cu/ZnO catalysts. The promotion effect of Au in bimetallic catalysts was correlated with the increase of active sites, facilitation of CO 2 activation and modification of intermediate adsorption. The present work for the first time develops a promising Au 0.005 Cu/ZnO bimetallic catalyst with trace amount of Au (only 0.4 wt%) and provides insight into the reaction mechanism over Au-promoted Cu/ZnO catalysts for methanol synthesis via CO 2 hydrogenation.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2022
·
IF 3.119
Tiantian Ping,Qinghai Long,Shufeng Shen
Solubility of N2O and CO2 in pure 2-butoxyethanol (2-BE) was determined in a stirred equilibrium cell at temperatures ranging from 283.2 to 333.2 K and correlated as an exponential function of temperature. Ratios of solubility of CO2 to N2O in several reported solvents were found to be strongly dependent on the order of solvent dielectric constants. Solubility of N2O in 2-(butylamino)ethanol (BAE) and the binary blends of 2-BE and BAE was measured over the temperature range from 283.2 to 333.2 K and with BAE concentration from 6.5 to 65.4 mass%. N2O solubility data were well represented by correlation models with AARDs within 0.8%. Physical solubility of CO2 in a nonaqueous 2-BE/BAE system can be estimated using the N2O analogy method.
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