JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Xin Li,Jiale Liu,Guocan Jiang,Xinyu Lin,Jin Wang,Zhengquan Li
Aerogels, especially MXene aerogels, are an ideal multifunctional platform for developing efficient photocatalysts for CO 2 reduction because they are featured by abundant catalytic sites, high electrical conductivity, high gas absorption ability and self-supported structure. However, the pristine MXene aerogel has almost no ability to utilize light, which requires additional photosensitizers to assist it in achieving efficient light harvesting. Herein, we immobilized colloidal CsPbBr 3 nanocrystals (NCs) onto the self-supported Ti 3 C 2 T x (where T x represents surface terminations such as fluorine, oxygen, and hydroxyl groups) MXene aerogels for photocatalytic CO 2 reduction. The resultant CsPbBr 3 /Ti 3 C 2 T x MXene aerogels exhibit a remarkable photocatalytic activity toward CO 2 reduction with total electron consumption rate of 112.6 μmol g -1 h - 1 , which is 6.6-fold higher than that of the pristine CsPbBr 3 NC powders. The improvement of the photocatalytic performance is presumably attributed to the strong light absorption, effective charge separation and CO 2 adsorption in the CsPbBr 3 /Ti 3 C 2 T x MXene aerogels. This work presents an effective perovskite-based photocatalyst in aerogel form and opens a new avenue for their solar-to-fuel conversions.
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INORGANIC CHEMISTRY
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2023
·
IF 4.6
Wen-Xiong Shi,Ru-Zhen Ren,Yao Cheng,Fu-Gui Zeng,Xiang-Wei Guo,Zhi-Ming Zhang
Metal–organic framework (MOF) materials have broad application prospects in catalysis because of their ordered structure and molecular adjustability. However, the large volume of bulky MOF usually leads to insufficient exposure of the active sites and the obstruction of charge/mass transfer, which greatly limits their catalytic performance. Herein, we developed a simple graphene oxide (GO) template method to fabricate ultrathin Co-metal–organic layer (2.0 nm) on reduced GO (Co-MOL@r-GO). The as-synthesized hybrid material Co-MOL@r-GO-2 exhibits highly efficient photocatalytic performance for CO2 reduction, and the CO yield can reach as high as 25,442 μmol/gCo-MOL, which is over 20 times higher than that of the bulky Co-MOF. Systematic investigations demonstrate that GO can act as a template for the synthesis of the ultrathin Co-MOL with more active sites and can be used as the electron transport medium between the photosensitizer and the Co-MOL to enhance the catalytic activity for CO2 photoreduction.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Linkai Wang,Yu Han,Jian Wei,Qingjie Ge,Shijian Lu,Yanpeng Mao,Jian Sun
Hydrogenation of CO 2 into light olefins is an important route to carbon neutrality . Most of traditional researches focus on the catalyst component, structure, and promoter to enhance the selectivity of light olefins while ignoring the diffusion of products. Here, we report a NaFeZr-MOR composite catalyst for light olefin synthesis in CO 2 hydrogenation via pore confinement. The selectivity in hydrocarbons and STY (Space-time yields) of C 2–4 = is gradually increasing maximum up to 51.3% and 12.2 (mmol·g cat −1 . h −1 ), which lie in a high level among reported Fe-based catalysts. Further characterization revealed that the essence of selectivity change period is the accumulation and evolution of carbonaceous species, which causes the change of product diffusion behavior. It suppresses the escape of heavy hydrocarbons from MOR pores, leading to an increased light olefin, especially ethylene, which is called “dynamic confinement”. These findings provide a new insight for controlling low-carbon product selectivity in CO 2 hydrogenation.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Guangping Lei,Guojun Xi,Zihan Liu,Qibin Li,Huiyuan Cheng,Hantao Liu
Efficient capture and separation of CO 2 from flue gas and natural gas are highly promising to reduce carbon emissions and promote fuel calorific value. Here, a novel adsorbent (FeTPPs@Cu-BTC) for CO 2 separation was synthesized by encapsulating 5, 10, 15, 20-tetrakis (4-sulfonatophenyl) porphyrinato iron (III) chloride (FeTPPs) into the cages of Cu-BTC through an in-situ packaging strategy. Such strategy efficiently overcomes the shortcoming of pore clogging and leaching induced by incorporating guest molecules through the wet impregnation method. Meanwhile, more tunable micropores and extra affinity sites for CO 2 adsorption were created after encapsulation of FeTPPs, which preferably enhanced the CO 2 uptakes of FeTPPs@Cu-BTC under low pressures and promoted the separation performances for CO 2 /N 2 (15:85, v/v) and CO 2 /CH 4 (50:50, v/v) mixtures. The corresponding selectivity of FeTPPs@Cu-BTC calculated by ideal adsorbed solution theory (IAST) respectively increase to 57.7 and 14.0 from 36.0 and 10.8 of the pristine Cu-BTC at 273 K and 100 kPa, which also exceeds most reported adsorbents. Grand Canonical Monte Carlo (GCMC) simulations further elucidated that extra interaction with CO 2 and ‘sieve effect’ for N 2 or CH 4 after FeTPPs encapsulation immediately boost CO 2 uptakes and separation performance of FeTPPs@Cu-BTC. This study provides a new design idea for the development of new adsorbent materials.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Ting Wang,Fuli Sun,Shoujie Liu,Guilin Zhuang,Benxia Li
Supported Cu single-atom (Cu-SA) catalysts have exhibited unique activity and selectivity in CO 2 reduction, but they generally suffer from the easy transformation of active Cu δ+ into inactive Cu 0 . Herein, porous TiO 2 supported Cu single atoms (Cu-SAs/TiO 2 ) photocatalyst was fabricated and dioxygen (O 2 ) enhanced photocatalytic CO 2 reduction performance of Cu-SAs/TiO 2 was investigated by in-situ characterizations and theoretical calculations. The results showed that both activity and stability of Cu-SAs/TiO 2 photocatalyst could be improved by feeding a small amount of O 2 (117.6 ppm) in the reaction system. The competitive electron transfer to O 2 on Cu-SAs/TiO 2 maintained dynamic stability of Cu δ+ active sites, and O 2 -derived *OOH species lowered the formation energy barrier of key intermediate *COOH as well as delivered *H species for accelerating intermediates protonation process. Total yield rate of CH 4 and CO reached 34.64 μmol·g cat ·h −1 for CO 2 photoreduction over Cu-SAs/TiO 2 after introducing 117.6 ppm O 2 , accompanied by enhanced durability.
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JOURNAL OF APPLIED POLYMER SCIENCE
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2019
·Vol. 136
·期 18
·47439
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IF 2.188
Shanshan Guo,Yangbufan Lv,Yangwei Chen,Shaojun Cai
Global decrease in crude oil resources and frequent crude oil leaks cause the energy crisis and ecological pollution. The absorption and release of leaked crude oil through absorption materials are a necessary process for environmental protection and recycling. In this article, a CO 2 -responsive olefin copolymer was obtained by copolymerization of styrene and an amine-containing olefin monomer. The structure of resultant copolymer was characterized by FTIR; thermal properties and CO 2 -responsive morphology changes were determined by DSC/TGA and SEM, respectively. Copolymers had certain absorption capacity for toluene with absorption rate up to 180.0%. The absorbed toluene could be released upon CO 2 stimulation with desorption rate up to 84.6%. The CO 2 -responsive copolymer could be regenerated through a simple heating process and showed stable absorption–desorption performance even after being recycled for 4 times. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019 , 136 , 47439.
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JOURNAL OF MEMBRANE SCIENCE
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2018
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IF 6.578
Bin Zhu,Jindun Liu,Shaofei Wang,Jingtao Wang,Min Liu,Zhikun Yan,Feng Shi,Jiahao Li,Yifan Li
Hollow fillers with tailored nanostructures and functionalities have become promising candidates for advanced mixed matrix membranes (MMMs). Herein, polydopamine/poly (ethylene glycol) (PEG) composite microcapsules are synthesized by hard template method and embedded into the Pebax matrix to fabricate MMMs for CO 2 capture. As a well-known biomimetic adhesive, polydopamine in the capsule wall renders adequate polymer-filler interfacial adhesion. The template removal process produces through-wall mesopores , which allow rapid gas diffusion into the lumen, further significantly reducing the trans-membrane mass transfer resistance. The remaining PEG in the capsule wall not only increases CO 2 affinity, but also avoids excessive chain rigidification at polymer-filler interface. In this way, the composite capsules, compared with those without PEG, confer significantly enhanced separation performance on membranes. The optimal gas transport property of the resultant membranes is obtained with a CO 2 permeability of 510 Barrer and an ideal selectivity of 84.6 for CO 2 /N 2 at humidified state, i.e., 108%, 98% higher than those of neat Pebax membrane, respectively. In addition, owing to dopamine-enabled strong adhesion, the MMMs exhibit better stability than Pebax membrane in the long-term test at 85 °C.
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Journal of Environmental Chemical Engineering
·
2018
·
IF 0
Yuan Wang,Cailv Zheng,Yilin Wang,Hanxiang Chen,Yun Xu
A new kind of ionic liquids has been synthesized which comprised double bonds in the structure of anions (DB-ILs). Their physical properties, including densities, viscosities, activation energies and diffusion coefficients were determined. Temperature-dependent Krichevsky-Kasarnovsky (K-K) was used to deal with the data of solubility of CO 2 in DB-ILs, thermo-properties including solve enthalpy (ΔH sol ), entropy (ΔS sol ) and Gibbs free energy (ΔG sol ) were obtained. The research shows that DB-ILs perform well at the capturing CO 2 and can be regenerated four times.
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JOURNAL OF PHYSICAL CHEMISTRY B
·
2019
·
IF 2.923
Xueqian Guan,Zhiyu Huang,Hongsheng Lu,Dejun Sun
Binary mixtures of water and organic solvents are described as the aqueous solutions of organic solvents, which are usually spatially heterogeneous on the scale of a few molecular sizes but homogeneous on longer length scales, that is, microheterogeneity. For the water–organic solvent binary mixtures with microheterogeneity, most organic solvents are miscible with water at any ratio. Interestingly, some slightly water-miscible organic solvents can also be used to prepare binary mixtures with microheterogeneity. In this study, N,N-dimethylcyclohexylamine (DMCHA) was used to prepare binary mixtures with microheterogeneity and CO2 switchability. With the help of conductivity, Fourier–transform infrared spectroscopy, ultraviolet–visible spectroscopy, and dynamic light scattering measurements, we found that water molecules are hydrogen-bonded together to form clusters over the water content range of 9 to 27 wt %, exhibiting microheterogeneity in the binary mixture. The size of the water clusters increases slightly with increasing water content. What is more, the DMCHA–water mixtures can be reversibly split into two phases by alternate bubbling of CO2 and N2, exhibiting excellent CO2 switchability. The binary mixtures can be used as reaction media for the synthesis of CaCO3 nanoparticles. Binary mixtures with microheterogeneity can also be formed under high salinity or high temperature conditions or be prepared using other slightly water-miscible organic solvents, opening up more interesting possibilities for binary mixtures with microheterogeneity.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2019
·
IF 3.375
Yuan Zhao,Yidi Zhu,Tianle Zhu,Guiping Lin,Mingpan Shao,Wei Hong,Shiyu Hou
The series of polyethylenimine (PEI)-based solid sorbents were prepared by the wet-impregnation of PEI (Mw = 600) on the surface of six porous materials, i.e., mesoporous silicas (MCM-41, SBA-15, and KIT-6), mesoporous carbon (CMK-3), protonated titanate nanotube (PTNT), and fumed silica (FS). The resultant materials, denominated PEI/supports, were characterized by N2 adsorption/desorption at 77 K, mercury intrusion porosimetry (MIP), scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FT-IR), and X-ray photoelectron spectroscopy (XPS). CO2 adsorption on the PEI/supports was evaluated using 2 vol % CO2 in flowing air on a self-assembled fixed bed reactor. The observations made here show that relative to the other four sorbent counterparts, PEI/PTNT and PEI/FS exhibit better performance of CO2 adsorption, mainly attributed to their more abundant secondary macropores, together with more homogeneous PEI surface dispersion. For all the PEI/supports, the adsorption data of CO2 at various pressure equilibriums were modeled by the Langmuir dual-site isotherms. And the values of the fitted model parameters offer some hints that both chemisorption and physisorption are synchronously involved in these sorbent systems, one of which will govern the CO2 adsorption process, dependent on the nature of the supports used.
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CHEMISTRY OF MATERIALS
·
2019
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IF 10.159
Jingsong Cai,Juner Chen,Pingmei Zeng,Zhenfeng Pang,Xueqian Kong
Graphene oxides (GOs) are layered carbon materials composed of a mixture of oxygenated functional groups that can react with different molecules. Alkyl diamine molecules (ethylenediamine, butanediamine, or hexanediamine) can insert into the layers of GO and systematically expand its interlayer spacing from 0.762 nm to over 1.030 nm. In this work, we found that CO2 uptake maximizes at the interlayer spacing of 0.860 nm in GOs cross-linked by diamines. We characterized the subtle chemical and compositional differences among samples by Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, and solid-state NMR. In situ 13C NMR was applied at variable temperatures to investigate the adsorption mechanisms of CO2, which revealed both physically and chemically adsorbed CO2 in diamine-cross-linked GO matrices. In particular, we observed the unique state of CO2 that are physically trapped in GO layers with 0.860 nm spacing by van der Waals interactions. This state of CO2 was not observed in GOs with either smaller or larger interlayer spacings.
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Energy Technology
·
2018
·Vol. 7
·期 2
·325-332
·
IF 3.175
Ke Wang,Jie Hong,Zhongyun Zhou,Zhiwei Lin,Pengfei Zhao
High efficiency alkali nitrate-containing Li 4 SiO 4 sorbents were synthesized by a hydration technique to improve their sorption performances at low CO 2 concentrations. X-ray diffraction (XRD), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), differential scanning calorimetry (DSC), and thermogravimetric analyses were used to detect the characteristics of the samples. The results showed that the presence of KNO 3 and NaNO 3 induced small crystallite size, corrugated morphologies and the formation of eutectic phases, noticeably facilitating sorption processes. At the optimized additive amount of 0.035 mol %, NaNO 3 -containing Li 4 SiO 4 reached a maximum absorption capacity (≈34.6 wt %). Moreover, both alkali nitrate-containing Li 4 SiO 4 sorbents showed good cyclic properties, demonstrating their great potential for high-temperature CO 2 capture.
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