APPLIED CATALYSIS A-GENERAL
·
2018
·
IF 4.521
Pengjing Chen,Guofeng Zhao,Ye Liu,Yong Lu
A series of Ni 5 Ga 3 / m -SiO 2 /Al 2 O 3 /Al-fiber ( m = 0, 0.5, 1.0, 3.0 and 5.0 wt%) catalysts have been developed for CO 2 hydrogenation to methanol at ambient pressure. Microfibrous-structured SiO 2 /Al 2 O 3 /Al-fiber supports are obtained though endogenous growth of free-standing boehmite (AlOOH) nanosheets onto a three-dimensional (3D) network of 60 μm-Al-fiber thin felt with the aid of steam-only hydrothermal oxidation reaction between Al metal and H 2 O (2 Al + 4H 2 O → 2 AlOOH + 3H 2 ), followed by calcination and SiO 2 -modification using silica sol. The bimetallic Ni 5 Ga 3 nanoparticles are then placed onto the pore surface of as-obtained SiO 2 /Al 2 O 3 /Al-fiber support by co-impregnation method using Ni and Ga nitrates as precursors followed by reduction in H 2 at 630 °C. The promising Ni 5 Ga 3 /1-SiO 2 /Al 2 O 3 /Al-fiber catalyst is capable of converting 2.3% CO 2 into CH 3 OH with a high selectivity of 86.7% as well as 10.3%/3.0% selectivities to CO/CH 4 at 210 °C, for a feed of CO 2 /H 2 /N 2 (2/6/1, molar ratio). Such microfibrous-structured catalyst design combines the promising catalytic performance of Ni 5 Ga 3 with the enhanced heat transfer and high permeability of the Al 2 O 3 /Al-fiber support. The effect of SiO 2 loading on the formation of Ni 5 Ga 3 alloy nanoparticles is also discussed.
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Chemical Engineering and Processing-Process Intensification
·
2020
·
IF 3.731
Yuxin Wu,An Chen,Xueyan Liu,Jianhong Xu,Yundong Wang,Kathryn Mumford,Geoffrey W. Stevens,Weiyang Fei
Considered as an important C1 source on earth, carbon dioxide (CO 2 ) utilization and fixation has aroused great attention. Synthesis of cyclic carbonate are one of the most widely industrialized routes. Ionic liquids have been studied for highly efficient cyclic carbonate production due to their distinguished characteristics. In this work, highly efficient synthesis of propylene carbonate catalyzed by [bmim]Br was achieved via a continuous-flow microreaction system. Based on that, influence factors and kinetics parameters for propylene carbonate synthesis were obtained. And the flow patterns were investigated via transparent tube, which were proved to be slug flow. The activation energy for [bmim]Br in this microreaction system was 57.4 kJ/mol with the temperature range from 110 to 140 ℃, and the reaction was found to follow first-order on PO and CO 2 concentrations, and first-order on [bmim]Br concentration. Verification of the kinetic models was also studied and proved a less than 12 % error range.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2022
·
IF 4.831
Kaixiang Ji,Fangshuo Liu,Tesfaye Hailemariam Barkae,Shuai Quan,Abdallah M. Zeid,Wei Zhang,Jianping Li,Guobao Xu
N -hydroxyphthalimide (NHPI) is an efficient organic catalyst and an important chemical raw material which can be used as an intermediate in organic synthesis of drugs and pesticides. In this study, NHPI has been used as a coreactant of lucigenin chemiluminescence (CL) for the first time. The CL of the developed system is significantly enhanced in the presence of Co 2+ . Therefore, we developed a novel lucigenin-NHPI CL method coupled with flow injection analysis for the sensitive, precise, and selective determination of Co 2+ . The linear range of this method is 1–1000 nM, and the detection limit is 67 pM (S/N = 3). In addition, this method has a good selectivity for Co 2+ . It has been applied to the detection of Co 2+ in lake water, and the standard recovery rate is 95.9–103.2%, indicating that the method is feasible.
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RSC Advances
·
2020
·Vol. 10
·期 59
·35740-35752
·
IF 3.119
Lei Wang,Tianzeng Ma,Shaomeng Dai,Ting Ren,Zheshao Chang,Mingkai Fu,Xin Li,Yong Li
The research of thermochemical CO2 splitting based on perovskites is a promising approach to green energy development. Performance evaluation was performed towards the doped perovskite LaCo0.7Zr0.3O3 (LCZ-73) based two-step thermochemical CO2 splitting process thermodynamically based on the experimentally derived parameters for the first time. The impacts of vacuum pump and inert gas purge to reduce oxygen partial pressure and CO2 heating on the performance parameter ηsolar-to-fuel have been analyzed. The results showed that at the PO2 of 10−5 bar, non-stoichiometric oxygen δ increased by more than 3 times as the reduction temperature varied from 1000 °C to 1300 °C, however, no significant deviation of δ was observed between 1300 °C and 1400 °C. The reaction enthalpy ranged from 60 to 130 kJ mol−1 corresponding to δ = 0.05–0.40. Comparing the abovementioned two ways to reduce the oxygen partial pressure, the ηsolar-to-fuel of 0.39% and 0.1% can be achieved with 75% and without heat recovery with the CO2 flow rate of 40 sccm under experimental conditions, respectively. The energy cost for CO2 heating during the thermodynamic process as the nCO2/nLCZ-73 increases was obtained from the perspective of energy analysis. The ratio of nCO2/nLCZ-73 at lower temperature required more demanding conditions for the aim of commercialization. Finally, the ability of perovskite to split CO2 and thermochemical performance were tested under different CO2 flow rates. The results showed that high CO2 flow rate was conducive to the production of CO, but at the cost of low ηsolar-to-fuel. The maximum solar-to-fuel efficiency of 1.36% was achieved experimentally at a CO2 flow rate of 10 sccm in the oxidation step and 75% heat recovery.
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Frontiers of Chemical Science and Engineering
·
2024
·Vol. 18
·期 11
·1-10
·
IF 4.3
Liang Haoting,Zhao Qiao,Liu Shengkun,Wei Chongyang,Wang Yidan,Wang Yue,Huang Shouying,Ma Xinbin
The Fe-Mn bimetallic catalyst is a potential candidate for the conversion of CO 2 into value-added chemicals. The interaction between the two metals plays a significant role in determining the catalytic performance, however which remains controversial. In this study, we aim to investigate the impact of tuning the proximity of Fe-Mn bimetallic catalysts with similar nanoparticle size. And its effect on the physicochemical properties of the catalysts and corresponding performance were investigated. It was found that closer Fe-Mn proximity resulted in enhanced CO 2 hydrogenation activity and inhibited CH 4 formation. The physiochemical properties of prepared catalysts were characterized using X-ray diffraction, H 2 temperature programmed reduction, and X-ray photoelectron spectroscopy, revealing that a closer Fe-Mn distance promoted electron transfer from Mn to Fe, thereby facilitating Fe carburization. The adsorption behavior of CO 2 and the identification of reaction intermediates were analyzed using CO 2 -temperature programed desorption and in situ Fourier transform infrared spectroscopy, confirming the intimate Fe-Mn sites contributed to CO 2 adsorption and the formation of HCOO* species, ultimately leading to increased CO 2 conversion and hydrocarbon production. The discovery of a synergistic effect at the intimate Fe-Mn sites in this study provides valuable insights into the relationship between active sites and promoters.
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MATERIALS SCIENCE FORUM
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2022
·
IF 0
Jin Yang Zhang,Jin Ling Li,Qian Qiao,Rui Wang,Fei Liu,Hai Ning Na,Jin Zhu
In this paper, cellulose solution was obtained by dissolving cellulose in CO2 switchable solvent, and the CNF spinning solution was prepared by mixing cellulose solution with cellulose nanofibrils (CNF) by physical blending. CNF reinforced all-cellulose composite fibers were prepared by wet-spinning. The spinning solution with good dispersion of CNF can be obtained. The rheological property test showed that the solution has spinnability. The composite fibers were subsequently prepared by wet-spinning. The structure and properties of the composite fibers were analyzed by FT-IR, XRD, SEM, TGA, and mechanical properties testing. The results showed that the chemical structure of the composite fiber was the same as that of cellulose, but the aggregate structure became amorphous, which resulted in deceased thermal stability. The composite fibers had dense and solid structure without any cavity. The mechanical strength of the composite fiber was upto 1.12cN/dtex.
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Frontiers of Chemical Science and Engineering
·
2024
·Vol. 18
·期 11
·1-11
·
IF 4.3
Fu Huiyu,Wu Jiewen,Liang Changhai,Chen Xiao
With the advantages of low raw material cost and 100% atom utilization, the synthesis of high value-added chemical product cyclic carbonates by the cycloaddition of CO 2 to epoxides has become one of the most prospective approaches to achieve the industrial utilization of CO 2 . In the reported catalytic systems, the complexity of the catalyst synthesis process, high cost, separation difficulties, and low CO 2 capture limit the catalytic efficiency and its large-scale application. In this paper, Ag nanoparticles loaded on polyethyleneimine (PEI)-modified UiO-66-NH 2 (Ag/PEI@UiO-66-NH 2 ) are successfully synthesized by in situ immersion reduction. The Ag nanoparticles and the amino groups on the surfaces of PEI@UiO-66-NH 2 contribute to the adsorption of CO 2 and polarization of C–O bonds in epoxides, thereby boosting the conversion capability for the CO 2 cycloaddition reaction. At the amount of propylene oxide of 0.25 mol and the catalyst dosage of 1% of the substrate, the yield and selectivity of propylene carbonate are up to 99%. In addition, the stability and recyclability of Ag/PEI@UiO-66-NH 2 catalyst are attained. The Ag/PEI@UiO-66-NH 2 catalyst also demonstrates a wide range of activity and distinctive selectivity toward cyclo-carbonates in the cycloaddition of CO 2 to epoxides. This work provides a guide to designing a highly efficient catalyst for in situ capture and high-value utilization of CO 2 in industrial applications.
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JOURNAL OF MATERIALS SCIENCE
·
2021
·Vol. 56
·期 18
·10990-10999
·
IF 4.22
Guo Ding,Zhang Juan,Liu Genyan,Luo Xiaogang,Wu Fengshou
Abstract The chemical fixation of CO 2 into epoxides to afford cyclic carbonates has received considerable attention due to the 100% atom economy, which is in accordance with the concept of green chemistry and sustainable development. Here, we develop a facile and high-output strategy to fabricate cobalt phthalocyanine-based nanodots (CoPc-NDs) by the carbonization of citric acid and cobalt phthalocyanine complex. Due to the high thermal stability of phthalocyanine, the macrocycle is well preserved in the core of nanodots under the controlled hydrothermal temperature. The as-prepared CoPc-NDs disperse well in water with a nanoscale size about 70 nm. The morphology and chemical composition of CoPc-NDs are characterized by transmission electron microscopy, dynamic laser scattering, X-ray powder diffraction, X-ray energy spectrum, and absorption spectrum. Compared with the organometallic complex, such as cobalt tetra-nitrophthalocyanine and cobalt tetra-aminophthalocyanine, CoPc-NDs show better catalytic performance for the conversion of epoxides into carbonates. The kinetic experiments of three catalysts are investigated and compared under the same conditions using styrene oxide as substrate. Finally, a tentative mechanism for the catalysis was proposed and described. Graphical abstract
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Chemical Engineering and Processing-Process Intensification
·
2019
·
IF 3.031
Yanchi Jiang,Zhongxiao Zhang,Aiwei Mu,Liu Yang,Jian Liu,Ziqi Zhao,Mengchuan Jia,Junjie Fan
Chemical absorption technology has been wildly demonstrated in industry, the absorbents have become one of the most decisive factors for the process intensification of CCS technology. In this work, two schemes about bended amine and nanofluid were adopted to develop high-performance TETA-based absorbent. A bubble reaction experimental system was established to extract key data of absorbents’ properties. An AHP model was applied by setting up characteristic matrices to determine the CO 2 capture capacities of the overall aspects. The results show that the configuration of 10 wt. %TETA + 5.0 wt. %AMP has the optimal CO 2 capture performance with the highest score of 0.763 in blended amine category. The performance of nanofluids are generally higher than the blank TETA solution, though it triggers a 0.6%–3.1% growth of Purchase cost. The AHP score increases first and then declines with the rising of nanoparticle’s mass fraction, and the highest score is given to the activator of 0.1 wt. % TiO 2 . For the configurations of nanofluids- surfactants, the citrate sodium shows a superior overall CO 2 capture performance than Triton X-100, and the reasonable mass fraction of citrate sodium is considered as 0.05 wt. % with the AHP score of 0.792.
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Nature Communications
·
2020
·Vol. 11
·期 1
·1-13
·
IF 12.121
Zhao Fulai,Feng Yiyu,Wang Yu,Zhang Xin,Liang Xuejing,Li Zhen,Zhang Fei,Wang Tuo,Gong Jinlong,Feng Wei
The discovery of graphene and graphene-like two-dimensional materials has brought fresh vitality to the field of photocatalysis. Bandgap engineering has always been an effective way to make semiconductors more suitable for specific applications such as photocatalysis and optoelectronics. Achieving control over the bandgap helps to improve the light absorption capacity of the semiconductor materials, thereby improving the photocatalytic performance. This work reports two-dimensional −H/−OH terminal-substituted siligenes (gersiloxenes) with tunable bandgap. All gersiloxenes are direct-gap semiconductors and have wide range of light absorption and suitable band positions for light driven water reduction into H 2 , and CO 2 reduction to CO under mild conditions. The gersiloxene with the best performance can provide a maximum CO production of 6.91 mmol g −1 h −1 , and a high apparent quantum efficiency (AQE) of 5.95% at 420 nm. This work may open up new insights into the discovery, research and application of new two-dimensional materials in photocatalysis.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Yikang Huang,Liang Zhu,Ning Zeng,Pinjie Wang,Ge Gao,Wufeng Jiang,Xiaoshan Li,Liqi Zhang
Developing amine solutions with low energy consumption is of great significance for CO 2 capture technology. Currently most of studies focused on reducing sensible heat and heat of vaporization by anhydrous absorbents and phase-change absorbents based on amines. It should be noted that CO 2 reaction heat of amines is also an important section for energy consumption. In this work, CO 2 reaction heat of 7 secondary amines was investigated aiming to reveal structure–activity relationship between CO 2 reaction heat and the length of the carbon chain, methyl side chain and hydroxyl group in secondary amines. The CO 2 reaction heat of 7 secondary amines was directly measured by microcalorimeter with high precision. Results showed that increasing the length of carbon chain, introducing hydroxyl group and removing methyl side chain in secondary amines could increase CO 2 reaction heat. The lengthening of carbon chain and the addition of the hydroxyl group led to an increase in the electronegativity in N atom of the secondary amines, thereby increasing the reactivity and reaction heat of the secondary amine. The steric hindrance caused by methyl side chain reduced the reactivity and reaction heat of secondary amine. This study could help to screen and develop energy-saving secondary amine absorbents for CO 2 capture.
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CATALYSIS LETTERS
·
2021
·Vol. 152
·期 3
·781-790
·
IF 3.186
Yao Jie,Sheng Mengdi,Bai Shiyang,Su Hongjing,Shang Hui,Deng Han,Sun Jihong
Three mesoporous silica materials (MCM-41, MSN and BMMs) possessing different morphologies but similar hexagonal arranged mesopores with almost the same pore size (2–3 nm) were functionalized by Zn and [1-(trimethoxysilyl)propyl-3-methylimidazolium] ionic liquid (ILs) via post-grafting treatment. The ILs grafted mesoporous silicas were then characterized by porosity, microscopy and SAXS techniques, and the successful loading of Zn and ILs, as well as the different distribution of functional groups in different supports were shown. Furthermore, the cycloaddition reaction of CO 2 with epoxide was employed to evaluate the influences of the ILs distribution, which was proved to be caused mainly by varying morphologies of different supports. All the catalysts showed good catalytic activities. Interestingly, at low temperature, the inter particle supported ILs in BMMs had the highest catalytic efficiency, while the aggregation grafting ILs on MCM-41 present the lowest activity. However, the mesoporous silicas with ordered arranged nanopores present the superiority at higher temperature. The results highlight the crucial role played by the morphology of the supports. Graphical abstract
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危险品化学品经营许可证（带存储）