CHEMICAL ENGINEERING SCIENCE
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2024
·
IF 4.1
Hongwei Chen,Xiangqiong Jiang,Binyu Wang,Yongheng Ren,Bin Zhang,Jiabao Gui,Xili Cui,Linbing Sun,Jiuxing Jiang,Wenfu Yan,Jinping Li,Libo Li
Utilizing physical adsorption for ethylene purification from complex mixtures can significantly reduce the energy cost for production. The purification of multi-component systems through a single adsorption process presents a considerable challenge, largely stemming from the absence of customized strategies and thorough investigations into adsorption behaviours. We aim to understand adsorbents through a unique cage recognition approach and leverage these insights to develop an effective purification adsorbent, with the successful synthesis of SSZ-16 zeolite meeting requirements for multi-component purification. This zeolite, featuring a long aft supercage and a narrow gme cage construct two adsorption cages. The dense π -electron cloud of C 2 H 2 enables a stronger interaction in aft cage, while CO 2 is selectively captured within the environmentally compatible gme cage, demonstrating significantly higher C 2 H 2 and CO 2 adsorption capacity. The separation experiments reveal that SSZ-16 exhibits exceptional performance, with an unprecedented polymer-grade C 2 H 4 productivity of 2099.16 L/kg from the CO 2 /C 2 H 2 /C 2 H 4 mixture.
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CHEMISTRY OF MATERIALS
·
2021
·
IF 9.811
Xiangyang Yao,Kaihong Chen,Li-Qi Qiu,Zhi-Wen Yang,Liang-Nian He
Visible light-induced photocatalytic CO2 reduction reaction (CO2RR) is a feasible and promising option to tackle the greenhouse effect and energy crisis. Herein, two ferric porphyrin-based porous organic polymer semiconductors, hereafter referred to as POPn-Fe (porous organic polymers, n = 1 or 2, corresponding to a benzene/biphenyl unit as a linker between porphyrin units), are synthesized for the visible light-driven CO2RR to produce syngas. The CO/H2 evolution rates for POP2-Fe under irradiation >420 nm are found to successfully reach up to 3043 and 3753 μmol g–1 h–1, respectively. Interestingly, the experiment results imply that the ferric porphyrin site could be responsible for CO evolution and the uncoordinated porphyrin unit in POPn or POPn-Fe semiconductors may be obligate for H2 formation. Furthermore, as evidenced by Mott–Schottky plots, the extended π-conjugation with the biphenyl linker makes POP2-Fe a lower conduction band potential, which helps the ferric porphyrin sites capture electrons from the photosensitizer, thus producing more CO to realize selectivity control. Also, the efficient catalytic activity of POP2-Fe is presumably attributed to the accelerated charge transfer as well as facilitates photogenerated electron and hole separation. This work offers an elegant strategy to design and optimize earth-abundant metal visible light photocatalysis for CO2 reduction to syngas with CO/H2 ratio control.
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HIGH PERFORMANCE POLYMERS
·
2022
·
IF 1.73
Shuo Yan,Haibin Yu,Zan Chen
Membranes with both good permeation and selectivity are highly desired for gas separations. In this study, we synthesized a new 6FDA-type polyimide copolymer 6FDA-BDTA-ODA, and then an organic polymer of poly (N-vinylimidazole) was doped into the polyimide to prepare mixed matrix membranes (MMMs). We also studied the effect of poly (N-vinylimidazole) contents on the separation performance of MMMs. The results showed that the ideal selectivity for CO2/CH4 was improved by adding the poly (N-vinylimidazole) filler. The ideal selectivity reached 63.5 with 6 wt% poly (N-vinylimidazole) loading with the permeability of 29.2 Barrer. The highly permeable MMMs showed a considerably enhanced performance for CO2/CH4 that close to the 2008 Robeson upper-bound. The gas separation performance of the prepared MMMs for CO2/CH4 was improved compared to that of the pure polymer membrane, indicating that the copolyimide/poly (N-vinylimidazole) MMMs have promising applications in CO2/CH4 gas separation.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2022
·
IF 4.326
Guo-Cui Mao,Xiao-Tian Kan,Ming-Xiu Xiao,Wen-Long Liu,Bao-Xia Dong,Yun-Lei Teng
CaO is promising to be widely used to capture CO2. The produced CaCO3 can be considered as solid CO2, which is also a plentiful, convenient, and useful carbon resource. Here, for the first time, we report that an alkaline earth metal can selectively induce the hydrogenation of the CaO-captured CO2 (namely, the produced CaCO3) to CH4 under room-temperature ball-milling conditions. The effects of ball-milling conditions and different catalysts on the methanation performance were studied. The results show that the CH4 yield can reach 56.1%, and the CH4 selectivity is 100%. When adding metal Ni, the CH4 yield can be further increased. The experimental and density functional theory calculation results indicate that the in situ formed metal hydride plays a key role in the process of methanation. This work provides a novel and energy-saving method to convert the metal oxide-captured CO2/carbonate to CH4 at room temperature.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Xiaoqian Li,Dechao Wang,Hailong Ning,Yangyang Xin,Zhongjie He,Fangfang Su,Yudeng Wang,Jing Zhang,Hongni Wang,Liwei Qian,Yaping Zheng,Dongdong Yao,Mingtao Li
Porous liquids (PLs), as a novel liquid sorbent with permanent porosity, still present challenges such as high viscosity and melting temperatures. Herein, an efficient electrostatic repulsion strategy is proposed to engineer zeolitic imidazolate frameworks (ZIFs) type III PLs employing ZIF-8- g -BPEI nanoparticle stability dispersed into BPEI. The viscosity and melting temperatures of ZIF-8- g -BPEI PLs could be tailored via control particle size, grafting polymer, and concentration of porous nanoparticles . The existence of BPEI on the surface of ZIF-8- g -BPEI facilitates the stable dispersion of ZIFs nanoparticles in BPEI via the electrostatic repulsion as well as enhances CO 2 adsorption capacity of PLs. Moreover, the CO 2 adsorption amount of ZIF-8- g -BPEI-30 PLs is 6.5 times high than that of neat BPEI, suggesting the permanent free volume of ZIFs is retained in their corresponding PLs. Benefiting from the branched structure of BPEI grafted onto the outer surface of ZIFs , ZIF-8- g -BPEI-10 PLs remain liquified down to -71.1 °C, together with viscosity as 1.7 Pa·s −1 at 25 °C. Therefore, the electrostatic repulsion strategy opens an effective avenue to prepare novel liquid materials and shows numerous potential applications in gas adsorption and separation.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Yonghong Wang,Zhuo Jin,Xinru Zhang,Jinping Li
The incorporation of lamellar materials into polymer matrix can improve the gas separation performance of mixed matrix membranes (MMMs), which have great potential in chemical separation process. However, few intrinsic selectivity sites on MoS 2 sheets suppress further employment in the membrane separation. In this work, the vacancies and defects-containing MoS 2 sheets were prepared by high temperature oxidation and hydrothermal reaction in NaOH solution, and then L-cysteine-functionalized MoS 2 (Cys-MoS 2 ) was synthesized by a thiol-click chemistry reaction between S vacancies and thiol groups as confirmed by transmission electron microscope (TEM), Fourier-transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and N 2 absorption. After blending with polyether-block-amide (Pebax), the as-prepared MMMs showed outstanding mechanical properties as a result of the homogeneous dispersion of Cys-MoS 2 and hydrogen bonding between two phases as evidenced by attenuated total reflectance-FTIR, scanning electron microscope (SEM), thermogravimetric analysis (TGA) and differential scanning calorimetry (DSC). The highest permeability of 297 Barrer accompanied with a CO 2 /N 2 selectivity of 120 was obtained for MMMs loaded with 1.5 wt% Cys-MoS 2 , which were enhanced by 206.2 % and 124.7 % over the pristine Pebax membrane, respectively. Meanwhile, this value was superior to that of the previously reported Pebax-based MMMs, transcending 2019 upper bound. The enhanced gas separation performance is due to the improved CO 2 adsorption selectivity by the vacancies and defects of Cys-MoS 2 , while the amine groups carrier enhanced CO 2 reactivity selectivity.
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CHINESE JOURNAL OF CHEMISTRY
·
2020
·Vol. 38
·期 10
·1057-1064
·
IF 3.826
Chongyang Du,Yaofeng Chen
Summary of main observation and conclusion Transformation of CO 2 into valuable organic compounds catalysed by cheap and biocompatible metal catalysts is one of important topics of current organic synthesis and catalysis. Herein, we report the zinc powder catalysed formylation and urealation of amines with CO 2 and (EtO) 3 SiH under solvent free condition. Using 2 mol% zinc powder as the catalyst, a series of secondary amines, both the aromatic ones and the aliphatic ones, can be formylated into formamides. When primary aromatic amines were used as the substrates, the reactions produce urea derivatives. The electronic and steric effects from the substrates on the formylation and urealation reactions were observed and discussed. The recovery and reusability of zinc powder were investigated, showing the zinc powder can be reused in the formylation reaction without loss of catalytic activity. The analysis on the reactants/products mixture after filtering out the zinc powder showed the zinc concentration in the mixture is low to 1 ppm. The pathways for the formylation and urealation of amines with this catalytic system were also investigated, and related to the different substrates.
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CARBOHYDRATE POLYMERS
·
2018
·
IF 5.158
Xiang Li,Qinqin Xu,Hongwei Shen,Yuanlong Guo,Mouyi Wu,Ya Peng,Lihua Zhang,Zongbao Kent Zhao,Yu Liu,Haibo Xie
To overcome the natural recalcitrance of cellulose for glucose production in aqueous media catalyzed by enzyme, in this study, a dissolution pretreatment strategy was developed by using in situ formed CO 2 -based reversible ionic compounds (RICs)/DMSO mixed organic electrolytes under mild conditions. The influences of the constitution of RICs, CO 2 pressure, dissolution pretreatment time on the physic-chemical structure of cellulose were investigated systematically by FTIR, XRD, SEM, AFM towards in-depth understanding of the correlations between the pretreatment conditions, micro-scale structure and enzymatic saccharification of cellulose. The results showed that the tetramethyl guanidine (TMG) based RICs solvent system [TMGH] 2 + [O 2 COCH 2 CH 2 OCO 2 ] 2− /DMSO (X RICs = 0.1, X RICs : the mole fraction of the formed RICs in the mixture) presented the best performance, which was evidenced by 100% glucose yield after the dissolution-regeneration pretreatment strategy under mild conditions (T = 60 °C, Pco 2 = 2.0 MPa, t = 2 h). Furthermore, the solvent system have good recyclability and usability.
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JOURNAL OF MEMBRANE SCIENCE
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2021
·
IF 8.742
Nan Li,Zhi Wang,Jixiao Wang
Developing efficient membrane technology for CO 2 capture has aroused wide interest for environment conservation and emission reduction. Developing facilitated transport membranes is a potential strategy for improving CO 2 permeance and CO 2 /N 2 selectivity synchronously, based on the reversible reactions among carriers and CO 2 molecules. The reaction activity can be optimized by tuning the carrier mobility due to the enhanced water-swelling capacity. Here, thin-film composite (TFC) membranes containing water-swelling carboxymethyl chitosan (CMC) chains were prepared via interfacial polymerization process, aiming to improve CO 2 separation performance. As-prepared TFC membranes with different CMC loading have exhibited different Turing nanostructures , such as corrugated structures, octopus-branched structures and nodular structures. Water can enhance the activity of carriers in reversible reaction for facilitated transport membranes. TFC membranes with CMC have exhibited the enhanced water-swelling capacity, showing high CO 2 permeance of 1278 GPU together with CO 2 /N 2 selectivity of 89. This work put forward a simple and effective method to tune the membrane structure and enhance the facilitated transport.
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高影响因子
Polymer Chemistry
·
2024
·Vol. 15
·期 27
·2780-2789
·
IF 4.1
Ke Wang,Zilong Wang,Meiyu Si,Xiaofang Liu,Guiyan Liu,Yongfei Zeng
Three novel temperature/pH/CO2-triple-responsive homopolymers namely P(Et-N-EO2MA), P(THP-N-EO2MA) and P(Ph-N-EO2MA) were prepared by reversible addition–fragmentation chain transfer (RAFT) polymerization. They have the same backbone structure but different types of end substituents i.e., ethyl, tetrahydropyran, and the benzene ring, respectively. Subsequently, their responsive properties were studied. P(Et-N-EO2MA) has a lower critical solution temperature (LCST)-type cloud point (CP) in aqueous solution and is affected by many factors such as the molecular structure and weight, concentration, additives, pH and CO2. P(THP-N-EO2MA) is soluble in water, but in different buffer solutions, it shows a soluble–LCST–insoluble transition, and its LCST-type CP can also be adjusted by molecular weight and concentration. P(Ph-N-EO2MA) is insoluble in water, but reversible phase transformation can be achieved by adjusting the pH of the solution or injecting CO2, and it also shows different properties in buffer solutions and an upper critical solution temperature (UCST)-type CP in n-butanol. In addition, since P(Ph-N-EO2MA) is amphiphilic, it can be self-assembled in solution, and the release of Nile Red (NR) can be achieved under the stimulation of acid. The different properties of these homopolymers show the effect of substituents on the responsiveness of multistimuli-responsive polymers, which provides ideas for the design of stimuli-responsive polymers, and have good application prospects in the fields of self-assembly and controlled release.
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ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Jianli Liang,Qianqian Song,Jing Lin,Gen Li,Yi Fang,Zhonglu Guo,Yang Huang,Chun-Sing Lee,Chengchun Tang
Porous boron nitride (BN) materials have been considered as a promising material for CO2 capture and storage. It was found that the Cu2+ ion can modify the nucleation mechanism during the synthetic reaction between boric acid and melamine leading to the formation of Cu-loaded BN nanofibers with uniform and smaller diameter. Interestingly, the introduction of Cu was found to dramatically enhance the CO2 adsorption capacity of the BN nanofibers from 1.34 to 2.77 mmol g–1 (at 1 bar, 273 K). The Cu-loaded BN nanofiber not only shows a CO2 adsorption capacity comparable to those of state-of-the-art BN-based CO2 absorbents but also shows unprecedented high recyclability for repeated uses. The mechanisms of the copper-induced CO2 adsorption capacity enhancement were investigated with density-functional theory calculations. It was found that the incorporation of Cu can change the electron transfer between porous BN and CO2 to promote the affinity and adsorption capacity of CO2.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2020
·Vol. 26
·期 35
·7918-7922
·
IF 4.857
Yichen Zhou,Mingmin Jia,Xiongfei Zhang,Jianfeng Yao
Graphical Filling the voids : Etched ZIF-8 (ZIF-8-E) crystals permeated by open through pores of size about 100 nm have been introduced into a polyethersulfone membrane matrix. The resulting material shows enhanced CO 2 /N 2 separation performance (see scheme). Zeolite ZIF-8 has been etched with acid to form microporous ZIF-8-E crystals. These were then introduced into a polyethersulfone (PES) membrane matrix to enhance its CO 2 /N 2 separation performance. Open through pores of size about 100 nm formed in the ZIF-8 crystals allow the ingrowth of polyethersulfone chains, ensuring a reduction in the number of nonselective voids, thereby achieving better interaction between ZIF-8-E and PES. As a result, the CO 2 /N 2 separation performance of the ZIF-8-E/PES membrane increased significantly, showing a CO 2 permeability of 15.7 Barrer and a CO 2 /N 2 ideal selectivity of 6.5.
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高影响因子
危险品化学品经营许可证（带存储）