JOURNAL OF MEMBRANE SCIENCE
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2021
·
IF 8.742
Bingbing Yang,Lu Bai,Tingting Li,Liyuan Deng,Lei Liu,Shaojuan Zeng,Jiuli Han,Xiangping Zhang
Efficient separation and recovery of ammonia (NH 3 ) is essential for environmental protection and resource utilization. In this work, hybrid membranes for NH 3 separation through multiple-site interaction were developed by combining the unique features of ionic liquids (ILs) and a midblock-sulfonated block copolymer . The functionalized ILs ([2-Mim][NTf 2 ] and [Im][NTf 2 ]) with ammonia interaction sites were incorporated into the Nexar™ matrix, which greatly improves the affinity for NH 3 over nitrogen (N 2 ) and hydrogen (H 2 ). Benefited from the self-assembly of the block copolymer, the hybrid membranes primarily exhibit lamellar morphology. More continuous ionic domains with well-distributed ILs were formed in the hybrid membranes, contributing to forming interconnected channels for enhanced gas transport. In this case, addition of the ILs into the Nexar matrix significantly enhances NH 3 separation performance. Nexar/[Im][NTf 2 ]-25 membrane achieves the highest NH 3 permeability of 3565 Barrer and a maximum NH 3 /N 2 and NH 3 /H 2 ideal selectivity of 1865 and 364, respectively. The significantly enhanced NH 3 permeation compared with the neat Nexar membrane indicates the positive role of ILs in the hybrid membranes.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Wenjie Xiong,Mingzhen Shi,Lingling Peng,Xiaomin Zhang,Xingbang Hu,Youting Wu
CO 2 and H 2 S are considered impurities in natural gas that moderate the pace of environmental health. Developing highly efficient and cost-effective absorbents is of significance for sweetening natural gas. Herein, four superbase protic ionic liquids (SPILs) were prepared in this study. Typical physical properties (density, viscosity, and decomposition temperature) were also examined at ambient pressure. These SPILs show low viscosity values at ranging from 5.1 cP to 18.3 cP at 313.2 K. The solubility of H 2 S (0–1.0 bar), CO 2 (0–1.0 bar), and CH 4 (0–5.0 bar) was systematically measured at temperatures in the range of 298.2 K to 333.2 K. Impressively, the absolute solubility of H 2 S under 0.1 bar was found to be located at 4.31–5.15 mol/kg at 313.2 K, which is the highest value obtained among the reported results in the literature. The ideal selectivity of H 2 S/CH 4 and CO 2 /CH 4 (H 2 S or CO 2 solubility at 0.1 bar vs CH 4 solubility at 1 bar) at 313.2 K are in the ranges of 367–653 and 92.4–240, respectively. The interaction mechanism we explored was characterized by NMR and FT-IR spectroscopy. Thermodynamic parameters, such as enthalpy, Gibbs free energy, and entropy of dissolution were calculated from the temperature dependent solubility using the “deactivated model”. These SPILs are promising alternative candidates for the simultaneous removal of H 2 S and CO 2 in natural gas upgrading.
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ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Jiajia Liu,Xiaochen Tang,Huiling Lu,Yingjie Xu
To reveal the interactions between azole-anion-based ionic liquids (AILs) and propargyl alcohol (PA) and their effect on the carboxylative cyclization reaction of PA with CO2, three AILs, namely, [P66614][Im], [P66614][4-MeIm], and [P66614][4-BrIm], were synthesized and characterized. The interactions between the AILs with 2-methyl-3-butyn-2-ol (MBY) were investigated through IR and 1H NMR spectra and DFT calculations. The results indicate that azole-based anions can form H-bonds with the hydroxyl (O–H) and the alkynyl hydrogen atoms (C≡C–H) of MBY simultaneously, with the former much stronger than the latter, which is supported by the interaction energy and the distance of the H-bond from DFT calculations. Interestingly, the strength of the former always increases with the mole fraction of AIL (xAIL), while that of the latter first decreases and then increases, reaching a minimum at xAIL ≈ 0.4. Furthermore, the order of the strength of the two H-bonds is as follows: [P66614][Im] > [P66614][4-MeIm] > [P66614][4-BrIm], which is in good agreement with their basicity. According to the interactions between the AILs with MBY and combined with the reaction mechanism of MBY with CO2 promoted by AILs, it is evident that the increase in the basicity of the AILs enhances the H-bond between the AILs with O–H, thereby enhancing the activation of MBY and the subsequent CO2 conversion. However, this will also increase the interaction between AILs and C≡C–H, resulting in the deprotonation of C≡C–H and hindering the activation of MBY. Therefore, choosing a suitable basic AIL and controlling its ratio are the keys to the reaction of PA and CO2.
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JOURNAL OF POWER SOURCES
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2021
·
IF 9.127
Hongying Tang,David Aili,Kang Geng,Jian Gao,Qingfeng Li,Nanwen Li
Polymers containing organic cations are considered as promising materials for phosphoric acid (PA) doped high temperature polymer electrolyte membranes (HT-PEMs) due to higher PA retention and wider operation temperature range. However, the thermal/acidic stability of the organic cations remains to be determined. Herein, a series of model cations based on various (benz)imidazoliums are designed and prepared to assess the stability on molecular level under simulated operating conditions for HT-PEM fuel cell. NMR analysis indicates that C2, C4 and C5 substitutions show little effect on the stability while N1 and N2 substitutions show opposite effect. Among the N -functionalized derivatives, N , N -dimethyl (benz)imidazolium cations are fully stable while N -benzyl imidazoliums degraded severely due nucleophilic substitution with H 2 PO 4 − . On this background, blend membranes based on fully methylated polybenzimidazole (PBI) are prepared, and the swelling is balanced by introducing pristine PBI. The proton conductivity of the PA doped blending membrane with IEC of 1.2 mmol g −1 reaches 165 mS cm −1 and a peak power density of 863 mW cm −2 is demonstrated in H 2 /O 2 fuel cell test. These results lay a solid foundation for designing and developing durable high-performance HT-PEMs and fuel cell devices for green energy conversion applications.
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Advanced Materials Interfaces
·
2021
·Vol. 8
·期 21
·2101544
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IF 6.147
Guozheng Xia,Mei Lin,Yi Jiayu,Hu Jinkang,Li Bowen,Youbing Mu,Xiaobo Wan
How to realize fast and strong underwater adhesion has gained much attention recently. Although some mussel-inspired adhesives that can be cured underwater have been reported, reports on underwater adhesion with both high bonding strength and rapid curing capability are still rare. Furthermore, organic solvents are generally utilized in these adhesives, which are eco-unfriendly. Here, by taking advantages of the strong underwater adhesion capability of catecholic groups in mussel adhesion proteins (MAPs) and the fast curing capability of polyurethane (PU) prepolymer, a facile yet powerful strategy towards a fast-curing mussel-inspired underwater adhesive is reported. The biomimetic adhesive, PUP-PPG-DBHP, is a liquid composed of isocyanate-terminated polypropylene glycol (PPG) and isocyanate-terminated dopamine bis(hydroxymethyl)propionate (DBHP), which can be directly applied underwater without solvent dilution and reach an average bonding strength around 1.2 MPa at a curing time of only around 30 s on glass substrates. Meanwhile, underwater curing process of PUP-PPG-DBHP shows good tolerance toward pH value, ionic strength, and temperature change. Such an engineering adhesive opens an innovative and facile route to a feasible solution for underwater engineering field.
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BIOTECHNOLOGY PROGRESS
·
2021
·Vol. 38
·期 1
·e3218
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IF 2.681
Xiao-Jian Zhang,Feng-Yu Qi,Jia-Mei Qi,Fei Yang,Jiang-Wei Shen,Xue Cai,Zhi-Qiang Liu,Yu-Guo Zheng
The Candida antarctica lipase B (CALB) was embedded in the metal-organic framework, zeolitic imidazolate framework-8 (ZIF-8), and applied in the enzymatic synthesis of L -ascorbic acid palmitate (ASP) for the first time. The obtained CALB@ZIF-8 achieved the enzyme loading of 80 mg g −1 with 11.3 U g −1 (dry weight) unit activity, 59.8% activity recovery, and 92.7% immobilization yield. Under the optimal condition, ASP was synthesized with over 75.9% conversion of L -ascorbic acid in a 10-batch reaction. Continuous synthesis of ASP was subsequently performed in a packed bed bioreactor with an outstanding average space–time yield of 58.1 g L −1 h −1 , which was higher than ever reported continuous ASP biosynthesis reactions.
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PubMed
高影响因子
Chemosensors
·
2021
·Vol. 9
·期 8
·236
·
IF 3.398
Chuqing Zhang,Yang He,Jianbo Wu,Manqing Ai,Wei Cai,Ying Ye,Chunhui Tao,Pingping Zhang,Quan Jin
Real-time measurements of carbonate ion concentrations in the ocean are critical to advancing marine environmental monitoring and research into deep-sea hydrothermal activity. Herein, we report the first example of deep-sea hydrothermal field exploration using a carbonate ion-selective electrode (ISE). The novel carbonate ISE was composed of a Ni wire as substrate, carbon film as transducers and carbonate-selective membrane layers. This paper describes the preparation process of the electrode and characterises its performance via scanning electron microscopy (SEM) and electrochemical analysis. The detection limit of the electrode for CO32−is 2.821 × 10−6mol/L, the linear response range is 1.0 × 10−5–1.0 × 10−1mol/L and the Nernst slope was −30.4 mV/decade. In April 2021, the carbonate ISE was mounted on multi-parameter sensors with pH and Eh (redox) electrodes for the search of hydrothermal activity at the Southwest Indian Ridge. The simultaneous potential anomalies appeared at this carbonate electrode with the pH and Eh electrodes when passing through the hydrothermal field. The study of the hydrothermal field was supported by the in situ camera video and the sulphide samples. Additionally, the carbonate electrode provides enhanced information of water chemistry for the study of the hydrothermal field.Keywords:ion-selective electrode;carbonate determination;carbon film;hydrothermal field
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GREEN CHEMISTRY
·
2021
·Vol. 23
·期 16
·6090-6100
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IF 10.182
Xinxin Wang,Wu Tang,Yang Hu,Wenqiang Liu,Yichao Yan,Liang Xu,Cong Fan
An insoluble small-molecule organic compound [N,N′-bis(2-anthraquinone)]-perylene-3,4,9,10-tetracarboxydiimide (PTCDI-DAQ) can be a high-performance cathode in Li-ion batteries (LIBs). In half cells, PTCDI-DAQ delivers a peak specific capacity of 229 mA h g−1, along with the good retention of 82% over 3 months. Meanwhile, PTCDI-DAQ can still hold a capacity of 46 mA h g−1 at 25 A g−1. By using the reduced state (Li4TP) of lithium terephthalate (Li2TP) as an organic anode in the all-organic Li-ion batteries (OLIBs), our OLIBs can realize a high-energy density of 296 W h kg−1cathode in the voltage range of 0.2–3.2 V and fulfill a long lifespan over 20 000 cycles. To the best of our knowledge, the comprehensive performance of our PTCDI-DAQ II Li4TP OLIBs is currently one of the best pure-organic LIBs in the world.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Hao Ling,Qiufeng Mao,Sen Liu,Hongxia Gao,Juan Lv,Yu Mao,Zhiwu Liang
Aqueous amine-based CO2 capture is considered as the most mature and applicable CO2 capture method for post-combustion. With the CO2 capture process running for a long time, the degradation of aqueous amine-based is inevitable, and the degradation products are numerous and complicated. Therefore, the performance evaluation of aqueous amine solutions containing degradation products is crucial in both guiding the selective removal of degradation products and maintaining or reducing of the solution cyclic utilization rate. Unfortunately, a simple and effective way to increase the economic feasibility of the CO2 capture process after accumulated degradation products remains absent, and little attention has been paid to the real effect of degradation products on the CO2 capture performance in aqueous amine solutions. In this work, we propose a simple method to evaluate the performance and regeneration energy of aqueous monoethanolamine (MEA) solutions accumulating single degradation products based on the fast-bubbling reactor. Using this method, it is possible to quickly determine the key degradation products that affect the performance of aqueous MEA solutions so as to achieving clearer optimization, more direct purification, and a reduced solution cyclic utilization rate.
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Nanoscale
·
2021
·Vol. 13
·期 7
·4140-4150
·
IF 7.79
Yongjie Zhang,Ning Feng,Shujin Zhou,Xia Xin
Gold nanoclusters (AuNCs) are among the most promising organic–inorganic hybrid luminescent materials for various applications. The current development of AuNCs majorly focuses on controlling their luminescence properties. Herein, we report a new strategy to facilely construct two different nanocomposites featuring enhanced photoluminescence based on mercaptopropionic acid-protected AuNCs (MPA-AuNCs). Through co-assembly with Zn2+ and 2-methylimidazole (2M-IM), the weak luminescence of MPA-AuNCs evolved into either intense blue-green or orange emission at different concentration ratios of additives. HR-TEM and spectroscopic characterization studies revealed that the intense blue-green emission was ascribed to the formation of ZnS quantum dots (QDs) on the outer surface of AuNCs (AuNCs@ZnS), while the strong orange emission originated from the primitive MPA-AuNC core encapsulated by a cubic ZIF-8 shell (AuNCs@ZIF-8). The AuNCs@ZnS nanocomposite was further applied as an exceptional chemical sensor for selective detection of Pb2+ and Fe3+via different quenching mechanisms, and the AuNCs@ZIF-8 composite was applied for fabricating light-converting devices. The co-assembly of AuNCs with Zn2+ and imidazole derivatives provides a facile strategy for acquiring differentiated nanomaterials that have versatile potential applications in chemical detection and light-converting devices.
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高影响因子
JOURNAL OF POWER SOURCES
·
2021
·
IF 9.127
Zhou Zhong,Xiao Xu,Aihui Cao,Weifeng You,Zhijie Tao,Longtian Kang
The sluggish oxygen evolution reaction (OER) attracts increasing attention for the storage and/or conversion of clean energy. However, the whole design of precursor and product is studied a few for efficient photocatalytic and electrocatalytic water oxidation . Here, we report the large-scale synthesis of one-dimensional (1D) nanohybrids (NHs) of 50-nm nickel perylene diimide (Ni-PDI) nanowires loading iron hydroxide (Fe(OH) 3 ) nanoparticles through one-step hydrothermal reaction . The Fe(OH) 3 @Ni-PDI NHs as OER photocatalyst possess the super activity, even high electrocatalytic performance after pyrolysis . Under visible light (λ > 420 nm), the photocatalytic oxygen evolution rate of 22,000 μmol g −1 h −1 can be achieved via the synergy between 1D Ni-PDI nanowires and in-situ generated iron (oxy)hydroxide as cocatalyst . Through pyrolysis of 1D Fe(OH) 3 @Ni-PDI NHs, the NiFe nanoparticles covered by NiFe 2 O 4 layer can be synthesized on 30-nm nitrogen-doped carbon nanowires (NiFe/NiFe 2 O 4 @NC). After optimizing the mole ratio of nickel to iron atoms (2:1) and pyrolysis temperature (800 °C), as-obtained sample exhibits the OER activity with the overpotential of 256 mV at 10 mA cm −2 and Tafel slope of 40 mV dec −1 in 1.0 M KOH. The work provides a universal strategy to design 1D nanostructure for efficient OER catalysis.
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Journal of Materials Chemistry C
·
2020
·Vol. 9
·期 1
·238-248
·
IF 7.059
Qigao Shang,Nannan Liu,Dan You,Qingrong Cheng,Guiying Liao,Zhiquan Pan
Two coordination polymers, {[Cu3(tib)4(NO3)4(H2O)]·2NO3·2.96H2O}n (1) and {[Ni(tib)2]·2NO3}n (2), were synthesized by a solvothermal reaction using a flexible tripodal ligand, 1,3,5-tris(imidazol-1-ylmethyl)benzene (TIB), and metal salts; the polymers were characterized by X-ray diffraction, Fourier transform infrared spectroscopy, thermogravimetric analysis, X-ray photoelectron spectroscopy and UV-vis diffuse reflectance spectra. The two complexes exhibited excellent active performance for photodegradation of tetracycline (TC) and photocatalytic hydrogen evolution under visible light. Control experiments revealed clearly that the pH value plays an important role in TC degradation, especially in alkaline solution; 93.21% of tetracycline was degraded by complex 1 within 60 min. In addition, using a Pt cocatalyst, the visible-light-driven photocatalytic H2 evolution rate of complex 2 reached 681.66 μmol h−1 g−1. Moreover, the photocatalysts can remain stable and retain high photocatalytic activity after several cycles of reuse. These MOF-based photocatalysts will provide new efforts for environmental purification and hydrogen evolution.
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