CHEMICAL ENGINEERING JOURNAL
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2019
·
IF 8.355
Tianqi Zhang,Jian Yin,Ying Pan,Enhua Liu,Dongxia Liu,Jianqiang Meng
Synthesis of cyclic carbonates via cycloaddition of CO 2 to epoxides is an important strategy for CO 2 valorization. However, efficient and easy-to-handle catalytic system for this type of reaction at mild conditions is still rare. In this work, we present a polyimide-based catalytic membrane with hierarchical pore structure for flow through synthesis of cyclic carbonates at mild conditions. The membrane was fabricated by incorporating a porous and metallized poly-melamine-formaldehyde (Zn@PMF) into phase inversed polyimide (PI) matrix. Upon in-situ crosslinking with tris(2-aminoethyl)amine, the solvent-resistant PI membrane can not only facilitate the CO 2 adsorption and immobilize the catalysts, but also promote mixing by flow-through operations. As a result, the nanocomposite membrane exhibited an excellent catalytic performance with a maximum TOF value of 3362 h −1 at ambient conditions. This catalytic activity is not only higher than the Zn@PMF particle but also is the highest among reported catalysts under the similar reaction conditions. Its high catalytic performance was also confirmed in CO 2 cycloaddition in a synthetic flue gas stream.
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ACS Applied Materials & Interfaces
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2019
·
IF 8.456
Liang Qiu,Haoran Zhang,Bo Wang,Yong Zhan,Chengfen Xing,Cai-Yuan Pan
CO2-responsive polymeric nano-objects with assembly-related aggregation-induced emission (AIE) are obtained via polymerization-induced self-assembly (PISA) of 2-(dimethylamino)ethyl methacrylate (DMAEMA), 2-(4-formylphenoxy)ethyl methacrylate (MAEBA), and 4-(1,2,2-triphenylvinyl)phenyl methacrylate (TPEMA). These nano-objects exhibit, depending on the feed of MAEBA, a morphology evolution process from spherical micelles to vesicles. Due to the presence of DMAEMA units, CO2 promotes morphology transformation of the nano-objects from spheres to a mixture of “jellyfish” and vesicles and vesicles to complex vesicles. Moreover, TPEMA endows the AIE feature to these nano-objects, offering a strategy to monitor the morphology evolution process in real time. Thus, this approach is significant for exploring the assembly mechanism of copolymer in polymerization-induced self-assembly and designing multistimuli-responsive polymeric nanomaterials with tunable morphologies and sizes.
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高影响因子
APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Huiqin Wang,Jingru Guan,Jinze Li,Xin Li,Changchang Ma,Pengwei Huo,Yongsheng Yan
In this work, the ordered mesoporous CeO 2 (m-CeO 2 ) was successfully fabricated via the nanocasting pathway, through using SBA-15 as a hard template. Besides, g-C 3 N 4 /Ag/m-CeO 2 composite was successfully constructed by calcination method. Meanwhile, the obtained samples were investigated by series of test techniques. The XRD, SEM and TEM results show that the m-CeO 2 and Ag/m-CeO 2 with the ordered mesoporous trait. Besides, the EPR, Raman and XPS results suggest that the oxygen vacancies (O v ) and Ce 3+ and Ce 4+ are in g-C 3 N 4 /Ag/m-CeO 2 . In addition, the ordered mesostructure is favorable for the CO 2 molecular movement and adsorption/desorption reaction. The g-C 3 N 4 nanosheets, a promising material possessing suitable conductor band, large specific area, non-toxicity, and outstanding chemical stability, is a candidate semiconductor for CO 2 conversion. The introduction of g-C 3 N 4 nanosheets to Ag/m-CeO 2 overcomes the photocorrosion of Ag nanoparticles and Ag facilitate the transfer of photogenerated electrons. The photocatalytic activity results show that when the loading of Ag is 7 wt%, the g-C 3 N 4 /7Ag/m-CeO 2 composite exhibits the superiority activity for CO 2 photoconversion to CO (13.94 μmol/g) and CH 4 (7.39 μmol/g) under UV-irradiation in 10 h.
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RSC Advances
·
2019
·Vol. 9
·期 65
·37733-37738
·
IF 3.049
Yanghe Fu,Jieyu Wu,Rongfei Du,Ke Guo,Rui Ma,Fumin Zhang,Weidong Zhu,Maohong Fan
Defect engineering can be a promising approach to improve the photocatalytic performance of metal–organic frameworks (MOFs). Herein, a series of defective NH2-UiO-66(Zr) materials were synthesized via simply controlling the synthesis temperature, with concentrated HCl as the modulator and then these as-prepared samples were used to systematically investigate the effects of their structural defects on photocatalytic CO2 reduction. Remarkably, these MOFs with defects exhibit significantly enhanced activities in photocatalytic CO2 reduction, compared with the material without defects. The defect engineering creates active binding sites and more open frameworks in the MOF, and thus facilitates the photo-induced charge transfer and restrains the recombination of photo-generated charges efficiently. The current work provides an instructive approach to improve the photocatalytic efficiency by taking advantage of the structural defects in MOFs, and could also inspire more work on the design of advanced defective MOFs.
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JOURNAL OF MOLECULAR LIQUIDS
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2019
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IF 4.561
Sehee Kang,Yongchul G. Chung,Jo Hong Kang,Hojun Song
In this study, dual amino group functionalized imidazolium amino acid ionic liquids (AAILs) were synthesized from imidazole , bromoalkylamine, and amino acids. 1-(3-aminopropyl)-3-(2-aminoethyl)imidazolium hydroxide ([Apaeim][OH]), 1-propyl-3-(2-aminoethyl)imidazolium hydroxide ([Paeim][OH]), and 1-ethyl-3-(2-aminoethyl)imidazolium hydroxide ([Eaeim][OH]) were synthesized in two-steps, while [Apaeim][amino acid], [Paeim][amino acid], and [Eaeim][amino acid] were synthesized in three-steps. The structures of the synthesized AAILs were confirmed by 1 H NMR analysis. Moreover, the CO 2 absorption mechanism of [Apaeim][OH] was confirmed by FT-IR and 13 C NMR analyses. Subsequently, CO 2 absorption-desorption tests were conducted under at 15 vol% CO 2 , 313 K and atmospheric pressure. The cation and anion effects on the ionic liquid absorbents were also investigated. Among the tested ionic liquid solutions, 30 wt% [Apaeim][OH] and 30 wt% 1-(3-aminopropyl)-3-(2-aminoethyl)imidazolium alaninate ([Apaeim][ala]) displayed the best performances. Thus, both presented CO 2 cyclic capacities 2.2-fold higher than that of the benchmark CO 2 absorbent 30 wt% monoethanolamine (MEA), while their viscosities were comparable to that of 30 wt% MEA. Notably, 30 wt% [Apaeim][ala] show great potential as a CO 2 absorbent due to its high CO 2 cyclic capacity and low viscosity.
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Solar RRL
·
2019
·Vol. 4
·期 8
·1900416
·
IF 0
Huang Jing Wei Li,Huimin Zhou,Kejun Chen,Kang Liu,Shi Li,Kexin Jiang,Wenhao Zhang,Yanbo Xie,Zhou Cao,Hongmei Li,Hui Liu,Xiaowen Xu,Hao Pan,Junhua Hu,Dongsheng Tang,Xiaoqing Qiu,Junwei Fu,Min Liu
Directly using solar energy to realize photocatalytic reduction of CO 2 to hydrocarbon fuels is an effective tactics to solve the energy crisis and carbon emission. Although graphite carbon nitride (g-C 3 N 4 ) has been widely studied as a star photocatalyst for CO 2 reduction, the extremely fast charge recombination rate seriously limits its performance. Loading suitable co-catalysts to construct an effective junction is considered an efficient way to solve this issue and promote photocatalytic performance. In this work, metallic molybdenum dioxide (MoO 2 ) is dispersed on g-C 3 N 4 nanosheets to construct a Schottky junction photocatalyst. The Schottky junction between MoO 2 and g-C 3 N 4 induces efficient charge separation and transfer. As a result, the optimal MoO 2 /g-C 3 N 4 Schottky junction photocatalyst exhibits a 15 times higher CH 4 yield and five times higher CO yield compared with pure g-C 3 N 4 . This article provides a new route to construct a Schottky junction for boosting photocatalytic activity.
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MATERIALS RESEARCH BULLETIN
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2019
·
IF 3.355
Houde She,Ziwei Zhao,Wencai Bai,Jingwei Huang,Lei Wang,Qizhao Wang
Photocatalytic CO 2 reduction is considered as a feasible approach for solving greenhouse effect and energy shortage. Promoting electron migration and inhibiting electron-hole recombination are key challenges for efficient photocatalytic CO 2 reduction. Here, we successfully synthesized Cu:TiO 2 -CS composite as photocatalyst by a facile solvothermal method to improve the high-catalytic effect on CO 2 reduction. The as-prepared composite exhibits excellent photocatalytic CO 2 reduction performance under 300 W xenon lamp irradiation, with the yields of CO and CH 4 up to 4.48 μmol/g and 5.34 μmol/g, which is 10 times higher than that of TiO 2 . This impressive amelioration can be attributed to the synergy of organic polymer (chitosan) and inorganic material (Cu:TiO 2 ). This work may provide a constructing guidance in designing the composite photocatalyst concerning CO 2 photocatalytic reduction.
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CARBOHYDRATE POLYMERS
·
2019
·
IF 6.044
Yingju Miao,Hongchao Luo,Manoj Pudukudy,Yunfei Zhi,Wenbo Zhao,Shaoyun Shan,Qingming Jia,Yonghao Ni
Old corrugated containers with low recyclability were used as raw materials to synthesize a series of aerogels with varying cellulose concentrations in NaOH/urea solution via a freeze-drying process. The resulting aerogels had a rich porous structure with specific surface areas in the range of 132.72–245.19 m 2 .g −1 and mesopore volumes in the range of 0.73–1.53 cm 3 .g −1 , and were tested for CO 2 sorption at ambient temperature and pressure, displaying excellent CO 2 adsorption capacities in the range of 1.96–11.78 mmol.g −1 . Furthermore, the CO 2 /N 2 selectivity of aerogels decreased with decreasing specific surface area, which was mainly caused by the decrease in CO 2 capture. In addition, the CO 2 sorption capacity of the sample with 2% cellulose content, CA-2, exceeded the values reported so far for many other sorbents with higher specific surface areas, and showed reasonable cyclic stability for CO 2 capture. Therefore, this adsorbent represents an attractive prospect for CO 2 uptake at room temperature .
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高影响因子
LANGMUIR
·
2019
·
IF 3.683
Gaihuan Ren,Xiaoyang Zheng,Hui Gu,Wenwen Di,Zengzi Wang,Yanlin Guo,Zhenghe Xu,Dejun Sun
Cellulose nanocrystals (CNCs) with excellent biodegradability are promising biomaterials for use as responsive Pickering emulsifiers. However, the high hydrophilicity of CNCs limits their emulsification ability. Some existing studies have utilized complicated covalent modification procedures to increase the hydrophobicity of CNCs. To simplify the modification process, we prepared hydrophobically modified CNCs (CNCs-M2005) via simple and controllable electrostatic interactions with thermosensitive M2005. The obtained CNCs-M2005 exhibited temperature and CO2 dual-responsive properties. Subsequently, stable oil/water Pickering emulsions were prepared using the partially hydrophobic CNCs-M2005 at 20 °C. However, demulsification occurred when the temperature increased to 60 °C. This temperature-induced demulsification resulted from the dehydration of polyethylene oxide and polypropylene oxide, causing the aggregation of the CNCs-M2005, as shown by dynamic light scattering and transmission electron microscopy experiments. In addition, demulsification was also achieved after bubbling CO2, which was attributed to the dissociation of the partially hydrophobic CNCs-M2005. The temperature and CO2 dual-responsive biosafe Pickering emulsions open up opportunity for the design of intelligent food, cosmetic, and drug delivery systems.
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CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
·
2022
·
IF 0.847
Zheyue Li,Di Wu,Wanbing Gong,Jiayi Li,Shuaikang Sang,Hengjie Liu,Ran Long,Yujie Xiong
Solar-driven CO 2 methanation is an imperative and promising approach to relieve the global warming and environmental crisis, yet remains a great challenge due to the low reaction efficiency, unsatisfactory selectivity and poor stability. In this work, we demonstrate a facile and efficient strategy to prepare Ru-doped TiO 2 photocatalyst with tunable oxygen vacancies using the ascorbic acid as a reducing agent for the CO 2 methanation reaction. The optimal Ru-TiO 2 -OV-50 exhibits a remarkable CH 4 production rate of 81.7 mmol g −1 h −1 with a 100% CH 4 selectivity under a 1.5 W cm −2 light illumination, which is significantly higher than commercial Ru/TiO 2 and other reported catalysts. We reveal that the superior photocatalytic CO 2 methanation performance is mainly due to the synergistic effect of Ru doping and TiO 2 with tunable oxygen vacancies. Impressively, the light rather than thermal effect is confirmed as the main influencing factor by experimental studies. In addition, in situ spectroscopic technology is performed to investigate the CO 2 methanation reaction pathway. This work will open an avenue to design and prepare highly efficient photocatalyst with tunable oxygen vacancies for CO 2 conversion and other related applications.
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BIOCHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 4.446
Jiabao Xv,Zeyang Zhang,Saizhao Pang,Jiahui Jia,Zixin Geng,Ruirui Wang,Peikun Li,Muhammad Bilal,Jiandong Cui,Shiru Jia
Immobilized carbonic anhydrase (CA, EC4.2.1.1) for CO 2 capture has been intensively investigated. Unfortunately, the immobilized CA usually shows low CO 2 capture efficiency due to lack of CO 2 capture function for the conventional CA supports. In this study, an acid-resistant metal-organic framework MOF-808 was first modified by co-deposition of PEI (polyethyleneimine) and PDA (polydopamine) (PEI/PDA-MOF-808). Subsequently, the PEI/PDA-MOF-808 with a large number of amino groups was used as the strengthening material of CO 2 capture to immobilize CA (CA@PEI/PDA-MOF-808). The resultant CA@PEI/PDA-MOF-808 showed a considerably improved CO 2 capture capacity compared with free CA and PEI/PDA-MOF-808. The amount of CaCO 3 produced by CA@PEI/PDA-MOF-808 was 11.0-fold and 2.5-fold higher than free CA and PEI/PDA-MOF-808, respectively. After 8 consecutive rounds of CO 2 conversion, the total production of CaCO 3 by CA@PEI/PDA-MOF-808 was 92-fold higher than free CA, reaching 294.0 mg. Furthermore, CA@PEI/PDA-MOF-808 displayed high thermostability , pH stability, storage stability, and reusability compared with free counterpart. After 1 h treatment at pH 3.0, CA@PEI/PDA-MOF-808 preserved 53.6% of its original activity while free CA was almost inactivated. In conclusion, this work provides a promising strategy for enzymatic CO 2 conversion.
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Journal of CO2 Utilization
·
2022
·
IF 8.321
Ren Wu,Agula Bao
With the development of large-scale animal husbandry, large amounts of manure have brought great harm to the ecological environment, thus limiting sustainable development of human and animal husbandry. Biomass carbon has been extensively studied as an adsorption material. The rational use of cow dung as biomass has important research significance for the ecological environment. However, most previous work has directly converted biomass to carbon, which limits its application due to the poor quality stability of the biomass porous carbon and large variations in performance resulting from the complexity of biomass composition and microstructure. In this work, porous carbons were prepared after pretreatment of cow dung with NaOH-urea solution to extract cellulose and activate KOH. The results showed that the materials prepared under the optimal conditions (pre-carbonization temperature of 600 °C, cellulose-to-KOH ratio of 1:1) exhibited an ultrahigh specific surface area (1345 m 2 /g) and micropore ratio (74.24%). The capacities for adsorption of CO 2 at 273 K and 298 K and 1 bar were as high as 4.61 mmol/g and 3.26 mmol/g, respectively. This study expands the application range for cellulose and has significance for future preparation of porous carbon materials by extracting cellulose from biomass.
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