Journal of CO2 Utilization
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2021
·
IF 7.132
Jiehong He,Shaoshuai Chang,Haoran Du,Bo Jiang,Wenzhao Yu,Zhenwu Wang,Weiwei Chu,Lanfang Han,Jian Zhu,Hexing Li
The hydrogenation of carbon dioxide (CO 2 ) to formic acid (FA) has been considered as a promising approach to utilize CO 2 and realize carbon-neutral energy supply. Development of efficient heterogeneous catalysts is an interesting yet challenging task. In this work, a reliable amorphous NiRu 0.1 B catalyst was presented and displayed a sufficient catalytic activity for the hydrogenation of CO 2 into FA. The amorphous structure of catalysts provided abundant dangling bonds and unsaturated atoms for enhancement of the reactant gas adsorption. Moreover, the electron-donating effect of B element is crucial for creating active electron-rich metal centres, which is proposed to facilitate the formation of the M H for activating CO 2 molecules. Owing to synergistic effect of amorphous structure and electron-donating, amorphous NiRu 0.1 B catalysts show a higher activity and stability than that of Ni-B and crystalline Ni-B at low temperature. This work not only exhibits a facile method to prepare amorphous bimetallic catalysts, also demonstrates that amorphous metals are promising heterogeneous catalysts for the hydrogenation of CO 2 to FA.
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CHEMICAL ENGINEERING JOURNAL
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2019
·
IF 8.355
Yafei Guo,Chang Tan,Jian Sun,Weiling Li,Jubing Zhang,Chuanwen Zhao
Business cost concern of solid CO 2 adsorbents has motivated the production of porous activated carbons from waste biomass materials. In this work, porous activated carbons were prepared from sugarcane bagasse using different activating agents (air, CO 2 , H 3 PO 4 and NaOH). Chemically activated porous carbons exhibited better physicochemical properties as compared to the physically activated carbons. Particularly, NaOH-activated carbon (CAC-S) featured a high specific surface area (1149 m 2 /g) and a large pore volume (1.73 cm 3 /g). X-ray photoelectron spectroscopy (XPS) analysis confirmed that the CAC-S adsorbent exhibited enhanced total basicity. The desired CAC-S adsorbent showed superior isothermal CO 2 uptakes of 5.50 and 4.28 mmol CO 2 /g at 0 °C and 25 °C and 1 bar. The isosteric heat of adsorption was predicted as 43.96 kJ/mol from the Clausius-Clapeyron equation and Toth model, which indicated intensified interaction between CO 2 molecules and the basic carbon surface. The excellent CO 2 adsorption performance should be associated with the improved textural properties and enriched surface basicity benefited from NaOH activation. Overall, CAC-S is considered as a promising adsorbent for CO 2 adsorption. The recycling of sugarcane bagasse as solid CO 2 adsorbents presents environmental implications with respect to waste management and pollutants mitigation.
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Journal of Cleaner Production
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2020
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IF 7.246
Shasha Wang,Yuelong Xu,Junfeng Miao,Mengshuai Liu,Bin Ren,Lihui Zhang,Zhenfa Liu
Microporous carbon xerogels (CXs) were successfully fabricated via a facile one-pot strategy using eutectic salt mixture (KCl and ZnCl 2 ) as dual activator and catalyst. Their pore structures, morphology, and selective CO 2 adsorption behaviors were thoroughly studied by varying the contents of eutectic salt mixture. The presented CXs herein showed excellent CO 2 adsorption selectivities , and the CX-4 with optimum salt concentration (12.9%) exhibited the highest CO 2 adsorption capacity of 4.39 mmol g −1 at 273 K, which was ascribed to their special microscopic pore structure. Compared with the reported carbon materials, the optimum CX-4 exhibits a comparable or superior CO 2 adsorption performance under similar conditions, showing great potential for efficient CO 2 capture and separation from flue gas and natural gas.
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Chemical Science
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2019
·Vol. 10
·期 45
·10640-10646
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IF 9.556
Jingjing Zhang,Qingli Qian,Ying Wang,Bernard Baffour Asare Bediako,Jiang Yan,Buxing Han
Currently, ethanol is produced via hydration of ethene or fermentation of foods. Lignin and CO2 are abundant, cheap and renewable feedstocks. Synthesis of ethanol using the lignin or its derivatives is of great importance, but is a great challenge and has rarely been reported. Herein, we propose a route to synthesize ethanol from CO2, H2, and lignin or various aryl methyl ethers, which can be derived from lignin. The reaction could be effectively conducted using Ru–Co bimetallic catalyst and the TON of ethanol could reach 145. Interestingly, ethanol was the only liquid product when lignin was used. A series of control experiments indicate that ethanol was formed via cleavage of aryl ether bond, reverse water gas shift (RWGS) reaction, and C–C bond formation. This protocol opens a way to produce ethanol using abundant renewable resources.
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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 PHYSICAL CHEMISTRY B
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2019
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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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CHEMICAL ENGINEERING JOURNAL
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2019
·
IF 8.355
Peng Wang,Jian Sun,Yafei Guo,Chuanwen Zhao,Weiling Li,Guodong Wang,Su Lei,Ping Lu
The development of K 2 CO 3 -based sorbents with desirable CO 2 capture capacity and mechanical property is highly necessary for its large-scale application. In this work, a range of extruded-spheronized K 2 CO 3 -based pellets containing different K 2 CO 3 loading (30–70 wt%) and Al 2 O 3 -based supports (i.e., activated alumina, Bayer aluminum hydroxide, kaolinite clay and calcium aluminate cement) were prepared for CO 2 capture. It is found that the distinct textural properties of different supports result in the obvious diversities in CO 2 uptake and mechanical property of K 2 CO 3 -based pellets. The activated alumina-supported sorbent pellets loaded with 50 wt% of K 2 CO 3 possess the highest CO 2 adsorption capacity of 2.29 mmol/g. It is mainly attributed to the moderate amounts of active component contributing to good textural properties and abundant CO 2 -philic sites, whereas excessive K 2 CO 3 loading will cause the destruction of porous structure, consequently the inferior CO 2 uptake. Moreover, the addition of 15 wt% of urea can furher enhace CO 2 uptake of the activated alumina-supported sorbent pellets loaded with 50 wt% of K 2 CO 3 , ∼3.10 mmol CO 2 /g. The improved CO 2 uptake is due to the significantly enhanced porosity of sorbent pellets as a result of urea decomposition. In addition, the urea-templated sorbent pellets still maintain the high compressive strength (18.96 MPa) and good attrition resistance (a weight loss of 0.59% after 4000 rotations).
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MOLECULES
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2019
·Vol. 24
·期 20
·3732
·
IF 3.06
Li Ji,Zhonghui Qiao,Xin Zhang,Xiaolei Cheng,Weiyang Wang,Fan Zhang,Yifa Zhou,Ye Yuan
Monosialotetrahexosylganglioside (GM1) has good activity on brain diseases and was developed to be a drug applied in clinics for neurological disorders and nerve injury. It is difficult to isolate GM1 in industry scale from the brains directly. In this work, a simple and highly efficient method with high yield was developed for the isolation, conversion, and purification of GM1 from a pig brain. Gangliosides (GLS) were first extracted by supercritical CO2(SCE). The optimum extraction time of GLS by SCE was 4 h, and the ratio of entrainer to acetone powder from the pig brain was 3:1 (v/w). GM1 was then prepared from GLS by immobilized sialidase and purified by reverse-phase silica gel. Sodium alginate embedding was used for the immobilization of sialidase. Under the optimized method, the yield of high-purity GM1 was around 0.056%. This method has the potential to be applied in the production of GM1 in the industry.Keywords:ganglioside;GM1;supercritical CO2extraction;immobilization;sialidase;purification
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2019
·
IF 6.361
Pengju Shi,Xueqin Chen,Zhengguang Sun,Cao Li,Ziqiang Xu,Xueliang Jiang,Bingbing Jiang
Thickness controllable porous polymer nanofilm with superior gas storage capacity has gradually emerged as promising adsorbents for capture of CO 2 , due to extremely high surface area and micro-scale pore. In this work, we have developed a novel and facile strategy to fabricate thickness controllable two or three dimensional ordered porous nanofilm based on poly(styrene-butyl acrylate), in combination with covalently layer by layer (LBL) self-assemble process and hypercrosslinked post-treatment. Abundant microporous structures and a small number of mesoporous structures are formed in hypercorsslinked nanofilm and corresponding surface area derived from Brunauer-Emmett-Teller method (BET) were determined to be 605.7 m 2 /g. The capacity of CO 2 capture was also measured, which reach up to 53.6 wt% (12.2 mmol/g) at 273 K/1 bar, which is comparable to highest record. We have found that all the as prepared nanofilm with different thickness exhibited apparently enhanced micro- and meso-porosity after hypercrosslinking. Moreover, with the increase of thickness of nanofilm, the adsorption capacity decreases gradually, as well as the CO 2 adsorption capacity. An excellent recycling capacity for CO 2 capture have also found for this porous polymer nanofilm via repetitive adsorption-desorption assay. Our work confirmed that thickness controllable porous polymer nanofilm with superior CO 2 capture capacity can be fabricated by a very simple strategy which can meet the challenges of the current CO 2 capture and storage technology.
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Journal of CO2 Utilization
·
2019
·
IF 5.189
Wei Zhang,Erhao Gao,Yu Li,Matthew T. Bernards,Yi He,Yao Shi
A mesoporous silica supported polyamine-based protic ionic liquid (PIL) sorbent has been prepared by impregnating tetraethylenepentammonium nitrate [TEPA][NO 3 ] onto the surface of SBA-15. This innovative hybrid adsorbent exhibits an excellent CO 2 adsorption rate in the rate-controlling step of 147 × 10 −3 mmol g −1 s −0.5 , at least threefold better than other IL-functionalized and amine-modified support systems. Moreover, the adsorption capacity is enhanced by up to 2.15 mmol/g for the adsorbent at 333 K and 0.15 bar, which represents excellent performance under low CO 2 partial pressures. This adsorption performance can be ascribed to the synergistic effect of strong affinity between the PILs and CO 2 and large surface area of the support which favors the diffusion of the PILs and CO 2 molecules in its pores. In addition, density functional theory (DFT) calculations further reveal that CO 2 preferentially reacts with the secondary amine –N(2)H in [TEPA][NO 3 ] forming carbamate due to the high binding energy. The cyclic adsorption/regeneration experiment shows that nearly 90% of original CO 2 adsorption capacity of the adsorbent is restored by N 2 steam desorption at 373 K. Therefore this novel silica supported PIL system shows promise for CO 2 removal and recovery applications.
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ENERGY & FUELS
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2018
·
IF 3.024
Kai Zhang,Yucui Hou,Yiming Wang,Kun Wang,Shuhang Ren,Weize Wu
Extremely low-volatility functional deep eutectic solvents (DESs), based on ethylene glycol (EG) and diethylene glycol (DG) as hydrogen-bond donor and the ammonium salts obtained from triethylenetetramine (TETA) and HCl at different mole ratios as hydrogen-bond acceptor, were designed and used to capture CO2. All of the designed DESs can efficiently capture CO2 even at low partial pressures. CO2 absorption capacity of [TETA]Cl-EG DES with n[TETA]Cl/nEG 1:3 is high up to 17.5 wt % (1.456 mol CO2/mol [TETA]Cl) at 40 °C and 1 atm. CO2 absorption capacity decreases with increasing temperature and decreasing CO2 partial pressure. Regeneration experiments show that CO2 absorption capacities in [TETA]Cl-EG DES and [TETA]Cl-DG DES do not vary after five absorption/desorption cycles. It is found that EG or DG can increase the absorption capacity via activating −NH– or −NH2 on [TETA]Cl and enhance the basicity of DESs. In addition, CO2 absorption mechanism in [TETA]Cl-EG DES based on the change of its viscosity during absorption and FTIR analysis indicates that there is a chemical interaction between CO2 and [TETA]Cl, and the stoichiometry for the reversible absorption is 1.5 molecules of CO2 per [TETA]Cl-EG DES molecule.
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RARE METALS
·
2018
·Vol. 37
·期 6
·520-526
·
IF 1.5
Mushtaq Muhammad,Guo Xian-Wei,Bi Jie-Peng,Wang Zhao-Xiang,Yu Hai-Jun
The rechargeable Li–CO 2 battery has attracted much attention for energy storage because of the high energy density and efficient utilization of greenhouse gas. However, it’s still suffered by low safety issue of liquid electrolyte. Herein, a composite cathode consisting of CNTs and polymer electrolytes was fabricated by the in-situ polymerization process for the polymer electrolyte-based solid-state Li–CO 2 batteries. With the good dispersion of CNTs and polymer electrolyte, the composite cathode is covered by film-like discharge products Li 2 CO 3 . Furthermore, the Li–CO 2 battery shows high reversible capacity (~ 11,000 mAh·g −1 ), excellent cycle stability (1000 mAh·g −1 for 100 cycles) under low charge potential (< 4.5 V), and outstanding rate performances at room temperature, which are much better than those of liquid electrolyte-based battery. Therefore, the polymer electrolyte-based Li–CO 2 battery prepared by this strategy can be a promising candidate to meet the demands of high safety and high-performance energy storage devices.
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