COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2026
·
IF 5.4
Meisi Chen,Dandan Hao,Yuwen Shao,Tong Zhao,Chengyi Qiu,Xiemin Liu,Muhua Chen,Gang Zhang,Xinbao Zhu,Bo Fu
Cellulose directs Mg/Ni-MOF-74 growth on fiber surfaces. • Tuning Mg/Ni ratio optimizes pore structure and open metal site characteristics. • MNC-1 exhibits high CO 2 capacity and CO 2 /N 2 selectivity (>200). • Hierarchical porosity facilitates both CO 2 confinement and gas mass transfer. • Low isosteric heat of adsorption promotes easy regeneration. To overcome the poor dispersibility and limited gas mass transfer of MOF powders, a series of Mg/Ni-MOF-74/cellulose composites (MNC-x) were fabricated via cellulose interface directed in situ growth. The effects of the Mg/Ni ratio on the material structure and CO 2 /N 2 adsorption performance were investigated. Results showed that the introduction of Ni altered the local environment and crystal size, regulating the pore structure and adsorption sites of the MNC-x series materials. The optimal sample (MNC-1) achieved a static CO 2 adsorption capacity of 2.67 mmol·g −1 at 298 K and exhibiting superior cycling performance. IAST theoretical calculations indicated that MNC-1 possessed high CO 2 /N 2 selectivity, with an initial isosteric heat of adsorption of only 34.51 kJ·mol −1 , indicating that physical adsorption was predominant. Combined with DFT analysis, the excellent CO 2 adsorption performance of MNC-1 was mainly attributed to the interaction between the open metal sites of Mg/Ni and CO 2 , as well as the hierarchical pore structure formed by the microporous adsorption sites and mesoporous mass transfer channels. This study provides a feasible strategy for designing cellulose-supported, processable bimetallic MOF adsorbents for CO 2 adsorption. Download: Download high-res image (269KB) Download: Download full-size image
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2020
·
IF 5.774
Chengli Jiao,Zedong Li,Xinxin Li,Mian Wu,Heqing Jiang
Poor interfacial compatibility that often led to low gas separation performance is one of key challenges for developing composite membranes. In the present study, nanosized polyethyleneimine (PEI) functionalized ZIF-8 (PEI-ZIF-8) with good dispersion, having a particle size around 15 nm, has been synthesized via in-situ method and used as filler to fabricate Pebax/PEI-ZIF-8 composite membranes. Excluding the intrinsic porous structure and higher affinity with CO 2 of PEI-ZIF-8 beneficial for CO 2 selective transport, the large density of amine groups on PEI chains provide a good interfacial compatibility, and introduce facilitated CO 2 transport path. Furthermore, PEI-ZIF-8 reduces the crystallinity of Pebax matrix, which is favorable for CO 2 transport. The composite membrane with 5 wt% PEI-ZIF-8 shows a CO 2 permeance of 13.0 GPU with a CO 2 /N 2 selectivity of 49.0, which increases by 80.6% and 118.8% respectively in contrast with pristine Pebax membrane. The results demonstrate that nanoparticles functionalized by amine-polymer with long chains is effective for constructing composite membranes with good interfacial compatibility.
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RENEWABLE ENERGY
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2022
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IF 8.634
Naveed Ahmad,Ying Chen,Xiaoxiao Wang,Peixu Sun,Yuting Bao,Xia Xu
Electrochemical CO 2 reduction reaction (ECO 2 RR) offers an eco-friendly way to produce value-added products by utilizing the waste CO 2 from the environment. Recently, amines have been utilized as electrolytes for direct conversion of CO 2 but processes were energy-intensive and lack selectivity due to the formation of highly stable carbamate. 2-amino-2-methyl-1-propanol (AMP) is a sterically hindered amine , produces less stable carbamate, and generates more HCO 3 − . Herein, ECO 2 RR performance using AMP aqueous solution as electrolyte was investigated over Ag, Cu, and Zn metal electrodes. Ultimately, 91 ± 7% CO selectivity on HCl modified polycrystalline Ag electrode at −0.91 V vs RHE in 1 M AMP aqueous solution in the presence of CTAB was achieved, 1.7 times greater than in 1 M aqueous ethanolamine (MEA) solution. Synergetic effects of unstable AMP-carbamate, generation of nano-agglomerates on pitted/porous Ag surface arising from HCl treatment, and a compact electrical double layer due to CTAB present are responsible for the high selectivity of CO. Our findings provide the understanding of electrode-electrolyte interactions and offer a facile strategy to directly convert CO 2 to CO from CO 2 capture solutions.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Jiarui Gu,Yuxin Yuan,Tianxiang Zhao,Fei Liu,Yun Xu,Duan-Jian Tao
Hyper-crosslinked polymers (HCPs) are a category of porous materials with the high specific surface area, abundant pore canal, and tunable structure. A very challenging topic is to fabricate ion-pair active sites into the skeleton structure of HCPs, which can endow HCPs with specific CO 2 separation and catalytic characters. In this work, a series of hyper-crosslinked polymers with the high specific surface area and tunable ion-pair active sites are fabricated by using a one-pot method with simultaneous quaternization and Friedel-Crafts reactions. These ion-pair-containing hyper-crosslinked polymers (IHCPs) are served as adsorbents for selective separation of CO 2 from CH 4 and N 2 . It is found that CO 2 uptake of IHCP-2 reaches 2.87 mmol·g −1 at 273 K and 1 bar, which is higher than that of the same type of ionic polymers that have been reported in the literature. The high CO 2 adsorption capacity is due to the abundant microporous and high specific surface area of as-prepared IHCPs. More importantly, these IHCPs can also be used as recyclable catalysts for cycloaddition of CO 2 and epoxides under metal- and cocatalyst-free conditions, affording corresponding cyclic carbonates in excellent yields. The high catalytic activity is attributed to synergistic contributions of the hierarchical pores and nucleophilic ion pair’s structure. This research provides an alternative strategy for development of bifunctional function materials towards efficient CO 2 capture and conversion.
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高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
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2021
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IF 2.495
Dan Liang,Yunfeng Hu,Qiang Bao,Jian Zhang,Jiawei Feng,Penglai Sun,Yutong Ma,Hongsheng Zhang
Rho zeolite was successfully synthesized by hydrothermal synthesis adopting 18-crown-6 as template, and the cations (H + , Na + , K + , Cs + , Cd 2+ and Pb 2+ ) of different radii were introduced into the framework of Rho by ion exchange. The samples were characterized by XRD, SEM-EDX, ICP and N 2 -BET. The adsorption behavior of CO 2 and CH 4 on cation-exchanged Rho was measured, and the adsorption isotherm was fitted by Langmuir equation to study the adsorption performance of these zeolites. The adsorption results show that the pore size of Rho is not solely dependent on the cation radius, the different positions of the cations are also more crucial in pore size adjustment. In all researched Rho, the introduction of Cd 2+ and Pb 2+ can more significantly reduce the pore size, and completely restrict the entry of CH 4 , thereby further improving the CO 2 /CH 4 selectivity. Therein, Cd-Rho has the best adsorption performance, with considerable CO 2 adsorption capacity, and extremely high CO 2 /CH 4 selectivity and CO 2 working capacity, which provides a new clue for the development of adsorbents for CO 2 and CH 4 separation in PSA process.
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高影响因子
CHINESE JOURNAL OF CHEMISTRY
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2017
·Vol. 36
·期 2
·147-152
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IF 1.852
Qing-Wen Song,Ping Liu,Li-Hua Han,Kan Zhang,Liang-Nian He
One-pot two-step stepwise reaction of terminal propargylic alcohols, carbon dioxide, and primary/secondary amines for the effective synthesis of various urethanes through robust silver-catalysed C-O/C-N bond formation is reported. Catalytic activities were investigated by controlling catalyst loading, reaction pressure and time, and very high turnover number (turnover frequency) was obtained: 3350 (35 h −1 ) with 0.01 mol% silver catalyst under 0.1 MPa, and up to 13360 (139 h −1 ) with 0.005 mol% silver catalyst under 2.0 MPa at room temperature. The strategy was ingeniously regulated, and synchronously afforded a wide range of β-oxopropylcarbamate and 1,3-oxazolidin-2-one motifs in excellent yields and selectivity together with unprecedented high turnover number (TON) and turnover frequency (TOF) value.
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CATALYSIS LETTERS
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2020
·Vol. 150
·期 11
·3071-3078
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IF 2.482
Guo Chunmei,Guo Biao,Gao Xiaosu,Liang Jing,Meng Qide,Liu Jinxuan
Abstract Efficient catalysts play an important role in photoreduction of greenhouse gases (CO 2 etc.) to value-added chemicals such as CO. In this work, we synthesized a series of Ni 1−x Co x WO 4 (x = 0–1) catalysts by chemical co-deposition method. Among the prepared materials, Ni 0.85 Co 0.15 WO 4 exhibits superior catalytic performance for photocatalytic reduction of CO 2 to CO with [Ru(bpy) 3 ]Cl 2 ·6H 2 O as the photosensitizer. The productivity and selectivity of CO are 14.33 mmol g −1 h −1 and 86.4%, respectively under visible light irradiation. The experimental results demonstrate that superiority of electron conductivity of metal tungstates and the high activity of Co active sites facilitate the separation and transfer of photo-induced charges and lead to the excellent performance of photcatalytic reduction of CO 2 to CO. Graphic Abstract Ni 0.85 Co 0.15 WO 4 ,
combining the superiority of electron conductivity of metal tungstates with the high activity of Co active sites, exhibits high productivity and selectivity of CO in photo-reduction of CO 2 .
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高影响因子
CATALYSIS LETTERS
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2017
·Vol. 148
·期 1
·11-22
·
IF 2.799
Wang Dong,Bi Qingyuan,Yin Guoheng,Wang Peng,Huang Fuqiang,Xie Xiaoming,Jiang Mianheng
Abstract Hydrogenation of the greenhouse gas CO 2 to higher alcohols through catalysis holds great promise for resource transformation in low-carbon energy supply system, but the efficient and selective synthesis of value-added ethanol by a robust heterogeneous catalyst under relatively mild conditions remains a major challenge. Based on our previous work on Au/TiO 2 as an active and selective catalyst for ethanol synthesis, we report here that a facile photochemical route can be used for the preparation of anatase TiO 2 supported gold catalyst (Au/a-TiO 2 ) for efficient hydrogenation of CO 2 . Compared with the conventional deposition-precipitation method requiring strong brønsted base and flammable H 2 gas in the complicated and time-consuming process, the photochemical way for the facile preparation of supported gold catalyst shows the advantages of green and energy-saving. Of significant importance is that an impressive space-time-yield of 869.3 mmol g Au
−1 h −1 , high selectivity, and excellent stability can be readily attained at 200 °C and total pressure of 6 MPa. The effects of irradiation time, solvent, and metal loading or Au particle size on ethanol synthesis are systematically investigated. Graphical Abstract
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Journal of CO2 Utilization
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2021
·
IF 7.132
Miaomiao Song,Zhongliang Huang,Bin Chen,Sihan Liu,Shafqat Ullah,Dongren Cai,Guowu Zhan
Catalyst design is one of the most critical factors in selectively converting CO 2 and renewable H 2 to value-added chemicals. In this work, Pt nanoparticles with an average size of 2.9 nm were uniformly loaded on hollow mesoporous nickel phyllosilicate which then underwent various reduction treatments to partial extraction of Ni atoms and formation of Ni-Pt bimetallic catalysts for the selective CO 2 hydrogenation in a fixed bed reactor. Experimental results reveal that Pt nanoparticles supported on SiO 2 are highly selective to CO via reversed water gas shift (RWGS) reaction with 100% CO selectivity, while Pt nanoparticles supported on nickel phyllosilicate show high selectivity for CH 4 , particularly, under high reduction temperature. By simply changing the reduction temperature or reaction pressure, the production selectivity can be facilely tuned, and the maximum CH 4 selectivity achieved in the bimetallic Pt/Ni@phyllosilicate catalyst is 100%. The metallic Ni 0 reduced from nickel phyllosilicate owns a high concentration of Lewis basic sites, which could enhance the adsorption strength of CO 2 but prevent the dissociated adsorption. The diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) in different transient states were applied to study the mechanistic insights into how Ni-Pt dual sites tune the product selectivity. The results suggest that CO* over Pt site is the key species for CO 2 conversion to CO, whereas the produced CO* could be further hydrogenated to CH x O* intermediate over Ni site, leading to the formation of CH 4 . The present work offers a new method to prepare Ni-Pt bimetallic catalysts with excellent CO 2 hydrogenation performance towards CH 4 .
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2018
·
IF 3.609
Jun Xiao,Weiyi Yang,Shuang Gao,Caixia Sun,Qi Li
A one-pot, solvent-thermal process was used to create the ultrafine ZnFe 2 O 4 nanoparticles photocatalyst . During the solvent-thermal process, the in situ self-forming NaCl not only served as a “cage” to confine the ion diffusion, but also acted as a microreactor for nanocrystallite growth. An average particle size of ∼10 nm and a high-specific surface area of ∼112.9 m 2 /g were observed for the ultrafine ZnFe 2 O 4 nanoparticles Owing to the synergistic effect of ultrafine particle size, the full utilization of the visible light region and high conduction band (CB) position, ultrafine ZnFe 2 O 4 photocatalyst displayed an efficient photocatalytic CO 2 reduction under visible light illumination. Besides, the ultrafine ZnFe 2 O 4 photocatalyst showed high production selectivity for CH 3 CHO and C 2 H 5 OH generation in aqueous CO 2 /NaHCO 3 solution. This work may provide a new idea for the synthesis of new high-efficiency photocatalysts.
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NEW JOURNAL OF CHEMISTRY
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2016
·Vol. 41
·期 1
·290-301
·
IF 3.277
Shokat Sarmad,Yujiao Xie,Jyri-Pekka Mikkola,Xiaoyan Ji
Deep eutectic solvents (DESs) as ionic liquid (IL) analogues show great potential for CO2 capture. They exhibit favorable solvent properties and are considered to be economical alternatives to conventional ILs. In this study, we prepare 35 DESs and screen them in terms of their CO2 solubility and viscosity, both crucial factors to be considered when designing efficient CO2 sorbents. The influence of salt and HBD type and structure, as well their molar ratio on the CO2 solubility and viscosity of the DESs is investigated. The viscosity and CO2 solubility of the DESs are compared with those of other DESs and conventional ILs. 15 DESs, which exhibit comparable CO2 absorption capacity to choline chloride–urea DESs, glycerol DESs and fluorinated ILs, are chosen as the promising ones. The viscosities of the selected DESs are below 200 mPa s and are lower than those of choline chloride-based DESs. Since the viscosity of the DESs is relatively high, on a par with those of conventional ILs, the effect of water as a co-solvent is investigated in order to decrease the viscosity. The addition of water to the glycerol-based DESs improves the kinetics of absorption by decreasing the viscosity, thus increasing the CO2 absorption capacity. Dry or aqueous DESs that demonstrate a high sorption capacity and low viscosity are chosen for additional analysis and characterization, and further functionalization will be carried out in the future to improve their sorption capacity.
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MATERIALS SCIENCE FORUM
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2020
·
IF 0
Yang Meng,Xin Yun Wu,Yu Xin Yan,Shuai Liu,Tao Wu,Cheng Heng Pang
Amine-modified solid sorbents have attracted extensive interests in post-combustion carbon capture for power plants. Among various amines, polyethyleneiemine (PEI) is likely to be the most effective and promising candidate. However, previous studies have mainly focused on examining various supports to increase PEI loading and then enhance CO2 adsorption capacity. In this study, one rare earth element (Ce) and 6 first-row transition metals (from V to Cu) in the oxidation states impregnated on PEI incorporated γ-Al2O3 were prepared and investigated as potential catalyst/promotor for base-catalyzed reaction. Thermodynamic analysis, including isothermal and quasi-static CO2 adsorption tests, were implemented to evaluate the performances amongst the 7 metal oxides. The results showed that MnO2, CeO2 and Fe2O3 showed a better performance in isothermal CO2 adsorption at 75°C. Upon quasi-static tests, the results also indicates that the peak adsorption temperatures (Tpeak, a) of V2O5 and Cr2O3 shifted to high temperature region, whilst opposite behavior of MnO2 was observed. In preliminary study, density functional theory (DFT) was also adopted to assist the screening of metal oxide in terms of bond length and adsorption energies.
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