SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Zhiyong Li,Kairui Shi,Liyong Zhai,Zhenzhen Wang,Huiyong Wang,Yang Zhao,Jianji Wang
Efficient capture and selective separation of CO 2 is of great significance for alleviating the greenhouse effect. However, it is still a challenge to achieve efficient, reversible and selective capture of CO 2 . Here, stable Al-based MOFs with multiple adsorption sites were constructed for capture and selective separation CO 2 . It was found that MOF-303(Al) with multiple active sites (μ-OH, N-H, N-N and H-C) demonstrated a high CO 2 capacity of 5.1 mmol/g, and can be recycled for more than 50 times. Moreover, MOF-303(Al) shows excellent selective separation performance of CO 2 from CO 2 /CH 4 and CO 2 /N 2 mixtures, which could be used as a potential material for natural gas purification. Mechanism results revealed that the excellent CO 2 adsorption and selective separation performance is arose from the multiple adsorption sites (μ-OH, N-H, N-N and C-H) of MOF-303(Al), where the contribution of μ-OH and N-H adsorption sites are higher than that of N-N and H-C sites.
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International Journal of Electrochemical Science
·
2023
·
IF 1.5
Lijuan Guo,Wen Chen,Cuiqiong Wang,Boran Dong
The CH 4 -CO 2 reforming reaction can realize the utilization of both CH 4 and CO 2 , which is important to control the greenhouse effect and protect the environment. The development of low-cost, high-activity and high-stability reforming catalysts is the focus of research. This work used electrochemical methods to synthesize Cu 3 (BTC) 2 in high yields. Cu 3 (BTC) 2 was subsequently used as a precursor and Cu 3 P was synthesized by direct phosphorylation at different temperatures. Both high and low phosphatization temperatures can reduce the hydrogen precipitation performance of the prepared catalyst. In the CH 4 -CO 2 reforming reaction, the Cu 3 P catalyst prepared at elevated temperature has more excellent activity and stability. However, the activity of the catalyst did not keep increasing with the increase of temperature. After the CH 4 -CO 2 reforming reaction at 700 ℃ for 6 h, the conversion of Cu 3 P-350 did not change significantly, and the stability was significantly higher than that of Cu 3 P-300 and Cu 3 P-325. At the same time, when the phosphating temperature is lower than 375 ℃ Cu 3 P carbon accumulation are less. The amount of carbon accumulation increases when the phosphating temperature reaches 400 °C.
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JOURNAL OF MEMBRANE SCIENCE
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2022
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IF 10.53
Li Yin,Dongfeng Li,Hongxia Guo,Shuai Wang,Tiexin Zhang,Yunling Liu,Fangyuan Gai,Xiaogang Zhao
Incorporating functional materials into polymer precursors is an effective way to prepare carbon molecular sieve (CMS) membranes for solving the trade-off problem between permeability and selectivity of gas separation. In this work, we induced ZIF-8 nanoparticles (from 5 to 20 wt%) as a doping agent to construct a series of phenolphthalein-based cardo poly (arylene ether ketone) (PEK-C) -based hybrid carbon molecular sieve (ZCMS) membranes for CO 2 /N 2 separation via an oxidation and a carbonization process with pyrolysis temperature in the range of 500–700 °C. The carbonized ligand and metal centre of ZIF-8 offered additional pores of carbon matrix, which tailored the ultramicropores of ZCMS membranes for both excellent CO 2 permeability and selectivity. By treating with the temperature of 600 °C, ZCMS-600-15 (ZCMS membrane based on 15 wt% of ZIF-8-doped PEK-C) exhibited the highest CO 2 permeability of 8902 Barrer, which was 1.8 times higher than that of CMS-600 (CMS membrane based on naked PEK-C). ZCMS-600-15 showed an ideal CO 2 /N 2 selectivity value of 42.2, which is also higher than that of other samples, indicating that the appropriate doping amount of ZIF-8 is 15 wt% and the proper carbonization temperature is 600 °C. Moreover, among all the samples, ZCMS-600-15 also showed a superior CO 2 permeability of 8285 Barrer and the highest CO 2 /N 2 selectivity of 24.08 for an equimolar mixture of CO 2 and N 2 , far exceeding the 2008 Robeson upper bound. Therefore, our results suggest that incorporating MOFs into polymer precursors to prepare hybrid carbon molecular sieve membranes by carbonization process could solving the trade-off problem between permeability and selectivity, introducing new possibilities for industrial application.
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KOREAN JOURNAL OF CHEMICAL ENGINEERING
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2022
·Vol. 39
·期 3
·475-483
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IF 3.146
Lv Xia,Li Xueqin,Huang Lu,Ding Siyuan,Lv Yin,Zhang Jinli
Pebax® MH 1657 (Pebax)-based blend membranes with different polyether-amine (PEA) loadings were designed and fabricated for efficient CO 2 separation. The CO 2 separation performance of Pebax/PEA blend membranes was greatly improved in comparison with that of pure membranes. This was mainly because the introduced PEA tailored the physical and chemical microenvironments in blend membranes. Specifically, PEA was a liquid-like additive, which was beneficial to reduce the mass transfer resistance of gases and increase CO 2 permeability. Meanwhile, PEA contained amino groups that acted as mobile carriers to tailor the chemical microenvironment in blend membranes. The mobile carriers preferentially reacted reversibly with CO 2 molecules, facilitating CO 2 transport in membranes. Compared with CO 2 /CH 4 separation performance of pure Pebax membrane, CO 2 permeability and CO 2 /CH 4 separation factor of Pebax/PEA-3 increased by 144.8% and 29.4%, respectively. This study suggests that PEA is a promising membrane material for tailoring the physical and chemical microenvironments in blend membranes for efficient CO 2 separation.
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Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 10
·5540-5549
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IF 14.511
Zixuan Xu,Ke Liu,He Huang,Yadong Zhang,Zhouyang Long,Minman Tong,Guojian Chen
In this work, we reported a facile catalyst-free and initiator-free strategy to fabricate a new class of viologen-linked ionic polyacetylenes (denoted as VIPAs) that can achieve simultaneous ionization and polymerization in one-pot and one-step. To our surprise, the ionic polymers VIPA-X (X = Br or Cl) were directly synthesized by quaternization-induced in situ polymerization from commercially available 4,4′-bipyridine with propargyl bromide or propargyl chloride. It was found that reaction temperatures have a remarkable influence on the synthesis of VIPAs, achieving the transformation from soluble oligomers to insoluble highly cross-linked polymers by adjusting the temperatures from 30 °C to 100 °C. At a higher temperature of 100 °C, the obtained highly cross-linked ionic polymers VIPA-Br and VIPA-Cl were insoluble in both hot water and even dimethyl sulfoxide (DMSO). By virtue of abundant halogen anions and the absorbed H-bonded water, both VIPA-Br and VIPA-Cl were employed as efficient heterogeneous catalysts for the conversion of CO2 with various epoxides into cyclic carbonates at atmospheric pressure and low temperatures. In particular, the catalytic activities of VIPA-Br for the conversion of various epoxides are much better than those of VIPA-Cl at low temperatures, which should be attributed to the higher nucleophilicity and better leaving ability of the Br− anion than those of the Cl− anion. The present work affords a succinct catalyst-free strategy to construct more task-specific ionic polyacetylenes by quaternization-induced polymerization of multi-N-heterocycle monomers and propargyl halides towards diverse applications.
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ULTRASONICS SONOCHEMISTRY
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2022
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IF 9.336
Hanyang Gao,Kunkun Pei,Guoxin Hu,Wenxing Liu,Aihua Meng,Hongcheng Wang,Huifeng Shao,Wenxin Li
CO 2 -expanded organic solvent is a kind of important fluid medium and has broad applications in chemical industry, environmental protection and other fields. Ultrasonic cavitation in gas expanded liquids (GXLs) is conducive to enhancing mass transfer and producing many exciting phenomena. In this paper, the ultrasonic cavitations and streaming in the saturated CO 2 -expanded liquid N, N-dimethylformamide (DMF) at 4.2 MPa and 5.2 MPa are observed by a high-speed camera. The cavitation intensity and time trace of pressure pulses are recorded using a PZT hydrophone. The influences of gas–liquid equilibrium pressure and ultrasonic power on the cluster dynamics of transient and stable cavitation are examined. The excess molar enthalpies required for CO 2 dissociation from DMF are calculated by Peng-Robinson equations of state and the change of surface free energy of CO 2 -expanded DMF is predicted. The results show that the excess enthalpy of the mixture is one of the key factors to control ultrasonic cavitation at high pressurized conditions, while the surface tension is the key factor for low pressure. As the increase of applied ultrasonic power, the formation and collapsing frequency of bubble clusters increases, and the amplitude and cyclic frequency of pressure pulse are enhanced. The transient cavitation intensity increases as it reaches a maximum value at a certain ultrasonic power and then decreases. The change trends of stable cavitation intensity under different pressures are basically same. It can be concluded from the evidence that ultrasonic cavitation in CO 2 -expanded DMF is affected by the combined effect of compression and substitution: compression depresses the nucleation and growth of bubbles, while the high solubility of CO 2 in DMF is conducive to the generation of bubbles in cavitation.
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CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Xiaoyu Li,Ruihong Li,Kang Peng,Liangjie Fu,Keping Zhao,Haoran Li,Jiahui Peng,Luxue Wang
Cyclic CO 2 adsorption via solid amine adsorbents is widely considered as a feasible technology for CO 2 mitigation from industrial flue gas. However, the high cost and rapid decline of adsorption capacity and insufficient cyclic stability limit their large-scale application. Herein, we demonstrated a facile and efficient interlayer functionalization approach, involving the synthesis of acid activated expanded vermiculite derived silica (AEV) support with hierarchical layered porous structure and the impregnation of PEI into the AEV support, to enhance CO 2 adsorption capacity and cycle stability of AEV/PEI adsorbents. The optimal AEVP50 adsorbent exhibited a high CO 2 uptake of 2.21 mmol/g at 75 °C and stable cyclic stability with a mere 1% decay after 10 cycles, owing to the superior hierarchical porous structure of synthesized AEV support. The interlayer functionalization of vermiculite was beneficial for enlarging interlayer volume and producing hierarchical porous structure and abundant Lewis acid sites, which could increase PEI loading content, form uniform amine distribution with less blocked pores/channels and enhance the interfacial interaction between PEI and AEV support. Furthermore, the interlayer spatial confinement effect significantly avoids the inactivation of functional amidogen during the regeneration stage. This strategy significantly enhanced the cyclic CO 2 adsorption of AEV/PEI adsorbents through the interlayer functionalization of VMT, and is promising for various practical CO 2 capture and separation processes.
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Journal of Physical Chemistry C
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2022
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IF 4.177
Yuyao Zhang,Yu Tian,Wen Chen,Min Zhou,Siyong Ou,Yueli Liu
The CO2 photoreduction process is becoming a promising strategy to solve the energy shortage problem and global warming in recent years. How to promote the separation of photoinduced carriers has attracted attention for the improvement of photocatalytic CO2 reduction. In the present work, an S-scheme heterojunction of Bismuthene/CsPbBr3 quantum dots (Bismuthene/CsPbBr3 QDs) is constructed as the photocatalyst for CO2 conversion. As a result, Bismuthene/CsPbBr3 QDs exhibit an optimal CH4 evolution rate of 43.1 μmol h–1 g–1 with 84.53% selectivity over CH4 under ultraviolet–vis light (UV–vis) irradiation. Construction of the S-scheme heterojunction with a narrow band gap semiconductor is the main factor for improving the photocatalytic performance, as the S-scheme heterojunction can suppress the recombination of photoinduced carriers and retain redox ability. The narrow band gap semiconductor Bismuthene can enhance light absorption abilities. This work probably provides some insights for the designing of heterojunction photocatalysts and the improvement of photocatalytic performance.
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Science Bulletin
·
2022
·
IF 20.577
Kunhao Liu,Chao Yang,Ruilin Wei,Xingyu Ma,Chen Peng,Zhengzheng Liu,Yangshen Chen,Yaqin Yan,Miao Kan,Yaoyue Yang,Gengfeng Zheng
Although many catalysts have been reported for the CO 2 electroreduction to C 1 or C 2 chemicals, the insufficient understanding of fundamental correlations among different products still hinders the development of universal catalyst design strategies. Herein, we first discover that the surface *CO coverage is stable over a wide potential range and reveal a linear correlation between the partial current densities of CH 4 and C 2 products in this potential range, also supported by the theoretical kinetic analysis. Based on the mechanism that *CHO is the common intermediate in the formation of both CH 4 (*CHO → CH 4 ) and C 2 (*CHO + *CO → C 2 ), we then unravel that this linear correlation is universal and the slope can be varied by tuning the surface *H or *CO coverage to promote the selectivity of CH 4 or C 2 products, respectively. As proofs-of-concept, using carbon-coated Cu particles, the surface *H coverage can be increased to enhance CH 4 production, presenting a high CO 2 -to-CH 4 Faradaic efficiency ( FE CH 4 ∼52%) and an outstanding CH 4 partial current density of –337 mA cm −2 . On the other hand, using an Ag-doped Cu catalyst, the CO 2 RR selectivity is switched to the C 2 pathway, with a substantially promoted FE C 2 of 79% and a high partial current density of –421 mA cm −2 . Our discovery of tuning intermediate coverages suggests a powerful catalyst design strategy for different CO 2 electroreduction pathways.
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AICHE JOURNAL
·
2022
·Vol. 68
·期 8
·e17706
·
IF 4.167
Qiang Sun,Hongxia Gao,Yu Mao,Teerawat Sema,Sen Liu,Zhiwu Liang
High heat duty is an urgent challenge for industrial applications of amine-based CO 2 capture. The temperature (>110°C) of carbamate breakdown in amine regeneration requires large energy consumption. In this work, we report a novel, stable, efficient, and inexpensive Ni-HZSM-5 catalyst to improve the CO 2 desorption rate and reduce the heat duty. The impregnation method was applied for varying nickel content in the catalysts from 2.16 to 9.80 wt% in HZSM-5. The catalysts were characterized by scanning electron microscope, X-ray powder diffraction, N 2 adsorption–desorption, inductively coupled plasma-optical emission spectrometry, ultraviolet-visible diffuse reflectance spectroscopy, X-ray photoelectron spectroscopy, NH 3 -temperature programmed desorption (TPD), Infrared spectroscopy of pyridine adsorption, and Fourier transform infrared spectroscopy. The catalytic performance was evaluated by CO 2 desorption of rich amine solvent at 90°C. It was found that the introduction of nickel increased the acid sites of catalysts compared with parent HZSM-5. This phenomenon plays a key role on improving the CO 2 desorption rate. The density functional theory (DFT) calculations successfully explain the catalytic performance. The catalytic activity associates with the combined properties of MSA × B/L × Ni 2+ . The 7.85-Ni-HZ catalyst presents an excellent catalytic activity for the CO 2 desorption: it increases the amount of desorbed CO 2 up to 36%, reduces the relative heat duty by 27.07% with the same reaction time, and possesses high stability during five cyclic tests. A possible catalytic mechanism for the Ni-HZSM-5 catalysts through assisting carbamate breakdown and promoting CO 2 desorption is proposed based on experimental results and theoretical calculations. Therefore, the results present that the 7.85-Ni-HZ catalyst significantly accelerates the protons transfer in CO 2 desorption and can potentially apply in industrial CO 2 capture.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2022
·
IF 3.898
Yachen Deng,Shifu Wang,Yanqiang Huang,Xuning Li
MOF-based materials have been widely explored in electrochemical CO 2 reduction reactions for the production of valuable chemicals. Understanding the reconstruction of those catalysts under working conditions is crucial for the identification of active sites and clarification of reaction mechanism. Herein, a series of six N coordinated Sn-based metal-organic frameworks (Sn-N6-MOFs) are newly developed for electrochemical CO 2 reduction (CO 2 RR). 2% Sn-N6-MOF achieves the optimal catalytic performance with a formate Faradaic efficiency of ∼85% and a current density of 23 mA·cm −2 at −1.23 V vs. RHE. In-situ Raman results combined with ex-situ 119 Sn Mössbauer measurements reveal the structural reconstruction of Sn-N6-MOFs during CO 2 RR, generating tin nanoclusters as the real active sites for CO 2 electroreduction to HCOOH.
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ChemSusChem
·
2022
·Vol. 15
·期 7
·e202200226
·
IF 9.14
Huaxin Li,Xian Yue,Jing Che,Zhou Xiao,Xianbo Yu,Fenglei Sun,Chao Xue,Junhui Xiang
Graphical Networking at its best : The 3D self-supporting nanonetwork structure of Cu−Bi aerogels provides abundant reactive sites and electron transport channels for efficient electrocatalytic reduction of CO 2 to formate. The electrocatalytic reduction of CO 2 (CO 2 RR) to CO, formate, methane, and other high-value compounds is a promising technique. However, current electrocatalysts suffer from drawbacks such as few active catalytic sites, poor selectivity and low stability, etc, which restrict the practical application. Although monatomic metal catalysts have been widely reported in recent years, high performance non-noble metal aerogels were rarely investigated for electrocatalytic CO 2 RR. Herein, Cu−Bi aerogels with boosted CO 2 RR activity were well constructed by a simple one-step self-assembly method. The resultant Cu 1 Bi 2 exhibits excellent CO 2 RR activity with high faradaic efficiency (FE) of 96.57 % towards HCOOH at a potential of −0.9 V vs. RHE, and the FE HCOOH remains over 80.18 % in a wide potential window (−0.8 V to −1.2 V vs. RHE). It demonstrated that the enhanced CO 2 RR activity of Cu−Bi aerogels could be attributed to the 3D self-supporting structure of the catalysis, synergistic effect, and low interfacial charge transfer resistance.
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