JOURNAL OF CLUSTER SCIENCE
·
2019
·Vol. 31
·期 2
·513-522
·
IF 2.125
Liu Qiang,Liu Yuqi,Zhang Qingqing,Wang Xinying,Li Wei
A new Pr(III)-based metal organic framework with formula {[Pr 2 (C 8 H 3 O 6 N)(SO 4 ) 2 ]·5H 2 O} n was hydrothermally synthesized and characterized by techniques of single crystal X-ray diffraction, infrared spectra (IR), thermogravimetric analysis (TGA), elemental analysis, powder X-ray diffraction (PXRD), and luminescent measurements. X-ray crystal structure analyses reveal that complex 1 is binuclear structure and all Pr(III) atoms show a coordination number of nine with a tricapped trigonal prismatic coordination geometry. Throughout the molecular structure, this lanthanide metal–organic frameworks exhibits a 3D architecture built by the 1D double-stranded chains of Pr ions linked by the 5-nitroisophthalic acid ligand and 2D Pr–SO 4 2− grid. In addition, the fluorescence, nitrogen adsorption properties and carbon dioxide adsorption properties of complex 1 were also investigated. The results indicate that the complex is not only a luminescent and mesoporous material, but also a potential material for selective absorption of carbon dioxide.
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高影响因子
FUEL
·
2022
·
IF 8.035
Xiaohe Wang,Hongwei Chen,Maosheng Zhang,Chaoran Wang,Yufei Wang,Pu Bai,Libo Li,Wenfu Yan
Silicoaluminophosphate (SAPO) zeolites as one of the most important members of zeolitic materials, providing equally high adsorption capacity of CO 2 as aluminosilicate zeolites, can be used as promising candidate materials for selective adsorption and separation of CO 2 . In this work, desirable from both economic and environmental viewpoints, a green and cost-effective one step synthesis strategy of K-SAPO-34 zeolite was developed in a wholly inorganic system under hydrothermal conditions. The pure K-SAPO-34 crystals can be obtained in a wide range of initial gel compositions. The as-synthesized K-SAPO-34 has high proportion of framework Si (Si / (Si + Al + P) = 0.37) and framework charge density ((Al – P) / (Si + Al + P) = 0.36). Because the presence of silica islands in K-SAPO-34 framework leads to a decrease in the number of extra framework cations per unit cell, the K-SAPO-34 in this work has a high CO 2 adsorption capacity (64.1 cm 3 /g) than the conventional K-SAPO-34 prepared by ion-exchange (1.9 cm 3 /g). Moreover, the K-SAPO-34 in this work has a superior separation performance for CO 2 /N 2 and CO 2 /CH 4 .
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Chemical Science
·
2018
·Vol. 9
·期 14
·3426-3437
·
IF 9.063
Xinyu Li,Zhi-Jian Zhao,Liang Zeng,Jiubing Zhao,Hao Tian,Sai Chen,Kang Li,Sier Sang,Jinlong Gong
La2O3 exhibits good performance for various catalytic applications, such as oxidative coupling of methane (OCM) and dry reforming of methane (DRM), during which coke formation may lead to the deactivation of catalysts. Typically, the reaction between CO2 adsorbed on La2O3 and coke is the rate-determining step of the coke elimination process. This paper describes the influence of Ce addition on the CO2 adsorption and activation over La2O3. Combined with in situ and ex situ characterization and density functional theory (DFT) calculation, we show that Ce addition promotes the formation of bidentate carbonate on La2O3via tuning CO2 adsorption energy. In addition, Ce addition adjusts the ratio of bidentate/monodentate carbonate, and affects the ratio of hexagonal/monoclinic La2O2CO3 on the binary oxides. DRM is used as a probe reaction to examine the coke elimination performance of Ce–La binary oxide. It is found that when the Ce/La ratio reaches the optimal value (0.15), Ce–La binary oxide has the highest CO2 adsorption energy and predominantly promotes the formation of bidentate carbonate, and hence possesses the highest basicity above 700 °C and finally exhibits the best coke elimination performance.
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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Xiaoqian Zhang,Chengli Jiao,Xinxin Li,Xiangju Song,Tatiana V. Plisko,Alexandr V. Bildyukevich,Heqing Jiang
Polyamide membrane, fabricated via interfacial polymerization process, is a typical class of facilitated transport membrane for CO 2 separation with amino groups serving as reactive CO 2 carriers. Herein, to further enhance the CO 2 -facilitated transport effect of polyamide membrane, Zn(NO 3 ) 2 is directly introduced into aqueous triethylenetetramine phase for constructing Zn-N coordination polyamide membrane taking advantage of the coordination interaction between Zn ions and amino groups from triethylenetetramine. The good solubility of Zn(NO 3 ) 2 in aqueous amine solution and moderate coordinative ability of Zn ions are beneficial to a uniform distribution of Zn in polyamide layer. The coordination of N from triethylenetetramine monomer to Zn ion centre produces more tertiary amino groups and free amino groups with stronger affinity to CO 2 in Zn-N coordination membrane for enhancing the facilitated transport effect. Additionally, the Zn-N coordination interaction generates smoother surface of membranes when sufficient Zn ions are introduced. The membrane with 0.1 wt% of Zn ions in aqueous phase exhibits the highest CO 2 /N 2 and CO 2 /CH 4 selectivity of 106.7 and 55.2, which increase, respectively, by 75.2% and 99.3% without compromising CO 2 permeance in contrast with pristine polyamide membrane.
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高影响因子
Catalysts
·
2023
·Vol. 13
·期 5
·857
·
IF 3.9
Qianqian Zhou,Yanxin Chen,Haoyan Shi,Rui Chen,Minghao Ji,Kexian Li,Hailong Wang,Xia Jiang,Canzhong Lu
Cu2O is a p-type direct bandgap semiconductor with a band gap of 2~2.2 eV, which has excellent visible light absorption and utilization. However, slow charge transfer and poor stability hinder its practical application. In this paper, a facile electrodeposition approach successfully synthesized the heterostructure of p-Cu2O and n-Cu2O. The protective layer of n-Cu2O on the surface of p-Cu2O nanoparticles forms a p/n heterojunction. Due to the p/n heterojunction, the PEC performance of p/n-Cu2O is enhanced significantly. The charge separation efficiency of photogenerated electron/hole pairs in p/n-Cu2O is greatly improved. Therefore, p/n-Cu2O shows superior photoelectrochemical (PEC) CO2reduction reaction (CO2RR) efficiency when used as a photocathode.Keywords:Cu2O;electrodeposition;p/n heterojunction;carbon dioxide reduction reaction
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高影响因子
ENERGY & FUELS
·
2021
·
IF 3.605
Shuanshi Fan,Hong Huang,Chi Yu,Yanhong Wang,Xuemei Lang,Shenglong Wang,Gang Li,Wangyang Yu
The product gas of natural gas hydrate production by CO2 replacement is the lean-CH4/CO2 binary gas which contains 85–95% CO2. In this work, the lean-CH4/CO2 (10 mol % CH4/90 mol % CO2) binary mixture was used to simulate the product gas of natural gas hydrate production via CO2 replacement, and a promising and mild (low pressure) hydrate-based gas separation (HBGS) technology was employed. This work innovatively proposes to inject the reaction liquid to maintain the constant pressure of the whole process, which makes hydrates form continuously to increase the gas consumption. First, the hydrate phase equilibrium of 10 mol % CH4/90 mol % CO2 + 5 wt % tetrabutylammonium bromide (TBAB, aq) was measured in the range of 280–287 K and 0.5–4 MPa. After that, hydrate-based mild separation of the lean-CH4/CO2 binary gas was conducted with the help of TBAB at a constant pressure in the range of 1–4 MPa. The results show that after HBGS in addition with 5 wt % TBAB(aq) at 1 MPa and 278 K, the CH4 concentration could be increased from 17.2 to 66.2 mol % under constant pressure operation, while it was just slightly increased to 17.2 mol % under nonconstant pressure operation. HBGS with 5 wt % TBAB under constant pressure had the best separation performance. Subcooling has a greater effect on the separation kinetics. HBGS of 10 mol % CH4/90 mol % CO2 under a constant pressure operation of 2 MPa, subcooling of 6 K, and 5 wt % TBAB has the highest separation factor above 37. It is suggested that hydrate-based lean-CH4/CO2 separation experiments are carried out at a mild pressure with low G/L and, more importantly, in a short time. This work proposed a mild HBGS of lean-CH4/CO2 separation, which could benefit the separation of gas produced by natural gas hydrate replacement exploitation. This work also simultaneously provides insights into other HBGS for other gas mixtures (flue gas, coalbed methane, biogas, and shift gas) to achieve low energy consumption, high gas consumption, and high efficiency.
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高影响因子
ACS Omega
·
2020
·
IF 2.87
Yangyang Guo,Lei Luo,Yang Zheng,Tingyu Zhu
For improving the CO2 adsorption capacity of solid-supported amines, five commercial porous supports have been selected and impregnated with tetraethylenepentamine (TEPA), and their CO2 adsorption performances have been evaluated using a fixed-bed reactor coupled with mass spectrometry. For solid-supported amines, CO2 adsorption capacities coincide with the texture characterization of the adsorbent supports (mesoporous alumina, montmorillonite, silica gel, porous resin, MCM-41 molecular sieve), and the optimum TEPA loading amount is mainly affected by the pore volume. The mesoporous supports were found to be more conducive to uniform loading of organic amine, with more than 370 mg/g CO2 adsorbed per unit TEPA. Other components in flue gas, especially H2O, favor CO2 adsorption on solid-supported amines. SO2 inhibited the CO2 adsorption, which was mainly attributable to the strong and irreversible binding of SO2 on some amine sites. NO had little effect on CO2 adsorption. Thermal stabilities of solid-supported amines have been tested based on thermogravimetry curves, and the main weight loss peak for TEPA appears at 513 K for solid-supported amines. Linear and step regeneration modes have been compared, revealing that the temperature for step regeneration is 37 K lower than that for the linear regeneration mode. Moreover, the desorption peak area for the step regeneration mode is 20% higher than that for the linear regeneration mode, indicating that the step regeneration mode can be used in practical applications, to reduce energy consumption during regeneration.
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高影响因子
CATALYSIS COMMUNICATIONS
·
2024
·
IF 3.4
Yan Kong,Long Tian,Guiming Xie,Xiaorui Wang,Yi Man,Zhou-jun Wang
Molybdenum phosphide (MoP) has attracted increasing attention as a novel catalytic material for CO 2 reforming of methane in virtue of superior coke resistance, but its catalytic reactivity is still relatively low. This work for the first time improved the reforming activity of MoP via ZrO 2 modification. The Zr 0.01 MoP catalyst with Zr/Mo molar ratio of 0.01 possessed much higher activity than bare MoP at 800–900 °C. Structural characterizations revealed that the introduction of ZrO 2 would decrease the particle size, modify the electronic structure and change the reducibility property of MoP, which may function together to deliver the higher activity.
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Guanhua Liu,Huaxun Chen,Hao Zhao,Ran Chen,Minghui Yang,Jing Gao,Fengshou Yu,Yanjun Jiang
Enzymatic conversion of CO2 to high value-added chemicals is in line with green chemistry. However, low solubility of CO2 under mild conditions and high cost of cofactor limit the efficiency of CO2 enzymatic conversion. Therefore, we designed a system for enzymatic electrocatalysis of CO2 by the combination of polyethylenimine (PEI)-enhanced enzyme immobilization and CO2 adsorption, and electrocatalytic nicotinamide adenine dinucleotide (NADH) regeneration. Furthermore, the PEI dendritic structure and SiO2 channel skeleton can effectively protect the enzyme structure from external damage. To be specific, PEI was first modified on mesoporous silica SBA-15 by glutaraldehyde, and then the enzyme was immobilized by electrostatic adsorption. The modified amount of PEI, the amount of enzyme for immobilization, and the amount of immobilized enzyme were optimized. The initial reaction rate increased from 1.3 to 1.9 times as the amount of PEI modification increased from 10 to 60 wt %. The optimized catalysis system could produce 1.118 mM formate after a 3 h reaction, with a productivity of 5323.8 μmol gcat–1h–1, which was 3.7 times more than that of the free enzyme system. Furthermore, the immobilized enzyme still retained over 80% activity after 12 cycles reuse with improved thermal stability.
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高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2015
·Vol. 29
·期 4
·240-243
·
IF 2.248
Dongsheng Bai,Zhiyong Zhang,Guangjian Wang,Fang Ma
The cycloaddition of epoxide and CO 2 to synthesize cyclic carbonate catalyzed by VO(IV) porphyrin was achieved under 1.4 MPa at 150°C. The effects of reaction temperature, time, CO 2 pressure, co-catalyst and porphyrin framework were investigated. The catalytic results showed that moderate to high yields of cyclic carbonates were obtained under the optimal reaction conditions. Copyright © 2015 John Wiley & Sons, Ltd.
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高影响因子
PROCESS BIOCHEMISTRY
·
2015
·
IF 2.516
Guohua Jing,Fujun Pan,Bihong Lv,Zuoming Zhou
Carbonic anhydrase (CA) is the most efficient catalyst for CO 2 hydration and dehydration. In the present work, magnetic polymer microspheres functionalized with epoxy group were prepared, and CA enzyme was immobilized on the carries by selective covalent binding. The parameters affecting CA immobilization, such as pH, temperature and enzyme dose were investigated. Based on the investigation and the characterization of the microspheres, the kinetic parameters of the immobilized and the free CA were also evaluated. The value of the Michaelis–Menten constant ( K m ) and the maximum velocity ( V max ) of the immobilized CA was 8.077 mmol/L (mM) and 0.027 μmol/(min mL), while that of the free CA was 6.091 mM and 0.091 μmol/(min mL), respectively. Moreover, the performance of the thermal stability, storage stability and reusability of the immobilized CA confirmed that CA immobilized on the epoxy-functionalized magnetic polymer microspheres owned a stable and efficient catalytic ability on CO 2 hydration, which seemed to be a suitable candidate for CO 2 capture.
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高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Weihua Cai,Xinyu Ma,Jin Chen,Ruochen Shi,Yabo Wang,Yawei Yang,Dengwei Jing,Hudie Yuan,Jing Du,Meidan Que
Great efforts have been devoted to developing efficient visible-light-driven photocatalysts for the conversion CO 2 into clean fuels. Nevertheless, the photoreduction of CO 2 is hampered by inadequate surface-active sites and ineffective electron-hole pair separation. Herein, we explore the wheat-heading BaTiO 3 with high surface area and piezoelectricity to facilitating their bulk charge separation. Meanwhile, oxygen vacancies were fabricated to extending the visible light absorption range and increasing the active sites of the wheat-heading BaTiO 3 , thus promoting the photocatalytic performance of CO 2 . Among the wheat-heading BaTiO 3 -X (X = 0, 0.5, 1.0, 1.5, 2.0) catalysts, BaTiO 3 -1.5 affords the optimal photocatalytic performance of CO, 6.41 μmol·g −1 under light, 9.17 μmol·g −1 under light and ultrasound, which were 3.22 and 1.86 times higher for pristine wheat-heading BaTiO 3 , respectively. This synergetic strategy sheds a new light on piezoelectric properties and surface defect engineering, while emphasizing the importance of surface properties in enhancing CO 2 conversion performance.
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高影响因子
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