JOURNAL OF NANOPARTICLE RESEARCH
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2020
·Vol. 22
·期 5
·1-13
·
IF 2.132
Maimaiti Halidan,Wang Shixin,Awati Abuduheiremu,Xu Bo
Graphene oxide/silica (GO/SiO 2 ) containing various inorganic particles is obtained by using the Xinjiang Wucaiwan coal as carbon source and silicon source. The ruthenium/graphene oxide/silica (Ru/GO/SiO 2 ) composite was prepared by loading Ru nanoparticles on the surface of GO/SiO 2 . Then, the photocatalytic ammonia synthesis performance was investigated while characterizing the structure of Ru/GO/SiO 2 . On the one hand, the Ru can be sufficiently dispersed to make the surface plasmon resonance (SPR) effect enhance significantly. On the other hand, the quantum confinement effect of the defect structure on the Ru/GO/SiO 2 can effectively separate electron and hole, and it can participate in the reducing/oxidizing reaction of photocatalytic ammonia synthesis.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2020
·
IF 5.774
Wenbo Chen,Zhenguo Zhang,Lei Hou,Cancan Yang,Hongcheng Shen,Kai Yang,Zhe Wang
This work mainly studies the CO 2 separation performance of a new type mixed-matrix membranes (MMMs) based on MOF-801 as the microporous filler and PIM-1 as the polymer matrix. MMMs was successfully formed via simple casting/solvent evaporation approach at room temperature. The samples were systematically characterized by SEM, XRD, TGA and FTIR, the permeability-selectivity of MMMs to CO 2 , O 2 and N 2 was studied by gas permeability test. The experimental results show that the uniform dispersion of the CO 2 -philic MOF-801 filler provides a channel for the rapid and selective transport of CO 2 , so the MOF-801/PIM-1 MMMs revealed much higher CO 2 permeability and CO 2 /N 2 ideal selectivity (CO 2 = 9686 Barrer, CO 2 /N 2 = 27, all selectivity in the paper is ideal) than pure polymer membrane. After 90-days aging test, the CO 2 permeability of MMMs remains above 70%, which reflects its good anti-aging performance. After 120 h continuous gas permeability test, it also shows good long-term working stability. The experimental results show that the good gas separation performance of MMMs exceeds the Robeson upper bound (2008), showing good application prospect for practical greenhouse gas CO 2 separation.
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JOURNAL OF SOLID STATE CHEMISTRY
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2020
·
IF 2.726
Guoqiang Li,Feifei Li,Jianxin Liu,Caimei Fan
The nitrogen activation is the Achilles’ heel of photocatalytic nitrogen fixation . Herein, metal-organic frameworks (MOFs), for first time, are proposed to solve the above bottleneck. A series of Fe-Based MOFs (MIL-101(Fe), MIL-100(Fe), MIL-88(Fe)) demonstrated excellent photocatalytic nitrogen fixation activity. To gain insight into the reaction mechanism, MIL-101(Cr) and MIL-101(Fe), with same molecular structure except the central metal ions , selected for system comparison. Photocatalytic nitrogen fixation activity of MIL-101(Fe) and MIL-101(Cr) are 50.355 μmol L −1 h −1 and inactive, respectively. This suggested that the nitrogen fixation activity originated from the Fe catalytic center. The results of in situ FTIR and quantum computation verifies Fe catalytic center have a higher electron density, a lower reaction activation energy and more generation of N–H bond than those of Cr catalytic center. In view of the analogous outer electron configuration of Cr and Fe, it was suspect that two extra d-orbitals electronics of Fe element are the basic reason of the excellent photocatalytic nitrogen fixation activity. This work provides a new application of MOFs in photocatalytic nitrogen fixation field and emphasizes the vital of d-orbitals electronics during the nitrogen activation process.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2020
·
IF 5.774
Jiuli Han,Lu Bai,Shuangjiang Luo,Bingbing Yang,Yinge Bai,Shaojuan Zeng,Xiangping Zhang
Ionic liquids (ILs) are attractive and prospective materials used in membranes due to the nonvolatility, structure tunability, and the ability to tune the interface compatibility. The cobalt IL Bmim 2 Co(NCS) 4 possesses the porphyrin-like N4-coordinated cobalt center which could selectively and reversibly interact with O 2 . Herein the Bmim 2 Co(NCS) 4 as liquid-phase oxygen carrier was used to fabricate thin-film composite (TFC) membrane with the polymer of intrinsic microporosity (PIM-1). The microstructures, properties and gas separation performance of the membrane were compared with the TFC membrane which takes cobalt porphyrin (T(4-Cl)PPCo) as a carrier. We found that the addition of a small amount of T(4-Cl)PPCo can enlarge the d -spacing of packed chains of PIM-1 and significantly increase the fractional free volume (FFV) and the gas permeability of the membrane, but the selectivity is unsatisfactory. It is worth noting that adding Bmim 2 Co(NCS) 4 into the polymer can increase greatly the O 2 /N 2 selectivity which is higher than that of the membrane with T(4-Cl)PPCo. Although the addition of Bmim 2 Co(NCS) 4 decreases the d -spacing of packed chains of PIM-1, resulting in the slight decline of FFV and gas permeability of the membrane, the Bmim 2 Co(NCS) 4 /PIM-1 TFC membranes exhibit better O 2 /N 2 separation performance than the T(4-Cl)PPCo/PIM-1 TFC membranes in consideration of the Robeson upper bound.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2021
·
IF 8.067
Tayiba Ilyas,Fazal Raziq,Nasir Ilyas,Liuxin Yang,Sharafat Ali,Amir Zada,Syedul Hasnain Bakhtiar,Yong Wang,Huahai Shen,Liang Qiao
The electrocatalytic nitrogen reduction reaction (NRR) has emerged as a promising renewable energy source and a feasible strategy as an alternative to Haber-Bosch ammonia (NH 3 ) synthesis. However, finding an efficient and cost-effective robust catalyst to activate and cleave the extremely strong triple bond in nitrogen (N 2 ) for electrocatalytic NRR is still a challenge. Herein, a FeNi@CNS nanocomposite as an efficient catalyst for N 2 fixation under ambient conditions is designed. This FeNi@CNS nanocomposite was prepared by a simple water bath process and post-calcination. The FeNi@CNS is demonstrated to be a highly efficient NRR catalyst, which exhibits better NRR performance with exceptional Faradaic efficiency of 9.83% and an NH 3 yield of 16.52 μg h −1 cm −2 in 0.1 M Na 2 SO 4 aqueous solution. Besides, high stability and reproducibility with consecutive 6 cycles for two hours are also demonstrated throughout the NRR electrocatalytic process for 12 h. Meanwhile, the FeNi@CNS catalyst encourages N 2 adsorption and activation as well as effectively suppressing competitive HER. Therefore, this earth-abundant FeNi@CNS catalyst with a subtle balance of activity and stability has excellent potential in NRR industrial applications.
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Membranes
·
2021
·Vol. 11
·期 9
·693
·
IF 4.106
Fei Guo,Bingzhang Li,Rui Ding,Dongsheng Li,Xiaobin Jiang,Gaohong He,Wu Xiao
Mixing a polymer matrix and nanofiller to prepare a mixed matrix membrane (MMM) is an effective method for enhancing gas separation performance. In this work, a unique UiO-66-decorated halloysite nanotubes composite material (UiO-66@HNT) was successfully synthesized via a solvothermal method and dispersed into the Pebax-1657 matrix to prepare MMMs for CO2/N2separation. A remarkable characteristic of this MMM was that the HNT lumen provided the highway for CO2diffusion due to the unique affinity of UiO-66 for CO2. Simultaneously, the close connection of the UiO-66 layer on the external surface of HNTs created relatively continuous pathways for gas permeation. A suite of microscopy, diffraction, and thermal techniques was used to characterize the morphology and structure of UiO-66@HNT and the membranes. As expected, the embedding UiO-66@HNT composite materials significantly improved the separation performances of the membranes. Impressively, the as-obtained membrane acquired a high CO2permeability of 119.08 Barrer and CO2/N2selectivity of 76.26. Additionally, the presence of UiO-66@HNT conferred good long-term stability and excellent interfacial compatibility on the MMMs. The results demonstrated that the composite filler with fast transport pathways designed in this study was an effective strategy to enhance gas separation performance of MMMs, verifying its application potential in the gas purification industry.Keywords:composite material;UiO-66;HNT;mixed matrix membrane;CO2/N2separation
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2019
·Vol. 43
·期 24
·9725-9731
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IF 3.069
Suresh Mutyala,Sobhy M. Yakout,Shebl S. Ibrahim,Madhavi Jonnalagadda,Harisekhar Mitta
Iron metal–organic framework, MIL-100(Fe) was prepared by a hydrothermal method and used as a support to incorporate diethylenetriamine (DETA) for the study of CO2 adsorption and separation of CO2/N2. All synthesized adsorbents were characterized by PXRD, N2 adsorption–desorption isotherms, FT-IR, TGA, SEM, and elemental analysis. Structural characterization results have revealed that the structure of MIL-100(Fe) was not changed by the incorporation of diethylenetriamine. The CO2 adsorption capacities were 29 cm3 g−1 and 41 cm3 g−1 at 298 K, 1 bar for MIL-100(Fe) and DETA–MIL-100(Fe), respectively. Adsorption of CO2 on DETA–MIL-100(Fe) was higher than that on MIL-100(Fe). The enhancement was due to the presence of amine groups which could form ammonium carbamate by interaction with CO2. Similarly, the N2 adsorption capacities were 3 cm3 g−1 and 0.9 cm3 g−1 at 298 K, 1 bar for MIL-100(Fe) and DETA–MIL-100(Fe), respectively. The decrease in N2 adsorption capacity was due to the decrease in surface area. The selectivity of CO2/N2 on DETA–MIL-100(Fe) was four times higher than that on MIL-100(Fe). The heat of CO2 adsorption was 74.2 kJ mol−1 at low coverage of CO2 on DETA–MIL-100(Fe) and the CO2 adsorption capacity was constant in each adsorption cycle over the same adsorbent.
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INORGANIC CHEMISTRY
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2018
·
IF 4.7
Lei Ji,Xifeng Shi,Abdullah M. Asiri,Baozhan Zheng,Xuping Sun
Electrochemical reduction has been regarded as a sustainable strategy to tackle energy-intensive operations by the Haber–Bosch process achieving catalytic conversion of N2 to NH3 under mild conditions. However, the challenge of N2 electroconversion emphasizes the requirement of efficient electrocatalysts. In this paper, we report the development of porous bromide-derived Ag film (BD-Ag/AF) as an efficient electrocatalyst for N2 reduction reaction. During electrochemical test, Br– anions are released and adsorbed onto the surfaces of the electrode, suppressing hydrogen evolution reaction. Such BD-Ag/AF shows a high Faradaic efficiency of 7.36% at −0.6 V vs reversible hydrogen electrode in 0.1 M Na2SO4, which is higher than that (0.38%) of porous Ag film without Br– anions. Moreover, it exhibits excellent long-term electrochemical durability.
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Nano Energy
·
2018
·
IF 13.12
Jingrui Han,Zaichun Liu,Yongjun Ma,Guanwei Cui,Fengyu Xie,Faxing Wang,Yuping Wu,Shuyan Gao,Yuanhong Xu,Xuping Sun
Electrochemical reduction has emerged as an environmentally-benign and sustainable approach alternative to the Haber–Bosch process for artificial N 2 fixation at ambient conditions, while the challenge associated with N 2 activation underlines the demand of efficient electrocatalysts for the N 2 reduction reaction (NRR). In this work, Nb 2 O 5 nanofiber is experimentally proved to act as a non-noble-metal NRR electrocatalyst for N 2 conversion to NH 3 with high activity and selectivity. When tested in 0.1 M HCl, such Nb 2 O 5 nanofiber achieves a high average NH 3 yield (43.6 µg h −1 mg −1 cat. ) and a high Faradaic efficiency (9.26%) at − 0.55 V vs. reversible hydrogen electrode , rivaling the performances of most reported aqueous-based NRR electrocatalysts under ambient conditions and even comparable with those under high temperature and pressure. Notably, it also shows high stability during electrolysis and recycling test. The catalytic mechanism of NRR on Nb 2 O 5 (181) surface is further discussed by density functional theory calculations.
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CHINESE CHEMICAL LETTERS
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2014
·
IF 1.178
Wei Wang,Ye Yuan,Fu-Xing Sun,Guang-Shan Zhu
Novel porous aromatic frameworks (PAF-53 and PAF-54) have been obtained by the polymerization of amino compound ( p -phenylenediamine and melamine) and cyanuric chloride. They display a certain amount of CO 2 adsorption capacity and highly selective separation of CO 2 /CH 4 and CO 2 /N 2 as 18.1 and 83 by Henry Law respectively. They may be applied as ideal adsorbents to separate and capture CO 2 .
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2015
·
IF 2.587
Song Zhao,Xiaochang Cao,Zijian Ma,Zhi Wang,Zhihua Qiao,Jixiao Wang,Shichang Wang
In this work, imidazolate framework ZIF-8 nanoparticles were synthesized and incorporated into a poly(vinylamine) (PVAm) coating solution. The chemical structure of a PVAm/ZIF-8 film was characterized by X-ray diffraction and attenuated total reflectance Fourier transform infrared spectroscopy techniques. Mixed-matrix membranes (MMMs) were developed by coating the PVAm/ZIF-8 mixed dispersion on a polysulfone (PSf) support membrane. Surface and cross-sectional scanning electron microscopy images of the MMMs were employed to observe the dispersion of nanoparticles in the polymer matrix. The CO2 permeance and CO2/N2 selectivity of the MMMs were evaluated by using a CO2/N2 mixture gas. Optimal preparation parameters for the MMMs were achieved by varying the incorporated ZIF-8 contents in the coating solution and the wet coating thickness. The effect of incorporated ZIF-8 on improving the gas permselectivity was revealed, and the mechanism of CO2-facilitated transport in the PVAm/ZIF-8/PSf membrane was analyzed. The CO2/N2 separation performance of PVAm/ZIF-8/PSf membranes with different wet coating thicknesses was also evaluated at 22–60 °C to analyze the changes of the gas permselectivity with increasing temperature.
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ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Xinyu Mao,Yu Chen,Shihao Li,Yang Yang,Chen Tao,Jiafu Shi,Zhongyi Jiang
Activation of the N≡N bond is of importance in photocatalytic nitrogen (N2) fixation, which strongly relies on the precise construction of catalytic active sites. Herein, we reported a dual-metal photocatalyst of Mo/UN(Zr) with a high proportion of Mo-coordinated Zr–O clusters (Zr–O–Mo dual-metal active sites) for photocatalytic N2 fixation, which was synthesized though post-modification to the defects of UN(Zr) by Mo. By contrast with the dual-metal photocatalyst of UN(Zr–Mo) synthesized via the co-mixing method, Mo/UN(Zr) possesses a higher proportion of Zr–O–Mo dual-metal active sites that is crucial for activating and polarizing N≡N bond as evidenced by in situ Fourier transform infrared (FTIR) spectroscopy combined with density functional theory (DFT) calculations. The synergistic effect of Zr–O–Mo dual-metal active sites resulted in a lower potential activation energy barrier for N2 activation which promoted the photocatalytic N2 fixation efficiency. The optimum photocatalytic N2 fixation rate of Mo/UN(Zr) was 255.7 μmol g–1 h–1 by adjusting the loading amount of Mo, which was enhanced about 2.5 times and 1.6 times compared with UN(Zr) and UN(Zr–Mo) photocatalyst, respectively. Our study will afford valuable guidance for designing efficient photocatalysts for photocatalytic N2 fixation.
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