JOURNAL OF MEMBRANE SCIENCE
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2023
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IF 9.5
Hongyong Zhao,Ting Song,Xiaoli Ding,Ruyi Cai,Xiaoyao Tan,Yuzhong Zhang
Membrane technology for O 2 /N 2 separation is a mature industrial unit. Membranes with excellent permeation-separation performance are still one of the critical requirements. The cobalt-based compounds have been well known for their good affinity for O 2 , which can facilitate O 2 transfer and improve the O 2 /N 2 selectivity in membranes. The cobalt-based compounds, moreover, have a magnetic responsive effect, which can lead to a further improvement in O 2 /N 2 separation under a magnetic field. A class of PIM-1 mixed matrix membranes (MMMs), containing cobalt-based ionic liquid (CILs)@polyarylate (aromatic polyester) (PAR) (core-shell) composite nanospheres (CILs@PAR (c-s) CNPs), were prepared. Chemical compositions of CILs@PAR (core-shell) CNPs were determined by Fourier transform infrared spectroscopy (FTIR). Morphologies and structures of CILs@PAR (core-shell) CNPs were observed by transmission electron microscopy (TEM). Gas adsorption properties of CILs@PAR (core-shell) CNPs were tested. Thermal properties of the (CILs@PAR (c-s) CNPs)/PIM MMMs were investigated by simultaneous thermal analysis (TGA-DSC). Gas permeation-separation performances of the (CILs@PAR (c-s) CNPs)/PIM MMMs were also reported. Compared with the original PIM-1 membrane, the (CILs@PAR (c-s) CNPs)/PIM MMMs display higher O 2 /N 2 selectivity because of cobalt-based ionic liquid as O 2 carrier, coupled with a reduction in O 2 permeability. With increasing the content of the CILs@PAR (c-s) CNPs, the O 2 /N 2 selectivity increases, and the O 2 permeability decreases. It is also found that, as a magnetic field on the MMMs, the O 2 /N 2 selectivity further increases; and it increases more, as a higher content of CILs@PAR (c-s) CNPs. Therefore, the (CILs@PAR (c-s) CNPs)/PIM MMMs exhibit excellent O 2 /N 2 selectivity of ∼5 coupled with good O 2 permeability of ∼140 Barrer under a 180 mT magnetic field and show great potential for air separation.
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Materials Science and Engineering B-Advanced Functional Solid-State Materials
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2023
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IF 3.6
Tianzhu Zhang,Jiaqin Liu,Kangwei Zhu,Yi Hu,Ruidong Liu,Jun Chen,Chunli Jiang,Jun Chen
Tungsten oxide is a promising electrocatalyst for water splitting reactions, due to its flexible chemical state, strong structural malleability and good corrosion resistance. Herein, the surface engineering on WO 3 was conducted by a controllable N 2 plasma for enhancing the performance of water splitting reactions. Under the specific N 2 plasma treatment, the surface crystalline phase and the surface morphology of the tungsten oxide can be changed, as well as the creation of oxygen vacancies. These changes lead to a greatly increased electrochemical surface area, a narrowed bandgap, and a distorted crystal lattice. For oxygen evolution reaction (OER) in 1.0 M KOH, the activity of the modified tungsten oxide electrodes presents a positive correlation with the input plasma, and an optimal overpotential of 269 mV @ 10 mA cm −2 is achieved with a Tafel slope of 122 mV dec -1 . With a high N 2 plasma flux, the W-N bond can be formed on the tungsten oxide surface, which contributes to the promotion of the hydrogen evolution reaction (HER) activity, and an overpotential of 93 mV @ 10 mA cm −2 in 1.0 M KOH is exhibited, and the Tafel slope largely reduced to 76 mV dec -1 . Such a facile strategy provides an engineering route of preparing efficient electrodes for water splitting reactions.
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Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 13
·8372-8377
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IF 12.732
Songliang Liu,You Xu,Shiqian Jiao,Wenjing Tian,Tongqing Zhou,Ziqiang Wang,Xiaonian Li,Liang Wang,Hongjing Wang
Current methods for industrial-scale ammonia synthesis rely excessively on fossil fuels, causing severe CO2 emissions. The electrochemical nitrogen reduction reaction (NRR) is a sustainable and environmentally friendly technology for ammonia synthesis under environmental conditions. Herein, we demonstrate the rational construction of Au3Cu@Cu nanocages with unique porous core–shell heterostructured walls by a facile two-step synthetic strategy. Due to the hollow cavities, porous core–shell heterostructured walls, and Au3Cu@Cu two-component composition, the as-constructed Au3Cu@Cu nanocages exhibit excellent NRR performance in 0.1 M Na2SO4 saturated with N2, achieving a high ammonia yield up to 33.97 μg h−1 mgcat.−1 and a faradaic efficiency of 21.41% at −0.2 V (vs. the reversible hydrogen electrode). This study will provide insight into the reasonable design and construction of hollow nanostructures with porous heterostructured walls for electrocatalytic applications.
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Nano Research
·
2020
·Vol. 13
·期 11
·2967-2972
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IF 8.183
Wei Peipei,Geng Qin,Channa Ali Imran,Tong Xin,Luo Yongsong,Lu Siyu,Chen Guang,Gao Shuyan,Wang Zhiming,Sun Xuping
To develop highly efficient electrochemical catalysts for N 2 fixation is important to sustainable ambient NH 3 production through the N 2 reduction reaction (NRR). Herein, we demonstrate the development of vanadium phosphide nanoparticle on V foil as a high-efficiency and stable catalyst for ambient NH 3 production with excellent selectivity. The high Faradaic efficiency of 22% with a large NH 3 yield of 8.35 × 10 −11 mol·s −1 ·cm −2 was obtained at 0 V vs. the reversible hydrogen electrode in acid solution, superior to all previously studied V-based NRR catalysts. Density functional theory calculations are also utilized to have an insight into the catalytic mechanism.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Jinxiu Zhao,Xuejing Liu,Xiang Ren,Xu Sun,Dongxu Tian,Qin Wei,Dan Wu
Electrochemical N 2 reduction is developing as an appealing carbon-neutral strategy for NH 3 artificial synthesis but seriously influenced by requiring high-efficiency electrocatalysts for the N 2 activation at ambient conditions. Here, we reported that defective-rich ZnS nanoparticles supported on reduced graphene oxide (DR ZnS-rGO) acts as a high-efficiency electrocatalyst for ambient N 2 -to-NH 3 conversion with excellent selectivity. In 0.1 M HCl, such DR ZnS-rGO presents a large NH 3 yield of 51.2 μg h –1 mg cat. –1 (−0.15 V vs . reversible hydrogen electrode, RHE) and a high faradic efficiency of 28.2 % (−0.10 V vs . RHE), as well as high electrochemical and structure stability. Isotopic labelling samples experiments reveal that the synthetic NH 3 directly arise from the supplied N 2 . Density functional theory calculations demonstrated that the engineering S vacancies in DR ZnS-rGO not only provide reaction sites for N 2 -to-NH 3 conversion but activate of N 2 molecules.
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Frontiers in Energy Research
·
2020
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IF 2.746
Wang Ning,Song Qing-Song,Liu Wen-Jing,Zhang Jian
A new ringlike V2O3 architecture was successfully synthesized by a template-free hydrothermal method, and the sulfur ions-assisted central-etching mechanism of the ringlike structure was proposed. Herein, as a proof-of-concept experiment, taking V2O3 nanorings as non-noble-metal-free nitrogen reduction reaction (NRR) catalysts, they show desired electrocatalytic performance toward NRR under ambient conditions (maximum yield: 47.2 µg h−1 mgcat.−1 at −0.6 V vs. reversible hydrogen electrode, maximum Faraday efficiency: 12.5% at −0.5 V vs. reversible hydrogen electrode), which is significantly higher than those of noble metal-based catalysts.
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ACS Nano
·
2020
·
IF 14.588
Feng Ma,Yangyang Wan,Xiaoming Wang,Xinchao Wang,Jiashun Liang,Zhengpei Miao,Tanyuan Wang,Cheng Ma,Gang Lu,Jiantao Han,Yunhui Huang,Qing Li
The sluggish kinetics of lithium polysulfides (LiPS) transformation is recognized as the main obstacle against the practical applications of the lithium–sulfur (Li–S) battery. Inspired by molybdoenzymes in biological catalysis with stable Mo–S bonds, porous Mo–N–C nanosheets with atomically dispersed Mo–N2/C sites are developed as a S cathode to boost the LiPS adsorption and conversion for Li–S batteries. Thanks to its high intrinsic activity and the Mo–N2/C coordination structure, the rate capability and cycling stability of S/Mo–N–C are greatly improved compared with S/N–C due to the accelerated kinetics and suppressed shuttle effect. The S/Mo–N–C delivers a high reversible capacity of 743.9 mAh g–1 at 5 C rate and an extremely low capacity decay rate of 0.018% per cycle after 550 cycles at 2 C rate, outperforming most of the reported cathode materials. Density functional theory calculations suggest that the Mo–N2/C sites can bifunctionally lower the activation energy for Li2S4 to Li2S conversion and the decomposition barrier of Li2S, accounting for its inherently high activity toward LiPS transformation.
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PubMed
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JOURNAL OF HAZARDOUS MATERIALS
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2020
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IF 9.038
Y.L. Zhao,G.G. Li,H.M. Hou,J.C. Shi,S.N. Luo
We investigate atomic and molecular emission of laser-ablated nitromethane in an Ar or N 2 buffer gas, with fs laser-induced breakdown spectroscopy. The electronic bands of CN, C 2 , and NH molecules and the atomic transition lines of C I, N I, and H α are identified. The time series of the emissions are obtained, and the formation mechanisms of CN and C 2 are deduced. The CN violet system, the B 2 Σ + -X 2 Σ + (0-0) band, is chosen to extract plasma temperature from the experimental spectra.
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ACS Omega
·
2021
·
IF 3.512
Shuangping Xu,Wenqiang Ma,Hailiang Zhou,Yushu Zhang,Hongge Jia,Jingyu Xu,Pengfei Jiang,Xintian Wang,Wenwen Zhao
The synthesis of poly(methyhydrosiloxane) (PMHS) and N,N′-bis(3-allyl)pyromellitic diimide was optimized for O2/N2 separation. The membrane exhibits excellent mechanical and thermal properties and shows an O2/N2 selectivity of up to 4.44 with an O2 permeability of 31.0 Barrer; compared with polydimethylsiloxane (PDMS) and pure polyimide (PI) membranes, the separation selectivity shows a 107% increase for PDMS, and the permeation shows a 660% increase for pure PI. The obtained results were well above the ones reported on the literature for similar conditions opening the door for the preparation of a stable polysiloxane (PMHS-I) gas separation membrane with extraordinary O2/N2 separation performance.
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PubMed
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2019
·
IF 5.107
Rui Ding,Wenji Zheng,Kai Yang,Yan Dai,Xuehua Ruan,Xiaoming Yan,Gaohong He
High permeability and selectivity are desirable for mixed matrix membranes (MMMs) based CO 2 separation. Herein, a microemulsion based mixed linker strategy is proposed to introduce amino groups during the growth of ZIF-8. Compared to post-synthetic modification, this method presents a less reduction in S BET of ZIF-8, which is beneficial for CO 2 adsorption. By controlling the ratio of 2-methylimidazole to 2-aminobenzimidazole, NH 2 -ZIF-8 with various morphologies and sizes were synthesized and serve as the filler to fabricate the MMMs for CO 2 capture. From the scanning electron microscopy (SEM), no obvious agglomerations or defects are observed in ZIF-8/Pebax MMMs, due to the amino groups in ZIF-8 can interact with the amide in Pebax chain, which can improve compatibility between ZIF-8 and Pebax. With the amino groups, NH 2 -ZIF-8 shows higher affinity with CO 2 than that of non-amine-functionalized ZIF-8, leading to an enhancement in the separation performances. When the MMM doped with 6 wt% of NH 2 -ZIF-8(10), the CO 2 permeability reaches up to 163.8 Barrer, which increases by around 53% and 107.6% in contrast with the ZIF-8/Pebax MMM and pure Pebax membrane. Besides, the CO 2 /N 2 selectivity is enhanced by around 10% and 27%, respectively. These results indicate that amine-functional modification by mixed ligands is a useful way to construct MOFs-based MMMs with high performance for CO 2 /N 2 separation.
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ELECTROCHIMICA ACTA
·
2018
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IF 5.116
Bo Xu,Zaichun Liu,Weibin Qiu,Qian Liu,Xuping Sun,Guanwei Cui,Yuping Wu,Xiaoli Xiong
Identification of new effective and selective N 2 reduction electrocatalyst is still of critical importance for fundamental and application research. Here, we report La 2 O 3 nanoplate performing as an efficient metal oxide catalyst for electrochemical N 2 fixation to NH 3 , which exhibits excellent selectivity and stability with a high Faradaic efficiency of 4.76% and a NH 3 yield rate of 17.04 μg h −1 mg −1 cat. at −0.8 V vs. reversible hydrogen electrode (RHE) in 0.1 M Na 2 SO 4 solution under atmospheric pressure. Density functional theory (DFT) calculation results show that La atoms in La 2 O 3 act as the active sites for efficiently adsorbing N 2 . The optimal adsorption approach of N 2 molecule on the (011) face of La 2 O 3 is end-on-two configuration which is highly activated. Thus La 2 O 3 exhibits high performance for electrochemical reduction of N 2 .
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2017
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IF 3.359
Cheng Tan,Lei Li,Kongzhai Li,Dapeng Zhong
A novel method to separate As from high As-Sb dust using Fe 2 O 3 as a fixative under an O 2 -N 2 atmosphere is proposed. Here, Sb is oxidised and converted to Sb 2 O 4 and FeSbO 4 that remain in the roasted residue, and As is volatilized in the form of As 4 O 6 . The Sb 2 O 3 can be selectively oxidised from the dust by using 21 vol% O 2 , but the formation of amorphous substance (As-Sb-O) hinders the effective separation of As and Sb. Adding Fe 2 O 3 hinders the amorphous substance formation and destroys the structure of the solid solution ((Sb, As) 2 O 3 ) in the raw material by converting the Sb component in it to FeSbO 4 . Therefore, the volatilization rates of As and Sb can reach up to 90.53% and only 13.20%, respectively at a roasting temperature of 723 K, roasting time of 90 min, an Fe 2 O 3 dosage of 15 mass%, and O 2 content of 21 vol%.
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