CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Yu Wang,Yunlei Shi,Dazhen Xiong,Zhiyong Li,Huiyong Wang,Xiaopeng Xuan,Jianji Wang
Ammonia (NH 3 ) is produced from nitrogen (N 2 ) and hydrogen (H 2 ) by the Harber-Bosch process at high pressure and high temperature. Due to the reversibility and low conversion efficiency of the reaction, the product contains a large amount of raw gas, which seriously affects the production efficiency of ammonia. Therefore, it is essential to exploit high-performance adsorbents for separating NH 3 from NH 3 /N 2 /H 2 mixtures. Herein, we designed and synthesized a kind of metal–organic framework (MOF) composites by anchoring metal chloride (NiCl 2 , CoCl 2 , or SnCl 2 ) on the bipyridinium groups in the MOF-253(Al) pores. It is found that the optimal composite shows an NH 3 uptake capacity of 18.0 mmol/g at 25.0 °C and 1.0 bar, which is 3.33 times that of the pristine MOF-253(Al), and the composite exhibits a much faster adsorption kinetics of NH 3 than the pristine MOF-253(Al). Significantly, the excellent NH 3 uptake capacity at low pressure allows selective trapping of NH 3 from NH 3 /N 2 /H 2 at 25.0 °C with the selectivity coefficients of 5708 to N 2 and 2320 to H 2 . Spectral measurements reveal that the synergistic action of NH 3 coordination to the metal in the MOF and the hydrogen bonding of NH 3 with both O atoms of the carboxyl groups and Cl − of the guest molecules account for such an excellent capture and selectivity. In general, the strategy developed here is simple and effective for improving the selectivity of NH 3 separation, which opens a new way for the design of high-performance solid adsorbents.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Chao-Ying Gao,Lin Ding,Yang Li,Ning Xu,Yakun Wu,Wenbo Wang,Jinghai Liu,Yang Yang
In the era of global warming, the conversion of carbon dioxide into high-value products has become a widely scrutinized emerging mitigation strategy. Metalation of bpy-containing MOF-253 led to the synthesis of MOF-253–0.5Ag, which acts as an efficient catalyst for the carbonylative cyclization of CO2 with alkyne molecules (such as propynyl alcohols and propynyl amines) at room temperature and ambient CO2 pressure, yielding the corresponding α-alkyl cyclic carbonates and oxazolidinones, thus endowing the catalytic system with bifunctional characteristics. Additionally, the MOF-253–0.5Ag catalyst demonstrated stability, high activity, and recyclability. The mechanisms were further elucidated through experimental results and NMR analysis, demonstrating that Ag(I) can effectively activate the C≡C bonds and hydroxy/amino groups of the substrates.
研究领域:
材料化学
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环境科学
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催化化学
✓ 已验证
DOI
PubMed
高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
·
2026
·
IF 5.9
Yang Li,Wen-Bo Wang,Chen-Yu Liu,Yang Yang,Chao-Ying Gao
The alcoholysis of epoxides is the core reaction for the synthesis of key intermediates of agricultural chemicals, drugs and polymers. Traditional catalysts have problems such as harsh synthesis conditions, difficult recovery or insufficient activity. In this paper, a new heterogeneous catalyst MOF-253-Cu was prepared by anchoring Cu (II) ions to the bipyridine N, N′ chelating site of MOF-253 through post-synthesis modification strategy. Characterized by PXRD, FTIR, XPS, etc., it was confirmed that Cu (II) was stably coordinated with the MOF-253 ligand, and the catalyst retained the original framework and the element distribution was uniform. The methanolysis of styrene oxide was used as a model reaction. The conversion rate of MOF-253-Cu reached 100% and the conversion frequency (TOF) was as high as 125 h −1 at room temperature. The performance was better than that of other metal functionalized derivatives such as Co, Ag and Ni. The catalyst has good universality for alcohols with different chain lengths/structures and various epoxides, and can be recycled for 5 times without obvious activity attenuation. The mechanism study shows that the reaction follows the S N 1 mechanism, and Cu (II) acts as a Lewis acid site to activate the epoxy ring. The MOF-253-Cu catalyst developed in this study has the advantages of simple synthesis, mild reaction conditions, high activity, recyclability and strong universality.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2026
·
IF 9.1
Chao-Ying Gao,Yang Li,Wenbo Wang,Chenyu Liu,Jinghai Liu,Yang Yang
Developing heterogeneous catalysts capable of activating inert CO 2 under mild conditions remains a central challenge in sustainable chemistry. Herein, we report the rational design of a robust bimetallic platform, MOF-253-0.5(Cu/Ag), constructed by post-synthetic incorporation of synergistic Cu(II) and Ag(I) sites within the 2,2′-bipyridine pockets of the MOF-253 framework. The catalyst exhibits high turnover frequencies (TOF) of 260 h −1 under ambient conditions, ranking among the highest reports. It also maintains robust stability over 5 cycles, achieving a cumulative turnover number (TON) of 999.2. Even under diluted CO 2 conditions mimicking industrial flue gas, its catalytical activity remains largely unaffected. 1 H NMR mechanistic analysis was used to monitor the reaction processes. Comparative experiments with monometallic and pristine MOF confirm the superior performance of the bimetallic system, attributed to Cu/Ag synergy that activates both the C≡C bond and CO 2 . Furthermore, comprehensive density functional theory (DFT) calculations provided clear insights into the energetics and elementary steps of the catalytic cycles. This work highlights the power of site-isolated bimetallic MOFs in CO 2 chemical fixation.
✓ 已验证
DOI
高影响因子
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