CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Xiaoting Feng,Chenlu Liu,Kunkun Ren,Xinglei Zhao,Longjie Liu,Keming Zhang,Xiaohe Tian,Qingnan Wang,Xiangyu Liu,Yueyangchao Yu,Tianhe Gu,Shaofei Wang
The urgent need for efficient CO 2 capture technologies to mitigate climate change has driven the advancement of membrane-based separation systems. We report a mixed matrix membrane design through the in-situ growth of a ZIF-8 gel network within a Pebax-1657 matrix. By tuning the solvent ratio and concentration of modulator, ZIF-8 gel rather than particles are formed within the polymer, establishing a three-dimensional interconnected MOF network that ensures homogeneous filler dispersion and creates continuous gas transport nanochannels. The optimized membrane achieves a remarkable CO 2 permeability of 183.9 Barrer and a CO 2 /N 2 selectivity of 73.3, surpassing the 2008 Robeson upper bound. These values represent 190.4 % and 34.9 % enhancements in permeability and selectivity, compared to the pristine polymer. The membrane also demonstrates robust operational stability and maintains > 95 % of its initial performance over 60 days. This work offers a promising solution to creating continuous channels in CO 2 separation membranes.
研究领域:
材料科学
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化学工程
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环境技术
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膜分离
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碳捕集
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高影响因子
INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Fei Ma,Chao Wang,Yutong An,Yajie Liu,Xiaorong Xin,Kaicai Fan,Lei Wang,Guanjun Chen,Zhiqiang Hu,Tianrong Zhan
Cheap and advanced electrocatalysts for the oxygen evolution reaction (OER) are vitally significant but challenging for seawater electrolysis. Herein, a glow discharge N2 plasma is used to etch the [Fe(CN)6]4– group of the NiCoFe Prussian blue analogue (PBA) framework by highly reactive nitrogen radicals (the catalyst named N2-NiCoFe-PBA). Abundant CN vacancies (VCN) generated by this etching effectively suppress the Fe loss from N2-NiCoFe-PBA, while the lack of VCN results in the Fe leaching from the NiCoFe-PBA precursor during the anodic process. Consequently, N2-NiCoFe-PBA and NiCoFe-PBA are transformed into real active phases of NiCoFeOOH and NiCoOOH during the OER process, respectively. Theoretical calculations display that NiCoFeOOH has superior adsorption capacity toward OH– over Cl– to NiCoOOH, which is beneficial to excellent OER activity and anticorrosion performance in alkaline seawaters. In alkaline simulated and natural seawater, N2-NiCoFe-PBA exhibits much better OER performance with smaller η100 (293 and 323 mV) than NiCoFe-PBA (405 and 434 mV). N2-NiCoFe-PBA can run stably over 110 h in an alkaline high-salty electrolyte (1 M KOH + 2.0 M NaCl) at 250 mA cm–2. This study provides a modification method without destroying the structure to develop efficient and stable OER catalysts for seawater electrolysis.
研究领域:
材料科学
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电化学
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催化科学
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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Nan Li,Penny Xiao,Weijie Liu,Liying Liu,Zijian Wang,Jian Wang,Peng Gao,Qi Wu,Xinchao Ma,Gang Kevin Li
Compared with traditional commercial adsorbent zeolite pellets, binder-free molecular sieves can provide better adsorption performance. In this paper, we reported a novel method to synthesize binder-free zeolite X pellets (BF-Z), that is, zeolite X powder was intricately combined with halloysite nanotubes (HNTs) using hydroxypropyl methylcellulose (HPMC), and then the sample was calcinated to form crystals, where HPMC was decomposed and HNTs was also completely converted into binder-free X zeolite. The synthesized BF-Z showed the highest CO 2 adsorption capacity of 4.98 mmol/g at 303 K and 1 bar, compared with commercial NaX zeolites produced by Jianlong, Sigma and UOP companies. Calculated by IAST model, the separation coefficient of CO 2 to N 2 (CO 2 /N 2 = 25/75) on BF-Z is 74 at 303 K and 1 bar. The great separation performance of CO 2 from N 2 (CO 2 /N 2 = 25/75) was also exhibited in breakthrough experiments and a designed VSA process. Compared with commercial NaX (UOP), in breakthrough experiment, BF-Z presented high CO 2 adsorption capacity and rapid adsorption rate; and in designed thirty six-step vacuum swing adsorption process (VSA), the six-bed VSA system using BF-Z as adsorbents demonstrated excellent separation performance such as high CO 2 purity and recovery, low energy consumption and enhanced CO 2 production capacity. The notable efficacy of BF-Z in CO 2 adsorption and separation underscores its promising utility in both commercial and industrial settings.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
Nature Chemistry
·
2024
·
IF 19.2
Zhang Yangyu,Peng Xuanbei,Tian Han-Rui,Yang Bo,Chen Zuo-Chang,Li Jiejie,Zhang Tianhua,Zhang Mingyuan,Liang Xiaocong,Yu Zhiyang,Zhou Yanliang,Zheng Lirong,Wang Xiuyun,Zheng Jian-Wei,Tang Yu,Au Chak-tong,Jiang Lilong,Xie Su-Yuan
Developing highly effective catalysts for ammonia (NH 3 ) synthesis is a challenging task. Even the current, prevalent iron-derived catalysts used for industrial NH 3 synthesis require harsh reaction conditions and involve massive energy consumption. Here we show that anchoring buckminsterfullerene (C 60 ) onto non-iron transition metals yields cluster-matrix co-catalysts that are highly efficient for NH 3 synthesis. Such co-catalysts feature separate catalytic active sites for hydrogen and nitrogen. The ‘electron buffer’ behaviour of C 60 balances the electron density at catalytic transition metal sites and enables the synergistic activation of nitrogen on transition metals in addition to the activation and migration of hydrogen on C 60 sites. As demonstrated in long-term, continuous runs, the C 60 -promoting transition metal co-catalysts exhibit higher NH 3 synthesis rates than catalysts without C 60 . With the involvement of C 60 , the rate-determining step in the cluster-matrix co-catalysis is found to be the hydrogenation of *NH 2 . C 60 incorporation exemplifies a practical approach for solving hydrogen poisoning on a wide variety of oxide-supported Ru catalysts.
研究领域:
化学
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材料科学
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催化
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氨生产
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING & TECHNOLOGY
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2017
·Vol. 41
·期 2
·353-366
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IF 2.051
Shumin Wang,Qingping Guo,Shujun Liang,Peng Li,Xin Li,Jujie Luo
For the evaluation of CH 4 /N 2 separation, mixed-matrix membranes (MMMs) were fabricated by adding [Ni 3 (HCOO) 6 ] as a filler into the poly(styrene- b -butadiene- b -styrene) (SBS) polymer. The structures and morphologies of [Ni 3 (HCOO) 6 ] and [Ni 3 (HCOO) 6 ]/SBS MMMs were characterized by different techniques, proving the crystalline structure of [Ni 3 (HCOO) 6 ] in SBS polymer matrices. The structural integrity of the MMMs and good compatibility between [Ni 3 (HCOO) 6 ] and SBS polymer were examined by scanning electron microscopy. Gas permeation measurements revealed that membranes containing various [Ni 3 (HCOO) 6 ] loadings exhibited different separation performances. The operational temperature exerted a significantly positive effect on the separation of CH 4 and N 2 .
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高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2026
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IF 9
Peng Li,De Ao,Zhenjie Gu,Zhihua Qiao,Chongli Zhong
Metal-organic framework (MOF)-based membranes show promising potential for gas separation. However, it remains challenging to fully exploit the synergistic advantages of MOF crystals and polymers for fabricating highly loaded mixed matrix membranes (MMMs). Herein, a highly loaded ZIF-8 ultrathin MMM was prepared in situ via a stepwise growth strategy. Driven by the diffusion rate difference between the ligand and polyethyleneimine (PEI-600), preferentially formed ZIF-8 crystals served as the dominant phase, while the subsequently developed PEI-Zn 2+ crosslinked network acted as an intergranular densification phase. Owing to the reduction in ZIF-8 crystal size induced by PEI, the MMMs exhibited an ultrathin thickness of only 160 nm. Furthermore, PEI enhanced the molecular sieving ability of crystals and membrane's CO 2 /N 2 solubility selectivity by regulating the pore structure and membrane composition. With a high ZIF-8 loading of 84.3 %, the resulting MMMs demonstrated an excellent CO 2 permeance of 3177.4 GPU, accompanied by a CO 2 /N 2 selectivity of 36.9. Notably, it maintained stable separation performance after bending and during long-term operation, showing good processability and industrial application potential. This strategy not only reinforces the advantages of MOF-based gas separation membranes but also provides a new paradigm for fabricating highly loaded MMMs.
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高影响因子
ACS Applied Polymer Materials
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2026
·
IF 5.2
Ziyi Yuan,Zhihong Lin,Kejing Li,Jian Li,Viatcheslav Freger,Xuezhong He
Polymers of intrinsic microporosity (PIMs) are promising membrane materials for CO2 separation due to their high permeability; however, their limited CO2/N2 selectivity restricts practical application. Herein, mixed-matrix membranes (MMMs) were fabricated by incorporating a CO2-molecularly imprinted UiO-66-NH2 filler (MIP@U) into amidoxime-functionalized PIM-1 (AOPIM-1), followed by thermal treatment at 160 or 250 °C under vacuum to regulate the membrane microstructure. Spectroscopic and porosity analyses (FTIR, XRD, and N2 physisorption) show that thermal treatment at 160 °C promoted oxadiazole-ring formation, leading to enhanced subnanometer microporosity and improved CO2/N2 selectivity. In contrast, treatment at 250 °C partially regenerates nitrile groups and generates larger micropores, resulting in higher CO2 permeability but reduced selectivity. The MIP@U filler introduces CO2-recognition cavities and improves interfacial compatibility, enabling synergistic control of polymer microporosity and interfacial transport pathways. The optimized 3 wt % MIP@U/AOPIM-1-TR160 membrane achieves a CO2 permeability of ∼1600 Barrer and a CO2/N2 selectivity of 50.8. The membrane also demonstrates stable performance under pressures up to 12 bar and during 30 h of continuous operation at 2 bar. This study highlights a dual-approach strategy combining thermally tailored PIM chemistry with molecularly imprinted MOF fillers for designing high-performance MMMs for CO2 capture.
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2026
·Vol. 14
·期 36
·16132-16144
·
IF 7.6
Sun Wenbo,Chen Yongning,Guo Xiaoxuan,Wang Yan,Wang Yin,Jiang Yijie,Sun Wenlong,Fu Zhiqiang,Li Jianan,Peng Chong
As a crucial anodic pathway, the urea oxidation reaction (UOR) holds immense potential for the purification of nitrogenous sewage as well as the energy-saving generation of hydrogen power. However, conventional nickel-based catalysts often trigger detrimental C–N bond cleavage of urea, yielding deleterious by-products such as nitrite (NO 2 – ) and nitrate (NO 3 – ), which severely constrains their practical viability. Inspired by bioenzymes that regulate substrate pathways via intricate hydrogen-bonding networks, this study employed Ni(OH) 2 as a scaffold to engineer an enzyme-mimetic dynamic hydrogen-bonding microenvironment through the coordination of terephthalic acid (TPA) with Ni sites. This strategy enables the precise modulation of the UOR pathway. Driven by a minimal potential of just 1.41 V vs. the reversible hydrogen electrode (RHE), the synthesized Ni(OH) 2 -TPA/NF electrode demonstrated exceptional UOR catalysis, achieving a response current density of 100 mA cm –2 . Furthermore, it demonstrated exceptional N 2 selectivity and Faradaic efficiency while maintaining robust structural and electrochemical stability over a 48 h chronoamperometric test. Mechanistic insights from density functional theory (DFT) simulations combined with in situ Fourier transform infrared (FTIR) analysis confirmed that the configuration of urea molecules was accurately constrained by the TPA-mediated hydrogen-bonded matrix. This spatial confinement optimized the N–N coupling process while successfully suppressed the rupture of C–N linkages. This work overcomes the critical bottleneck of suboptimal UOR selectivity in traditional nickel-based systems, offering a new paradigm for the development of high-efficiency, sustainable catalysts and providing a theoretical foundation for the industrialization of urea electrolysis in environmental and energy applications.
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高影响因子
JOURNAL OF CHEMICAL THERMODYNAMICS
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2017
·
IF 2.726
Dong Fu,Xue Feng,Pan Zhang
Amino acid ionic liquids (AAILs) including 1-butyl-3-methylimidazolium glycinate ([Bmim][Gly]), 1-butyl-3-methylimidazolium L -lysinate ([Bmim][Lys]) and tetramethylammonium glycinate ([N 1111 ][Gly]) were used to enhance the absorption of CO 2 in N -methyldiethanolamine (MDEA) aqueous solutions. The mole fractions of CO 2 in N 2 + CO 2 gas mixtures ranged from 0.2 to 1.0. The mass fractions of MDEA and AAILs respectively ranged from 0.300 to 0.400 and 0.050 to 0.100. The absorption capacity and absorption rate under series of conditions were presented and the influences of CO 2 partial pressure and the types of AAILs on the absorption performance were demonstrated.
研究领域:
化学工程
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环境科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Qingping Xin,Shuo Li,Faxin Ma,Jianping Guo,Shaofei Wang,Guangyu Xuan,Xiaoli Ding,Lei Zhang,Yuzhong Zhang
The preparation of mixed matrix membranes (MMMs) using metal–organic framework (MOF) as fillers is one of the simple and effective methods to improve the gas permeability and selectivity of membranes, and it has an attractive prospect to achieve controllable gas separation process. Herein, NH 2 -MIL-53 nanoparticles are synthesized by hydrothermal method and modified by aminoazobenzene (Azo) by decompression loading technology. The multifunctional Azo@NH 2 -MIL-53 nanoparticles are incorporated into the Pebax matrix to fabricate MMMs for efficient and controllable SO 2 separation. Pebax/Azo@NH 2 -MIL-53–20% membrane exhibits the maximum SO 2 permeability of 2570 Barrer with a SO 2 /N 2 selectivity of 717 and the separation process of SO 2 /N 2 has dynamic photo-responsive characteristics under different light conditions, which is attributed to the incorporation of the Azo@NH 2 -MIL-53. First, the NH 2 -MIL-53 nanoparticles with high specific surface area of 637 m 2 .g −1 and pore size of 1.50 nm are introduced into MMMs to construct rich SO 2 transport channels, increasing the diffusivity selectivity. Second, the inherent –NH 2 groups and introduced -N = N- groups in Azo@NH 2 -MIL-53 increase the affinity of SO 2 , enhancing the solubility selectivity. Third, by artificially changing the light conditions to accurately control the conformation of Azo and the pore structure of NH 2 -MIL-53 is changed, which significantly changes the SO 2 adsorption capacity of NH 2 -MIL-53. Due to light is available in abundance in the form of sunlight, the mixed matrix membrane coupled with photo-responsive MOF can achieve more efficient and energy-saving gas separation process.
研究领域:
材料科学
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环境工程
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Xiaoya Zhao,Yuchao Chen,Qichao Ding,Tonghu Xiao,Xing Yang
Membranes made of polyoctylmethylsiloxane (POMS) have emerged as an attractive alternative for volatile organic compound (VOC) separation and recovery. We developed an octyl-modified silicone rubber (OMSR) membrane for VOC/N2 separation by a novel strategy. The OMSR membrane was made via the side-chain cross-linking of the poly(vinylmethylsiloxane) and a tailored octyl-grafted poly(hydromethylsiloxane). The octyl side chains were enriched around the cross-linking points composed of the supramolecular structure with octyl-rich parallel polysiloxane domain, which determined the selective transport of VOCs relative to N2. Compared to membranes without octyl, the OMSR membranes exhibited excellent thermal and mechanical stability and simultaneously high permeability and selectivity in VOC/N2 separation, e.g., with >70,000 Barrer of permeability (5.7 times higher) and >240 (3.5 times higher) of selectivity with toluene/N2. We demonstrated that this unique structure has the potential to overcome the permeability–selectivity trade-off relationship, producing a promising class of membranes for removal of VOCs.
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高影响因子
ELECTROCHIMICA ACTA
·
2022
·
IF 7.336
Xiaobo Ma,Lijun Gao,Qiyu Zhang,Weibo Hua,Yating Zhang,Xinyang Li,Juan Yang,Shujiang Ding,Chao Hu
The traditional Haber-Bosch N 2 fixation process suffers from rigorous reaction conditions and massive CO 2 emission. By contrast, N 2 electroreduction by water to the direct production of NH 3 can be conducted at room temperature and atmospheric pressure, and thus has been attracting increasingly attention. Herein, we develop a nano-CaCO 3 template route for the synthesis of Fe, N co-doped porous carbon materials from zeolitic imidazolate framework-8 (ZIF-8). The Fe atoms are atomically dispersed in the skeleton of carbon and bonded with four nitrogen atoms . Interestingly, the morphology and pore structure of these carbons have notable effects on their performance for the electrocatalytic reduction of N 2 . With an optimized morphology and pore structure tuned by the addition of nano-CaCO 3 template, the ZIF-8 derived Fe, N co-doped carbon catalyst shows a Faradaic efficiency of 13.14% and a NH 3 yield as high as 13.01 µg h −1 mg cat −1 (−0.2 vs . reversible hydrogen electrode) for N 2 reduction reaction in 0.1 M KOH aqueous electrolyte . Morphology engineering strategy may open a new path to designing and synthesizing high-performance carbon-based catalysts for the electroreduction of N 2 to NH 3 .
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高影响因子
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