ACS Sustainable Chemistry & Engineering
·
2024
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IF 7.1
Jitong Deng,Yanan Zhang,Hongjing Han,Yongjun Zhang,Haiying Wang,Xuzhong Gong,Yanguang Chen
The chemical looping conversion of CH4 has been one of the most promising technologies for achieving the “two-carbon” strategy. Fe2O3 oxygen carrier cannot maintain the excellent release performance of lattice oxygen at high temperature due to the sintering and carbon deposition. Therefore, quaternary La1–xSrxFe1–y CoyO3 perovskite was selected as the transfer support of oxygen ions. By using the MOF precursor method, ternary La0.8Sr0.2FeO3 was prepared via the introduction of metal Sr into the binary LaFeO3. The adsorption energy of CH4 on the La0.8Sr0.2FeO3 was the lowest (−0.054 eV), compared with separate Fe2O3 and LaFeO3, and the adsorption energy of free H at the adjacent Fe site was the lowest (1.650 eV). Furthermore, the La1–xSrxFe1–yCoyO3 perovskite was successfully synthesized by the doping of Co into the ternary La0.8Sr0.2FeO3. La0.8Sr0.2Fe0.8Co0.2O3 was chosen to composite Fe2O3 oxygen carrier. As m(Fe2O3):m(La0.8Sr0.2Fe0.8Co0.2O3) = 1:1, the lattice oxygen conversion rate was less than 47% and the selectivity of CO2 reached 99.5% through the synergistic effect of lattice oxygen and oxygen vacancies. Fe2O3–La0.8Sr0.2Fe0.8Co0.2O3 increased the lattice oxygen conversion by 17.6%, compared with Fe2O3–La0.8Sr0.2FeO3. After the CH4 chemical looping conversion cycles five times, Fe2O3–La0.8Sr0.2Fe0.8Co0.2O3 still had favorable structural stability and oxidation performance, and the lattice oxygen conversion rate still reached >95%.
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Advanced Science
·
2024
·Vol. 11
·期 30
·2401990
·
IF 14.3
Qinhui Guan,Weiguang Ran,Dapeng Zhang,Wenjuan Li,Na Li,Baibiao Huang,Tingjiang Yan
Photocatalytic CO 2 reduction is considered as a promising strategy for CO 2 utilization and producing renewable energy, however, it remains challenge in the improvement of photocatalytic performance for wide-band-gap photocatalyst with controllable product selectivity. Herein, the sulfur-doped In(OH) 3 (In(OH) x S y -z) nanocubes are developed for selective photocatalytic reduction of CO 2 to CH 4 under simulated light irradiation. The CH 4 yield of the optimal In(OH) x S y -1.0 can be enhanced up to 39 times and the CH 4 selectivity can be regulated as high as 80.75% compared to that of pristine In(OH) 3 . The substitution of sulfur atoms for hydroxyl groups in In(OH) 3 enhances the visible light absorption capability, and further improves the hydrophilicity behavior, which promotes the H 2 O dissociation into protons (H * ) and accelerates the dynamic proton-feeding CO 2 hydrogenation. In situ DRIFTs and DFT calculation confirm that the non-metal sulfur sites significantly weaken the over-potential of the H 2 O oxidation and prevent the formation of ·OH radicals, enabling the stabilization of * CHO intermediates and thus facilitating CH 4 production. This work highlights the promotion effect of the non-metal doping engineering on wide-band-gap photocatalysts for tailoring the product selectivity in photocatalytic CO 2 reduction.
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JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Zikang Li,Guangyao Fan,Muning Chen,Qin Shen,Shenzhen Cong,Roberto Castro-Muñoz,Dongyang Li,Jing Wang,Yatao Zhang
By combining the advantages of polymers and porous nano-fillers, mixed matrix membranes (MMMs) have demonstrated outstanding gas separation performance. However, the ideal matching between polymers and nano-fillers is still a challenge especially under high filler loading conditions. To address this interfacial challenge, an in-situ grown amino-functionalized ZIF-8 (NH 2 -ZIF-8) is embedded in 6FDA-DAM to prepare MMMs. Compared to ZIF-8, NH 2 -ZIF-8 not only can enhance compatibility and interfacial adhesion because of the extensive hydrogen bonding, but also effectively modulates its structural flexibility by increasing the rigidity of Zn–N bonds within the ZIF-8 framework. The enhanced framework rigidity of NH 2 -ZIF-8 successfully improves the CO 2 /CH 4 separation capability of the MMMs. Under a high filler loading of 30 wt%, the CO 2 /CH 4 selectivity of the optimized NH 2 -ZIF-8/6FDA-DAM MMMs reached 35.1 and the permeability reached 1225.9 Barrer, which increased by 25.36 %, and 8.94 % respectively compared to the ZIF-8 MMMs, exceeding the 2008 Robeson upper bound. Molecular simulations further reveal the enhanced diffusion selectivity of NH 2 -ZIF-8 and the strong interactions between surface –NH 2 groups and electron-rich O/F heteroatoms in the 6FDA-DAM polyimide matrix. These simulations quantitatively elucidated the critical role of interfacial structure in determining gas separation performance. The mechanistic insights provided in this study offer valuable theoretical guidance for the development of high-performance membrane materials for CO 2 capture and gas purification applications.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Jiepeng Zhao,Zijian Li,Yu Zuo,Sai Huang,Zhaomin Tong,Yifei Ma,Liantuan Xiao,Suotang Jia,Xuyuan Chen,Mei Wang
NH 2 -MIL-125(Ti) (NM) is a prototypical metal–organic framework (MOF) photocatalyst with visible-light responsiveness. However, its practical application in CO 2 reduction is significantly limited by fast charge carrier recombination and poor product selectivity. Constructing heterojunctions with appropriately matched semiconductors offers an effective strategy to overcome these limitations, where coupling material selection and precise interfacial engineering are key. ZnO, a stable n-type wide-bandgap semiconductor, not only possesses excellent electron mobility but also exhibits suitable conduction band alignment with NM, enabling favorable interfacial charge transfer. Moreover, ZnO can form an interfacial Ti–O–Zn bonding bridge with NM, facilitating directional electron transport and suppressing charge recombination. In this work, we employed atomic layer deposition (ALD) to construct uniform ZnO shells on NM with sub-nanometer precision, thereby finely tuning the ZnO loading and interface structure. A series of ZnO@NH 2 -MIL-125 (ZnO@NM) composites are obtained by controlling the ZnO loading, with the optimal sample showing the highest activity, yielding 13.30 μmol h −1 g −1 of CO and 5.47 μmol h −1 g −1 of CH 4 . Notably, CH 4 selectivity is significantly improved from 16 % to 29 %, and further increases to 31 % under gas-solid conditions. In situ Fourier Transform Infrared (FTIR) spectroscopy and Density Functional Theory (DFT) calculations reveal that ZnO not only promotes directional interfacial electron transfer but also facilitates the hydrogenation of *CO to *CHO, thus enhancing CH 4 selectivity. This study demonstrates an ALD-enabled interface engineering strategy to construct MOF-semiconductor heterojunctions, offering mechanistic insights and design principles for advancing efficient and selective photocatalytic systems for carbon dioxide reduction.
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FLUID PHASE EQUILIBRIA
·
2026
·
IF 2.7
Yufan Ma,Cong Liu,Hongxing Wang,Jie Li,Qingli Qian
The solubilities of CO 2 , H 2 , and CH 4 in 1-ethyl-2-pyrrolidone (NEP) were measured using the isochoric saturation method at 413.15–453.15 K under pressures of 0.45–3.89 MPa (CO 2 ), 4.42–7.64 MPa (H 2 ), and 0.59–3.49 MPa (CH 4 ). The reliability of the apparatus was verified by measuring CO 2 solubility in N-methyl-2-pyrrolidone (NMP) at 323.15–353.15 K. The solubility order in NEP was found to be CO 2 > CH 4 > H 2 . Temperature-dependent Henry’s constants were obtained, and the experimental data were correlated using the Krichevsky–Kasarnovsky equation and the generic Redlich–Kwong (RK) cubic equation of state, with the RK model providing better accuracy. These results offer essential thermodynamic data for describing gas–liquid equilibrium in NEP and support solvent selection and process design in high-temperature CO 2 conversion systems.
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JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Yong Liu,Chao Wu,Zhongming Zhou,Wei Liu,Hongyu Guo,Baoquan Zhang
The development of high-performance mixed matrix membranes (MMMs) with satisfactory structure stability has attracted much attention for the past few years. The rational design and synthesis of fillers to well coordinate themselves in the polymeric matrix is still challenging. The core-shell structured fillers were synthesized via the heteroepitaxial growth of ZIF-8 on ZIF-L(Co) surface (ZIF-L(Co)@ZIF-8), which were then embedded into Pebax to fabricate MMMs for enhanced CO 2 /CH 4 separation. The synthesized fillers and MMMs were characterized via SEM with EDS mapping, TEM, XRD , FIIR and nanoindentation measurements. The effects of ZIF-L(Co)@ZIF-8 loading and filler components on gas separation performance were studied with the evaluation of membrane stability. The experimental results indicated that the filled ZIF-L(Co)@ZIF-8 could be evenly distributed within the bulky Pebax. The synergistic effect of the core-shell structured fillers in adsorption and molecular sieving endowed the synthesized MMMs with superior gas separation performances. The optimal separation performance is achieved for the MMM containing 3 wt% of ZIF-L(Co)@ZIF-8 with a CO 2 permeability of 145.7 Barrer and a CO 2 /CH 4 selectivity of 40.9, corresponding to 79.1% and 110.1% increases over pure Pebax membrane.
研究领域:
材料科学
·
膜技术
·
气体分离
·
聚合物纳米复合材料
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金属有机框架材料（MOFs）
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Sustainable Materials and Technologies
·
2026
·
IF 9.7
Ming Liu,Tiejun Ma,Xuanxuan Sun,Tallat Munir,Shiyang Bai,Jihong Sun
Surfactant effect on the crystallization behavior of clinoptilolite is proposed. • Fractal evolution of the aluminosilicate sol is tracked via SAXS method. • Nucleation and growth behavior of clinoptilolite was clarified via DFT simulations. • Gas separation performance of the surfactant-assisted clinoptilolite was explored. The incorporation of organic additives into hydrothermal synthesis systems provides an effective strategy for regulating the crystallization and morphological evolution of HEU-type clinoptilolite (CP). Such organic additive-assisted regulation can modify platelet development, particle aggregation, interfacial characteristics, and pore accessibility, thereby influencing gas adsorption and transport behavior. Despite extensive studies on CP modification, the comparative effects of different organic additives on nucleation, growth, fractal evolution, and gas-separation behavior remain insufficiently understood. Herein, the influences of cetyltrimethylammonium bromide (CTAB), o -phenylenediamine (OPD), and polyethylene glycol (PEG) on CP crystallization were systematically investigated using X-ray diffraction (XRD), UV-Raman spectroscopy, solid-state 29 Si nuclear magnetic resonance, scanning electron microscopy, small-angle X-ray scattering (SAXS), gas adsorption measurements, and molecular simulations. In particular, SAXS patterns were employed to elucidate fractal evolution of aluminosilicate species during CP crystallization. The results revealed that organic additive-mediated interfacial interactions modified aluminosilicate evolution during the induction stage and delayed framework organization to different extents. During the growth stage, the CTAB-, OPD-, and PEG-containing systems exhibited formulation-dependent differences in crystallization retardation and anisotropic crystal growth. Gas adsorption and GCMC-MD simulations showed formulation-dependent changes in CO 2 , CH 4 , and N 2 adsorption and diffusion; notably, additive-containing samples generally exhibited lower absolute capacities, while mixed-gas breakthrough showed the strongest CO 2 /CH 4 kinetic separation for pure-CP, revealing a structure-transport trade-off rather than universal performance enhancement. These findings link additive-regulated crystallization and platelet-like morphological evolution with adsorption transport behavior, providing a mechanistic framework for tuning CP structure and CO 2 /CH 4 separation.
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ACS Catalysis
·
2026
·
IF 13.6
Li-Nan Huang,Han Zhao,Lei Jiang,Jiahao Geng,Zhiqiang Li,Yuelun Li,Kongzhai Li
The activation of CH4 and CO2 as well as the formation of carbon deposit are crucial for dry reforming of methane (DRM), and mechanistic insights into the relationship between reactant activation and carbon evolution during the DRM process are expected to provide guidance for the design of high-performance catalysts. Herein, by utilizing carefully defined Ni/CeO2 model catalysts with different CeO2 crystal planes, we elucidate at the atomic scale the roles of crystal plane in determining the reactant activation and carbon deposit formation in DRM by a joint experimental–theoretical method. The crystal planes of CeO2 determine the active sites and activation ability for CH4 and CO2 by influencing Ni–CeO2 interactions and oxygen vacancy (OV) concentrations. Both the metal and interface active sites of Ni/CeO2(111) and Ni/CeO2(110) can activate CH4 and exhibit good DRM activity. In contrast, only the metal site on Ni/CeO2(100) can activate CH4, leading to a reduced DRM activity. The relatively balanced CH4 and CO2 activation pathways for Ni/CeO2(110) and Ni/CeO2(100) catalysts ensured the stability of the catalysts, whereas Ni/CeO2(111) was rapidly deactivated due to carbon deposits. This study provides insights into the roles of metal–support interactions and OV sites on catalysts for CH4 dissociation activity, CO2 activation, and carbon deposit elimination in the DRM process, which can provide valuable guidance for the design of efficient catalysts with high activity and stability in DRM.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Yuxin Mei,Nicui Yuan,Yating Xie,Yaping Li,Baining Lin,Yonghua Zhou
NH 2 -UiO-66 is recently regarded as a potential photocatalyst for CO 2 reduction reaction due to the high CO 2 adsorption capacity, high UV–vis light absorption capacity and chemical stability. Aiming to further improve its activity, in this paper, a composite of NH 2 -UiO-66 and CeCO 3 OH (NU/CC) was fabricated via an in-situ growth method of NH 2 -UiO-66 on CeCO 3 OH. The X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and electron spin resonance (ESR) characterizations indicated that a direct Z-scheme heterojunction between CeCO 3 OH and NH 2 -UiO-66 was formed via the formation of O-Zr-CO 3 2- bond. The CO 2 adsorption measurement, UV–vis DRS spectra and photo(electro)chemical measurements indicated that the optimal composite NU/CC-1.6–90 exhibited the higher CO 2 adsorption capacity, stronger respond and wider absorption range to UV–vis light, as well as the significantly delayed recombination of photogenerated electron-hole pairs, compared with other control samples. As a result, NU/CC-1.6–90 delivered the obviously enhanced photocatalytic activity of CO 2 to both CO and CH 4 , and the rate of electron consumption reached 152.8 μmol/g h, 5-fold of that of NH 2 -UiO-66.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Yeyin Zhang,Ruting Huang,Yong Fang,Jiacheng Wang,Zijie Yuan,Xinwei Chen,Wenjie Zhu,Yuan Cai,Xianyang Shi
This study developed metal–organic frameworks (MOFs) with enhanced properties for CO 2 conversion by doping second- transition metal ions (Ti, Mn, Zn, and Cu) into Fe–MOF, which resulted in Fe-M−MOF (M = Ti, Mn, Zn, or Cu). The selection of different metal species in the metal cluster nodes of the MOFs significantly impacted the CO 2 conversion efficiency. Among the different combinations, the Fe–Cu bimetallic cluster node was identified as the most optimal node. In addition, we investigated various variables and preparation conditions for determining the optimal synthesis conditions for Fe–Cu-MOFs. We observed that a synthesis temperature, time, and pH of 130 °C, 15 h, and 3.2, respectively, yielded the best results. The 13 CO 2 isotope labeling method confirmed that the carbon source of CO and CH 4 were derived from CO 2 . Under simulated visible-light irradiation (λ ≥ 420 nm), Fe–Cu-T130 exhibited the highest photocatalytic activity, with a CH 4 generation rate of up to 444.2 μmol g −1 h −1 . This high activity was attributed to several factors. First, the presence of Fe 2+ , Fe 3+ , and Cu 2+ on the surface of Fe–Cu-T130 resulted in photogenerated electrons and holes under visible-light excitation. Fe 2+ accepted electrons to reduce CO 2 , whereas Fe 3+ and Cu 2+ oxidized H 2 O through holes. Second, the polycrystalline structure of Fe–Cu-T130 with abundant surface oxygen vacancies enhanced the chemical reactivity. Finally, the low conduction band position and narrower bandgap of Fe–Cu-T130 facilitated the excitation of electrons into the conduction band, thereby promoting the CO 2 reduction reaction. This study successfully demonstrated the enhanced photocatalytic activity of Fe–Cu-T130 for CO 2 conversion under visible light. The findings provide insight into the development of MOFs with improved properties for the sustainable and efficient utilization of CO 2 .
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jian-Feng Diao,Teng Zhang,Zhong-Ning Xu,Guo-Cong Guo
The plasma technology can effectively reduce the high temperature (≥700 °C) reaction condition of dry reforming of methane (DRM) reaction. But the inevitable carbon deposition problem seriously hinders the progress of plasma-involved DRM reaction. In order to promote the carbon elimination reaction between the adsorbed CO 2 and carbon deposition produced by CH 4 cracking, we have developed an effective atomic-level adjacent NiFe bimetallic catalyst. Compared to the Ni-based monometallic catalyst, the atomic-level adjacent NiFe bimetallic catalyst shows high activity and excellent stability in the plasma-involved DRM reaction. The conversions of CO 2 and CH 4 are 80.5% and 73.8%, respectively. Meanwhile, the catalytic performance remains well stable during the 100 h time-on-stream evaluation. The atomic-level adjacent NiFe bimetals were characterized by XRD, TEM and EXAFS et al., which are responsible for the improved activities. Most importantly, the addition of Fe can increase the surface oxygen and enhance CO 2 adsorption confirmed by XPS and CO 2 -TPD, which beneficial to improve the ability to convert carbon deposition and improve the stability of catalyst. This work provides a feasible synthetic strategy for designing the high activity and well stability catalyst for the plasma-involved DRM reaction.
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Nanomaterials
·
2023
·Vol. 13
·期 12
·1860
·
IF 5.3
Mingxuan Zhang,Jiawei Zhou,Chunlei Wan,Ming Liu,Xia Wu,Jihong Sun
Clinoptilolite (CP) was successfully synthesized via a hydrothermal route in the presence of polyethylene glycol (PEG), and it was then delaminated by washing using Zn2+containing acid. HKUST-1, as one kind of the Cu-based MOFs, showed a high CO2adsorption capacity owing to its large pore volume and specific surface area. In the present work, we selected one of the most efficient ways for preparing the HKUST-1@CP compounds via coordination between exchanged Cu2+and ligand (trimesic acid). Their structural and textural properties were characterized by XRD, SAXS, N2sorption isotherms, SEM, and TG-DSC profiles. Particularly, the effect of the additive PEG (average molecular weight of 600) on the induction (nucleation) periods and growth behaviors were detailed and investigated in the hydrothermal crystallization procedures of synthetic CPs. The corresponding activation energies of induction (En) and growth (Eg) periods during crystallization intervals were calculated. Meanwhile, the pore size of the inter-particles of HKUST-1@CP was 14.16 nm, and the BET specific area and pore volume were 55.2 m2/g and 0.20 cm3/g, respectively. Their CO2and CH4adsorption capacities and selectivity were preliminarily explored, showing 0.93 mmol/g for HKUST-1@CP at 298 K with the highest selective factor of 5.87 for CO2/CH4, and the dynamic separation performance was evaluated in column breakthrough experiments. These results suggested an efficient way of preparing zeolites and MOFs composites that is conducive to being a promising adsorbent for applications in gas separation.Keywords:clinoptilolite;HKUST-1;composites;fractal structures;delamination;adsorptive separations
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