Science Advances
·
2023
·Vol. 9
·期 24
·
IF 13.6
Meng Zhao,Dong-Dong Zhou,Pin Chen,Yujie Ban,Yuecheng Wang,Ziyi Hu,Yutong Lu,Mu-Yang Zhou,Xiao-Ming Chen,Weishen Yang
Hydrogen/carbon dioxide (H 2 /CO 2 ) separation for sustainable energy is in desperate need of reliable membranes at high temperatures. Molecular sieve membranes take their nanopores to differentiate sizes between H 2 and CO 2 but have compromised at a marked loss of selectivity at high temperatures owing to diffusion activation of CO 2 . We used molecule gatekeepers that were locked in the cavities of the metal-organic framework membrane to meet this challenge. Ab initio calculations and in situ characterizations demonstrate that the molecule gatekeepers make a notable move at high temperatures to dynamically reshape the sieving apertures as being extremely tight for CO 2 and restitute with cool conditions. The H 2 /CO 2 selectivity was improved by an order of magnitude at 513 kelvin (K) relative to that at the ambient temperature.
研究领域:
膜科学
·
材料科学
·
能源可持续性
·
气体分离
·
计算化学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Mengqi Xiao,Jibao Zhang,Yang Li,Yan Li,Xuejian Liu,Xiaolin Wang,Zhenyuan Yin
Hydrate-based H 2 storage has emerged as a promising solution for offshore wind-to-hydrogen applications. Seawater is widely accessible on offshore platforms and can be directly used as a hydrate former. However, effects of salt in seawater on the kinetics of hydrogen hydrate are less understood and warrants investigation. This study systematically examines the influence of NaCl on the H 2 hydrates formation in the presence of a thermodynamic promoter, 1,3-dioxolane (DIOX). Effects of NaCl on the thermodynamics, kinetics, and morphology of H 2 -DIOX hydrates were investigated. The thermodynamic inhibition on DIOX hydrates is more pronounced than that on H 2 -DIOX hydrates in simulated seawater, resulting in a slurry-like hydrate morphology that improves gas-liquid contact. H 2 final gas uptake achieved in simulated seawater is seven-fold that of pure water with H 2 only occupying 5 12 cages of sII hydrate. Our study provides insights into the direct use of seawater for offshore hydrate-based H 2 storage.
研究领域:
储能技术
·
化学工程
·
海洋技术
·
氢能
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Lan Yang,Yuanzhi Hong,Enli Liu,Xue Zhang,Longyan Wang,Xue Lin,Junyou Shi
The photocatalytic H 2 production simultaneous with organic pollutant degradation has been received wide attention in resolving the problems of energy crisis and environmental pollution. In this study, for the first time, the Ni 2 P (NIP) nanoparticles are successfully loaded on the surface of In 2 O 3 (INO) nanocubes, and the physical-chemical features of as-formed NIP/INO samples are comprehensively characterized by various technologies. Moreover, the photoreactivities of as-prepared NIP/INO nanocomposites are carefully investigated through the photocatalytic H 2 evolution simultaneous with dye (Rhodamine B, RhB) degradation under simulated sunlight irradiation. It was found that the as-fabricated NIP/INO nanocomposites present the significantly enhanced H 2 production and RhB degradation rates than that of pure INO nanocubes. Consequently, the optimum photocatalytic performance of as-synthesized photocatalyst is loaded by 7 wt% NIP (7-NIP/INO), whose the H 2 evolution and RhB degradation rates are reached at 0.138 μmol h −1 and 16.12%, respectively, which are 10.6-folds and 1.6-folds higher than that of individual INO, even its photoactivity is superior than the 1 wt% Pt decorated INO. The greatly improved photocatalytic performance is due to the NIP as co-catalyst can not only promote the charge carries separation and transfer efficiency, but also provide the abundant reaction active sites. Our work highlights a simple strategy for the preparation of non-noble metal nanocomposites towards the renewable solar-driven photocatalysis applications by combining with earth-abundant Ni-based co-catalyst.
研究领域:
材料科学
·
环境科学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Mide Luo,Yali Zhao,Yanying Wei,Haihui Wang
Construction of large-area two-dimensional (2D) nanosheet membranes for gas separation, particularly tubular membranes, is extremely challenging. Here, electrophoretic deposition technology was employed to construct large-area tubular 2D MXene membranes for H 2 /CO 2 gas separation, where the membrane with a single tube area of 25 cm 2 could be successfully manufactured in approximately 5 min under optimal process conditions. The membrane exhibited good H 2 /CO 2 separation performance with H 2 /CO 2 selectivity of 53.0 and hydrogen permeance of 133.8 GPU, exceeding the 2008 Robeson upper bound, and showed excellent stability in long-term test with water vapor evaluations for more than 350 h. Additionally, some engineering issues and operation parameters concerning the separation performance of H 2 /CO 2 in single-module and dual-module separators have been thoroughly investigated and analyzed. This work has taken an important step toward the industrialization of 2D MXene membranes and also provided significant guidance to other 2D material-based membranes in approaching practical applications.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 67
·54769-54776
·
IF 3.84
Chunxiao Lu,Yang Chen,Yun Li,Chunhong Ma,Hongbo Zhang,Yuwei Guo,Jun Wang
A highly effective and stable up-conversion luminescence agent, Er3+:Y3Al5O12, was synthesized by sol–gel and calcination methods. Then, as a novel visible-light photocatalyst, Er3+:Y3Al5O12, Pt and PdS (as dual co-catalysts) decorated ZnS nano-sized composites, Er3+:Y3Al5O12/Pt–PdS/ZnS, were fabricated by deposition–precipitation and ultrasonic dispersion methods. All prepared samples were characterized by X-ray diffractometry (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS) and energy dispersive X-ray spectroscopy (EDX). UV-vis absorption and PL spectra of Er3+:Y3Al5O12 were also determined. The visible-light photocatalytic H2 production activity of the prepared Er3+:Y3Al5O12/Pt–PdS/ZnS was evaluated by using Na2S and Na2SO3 as sacrificial reagents in an aqueous solution under 300 W irradiation from a xenon lamp. In addition, some influential factors such as Er3+:Y3Al5O12 and ZnS mass ratio, catalyst amount, irradiation time and irradiation intensity on visible-light photocatalytic H2 production of Er3+:Y3Al5O12/Pt–PdS/ZnS were investigated in detail. It was found that Er3+:Y3Al5O12 can effectively improve the visible-light photocatalytic activity of ZnS. Particularly, Er3+:Y3Al5O12/Pt–PdS/ZnS with 0.13 wt% PdS and 0.3 wt% Pt and a 0.30 : 1.00 mass ratio shows the highest photocatalytic H2 production activity in the sulfide/sulfite (0.2 mol L−1 Na2S and 0.3 mol L−1 Na2SO3) aqueous solution as sacrificial reagents.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Jiayi Liu,Yaohui Zhang,Yujie Ban,Weishen Yang
Emissions from the petrochemical industry often contain by-product hydrogen alongside various hydrocarbons, leading to both resource wastage and increased air pollution. The separation of H 2 from these hydrocarbons is thus of considerable economic and environmental importance. Conventional polymer membranes face inherent trade-offs between gas permeability and selectivity. To overcome this limitation, this study introduces a strategy to assemble metal–organic framework (MOF) nanoparticles into a sponge-like architecture on the surface of an ultrathin rubbery polysiloxane membrane, achieved by synergistically harnessing spin-coating-induced centrifugal forces and polymer–MOF chemical pinning forces. The resulting intricate sponge-like structure greatly promotes repeated adsorption–desorption cycles for the more condensable hydrocarbons, thereby markedly slowing their permeation through the membrane. The composite membrane achieves H 2 /CH 4 , H 2 /C 2 H 6 , and H 2 /C 3 H 8 separation factors of 136, 1370, and 1610, respectively, while maintaining H 2 permeances of 439 to 473 GPU. The membrane's effectiveness is further demonstrated for hydrogen separation from a simulated hydrocarbon-rich industrial tail gas: H 2 is enriched from 10% to 83% in the permeate. In doing so, the membrane not only efficiently recovers hydrogen but also reduce the combined emissions of six representative C 1 –C 4 hydrocarbons by 78%. This sponge-like MOF-polymer composite introduces a new paradigm for advanced H 2 /hydrocarbon separation membranes.
研究领域:
材料科学
·
膜技术
·
气体分离
·
石油化工工程
·
纳米材料
·
环境工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2018
·
IF 3.306
Qing Li,Xiaofang Zhu,Ying Zhang,Zhigang Zak Fang,Shili Zheng,Pei Sun,Yang Xia,Ping Li,Yang Zhang,Xing Zou
Hydrogen assisted magnesiothermic reduction (HAMR) of TiO 2 is a promising new process developed recently to produce Ti metal with low cost and less energy consumption. This work focuses on the understanding and optimization of the reduction process to control the quality of the reduced product. TiO 2 precursor particles with different relative densities were prepared, and the effects of the relative densities on reduction by Mg in H 2 were studied. The changes of oxygen contents vs. reduction time at various temperatures were investigated. The phase transformations during the reduction were analyzed both theoretically and experimentally. The relationship between the morphology of the reduced products and the relative densities of the TiO 2 precursors was analyzed by SEM characterization and the likely reason for the morphology evolution was discussed.
研究领域:
材料科学
·
冶金工程
✓ 已验证
产品关联
DOI
高影响因子
RENEWABLE ENERGY
·
2022
·
IF 8.634
Zhuoheng Tu,Ping Zhang,Mingzhen Shi,Xiaomin Zhang,Youting Wu,Xingbang Hu
Efficient recovery of CO and H 2 from offgas streams is environmentally and economically meaningful from the view point of the wide use of syngas (CO/H 2 ) in the chemical industry. This work reports selective and simultaneous separation of CO and H 2 from N 2 using protic chlorocuprate ionic liquids (PCILs)-based membranes. The chemical structures of the prepared PCILs were characterized using FTIR , NMR and ESI-MS, and the thermal stability, melting points, viscosity and density of PCILs were determined. The morphology and elemental distribution of PCIL-based membranes were characterized by SEM and EDS. Facilitated transport of CO is observed in these membranes, and the CO permeability is up to 178.3 barrers (0.1 bar, 40 °C) in [TEAH][CuCl 2 ], with a CO/N 2 selectivity of 26.2. H 2 permeability and H 2 /N 2 selectivity are also found to reach 198.2 barrers (0.5 bar, 40 °C) and 29.1, respectively. The permeability of CO and the selectivity of CO/N 2 can be further optimized to 405.9 barrers and 69.9 by altering the Cu(I) content, respectively. In addition, the selectivity of CO/H 2 can be tuned drastically via varying the Cu(I) content (from 0.77 to 12.0) and the operating temperature (from 2.14 to 0.42), which may be applied to the composition adjustment of syngas. In a word, this work offers a new strategy for designing IL-based membranes that used for CO and H 2 capture.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2018
·
IF 3.306
Jiamin Hou,Yanying Wei,Sheng Zhou,Yanjie Wang,Haihui Wang
We propose a strategy for rapid in situ fabrication of zeolitic imidazolate framework-8 (ZIF-8) hybrid membrane with assistance of the two dimensional (2D) graphitic carbon nitride (g-C 3 N 4 ) nanosheets at room temperature. The negatively charged g-C 3 N 4 nanosheets with abundant nitrogen coordinating sites are capable to capture and anchor Zn 2+ and thus provide a large number of heterogeneous nucleation sites for the formation of initial ZIF-8 crystals. During the cyclical spin coating of the Zn 2+ /g-C 3 N 4 nanosheets and the ligand (2-methylimidazole), the in situ formed ZIF-8 crystal nucleus on g-C 3 N 4 nanosheets promote the further growth of continues defect-free membranes. The ZIF-8/g-C 3 N 4 membrane with thickness of ∼240 nm can be obtained using this strategy within 30 min at room temperature, which is attractive for fast and facile preparation of molecular sieving membranes. Moreover, it exhibits promising H 2 /CO 2 separation performance with the selectivity up to 42, which is superior to many other ZIF-8 membranes.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
APPLIED ENERGY
·
2024
·
IF 10.1
Jiecheng Zou,Lanxun Zhao,Qiang Hu,Dingding Yao,Haiping Yang
The gasification technology has shown great potential to upcycle plastic waste for clean and high-value fuel. Gasification of disposable plastic masks was investigated in a two-stage pyrolysis-catalytic reforming system, aiming at producing the syngas with flexible H 2 to CO ratio which can be tuned for various downstream applications without further purification and adjustment. To maximize the syngas yield and minimize the carbon deposition, different gasifying agents in the staged catalytic process was explored. The results showed that CO 2 significantly promoted syngas production mainly by increasing CO yield. However, H 2 -rich syngas was obtained via using steam as the gasifying agent. Competitive and synergistic relationships between CO 2 and H 2 O agent at co-feeding process were further revealed. CO 2 facilitated the reforming of H 2 O at low dose of steam while exhibiting a main competition with adequate steam except for synergy at 5 mL/min CO 2 flow rate. An optimum H 2 -rich syngas yield of 135.59 mmol/g plastic with H 2 /CO ratio of 2 was obtained at co-feeding reactants. Therefore, the co-feeding of H 2 O and CO 2 could show positive effect for both coke removal and syngas quality regulation. Results found in this work increased the overall operational flexibility and economy of pyrolysis and catalytic reforming of plastic waste.
研究领域:
能源与环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Journal of CO2 Utilization
·
2024
·
IF 7.2
Heming Deng,Haoshuang Gu
Two-dimensional membranes are considered the next generation separation membrane with great application potential due to their excellent separation performance, good mechanical strength and thermal stability compared with traditional membrane materials. In this work, the flexible NH 2 -UIO-66@MXene membrane was successfully prepared for gas separation by loading NH 2 -UIO-66 particles onto Ti 3 C 2 nanosheets based on an in-situ growth strategy. A LiF-HCl mixed solution was used as the etchant to obtain the Ti 3 C 2 nanosheets. The loading of NH 2 -UIO-66 particles can regulate the interlayer spacing of Ti 3 C 2 nanosheets, improving the specific surface area of Ti 3 C 2 and the adsorption capacity for specific gases. The -NH 2 group in NH 2 -UIO-66 enabled preferential adsorption of CO 2 over H 2 , and the CO 2 molecules adsorbed in the channel can even block the molecules passing through, increasing the resistance of CO 2 diffusion. As a result, the NH 2 -UIO-66@Ti 3 C 2 hybrid membrane realizes the selective separation of H 2 /CO 2 mixed gas, and the separation selectivity is as high as 155. The gas separation selectivity and permeation of the final prepared NH 2 -UIO-66@MXene were enhanced and exceeded the upper limit of Robeson upper bound (2017).
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
ChemCatChem
·
2020
·Vol. 12
·期 21
·5504-5510
·
IF 4.853
Zi-Cheng Fu,Joshua T. Moore,Zi-Xin Yang,Jia-Jun Hu,Wen-Fu Fu
Graphical CoP for photocatalysis : Sphericalmesoporous SBA-15-supported CoP nanoparticlecatalysts tuning the highly efficient photocatalytic CO-and H 2 -generating pathways with product selectivity of up to 76.3 %and 99.9 % through switching solvent, respectively, were in situ fabricated by CoP embedded on the surface and interior of the porous s-SBA-15. The highly active spherical hybrid catalysts with diameters of 3–8 μm for robust selective CO 2 photoreduction and hydrogen production by switching solvent, CoP/(i)s-SBA-15 and CoP/(o)s-SBA-15, were in situ synthesized for the first time by incorporating CoP nanoparticles on the interior and outside of the spherical mesoporous Santa Barbara Amorphous (s-SBA)-type material s-SBA-15. CoP/(i)s-SBA-15 has a larger pore diameter of ∼9.5 nm, relative to ∼5.7 nm of CoP/(o)s-SBA-15, and a calculated Brunauer-Emmett-Teller surface area of ∼214 m 2 g −1 compared with ∼336 m 2 g −1 for the latter. In comparison with bare CoP, the composites exhibited excellent catalytic CO- and H 2 -generating performance with product selectivity of up to 76.3 % and 99.9 % through switching solvents containing Ru-based photosensitizer under ambient conditions, respectively. The influences of various solvents and electron donors, as well as the amounts of H 2 O, and catalyst on reaction kinetics for CO 2 reduction and H 2 production, and intrinsic properties of both catalysts were investigated and compared.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）