Nature Communications
·
2024
·Vol. 15
·期 1
·1-11
·
IF 14.7
Zheng Yue,Wang Huan,Liu Yan,Liu Peiyu,Zhu Baoli,Zheng Yanning,Li Jinhua,Chistoserdova Ludmila,Ren Zhiyong Jason,Zhao Feng
The chemical transformations of methane (CH 4 ) and carbon dioxide (CO 2 ) greenhouse gases typically have high energy barriers. Here we present an approach of strategic coupling of CH 4 oxidation and CO 2 reduction in a switched microbial process governed by redox cycling of iron minerals under temperate conditions. The presence of iron minerals leads to an obvious enhancement of carbon fixation, with the minerals acting as the electron acceptor for CH 4 oxidation and the electron donor for CO 2 reduction, facilitated by changes in the mineral structure. The electron flow between the two functionally active microbial consortia is tracked through electrochemistry, and the energy metabolism in these consortia is predicted at the genetic level. This study offers a promising strategy for the removal of CH 4 and CO 2 in the natural environment and proposes an engineering technique for the utilization of major greenhouse gases.
研究领域:
环境科学
·
微生物学
·
化学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2024
·
IF 4.8
Kunpeng Liu,Yixuan Yu,Qi Wang,Lingtong Kong,Tianjun Sun
A comprehensive investigation was conducted to explore the adsorption behaviors of CH 4 over N 2 on ultra-microporous Al/Zr-FDCA frameworks, which were synthesized specifically using the eco-friendly and bio-sourced 2,5-furandicarboxylic acid (FDCA). Characterization results revealed that both Al-FDCA and Zr-FDCA exhibited similar specific surface area and surface groups, leading to comparable methane uptake per-unit mass at atmospheric pressure. However, the presence of Zr nodes generated ultra-micropores around 0.43 nm in size, leading to a pronounced affinity for CH 4 . Zr-FDCA demonstrated a higher CH 4 /N 2 selectivity (8.90) calculated from the isotherms compared to Al-FDCA (3.86). Furthermore, breakthrough experiments indicated that under the same dynamic conditions, Zr-FDCA exhibited 1.5 times higher CH 4 uptake per unit volume and 2.5 times higher CH 4 /N 2 selectivity when compared to Al-FDCA. Initially, a four-step VPSA process was simulated to investigate the separation of CH 4 /N 2 mixture, in which the effects of feed-gas flow rate, adsorption time, adsorption pressure, and desorption pressure in VPSA cycle were extensively evaluated to enhance the purity and recovery of methane. Subsequently, a six-step process was employed for further optimization, achieving a purity of 95.9 % and a recovery of 99.1 %. The obtained results demonstrated the reliability of the established model and highlighted the significant potential of Zr-FDCA for CH 4 /N 2 separation.
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
SEPARATION SCIENCE AND TECHNOLOGY
·
2016
·
IF 1.083
Yaqiong Zhu,Qian Liu,Aisheng Huang
The separation of CO2/CH4 is reported in detail by using zeolitic imidazolate framework (ZIF-8) membrane which was prepared on 3-aminopropyltriethoxysilane modified Al2O3 tube through microwave heating synthesis. Attributed to the preferential adsorption affinity of CO2 over CH4 and a narrow pore window of 0.34 nm, the ZIF-8 membrane shows high separation performances for the separation of CO2/CH4 mixtures. For the separation of equimolar CO2/CH4 mixture at 100°C and 2 bar feed (1 bar permeate) pressure, a CO2 permeance of 1.02 × 10−8 mol/m2· s· Pa and a CO2/CH4 selectivity of 6.8 are obtained, which is promising for CO2 separation.
研究领域:
材料科学
·
环境工程
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2023
·
IF 7.4
Hongxia Fang,Chuncai Zhou,Shihai Xu,Jiaqian Shi,Yunhu Hu,Guijian Liu,Lei Wu
Metal-organic frameworks (MOFs) are considered one of the promising adsorbents for CH 4 /N 2 separation. However, MOFs commercialization is a big challenge since their synthetic materials are expensive and not environmentally friendly. Herein, the dealumination solution obtained from coal fly ash (CFA) using sulfuric acid as an extracting agent through direct leaching and roasting technologies was applied as metal feedstock to prepare CFAx-FumMOF-y and compared to aluminum fumarate MOF (Al-FumMOF) in morphology, surface area, micropore volume, and CH 4 /N 2 selective separation. The results indicated that CFAx-FumMOF-y exhibited closely similar surface area (1164.94–1073.08 m 2 /g) and micropore volume (0.40–0.36 cm 3 /g) to Al-FumMOF (1287.55 m 2 /g, 0.42 cm 3 /g), even there were no detectable differences in CH 4 uptakes (CFAx-FumMOF-y, 21.93–20.69 cm 3 /g; Al-FumMOF, 22.13 cm 3 /g) at 298 K and 1.0 bar, suggesting that the impurity metal species in dealumination solution hardly affect textural properties and gas uptakes. Moreover, the isosteric heat of adsorption (Q st ) and IAST CH 4 /N 2 selectivity of CFAs-FumMOF-1 (19.25–17.84 kJ/mol) and CFAb-FumMOF-1 (18.83–18.64 kJ/mol) were slightly superior to Al-FumMOF (17.83.64–16.86 kJ/mol, 4.87), suggesting that CFAx-FumMOF-1 played an identical role as Al-FumMOF in gases separation. The cyclic regeneration experiments and binary breakthrough tests further confirmed that CFAx-FumMOF-y was feasible for practical application. This study provides a new perspective for reducing the production cost of MOFs as well as realizing high-value utilization of CFA.
研究领域:
材料科学
·
环境科学
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Tongxin Liu,Ruili Zhang,Guang-Rui Si,Bin Liu,Yabo Xie,Lin-Hua Xie,Jian-Rong Li
The rational design of mixed matrix membranes (MMMs) combining appropriate additives and industrial processable polymers offers a new prospect for highly efficient membrane separations. However, the difficulty in their fabrication due to the lack of processability of most additives and the formation of segregated filler domains in polymer matrices hampers the development and application of MMMs. Herein, we present two new zirconocene-based metallocavitands (ZRA and ZRT) and a series of MMMs fabricated by blending ZRA, ZRT, and MOC-1-NH2 (a zirconocene-based metal–organic cage) with the polyimide (6FDA-DAM), respectively. It was found that ZRA exhibited high thermal stability and good solubility in various solvents, which can be homogeneously mixed with polymers to prepare ZRA-based MMMs without any indication of filler agglomeration. Compared to the pure 6FDA-DAM membrane, a low ZRA-loading MMM (ZRA-2.2%) exhibited better mechanical properties and 50% improved CO2 permeability for CO2/CH4 separation. ZRA-2.2% also exhibited a good performance after 6 months of aging and significantly alleviated the plasticization effect under high pressures. These results suggest the great potential of the ZRA-2.2% for CO2/CH4 separation and that the simple metallocavitands may serve as promising additives in fabricating MMMs for gas separations.
研究领域:
材料科学
·
化学工程
·
气体分离技术
✓ 已验证
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2018
·
IF 6.578
Ke Chen,Kai Xu,Long Xiang,Xiao Dong,Yue Han,Chongqing Wang,Lin-Bing Sun,Yichang Pan
Mixed matrix membranes (MMMs) derived from metal-organic frameworks (MOFs) nanocrystals represent a promising alternative for overcoming the trade-off between permeability and selectivity derived from the pristine polymeric membrane . The selection of MOFs fillers are mainly focused on their diffusion-selectivity property for gas-pairs. However, the improvement of both gas-permeability and selectivity through addition of sorption-selective MOFs are rarely reported. Herein, the incorporation of CO 2 -philic KAUST-7 (also referred to as NbOFFIVE-1-Ni) nanocrystals makes the neat 6FDA-Durene polyimide membrane more permeable and more selective, surpassing the state-of-the-art 2008 Robeson upper bound for CO 2 /CH 4 . Nano-sized (~ 80 nm) KAUST-7 crystals with sharp particle size distribution were first fabricated through a co-solvent synthesis method. The explored gas transportation mechanism indicates that the improvement of CO 2 /CH 4 selectivity on MMMs are attributed to the significant raise of the sorption-selectivity rather than the diffusion-selectivity. The favorable interfacial interaction between the imide groups of the 6FDA and the H of the pyrazine in the KAUST-7 enhances plasticization resistance of the neat polymer membrane. The developed MMMs exhibit a promising application in CO 2 capture from natural- and bio-gas.
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 27
·70884-70896
·
IF 5.8
Li Ke,Zhu Yuqiu,Wang Zixuan,Chen Dingkai,Wu Wenwei,Luo Yongming,He Dedong
High concentration of H 2 S in acidic natural gas will lead to poisoning of catalysts for hydrogen production by methane steam reforming, thus limiting the further use of natural gas. Reforming CH 4 by H 2 S can be considered as an alternative route to hydrogen production from methane. This process not only achieves the removal of H 2 S but also obtains chemical raw material CS 2 and clean energy H 2 . By impregnating the Mo source on SiO 2 treated with hydrogen peroxide and then using the catalyst in the CH 4 /H 2 S reforming reaction, we surprisingly found that the conversion rate of CH 4 and H 2 S increased from 28 and 32% to 34% and 43%, respectively, after hydrogen peroxide treatment. The H 2 production rate and the yield of CS 2 increased from 20 mmolH 2 /(g Mo *min) and 52% to 30 mmolH 2 /(g Mo *min) and 65%, respectively. Combining with characterization methods such as X-ray diffraction (XRD), hydrogen temperature programmed reduction (H 2 -TPR), 1 H-based solid-state nuclear magnetic resonance ( 1 H MAS NMR), X-ray photoelectron spectroscopy (XPS), Raman spectra (RS), and transmission electron microscopy (TEM), we found that the hydroxyl concentration of the support increased after hydrogen peroxide treatment, which led to the strengthening of the force between the metal and the support, which was easy to form low-level and small-size MoS 2 , exposing more active sites, and further improving the catalytic activity. This method provides a new idea for hydrogen production by CH 4 /H 2 S reforming and the development of high-performance MoS 2 -based catalysts.
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2024
·
IF 4.7
Yating Xie,Nicui Yuan,Hongyang Liu,Lukai Luo,Jun Gong,Xiping Yin,Tengfei Li,Yonghua Zhou
Defect engineering by creating oxygen vacancies (OVs) and heterogeneous frustrated Lewis acid-base pairs (FLPs) emerged as an efficient strategy to enhance the selective conversion CO 2 to CH 4 . Considering the intrinsic FLPs contained in UiO-66-NH 2 (UNH for abbreviation), in this paper, the OVs was introduced therein by fabricating the Ce-doped UNH (denoted as UNH(Ce/Zr)) via one-step solvothermal route. The as-prepared UNH(Ce/Zr) catalyst exhibited the CH 4 yield of 31.02 μmol·g −1 ·h −1 accompanied with the CH 4 selectivity of 93 % and satisfying recycling stability. The XRD, SEM, FT-IR, XPS, TG, TPD and NH 3 in situ DRIFTS and in situ FT-IR characterization results justified that the UNH(Ce/Zr) possess the obviously increased OVs sites and enhanced Lewis acidic and basic properties. Additionally, the photoelectrochemical characterization results showed that UNH(Ce/Zr)−0.014 efficiently improved photogenerated electron-hole separation efficiency and charge transfer rate. It could be concluded that it was the cooperative action of OVs and FLPs that led to the high CH 4 selectivity and CH 4 yield.
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
MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Xiaoli Ding,Yongfu Tang,Hongyong Zhao,Qingping Xin,Yuzhong Zhang
Hollow SAPO-34 with an average particle size of ca .370 nm was synthesized by selective etching its precursor under the controlled alkaline condition. Subsequently, freestanding mixed matrix membranes were synthesized by UV-induced in-situ polymerization of the mixture of hollow SAPO-34, the fluorinated monomer , and the trifunctional cross-linker. The structure and the physical characteristic of hollow SAPO-34 and membranes were characterized by scan electron microscope, wide-angle X-ray diffraction, etc. The effect of the hollow SAPO-34 loading amount on the gas permeation-separation performance of mixed matrix membranes was investigated. The results showed that hollowing out SAPO-34 improved the N 2 /CH 4 sorption selectivity and converted the crystals from preferential adsorption of N 2 to preferential adsorption of CH 4 , the incorporation of hollow SAPO-34 into membranes increased the N 2 /CH 4 solubility selectivity and the permeability. The optimal membrane exhibited a 39-fold increase in N 2 permeability from 6.9 × 10 −13 to 2.7 × 10 −11 cm 3 (STP)cm·cm −2 ·s −1 ·Pa −1 at 0.2 MPa and 35 °C without the loss of N 2 /CH 4 permselectivity, which exceeded the 2008 Robeson upper bound.
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
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Ziyi Li,Jia Xiong,Yufei Huang,Yangqiang Huang,Geoffrey I.N. Waterhouse,Ziyun Wang,Yu Mao,Zhiwu Liang,Xiao Luo
Photocatalytic CO 2 reduction reaction (CO 2 RR) is usually constrained by sluggish kinetics and low product selectivity. Herein, a Cu-doping multi-tier hierarchical S-scheme heterostructure Cu-ZnIn 2 S 4 /ZIF-67 was fabricated, achieving highly efficient photocatalytic CO 2 RR under visible light without additional thermal input. At low pressure (absolute pressure 40 kPa), the optimized catalyst 2Cu-ZISF demonstrated a CH 4 yield of 22.27 μmol g −1 h −1 with a selectivity of 94.7 %. In situ XPS and EPR confirmed that the photogenerated charge transfer obeys an S-scheme mechanism, with Cu sites serving as electron-rich centers, facilitating spatial charge separation. In situ DRIFT detected reaction intermediates of photocatalytic CO 2 RR mechanism, and Gibbs free energy calculations via Density Functional Theory revealed that Cu incorporation significantly stabilizes surface CO* species, thus reducing CO(g) production and facilitating hydrogenation, thereby acting as targeted active sites for CH 4 production. This work overcomes the limitations of slow reaction kinetics and offers an in-depth understanding of how to design effective S-scheme heterojunction photocatalysts and their charge transfer mechanisms.
研究领域:
材料科学
·
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2022
·
IF 8.047
Wenhao Li,De-Kun Ma,Xia Hu,Faliang Gou,Xiaogang Yang,Walker MacSwain,ChenZe Qi,Weiwei Zheng
Rationally designing and controlling the interactions between reaction intermediates and the surface of photocatalysts is critical to obtain high product selectivity in photocatalysis. Herein, using CdS-based photocatalytic CO 2 reduction reaction (CO 2 RR) as a model system, we demonstrate that CH 4 selectivity can be significantly enhanced through the introduction of La 3+ ions with high oxophilicity on the surface of the photocatalysts. The high surface oxophilicity of the photocatalysts can increase CO* desorption energy and promote further hydrogenation to CH 4 . In contrast, when Au 3+ ions with low oxophilicity were doped in CdS, reduced CH 4 selectivity was observed in the CO 2 RR. Significantly, enhanced CH 4 selectivity can be achieved by doping oxophilic La 3+ ions into a broad range of alternative photocatalysts including ZnO, SnS 2 , BiOBr, BiVO 4 , TaON, and CsPbBr 3 , which demonstrates the general strategy to enhance CH 4 selectivity of photocatalytic CO 2 RR through increased surface oxophilicity of the photocatalysts by rare earth La 3+ ion doping.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Ke Chen,Linhan Ni,Hao Zhang,Jia Xie,Xin Yan,Saisai Chen,Junwen Qi,Chaohai Wang,Xiuyun Sun,Jiansheng Li
The interfacial compatibility between fillers and polymers essentially influences the separation performance of mixed matrix membranes (MMMs). In this work, an one-pot synthesized functional layer veiled zeolite imidazolate frameworks-67 (VZIF-67) was used as an efficient nanofillers to fabricate MMMs via physical blending with 6FDA-Durene polyimide. Benefiting from the CO 2 affinity from functional layer and the intrinsic characteristics of porous nanofillers, significant enhancement on separation performance was observed on the resultant MMMs. Specifically, the optimized VZIF-67 MMMs (30 wt% loading) exhibited CO 2 /CH 4 selectivity of 32.5 with CO 2 permeability of 1210 Barrer, which is 1.7 and 1.5 times higher than those of the control membrane, respectively. More importantly, the surface organic attribute and abundant amine groups of VZIF-67 reinforced the interfacial compatibility between the nanofillers and polymer matrix, leading to a doubled CO 2 /CH 4 selectivity compared with the ZIF-67 MMMs. Overall, the performance of the VZIF-67 membrane toward CO 2 /CH 4 separation surpasses the 2008-updated Robeson upper bound. These results indicate the functionalization strategy on porous nanofillers is a promising approach to fabrication of high performance of MMMs.
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
危险品化学品经营许可证（带存储）