Journal of CO2 Utilization
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2022
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IF 8.321
Nicui Yuan,Yuxin Mei,Yuwei Liu,Yating Xie,Baining Lin,Yonghua Zhou
The development of efficient and highly selective photocatalysts is a key point for the photocatalytic conversion of CO 2 . In this paper, a composite catalyst UiO-66-NH 2 /Ce(HCOO) 3 (simplified to UNH/Ce(HCOO) 3 ) was fabricated by one pot method with CeCO 3 OH as the precursor. Scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS) characterizations results confirmed that UNH was dispersed on the surface of Ce(HCOO) 3 and strongly interacted with it via Ce-N bond. The yield of CH 4 on the optimal UNH/Ce(HCOO) 3 catalyst reached 3 times of that on pristine UNH, up to 128.81 μmol g −1 , with the CH 4 selectivity of 71.9 %, and the R electron reached 286.46 μmol g −1 h −1 . The UV–vis diffuse reflection spectra and photoelectrochemical tests results confirmed that the improved photocatalytic CO 2 reduction performance and high CH 4 selectivity could be attributed to the formation of the type-Ⅱheterojunction of UNH/Ce(HCOO) 3 with abundant Ce 3+ , which expanded the visible light absorption range, accelerated the separation and transfer rates of photogenerated charges, and thus efficiently promoted the multi-electron reduction reaction of CO 2 to CH 4 . In addition, the reaction temperature affected profoundly the cycle performance of the catalyst. The results presented here illustrated the possibility for improving the stability of UNH/Ce(HCOO) 3 -1.80 by decreasing reaction temperature.
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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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Zhi-Wen Wang,Qiang Wan,Ying-Zhang Shi,Huan Wang,Yue-Yue Kang,Shu-Ying Zhu,Sen Lin,Ling Wu
Ultrathin TiO 2 nanosheet (NST) with abundant Ti 3+ sites is developed as a photocatalyst which exhibits a high yield (147.2 μmol g −1 h −1 ) and selectivity (96.8%) for CO 2 to CH 4 . The results of in situ FTIR, in situ EPR and density functional theory (DFT) calculation suggest that CO 2 would be selectively activated on NST surface via forming the bridging Ti···CO 2 − ···Ti coordination species which not only lowers the activation energy barrier, but also determines the selectivity of CH 4 . Additionally, NST with the better separation and transfer ability for photogenerated electrons-holes can fleetly supply the electrons to CO 2 molecules for high efficiently producing CH 4 via the Ti-C coordination bond. Finally, a possible mechanism of the synergistic effect about coordination-activation and photocatalysis is discussed at a molecule level. This work would offer a perspective for designing an effective photocatalyst and tailoring the selectivity of products by coordination activation.
研究领域:
材料科学
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环境科学
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化学
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高影响因子
Membranes
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2021
·Vol. 11
·期 2
·118
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IF 4.106
Chunwei Zhang,Menglong Sheng,Yaoqiang Hu,Ye Yuan,Yulong Kang,Xiao Sun,Tao Wang,Qinghua Li,Xisen Zhao,Zhi Wang
CO2enhanced oil recovery (CO2-EOR) technology is a competitive strategy to improve oil field economic returns and reduce greenhouse gas emissions. However, the arbitrary emissions or combustion of the associated gas, which mainly consists of CO2and CH4, will cause the aggravation of the greenhouse effect and a huge waste of resources. In this paper, the high-performance facilitated transport multilayer composite membrane for CO2/CH4separation was prepared by individually adjusting the membrane structure of each layer. The effect of test conditions on the CO2/CH4separation performance was systematically investigated. The membrane exhibits high CO2permeance of 3.451 × 10−7mol·m−2·s−1·Pa−1and CO2/CH4selectivity of 62 at 298 K and 0.15 MPa feed gas pressure. The cost analysis was investigated by simulating the two-stage system. When the recovery rate and purity of CH4are 98%, the minimum specific cost of separating CO2/CH4(45/55 vol%) can be reduced to 0.046$·Nm−3CH4. The excellent short-to-mid-term stability indicates the great potential of large industrial application in the CH4recovery and CO2reinjection from oilfield associated gas.Keywords:oilfield associated gas;CO2capture;multilayer composite membrane;facilitated transport;CO2/CH4separation
研究领域:
化学工程
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环境科学
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DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
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2018
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IF 8.097
Dongxing Tan,Jianling Zhang,Jinbiao Shi,Shaopeng Li,Bingxing Zhang,Xiuniang Tan,Fanyu Zhang,Lifei Liu,Dan Shao,Buxing Han
To develop photocatalysts with desirable compositions and structures for improving the efficiency and selectivity of CO2 conversion to CH4 under mild conditions is of great importance. Here, we design an effective photocatalyst of bimetal (Ag/Pd) nanoalloys supported on nitrogen-doped TiO2 nanosheet for CO2 conversion. Such a novel photocatalyst combines multiple advantages of abundant Ti3+ ions, oxygen vacancies, and substitutional nitrogen that are favorable for catalyzing CO2 reduction. It was found that CO2 could be efficiently transformed to CH4 under mild conditions, i.e., in aqueous solution and at atmospheric pressure and room temperature. The maximum production rate of CH4 can reach 79.0 μmol g–1 h–1. Moreover, the Ag/Pd bimetals supported on N-doped TiO2 nanosheet exhibit high selectivity to CH4. The as-synthesized photocatalyst can be well recycled for CO2 reduction.
研究领域:
材料科学
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环境科学
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DOI
PubMed
高影响因子
AICHE JOURNAL
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2025
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IF 4
Xinrui Liu,De Ao,Mao Ye,Zhi Wang,Zhihua Qiao,Song Zhao
Metal–organic framework (MOF) glass holds great promise for gas separation applications. However, the inherent low porosity of MOF glass poses a considerable challenge in improving membrane permeability. In this work, a self-supporting MOF crystal-glass composite (CGC) membrane was synthesized via an innovative blending and melting approach, in which ZIF-62 powder was converted into an amorphous glassy phase and ZIF-9 powder was partially flux-melted, effectively preventing the reorganization of Zn─N bonds within ZIF-62. Consequently, the composite component structure significantly enhances the porosity and permeability of the MOF glass membrane. Furthermore, the incorporation of cobalt into the membrane matrix has notably enhanced its adsorption affinity for CO 2 , thereby boosting CO 2 /CH 4 selectivity. The resultant a g [(ZIF-9) 0.2 /(ZIF-62) 0.8 ] membrane has demonstrated exceptional CO 2 permeability of 20,324 barrer and superior CO 2 /CH 4 selectivity, both surpassing the 2018 upper bound. Thus, the innovative strategy for the design of MOF CGC membranes offers effective solutions to the challenges inherent in gas separation processes.
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
SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Zhenggang Wang,Jianwei Yuan,Renhao Li,Haipeng Zhu,Jingui Duan,Yanan Guo,Gongping Liu,Wanqin Jin
Compared with traditional separation methods, membrane-based technology shows advantages in energy efficiency for natural gas purification. To overcome the performance trade-off of conventional polymeric membranes, in this study, ZIF-301 MOF was employed as novel filler to fabricate 6FDA-DAM polyimide mixed-matrix membranes (MMMs) for CO 2 /CH 4 separation. A solvent exchange approach was proposed to remove the high-boiling-point solvent used for fabricating the MMMs. The microstructures and physico-chemical properties of the ZIF-301 fillers and ZIF-301/6FDA-DAM MMMs were characterized by SEM, EDX, XRD, IR, TGA, DSC and high-pressure sorption isotherms. The CO 2 /CH 4 transport properties through the MMMs were evaluated by permeation measurement at various feed pressures and analyzed by solution-diffusion model. The results showed that the incorporation of ZIF-301 into 6FDA-DAM enhanced both the CO 2 permeability and CO 2 /CH 4 selectivity, attributing to the preferential CO 2 sorption and aperture molecular sieving effect of the ZIF-301 filler. The MMM with optimal ZIF-301 loading of 20 wt% exhibited CO 2 permeability of 891 barrer and CO 2 /CH 4 of 29.3 that surpassed the 2008 Robeson upper-bound, suggesting that ZIF-301 based membrane could be a potential candidate for natural gas purification.
研究领域:
材料科学
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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
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2018
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IF 3.927
Shumin Wang,Qingping Guo,Shujun Liang,Peng Li,Jujie Luo
A series of mixed matrix membranes (MMMs) were fabricated with Ni-MOF-74 as filler and poly (styrene-b-butadiene-b-styrene) (SBS) polymer as matrix materials for CH 4 /N 2 separation. MMMs were characterized by Fourier transform infrared (FTIR) spectra, X-ray diffraction (XRD), scanning electron microscopy (SEM), and thermogravimetric analysis (TGA). Gas separation behavior was investigated by measuring single and mixed gases. For the single gas, the CH 4 permeability of the MMMs incorporated with 15 wt% Ni-MOF-74 (Ni-MOF-74/SBS-15) reached 83.5 Barrer, which was 116% higher than that of SBS (38.6 Barrer), while its ideal selectivity remained the same. CH 4 permeability can further increase to 176.6 Barrer with the increase in temperature to 55 °C. For the CH 4 /N 2 (50/50 vol%) mixed gas, the Ni-MOF-74/SBS-15 sample exhibited increasing CH 4 permeability (74.7 vs 36.7 Barrer), while selectivity remained unchanged relative to that of the pure SBS membrane.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
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2022
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IF 5.876
Yanyong Sun,Minmin Gou
Based on the one-dimensional tubular structure of halloysite nanotubes (HNTs), plant polyphenols and polyamines were used for in situ polymerization on the surface of HNTs to form amino-rich polymers, which were then removed as templates to synthesize polymer nanotubes. These nanotubes were then incorporated into a Pebax matrix to prepare mixed-matrix membranes (MMMs) for CO 2 /CH 4 gas separation. The removal of the HNT template increased the lumen diameter of the filler and significantly improved its gas permeability . And the amino groups on the inner surface of the polymer nanotubes were exposed. Further, the number of CO 2 reaction sites increased, which improved the reaction selectivity of CO 2 . In addition, the presence of amine groups on the inner and outer surfaces of the polymer nanotubes provided various transfer channels for CO 2 , which were conducive for CO 2 gas transfer in the membrane. When the CC-PEINT content was 8 wt%, the CO 2 permeability was 710 Barrer and CO 2 /CH 4 selectivity was 60. The CO 2 permeability and CO 2 /CH 4 selectivity of the Pebax/CC-PEINTs membranes increased by 163% and 132%, respectively, compared with those of the pure Pebax membrane.
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
RSC Advances
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2024
·Vol. 14
·期 29
·21151-21157
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IF 3.9
Jianwei Yang,Xianghao Han,Xiao Feng
As an emerging category of crystalline porous materials, covalent organic frameworks (COFs) are primarily synthesized via solvothermal methods. However, achieving rapid synthesis of COFs through this approach poses a significant challenge. To address the issue of slow synthesis, we studied the crystallization process of aminal-linked COFs via the condensation of a cost-effective aldehyde and secondary amine, and successfully expedited the synthesis of COFs within a one-hour duration. Furthermore, gram-scale aminal-linked COFs with abundant ultra-microporous channels demonstrated promising potential for CO2/CH4 separation. This study enables the rapid synthesis of aminal-linked COFs from cheap raw materials, which lays a foundation for their practical applications.
研究领域:
材料科学
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化学工程
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DOI
PubMed
高影响因子
Surfaces and Interfaces
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2025
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IF 6.3
Chaoqiang Li,Xiangyu Xu,Aizhong Jia
Photocatalytic reduction of CO 2 to chemical fuels is a promising strategy to alleviate the greenhouse effect and energy crisis. This article successfully fabricated Ag/CdS composites with ohmic junction using a two-step method and further verified them by DFT calculations. Meanwhile, photoelectrochemical and electron paramagnetic resonance tests show that Ag/CdS has higher photocurrent density and lower charge transfer resistance, suggesting that the ohmic junction achieves ultrafast electron transfer from CdS to Ag under light irradiation, significantly promoting the separation of photogenerated carriers. Furthermore, the localized plasmon resonance (LSPR) of Ag enhances the light absorption of the catalyst and generates a large number of hot electrons for the photocatalytic reduction reaction. The synergistic effect of ohmic junction and LSPR gives high electron density at the reaction site, which promotes the multiple proton-coupled electron reactions leading to highly selective photoconversion of CO 2 to CH 4 . Under the optimized conditions, the CH 4 yield of the synthesized Ag/CdS is 68.6 μmol·g −1 ·h −1 , which is 25.4 times higher than that of bare CdS, and the CH 4 selectivity increases from 53.8% to 90.1%. This study provides a new idea for the design of CdS-based materials for highly selective reduction of CO 2 to CH 4 .
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
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Wang Boxuan,Bao Qiang,Chen Zhirui,Qiao Xue,Hu Yunfeng,Zhang Jian,Liang Dan,Sun Penglai,Xia Haiyue,Wang Xiangyang
Zeolite RHO, a microporous zeolite, has the great possibility for N 2 /CH 4 separation by regulating the size of the eight-membered ring window on the RHO framework. In this work, the ability of ion-exchanged RHO zeolites for N 2 /CH 4 separation is investigated, and a highly nitrogen selectivity adsorbents are developed. RHO samples were prepared by hydrothermal synthesis. Alkali metal cations (Na + , K + , Cs + ) was used for ion exchange. Adsorption equilibrium isotherms of N 2 and CH 4 were measured at normal temperature and fitted by the Langmuir equation. The adsorbent selection parameters ( S parameters) were calculated based on the working capacity and equilibrium selectivity of N 2 /CH 4 , which are used to comprehensively evaluate the selectivity of N 2 /CH 4 . The results indicate that the cations have effects on the regulation of the eight-membered ring window. In particularly, K-RHO no.2 sample which is obtained by ion exchange of K + cations exhibit the best N 2 /CH 4 separation performance, which is a potential nitrogen selective adsorbent. In addition, the product throughputs of RHO and the commercial adsorbent ETS-4 were compared by common PSA simulation process with essentially the same product purity and recovery. The results show that K-RHO no.2 has 36 % higher product throughput than ETS-4, which can compensate for the problem of low N 2 working capacity of ETS-4 in industrial application.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Qiaoshan Chen,Yueling Chen,Mingfei Yu,Bin Xu,Houyi Wu,Liuyi Li,Jinhong Bi
A metal–insulator-semiconductor (MIS) ternary photo-system was intricately crafted through precise amalgamation polyvinylpyrrolidone (PVP)-capped metal Cu with typical covalent triazine framework CTF-1 via electrostatic self-assembly. The 2 % Cu-PVP-CTF exhibited an impressive CH 4 yield of 80.7 μmol·g −1 ·h −1 with selectivity of 96.8 % under visible light, representing a 2.3-fold and 112-fold improvement over Schottky-type Cu-CTF and pristine CTF-1, respectively. In-situ XPS and VASP-diff calculations unfolded that the ultrathin PVP insulating layer significantly expedited interfacial charges tunneling, corroborated by smaller lifetime τ 2 determined via femtosecond transient absorption spectroscopy. The intermediates of paramount importance in CO 2 reduction like *COOH and *HCHO were meticulously monitored by in-situ Fourier infrared spectroscopy. DFT calculations elucidated that Cu-PVP-CTF was notably more adept at facillitating the rate-determining step (*COOH → *CO) to produce CH 4 than Cu-CTF. This work tamps the groundwork for conceptional roadmap in designing novel MIS photo-system for CO 2 conversion.
研究领域:
材料科学
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催化化学
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能源转换
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DOI
高影响因子
危险品化学品经营许可证（带存储）