Journal of Materials Chemistry A
·
2015
·Vol. 3
·期 32
·16746-16761
·
IF 7.443
Jiayou Liao,Zhi Wang,Chengyun Gao,Ming Wang,Kai Yan,Xianmei Xie,Song Zhao,Jixiao Wang,Shichang Wang
A PVAm–HT membrane is fabricated by establishing a hydrotalcite (HT) channel in a polyvinylamine (PVAm) fixed carrier membrane. The flexible PVAm fixed carrier membrane material as a matrix membrane is beneficial to get high permeance. Simultaneously, the HT channels can be used as high-speed facilitated transport channels, in which the movable carbonate can actively meet CO2 and help to increase the CO2/N2 selectivity of membranes as in liquid membranes or in ion exchange membranes. Moreover, the unobstructed HT channels are conducive to transport CO2 rapidly and they can increase the chain spacing of polymers; these are beneficial to further enhance the permeance of membranes. In addition, the charged layers of HT provide necessary stability for movable carriers due to the electrostatic attraction. Thus, the PVAm–HT membrane obtains high permeance and high selectivity, as well as good stability. The CO2 permeance of the PVAm–HT membrane reaches 3187 GPU and the CO2/N2 selectivity of the PVAm–HT membrane reaches 296 at 0.11 MPa.
研究领域:
材料科学
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环境工程
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化学工程
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DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
·
IF 15.7
Xu Guangyuan,Peng Xingjie,Wu Chuanqiang,Xi Shibo,Xiang Huixin,Feng Lei,Liu Zhendong,Duan Yi,Gan Lijin,Chen Si,Kong Yuan,Ma Yanzhe,Nie Fujing,Zhao Jie,Hai Xiao,Wei Wei,Zhou Meng,Wang Tianfu,Yao Chuanhao,Zhou Wu,Yan Huan
CO 2 electroreduction to CO promises to give an efficient strategy for CO 2 fixation and transformation. However, current reported active sites fail to deliver sufficient activity with high CO Faradic efficiency (FEco) over a wide range of potential. Here, we show a general synthetic protocol to fabricate a batch of highly pure and active NiN 2 catalysts with precise engineering of the uniform-large ( UL ) vacancy around the active sites, which is accomplished through the ‘pre-deposition + pyrolysis’ of various atomically precise Ni clusters (Ni n ) and in-situ etching of the support by the ‘nano bomb’ (sulfur-ligand in the clusters). The NiN 2 sites with UL vacancies could achieve a high turnover frequency (TOF) of 350000 h −1 with ~100% FEco in a wide potential range of 1500 mV. In-situ infrared spectra and theoretical calculations reveal that a highly pure NiN 2 site with UL vacancy contributes to this remarkable catalytic performance compared to the counterparts. This general synthetic strategy enables us to simultaneously engineer active sites and surrounding vacancies with the employment of atomically precise metal clusters, thereby enhancing catalytic performance for other specific reactions.
研究领域:
材料科学
·
电化学
·
催化反应
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DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Xiaohang Sun,Zhengzuo Liu,Shuairen Qian,Kaiqi Nie,Zhengwen Li,Weiming Wan,Binhang Yan
Designing an active Cu/ZnO interface is crucial for efficient catalytic hydrogenation of CO 2 to methanol. In this study, we introduce a straightforward impregnation method to synthesize HKUST-1-derived inverse ZnO x /Cu catalysts. The resulting ZnO x /Cu interface exhibits outstanding methanol space-time yield and selectivity, surpassing conventional Cu/ZnO catalysts synthesized via the co-precipitation and impregnation methods. In situ characterization reveals that small, well-dispersed ZnO x nanoparticles are located on moderately sized Cu nanoparticles, which is attributed to the high specific surface area and ligand coordination of HKUST-1. The inverse ZnO x /Cu structure promotes the formation of reduced ZnO x nanoparticles, which significantly enhance CO 2 and H 2 activation, resulting in increased methanol production. Additionally, the moderate size of Cu nanoparticles minimizes CO* intermediate formation, further enhancing methanol selectivity. This work not only offers valuable insights for the development of new Cu/ZnO catalysts but also provides guidance for the synthesis of inverse metal oxide/metal catalysts for other catalytic systems.
研究领域:
催化化学
·
材料科学
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产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
·
2025
·
IF 4.7
Xiaojing Mao,Huachang Li,Yehong Shi,Jiemin Liu,Lijun Kuai,Jijun Liu,Yan Han,Yuexi Huang,Haijiao Xie
Two zinc-based metal-organic frameworks, namely [Zn(L 1 )(Phen)H 2 O] n ( 1 ) and {[Zn(L 2 )(Phen)]⋅(H 2 O)} n ( 2 ), were successfully constructed by mixed ligands strategy (HL 1 =1,4-benzendicarboxylic acid, Phen=1,10-phenanthroline monohydrate, HL 2 =5-hydroxyisophthalic acid), and characterized by X-ray single crystal diffraction, elemental analysis, powder X-ray diffraction (PXRD), etc. The X-ray single crystal diffraction demonstrate that both 1 and 2 show 1D chain structure. The orbital energies of 1, 2 and ligands have been investigated using the Density Functional Theory (DFT) calculations. The fluorescent sensing experimental revealed that both 1 and 2 exhibited excellent selectivity and sensitivity towards Cu 2+ and Co 2+ ions over other metal ions, and the detection limit (LOD) of Cu 2+ and Co 2+ for 1 were 0.077 μM and 0.15 μM, and the LOD of Cu 2+ and Co 2+ for 2 were 0.81 μM and 0.48 μM, respectively. In addition, the fluorescence quenching mechanism of Cu 2+ and Co 2+ can be attributed to energy competitive absorption. Furthermore, in the real sample detection, the recoveries of Cu 2+ and Co 2+ were 92.6 - 109.1 % and 96.7 - 110.0 %, respectively. This work provided a reliable method for the quantitative detection of Cu 2+ and Co 2+ and was successfully applied in river water with satisfactory recovery and precision.
研究领域:
材料科学
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分析化学
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产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Jiahe Li,Xing-Yue He,Xiaowen Wang,Yiwei Lv,Jian-Gong Ma,Bo Li,Peng Cheng
CO2 hydrogenation is one of the key technologies for carbon recycling and greenhouse effect mitigation. Cu-based catalysts have been widely used in the hydrogenation of CO2 to methanol. However, the low catalytic efficiency and instability of Cu-based catalysts limit their industrial application. Herein, a Zr-based metal−organic framework was used to synthesize a Cu NWs@ZrO2 catalyst with a Cu-ZrO2 interface. The Cu NWs@ZrO2 catalyst shows high activity with promising selectivity and excellent stability for the synthesis of methanol from CO2 hydrogenation. Density functional theory calculations and in situ diffuse reflectance Fourier transform infrared spectroscopy confirmed that the CO2 hydrogenation on Cu NWs@ZrO2 followed the HCOO* pathway, and the Cu-ZrO2 interface made a significant contribution to the key intermediate step of CO2 to HCOO* and accelerated the CO2 hydrogenation.
研究领域:
化学工程
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催化材料
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环境科学
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产品关联
DOI
PubMed
高影响因子
MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Zongtao Li,Xiaofang Yang,Yan Zhou,Anqi Huang,Yiping Sun,Zhenjuan Duan,Shengchun Yang,Chaofu Liao,Yong Liu,Xiaodong Wen
Excessive residues of Co 2+ in Chinese herbal medicines (CHMs) have attracted much attention because of their potential health hazards. This research synthesized sulfur quantum dots (SQDs) with excellent stability and water solubility via a facile one-pot route. During the illumination with ultraviolet light (λ max = 320 nm), the as-prepared SQDs emitted bright blue fluorescence at 431 nm. Meanwhile, the prepared SQDs could be used as fluorescent nanoprobes for detecting Co 2+ , showing an excellent linear relationship (R 2 = 0.998) when the Co 2+ concentrations were 5–50 μM, and the determination of the limit of detection (LOD) yielded a value of 4.51 μM. The introduction of Co 2+ resulted in the efficient quenching of SQD luminescence, attributable to the inner filter effect (IFE) that occurs between SQDs and Co 2+ . Finally, the feasibility of the proposed methodology was demonstrated by achieving a recovery rate of 98%–106% and a relative standard deviation (RSD) of 0.75%–3.51% during the detection of Co 2+ in Salviae miltiorrhizae Radix et Rhizoma . The results demonstrated that the fluorescent nanoprobes had broad application prospects in analyzing and detecting heavy metal ions in CHMs.
研究领域:
药学
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分析化学
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环境科学
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
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IF 9.229
Jia Wang,Yinghui Xu,Hongqiang Qu,Haiyun Ma,Ran Chang,Jing Ma
Delicately regulating the distribution morphology of a filler is an effective strategy to promote the separation performance of mixed matrix membranes (MMMs). Herein, we describe a highly permeable metal–organic framework (MOF)-based MMM comprising vertically aligned ZIF-8 (V-ZIF-8) and polysulfone (PSF). The V-ZIF-8 is distributed uniformly within the PSF matrix. With this unique distribution morphology of ZIF-8, the shortest gas transport pathways are formed in the membrane. Meanwhile, the molecular-sieving pores of ZIF-8 can allow CO2 to pass through and crowding out N2. The obtained V-ZIF-8/PSF membrane shows a high CO2 permeability of 89.7 Barrer and a CO2/N2 selectivity of 30.0 that is stable over a period of 50 h. The CO2 permeability is enhanced about 11.8 times than that of the pure PSF membrane. The results prove that the vertically aligned distribution morphology of an MOF in a polymer matrix is an effective method to improve the separation performance of a membrane, providing a new concept for designing more advanced membranes.
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
Journal of Materials Chemistry A
·
2017
·Vol. 5
·期 6
·2619-2628
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IF 8.867
Yuzhen Zhu,Zaixiang Xu,Wenya Jiang,Shuxian Zhong,Leihong Zhao,Song Bai
The utilization of a metal cocatalyst is a promising route to improve the solar-to-chemical conversion efficiency of semiconductor-based photocatalysts. The efficiency of the improvement is greatly dependent on the architectural structure of the metal cocatalysts, especially the catalytically active sites on the surface of the cocatalysts. In this article, Pd nanosheets with different sizes have been hybridized with TiO2 nanosheets to disclose how the edge of Pd cocatalysts influences the photocatalytic performance of TiO2–Pd hybrid structures in the reduction of CO2 to fuels. It was found that the highest photocatalytic activity was realized by small Pd nanosheets with the highest edge density on the TiO2 nanosheets. The reason is that the edges of the nanosheets act as the highly active sites for the CO2 reduction reaction. To further verify the edge-dependent photocatalytic performance, Pd nanorings were also deposited on the TiO2 nanosheets, which further improve the photocatalytic activity as compared with original nanosheets resulting from the additional edge sites exposed on the side of the hollow interior in the rings. This work underlines the importance in the edge engineering on the surface of cocatalysts in realizing high-performance photocatalytic applications.
研究领域:
材料科学
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能源化学
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环境科学
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产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2015
·
IF 2.587
Song Zhao,Xiaochang Cao,Zijian Ma,Zhi Wang,Zhihua Qiao,Jixiao Wang,Shichang Wang
In this work, imidazolate framework ZIF-8 nanoparticles were synthesized and incorporated into a poly(vinylamine) (PVAm) coating solution. The chemical structure of a PVAm/ZIF-8 film was characterized by X-ray diffraction and attenuated total reflectance Fourier transform infrared spectroscopy techniques. Mixed-matrix membranes (MMMs) were developed by coating the PVAm/ZIF-8 mixed dispersion on a polysulfone (PSf) support membrane. Surface and cross-sectional scanning electron microscopy images of the MMMs were employed to observe the dispersion of nanoparticles in the polymer matrix. The CO2 permeance and CO2/N2 selectivity of the MMMs were evaluated by using a CO2/N2 mixture gas. Optimal preparation parameters for the MMMs were achieved by varying the incorporated ZIF-8 contents in the coating solution and the wet coating thickness. The effect of incorporated ZIF-8 on improving the gas permselectivity was revealed, and the mechanism of CO2-facilitated transport in the PVAm/ZIF-8/PSf membrane was analyzed. The CO2/N2 separation performance of PVAm/ZIF-8/PSf membranes with different wet coating thicknesses was also evaluated at 22–60 °C to analyze the changes of the gas permselectivity with increasing temperature.
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
CHEMICAL PAPERS
·
2025
·
IF 2.5
Zhao Chun-Yan,Hu Xiu-Li,Zhou Wei
Calcium looping represents a high-temperature method designed to capture CO 2 , making it appropriate for CO 2 capture from flue gases post-combustion in power plants after combustion or for integration with fuel transformation techniques in pre-combustion CO 2 sequestration systems. This method employs solid sorbents of CaO sourced from natural limestone, leveraging the chemical interaction of CaO with CO 2 , which ultimately results in the formation of CaCO 3 , thereby facilitating effective CO 2 capture. In this research, multiple metal-incorporated CaO-based sorbents were produced through the sol–gel method. Notably, the CaO-based sorbent with a Ca/Ce doping ratio of 15 demonstrates exceptional CO 2 capture ability and stability, maintaining 13.20 mmol/g of CO 2 adsorption capacity after 20 carbonation/calcination cycles. Various characterization techniques, including X-ray diffraction (XRD), N 2 physisorption, scanning electron microscopy (SEM), high-angle annular dark field scanning transmission electron microscopy/energy dispersive spectroscopy (HAADF-STEM/EDS), temperature-programmed-desorption with CO 2 (CO 2 -TPD), Fourier Transform Infrared Spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS) are employed to demonstrate that the presence of nanoscale CeO 2 significantly enhanced the diffusion of CO 2 during the adsorption process.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Fangfang Li,Xiaofang Hou,Wei Fu,Jinjin Wang,Ying-Hua Zhou
The efficient transformation of CO 2 into high-value chemicals remains a significant challenge, particularly in the design of heterocatalysts capable of simultaneous multi-site activation towards the substrate. In this work, we develop the novel Zr-MOF catalysts incorporating both cobalt(II) meso-tetra(4-carboxyphenyl)porphine (CoTCPP) complex and the imidazolium bromide-based ionic liquid (IL) containing different alkyl chain (RImBr), where R = Et, Pr, Bu, and Pe), denoted as CoTCPP-UiO-66-IL(RImBr). The catalysts were synthesized through a solvothermal method followed by a post-synthetic modification. Among the prepared catalysts, CoTCPP-UiO-66-IL(BuImBr) demonstrated exceptional performance on the solventless and cocatalyst-free conversion of epichlorohydrin into chloropropene carbonate, achieving a remarkable 99% yield under mild conditions (90 °C and 1.0 bar CO 2 ). This outstanding catalytic efficiency was attributed to the synergistic effects of the dual Lewis-acid active sites offered by Zr-MOF node and the integrated CoTCPP complex, the strong nucleophilicity resulting from the incorporated imidazolium bromide-type IL, and the improved CO 2 adsorption capacity. Additionally, the CoTCPP-UiO-66-IL(BuImBr) catalyst exhibited excellent recyclability and broad substrate versatility in epoxide cycloaddition. These findings provide valuable insights into the development of multifunctional MOF-based heterogeneous catalysts with high activity and sustainability for CO 2 conversion applications.
研究领域:
材料科学
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催化化学
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环境科学
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产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2024
·
IF 4.8
Dandan Ma,Zhonghan Cheng,Ye Yuan,Somboon Chaemchuen
The heterometal functionalization on zeolitic-imidazole frameworks (ZIFs) is a strategy to modify properties over the homometal ZIFs. A green strategy for simultaneously functionalized iron atoms during the crystal formation of ZIF-67 (Fe@ZIF-67) through the solid-solid thermal (SST) method is newly developed. The single-step process and absent solvent conditions are beneficial advantages of this SST method over the early reported synthetic methods. The results show that the iron is well-dispersed and homogeneously coordinated in the structure of Fe@ZIF-67. Moreover, the optimal iron-functionalized ZIF-67 (20Fe@ZIF-67) significantly enhances the catalytic performance of CO 2 cycloaddition epoxide by 2.3 times compared to pristine ZIF-67 under mild reaction conditions. The DFT calculation reveals that the iron atom induces the unsaturated sites or defect structure on the Fe@ZIF-67 catalyst, providing more reactive sites for the catalytic activity of the reaction.
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
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