APPLIED SURFACE SCIENCE
·
2019
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IF 5.155
Huiqin Wang,Jingru Guan,Jinze Li,Xin Li,Changchang Ma,Pengwei Huo,Yongsheng Yan
In this work, the ordered mesoporous CeO 2 (m-CeO 2 ) was successfully fabricated via the nanocasting pathway, through using SBA-15 as a hard template. Besides, g-C 3 N 4 /Ag/m-CeO 2 composite was successfully constructed by calcination method. Meanwhile, the obtained samples were investigated by series of test techniques. The XRD, SEM and TEM results show that the m-CeO 2 and Ag/m-CeO 2 with the ordered mesoporous trait. Besides, the EPR, Raman and XPS results suggest that the oxygen vacancies (O v ) and Ce 3+ and Ce 4+ are in g-C 3 N 4 /Ag/m-CeO 2 . In addition, the ordered mesostructure is favorable for the CO 2 molecular movement and adsorption/desorption reaction. The g-C 3 N 4 nanosheets, a promising material possessing suitable conductor band, large specific area, non-toxicity, and outstanding chemical stability, is a candidate semiconductor for CO 2 conversion. The introduction of g-C 3 N 4 nanosheets to Ag/m-CeO 2 overcomes the photocorrosion of Ag nanoparticles and Ag facilitate the transfer of photogenerated electrons. The photocatalytic activity results show that when the loading of Ag is 7 wt%, the g-C 3 N 4 /7Ag/m-CeO 2 composite exhibits the superiority activity for CO 2 photoconversion to CO (13.94 μmol/g) and CH 4 (7.39 μmol/g) under UV-irradiation in 10 h.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
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2025
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IF 19
Shuai Yue,Guobin Xiao,Qiujin Shi,Xijiao Mu,Manke Zhang,Mingzheng Xie,Jing Cao
As a promising technology with both environmental and economic benefits, photocatalytic CO 2 conversion relies heavily on photo-carrier transport properties. However, oxide photocatalysts often face a significant limitation due to their restricted carrier transport distances, typically below 100 nm. Here, a surface electric field regulation strategy is proposed that enhances carrier transport in metal oxide photocatalysts by integrating specific porphyrin supramolecular assemblies. Through spin-coating, monoamine metal porphyrin assemblies are uniformly deposited on the BiVO 4 photocatalyst via van der Waals interactions. The electronic coupling between amine groups and Co atoms in adjacent porphyrin units generates unoccupied orbitals, which facilitate the accumulation of holes within the Co-porphyrin supramolecular system. This coupling induces interfacial electron redistribution and charge density reorganization, creating an intense surface electric field on BiVO 4 with an intensity of 17.4 V m −1 . As a result, the mobility of photo-carriers within BiVO 4 is significantly enhanced, extending the hole diffusion length from 46.7 to 232.9 nm and enabling more efficient charge extraction at the surface. This improvement results in a 7.3-fold increase in the photocatalytic CO 2 reduction performance, achieving an external quantum efficiency of 1.86%. The proposed approach offers a generalizable method for enhancing photo-carrier properties in photocatalytic systems.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
WATER AIR AND SOIL POLLUTION
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2025
·Vol. 236
·期 4
·1-13
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IF 3
Liu Lian,Wang Xin,Gao Zixin,Zhan Yue,Yao Mengqin,Bao Jia
Carbon capture, utilization, and storage (CCUS) has emerged as a critical strategy in combating climate change and global warming. Carbonic anhydrase (CA) exhibits exceptional potential as a biocatalyst for CCUS processes due to its remarkable ability to accelerate CO 2 hydration. In this study, CA was immobilized on ZnO nanocarriers of varying morphologies. The optimal immobilization conditions and enzymatic properties of the immobilized CA were investigated, followed by catalytic CO 2 uptake and mineralization experiments. The immobilization process resulted in several improvements: enhanced overall thermal stability, an elevated optimal reaction pH of 8.50 (compared to 8.00 for free CA), retention of 84.98% original activity after 30 days of storage at 4 °C, and preservation of 85.36% initial activity after five recycling cycles. While the affinity between immobilized CA and its substrate increased, a decrease in activity was observed. The Michaelis constant (Km) for immobilized and free CA were determined to be 17.22 mM and 34.92 mM, respectively, with corresponding catalytic efficiency (Kcat/Km) of 20.49 M −1 -S −1 and 148.91 M −1 -S −1 . The catalytic performance of immobilized CA was investigated by carrying out the CO 2 adsorption assay. Notably, the catalytic efficiency of immobilized CA in CO 2 absorption and mineralization under various conditions was significantly enhanced. Graphical
研究领域:
生物化学
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环境科学
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纳米技术
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DOI
高影响因子
Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Renbo Wei,Feng Gao,Hua Hou,Ben Bin Xu,Hongyun Yang,Xin Zhang,Zhanhu Guo,Lingling Wang
Synthesizing high-value-added products through the chemical conversion of CO 2 offers not only environmental benefits but also the potential for significant economic value. The development of practical catalyst is paramount to advancing CO 2 conversion and the synthesis of high-value chemicals. In this context, we present the fabrication of triazine and urea-constructed polyurea microsphere (TUC-PUMS) as a promising catalyst for converting CO 2 into cyclic carbonates using an enhanced dispersion polymerization method. Microscopic observations reveal that TUC-PUMS manifest as uniform microspheres with diameters ranging from 2 to 8 μm, suitable size for suspended bed or fluidized bed. Analytical techniques such as Fourier-transform infrared spectroscopy (FTIR), 13 C nuclear magnetic resonance (NMR), X-ray photoelectron spectroscopy (XPS), and X-ray diffraction analysis (XRD) spectra confirm the chemical structure of TUC-PUMS. By integrating triazine and urea groups, TUC-PUMS exhibits excellent catalytic activity for CO 2 conversion into cyclic carbonates under mild conditions when combined with tetrabutylammonium iodide. The achieved yield and selectivity approach 100 %, as well as excellent stability and versatility. The simultaneous integration of multiple functional groups, coupled with precise control over spherical morphology and microscopic size, enhances the competitiveness of TUC-PUMS as a promising catalyst for CO 2 conversion.
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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DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Yuxin Yuan,Quanlan Liao,Tianxiang Zhao
Metal-organic frameworks (MOFs) have been hybridized with other functional materials, such as ionic liquids, covalent organic frameworks (COFs), and metallic nanoclusters, to fabricate composite materials. These composites possess the structural characteristics of their individual components and exhibit synergistic properties. In this work, we demonstrate the synthesis of core-shell structure UiO-66-NH 2 @PILs-x composite materials by encapsulating MOFs within ionic polymers (PILs) with varying thicknesses of PILs shell. These hybrid materials serve as bifunctional catalysts for the conversion of CO 2 into cyclic carbonates under solvent- and additive-free conditions through a synergistic catalytic effect facilitating the conversion of CO 2 into cyclic carbonates under solvent- and additive-free conditions through synergistic catalytic effect, exhibiting superior catalytic performance and excellent recyclability. This MOFs-based composite material provides a competitive approach for CO 2 catalytic conversion.
研究领域:
材料科学
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催化化学
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DOI
高影响因子
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2025
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IF 6.2
Mingqiang Chen,Quan Wang,Defang Liang,Yishuang Wang,Chang Li,Xuemei Shen,Chunyue cheng,Jun Wang
Herein, a series of Fe-based biochar catalysts (xFe/WSBC) were synthesised via impregnation using wheat straw as a carbon precursor and applied to the Fischer–Tropsch synthesis of olefins (FTO) from syngas. Various characterisations of fresh catalysts demonstrated that Fe content significantly affected the dispersion of iron particles and the surface distribution of Fe 3 + /Fe 2+ . Among the samples, 5Fe/WSBC exhibited the highest surface Fe 3+ /Fe 2+ ratio and thus the lowest surface electron density, which enhanced the adsorption and activation of H 2 . In addition, an appropriate amount of the Fe additive (5 wt%) significantly decreased the Fe 3 O 4 particle size, which promoted the continuous reduction and carbonisation processes during FTO to generate iron carbide phases, which boosted CO activation and the subsequent C–C coupling. Therefore, 5Fe/WSBC exhibited the highest CO conversion (46.9 %) and iron time yield (348.9 μmol CO ·g Fe −1 ·s −1 ) as well as the major enhancement of selectivity to light olefins (C 2 = –C 4 = ). The results for the used catalysts demonstrated that 5 wt% Fe clearly inhibited the sintering of iron particle size and improved the catalytic stability of FTO.
研究领域:
催化化学
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能源科学
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环境工程
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Quan Shi,Ming-Hui Chen,Ji Xiong,Ting Li,Ya-Qing Feng,Bao Zhang
2D metal − organic framework (MOF) nanosheets have been demonstrated to exhibit excellent properties and prospects in various aspects, especially in photocatalysis . However, the design and direct preparation of 2D MOF photocatalyst is highly desirable but still challenging. Herein, a novel 2D porphyrin-based MOF Fe-DBP(Co), which is assembled by dicarboxylic porphyrin ligands and the unprecedented undecametallic ferric-oxo clusters, is designed and developed. The unique nanosheet morphology and assembled layered structure endows the photocatalyst with higher electron-hole separation efficiency and longer photogenerated carrier lifetime compared to the analogous MOFs. Consequently, Fe-DBP(Co) exhibits strikingly excellent and stable photocatalytic performance in CO 2 cycloaddition, and the reaction rate of 103.2 mmol∙g −1 ∙h −1 is among the state-of-the-art cases for MOF-photocatalyzed CO 2 cycloaddition. The underlying mechanism investigation suggested that photogenerated electrons transferred from CoDBP ligands to the Fe clusters, and the abundant electrons and holes promoted the generation of Fe(II) and Co(III) respectively, leading to excellent catalytic performance. This work proposes a new strategy to design and develop efficient MOF photocatalysts for photocatalytic transformation of CO 2 .
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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DOI
高影响因子
ENERGY
·
2024
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IF 9
Xu Ma,Wei-Wei Yang,Ju-Wen Su,Lan-Xin Liang,Wang-Xin Yang,Ya-Ling He
This study employed a novel one-pot method to encapsulate cerium species on the Ni–Al heterogeneous interface, aiming to achieve the capture and efficient utilization of greenhouse gas (CO 2 ). Characterization results revealed that nickel species experienced various forms such as oxides and carbon-nickel compounds at the heterogeneous interface. The presence of cerium groups within the catalytic system induces the precipitation of nickel grain monomers on the support, decomposing the CH 4 –CO 2 reforming process into a multistep reaction that breaks the thermodynamic barrier and kinetic limitation of the multicarbon coupling phenomenon, and greatly reduces the energy consumption of the reaction. Results showed that at a temperature of 800 °C and a Ni/Ce molar ratio of 0.2 in the catalyst, the activity was stable and the CO 2 conversion reached 81.69 %, which was a 15.33 % enhancement compared to the base catalyst. Additionally, the mutual conversion of Ce 3+ /Ce 4+ promoted the internal electron interaction process in the catalytic system, increasing the number of oxygen vacancies and reducing acidic sites, which facilitated reactant activation and carbon elimination. This work provides insights for the efficient utilization of greenhouse gases.
研究领域:
催化化学
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环境科学
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DOI
高影响因子
Surfaces and Interfaces
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2024
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IF 5.7
Leizhi Zheng,Yang Xu,Chenyang Huang,Jia Liu,Lei Zhou,Chengbao Liu
Graphitic carbon nitride (g-C 3 N 4 ) containing conjugated tri-s-triazine units has a high abundance of amine and guanidine groups, which are ideal for the application of CO 2 conversion. However, absolute g-C 3 N 4 is inherently scarce in Lewis base sites, which leads to low catalytic activities. In this study, we present a simple and green method to in situ construct chrysanthemum stalk-derived porous carbon/ highly active defective g-C 3 N 4 (PC/g-C 3 N 4 ) through hydrogen bond, increasing the surface area and a high density of Lewis base sites. The chrysanthemum stalk contains cellulose, hemicellulose and lignin, which possess a significant number of hydroxyl functional groups and drain channels, thereby providing more hydrogen bonding for highly active defective g-C 3 N 4 . The XPS spectra revealed that, in comparison to PC/g-C 3 N 4 –1 and PC/ g-C 3 N 4 –2.5, PC/g-C 3 N 4 –2 exhibited a higher C-NH 2 content at the edge of the nitrogen element. PC/g-C 3 N 4 –2 had a high specific surface area to expose more active sites for absorbing CO 2 . The quantification of the base sites is determined by the peak area of the thermal programmed desorption of CO 2 and is 229.6 μmol/g for PC/g-C 3 N 4 –2. PC/g-C 3 N 4 –2 demonstrated excellent catalytic activity in the cycloaddition with hierarchical pores. The yield of cyclic carbonate was up to 99% with a selectivity of 99% under mild solvent-free conditions. The mechanistic studies indicate that PC/g-C 3 N 4 –2 not only captured CO 2 , but also provided hydrogen bonds to activate the oxygen atom of epichlorohydrin (ECH). It is our contention that the multifunctional organic-inorganic hybrid materials have considerable potential for the production of cyclic carbonate.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
Journal of CO2 Utilization
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2018
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IF 5.503
Yu-Nong Li,Xiao-Fang Liu,Liang-Nian He
The oxazolidinone as one kind of annular CO 2 derivatives has been hydrogenated by a new catalytic system Pd/C-TMGPEG 150 Me (polyethylene glycol-functionalized 1,1,3,3-tetramethyl guanidine), affording two valuable products i.e. formic acid and the corresponding secondary alkyl-(2-arylethyl)amines in the high yields of 89% and 98%, respectively. This hydrogenation can be carried out smoothly under relatively mild conditions of 60 °C, 4 MPa of H 2 with a liquid/solid carbon source (oxazolidinone) instead of high pressure CO 2 . The notable results can be successfully obtained even at room temperature under atmospheric H 2 pressure. This one stone two bird strategy is applicable to series of 5-aryl-2-oxazolidinones and opens up a novel way of synthesizing linear secondary alkyl-(2-arylethyl)amines without the selectivity issues, and validates a potential alternative approach for indirect conversion of CO 2 to energy-related products formic acid, as oxazolidinones can be readily obtained from hydrogenation of CO 2 .
研究领域:
化学
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催化科学
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绿色化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
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IF 16.744
Xiaoshan Dong,Xiaochao Zhu,Fawei Lin,Beibei Yan,Jian Li,Guanyi Chen
Tar formation during biomass gasification reduces energy efficiency and poses a negative impact on downstream applications. A photothermal steam reforming (PTR) system based on LaMn x Ni 1-x O 3 (0 ≤ x ≤ 1) perovskite was developed to convert tar into combustible gas. The effects of Mn substitution, temperature, and the steam to carbon ratio on PTR activity were investigated. Mn substitution increased the content of surface adsorbed oxygen and maintained the perovskite structure of LaMn 0.4 Ni 0.6 O 3 (LM4N6). Moreover, LM4N6 showed improved optical absorption and electron-hole separation properties. LM4N6 presented 90 % carbon conversion during PTR at 400 °C. Due to the introduction of ultraviolet–visible light (UV–vis), LM4N6 obtained better catalytic activity and stability in PTR than in the thermal catalytic reforming process. Detailed characterization and experiments proved that UV–vis effectively activated Ni sites and the oxygen species on LM4N6 and formed a photothermal synergistic effect, which inhibited carbon deposition and improved catalytic activity and stability. This work provides a novel concept for the conversion and utilization of biomass tar at low temperatures.
研究领域:
能源科学
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催化化学
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DOI
高影响因子
Small
·
2023
·Vol. 19
·期 27
·2207915
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IF 13.3
Jinchen Zhou,Daofu Wu,Changqing Tian,Zhiyu Liang,Hongmei Ran,Bo Gao,Zhongtao Luo,Qiang Huang,Xiaosheng Tang
Lead halide perovskite materials have great potential for photocatalytic reaction due to their low fabrication cost, unique optical absorption coefficient, and suitable band structures. However, the main problems are the toxicity and instability of the lead halide perovskite materials. Therefore, a facile synthetic method is used to prepare lead-free environmentally friendly Cs 2 TiX 6 (X = Cl, Cl 0.5 Br 0.5 , Br) perovskite materials. Their structural and optical characteristics are systematically investigated. The band gaps of the produced samples are illustrated to be from 1.87 to 2.73 eV. Moreover, these materials can keep high stability in harsh environments such as illumination and heating, and the Cs 2 Ti(Cl 0.5 Br 0.5 ) 6 microcrystals demonstrate the yields of 176 µmol g −1 for CO and 78.9 µmol g −1 for CH 4 after light irradiation for 3 h, which is of the first report of Ti-based perovskite photocatalysts. This finding demonstrates that the Ti-based perovskites will create opportunities for photocatalytic applications, which may offer a new idea to construct low-cost, eco-friendly, and bio-friendly photocatalysts.
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
PubMed
高影响因子
危险品化学品经营许可证（带存储）