ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2023
·
IF 11.4
Ruimeng Wang,Xinqi Luan,Muhammad Yaseen,Jingyu Bao,Jing Li,Zhongxing Zhao,Zhenxia Zhao
High-capacity adsorption and removal of complex volatile organic compounds (VOCs) from real-world environments is a tough challenge for researchers. Herein, a swellable array adsorption strategy was proposed to realize the synergistic adsorption of toluene and formaldehyde on the flexible double hypercross-linked polymers (FD-HCPs). FD-HCPs exhibited multiple adsorption sites awarded by a hydrophobic benzene ring/pyrrole ring and a hydrophilic hydroxyl structural unit. The array benzene ring, hydroxyl, and pyrrole N sites in FD-HCPs effectively captured toluene and formaldehyde molecules through π–π conjugation and electrostatic interaction and weakened their mutual competitive adsorption. Interestingly, the strong binding force of toluene molecules to the skeleton deformed the pore structure of FD-HCPs and generated new adsorption microenvironments for the other adsorbate. This behavior significantly improved the adsorption capacity of FD-HCPs for toluene and formaldehyde by 20% under multiple VOCs. Moreover, the pyrrole group in FD-HCPs greatly hindered H2O molecule diffusion in the pore, thus efficiently weakening the competitive adsorption of H2O toward VOCs. These fascinating properties enabled FD-HCPs to achieve synergistic adsorption for multicomponent VOC vapor under a highly humid environment and overcame single-species VOC adsorption properties on state-of-the-art porous adsorbents. This work provides the practical feasibility of synergistic adsorption to remove complex VOCs in real-world environments.
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Catalysis Science & Technology
·
2023
·Vol. 13
·期 12
·3558-3567
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IF 5
Lihua Wang,Shuangxiu Ma,Chunhong Chen,Bing Lu,Zhe Wang,Yong Wang,Shanjun Mao
The high-loading, good distribution and stable heterogenization of polyoxometalate (POMs) salts with supports, such as oxides, is rather challenging since the structural integrity of POMs is easily destroyed if strong interactions exist. Here, we developed a novel route to achieve the in situ anchoring of high-loading ammonium phosphomolybdate (APMo, with a mass fraction as high as 49%) on alumina with coordinatively unsaturated Al3+ sites without the deformation of the Keggin structures of POMs. The anchoring effect of Al3+penta to polyoxometalates originating from the strong APMo–alumina interaction effectively promotes the dispersion and stability of APMo compared to the samples made by impregnation. The remaining heteropoly acid structure and synergistic effect between APMo and alumina make the hybrid materials exhibit superior redox and acid catalytic performances, achieving >99% selectivity of benzaldehyde for benzyl alcohol oxidation and double the yield for fatty acid esterification compared with that of the impregnated catalyst. This work offers an alternative to the trade-off problem for the heterogenization of POM catalysts and provides a green and recyclable catalyst for the efficient valorization of biomass-derived feed blocks into value-added chemicals.
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Catalysts
·
2023
·Vol. 13
·期 5
·864
·
IF 3.9
Xiya Chen,Hangwei Jiang,Danlan Cui,Kun Lu,Xiao Kong,Junmeng Cai,Shirui Yu,Xingguang Zhang
In organic synthesis, it is important to control the selectivity target product with high purity and reduce the cost of energy and equipment for separation. This study investigated supported gold catalysts on biochar-modified titanate-based nanofibers in order to regulate the catalytic performances by biochar content and surface properties. The catalysts were characterized by SEM, TEM, XRD, XPS, ICP-OES, UV-Vis to confirm their morphology, particle size distribution of Au NPs, crystal structures, oxidation state of Au and other key elements, real Au loading, and optical properties. In the test of selective oxidation of benzyl alcohol to benzaldehyde, the biochar modification could improve the selectivity toward benzaldehyde. Moreover, the influence of catalyst calcination conditions, reaction time, reaction atmospheres, reaction temperatures and solvent were systematically investigated. These results are useful for peer researchers in rational catalyst design.Keywords:gold catalysts;selectivity regulation;selective oxidation;benzyl alcohol
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Catalysis Science & Technology
·
2023
·Vol. 13
·期 12
·3568-3578
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IF 5
Menghui Liu,Chenhui Wang,Zifan Cao,Aiqun Kong,Yusheng Gao,Jinli Zhang,You Han,Wei Li,Yan Fu
A series of 3D self-standing PtRu/Ni(OH)2/NF electrodes is fabricated for electrocatalytic hydrogenation (ECH) of benzoic acid (BA) to cyclohexanecarboxylic acid (CCA). The PtRu/Ni(OH)2 electrocatalyst with a unique coral-shaped architecture possesses outstanding charge transfer ability and abundant active sites. The optimized electrode achieves a BA conversion of 99.00% and a CCA selectivity of 100% in 0.05 M H2SO4 within 80 min, showing a record faradaic efficiency of 43.90% and high performance during 20 cycles of ECH. In situ Raman tests verify the mechanism of the selective hydrogenation of the aromatic ring and density functional theory (DFT) calculations reveal that the electronic interaction between Pt and Ru in the PtRu nanoalloy as well as the electron transfer from the PtRu alloy to the Ni(OH)2 nanosheet tunes the electronic states of PtRu/Ni(OH)2, thereby enhancing the adsorption strength of BA on the electrocatalyst surface. This work offers a promising alternative to the traditional catalytic hydrogenation of BA.
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Food Chemistry-X
·
2023
·
IF 6.1
Chang He,Jingtao Zhou,Yuchuan Li,De zhang,Bernard Ntezimana,Junyu Zhu,Xiaoyong Wang,Wenluan Xu,Xiaoju Wen,Yuqiong Chen,Zhi Yu,Yu Wang,Dejiang Ni
This study delved into the aroma characteristics of “Qingxiang” oolong tea, analyzing six different cultivars and their processing modes. The findings showed that both cultivars and processing modes have a significant impact on the oolong tea aroma system. The study identified 18 terpenoid volatiles (VTs), 11 amino-acid-derived volatiles (AADVs), 15 fatty-acid-derived volatiles (FADVs), 3 carotenoid-derived volatiles (CDVs), and 10 other compounds in oolong tea that differentiate it from green and black tea. The turn-over stage was found to be the primary processing stage for oolong tea aroma formation. Molecular sensory analysis revealed that the “fresh” odor attribute is the basis for its aroma, while “floral and fruity” fragrances are its aroma characteristics. The perception of oolong tea as “fresh” and “floral and fruity” is influenced by the interactions of its aroma components. These findings provide a new basis for breed improvement and process enhancement in oolong tea production.
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高影响因子
GREEN CHEMISTRY
·
2023
·Vol. 25
·期 11
·4453-4462
·
IF 9.8
Ye Meng,Jinshu Huang,Jie Li,Yumei Jian,Song Yang,Hu Li
Nitriles are versatile nitrogen-containing scaffolds that exist widely in medicines, dyes and functional materials, and are typically synthesized over homogeneous catalysts under relatively harsh conditions. Herein, through mimicking the key active species of hemoglobin p450 heme monooxygenase in most organisms, a Fe–N4 single atom-doped sulfur-containing carbon nitride (Fe/CNS) photocatalyst was facilely prepared by one-step thermal polymerization, which was illustrated to be efficient for renewable conversion of bio-based alcohols and NH2OH·HCl to a wide range of nitriles (80–92% yields) via cascade oxidation–ammoxidation at room temperature, or to quantitatively furnish benzaldehyde via oxidation in the absence of a nitrogen source. Theoretical calculations showed that the isolated Fe–N4 sites directly capture photogenerated electrons (e−) and molecular oxygen (O2) to generate superoxide radicals (˙O2−), while the surrounding S atoms confine photogenerated holes (h+). The high efficiency of Fe/CNS in the photo-generation of ˙O2− and holes may contribute to the smooth formation of nitriles by cascade photocatalytic oxidation of alcohol and ammoxidation via an in situ formed oxime, respectively. Moreover, Fe/CNS was also applicable to the selective synthesis of various imines (83–98% yields) from the oxidation of benzylamines or heterocyclic amines under visible-light irradiation, and could be recycled at least 5 times with no evident decline in catalytic activity. The strategy of rationally constructing atomic sites to spatially isolate paired electron–holes and form specific reactive species for enhanced photocatalytic activity/selectivity provides an efficient and green approach for biomass valorization.
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Foods
·
2022
·Vol. 11
·期 24
·3997
·
IF 5.561
Youyou Yang,Jing Li,Jiangtao Xing,Weihai Xing,Chaohua Tang,Zhenghua Rao,Junmin Zhang
Volatile compounds play vital roles in food sensory attributes and food quality. An analysis of volatile compounds could illustrate the sensory attributes at the microscale level. Here, untargeted profiling approaches for volatiles in five most-consumed meat species were established using headspace SPME-GC/high resolution Orbitrap MS. An extended high-resolution database of meat volatile compounds was established to enhance the qualification accuracy. Using sulfur-containing compounds, aldehydes, and ketones as the research model, the parameters including fiber coating types, extraction temperature, extraction time, and desorbing time were optimized. Principle component analysis, volcano analysis and partial least squares discriminant analysis were applied to run the classification and the selection of discriminant markers between meat varieties, respectively. Different varieties could be largely distinguished according to the volatiles’ profiles. 1-Octen-3-ol, 1-octen-3-one, 2-pentyl furan and some other furans degraded from n-6 fatty acids would contribute to distinguishing duck meat from other categories, while methyl esters mainly from oleic acid as well as dimethyl sulfoxide and carbon disulfide possibly produced from the sulfur-containing amino acids contributed to the discrimination of beef. Therefore, volatiles’ profiling not only could interpret the aroma style in meat but also could be another promising method for meat differentiation and authentication.Keywords:differentiation;GC-HRMS;SPME;statistical analysis;untargeted profiling;volatiles
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LWT-FOOD SCIENCE AND TECHNOLOGY
·
2022
·
IF 6.056
Xiaoqing Ye,Yan Liu,Changbo Peng,Xi Guan,Yi Liu,Zhenming Che,Hongbin Lin,Xu Min,Qi Zhu,Wenwu Ding
In this study, Pixian Douban (PXDB) was produced in a closed system of multi-scale temperature and flow fields constructed with the materials of pseudoplastic fluid in a gradient steady-state temperature field. The flavors and microorganisms of PXDB in the MTFF were compared with those in the traditional process with original materials (TPOM) and the traditional process with materials of pseudoplastic fluid (TPPF). The contents of organic acids, free amino acids and flavors in the MTFF were higher than those in the TPPF and TPOM. Chitinophagaceae_Unclassified and Bradyrhizobium_Unclassified were the predominant bacteria while Phyllachora sp . UB03986 and Rhizopus oryzae were identified as the core fungi at the species levels in the processes. The correlation analysis showed that 26 bacterial and 6 fungal were significantly correlated with the flavors. The results indicated that the closed system of MTFF could improve the product quality and was helpful to realize the controllable PXDB production.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
He Huang,Huahua Fan,Yuzhen Ge,Wanyue Ye,Yingcen Liu,Caicheng Song,Hua Lin,Xiaotong Zhang,Bing Li,Xiaowa Nie,Shufen Zhang,Rongwen Lu
The selective oxidation of the primary C H bonds in hydrocarbons to corresponding high-valued oxygenates is highly desired but challenging to realize. The difficulty arises from the high homolytic bond dissociation enthalpy of the C H bond, the relatively high reactivity of oxygenated intermediates, and the diversity of resultant products. Herein, we reported the in situ confinement of Au clusters in Silicalite-1 for the selective solvent-free oxidation of toluene to benzaldehyde. The doping of an alkali metal (K or Na) resulted in the formation of electron-rich Au species, which readily facilitate the activation of oxygen, In turn, toluene is activated by the produced reactive oxygen species in a single step, as confirmed through density functional theory (DFT) calculations. At optimal alkali metal doping, the selectivity to benzaldehyde could reach > 90 %, with the toluene conversion being 19.8 %. Remarkably, the total turnover number (TTN) of Au@Silicalite-1–0.2 K was found to be 29,658, which is one or two orders of magnitudes higher than the previously reported values. These findings are expected to inspire the design of highly efficient catalysts for the activation of fundamental feedstock with C H bonds.
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ACS Catalysis
·
2023
·
IF 12.9
Yaming Hao,Jili Li,Xueting Cao,Lingshen Meng,Jianxiang Wu,Xuejing Yang,Yefei Li,Zhipan Liu,Ming Gong
The paired electrolysis via anodic organic oxidation and cathodic hydrogen evolution has been an emerging hydrogen production technology with high efficiency and high values. Nickel oxyhydroxide is a special electrocatalyst that is capable of selectively oxidizing various alcohols, aldehydes, and amines to the corresponding carboxylates and nitriles at more favorable potentials compared to the oxygen evolution reaction. However, its detailed molecular-level mechanism is still in debate, especially for the potential-dependent behavior of some organic substrates. In this study, we revealed that the nickel oxyhydroxide can be dissected into two functional regions with a more facilely oxidized surface for facilitated substrate adsorption and a relatively inert bulk phase for accelerated electron transfer via probe-assisted kinetics and in situ surface-enhanced Raman spectroscopy. The prerequisite of the two regions conceals a universal potential-dependent oxidation behavior for almost all organic substrates. Further combining with the computational investigation unravels the origin of this potential dependence from the exothermic O/N-centered adsorption process on the surface and the rate-limiting proton-coupled electron-transfer (PCET) steps for the C–H bond breaking that demands bulk electron conductivity. This provides a rationale for designing more conductive underlayers to break the intrinsic limitations of nickel oxyhydroxide toward more efficient organic electrooxidation processes.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Baoyu Wang,Mingrui Li,Songdang Zhang,Hongguo Wu,Yuhe Liao,Hu Li
Finite size effect is closely correlated with heterogeneous catalytic activity and selectivity as reducing the metal to a few nanometers, but may suffer from deficient active sites for cascade reactions. Here, a type of dual-size heterogeneous N-doped cobalt catalysts (Co SAs-NPs /NC(n)) with the coexistence of Co single-atoms (Co-SAs) and Co nanoparticles (Co-NPs) were prepared for efficient synthesis of benzimidazoles (up to 91% yield) from 2-nitroanilines and bio-based alcohols via cascade hydrogen transfer-dehydrogenative cyclization. Experimental results and density functional theory calculations suggested that the bio-alcohol dehydrogenation mainly occurs at Co-SAs sites, while Co-NPs sites remarkably facilitate the subsequent reduction of nitro species, indicating the synergistic effect between Co-SAs and Co-NPs in the coupled hydrogen transfer process. The Co SAs-NPs /NC(0.25) catalyst can be recycled and applied to a wide range of substrates (28 examples). This catalytic approach based on the metal size effect opens a new route for the direct upgrading of biomass feedstocks involving multiple reactions.
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INTERNATIONAL JOURNAL OF HEAT AND MASS TRANSFER
·
2023
·
IF 5.2
Shuai Yuan,Mingyong Zhou,Xijiang Liu,Bingyan Jiang
The coupling of pressure-driven flow (PDF) and electroosmotic flow (EOF) has been widely applied in the field of microfluidics. However, the adverse effects of pressure induced by PDF on EOF in a confined space cannot be ignored. Herein, the interactions of these two streams when the Reynolds number ( Re ) varies from 0.1 to 10 are systematically explored through numerical simulations to gain an in-depth understanding of the mechanism of the pressure effect on mass species transport and to generate optimal separation of samples. The simulation results show that the length of the sample increases linearly and the molecular diffusion is accelerated due to the pressure effect caused by the EOF channel structure and PDF extrusion, which reduces the separation quality and even leads to the failure of electrophoresis . However, the deformation of the sample cannot be effectively resisted by increasing the applied voltage . A better separation effect can be obtained only when Re =0.1. To surmount the above disadvantages, a novel porous polymer plug with pores smaller than 5 μm that provides a region that has high flow resistance but allows the electromigration of charged analytes is established in the EOF channel. The experimental results show that this plug can effectively neutralize the EOF outlet pressure when Re ≤5. The shape of the sample is not distorted and the maximum gray values decreased by 26%, 30% and 49% respectively in 7 s when Re =0.1, 1 and 5, which are much better than the results without the plug.
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