Nature Communications
·
2025
·Vol. 16
·期 1
·1-16
·
IF 15.7
Kang Wei,Wu Zhiyue,Huang Xinzhi,Qi Hongbin,Wu Jiaxuan,Wang Jiahui,Li Jing,Wu Sijin,Kang Byung-Ho,Li Bo,Ma Juncai,Xue Chuang
Biomolecular condensates are dynamic cellular compartments that concentrate proteins and enzymes to regulate biochemical reactions in time and space. While these condensates can enhance enzyme activity, how this function changes as condensates age remains poorly understood. Here, we design synthetic catalytic condensates that selectively recruit enzymes to investigate this temporal evolution. We show that catalytic condensates exhibit time-dependent activity: they initially accelerate enzymatic reactions but gradually lose efficiency due to the transition from liquid-like to solid-like states. This aging process, characterized by protein aggregation and loss of selective barriers, impairs enzyme function both in vitro and living cells. We further demonstrate that small molecules which influence aging dynamics can modulate catalytic efficiency of condensates. Our findings show that condensate aging as a key regulator of enzymatic activity and provide crucial insights for designing functional synthetic condensates.
研究领域:
分子生物学
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生物化学
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细胞生物学
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合成生物学
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产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Yakai Chen,Xinya Feng,Xiaohan Yu,Xingliang Xu,Jing Xu
Catalytic aldol condensation of biomass-derived furfural (FAL) with acetone (AC) into the single-condensation product 4-(2-furyl)-3-buten-2-one (FAC) is a potential and promising strategy for biomass improvement process and still challenging. Metal oxides exposed different crystal facets can regulate their surface structure and adsorption activation ability, which can provide an opportunity to enhance aldol condensation performance. Here, nanoparticles-CeO 2 (P-CeO 2 ), nanorods-CeO 2 (R-CeO 2 ) and nanocubes-CeO 2 (C-CeO 2 ) with (111), (110) and (100) plane predominant exposure was prepared to explore their catalytic performance for the aldol condensation of FAL with AC to obtain FAC. The serial detailed characterizations, experimental results and density functional theory calculation revealed that R-CeO 2 with a dominant (110) facet possesses appropriate surface adsorption energy, abundant oxygen vacancy (Ov) and excellent acid-base properties, which can effectively boost the adsorption and activation of FAL and AC and reduce the barrier of aldol condensation reaction based on the acid-base catalysis mechanism. The work would reveal the influence of CeO 2 crystal facet on the aldol condensation and provide a broad potential for the rational design of metal oxide catalysts for other acid-base catalytic reactions.
研究领域:
催化化学
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生物质能
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材料科学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
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2013
·
IF 3.41
Jin Zhao,Jun Xie,Chak-Tong Au,Shuang-Feng Yin
We report a new strategy for one-pot synthesis of potassium-loaded MgAl oxides using KOH to adjust the pH value of the reaction system. The as-prepared solid superbases were studied by N 2 physisorption method, energy-dispersive X-ray spectroscopy, powder X-ray diffraction, and Fourier transform infrared. The superbasic sites were characterized by the use of Hammett indicators and CO 2 temperature-programmed desorption. We found that with a base strength ( H – ) above 26.5, the potassium-loaded MgAl oxides showed high catalytic activity for Knoevenagel condensation at room temperature. Furthermore, the higher the superbasicity and/or the more the amount of superbasic sites, the better is the catalytic activity. The findings open up a new route for the synthesis of new functional superbases using composite oxides as supports.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ENERGY & FUELS
·
2018
·
IF 3.024
Jin Tan,Chenguang Wang,Qi Zhang,Longlong Ma,Minghong He
A novel and efficient method for the use of non-edible cassava to synthesize biofuel precursors with long carbon chains in two steps was proposed. The finally produced precursors were based on the decomposition of cassava and condensation between furans and levulinates. The reaction parameters for levulinate production from cassava were optimized, and the results showed that the highest carbon mole yield of levulinates was up to 51.3% at 473 K, 4.0 MPa N2, and 6.0 h. After that, precursors with yields of 88.0 and 90.5% could be obtained when the mole ratios between furans and levulinates were 1:1 and 2:1, respectively. Characterization of precursors using elemental analysis, 13C nuclear magnetic resonance, gel permeation chromatography, and Fourier transform infrared spectroscopy demonstrated that different and intersecting routes of condensation resulted in the complex components of precursors. Moreover, the mechanism of condensation was proven to excessively depend upon the mole ratio between furans and levulinates in this investigation. This technical route indicates a simple and feasible method to produce renewable biofuel with long carbon chains from cassava directly.
研究领域:
生物化学
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可再生能源
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有机合成
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产品关联
DOI
高影响因子
Catalysts
·
2020
·Vol. 10
·期 2
·211
·
IF 3.52
Yongxin Zhang,Long Lin,Xiaoming Zheng,Chunyan Liu,Quanren Zhu,Hongchen Guo
In this study, a series of SnO2modified zeolite catalysts (Snx-S-1; x is the weight percentage of Sn) were prepared with SnCl2and a defective Silicalite-1 (S-1) zeolite via facile deposition–precipitation method. It was found that the stannic species modified all-silica zeolite catalysts were active for the intermolecular condensation of ethylenediamine (EDA) to 1, 2-Diazabicyclo [2, 2, 2] octane (TEDA) and piperazine (PIP). The best catalyst Sn6-S-1 (6 wt.% Sn loading) showed 86% EDA conversion and 93% total selectivity to TEDA and PIP. By contrast, the defective S-1 zeolite parent showed only approximately 9% EDA conversion under the same conditions. With the help of catalyst characterization techniques including hydroxyl vibration and pyridine adsorption FT-IR spectroscopy (transmission mode), the enhancement of the catalytic activity of the SnO2modified zeolite catalysts (Snx-S-1) was mainly attributed to the formation of mild Lewis acid sites in the siliceous zeolite. Both the hydroxyl nests of the defective S-1 zeolite and the dispersed SnO2clusters should be the important factors for the formation of mild Lewis acid sites on the modified zeolite. Based on the catalytic performance of the modified zeolite in the conversion of EDA to PIP and TEDA, it is inferred that the mildly acidified defective S-1 zeolite by the SnO2deposition modification might become a very active and durable catalyst for reactions involving strongly alkaline reactants and products.Keywords:defective Silicalite-1;SnO2modification;acidity;condensation of ethylenediamine
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
Polymers
·
2020
·Vol. 12
·期 3
·521
·
IF 3.426
Lei Han,Haifeng Cai,Xu Chen,Cheng Zheng,Weihong Guo
Ultra-high molecular weight polyethylene (UHMWPE)/epoxy composites with excellent adhesive properties were prepared by forming an interface membrane on the UHMWPE fiber surface. The interface membrane of the UHMWPE fiber and epoxy resin was polymerized by an aldol condensation between polyvinyl alcohol (PVA) and glutaraldehyde. Different surface treatment methods of UHMWPE fibers were optimized and the two-step PVA-glutaraldehyde condensation (Corona-PG-2S) method is the best. The interfacial adhesion between UHMWPE fiber and epoxy resin was enhanced, and the adhesive properties of the composite were improved. X-ray photoelectron spectroscopy (XPS) and energy dispersive spectrum (EDS) results of the fiber treated by Corona-PG-2S shows that the surface oxygen content was up to 25.0 wt %, with an increase of 17.3 wt % compared with the surface oxygen content of unmodified UHMWPE fiber, which indicated that the surface polarity was greatly enhanced. The adhesive properties were improved by improving the polarity of the surface. The peel strength, ultimate cohesive force, tensile strength and flexural strength of the composite treated by Corona-PG-2S were greatly increased to 262.8%, 166.9%, 139.7%, 200.6% compared with those of unmodified samples. The composite prepared by Corona-PG-2S had excellent adhesive properties, demonstrating that the Corona-PG-2S method plays a major role in significantly improving the composite adhesive properties.Keywords:UHMWPE fiber;epoxy resin;PVA;adhesive property;aldol condensation
研究领域:
材料科学
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复合材料
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产品关联
DOI
PubMed
高影响因子
FIBERS AND POLYMERS
·
2018
·Vol. 19
·期 8
·1611-1617
·
IF 1.353
Wang Cuie,Wang Ning,Liu Xinhua,Wan Peng,He Xinwei,Shang Yongjia
We propose a green synthesis of benzopyran compound based on immobilized lipase. Firstly, by using a combined electrospun membrane and biocompatible chitosan, we show that the chitosan-functionalized electrospun PMA-co-PAA fibrous membrane can provide effective anchoring sites for immobilization of the Candida antarctica lipase B (CALB), and a maximum loading amount of CALB (152 mg/g) can be achieved. Then, the resulting membrane displays enhanced stability in catalyzing Knoevenagel condensation reaction of salicylaldehyde with active methylene compound in mixed aqueousorganic media. The catalytic activity and stability of the CALB on chitosan-modified fiber is better than its non-immobilized counterpart. Furthermore, this immobilize CALB catalyst still retained about 45 % of the initial activity after 5 cycles, which potentially had implications for the design of “green” enzyme catalyst for sustainable organic synthesis.
研究领域:
生物化学
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绿色化学
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材料科学
✓ 已验证
DOI
高影响因子
ENERGY & FUELS
·
2020
·
IF 3.421
Qiang Liu,Xinghua Zhang,Qi Zhang,Qiying Liu,Chenguang Wang,Longlong Ma
In this work, high-density jet fuel range cycloalkanes were synthesized in high yields (∼80%) by solvent-free aldol condensation of cyclopentanone and furfural followed by hydrodeoxygenation (HDO). Sodium-promoted magnesium–aluminum mixed oxides (Na–MgAlO) exhibited a high catalytic activity in the aldol condensation of cyclopentanone and furfural under a solvent-free condition. Furfural conversion of 99.4% with almost 100% selectivity for 2-(2-furylmethylidene) cyclopentanone and 2,5-bis(2-furylmethylidene) cyclopentanone were obtained over the 5.7%Na–MgAlO catalyst under mild conditions (80 °C, 2 h). The Na–MgAlO catalysts were characterized by multiple technologies, such as N2 physisorption, powder X-ray diffraction, Fourier transform infrared spectra, and CO2 temperature-programmed desorption, and so on. It was found that the high catalytic activity for aldol condensation of cyclopentanone and furfural was clearly related to the amount and strength of basicity of Na–MgAlO catalysts. Finally, the condensation products were converted to jet fuel range cycloalkanes by HDO over Pd/C and HZSM-5 catalysts. The density, heating value, and freezing point of the HDO liquid products were 0.83 g/cm3, 43.1 MJ/Kg, and −27.7 °C, respectively. The results suggest that these cycloalkanes are promising as blending components for jet fuel.
研究领域:
能源化学
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催化化学
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产品关联
DOI
高影响因子
ChemistryOpen
·
2021
·Vol. 10
·期 5
·560-566
·
IF 2.911
Yingshuang Hui,Yulu Zhan,Wenrong Hou,Lou Gao,Yahong Zhang,Yi Tang
Graphical The product control of C6 aldose toward C6, C4 and C2 alditols have been achieved, which have depended on the well-matched between retro-aldol condensation and hydrogenation process driving by temperature, H 2 pressure and injection modes. Alcohols have a wide range of applicability, and their functions vary with the carbon numbers. C6 and C4 alditols are alternative of sweetener, as well as significant pharmaceutical and chemical intermediates, which are mainly obtained through the fermentation of microorganism currently. Similarly, as a bulk chemical, C2 alditol plays a decisive role in chemical synthesis. However, among them, few works have been focused on the chemical production of C4 alditol yet due to its difficult accumulation. In this paper, under a static and semi-flowing procedure, we have achieved the product control during the conversion of C6 aldose toward C6 alditol, C4 alditol and C2 alditol, respectively. About C4 alditol yield of 20 % and C4 plus C6 alditols yield of 60 % are acquired in the one-pot conversion via a cascade retro-aldol condensation and hydrogenation process. Furthermore, in the semi-flowing condition, the yield of ethylene glycol is up to 73 % thanks to its low instantaneous concentration.
研究领域:
生物化学
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有机化学
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产品关联
DOI
PubMed
高影响因子
DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 21
·7119-7128
·
IF 4
Zhengguo Zhang,Hongxiao Lv,Kun Yang,Xiutang Zhang
Developing materials with excellent properties has become the norm in the field of basic research, prompting us to explore highly robust hybrid materials based on electron-rich POMs and electron-deficient MOFs. Herein, a θ-[Mo8O26]4−-based hybrid material of [Cu2(BPPP)2]{θ-[Mo8O26]} (NUC-62) with excellent physicochemical stability was self-assembled under acidic solvothermal conditions from Na2MoO4 and CuCl2 in the presence of a designed chelated ligand of 1,3-bis(3-(2-pyridyl)pyrazol-1-yl)propane (BPPP), which has sufficient coordination sites, spatial self-regulation and great deformation ability. In NUC-62, each of two tetra-coordinated CuII ions and two BPPP are unified into one dinuclear unit serving as the cation, which is interactively linked to θ-[Mo8O26]4− anions via rich hydrogen bonds of C–H⋯O. Because of the unsaturated Lewis acidic CuII sites, NUC-62 exhibits high catalytic performance on the cycloaddition reactions of CO2 with epoxides under mild conditions with a high turnover number and turnover frequency. Furthermore, NUC-62, as a recyclable heterogeneous catalyst, shows high catalytic activity for the esterification of aromatic acid under refluxing, which is much better than the inorganic acid catalyst of H2SO4 in terms of turnover number and turnover frequency. Moreover, because of open metal sites and rich terminal oxygen atoms, NUC-62 shows high catalytic activity for Knoevenagel condensation reactions of aldehydes and malononitrile. Hence, this study lays the groundwork for constructing heterometallic cluster-based microporous MOFs with excellent Lewis acidic catalysis and chemical stability. Therefore, this study lays a foundation for the construction of functional polyoxometalate complexes.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CATALYSIS LETTERS
·
2021
·Vol. 152
·期 4
·1215-1223
·
IF 3.186
Wang Yun,Cheng Hong,He Jia-Rui,Yao Qiao-Xia,Li Li-Ling,Liang Zhi-Hui,Li Xiang
The Knoevenagel condensation of acetylacetone and aromatic aldehyde catalyzed by lipase from porcine pancreas(PPL) and α-amylase from hog pancreas in ionic liquids and deep eutectic solvents was achieved for the first time. The highest yields is up to 96.1%. Mild reaction conditions, enhanced rates, improved yields and reagents’ reactivity which is different from that in standard organic solvents are the remarkable features observed in ionic liquids and deep eutectic solvents. Graphical Abstract
研究领域:
生物化学
·
有机化学
✓ 已验证
DOI
高影响因子
Chemical Science
·
2025
·
IF 7.4
Yue-Wen Zhou,Ming-Yang Jia,Jun-Lei Yang,Qinlei Liu,Zhenfeng Cai
The influence of electric fields (EFs) on chemical reactions has attracted significant interest due to their ability to modulate reaction rates, pathways, and selectivity. Although EFs have been experimentally demonstrated to facilitate various reactions, clearer evidence for their role in covalent condensation has remained limited. Herein, we provide experimental evidence of electric-field-induced covalent condensation of boronic acids, utilizing the strong EFs at the air-liquid interface of microdroplets to induce the reaction. Microdroplet-based chemistry provides interfacial electric field intensities as high as ca. 109 V/m, offering a robust platform for the systematic investigation of boronate linkage formation and subsequent condensation of boronic acids. Our results confirm the role of EFs in facilitating room-temperature condensation of boronic acids, providing direct insights into the electric-field-induced polymerization process and presenting an experimental approach for investigating these processes in solution.
研究领域:
化学
·
材料科学
✓ 已验证
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）