Applications in Energy and Combustion Science
·
2021
·
IF 0
Huiyan Zhang,Bingbing Luo,Kai Wu,Han Wu,Jiajun Yu,Siyu Wang
Catalytic fast pyrolysis of lignin is easy to cause agglomeration and coking, resulting in low-yield aromatic hydrocarbons. Catalytic pyrolysis of modified lignin combined with metal-modified HZSM-5 was proposed to enhance the aromatic yield. The experiment results showed that chemical modification with Ca(OH) 2 not only inhibited the agglomeration behavior of lignin but also increased the yield of light phenolic compounds. Moreover, Ca 2+ -loaded lignin combined with metal-modified HZSM-5 was conducive to the formation of aromatics. The total yield of aromatics from the catalytic fast pyrolysis of Ca 2+ -loaded lignin over Zn/HZSM-5 was improved from 31.1 to 46.1 mg/g. The mechanism insight showed that Ca 2+ modification realized the chemical combination between Ca 2+ and the functional groups which are responsible for the agglomeration of lignin, and then the introduction of the Zn species suppressed the hydrogen transfer reaction and enhanced the dehydrogenation pathway, resulting in the increase of aromatic yield.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Yu-Xuan Dai,Wen-Li Xin,Lian-Hua Xu,Ji Li,Yi-Xuan Li,Junji Li,Serge Cosnier,Xue-Ji Zhang,Robert S. Marks,Dan Shan
Rational design highly active transition metal or transition metal oxides/nanocarbon hybrids is one of the feasible way to deliver a cooperative oxygen reduction (ORR) with a synergistic effect of the hybrid interface. Herein, based on benzimidazole-5-carboxylate (BIMC), CoO/Co-N-C nanocomposites are fabricated via 2-methylimidazole (2-MeIm)-tuned “4-Self” strategy, namely, self-templating, self-adapting, self-assembly and self-catalysis. As a base competitive ligand with N and C sources, 2-MeIm modulates the dispersion of BIMC in methanol to generate collodial-like BIMC tiny particles, the coordination ability of BIMC to Co(II), the composition and morphology of the self-assembled precursor (Co-BM), and as well as the conductivity of the resultant electrocatalyst. Impressing, carbonization of Co-BM at 800 °C under N 2 atmosphere endows the pyrolysis product (Co-BM-800) with the well-dispersed Co/CoO riveted on nitrogen-doped carbon, as well as the enhanced ORR performance in terms of positive onset-potential (0.890 V vs. RHE), large diffusion limiting current density (5.21 mA cm −2 ), and high stability.
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高影响因子
Bioresource Technology Reports
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2022
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IF 0
Jiali Mi,Simin Liu,Yan Du,Haishan Qi,Lei Zhang
Cadaverine (1,5-diaminopentane) has widespread applications in industry, agriculture and medicine. Cadaverine can be biotransformed from l -lysine by lysine decarboxylasey which is a pyridoxal 5′-phosphate (PLP)-dependent enzyme. Herein, barium alginate microspheres were fabricated by electro-dripping and employed as immobilized metal ion affinity chromatography matrix to purify and immobilize engineered lysine decarboxylase CadA-EK. Besides, polyethyleneimine (PEI) was employed for co-immobilizing PLP and enzymes (cCadA-EK-PEI/PLP). The cCadA-EK-PEI/PLP can produced 184.53 g/L cadaverine with yield of 90.03% in 2 mol/L lysine solution. And the stability of co-immobilized CadA-EK was 1–4 times higher than that of iCadA-EK + PLP in environmental factors, and the catalytic efficiency k cat / K m was increased by 3.4-fold. Furthermore, a continuous flow microreactor with the co-immobilized enzymes and cofactors was developed to catalyze lysine, with 14.28 g/(L·h) productivity of cadaverine, which displayed great potential for cadaverine biosynthesis. This work provides alternative strategy for the one-step purification and co-immobilization of enzyme and cofactor.
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ChemCatChem
·
2016
·Vol. 8
·期 23
·3636-3643
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IF 4.724
Zhenyou Gui,Wenrong Cao,Shunmugavel Saravanamurugan,Anders Riisager,Lifang Chen,Zhiwen Qi
Graphical Efficient noble alloy : Au–Pd supported on zinc hydroxycarbonate (ZOC) catalysts shows high activity for 5-hydroxymethylfurfural oxidation. The basicity of ZOC can play a crucial role in enhancing the yield of FDCA. Moreover, Au–Pd/ZOC can be recycled at least six times without significant loss of its activity. Bimetallic catalysts with Au–Pd supported on zinc hydroxycarbonate (ZOC) were synthesized by a simple deposition–precipitation method and analyzed by transmission electron microscopy to have a narrow-size distribution of predominantly 1–2 nm. The prepared Au–Pd/ZOC catalysts exhibited excellent activity towards 5-hydoxymethylfurfural (HMF) oxidation in water in the presence of the base NaHCO 3 at benign conditions of 80 °C and 3 bar O 2 , resulting in quantitative yield of 2,5-furandicarboxylic acid (FDCA). The addition of base not only enhanced the yield of FDCA but also stabilized the support ZOC by preventing ZOC from the reaction with formed carboxylic acid intermediates/products, thus allowing Au–Pd/ZOC to be recycled for at least six times without significant loss of activity. The basicity of ZOC could play an important role in obtaining the improved yield of FDCA as compared to other supports.
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CATALYSIS LETTERS
·
2022
·Vol. 153
·期 6
·1743-1755
·
IF 2.936
Zhou Yi,Yao Tiantian,Tan Yawen,Chen Yongbo,Chen Zhiyue,Zhang Jin
In this study, a novel composite DUT-5/Bi 2 MoO 6 (DUT-5/BMO) photocatalytic material was prepared by two-step hydrothermal method for the first time. The materials were characterized by SEM, XPS, etc. Studies have shown that material with a new n–n heterojunction structure can quickly degrade tetracycline. DUT-5 was embedded between the Bi 2 MoO 6 nanosheets, which promotes the photogenerated electrons from DUT-5 flows to Bi 2 MoO 6 , thereby reducing the recombination rate of photo-generated electron–hole pairs. The BET results show that the composite material has a larger specific surface area than the monomer Bi 2 MoO 6 . It can provide more active sites. After 60 min of visible light irradiation, the photocatalytic degradation efficiency of TC with 15% DUT-5/BMO reached 84.22%, which is 5.37 and 2.12 times higher than that of pure DUT-5 and Bi 2 MoO 6 , ·O 2 − and h + were the main active substances in the photocatalysis process. In addition, DUT-5/BMO composites show excellent stability and recyclability in 5 times cyclic experiments. In conclusion, DUT-5/BMO has good stability in the environment, and can be used for environmental remediation without pollution. Graphical
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2023
·
IF 4.2
Xuemin Cao,Kun Zhang,Yu Wang,Peng He
The carbonylation of formaldehyde offers a promising, cost-effective, and environmentally friendly method for synthesizing glycolic acid, a crucial monomer in biodegradable plastics. This study highlights the development and optimization of a bifunctional PdO/ZSM-5 zeolite catalyst for this process. Investigations via various spectroscopic techniques reveal that Pd species, predominantly in the form of PdO, enhance the CO activation, thereby boosting the formaldehyde carbonylation reaction rate significantly. The optimal catalytic performance was observed with a Pd-loading of 2 wt %. Notably, excessive Pd loading was found to impede the catalytic performance by overoccupying acid sites, thereby reducing its capacity to activate formaldehyde. The concurrent activation of formaldehyde and CO at the Brønsted acid site and the PdO site, respectively, through a Langmuir–Hinshelwood mechanism is key to the enhanced catalytic performance. These findings underscore the importance of CO activation in improving the formaldehyde carbonylation process, offering vital insights for catalyst optimization.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Yi Yang,Yuxi Si,Libin Liu,Hairui Lin,Chuan Qin,Dangguo Cheng,Youwei Cheng
The chemical conversion of 5-hydroxymethylfurfural (HMF) into high-value-added products offers a potential substitute for fossil-based products, which has garnered significant attention in light of energy depletion and environmental concerns. Among the various HMF derivatives, 2,5-bis(hydroxymethyl)furan (BHMF), applicable in polyester manufacturing, pharmaceutical intermediates, biodiesel, and other sectors, can be synthesized through the C═O hydrogenation of HMF. However, the inevitable humins formation and the over-hydrogenation/hydrogenolysis constrain the further application of this process. In this study, a series of hydroxyl-enriched Pt-based catalysts have been prepared and applied in the hydrogenation of HMF. For 1% Pt/CeO2, the selectivity for BHMF over 85% can be consistently maintained at 30 °C or at a substrate concentration of 100 g/L. Experiments and characterization studies indicate that hydroxyl groups presented on the catalyst surface could protect BHMF, inhibiting side reactions and thereby increasing carbon balance and main product selectivity. This superior selective catalytic performance was further demonstrated in the C═O hydrogenation over various aromatic aldehyde substrates, providing a novel approach for biomass compounds conversion to value-added chemicals and providing a perspective for catalyst design.
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CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Kairui Zhang,Qiong Tang,Lei Liu,Jinxiang Dong
The alkylation reaction of benzene with n- butene can not only significantly improve the utilization rate of n- butene, but also solve the shortage problem of phenol and methyl ethyl ketone, and alleviate the surplus problem of acetone. This study demonstrates a strategic approach to engineering hierarchical ZSM-5 zeolites with controlled aluminum distributions for enhanced benzene-butene alkylation catalysis. Through aluminum precursor selection (aluminum isopropoxide, sulfate, and sodium aluminate) coupled with resin-templated synthesis, the framework Al speciation and mesopore architecture in ZSM-5 could be regulated. Advanced characterization revealed that aluminum source chemistry governs Brønsted/Lewis acid ratios, Al spatial positioning (sinusoidal/straight channels), and mesopore volume. The synthetic hierarchical ZSM-5 zeolites exhibited significant difference in catalytic performance toward benzene-butene alkylation, the Al atoms in HZ5-AIP zeolite with the largest pore size mainly in straight and sinusoidal channels, achieving 99 % conversion of n -butene (210 °C, 3 MPa, benzene/butene molar ratio = 5:1, WHSV Bu = 6 h −1 ).
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Microbial Cell Factories
·
2025
·Vol. 24
·期 1
·1-11
·
IF 4.9
Liu Wen,Guo Jing,Lu Wei,Cheng Tao,Li Yiting,Xian Mo,Zhang Rubing
Background L -5-Methyltetrahydrofolate (5-MTHF) is the sole biologically active form of folate present in human blood and serves as an essential nutritional supplement. While microbial biosynthesis of 5-MTHF offers a sustainable alternative to chemical synthesis, its low yield limits industrial potential. Results In this study, strategies for improving the methyl supply combined with engineering the tetrahydrofolate (THF) synthetic pathway were employed in E. coli to increase 5-MTHF production. First, a new exogenous C1 pathway was introduced to improve the intracellular methyl supply through acetyl-CoA breakdown. High expression of key rate-limiting genes folE , folP and purU enhanced metabolic flux of THF pathway, resulting in a 5-MTHF titer of 1.075 mg/L during shake-flask fermentation. A subsequent increase in 5-MTHF production was achieved by knocking out the metE gene, which is involved in the consumption of 5-MTHF. The best engineered strain, M3012, produced 8.2 mg/L 5-MTHF in a 5 L bioreactor via fed-batch fermentation, which presented the highest 5-MTHF titer to date. Conclusion We successfully engineered E. coli by introducing a novel exogenous C1 metabolic pathway to augment the methyl donor pool essential for the biosynthesis of 5-MTHF. Further metabolic optimizations, including the enhancement of the THF precursor flux and the elimination of competing degradation pathways, developed a recombinant strain with significantly increased yield, which paves the way for industrial production of 5-MTHF.
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PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Yixuan Wang,Shijia Fu,Yao Zeng,Siwen Jiao,Guihong Chai,Yuehong Xu
5-aminolevulinic acid photodynamic therapy (ALA-PDT) is an emerging therapeutic strategy for skin cancer due to its noninvasiveness and high spatiotemporal selectivity. However, poor skin penetration, poor intratumoral delivery, the instability of aqueous ALA, and the tumor’s inherent hypoxia microenvironment are major hurdles hindering the efficacy of ALA-PDT. Herein, we aim to address these challenges by using microneedles (MNs) to assist in delivering nanoparticles based on natural polymeric tea polyphenols (TP NPs) to self-assemble and load ALA (ALA@TP NPs). The TP NPs specifically increase cellular uptake of ALA by A375 and A431 cells and reduce mitochondrial membrane potential. Subsequently, the photosensitizer protoporphyrin IX derived from ALA accumulates in the tumor cells in a dose-dependent manner with TP NPs, generating reactive oxygen species to promote apoptosis and necrosis of A375 and A431 cells. Interestingly, TP NPs can ameliorate the tumor’s inherent hypoxia microenvironment and rapid oxygen consumption during PDT by inhibiting hypoxia inducible factor-1α, thereby boosting reactive oxygen species (ROS) generation and enhancing ALA-PDT efficacy through a positive feedback loop. After ALA@TP NPs are loaded into MNs to fabricate ALA@TP NPs@MNs, the MNs enhance skin penetration and storage stability of ALA. Importantly, they exhibit remarkable antitumor efficacy in A375-induced melanoma and A431-induced squamous cell carcinoma with a reduced dose of ALA and reverse hypoxia in vivo . This study provides a facile and novel strategy that integrates MNs and green NPs of TP for addressing the bottlenecks of ALA-PDT and enhancing the ALA-PDT efficacy against skin cancers for future clinical translation.
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PubMed
高影响因子
LANGMUIR
·
2024
·
IF 3.7
Yiheng Wu,Yangping Lv,Ruipu Wang,Lixia Bao,Zhongdong Zhang,Dejun Shi,Anlv Zhang,Yaoyuan Zhang,Qi Liu,Qin Wu,Daxin Shi,Kangcheng Chen,Guiyuan Jiang,Hansheng Li
The aromatization of light alkane is an important process for increasing the aromatic production and utilization efficiency of light alkane resources simultaneously. Herein, Ga-modified HZSM-5 catalysts were prepared and investigated by a series of characterization techniques such as X-ray diffraction, nuclear magnetic resonance spectroscopy, transmission electron microscopy, N2 adsorption–desorption, and NH3 temperature-programmed desorption to study their physicochemical properties. The catalytic performance in propane aromatization was also tested. Importantly, the structure–activity relationship, reaction pathway, and coke formation mechanism in propane aromatization were systematically explored. It was found that different Ga introduction methods would affect the amounts of Brønsted and Lewis acid sites, and Ga-HZSM-5 prepared by the hydrothermal method exhibited higher amounts of Brønsted and Lewis acid sites but a lower B/L ratio. As a result, Ga-HZSM-5 showed higher propane conversion and benzene, toluene, and xylene yield compared with that of Ga2O3/HZSM-5. The propane aromatization reaction pathway indicated that propane dehydrogenation to propene was a crucial step for aromatic formation. The increase of the Lewis acid density in Ga-HZSM-5 can effectively improve the dehydrogenation rate and promote the aromatization reaction. Furthermore, the formation of coke species was studied by thermogravimetry–mass spectrometry and Raman approaches, the results of which indicated that the graphitization degree of coke formed over spent Ga-HZSM-5 is lower, resulting in enhanced anticoking stability.
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PubMed
高影响因子
CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Yiyuan Peng,Mengbiao Liang,Ting Chen,Mengdi Zhao,Zhixiang Xie,Chunxian Guo
All-inorganic perovskite nanocrystals (CsPbX 3 NCs, X = Cl, Br, I) have emerged as promising candidates for applications in light-emitting diodes (LEDs), solar cells, photodetectors, and backlight displays, owing to their exceptional optoelectronic properties, including high photoluminescence quantum yield (PLQY), long carrier lifetimes, and narrow emission bandwidths. However, the intrinsic ionic nature of these nanocrystals renders them highly susceptible to environmental degradation, limiting their practical applications. Herein, we report the synthesis of CsPbBr 3 @MOF-5 composites through a physical mixing method: room-temperature supersaturated recrystallization of CsPbBr 3 NCs, followed by encapsulation within a hierarchical porous zinc-based metal-organic framework (MOF-5). By incorporating poly(ethylene oxide)-block-poly(propyleneoxide)-block-poly(ethylene oxide) Pluronic (P123) and 1,3,5-trimethylbenzene (TMB) as structure-directing agents, the pore architecture of MOF-5 was tailored to exhibit hierarchical porosity (2-35 nm), significantly enhancing both the PLQY and stability of CsPbBr 3 NCs. The CsPbBr 3 @MOF-5 composites achieved a remarkable PLQY improvement from 22% to 56%, retained 55% of their initial PL intensity after 60 days of ambient storage, and maintained 65% of PL emission under thermal stress (298-498 K). In contrast, pristine CsPbBr 3 NCs experienced complete quenching under identical conditions. Additionally, the composite exhibited superior resistance to anion exchange when combined with CsPbBr x I 3-x NCs. A white LED (WLED) device fabricated using CsPbBr 3 @MOF-5 composite and K 2 SiF 6 :Mn 2+ (KSF) red phosphor exhibited a luminous efficiency of 20.71 lm/W, a correlated color temperature (CCT) of 5486 K, and a broad color gamut covering 133.3% of the National Television Standards Committee (NTSC) standard, underscoring its potential for advanced lighting and display technologies.
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