COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Libo Sun,Qingtai Xie,Heshun Jing,Jindong Xie,Wenyu Tan,Baorong Duan,Xun Sun,Caixia Qi,Huijuan Su
The development of nanogold catalysts with high activity and high stability is of great significance for their industrial applications. In this paper, Au-PDA@Fe 3 O 4 catalysts were prepared through the gold sol adsorption method. First, micron-sized magnetic Fe 3 O 4 spheres were synthesized via a solvothermal method, serving as the core to endow the catalyst with excellent recyclability. Subsequently, a layer of polydopamine (PDA) shell was polymerized on the magnetic core surface. By controlling the timing of introducing the gold sol containing Au nanoparticles (NPs), the spatial position of Au NPs within the PDA layer was regulated, leading to a series of magnetic core-shell nano gold catalysts with varying spatial positions of Au. Using the 4-nitrophenol (4-NP) hydrogenation as the probe, the influence of Au spatial position, Au size, and other conditions on the catalytic performance was investigated. Results showed that, in the prepared Au-PDA@Fe 3 O 4 -16 catalyst, the Au NPs are encapsulated within the PDA shell and positioned close to the outer layer. This not only provides remarkable stability to the Au NPs but also maintains their proximity to the surface of the PDA shell, allowing easier access of the substrate 4-NP to the Au NPs and conferring good reactivity upon the catalyst. The strong electron metal-support interaction between PDA and Au enables PDA to effectively stabilize Au NPs. The prepared Au-PDA@Fe 3 O 4 -16 catalyst exhibits excellent stability, maintaining a high conversion rate of 91 % even after 14 cycles of use. Our findings not only deepen the understanding of the catalytic mechanisms involved but also pave the path towards the creation of highly efficient and robust gold-based catalysts, facilitating their widespread utilization in industrial applications.
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ARCHIVES OF BIOCHEMISTRY AND BIOPHYSICS
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2014
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IF 3.043
Chenxi Ning,Erzheng Su,Dongzhi Wei
Lodderomyces elongisporus LH703 isolated from soil samples contained three novel aldo–keto reductases (AKRs) (LEAKR 48, LEAKR 49, and LEAKR 50). The three enzymes were cloned, expressed, and purified to homogeneity for characterization. These three AKRs shared <40% amino acid identity with each other. LEAKR 50 was identified as a member of AKR3 family, whereas the other two LEAKRs were identified as members of two novel AKR families, respectively. All the three AKRs required nicotinamide adenine dinucleotide phosphate as a cofactor. However, they showed diverse characteristics, including optimum catalyzing conditions, resistance to adverse reaction conditions, and substrate specificity. LEAKR 50 was estimated to be a promising biocatalyst that could reduce ethyl 4-chloroacetoacetate with high enantiomeric excess (98% e. e.) and high activity residue under adverse conditions.
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Advanced Science
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2024
·
IF 14.3
Kang Chen,Keyuan Pan,Shang He,Rui Liu,Zhe Zhou,Duoyi Zhu,Zhengdong Liu,Zixi He,Hongchao Sun,Min Wang,Kaili Wang,Minghua Tang,Juqing Liu
Ionic memristors can emulate brain-like functions of biological synapses for neuromorphic technologies. Apart from the widely studied excitatory-excitatory and excitatory-inhibitory synapses, reports on memristors with the inhibitory-inhibitory synaptic behaviors remain a challenge. Here, the first biaxially inhibited artificial synapse is demonstrated, consisting of a solid electrolyte and conjugated microporous polymers bilayer as neurotransmitter, with the former serving as an ion reservoir and the latter acting as a confined transport. Due to the migration, trapping, and de-trapping of ions within the nanoslits, the device poses inhibitory synaptic plasticity under both positive and negative stimuli. Remarkably, the artificial synapse is able to maintain a low level of stable nonvolatile memory over a long period of time (≈60 min) after multiple stimuli, with feature-inferencing/-training capabilities of neural node in neuromorphic computing. This work paves a reliable strategy for constructing nanochannel ionic memristive materials toward fully inhibitory synaptic devices.
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CERAMICS INTERNATIONAL
·
2025
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IF 5.6
Shuaiqian Wang,Baoji Miao,Muhammad Shahid Nadeem,Huaizhi He,Yao Zhao,Muhammad Yasir,Qiuling Chen,Guoqin Liu,Jinbo Bai
This study successfully prepared a novel high-entropy MAX phase (Ti 1/4 V 1/4 Zr 1/4 Nb 1/4 ) 2 AlC and conducted a comprehensive investigation of its microwave absorption performance. The material was synthesized using a pressure less sintering method, and by optimizing the selection of raw materials and synthesis processes, high purity, and excellent microwave absorption performance were achieved. The composition, structure, morphology, and electromagnetic parameters of the material were analyzed in detail using characterization methods such as XRD, SEM, EDS, TEM, XPS, and vector network analyzer (VNA). Experimental results exhibit that (Ti 1/4 V 1/4 Zr 1/4 Nb 1/4 ) 2 AlC can achieve a lowest RL of -62.56 dB at a thickness of 2.25 mm with frequency of 13.26 GHz, demonstrating outstanding microwave absorption capabilities. The study also explored the microwave absorption mechanisms of grown material, including conductivity, dipole polarization relaxation processes, internal lattice defects, and magnetic loss. This research not only delivers new approaches and development of effective microwave absorption materials but also lays the foundation for subsequent studies on MXene and more multi-element high-entropy MAX phase materials.
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FUEL
·
2024
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IF 6.7
Fa-Peng Wu,Le-Le Qiu,Yun-Peng Zhao,Zong-Pin Fu,Jing Liang,Jian Xiao,Jian Li,Fang-Jing Liu,Jing-Pei Cao
Hydrogenolysis of β-O-4 linkages in lignin to produce aromatic compounds is attractive but challenging. Currently, external hydrogen source like hydrogen gas or hydrogen-donor solvent is necessary during hydrogenolysis, leading to high cost and low selectivity of products. Herein, a NiCu/Al 2 O 3 catalyst was prepared for self-hydrogen transfer hydrogenolysis (SHTH) of C β -O bond using inherent C α H-OH structure as H-source. A β-O-4 model compound, 2-phenoxy-1-phenethanol, was completely transformed into acetophenone and phenol at 220 ℃ under 1 MPa N 2 for 2h. The SHTH reaction proceeded through a dehydrogenation reaction followed by a hydrogenolysis reaction. Hydrogen radicals released from C α H-OH group generated a “hydrogen pool” on the catalyst surface, which inserted into the formed β-O-4 ketone intermediate to cleave the C β -O bond. The catalyst presented outstanding reusability and universality during the SHTH reaction. Moreover, the methoxy groups at aryl positions impeded the SHTH process, and the steric effect was related to the amount and position of methoxy groups. This study realizes the utilization of structural hydrogen from lignin model compounds for its C β -O bond cleavage , providing an economical and sustainable method toward lignin valorization.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2024
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IF 5.8
Shuang Wang,Huihui Zhang,Chunyan Yu,Yue Liu,Yanju Lu,Lu Li
In this study, Co-Corrin/C catalysts with corrin active skeleton were prepared by pyrolysis under anaerobic conditions using vitamin B12 (VB12) as a precursor and activated carbon with rich mesoporous structure as a carrier. The Co-Corrin/C catalyst was applied to the oxidative cleavage reaction of lignin, showing a 92.74 % breakage of β-O-4 bonds. Density functional theory (DFT) calculations indicate that the low energy gap difference of Co-Corrin/C promotes electron transfer between Co and O. Meanwhile, the pyrrole ring in the corrin structure will be adsorbed and bonded to oxygen, which promotes the generation of large amounts of oxygen free radicals. The C α -OH bond in the lignin aliphatic chain is oxidized to C α =O bond under the action of oxygen radicals, which reduces the dissociation energy of the β-O-4 bond and significantly improves the oxidation efficiency. Cycling experiments proved that Co-Corrin/C has good stability.
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CHEMISTRY & BIODIVERSITY
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2024
·Vol. 21
·期 7
·e202400929
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IF 2.3
Yuee Tian,Shiyue Ma,Yibo Liu,Yan Li,Genqiang Chen,Zhiping Che
In order to explore novel natural product-based insecticidal agent, two important intermediates ( 2 and 3 ) and 4-acyloxy-2′-bromo-6′-chloropodophyllotoxin derivatives ( 4 a – f and 5 a – f ) were designed and prepared, and their structures were confirmed by 1 H-NMR, 13 C NMR, HRMS, ESI-MS, optical rotation and melting point (mp). The stereochemical configuration of compound 4 b was unambiguously confirmed by single-crystal X-ray diffraction. Moreover, we evaluated the insecticidal activity of target compounds 4 a – f and 5 a – f against a serious agricultural pest of Mythimna separata by using the leaf-dipping method. Among all tested compounds, compounds 4 d , 5 d and 5 f exhibited stronger insecticidal activity with a final mortality rate exceeding 60 %. Especially compound 5 d exhibited the best insecticidal activity, with a final mortality rate of 74.1 %. It has been proven that introducing bromine or chlorine atoms at the C-2′, C-2′ and C-6′ positions of the E ring of podophyllotoxin can produce more potent compounds. In addition, the configuration of the C-4 position is important for insecticidal activity, and 4β-configuration is optimal. This will pave the way for further design, structural modification, and development of derivatives of podophyllotoxin as insecticidal agents. Graphical
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DALTON TRANSACTIONS
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2024
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IF 3.5
Xiaoyu Chu,Xinrui Wang,Shuo Tian,Yongkuo Zhao,Shikai Liu,Hong Yan,Yan Shang
Modulating the photogenerated electrons of CeO2 to activate O2 and efficiently photocatalytic degradation of chlorophenols is a highly desired goal. Herein, we have successfully fabricated FePc/CeO2 heterojunction through H-bond induced assembly. The photocatalytic degradation of 2, 4-DCP by the amount-optimized FePc/CeO2 nanocomposite was improved by 3 times compared with pure CeO2. By means of electron paramagnetic resonance (EPR) and single wavelength photocurrent spectroscopy, it is confirmed that the excellent photocatalytic performance is mainly attributed to the formation of Z-scheme heterojunction, which promotes charge separation and transfer, and the introduction of FePc broadens the visible light absorption range of heterojunction. Moreover, O2 temperature-programmed-desorbed curves and electrochemical O2 reduction measurements results demonstrate that the single Fe-N4(II) site in FePc is more conducive to promoting O2 activation than that of other metal phthalocyanines. Based on in situ FT-IR and liquid chromatography-tandem mass spectrometry (LC-MS), a possible reaction pathway of 2, 4-DCP degradation was proposed. This study provides a novel strategy to prepare CeO2 based Z-scheme heterojunctions with abundant monoatomic sites for pollutant degradation.
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PLANT CELL AND ENVIRONMENT
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2025
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IF 6.3
Hongcheng Zhao,Jiarui Xu,Lin Huang,Yizhe Ding,Xianyong Lin,Chengliang Sun
Beneficial microbiomes significantly modulate root hair morphogenesis, yet the underlying signalling pathways remain unclear. Through comprehensive phenotypic analysis, we demonstrated that Azospirillum brasilense , a well-known plant-growth-promoting rhizobacteria (PGPR), promotes root hair development by prolonging the elongation period. The promotion of root hair growth by A. brasilense is attributed to increased auxin accumulation in root apices and enhanced shootward transport from the root tip, which is mediated by the accumulation of the auxin importer auxin transporter protein 1 (AUX1) in the lateral root cap and the overlying epidermis. Chemical or genetic disruption of auxin signalling abolished bacteria-induced root hair responses. Furthermore, A. brasilense upregulated several root hair-related basic helix-loop-helix family transcription factors, including root hair defective 6 (RHD6) and RHD6-LIKE 1 (RSL1), which control root hair development through RSL4. Morphological analysis revealed that while the rsl2rsl4 double mutant remained hairless after inoculation, A. brasilense successfully rescued root hair growth in rhd6rsl1 . These findings suggest that A. brasilense can bypass RHD6 to activate RSL4, which then drives root hair development dependent on ROS. Collectively, our study uncovers the core signalling components modulated by A. brasilense to fine-tune root hair responses.
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ENVIRONMENTAL RESEARCH
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2025
·
IF 7.7
Liang Zeng,Qilin Wang,Xinyi Lou,Chang Peng,Ruoxi Wu,Shu Chen
Responsive catalysts with self-healing response capabilities will have great potential in sustainable catalytic applications, effectively extending the lifespan of catalysts. Herein, a near-infrared-responsive self-repairing composite gel catalyst is presented for efficient and sustainable reduction of 4-nitrophenol (4-NP, i.e., a specific organic pollutant). Copper nanoparticles (CuNPs) serve as catalytic species, while transition metal carbide (Ti 3 C 2 T x ) acts as efficient electron transfer medium in the composite gel. The synergistic effect of these components significantly enhances catalytic activity of the gel (e.g., the catalytic rate constant k for 4-NP reduction reaches up to 0.6159 min −1 ). More importantly, by leveraging the self-healing of poly(N, N-dimethylacrylamide) (PDMAA, i.e., the third component in the gel) and combining the photothermal conversion of Ti 3 C 2 T x , the gel is endowed with the ability to rapidly repair itself by near-infrared light induction, thereby ensuring its sustainability in the catalytic application. This photo-induction way not only effectively repairs the damaged gel catalyst but also preserves its catalytic efficiency, making it ideal for prolonged application. This research offers novel insights into using responsive catalysts to achieve sustainable and efficient catalytic application.
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INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Jing Cao,Kejun Chen,Fangmei Teng,Jialing Liu,Xinyi Liu,Cen Zhang
Maximizing the exposure of edge sites and achieving sufficient promotion remain arduous tasks for designing efficient bimetallic MoS2-based catalysts. Herein, ultrathin CoMoS nanosheets vertically grown on reduced graphene oxide (CoMoS/rGO–DMF) were fabricated by a facile one-pot solvothermal method using dimethylformamide (DMF) as solvent. The vertically aligned structure and good Co promotion endow CoMoS/rGO–DMF with abundant Co–Mo–S active sites and excellent catalytic performance in the hydrodeoxygenation (HDO) reaction. Consequently, CoMoS/rGO–DMF afforded a conversion of 98.2% and a toluene selectivity of 98.8% at 240 °C, 3.0 MPa, and 4 h in the HDO of 4-methylphenol. In addition, CoMoS/rGO–DMF showed a 3-fold larger turnover frequency value than that of CoMoS/rGO–DW prepared in deionized water. The reusability test of CoMoS/rGO–DMF showed a slight activity loss after six catalytic cycles, which resulted from the surface oxidation by water product, but the HDO performance of the spent catalyst can be easily regenerated by a simple sulfidation process. This work provides new insights for the rational design of sulfide catalysts with excellent HDO activity and arene selectivity.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
·
IF 7.7
Hongxi Zhang,Zhongke Li,Xiande Yang,Meng Li,Liang Wei,Jing Yang
Lignin is anticipated to serve as a replacement for dwindling fossil fuel resources owing to its abundant sources and renewable nature. The electrochemical oxidation technique for depolymerizing lignin has garnered significant interest for its environmentally friendly and mild operating conditions. Nevertheless, the current utilization of auxiliary electrolytes, predominantly organic bases, ionic liquids, and other specialized substances, poses a constraint on the widespread adoption of this approach. Furthermore, there is a scarcity of instances where electrochemical technology has been employed to depolymerize the α-O-4 bond in lignin for the production of highly selective acetals. In this study, a sodium chloride/methanol (NaCl/MeOH) system was utilized for the direct depolymerization of the α-O-4 bond in a lignin model molecule, specifically benzyl phenyl ether (BPE). The optimal conditions resulted in a 95.2 % conversion rate of the BPE substrate and a high yield of 94.5 % for the main product, benzaldehyde dimethyl acetal(Bda). This research offers a promising approach for the electrocatalytic depolymerization of α-O-4 bonds in lignin, leading to the selective production of acetal chemicals using a common auxiliary electrolyte at room temperature in just 2 h.
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