Nano Research
·
2016
·Vol. 9
·期 12
·3683-3694
·
IF 8.893
Deng Jun,Zheng Honghao,Zheng Xiaowen,Yao Mengyun,Li Zheng,Gao Changyou
Chirality is one of the most distinctive biochemical signatures of life, and plays crucial roles in maintaining normal functions of living cells or organisms. Pioneering work from another group has demonstrated the dependency of cell differentiation on the chirality of nano-coated substrates, but the effect of the chiral surface of nanoparticles on stem cell fates has not been investigated. In this study, the influence of molecular chiral poly(acryloyl-L(D)-valine) (L(D)- PAV)-anchored gold nanoparticles (L(D)-PAV-AuNPs) on the differentiation of mesenchymal stem cells (MSCs) was investigated. Though osteogenic differentiation of MSCs was not affected by D-PAV-AuNPs, it was significantly promoted by L-PAV-AuNPs in terms of calcium deposition, alkaline phosphatase (ALP) activity, and expression of collagen type I and osteocalcin (OCN) at both mRNA and protein levels. L-PAV-AuNPs could activate the P38 mitogen-activated protein kinase (MAPK) pathway, and may exert mechanical stress on MSCs because of high amounts of internalization. These results provide new insights on surface chirality at the nanoscale as a direct regulator to guide the differentiation of MSCs, and the use of these nanomaterials for strategic regenerative medicine.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Xinyi Li,Jingjing Liu,Qinghai Cai,Ziwang Kan,Song Liu,Jingxiang Zhao
Modulating the microenvironment of single-metal active sites holds excellent promises for developing highly efficiently oxygen electrocatalysts. Herein, by combining theoretical predictions and experiments, we reported a general strategy to engineer the electronic properties of iron-nitrogen-carbon (FeN 4 /C) catalysts via the incorporation of the boron (B) atom for achieving improved catalytic activity in oxygen electrocatalysis. Our theoretical results revealed that B modulation effectively tunes the d-band center of the iron (Fe) active site to optimize its adsorption strength with oxygenated species, greatly enhancing oxygen reduction reaction (ORR) and oxygen evolution reactions (OER) activity. Our experimental measurements then confirmed the above theoretical predictions: the as-synthesized B-doped FeN 4 /C (Fe-N 4 -B) material can perform as an eligible bifunctional catalyst for ORR and OER in alkaline media, and its catalytic activity even outperforms the commercial noble metal benchmarks. The present findings provide a promising strategy to further design the advanced catalysts for a wide range of electrochemical applications.
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CONSTRUCTION AND BUILDING MATERIALS
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2025
·
IF 8
Wen Yang,Yunbo Tong,Yong Yang,Qianping Ran,Lei Dong
The application of corrosion inhibitors is a widely adopted strategy for protecting reinforcing steel against electrochemical degradation. However, conventional direct-addition approaches often lead to premature inhibitor depletion and lack controlled-release functionality. In this study, a novel sustained-release capsule-type inhibitor was developed to combat chloride-induced steel corrosion. Ethyl cellulose with high alkali resistance, controllable release and good mechanical properties was used as the shell material and D -sodium gluconate as the core, using a phase separation method and the preparation of the capsule was verified by TG, FT-IR and SEM. The experiment showed that the resulting capsules displayed a "pea-pod" shape (about 0.5–1.0 μm in length and 0.2 μm in diameter) with a compact core/shell structure and when the core/shell ratio was 1:5, the maximum encapsulation efficiency of the capsules was 73.3 %. When dispersed in simulated concrete pore solution, the capsules enabled sustained release of D -sodium gluconate over multiple days. EIS and LPR were used for electrochemical test. And the electrochemical analysis confirmed that the capsule-based inhibitor effectively suppressed corrosion and improved corrosion resistance. Specifically, a dosage of 0.05 % resulted in an inhibition efficiency of 90.7 ± 1.2 % after 7 days. The core-to-shell ratio was identified as a critical factor governing both the release kinetics and the overall protective performance, with the 1:5 formulation demonstrating optimal corrosion inhibition. This study offers a promising strategy for the design and application of intelligent corrosion inhibitors in reinforced concrete structures.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2025
·
IF 8.5
Kai Yang,Yueshan Huang,Liyi Yao,Bin Huang,Weimin Zeng,Jin Huang
D-amino acid oxidase (DAAO) has long been recognized as a promising catalyst for chiral amino acid biosynthesis owing to its pronounced stereospecificity. However, its limited thermostability restricts industrial utility and poses challenges for protein engineering. Herein, we engineered a DAAO variant, M5 (S42D/T84D/H138N/A193R/E195Y/C234L), via a ProteinMPNN-guided multiple codon saturation mutagenesis approach. This variant exhibited superior catalytic efficiency (27.3 mM −1 s −1 , 29-fold relative to the starting enzyme) toward the non-natural compound D-glufosinate (D-PPT) and enhanced thermostability (519 min half-life at 50 °C, 208-fold relative to the starting enzyme). The evolution also expanded the enzyme's substrate scope toward several D-amino acids with different properties. The variant was proven able to completely transform 500 mM D-PPT in 7 h at a 100 mL scale with excellent stereospecificity. Molecular dynamics (MD) simulations gave the insight that the enhanced performance stems from altered surface charges and intramolecular/intermolecular networks. This strategy thus holds potential for engineering other enzymes involved in the biosynthesis of valuable products while reducing the screening costs during directed evolution.
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ANALYTICAL CHEMISTRY
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2025
·
IF 6.7
Huixiang Huo,Xuhua Wei,Chao Peng,Jing Li,Erkang Wang
Optimization of p-d orbital hybridization enhances charge interactions through increased orbital overlap, reduced electron transfer energy barriers, and regulated reaction activation energies, thereby significantly improving the catalytic kinetics. To implement the strategy, atomic substitution of Ru for Fe is employed in parent FeMnCuCoNi high-entropy nanozymes (HEzymes), yielding the RuMnCuCoNi HEzymes variant with outstanding peroxidase-like activity, demonstrating a 7-fold increase in activity over the parent alloy. Mechanistic studies reveal that the Ru 4dyz orbital, as the optimal catalytic site, exhibits stronger hybridization with the pz orbital of H2O2, which significantly enhances substrate adsorption. Concurrently, the reduced electron occupancy in antibonding orbitals strengthens orbital interactions with H2O2 while elevated electron density near the Fermi level accelerates electron transfer. The tripartite synergy, including enhanced adsorption, strengthened orbital interactions, and facilitated electron transfer, collectively drives the catalytic enhancement. Leveraging this nanozyme, an on-site detection platform is constructed for gastric cancer biomarkers (d-proline and d-alanine), achieving exceptional sensitivity and selectivity. Our work underscores the significance of p-d orbital hybridization regulation, providing a rational design principle for high-performance nanozymes.
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ORGANIC & BIOMOLECULAR CHEMISTRY
·
2024
·Vol. 22
·期 14
·2764-2773
·
IF 2.9
Yue Song,Wenjie Fan,Chen Yao,Heng Wang,Xiuxiang Lu,Yumin Wang,Pengxiang Liu,Yanjie Ma,Zhen Zhang,Jiang Wang,BeiBei Chu,Lijun Shi,Guoyu Yang,Mengdi Wang
Pattern recognition receptors (PRRs) play a critical role in the innate immune response, and toll-like receptor 7 (TLR7) is an important member of PRRs. Although several TLR7 agonists are available, most of them are being tested clinically, with only one available on the market. Thus, it is imperative to develop new TLR7 agonists. In this study, we designed and synthesized three kinds of quinazoline derivatives and five kinds of pyrrolo[3,2-d]pyrimidine derivatives targeting TLR7. The antiviral efficacy of these compounds was evaluated in vitro and in vivo. Our findings indicated that four kinds of compounds showed exceptional antiviral activity. Furthermore, molecular docking studies confirmed that compound 11 successfully positioned itself in the pocket of the TLR7 guanosine loading site with a binding energy of −4.45 kcal mol−1. These results suggested that these compounds might be potential antiviral agents.
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CARBOHYDRATE POLYMERS
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2021
·
IF 9.381
Zhixiang Cai,Hongbin Zhang
The chain conformational change in curdlan during carboxymethylation was investigated using nuclear magnetic resonance (NMR), circular dichroism (CD) spectroscopy, and atomic force microscopy (AFM). The distributions of carboxymethyl substituents within anhydroglucose unit (AGU) of CMCD were found to follow the order of OH (6) > OH (4) > OH (2) for CMCD with a low DS and OH (6) > OH (2) > OH (4) for CMCD with relatively high DS. The increased carboxymethylation level induced the chain conformation transition of curdlan from triple helix to random coil in water. The DS of 0.25 was the critical value of chain conformation transition, below which CMCD chains were triple helices. For DS larger than 0.25, CMCD existed in the state of random coils. The intermolecular hydrogen bonding between C2 hydroxyls in AGU sustained the triple helical conformation and stiffness of the polymer chain, which weakened with the increase in DS.
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Journal of Energy Storage
·
2025
·
IF 9.8
Yixuan Wen,Qingsheng Li,Yuxiang Yang,Wei Zhou,Xingao Dong,Shuo Zhang,Liqiang Zhang,Tongde Shen,Peng Jia,Yuqing Qiao
Lithium hydroxide (LiOH) as a discharge product with high conductivity and low overpotential in lithium-oxygen batteries (Li O 2 batteries) has received extensive attention. However, the incomplete decomposition of LiOH during the charge process remains a critical issue hindering the practical application of high-performance Li O 2 batteries. Developing suitable cathode catalysts is essential to address this challenge. Here, we constructed an Ag-regulated MnO cathode catalyst with disordered structure to promote LiOH decomposition, thereby improving the electrochemical performance. The introduction of Ag breaks the long-range ordered structure of MnO. Compared to that of MnO, the d-band center of Ag/MnO shifts downward from the Fermi level. This weakens the strong adsorption strength between the cathode and oxygen-containing intermediates, resulting in more moderate adsorption energy of these intermediates on the cathode surface, which facilitates the complete decomposition of discharge product. Additionally, the active sites of the Ag/MnO cathode remained stable, with LiOH decomposed completely. This work provides new insights into the development of efficient LiOH-decomposing cathode catalysts for Li O 2 batteries.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
·
IF 10.588
Dandan Zhu,Meijuan Chen,Yu Huang,Rong Li,Tingting Huang,Jun-ji Cao,Zhenxing Shen,Shun Cheng Lee
Formaldehyde is a typical indoor air pollutant that has posed severely adverse effects on human health. Herein, a novel FeCo alloy nanoparticle-embedded nitrogen-doped carbon (FeCo@NC) was synthesized with the aim of tailoring the transition-metal d-band structure toward an improved formaldehyde oxidation activity for the first time. A unique core@shell metal–organic frameworks (MOFs) architecture with a Fe-based Prussian blue analogue core and Co-containing zeolite imidazole framework shell was firstly fabricated. Then, Fe and Co ion alloying was readily achieved owing to the inherent MOF porosity and interionic nonequilibrium diffusion occurring during pyrolysis . High-angle annular dark-field scanning transmission electron microscopy and X-ray absorption fine structure spectra confirm that small FeCo alloys in situ form in FeCo@NC, which exhibits a higher formaldehyde removal efficiency (93%) than the monometallic Fe-based catalyst and a remarkable CO 2 selectivity (85%) at room temperature. Density functional theory calculations indicate the number of electrons transferred from the metal core to the outer carbon layer is altered by alloying Fe and Co. More importantly, a downshift in the d-band center relative to the Fermi level occurs from − 0.93 to − 1.04 eV after introducing Co, which could alleviate the adsorption of reaction intermediates and greatly improve the catalytic performance.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2025
·
IF 14.3
Yanhui Cao,Junhao Zeng,Xuerong Zheng,Yuan Liu,Junda Lu,Jinfeng Zhang,Yang Wang,Yida Deng,Wenbin Hu
Oxygen reduction reaction (ORR) in neutral electrolyte is urgently needed in various areas, such as metal-air batteries. However, the N-coordinated transition-metal single-atom electrocatalysts confront sluggish catalytic kinetics due to the inappropriate electronic structure and the as-resulted unreasonable adsorption strength towards oxygen-containing intermediates. In this work, we develop a strategy to tune the Fe d-orbital spin state by introducing inert Si atom into the first coordination sphere of Fe-N 4 moieties. The experimental and theoretical results suggest that Si atom generates the coordination field distortion of Fe and induces the Fe d-orbital spin state transforming from low to medium spin state. The optimized spin-electron filled state (t 2g 4 e g 1 ) of Fe sites weakens the adsorption strength to intermediates and reduces the energy barrier of *OH desorption. Consequently, Fe-Si/NC catalyst exhibits superior ORR performance compared with that of Fe-NC and commercial Pt/C, showing a more positive half-wave potential of 0.751 V (vs. RHE) in 0.1 mol/L phosphate buffered saline. In addition, Fe-Si/NC-based neutral zinc-air batteries show a maximum power density of 108.9 mW cm −2 and long-term stability for more than 200 h. This work represents the possibility of constructing distorted coordination configurations of single-atom catalysts to modulate electronic structure and enhance ORR activity in neutral electrolyte.
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Bioactive Materials
·
2025
·
IF 20.3
Qi Zhang,Zhe Zheng,Yiting Zhao,Qing Wu,Chu Wu,Xiuli Wang,Xia Wang,Qigang Wang,Peiru Wang
The transformation of O 2 is primarily facilitated by the catalytic action of redox enzymes, which play a pivotal role in sustaining cellular energy metabolism and redox balance. Bioinspired by O 2 distribution and ROS regulation related to cascade biocatalytic process, a D-peptide NapG D F D F D Y engineered hydrogel has been constructed with encapsulated dual-enzyme superoxide (SOD) and chloroperoxidase (CPO) cascade catalytic circuit and co-assembled photosensitizer of 5-aminolevulinic acid molecules (ALA). Multimodal oxygen modulation has been conducted by the concurrent oxygen generation via SOD-catalyzed ⋅O 2 − dismutation and oxygen consumption for 1 O 2 production by CPO and ALA, achieving self-sustaining enzymatic dynamic therapy (EDT)-photodynamic therapy (PDT) (EDT-PDT) synergy. The endogenous cascade-amplified EDT not only enhances the 1 O 2 efficacy in exogenous PDT therapy, but the intermediate O 2 can also alleviate local neuropathic pain caused by hypoxia for safe PDT treatment. This work pioneers enzyme-mediated dynamic control of tumor redox homeostasis, establishing a new therapeutic axis between biocatalytic amplification and photodynamic processes.
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ADVANCED MATERIALS
·
2025
·
IF 26.8
Miaomiao He,Qiancun Wang,Zhijie Lin,Dan Sun,Guangfu Yin,Yi Deng,Weizhong Yang
Pathogenic infections pose a persistent threat to global public health, necessitating innovative antibacterial strategies with well-defined disinfection pathway. The antibacterial efficiency is confined in the contradiction between reactants adsorption and intermediates desorption. Here, the FeMoS 4 /MXene bio-heterojunction enzyme (FM BioHJzyme) is proposed and constructed. Under the inspiration of near-infrared light (NIR), the heterostructures between the FeMoS 4 and MXene facilitates efficient electron-hole separation with localized electron accumulation at FeMoS 4 sites. Crucially, the electronic push-pull effect induced by Mo polarizes oxygen-containing reactants (H 2 O 2 , H 2 O, O2) toward Fe active centers, enabling sequential electron capture for reactive oxygen species (ROS) generation. The results also reveal an enhancement in electron density at Fe sites compared to FeS/MXene controls, which is accompanied by a downshift in the Fe d-band center that reduces intermediates adsorption energy. The therapeutic efficacy is systematically evaluated using an S. aureus -infected full-thickness skin defect model. The bi-modulated FM BioHJzyme exhibits favorable antibacterial efficiency under NIR irradiation, while subsequent wound healing is facilitated through collagen deposition and angiogenesis in the following absence of NIR irradiation. This work offers a deep insight into the intricate mechanism-performance relationship of BioHJzyme platform in catalytic anti-bacterial application and proposes a sustainable approach of mechanism-guided materials design.
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