JOURNAL OF MOLECULAR STRUCTURE
·
2025
·
IF 4.7
Xinru Dong,Yang Li,Xuejun Zhang,Nan Liu,Peng Gao
A donor–acceptor (D–A) covalent organic framework (CoPcPA-COF) was constructed from a metal phthalocyanine donor and a polycarboxylic acid acceptor unit. Molecular structure modulation endowed the material with exceptional visible-light absorption (bandgap: 1.34 eV) and a strong photoelectronic response. In photocatalytic tetracycline degradation, CoPcPA-COF achieved 91.1% removal within 60 min and maintained stable performance in various real water matrices, demonstrating excellent environmental adaptability. Density functional theory (DFT) analysis revealed pronounced spatial charge separation (CT ratio: 88.97%), a high exciton binding energy (4.314 eV), and a ligand-to-metal charge transfer tendency. Density of states (DOS) calculations indicated a theoretical bandgap of 0.5 eV, corroborating its broad-spectrum light response and favorable electronic structure. This work provides a theoretical foundation for the development of visible-light-driven COF photocatalysts and offers a promising strategy for efficient remediation of antibiotic contamination in water.
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高影响因子
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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高影响因子
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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高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Ren Ma,Yujing Zhang,Feiyang Yu,Shilong Wei,Yang Xing,Chengfang Qiao,Zhengqiang Xia,Qi Yang,Gang Xie,Sanping Chen
High energy level difference between electron donor (D) and electron acceptor (A) and low energy loss during charge transfer are prerequisites for the construction of efficient D–A-type covalent-organic framework (COF) photocatalysts. However, the spatial structure characteristics of the building blocks inevitably lead to the torsion of the D–A COF skeleton during the construction process and thus prevent effective charge migration. Herein, with the high-energy-level triphenylamine (TPA) as a model electron donor, the formyl positional isomers of tris(3-formylbiphenyl) amine (NDC) and tri(4-formylbiphenyl) amine (NBC) react with an acceptor 1,3,5-tris(4-aminophenyl) triazine (TTA), producing both D–A COFs for photocatalytic CO2 reduction and benzylamine coupling reactions. Structural investigations evidence that the formyl positional isomerism imparts the dihedral angle of TPA single arm reducing from 51.09 to 2.12°, the interlayer spacing from 3.89 to 3.55 Å, and the exciton binding energy from 97.25 to 85.86 meV in TTA-COFs. Such the “near-flat” TTA-NDC structure with confined clover-like channels dramatically accelerates the intralayer and interlayer charge migration efficiency and improves CO2 adsorption and oxygen activation ability (O2•– concentration of 48.01 μmol·L–1 in 3 h). To the best of our knowledge, TTA-NDC exhibits the highest benzylamine coupling efficiency with a turnover frequency value of 518.4 h–1 among the pristine COF photocatalysts, and its electron consumption rate for photocatalytic CO2 reduction reaches 1632.2 μmol·g–1·h–1, 3.85-fold higher than TTA-NBC, far surpassing most COF-based photocatalysts. Parallelly, the protonated H-TTA-NDC shows high CO2 reduction to CH4 yield (310.1 μmol·g–1·h–1) and selectivity (85.1%) due to the improved proton conductivity (σ = 1.07 × 10–2 S·cm–1). Additionally, the durability, stability, and possible photocatalytic mechanisms of TTA-NDC were systematically investigated.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Lili Yin,Wenjia Feng,Yang Hu,Xiangzhao Mao
Phosphatidylserine (PS), a rare phospholipid in Antarctic krill oil (AKO) critical for brain development, can be produced from the abundant phosphatidylcholine (PC) using phospholipase D (PLD) in Pickering emulsion interfacial catalysis (PIC) systems. However, the exposure of PLD to organic solvent around the emulsion interface diminished PLD activity, limiting the conversion efficiency of PS. In this study, we proposed a strategy to fabricate a PIC system with high efficiency and stability by immobilizing PLD in a specific phase on the emulsion interface, based on investigating the effect of the interfacial microenvironment on PLD activity. Janus-poly(acrylic acid)/polystyrene (JPP) and Janus-polyethylenimine/octadecane (JPO) particles were fabricated as carriers to realize the specific-phase immobilization of PLD. The highest activity was observed when PLD was immobilized on the hydrophilic side of JPP (PLD@JPP(W)), 1.9-fold that of free PLD. The catalytic efficiency of PLD@JPP(W) was 1.7-fold that of free PLD, confirmed by the kcat/Km value enhancement. Immobilization on the hydrophilic side also enhanced the thermal stability of PLD. The half-lives of PLD were extended from 4 to 36 h at 40 °C and from 6 to 28 days at 4 °C. Importantly, PLD@JPP(W) showed excellent catalytic efficiency as a PIC system, achieving a PS productivity of 93% within a short time of 2 h at an enzyme dosage of 0.05 mg. PLD@JPP(W) exhibited a 3.6 times higher yield than free PLD in the production of PS from PC rich in Antarctic krill oil. The strategy in this work could also be applied to other lipases, providing a promising method for the efficient conversion of functional lipids.
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JOURNAL OF CATALYSIS
·
2025
·
IF 6.5
Huabin Lian,Riming Hu,Lin Zheng,Daowei Gao,Shuai Wang,Rongyao Wang,Bin Wang,Guozhu Chen
The electrocatalytic reduction of biomass-derived furfural represents a sustainable pathway for the production of furfuryl alcohol and 2-methylfuran, serving respectively as value-added chemicals and biofuels. However, the production of these high-value-added products under mild conditions is hampered by low Faradaic efficiency. In this study, we develop a strategy to establish strong metal-support interactions, enabling Cu/NC (nitrogen-doped carbon) catalysts to efficiently produce value-added products under mild conditions. Specifically, we prepare a cost-effective NC support with highly dispersed ultrafine nano-Cu particles of approximately 1 nm in diameter. Under mild pH conditions, our comparative experiments show that the Faradaic efficiency for value-added products (furfuryl alcohol and 2-methylfuran) is nearly four times higher than that of commercial foam copper. We elucidate the influence of nitrogen-doped supports on the behavior of the supported metal Cu. Comprehensive in-situ infrared reflection absorption spectroscopy characterization and DFT theoretical calculations reveal a positive shift in the d-band center of the Cu 3d orbitals. This shift enhances the adsorption of furfural C1=O1 bonds on the Cu/NC catalyst and improves its capacity to bind active hydrogen, thereby increasing the Faradaic efficiency of the value-added products. Our findings advance theoretical understanding and providing practical insights for electrocatalytic hydrogenation of furfural under mild pH conditions.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Yutong Tong,Butian Chen,Chong Liu,Ruoyu Wang,Dewen Wang,Tianran Zhang,Xiaobai Ma,Limei Sun,Jinbo Yang,Wenyun Yang,Xiangfeng Liu
Halide solid electrolytes (SEs) show great potential in all-solid-state batteries (ASSBs) because of their high ionic conductivity and high oxidative stability. But the long-term cycling stability remains a major concern due to the cathode/halide interface side reactions, especially under high current density. Herein, a s-p-d orbital hybridization strategy is proposed via introducing Zr 4+ and F − into Li 3 InCl 6 (LIC-ZrF 4 ) to regulate the electron localization structure around the central In 3+ . The electron transfer between the cation and Cl is alleviated by the enlarged bandgap (4.485–4.894 eV) with ZrF 4 introduction, and more electrons aggregate around In 3+ after s-p-d hybridization among Zr, In, and Cl. This effectively prevents LIC-ZrF 4 from being attacked by O atoms in LiNi 0 . 8 Co 0 . 1 Mn 0 . 1 (NCM811) and significantly suppresses the interface side reactions. The in situ formed LiF-containing layer further enhances the interface stability. The assembled ASSB (NCM811/LIC-ZrF 4 /LPSC/Li-In) exhibits a state-of-the-art capacity retention (96.7%@500cycles@1C; 80.7%@1600 cycles@2C). Furthermore, the ionic conductivity of LIC-ZrF 4 is also enhanced from 0.6 to 1.5 mS cm −1 while the electronic conductivity is decreased from 3.66 × 10 −8 to 8.39 × 10 −9 S cm −1 . This work highlights the crucial role of s-p-d hybridization on the electron localization regulation and the interface stability, and presents some distinct insights into developing high-performance halides-based ASSBs.
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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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高影响因子
Redox Biology
·
2019
·
IF 7.793
Shen-Fei Wang,Xin Liu,Mo-Yu Ding,Shuangcheng Ma,Jing Zhao,Ying Wang,Shaoping Li
Reducing agents are crucial for the management of maladaptive inflammation-induced macrophage death and hematopoietic toxicity of chemotherapy. 2- O - β - d -glucopyranosyl- l -ascorbic acid (AA-2 β G), a unique AA (or vitamin C) derivative identified in Lycium barbarum , exhibited enhanced free radical scavenging activity compared with AA and its synthetic derivative AA-2 α G. AA-2 β G protected hydrogen peroxide-induced cell death in murine macrophage RAW264.7 cells. Treatment with AA-2 β G eliminated oxidative stress and the ratio of cellular glutathione to glutathione disulfide more effectively than AA and AA-2 α G. AA-2 β G also significantly reduced the fluorescent intensity of DCFH-DA triggered by chemotherapeutic agent camptotehcin-11 but not fluorouracil. AA, AA-2 α G, and AA-2 β G significantly decreased Keap-1expression, and increased the expression levels of nuclear factor E2-related factor 2 (Nrf2) and heme oxygenase-1. All compounds triggered the nuclear translocation of Nrf2, while the ability of AA-2 β G to enhance the Nrf2-DNA binding affinity was approximately two fold as those of AA and AA-2 α G. Sodium ascorbate cotransporters (SVCT) inhibitors, sulfinpyrazone, phloretin, and 3- O -methyglucose, potently abrogated the free radical scavenging activities of AA, AA-2 α G, and AA-2 β G. The cellular uptake efficacy of AA-2 α G and AA-2 β G was less than 10% of AA, while the inhibition of SVCT with sulfinpyrazone considerably diminished the uptake efficacy of these compounds. AA-2 α G and AA-2 β G are more stable in the Fenton reagents than AA. In summary, AA-2 β G from L. barbarum with excellent free radical scavenging activity is a promising natural AA derivative for further pharmacological evaluation.
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高影响因子
CARBON
·
2018
·
IF 7.082
Dongqi Li,Bin Zhang,Chunxuan Zhu,Xiangyu Tian,Zhizheng Zhao,Yu Chen
As the cornerstone of the modern information technology, the development of memory devices with high speed, large capacity, long life time, low power consumption and ease of operation characteristics is beneficial for the fast revolution of the digital world. Using soluble 4-bromobenzene functionalized reduced graphene oxide (RGBr) as two dimensional template, in-situ growing of a novel donor-accept type conjugated polymer “poly[(1,4-diethynyl- benzene)- alt -(4,4′-(quinoxaline-2,3-diyl)bis( N , N -diphenylaniline))](PDQ)” from the RGO surface has been successfully realized via the palladium-catalyzed Sonogashira-Hagihara polymerization. The resultant material called as RGO-PDQ is highly soluble in some common organic solvents . The nonvolatile ternary rewritable memory performance has been observed in an electronic device with the RGO-PDQ film sandwiched between the Al and ITO electrodes. The switching threshold voltages on the ON-1 and ON-2 states are −0.74 and −1.44 V, respectively. The achieved current ratio of OFF: ON-1: ON-2 is about 1: 10: 10 4 . The memory effect of the Al/RGO-PDQ/ITO device on the ON-1state can be assigned to the contribution of the PDQ moieties in the structure of RGO-PDQ. By using conductive atomic force microscopy (C-AFM) technique, the conductive nature of the RGO-PDQ film-based device was in-situ observed.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xin Tao,Jingyu Ren,Danjun Wang,Hua Huang,Yani Li,Di Guo,Baoqin Shan,Yu Liu,Jian Wang,Yanzhong Zhen,Zhirui Niu
The low activity of photocatalysts is mainly due to inefficient charge separation and low production of the active species. To overcome this challenge, we constructed an S-scheme CdIn 2 S 4 /MnZnFe 2 O 4 (CIS/MZFO) heterostructure, where the strong interface of the heterostructure leads to an upshift of the d-band center. CIS/MZFO shows higher charge transfer efficiency and oxygen adsorption/activation performance compared to CIS and MZFO separately, thereby increasing the production of ·O 2 − and h + active species. As a result, it demonstrats efficient photocatalytic degradation of tetracycline hydrochloride. The optimized CIS/MZFO heterostructure also shows good tolerance to various factors, such as inorganic ions, organic acids, pH and real water environments. The heterostructure also exhibits excellent magnetic recyclability and stability. Additionally, we propose a photocatalytic degradation pathway for tetracycline hydrochloride and evaluate the ecological toxicity that may arise from intermediates. This study provides an effective approach for the design of advanced photocatalysts.
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JOURNAL OF HAZARDOUS MATERIALS
·
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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