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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高影响因子
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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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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ACS Nano
·
2025
·
IF 16
Xuyu Li,Qingfu Zhao,Xiaolin Feng,Pinyuan Cui,Jingjing Yu,Binyong Liang,Chao Liu,Ye Wang,Yiting Wu,Ruiqi Wang,Bo Hu,Yihan Lin,Lichong Zhu,Xuan Zhu,Ban Luo,Xiangliang Yang,Jun Hu
Immunoradiotherapy (iRT) has emerged as a promising strategy for liver hepatocellular carcinoma (LIHC) treatment to synergistically activate both localized antitumor immunity and systemic immune responses. However, radiation will aggravate LIHC hypoxia, resulting in an adenosine metabolism level elevation, which promotes the differentiation of T cells into terminally exhausted phenotypes and weakens the efficacy of immunotherapy. To overcome this challenge, we engineered a nanocatalytic probiotic-based radiation-metabolic modulator, in which Escherichia coli Nissle 1917 (EcN) was programmed to in situ synthesize gold–palladium bimetallic nanocatalysts (EcNcGP) via biodirected mineralization. Guided by lattice mismatch and interfacial strain engineering, engineered EcN orchestrates the epitaxial assembly of Au atoms on Pd nanoclusters, yielding a precisely strain-tuned heterostructure with a modulated d-band electronic structure. This architectural design optimizes oxygen intermediate adsorption–desorption kinetics and significantly enhances the catalytic efficiency. This design enables EcNcGP to exhibit robust catalase- and peroxidase-like activities, which effectively catalyze intratumoral H2O2 into O2 and hydroxyl radicals, intensifying radiation damage and alleviating tumor hypoxia to inhibit adenosine metabolism by downregulating the expression of ectonucleoside triphosphate diphosphate hydrolase 1 (CD39) and ecto-5′-nucleotidase (CD73). By blocking the binding of adenosine (ADO)–adenosine receptor A2A (ADORA2A) to inhibit the following cyclic adenosine monophosphate (cAMP)–protein kinase A (PKA)–phosphorylation of cAMP response element binding (pCREB) signaling transduction, radiation-induced T-cell exhaustion could be inhibited. Compared to stereotactic body radiotherapy (SBRT), the combination of EcNcGP with SBRT increased CD8+ T-cell infiltration by 99.8% and reduced PD-1hi-exhausted T cells by 63.9%. Integration with anti-PD-L1 therapy (αPD-L1) achieved complete tumor regression in 60% of the treated mice-bearing orthotopic hepatocellular carcinoma. These findings establish a paradigm-shifting strategy for reprogramming tumor-immune metabolic checkpoints using strain-engineered nanocatalytic probiotics, thereby enhancing iRT and overcoming radioresistance.
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PubMed
高影响因子
ANALYTICAL CHEMISTRY
·
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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PubMed
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
·
IF 15.7
Sang Zhiyuan,Qiao Yuqian,Chen Rui,Yin Lichang,Hou Feng,Liang Ji
Tailoring the electronic structure of electrocatalysts for oxygen reduction reaction (ORR) has been widely adopted to optimize their performance. However, the steric effect originating from the layered or crystal structure of a catalyst is often neglected. Herein, we demonstrate the importance of such steric effect in a one-dimensional π-d conjugated metal-organic framework with Ni-(NH) 4 nodes (Ni-BTA) for optimizing its electrocatalytic performance, where the activity and selectivity towards two-electron ORR for H 2 O 2 production are largely enhanced. Theoretical simulation and in-situ characterization demonstrate the formation of inter-layer H-bonds between *OOH intermediates and -N-H groups in the adjacent top layers of the Ni-sites, enhancing the *OOH binding energy to an optimum value. Thus, the as-prepared Ni-BTA catalyst exhibits an outstanding electrocatalytic 2e − -ORR performances under neutral and alkaline conditions (e.g., >85% H 2 O 2 selectivity from −0.1-0.4 V vs. RHE and >13.5 mol g −1 h −1 H 2 O 2 yield in neutral electrolytes), also showing great potential on water treatment and disinfection. Here, we highlight the alternative avenues for utilizing the non-coordinated structure to regulate the catalytic performance, thus providing opportunities for the design of catalysts and beyond.
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高影响因子
Foods
·
2025
·Vol. 14
·期 9
·1538
·
IF 5.1
Zepeng Li,Runmin Wang,Xiantai Lai,Wenyi Liao,Runfeng Liao,Zhuohong Wu,Guoyan Zhang,Xianghui Qi
D-tagatose is a functional sweetener with glucose-regulating and prebiotic properties, but its bioproduction from D-galactose faces many limitations, particularly the high production costs. In particular, the current biosynthesis of D-tagatose suffers from thermal instability and the substrate selectivity issues of L-arabinose isomerase (L-AI) required to convert D-galactose into D-tagatose. In this study, recombinantEscherichia coliBW25113/pQE-80L-araAF118M/F279Iexpressing double mutant L-AI was immobilized to enhance its stability and reusability. The optimal conditions for whole-cell catalysis were 60 °C, pH 6.5, 5 mM Mn2+, and 20 h, with a yield of 55.2 g/L of D-tagatose. Immobilization with 3% sodium alginate and 2% CaCl2retained 90% of the production efficiency displayed by free cells. Notably, the immobilized cells exhibited enhanced heat resistance (60–70 °C) and operational stability, retaining 76% activity after five cycles. The D-tagatose production was further increased to 129.43 g/L by increasing the substrate concentration to 250 g/L. Compared to free cells, immobilized cells retained 83.6% of the initial yield up to 10 batches. This study presents a cost-effective and sustainable method for the production of D-tagatose using optimized whole-cell catalysis through immobilization, which paves the way to solve industrial challenges such as thermal instability and low substrate efficiency.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Xingyu Zhao,Jiaping Shen,Huixuan Qi,Juan Sun,Bin Xu,Lei Tao,Wenhai Lin,Shengliang Li,Zhiyuan Zhong
Phototherapy including photothermal therapy (PTT) and photodynamic therapy (PDT) is widely used for cancer treatment because of its non-invasiveness, spatiotemporal controllability, and low side effects. However, the PTT and PDT capabilities of photosensitizers (PSs) compete so it’s still a crucial challenge to simultaneously enhance the PDT and PTT capabilities of PSs. In this work, donor-π-acceptor (D-π-A)-based boron dipyrromethene (BODIPY) dyes were developed via molecular engineering and applied for enhanced phototherapy of triple-negative breast cancer. With thiophene engineering and iodine addition, D-π-A BDP dyes possessed a low energy gap between the singlet and triplet states (ΔE S1-T1 ). After the BDP dyes were prepared into nanoparticles (NPs), the BDP4 NPs showed increased generation of type I and II reactive oxygen species (ROS) as well as a high photothermal conversion efficiency (44 %). Furthermore, folate (FA)-modified BDP4 NPs achieved high tumor targeting via near-infrared bioimaging. With these advantages, BDP4 NPs with FA achieved total tumor eradication and tumor metastasis suppression via a single injection and 808 nm laser irradiation. This work provided a rational design of D-π-A PSs for simultaneously enhancing their photodynamic and photothermal performance, achieving efficient cancer therapy.
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高影响因子
DALTON TRANSACTIONS
·
2019
·Vol. 48
·期 15
·5072-5082
·
IF 4.052
Shuang Huang,Xi Hong,He-Zhen Cui,Quan Zhou,Yue-Jian Lin,Xiu-Feng Hou
Seven new chelated cyclometalated Ir complexes of ABON,P, ABON,O, and ABON,C(carbene) based on a rigid and tunable 2-arylbenzo[d]oxazole backbone have been prepared for the N-methylation of amines. Among these three coordinated modes, ABON,C(carbene)-chelated iridium-based catalysts exhibited good performance in the monomethylation of aromatic amines with methanol (MeOH) as the green methylation reagent. The steric-modified synthesis of ABON,C(carbene) complexes was described. The most active ABON,C(carbene) complex with marginal steric hindrance as a catalyst was obtained from the benzoxazole ring without a substituent and methyl group of the benzimidazole ring on the N-heterocyclic carbene (NHC) ligand. A variety of amines including para- and meta-substituted aromatic amines, as well as heterocyclic amines, were formulated as suitable substrates. Importantly, this catalyst considerably promoted the yield of the N-methylation of ortho-substituted aromatic amines. Controlled kinetic experiments and deuterium-labeling reactions of these ortho-substituted amines were conducted under optimized conditions. On the basis of the experimental results, a plausible mechanism was proposed.
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高影响因子
Materials Today Communications
·
2022
·
IF 3.662
Yuanyang Zhang,Xiaoping Liang,Tao Jiang,Zishang Chen,Xiujie Ji
Waste water with boron is a widespread environmental problem. This work presents a kind of novel organic-inorganic composite boron adsorbent of NGN, N-methyl- D -glucamine (NMDG) @γ-glycidoxypropyl-trimethoxysilane (GPTMS) on the nonwoven basalt fibers (NBF), which is environmentally friendly, water resistance, non-toxicity and low cost. The effect of various parameters on the adsorption performance of NGN, such as pH value, boron concentration, contact time and different ion concentrations, was investigated. The optimum adsorption capacity of 1.64 mmol/g occurred in the vicinity of pH 9.0, and NGN possessed the fast adsorption equilibrium of boron within 40 min. In the presence of competing ions, Na + and Li + had little effect on the adsorption of boron, while Mg 2+ promoted the adsorption of boron. The features of NGN adsorption process were assessed by Langmuir and Freundlich adsorption isotherms . The experimental data of NGN boron adsorbent was well described by using the pseudo-second-order kinetic model. In addition, after eight times adsorption-desorption cycles, NGN still featured excellent regeneration performance. All the experimental results illustrate that NGN could be efficiently utilized for separating and recycling boron from aqueous solutions.
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TALANTA
·
2020
·
IF 5.339
Lili Liu,Peng Bao,Juan Qiao,Hongyi Zhang,Li Qi
Herein, D- and L-oligopeptides were explored for the first time as chiral ligands in a chiral ligand exchange capillary electrophoresis (CLE-CE) protocol with Zn(II) as central ion for separation of derived d , l -amino acid enantiomers (Dns-D,L-AAs). The effect of four D- and L-oligopeptides, including glycine- l -lysine (Gly-L-Lys), glycine- d -lysine (Gly-D-Lys), l -lysine-lysine-OH and l -lysine-lysine-lysine-lysine-OH on the CLE-CE separation efficiency were evaluated. Thermodynamic calculations and circular dichroism spectra properties showed that the ternary species [(Gly-L-Lys)Zn(II)(D-AAs)] and [(Gly-L-Lys)Zn(II)(L-AAs)] presented the best stereoselectivity , possibly due to entropic effects. Notably, the migration order of Dns-D-AAs and Dns-L-AAs could be tuned by using Gly-D-Lys as the ligand for the CLE-CE system. To obtain satisfactory CLE-CE performance, the concentration ratio of Zn(II) to Gly-L-Lys, the pH of the buffer solution, and the concentration of Zn(II) were investigated. Under the optimized CLE-CE conditions using 100.0 mM H 3 BO 3 , 10.0 mM NH 4 Ac, 3.0 mM Zn (II) and 12.0 mM Gly-L-Lys as the buffer solution at pH 8.30, nine pairs of Dns-D,L-AAs achieved baseline separation, with the partial separation of another five pairs. Furthermore, the proposed CLE-CE protocol, which presented a good linear relationship with the concentration of the test analytes in the range of 75.0–625.0 μM (r 2 ≥ 0.994) and the limit of detection of the method was 5.0 μM, was successfully applied in the kinetics study of l -asparaginase using l -asparagine as the substrate. Our strategy shows the great potential of L-dipeptides in the CLE-CE separation of D,L-AAs enantiomers and bio-applications.
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高影响因子
JOURNAL OF THE AMERICAN OIL CHEMISTS SOCIETY
·
2018
·Vol. 96
·期 1
·15-23
·
IF 1.601
Saisai Li,Yan Li,Nengbing Long,Ruifeng Zhang
Phospholipase D (PLD) was effectively immobilized on a nanocomposite support composed of ZnO nanowires and SiO 2 through in-situ co-cross-linking with poly-L-lysine (PLL). An anionic and long-chained bisepoxide cross-linker was electrostatically adsorbed on the surface of ZnO nanowires prior to co-cross-linking. Under the optimal pH, 6.5, the loading amount of PLD reached an average of 114 mg per g support for PLL concentrations in the range of 0–0.6 mg mL −1 . Co-cross-linking of PLD with PLL enhanced the activity of PLD remarkably. The highest specific activity of co-cross-linked PLD reached 25.8 U per mg protein , which was 1.62 times as high as that of the cross-linked PLD (15.9 U per mg protein ). (One unit of PLD activity [U] refers to the amount of PLD, which liberates 1 μmol of p-nitrophenol per min via hydrolysis of phosphatidyl-p-nitrophenol at pH 8.0 and 30 °C). Under the optimized conditions, the yield of phosphatidylglycerol (PtdGro) reached 98.6% within 80 min at 45 °C and pH 6.5. The co-cross-linked PLD not only exhibited good resistance to pH and heat inactivation but also improved storage stability and reusability. The yield of PtdGro remained ≥85.4% after 13 repeat uses.
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