ACS Applied Nano Materials
·
2025
·
IF 5.5
Ai-Hui Cao,Xin-Tai Su,Min Zhang,Qi-Long Zhu
Photocatalytic water decomposition is a cost-effective way to convert sustainable solar energy into chemical energy. While semiconductor photocatalysis has generated considerable interest in photocatalytic hydrogen evolution, it is hampered by fast electron–hole complexation and suboptimal efficiency. Herein, an NH2-MIL-101(Cr)/doped-C3N4 heterojunction possessing a static internal electric field (IEF) is successfully prepared, characterized, and assessed for photocatalytic hydrogen production. The optimized photocatalytic H2 evolution rate of the resultant NH2-MIL-101(Cr)/O–C3N4 is 460 μmol g–1 h–1 under visible light, with an AQY of 2.5% at 450 nm. Spectral evidence indicates that the static IEF facilitates rapid electron transfer from NH2-MIL-101(Cr) to O–C3N4, achieving efficient photogenerated charge separation and a consequent significant enhancement in catalytic activity. This work not only presents a case of construction of an IEF through assembling NH2-MIL-101(Cr) with O–C3N4 but also deepens the insight of the rudimentary mechanisms of the static IEF in heterojunctions for photocatalytic hydrogen evolution.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2025
·
IF 5.4
Yongxing Shang,Jian Xiong,Shuo Chen,Junjie Zhu,Xiaodie Zhao,Bitao Xiong,Xing’ao Li
Acid Orange 7 (AO7) is a recalcitrant contaminant exhibiting persistent resistance to degradation in aquatic environments. Materials based on graphitic carbon nitride (
) demonstrate significant potential in removing pollutants like AO7 through synergistic interactions with oxidants, utilizing their exceptional catalytic properties and high surface area for adsorption. However, their effectiveness is limited by a relatively large band gap, which hinders their catalytic performance. This study reveals that Ni/O dual-doped
(NiOCN) effectively optimizes the structure and catalytic performance of
. Experimental results indicate that the NiOCN/peroxymonosulfate (PMS) system exhibits optimal AO7 degradation performance, achieving 92.3% degradation within 10 min while maintaining 80% efficiency in simulated aqueous matrices. Quenching experiments further identified superoxide anion radicals ( ⋅ O 2 − ) as the predominant reactive species governing AO7 degradation. Using density functional theory (DFT) calculations, we confirmed that Ni/O dual-doping narrows the band gap and boosts catalytic activity. Our findings mechanistically demonstrate that Ni/O dual-doping augments PMS activation performance by introducing impurity energy levels, increasing adsorption sites, and accelerating electron migration kinetics.
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FOOD HYDROCOLLOIDS
·
2025
·
IF 12.4
Chao Zhang,Xuan Hu,Yu Zhang,Lingfei Li,Shufang Zhao,Quanfang Zhang,Yanli Yu,Wei Liu
This study developed and optimized a fully natural W1/O/W2 double emulsion system for oral iron delivery, using diosgenin, a natural triterpenoid saponin, to stabilize the inner water–oil (W1/O) interface and pea protein nanoparticles (PPNs) to stabilize the outer oil–water (O/W2) interface. The optimal primary emulsion, containing 9 % diosgenin in the oil phase and a W1:O ratio of 2:8, exhibited excellent centrifugal and storage stability. External aqueous phases (W2) were prepared from 2 %, 4 %, and 6 % pea protein dispersions, which underwent ultrasound treatment followed by centrifugation to produce corresponding PPNs suspensions designated as PPN-2 %, PPN-4 %, and PPN-6 %, respectively. The primary iron-containing W1/O emulsion was dispersed into these W2 phases at a W1/O: W2 ratio of 2:8, yielding stable W1/O/W2 emulsions with iron encapsulation efficiencies exceeding 99 %. In vitro simulated digestion revealed that the emulsions with PPN-6 % effectively minimized iron release in the gastric phase (<1 %) while promoting controlled release in the intestinal phase, thereby improving bioavailability and potentially reducing gastric irritation. Compared to synthetic PGPR-stabilized emulsions, the diosgenin-PPNs system demonstrated superior structural stability and digestive performance. This multilayered, food-grade emulsion system offers a promising, health-oriented alternative for iron fortification in functional foods.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Bolong Zhao,Yuyu Wang,Min Xu,Duoning Zhao,Li Zhu,Liqiong Wang,Wenxin Ji,Yuanyuan Li,Guangsuo Yu,Yulong Ma,Yonggang Sun
Low-nuclearity cobalt-oxygen/nitrogen heterogeneous clusters (Co-O/N HCs) activated H 2 O 2 for non-radical oxidation of organic pollutants via unique oxygen atom transfer (OAT) and singlet oxygen ( 1 O 2 ) pathways. The novel Co-O/N HCs were synthesized using a ligand self-polymerization strategy. When applied to high-salinity wastewater, they efficiently degraded tetracycline via 100 % non-radical pathways over a wide pH range, with degradation rates greater than 0.1758 min −1 and no inhibition by Cl - . The confined cluster size (3–5 Co atomic units) and asymmetric nitrogen distribution modified the cobalt atoms' electronic structure, promoting two H 2 O 2 adsorption modes: bridge-adsorbed *O-O* mediated direct oxidation via OAT, while edge-adsorbed *OOH species selectively generated 1 O 2 . This work elucidates the active sites and mechanisms of H 2 O 2 activation, offering key insights for the design of advanced Fenton-like catalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Dong Yan,Xuetao Cheng,Xiaoxiao Dong,Han Wang,Xingchen Chang,Chenghui Xia,Yongcheng Jin,Chun-Chao Hou
Electrolysis of seawater driven by renewable energy holds great promise for sustainable hydrogen production. However, both catalyst corrosion caused by competitive Cl − adsorption and sluggish reaction kinetics are major challenges in seawater electrolysis. Here, inspired by the concept of hard and soft acids and bases (HSAB), a unique interfacial W-O-Co electron bridge is constructed on the catalyst surface to achieve the electronic coupling of hard-acid W site and borderline-acid Co site via the oxygen bridge, which demonstrates exceptional performance for both the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER) in alkaline water and seawater, as well as high anti-corrosion stability. Remarkably, WO 3 /CoP electrode requires low overpotentials of merely 154 mV (alkaline freshwater) and 189 mV (alkaline seawater) for HER, and 334 mV (alkaline freshwater) and 343 mV (alkaline seawater) for OER to achieve 100 mA cm −2 , respectively. When deployed our bifunctional catalyst as both anode and cathode in an alkaline anion-exchange membrane seawater electrolyzer, the system achieves 1 A cm −2 at a low cell voltage of 1.80 V and maintains stable electrolysis for over 250 h at 100 mA cm −2 . Theoretical and experimental investigations reveal that the hard-acid W site of the electronic W-O-Co bonded bridge prefers adsorption of hard-base OH - rather than soft-base Cl - , thereby mitigating Cl - interference and suppressing chloride corrosion. Simultaneously such interfacial W-O-Co bridging significantly accelerates charge transfer from Co site to W site, thereby regulating the electronic structures of catalysts and optimizing the sorption behaviors of reaction intermediates. This work provides a feasible anti-corrosion engineering strategy to design efficient and robust electrocatalysts for practical seawater electrolysis.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yilin Wang,Xiaoli Sun,Yunmei Du,Shuangshuang Li,Mengmeng Wang,Yanru Liu,Lei Wang
Optimizing the electronic structure of Ru by introducing N dopants or O vacancies (V O ) into RuO 2 is expected to be a promising strategy to stimulate the hydrogen evolution reaction (HER) performance. However, it is a challenge to develop a fast and low-energy method to simultaneously achieve the construction of N dopants and V O . This work was the first to optimize the quenching technique for achieving the co-introduction of V O and N in Co-RuO 2 nanosheets (N,Co-RuO 2 -V O ). Related characterizations confirmed that V O and N dopants synergistically optimized the electronic configuration of Ru and the reaction path of alkaline HER. As expected, the mass activity of N,Co-RuO 2 -V O (2208.63 mA m g R u - 1 ) was 8.05-fold that of Pt/C at 100 mV for alkaline HER. Surprisingly, N,Co-RuO 2 -V O required only 148.6 mV to achieve an industrial-grade current density of 1 A cm −2 , which was much lower than the commercial Pt/C catalyst (312 mV). Overall, this work provides an energy-efficient new strategy for the development of Ru-based catalysts with ampere-level currents.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Yunlong Li,Chunsheng Li,Shuang Liu,Qiang Wang,Zhengyang Tang,Jiawei Qu,Jin Ye,Yong Lu,Jun Wang,Kefen Zhang,Yujie Fu,Jiating Xu
NH 2 -MIL-88B (Fe) (MOF) is a promising photocatalytic material for antitumor therapy because of its distinctive electronic structure. However, inadequate separation of photo-generated electrons and slow reaction rate in low/high-valence iron (Fe) cycles limit their clinical application. In the present study, “electronic storage station” as a ligand-to-metal charge transfer bridge bond was constructed to inhibit recombination of electron/hole under 650 nm laser irradiation. Cupric (Cu) ions and gallic acid (GA) were self-assembled into a MOF (denoted as CGMOF) to create an Fe O(GA) Cu bridge bond. GA, characterized by robust electron delocalization and abundant electron-donating groups, significantly enhances electron transfer efficiency for photodynamic therapy (PDT). CGMOF can respond to endogenous glutathione and release cuprous ions, accelerating the iron ion/ferrous ion cycles for chemodynamic therapy (CDT). The released Fe species can serve as T 2 -weighted magnetic resonance imaging contrast. Extended X-ray absorption fine structure spectra confirmed the presence of GA-containing Fe O Cu bonds in CGMOF. Furthermore, a series of photo-electrochemical tests confirmed that the formation of Fe O(GA) Cu bond prominently elevated the redox capacity and increased the carrier density of CGMOF by 2.74-fold compared to that of MOF. In addition, cinnamaldehyde was grafted onto CGMOF for tumor-responsive hydrogen peroxide self-supply. Concurrently, hyaluronic acid was surface-modified to achieve the targeted delivery of nano-photosensitizers. In summary, this study presents an innovative approach for engineering Fe-based metal–organic frameworks for synergetic PDT/CDT applications.
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高影响因子
MICROCHIMICA ACTA
·
2024
·Vol. 191
·期 7
·1-9
·
IF 5.3
Zhang Yue,Yu Wei,Zhang Wei,Lai Jinyu,Liu Lin,Wang Wei,Wang Xinghua
Abstract Ratiometric fluorescence and colorimetric strategies for detecting activity of butyrylcholinesterase (BChE) in human serum were developed by using g-C 3 N 4 nanosheets, silver ion (Ag + ) and o-phenylenediamine (OPD) as chromogenic agents. The oxidation-reduction reaction of OPD and Ag + generates 2,3-diaminophenazine (oxOPD). Under exciation at 370 nm, g-C 3 N 4 nanosheets and oxOPD emit fluorescence at 440 nm ( F 440 ) and 560 nm ( F 560 ), respectively. Additionally, oxOPD exhibits quenching ability towards g-C 3 N 4 nanosheets via photoinduced electron transfer (PET) process. Thiocholine (TCh), as a product of BChE-catalyzed hydrolysis reaction of butylthiocholine iodide (BTCh), can coordinate with Ag + intensively, and consequently diminish the amount of free Ag + in the testing system. Less amount of free Ag + leads to less production of oxOPD, resulting in less fluorescence quenching towards g-C 3 N 4 nanosheets as well as less fluorescence emission of oxOPD. Therefore, by using g-C 3 N 4 nanosheets and oxOPD as fluorescence indicators, the intensity ratio of their fluorescence ( F 440 /F 560 ) was calculated and employed to evaluate the activity of BChE. Similarly, the color variation of oxOPD indicated by the absorbance at 420 nm ( ΔA 420 ) was monitored for the same purpose. These strategies were validated to be sensitive and selective for detecting BChE activity in human serum, with limits of detection (LODs) of 0.1 U L −1 for ratiometric fluorescence mode and 0.7 U L −1 for colorimetric mode. Graphical abstract
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FOOD HYDROCOLLOIDS
·
2024
·
IF 11
Biyang Zhu,Siyu Guo,Peter Chi-Keung Cheung,Kseniya Hileuskaya,Lijun You
Probiotics as pharmaceutical and nutraceutical products are essential to human health, whereas maintaining their viability in adverse environments remains an obstacle. This study presents a well-designed W 1 /O/W 2 emulsion system incorporated in calcium-alginate hydrogel particles for the targeted delivery and sustained release of Lactobacillus bulgaricus in the gastrointestinal tract. Firstly, the degraded fucoidan (DF) with the highest carboxyl content (2.99%), prepared using UV/H 2 O 2 treatment, was more favorable for forming DF-CS nanogel through ionic cross-linking with chitosan (CS). The W 1 /O/W 2 double emulsion fabricated by 0.4 mg/mL DF-CS nanogel possessed the highest interface stability, as concluded from visual appearance, confocal laser scanning microscope (CLSM), droplet size distribution, and ζ-potential results. The double emulsion loaded in 2% alginate hydrogel showed desirable textural properties and swelling behavior, thereby offering a high encapsulation efficiency of Lactobacillus bulgaricus (74.5%). Additionally, the hydrogel delivery system not only achieved sustained release of Lactobacillus bulgaricus in the simulated gastrointestinal condition (>10 7 CFU/g) but also maintained at least 71.3% and 55.1% survival of probiotics at −20 °C and 4 °C, respectively, after 28 d of long-term storage. Overall, these W 1 /O/W 2 double emulsion-filled multilayer self-assembled hydrogel particles can be utilized for better protection and delivery of probiotics in the food and pharmaceutical industries.
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JOURNAL OF CHROMATOGRAPHY B-ANALYTICAL TECHNOLOGIES IN THE BIOMEDICAL AND LIFE SCIENCES
·
2017
·
IF 2.603
Yang Xu,Dongwen Hu,Yuting Li,Chongde Sun,Wei Chen
Accumulating evidence indicates that consumption of berries may exert beneficial effects against oxidative stress mediated diseases. Pelargonidin -3-O- glucoside (Pg3G), a bioactive ingredient in strawberry, has been reported to possess a potent antioxidant capacity. This study was therefore designed to develop an effective method to prepare pure Pg3G from strawberry and investigate its protective effect against H 2 O 2 -induced oxidative stress. According to our results, Pg3G occupied 85.55% of total anthocyanin content in strawberry. 240 mg of Pg3G with the purity of 97.26% was finally isolated from 320 g of strawberry lyophilized powder (SLP) by combination of AB-8 macroporous resin and high-speed counter-current chromatography (HSCCC) technologies. Further study unveiled that Pg3G significantly inhibited H 2 O 2 -induced ROS generation, GSH depletion and mitochondrial dysfunction, thereby ameliorating H 2 O 2 -induced oxidative stress. Overall, this study suggests that pelargonidin -3-O- glucoside can be used as a natural bioactive agent to prevent cellular oxidative stress.
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BIOMATERIALS
·
2012
·
IF 7.404
Meirong Huo,Aifeng Zou,Chengli Yao,Yong Zhang,Jianping Zhou,Jing Wang,Qinnv Zhu,Jing Li,Qiang Zhang
In this study, a ligand-PEG-lipid conjugate , octreotide-polyethene glycol-deoxycholic acid (OCT(Phe)-PEG-DOCA, or OPD) was successfully synthesized and used as a targeting molecule for N-deoxycholic acid-O, N-hydroxyethylation chitosan (DAHC) micelles for efficient cancer therapy. DAHC micelles exhibited good loading capacities for doxorubicin (DOX), a model anti-cancer drug, and the modification of OPD showed no significant effect on drug load while slightly increasing the particle size and partly shielding the positive charges on the surface of micelles. Accelerated release rate of DOX from micelles were also observed after OPD modification and the release profile exhibited pH-sensitive properties. Compared with DAHC-DOX micelles, OPD-DAHC-DOX micelles exhibited significantly stronger cytotoxicity to MCF-7 cells (SSTRs overexpression) but with hardly any difference from WI-38 cells (no SSTRs expression). The results of flow cytometry and confocal laser scanning microscopy further revealed that OPD-DAHC-DOX micelles could be selectively taken into tumor cells by SSTRs-mediated endocytosis . In vivo investigation of micelles on nude mice bearing MCF-7 cancer xenografts confirmed that OPD-DAHC micelles possessed much higher tumor-targeting capacity than the DAHC control and exhibited enhanced anti-tumor efficacy and decreased systemic toxicity. These results suggest that OPD-DAHC micelles might be a promising anti-cancer drug delivery carrier for targeted cancer therapy.
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Sustainable Energy & Fuels
·
2022
·Vol. 6
·期 11
·2745-2754
·
IF 6.813
Hua Tan,Xuecheng Li,Hao Ma,Xiaolin Yang,Tong Zhan,Wenyu Xie,Suhua Wang,Jiaping Zhu
Herein, N-doped carbon embedded Ni catalysts were prepared by a co-impregnation method followed by pyrolysis in a N2 atmosphere for transfer hydrogenolysis of lignin β-O-4 alcohol and ketone model compounds using isopropanol as the hydrogen source. It was found that pyrolysis at 800 °C resulted in the formation of graphitic N-doped carbon shell encapsulated Ni nanoparticles (Ni@NC-800). The obtained Ni@NC-800 exhibited higher activity and selectivity to aromatics in the conversion of 2-phenoxy-1-phenylthanol and 2-phenoxyacetophenone, compared with Ni@NC-600 and Ni/NC-800. Moreover, the selectivity to aromatics could be further improved over Ni@NC-800-H, which is Ni@NC-800 after strong acid leaching. However, the presence of Cα–OH in lignin β-O-4 model compounds was essential for their product distributions. The control and characterization experiments suggested that the catalytic reaction occurred on the surface of N-doped carbon shells, because the encapsulated Ni NPs could donate electrons to the outer shells, leading to surface electron enrichment, thus making inert shells the new active sites in Ni@NC-800-H. In addition, Ni@NC-800-H was efficient for the conversion of various lignin β-O-4 alcohol and ketone model compounds with methoxyl groups with high yields of the aromatic products and also possessed high stability during consecutive reaction runs, which is because Ni nanoparticles are physically isolated from the reactive environment.
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