INORGANIC CHEMISTRY
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2023
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IF 4.6
Tuohetijiang Baiheti,Abudukadi Tudi,Minqiang Gai,Xuping Wang,Shujuan Han
Fluorooxoborates are promising yet largely untapped crystal materials for linear and nonlinear optical applications. The introduction of a strong electronegative F atom into an oxyboron anionic group offers a virtually unlimited chance for structural engineering and ultimately purposeful tuning of the macroscopic optical properties of the crystal. Herein, a new mixed alkali/alkaline-earth fluorooxoborate, Na2BaB12O18F4, was synthesized in a closed system. Na2BaB12O18F4 features a [B6O11F2] fundamental building unit (FBB), which polymerizes into two new (first example) independent interpenetrating three-dimensional (3D) B–O/F anionic networks constructed entirely from BO3 and BO3F units. Based on optical characterizations and the first-principles calculations, Na2BaB12O18F4 exhibits a moderate birefringence (0.054 @ 1064 nm) and a short ultraviolet (UV) cutoff edge (below 190 nm). The successful synthesis and characterization of Na2BaB12O18F4 may speed up the subsequent discovery of other mixed alkali/alkaline-earth metal fluorooxoborates.
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高影响因子
CATALYSIS TODAY
·
2019
·
IF 4.888
Tianyu Gao,Yongxuan Yin,Guanghui Zhu,Qiue Cao,Wenhao Fang
Oxidative transformations of HMF are key routes toward a wide variety of chemicals and biofuels through an environmental friendly process. Co 3 O 4 NPs decorated Mn-Co-O solid solution, donated as Co 3 O 4 /Mn X Co, was prepared by co-precipitation method and used as non-precious metal catalyst for base-free oxidation of HMF to FDCA in the presence of O 2 and water. Comprehensive characterizations such as XRD, H 2 -TPR, O 2 -TPD, XPS, NH 3 /CO 2 -TPD and TEM were used to study materials properties especially the oxygen mobility and acidity-basicity. The effect of Mn/Co molar ratio in catalyst and the reaction conditions were investigated and optimized. In addition, the kinetics of the reaction was monitored to reveal the reaction route and rate-determining step. The variation of Mn/Co molar ratio was found to affect not only HMF conversion but also distribution of products. When the Mn/Co ratio was of 0.2, the Co 3 O 4 /Mn 0.2 Co catalyst showed the optimal catalytic performance (i.e., >99% yield of FDCA obtained under 1 bar O 2 at 140 °C after 24 h) due to the highest content of both Lewis and Brønsted acid sites on the surface, leading to the strongest ability of HMF adsorption and COOH group formation, as well as the enhanced oxygen mobility. This catalyst was shown stable after a minor deactivation (≤8%) during six recycling uses and its activity can be entirely regenerated by calcination in air.
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MICROCHIMICA ACTA
·
2017
·Vol. 184
·期 6
·1791-1799
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IF 4.58
Wang Xiangyan,Sun Duanping,Tong Yanli,Zhong Yongsheng,Chen Zuanguang
A regenerable and ultrasensitive voltammetric biosensor is described for the determination of thrombin. It relies on a combination of (a) enzymatic catalysis, (b) a G-quadruplex/hemin DNAzyme system, and (c) AuPd nanoparticles for signal amplification. Poly(o-phenylenediamine) was decorated with AuPd nanoparticles and loaded with horseradish peroxidase (HRP) and thrombin aptamer (TBA), and the mixture was allowed to interact with hemin to form the G-quadruplex/hemin/HRP/AuPd/poly(o-phenylenediamine) bioconjugates. In the presence of thrombin, the bioconjugates remain immobilized on the surface of the modified glassy carbon electrode through a sandwich reaction. Poly(o-phenylenediamine) also acts as a redox mediator, and the electrochemical reaction of poly(o-phenylenediamine) in the presence of H 2 O 2 is efficiently catalyzed by HRP, AuPd nanoparticles and G-quadruplex/hemin as the peroxidase mimics. Thus, a remarkably amplified electrochemical signal is obtained by the triple catalytic amplification. The biosensor has a dynamic range that spans the 100 f. to 20 nM thrombin concentration range, and the detection limit is 20 fM. The biosensor can be regenerated by applying an electrochemical desorption technique that breaks the gold-thiol bond and releases the components from the surface. In our perception, the mediator-free and signal-amplified biosensor demonstrated here has a large potential with respect to the quantitation of thrombin in clinical samples.
Schematic of the assay: The peroxidase-like AuPd nanoparticles, G-quadruplex/hemin DNAzyme and horseradish peroxidase synergistically catalyze the electrochemical reaction of poly(o-phenylenediamine) in the presence of H 2 O 2 , thereby amplifying the electrochemical detection signal of thrombin.
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CARBOHYDRATE POLYMERS
·
2025
·
IF 12.5
Lijia Li,Xumei Feng,Mengjie Geng,Fei Teng,Yang Li
The advancement and utilization of functional foods hold the capacity to efficaciously enhance human nutrition and well-being. However, within the present epoch characterized by recurrent food safety and quality concerns, there exists a paucity of suitable food systems that are capable of concurrently amalgamating the merits of nutritional enrichment and high stability. Therefore, in this study, heteroprotein aggregates were synthesized with modified-soy lipophilic protein (SLP) and lysozyme (LY) as the main components. Subsequently, an interpenetrating network (IPN) was constructed using sugar beet pectin (SBP) and heteroprotein aggregates to form W-O-W emulsion gels. The heteroprotein aggregates formed by SLP and LY provided a stable oil-water interface, allowing the IPN to maximally confine the internal oil droplets and improve the mechanical properties and water retention capacity of the W-O-W emulsion gels. Meanwhile, the W-O-W emulsion gels also possessed pH-responsiveness, endowing them with the ability to modulate their self-morphology and network structure in accordance with pH fluctuations. Moreover, they possessed outstanding protective and slow-release efficacies, which were conducive to the targeted release of the delivered substances. Thus, W-O-W emulsion gels based on heteroprotein aggregation and SBP show great potential as an option for functional food applications.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Xiaoyan Feng,Qiong Wu,Li Li,Ping Wang,Qiang Wang,Jun Liang
Simulating natural photosynthesis to convert CO 2 and H 2 O into fuels achieving overall reaction is a promising solution for addressing environmental problems and energy crises. Constructing an S-scheme catalyst of two or more catalytic sites with rapid electron transfer and strong redox capability may be an effective strategy for coupling photocatalytic CO 2 reduction and H 2 O oxidation. Here, an oxygen vacancies-rich S-scheme semiconductor photocatalyst composed of monoclinic lead chromate oxide (Pb 2 (CrO 4 )O) coupled with Mn 3 O 4 quantum dots (QDs) (Pb 2 (CrO 4 )O@Mn 3 O 4 QDs) are synthesized and tested for photoconversion of CO 2 with H 2 O under visible light. Through the integration of Pb 2 (CrO 4 )O with Mn 3 O 4 QDs, the photocatalytic C1-evolution rate on Pb 2 (CrO 4 )O@Mn 3 O 4 QDs is radically increased by 6.0 and 8.1 times, which is much faster than that of pristine Pb 2 (CrO 4 )O and Mn 3 O 4 . The origin of the greatly raised activity is revealed by advanced characterizations, and in situ X-ray photoelectron spectroscopy (XPS) confirms the electron transport pathway in Pb 2 (CrO 4 )O@Mn 3 O 4 QDs with light illumination, unveiling the efficient spatial separation/transfer of charge carriers in oxygen vacancies-rich Pb 2 (CrO 4 )O@Mn 3 O 4 QDs S-scheme heterojunction. Consequently, powerful photoelectrons and holes accumulate in the Mn 3 O 4 conduction band and Pb 2 (CrO 4 )O valence band, respectively, exhibiting prolonged long lifetimes and facilitating their involvement in CO 2 photoreduction and H 2 O photooxidation through altering the interfacial charge dynamics.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Jinqiu Ye,Tiancheng Ge,Xin Qu,Mohamedazeem M. Mohideen,Ce Wang,Ping Hu,Yong Liu
The widespread application of aqueous zinc-ion batteries (AZIBs) is hindered by anode dendrite formation and side reactions, reducing cycling life and performance. This study introduces Bi-Bi₂O₃-loaded carbon nanofibers (Bi-Bi₂O₃@CNF) with hierarchical hollow structures and surface grooves fabricated via electrospinning, thermal treatment, and in situ growth. Experimental characterization and density functional theory reveal that the high surface area and fibrous network of Bi-Bi₂O₃@CNF enhance electron transport and electrolyte distribution, effectively reducing ohmic resistance and concentration polarization. This “Spatial Effect” provides ample space for uniform Zn deposition. Additionally, the in situ-grown Bi-Bi₂O₃, pyridinic nitrogen, pyrrolic nitrogen, and C─O─Bi bonds induce strong zinc affinity and electronegativity, generating an “Electrostatic Confinement Effect” that amplifies the “spatial effect” into a “Dual-Confinement Effect.” This synergy ensures uniform Zn deposition, suppresses dendrites and side reactions, and mitigates polarization. Compared to pure Zn anodes, Bi-Bi₂O₃@CNF reduces polarization overpotential by 17.6%, increases hydrogen evolution overpotential by 11.52%, and maintains a Coulombic efficiency of 98.8% for over 200 h. In full cells, Zn@Bi-Bi₂O₃@CNF//MnO₂ achieves 73.0% capacity retention after 1000 cycles at 1000 mA g⁻¹. This work provides a promising strategy for high-efficiency, durable, and safe AZIBs and offers valuable insights into the design of advanced aqueous energy storage materials.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Cong Wan,Jianwen Zhang,Honglei Zhang,Min Liu,Yiming Li,Zijun Yan,Chengheng Pang,Tao Wu
The catalytic reduction of CO₂ into valuable chemicals and fuels is a promising strategy for mitigating global carbon emissions. This study explores the synergistic co-reduction of CO₂ and H₂O using nanoscale zero-valent iron (NZVI) as a dual-function catalyst. Under light irradiation at 300 °C, the CO₂ reduction rate increased by more than 10-fold compared to dark conditions, demonstrating significant photothermal synergy. The study reveals that NZVI undergoes a phase transformation, where Fe₃O₄ functions as a photocatalyst while Fe 0 serves as an electron donor, enabling a unique dual-functionality that facilitates efficient electron transfer. The addition of 10 vol% H₂ stabilizes the reaction, leading to a higher and more consistent CO yield. When investigating the simultaneous reduction of CO₂ and H₂O, we discovered competitive adsorption and reaction pathways that significantly influence product distribution. In-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and density functional theory (DFT) calculations revealed three distinct mechanistic pathways for CO₂ conversion: direct C O bond cleavage, a carboxylate-mediated pathway and bicarbonate-mediated pathway, with the carboxylate and bicarbonate pathways being uniquely promoted by H and OH from H₂O dissociation. The addition of H₂O into the CO₂ and H₂ reaction significantly enhanced CH₄ generation due to the extra H source from H₂O dissociation. These findings offer valuable insights into the competitive mechanistic pathways of CO₂-H₂O co-reduction and contribute to the design of more efficient iron-based catalysts for sustainable CO₂ conversion and water splitting in energy and environmental applications.
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ACS Catalysis
·
2025
·
IF 13.1
Junjie Zhu,Hongyan Zhao,Qi Wang,Haijiao Kong,Xiaoyue Tu,Yu Zhang,Zhi-Hui Lv,Zhenbao Zhang,Xiangjian Liu,Zhen Xue,Lei Shi,Xin-Ming Hu,Jiawei Zhu,Heqing Jiang,Yongfa Zhu
Sn-based catalysts feature significant potential for acidic CO2 electroreduction (CO2RR) to HCOOH, but encounter unsatisfactory selectivity and poor stability, especially at high current densities. Here, we report In3+-induced In–O–Sn superexchange and oxygen vacancies synergistically enabling ampere-level, selective, and stable CO2-to-HCOOH electroreduction over Sn-based perovskite oxides in a strong acid. For the proof-of-concept catalysts of SrSn1–xInxO3−δ (x = 0.05, 0.1, and 0.2), In3+ introduction not only generates additional oxygen vacancies but also engenders marked In–O–Sn superexchange. This superexchange modulates electronic structures, including the upward-shifted band center (e.g., Sn 5p) and the strengthened Sn–O bond covalency. In HCOOH production, relative to the parent SrSnO3, the SrSn1–xInxO3−δ series demonstrate enhancements in activity and selectivity (more pronounced with In3+ content) while also featuring significantly boosted stability. In strong acid (pH = 1), SrSn0.8In0.2O3−δ achieves high HCOOH selectivity of 91.2% at 1 A cm–2 and a single-pass carbon efficiency of up to 81.0%, together with a steady operation over 80 h, outperforming previously reported Sn-based catalysts. Our experiments and theoretical calculations attribute these performance improvements to the following factors: the superexchange-shifted band centers and the additional oxygen vacancies synergistically facilitating *CO2 protonation to *OCHO; the superexchange-strengthened Sn–O bond covalency stabilizing the Sn–O lattice.
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Carbon Letters
·
2025
·
IF 5.8
Hu Chaoshuai,Liu Yuanxin,Zhang Jian,Zhu Yaming,Yin Xitao,Zhao Xuefei
Using durian shell as a carbon source and triethanolamine as a nitrogen dopant, nitrogen-doped carbon dots (N-CDs) were prepared via the hydrothermal method. First, by exploring different reaction times, reaction temperatures, and carbon source/dopant ratios to synthesize nitrogen-doped carbon dots, it is concluded that the best process conditions are 200 ℃, reaction time being 15h, and the dopant addition amount being 2mL. Structure and characteristics of the synthesized CDs were analyzed using X-ray photoelectron spectroscopy, Fourier-transform infrared, fluorescence (FL), ultraviolet–visible absorption, and Raman spectra. The N-CDs showed blue FL with a quantum efficiency of 4.28%. The FL characteristics of the N-CDs were utilized for ion detection, which demonstrated that \({\text{MnO}}_{4}^{ - }\) and \({\text{Cr}}_{{2}} {\text{O}}_{7}^{2 - }\) ions caused distinct FL quenching through static quenching, while other ions had no significant quenching effect. The detection limits for \({\text{MnO}}_{4}^{ - }\) and \({\text{Cr}}_{{2}} {\text{O}}_{7}^{2 - }\) were 37.5 and 46.2 nM, respectively. The N-CDs were subsequently employed to detect these ions in actual water samples, producing satisfactory results. Therefore, the preparation of N-CDs using durian shell as raw material and its application in practical detection work have good application feedback, which not only provides a new way for the reuse of fruit and vegetable wastes but also provides a new detection means for environmental monitoring pollutants.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Zhichen Liu,Tiantian Xiao,Xinru Wu,Cejun Hu,Xue Feng Lu,Hongwei Zhang,Jiujun Zhang,Xiaojun Bao,Pei Yuan
2,5-Furandicarboxylic acid (FDCA), a crucial precursor for synthesizing biodegradable polymers as a sustainable alternative to petroleum-derived plastics, has garnered significant interest for its production via electrolysis. However, this approach remains hindered by the inherent weak reactant-catalyst adsorption and sluggish interfacial kinetics. Herein, we report Cu-incorporated NiFe Prussian blue analogues (PBA) that enable rapid electrooxidation of 5-hydroxymethylfurfural (HMF) to FDCA with nearly 100 % conversion, selectivity, and Faradaic efficiency, even at an industrial-scale concentration of 100 mM. In situ Raman and electrochemical characterizations reveal that Cu-incorporation elongates Ni-N bonds and accelerates their reconstruction into defect-rich Ni 2+ -OH species, which undergo deprotonation to form highly active Ni 3+ -O species. X-ray technology and theoretical calculations show that the electronegative Cu 2+ prompts a shift of the d-band center of neighboring Ni atoms toward the Fermi level, thereby enhancing the adsorption of both hydroxyl (-OH) and aldehyde (-CHO) groups in HMF and thus accelerating electrooxidation of HMF to FDCA. Practical applicability using a continuous flow electrolyzer demonstrates the potential for industrial application, achieving a kilogram-scale FDCA production with 99 % purity and a yield exceeding 90 % over 1200 h. This work realizes the valence regulation of active sites in PBA through a cation engineering approach and verifies its feasibility in sustainable biomass electro-oxidation upgrading.
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APPLIED BIOCHEMISTRY AND BIOTECHNOLOGY
·
2021
·Vol. 195
·期 4
·2432-2450
·
IF 2.926
Zhang Yueqi,Ding Liping,Yan Zhenzhen,Zhou Dandan,Jiang Junwei,Qiu Jiarong,Xin Zhihong
An alkaline esterase, designated as EstXT1, was identified through functional screening from a metagenomic library. Sequence analysis revealed that EstXT1 belonged to the family VIII carboxylesterases and contained a characteristic conserved S-x-x-K motif and a deduced catalytic triad Ser56-Lys59-Tyr165. EstXT1 exhibited the strongest activity toward methyl ferulate at pH 8.0 and temperature 55°C and retained over 80% of its original activity after incubation in the pH range of 7.0–10.6 buffers. Biochemical characterization of the recombinant enzyme showed that it was activated by Zn 2+ and Co 2+ metal ion, while inhibited by Cu 2+ and CTAB. EstXT1 exhibited significant promiscuous acyltransferase activity preferred to the acylation of benzyl alcohol acceptor using short-chain p NP-esters (C2-C8) as acyl-donors. A structure–function analysis indicated that a WAG motif is essential to acyltransferase activity. This is the first report example that WAG motif plays a pivotal role in acyltransferase activity in family VIII carboxylesterases beside WGG motif. Further experiment indicated that EstXT1 successfully acylated cyanidin-3-O-glucoside in aqueous solution. The results from the current investigation provided new insights for the family VIII carboxylesterase and lay a foundation for the potential applications of EstXT1 in food and biotechnology fields.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2026
·
IF 5.4
Youjie Sheng,Haoyu Li,Hanling Zhang,Yang Li,Baohu Li,Li Ma
Nanoparticles (NPs) and polymers are frequently combined to improve firefighting foam performance, but whether the effect of polymer addition depends on NP type remains unclear. In this study, Al(OH)₃ and β-Al₂O₃ NPs were separately incorporated into an FS-50/APG-0810 surfactant system and further combined with xanthan gum (XG) or guar gum (GG). The foaming ability, rheology, and drainage resistance of the resulting foams were systematically compared, while crossover strain and modulus of cohesion (MOC) were used to characterize deformation tolerance and resistance to structural breakdown. Polymer addition produced opposite effects in the two NP systems: XG and GG generally weakened the rheological properties and drainage resistance of Al(OH)₃ NP-stabilized foams, but enhanced those of β-Al₂O₃ NP-stabilized foams. Selected β-Al₂O₃ formulations were further evaluated for fire suppression performance. Among the tested formulations, the β-Al₂O₃/XG foam achieved the shortest extinguishment time of 22 s, whereas the β-Al₂O₃/GG foam exhibited the longest burn-back time of 1243 s. Unlike previous studies focusing on individual NP or NP/polymer systems, this work demonstrates that polymer-induced foam regulation is strongly dependent on NP type and that nanoparticle/polymer combinations do not necessarily produce universal synergistic effects. These findings provide a basis for rational NP/polymer matching to balance rapid extinguishment and burn-back resistance in firefighting foam formulation. Download: Download high-res image (243KB) Download: Download full-size image
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危险品化学品经营许可证（带存储）