Molecular Catalysis
·
2022
·
IF 5.089
Canshuo Gu,Lungang Chen,Yong Liu,Xinghua Zhang,Jianguo Liu,Qi Zhang,Chenguang Wang,Longlong Ma
The production of furanic biofuel 2-methyltetrahydrofuran (2-MTHF) has been studied by hydrodeoxygenation of biomass-derived levulinic acid (LA) over bimetallic NiCo/γ-Al 2 O 3 catalyst. The contents of Ni and Co in NiCo/γ-Al 2 O 3 were investigated. The Ni 5 Co 25 /γ-Al 2 O 3 catalyst gave high activity in hydrodeoxygenation of LA with a 73.4% yield of 2-MTHF under optimal conditions. The crystal phase, valence states, acidity and basicity of catalysts were measured by multiple characterizations to understand the relationships among 2-MTHF yields and catalyst properties. XPS characterization revealed that the number of metal oxides increased on bimetallic catalysts while the reduced metals occupied on monometallic catalysts. The bimetallic catalysts also presented increased acidity than that of monometallic catalysts. These distinct properties were also observed among bimetallic catalysts with different contents of Ni and Co, which were responsible for different performances. Besides, the solvent effect on the structure of 1,4-pentanediol, which was further converted to 2-methyltetrahydrofuran, was disclosed by molecular dynamics simulations.
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ACS Applied Nano Materials
·
2022
·
IF 6.14
Chengyan Wang,Yangsai Lyu,Jia Li,Li Li,Tingting Li,Jie Yang,Ningning Xing,Xiaolei Zhang
Excessive fluorine can cause a serious threat to human health. It is significant but challenging to develop a straightforward and rapid way to simultaneously detect and remove excess F– from water. Herein, we presented a three-dimensional (3D) hierarchical UiO-66-NH2 nanoparticle/γ-AlO(OH) nanowire hybrid synthesized by a facile biotemplate route for simultaneous detection and removal of F– from water. We elaborately assembled two kinds of materials in a bioinspired 3D hierarchical structure as a functional unit to achieve detection and removal of dual functions. The outer UiO-66-NH2 nanoparticles served as a fluorescent sensor to detect and capture F– via a strong fluorescence enhancement effect caused by the electron transfer from F– and γ-AlO(OH) and acted as the capture unit of F–. The inner γ-AlO(OH) nanowire layer served as a F– absorbent through ion exchange between F– and γ-AlO(OH). The resulting UiO-66-NH2 nanoparticle/γ-AlO(OH) nanowire hybrid displayed excellent selectivity and sensitivity for F– detection (the detection range was 0–5 mM and the limit of detection was as low as 0.77 μM) and high capacity for F– removal (the maximum equilibrium adsorption capacity qmax was as high as 87.0 mg g–1). This dual-function material provided a strategy for simultaneously selective sensing and efficient removal of anionic pollutants from water.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Zhuan Wang,Bo Yang,Xueying Zhao,Yushuai Chen,Dandi Wei,Lijuan Zhang,Xintai Su
Oxygen evolution reaction (OER) is the bottleneck of photocatalytic water splitting due to the slow four-electron transfer kinetics, and the construction of ultrathin materials is considered to be an effective means to solve the above problem. Herein, ultrathin γ-Fe 2 O 3 nanosheets (Fe 2 O 3 -NS) were prepared by a facile solution reduction-low temperature calcination method. The prepared photocatalyst has a leaf-like morphology with an average thickness of 2.0 nm and a large number of slit-like pores. Compared with γ-Fe 2 O 3 bulk, Fe 2 O 3 -NS exhibits excellent photocatalytic OER activity. The apparent quantum yield (AQE) and oxygen yield (measured at 420 nm) are 12.95% and 57.04%, respectively. The OER efficiency is superior to those reported iron oxide photocatalysts. This excellent performance may benefit from the ultrathin porous structure, appropriately narrow bandgap, and abundant oxygen vacancies . In addition, the photocatalyst shows good cycling stability, retaining 91.5% of the initial capacity in the fifth cycle test, which may be attributed to the magnetic cycling capability and good structural stability. This study confirms that Fe 2 O 3 -NS is a competitive candidate material for photocatalytic oxygen evolution and provides ideas for the design and construction of other defect-rich metal oxide nanosheets.
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Biotechnology for Biofuels and Bioproducts
·
2024
·Vol. 17
·期 1
·1-16
·
IF 3.3
Wei Xiaoyu,Yang Lijie,Chen Zhen,Xia Wenhao,Chen Yongbin,Cao Mingfeng,He Ning
Background The structural diversity of extracellular polymeric substances produced by microorganisms is attracting particular attention. Poly-gamma-glutamic acid (γ-PGA) is a widely studied extracellular polymeric substance from Bacillus species. The function of γ-PGA varies with its molecular weight (Mw). Results Herein, different endogenous promoters in Bacillus licheniformis were selected to regulate the expression levels of pgdS , resulting in the formation of γ-PGA with Mw values ranging from 1.61 × 10 3 to 2.03 × 10 4 kDa. The yields of γ-PGA and exopolysaccharides (EPS) both increased in the pgdS engineered strain with the lowest Mw and viscosity, in which the EPS content was almost tenfold higher than that of the wild-type strain. Subsequently, the compositions of EPS from the pgdS engineered strain also changed. Metabolomics and RT-qPCR further revealed that improving the transportation efficiency of EPS and the regulation of carbon flow of monosaccharide synthesis could affect the EPS yield. Conclusions Here, we present a novel insight that increased pgdS expression led to the degradation of γ-PGA Mw and changes in EPS composition, thereby stimulating EPS and γ-PGA production. The results indicated a close relationship between γ-PGA and EPS in B. licheniformis and provided an effective strategy for the controlled synthesis of extracellular polymeric substances.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2025
·
IF 8.5
Tianyuan Xiao,Jiahui Song,Wenchao Jia,Yanning Sun,Yanzhu Guo,Pedram Fatehi,Haiqiang Shi
The chemical bond cleavage of lignin is a research focus for achieving depolymerized lignin for such applications as adhesives, fuels, fertilizers, etc. The depolymerization of an industrially available sustainable material, i.e., industrial alkali lignin, in LiBr·3H 2 O/HBr-γ-valerolactone (GVL) was systematically investigated in this study. It was observed that using 3/1 mL/g of HBr/lignin and 8/1 mL/g of GVL/lignin at 110 °C for 90 min, i.e., optimized conditions, resulted in lignin derivatives with an M w of 1889 g/mol and M n of 895 g/mol. The characteristics of the products were studied using FTIR, NMR, SEM, and DLS techniques. The results confirmed that the Hibbert-ketone end group was formed, while the structure of the aromatic ring was not changed on the depolymerized lignin. After the depolymerization process, the hydroxyl content in lignin increased from 1.91 mmol/g to 2.96 mmol/g. The product derived from the LiBr·3H 2 O/HBr-GVL depolymerization system displayed a spherical particle morphology. The addition of GVL to lignin depolymerization processes improved the bonding between lignin and inorganic molten salts, thereby promoting the acid-catalyzed cleavage of aryl ether bonds in lignin. Current research supports the conclusion that LiBr·3H 2 O/HBr-GVL lignin depolymerization is a sustainable and effective chemical pathway for generating depolymerized lignin.
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高影响因子
BIOCONJUGATE CHEMISTRY
·
2020
·
IF 4.031
Siqin Ye,Shijie Wang,Dingyao Gao,Ke Li,Qingzhu Liu,Bainian Feng,Ling Qiu,Jianguo Lin
γ-Glutamyltranspeptidase (GGT) is a cell -membrane-associated enzyme which has been recognized as a promising biomarker for the diagnosis of many malignant tumors. Herein, we rationally designed a fluorine-18 labeled small-molecule probe, [18F]γ-Glu-Cys(StBu)-PPG(CBT)-AmBF3 (18F-1G), by applying a biocompatible CBT-Cys condensation reaction and ingeniously decorating it with a GGT-recognizable substrate, γ-glutamate (γ-Glu), for enhancing PET imaging to detect GGT level of tumors in living nude mice. The probe had exceptional stability at physiological conditions, but could be efficiently cleaved by GGT, followed by a reduction-triggered self-assembly and formation of nanoparticles (NPs) progressively that could be directly observed by transmission electron microscopy (TEM). In in vitro cell experiments, 18F-1G showed GGT-targeted uptake contrast of 2.7-fold to that of 18F-1 for the detection of intracellular GGT level. Moreover, the higher uptake in GGT overexpressed HCT116 tumor cells (∼4-fold) compared to GGT-deficient L929 normal cells demonstrated that 18F-1G was also capable of distinguishing some tumor cells from normal cells. In vivo PET imaging revealed enhanced and durable radioactive signal in tumor regions after 18F-1G coinjecting with 1G, thus allowing real-time detection of endogenous GGT level with high sensitivity and noninvasive effect. We anticipated that our probe could serve as a new tool to investigate GGT-related diseases in the near future.
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RSC Advances
·
2020
·Vol. 10
·期 29
·17154-17162
·
IF 3.119
Ang Li,Yuxiang Liu,Xuejun Xu,Yuanyuan Zhang,Zhichun Si,Xiaodong Wu,Rui Ran,Duan Weng
Constructing Z-scheme heterojunctions is considered as an effective strategy to obtain catalysts of high efficiency in electron–hole separation in photocatalysis. Unfortunately, suitable heterojunctions are difficult to fabricate because the direct interaction between two semiconductors may lead to unpredictable negative effects such as electron scattering or electron trapping due to the existence of defects which causes the formation of new substances. Furthermore, the van der Waals contact between two semiconductors also results in bad electron diffusion. In this work, a MOF-derived carbon material as a Z-scheme photocatalyst was synthesized via one-step thermal treatment of MoS2 dots @Fe-MOF (MIL-101). Under visible light irradiation, the well-constructed Z-scheme (MoS2, γ-Fe2O3)/graphene photocatalyst shows 2-fold photocatalytic oxygen evolution activity (4400 μmol g−1 h−1) compared to that of γ-Fe2O3/graphene (2053 μmol g−1 h−1). Based on ultraviolet photoelectron spectrometry (UPS), Mott–Schottky plot, photocurrent and photoluminescence spectroscopy (PL) results, the photo-induced electrons from the conduction band of γ-Fe2O3 could transport quickly to the valence band of MoS2 via highly conductive graphene as an electron transport channel, which could significantly enhance the electron–hole separation efficiency as well as photocatalytic performance.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2020
·
IF 6.551
Caifeng Zhao,Yahui Yang,Lin Luo,Sai Shao,Yiji Zhou,Ying Shao,Faqi Zhan,Jian Yang,Yaoyu Zhou
Oxygen vacancies and Ti 3+ defects in anatase TiO 2 have attracted great attention to address the insufficient optical absorption and photoinduced charge-carrier separation in photocatalysis . In this study, we demonstrate a superficial and innovative approach for synthesizing anatase TiO 2 nanoparticles with abundant oxygen vacancies via γ-ray irradiation reduction at room temperature. X-ray photoelectron spectroscopy (XPS) and electron paramagnetic resonance (EPR) confirm that oxygen vacancies and Ti 3+ defects can be quantitatively and extensively obtained by merely regulating the irradiation dosage. Photoelectrochemical measurements suggest that oxygen vacancies and Ti 3+ defects promoted the separation of electron-hole pairs and then enhanced the photocatalytic degradation performance for organic pollutant. In comparison with TiO 2 (no irradiation), the sample (49.5 kGy irradiation) exhibited a 20.0-fold enhancement in visible-light decomposition of phenol. In addition, the results of scavenge experiments and mechanism analysis revealed that O 2 − are the dominant active species. The excited electrons generated at the conduction band and oxygen vacancy level of TiO 2−x -49.5 conspicuously contributes to generate much more ·O 2 − species. This novel study shows at room temperature, the γ-ray approach of irradiation leads to faster formation and quantification of oxygen vacancies in the semiconductor materials .
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Advanced Science
·
2025
·Vol. 12
·期 26
·2501875
·
IF 14.1
Bao Xiao,Yuquan Wang,Ning Ding,Haoming Qin,Nannan Shen,Xuchang He,Qihao Sun,Yihui He
Perovskite semiconductor cesium lead bromide (CsPbBr 3 ) has demonstrated great promise as a new-generation gamma-ray detector. However, substantial challenges still present in reproducibly achieving optimal spectroscopic performance. The specific strategy for producing spectroscopic-grade CsPbBr 3 crystals with high reproducibility and uniformity are still not clarified. Herein, efficient zone refining processing is developed for CsPbBr 3 crystals that facilitates impurity segregation to achieve an ultrahigh purity level of ≈1.42 ppm, therefore lowers trap density and balances charge transport. In a typical 30 mm diameter zone-refined CsPbBr 3 ingot, all wafers exhibited remarkable energy resolutions of 6–12% and 3–8% for 241 Am and 57 Co γ-rays under comparable electric fields. The crystals also exhibited an ambipolar charge transport characteristic, resemble to elemental semiconductors, with equivalent hole and electron mobility-lifetime products averaging 5.42 × 10 −3 and 2.27 × 10 −3 cm 2 ∙V −1 , respectively. Consequently, over 95% of wafers achieved energy resolutions below 5% whereas 70% exceeded 3% for 137 Cs γ-rays, demonstrating exceptional reproducibility and uniformity. Notably, a champion energy resolution of 1.3% with an outstanding photopeak-to-Compton (P/C) ratio of ≈5.3 is attained in an ambipolar planar detector. It is anticipated that this work shall expedite scalable manufacturing and practical applications of CsPbBr 3 detectors.
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PARTICLE & PARTICLE SYSTEMS CHARACTERIZATION
·
2017
·Vol. 34
·期 3
·1600430
·
IF 4.474
Jie Wang,Jielin Rong,Zhong Fang,Mozhen Wang,Anila Asif,Qichao Wu,Xiao Zhou,Xuewu Ge
Biosafe nanoparticles with strong near-infrared (NIR) light photothermal conversion effect can bring effective hyperthermia as one of the promising approaches in cancer therapy. In this work, a new facile and green preparation method of polypyrrole (PPy) nanoparticles based on 60 Co γ-ray radiation on a simple air-saturated strong acidic aqueous solution of pyrrole (pH ≤ 1) is studied. According to the MCAP-FACSIMILE simulation on the concentrations of the radiolysis products of water at the presence of H + and O 2 , the main strong oxidative radiolysis products · OH and H 2 O 2 rapidly induce the polymerization of pyrrole. The size of the prepared PPy nanoparticles is about several tens of nanometers and can be controlled by the pH, the concentration of the stabilizer poly(vinyl alcohol), and the absorbed dose rate (the amount of energy absorbed per unit mass of the irradiated material within per unit of time). The PPy nanoparticles show rapid and remarkable NIR (808 nm) photothermal conversion efficiency up to 40.1% in water. Furthermore, the in vitro and in vivo experiments confirm that the prepared PPy nanoparticles exhibit enough strong NIR photothermal effect in tumor cells (4T1 and HeLa) and show a promising prospect as the NIR photothermal agent for the future cancer therapy.
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RSC Advances
·
2013
·Vol. 3
·期 26
·10277-10284
·
IF 2.562
Xing Tang,Lei Hu,Yong Sun,Geng Zhao,Weiwei Hao,Lu Lin
A green and efficient process was developed for the conversion of biomass-derived ethyl levulinate (EL) into γ-valerolactone (GVL) using supercritical ethanol as the hydrogen donor and the reaction medium over low-cost and eco-friendly ZrO2 catalysts, which were prepared by the precipitation method and characterized by BET, SEM, XRD, FT-IR, TGA-DTA, TPD-NH3 and TPD-CO2. The results indicated that amorphous ZrO2 with a high specific surface area and a large number of acid–base sites exhibited the highest catalytic activity, an excellent GVL yield of 81.5% with 95.5% EL conversion was achieved at 523 K over 3 h. In addition, combined with the results of poisoning experiments, a plausible mechanism of catalytic transfer hydrogenation (CTH) via a six-membered ring transition state was also presented.
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Nanoscale
·
2021
·Vol. 13
·期 31
·13310-13317
·
IF 7.79
Mengmeng Gao,Xiaolei Wu,Shuhong Yi,Shuwei Sun,Caiyan Yu,Dong Yan,Hui Ying Yang,Huiling Zhao,Ying Bai
Upgrading liquid electrolytes with all-solid-state electrolytes (ASEs) or quasi-solid-state electrolytes (QSEs) for solid-state batteries (SBs) have emerged not only to address the intrinsic disadvantages of traditional liquid lithium ion batteries, but also to offer more possibilities for the development of new battery chemistries. In this work, a novel rambutan-like yolk–shell-structured porous γ-AlOOH microsphere with a large specific surface area of 262.92 m2 g−1 was firstly obtained by a simple hydrothermal synthesis route, which was then utilized as a robust framework to assemble QSE via encapsulating abundant liquid electrolyte (LE). The obtained γ-AlOOH-QSE exhibits a high ionic conductivity of 4.0 × 10−3 S cm−1, a large lithium ion transference number (tLi+) of 0.76, as well as a wide electrochemical window of 4.72 V vs. Li/Li+. Moreover, the assembled cell of LiFePO4/γ-AlOOH-QSE/Li could maintain a high specific capacity of 144.4 mA h g−1 even after 120 cycles with almost negligible capacity decay, which could be mainly attributed to the excellent interfacial compatibility, prominent performance in suppressing lithium dendrite growth upon cycling (rigid characteristic), as well as the high ionic conductivity of γ-AlOOH-QSE (intrinsic advantage). This work could not only expand the applications of QSE with cost-effective aluminum-based oxides with facile fabrication strategy, but also will shed light on the construction of SEs with more integrated QSEs and ASEs in the field of advanced energy storage.
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