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ENVIRONMENTAL ENGINEERING SCIENCE · 2022 ·Vol. 39 ·期 1 ·56-63 · IF 2.172

The Role of Mn Doping on Ce-Based γ-Al2O3 Catalysts for Phenol Degradation

Jie Zhang,Ben Dong,Jing Liu,Wuxu Yang,Sijie Ge,Shilong He

In this article, Mn doping on Ce-based γ-Al2O3 (i.e., Mn-Ce-γ-Al2O3) was synthesized and then employed as catalysts to study the removal of phenol from aqueous solutions through catalytic ozonation process. The results showed that the phenol removal was remarkably increased to 97.50% if Mn-Ce-γ-Al2O3 was adopted as the catalyst. In addition, the kinetic rate of the reaction was increased, approximately, about 1.49 times when using Ce-γ-Al2O3 catalyst with Mn doping. Moreover, X-ray diffraction, transmission electron microscopy, Brunner-Emmet-Teller measurements, and X-ray photoelectron spectroscopy techniques were used to comprehensively characterize the physicochemical properties of the synthesized Mn-Ce-γ-Al2O3 catalyst, including the phases, morphologies, textural properties, and dispersity of the surface active species. More uniform channel mesoporous structures were obtained after Mn doping on Ce-γ-Al2O3, which could enhance the gas-liquid mass transfer rate, surface hydroxyl groups, Ce3+/Ce4+ ratio, and the formation of Mn-Ce solid solution. In this study, the effects of Mn doping on Ce-based γ-Al2O3 on phenol degradation were investigated and the removal mechanisms were suggested for a better understanding of the improved removal efficiency.

CAS / MDL: 1302-74-5
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Materials Advances · 2022 ·Vol. 3 ·期 5 ·2505-2514 · IF 0

Vaccine adjuvant platform and fluorescence imaging of amphiphilic γ-PGA-IMQ-LA-FL conjugates

Wenzhu Yin,Dechun Xuan,Bihua Deng,Mingxu Zhou,Fang Ma,Jinqiu Zhang,Yu Lu

Adjuvants have proven to be integral components in most vaccines for promoting appropriate immune responses at both innate and adaptive levels. Imiquimod (IMQ, R837), an agonist for Toll-like receptors 7 (TLR7), is a potent molecular activator of the innate immune system and has been developed as an adjuvant for immunotherapy. However, due to its pharmacokinetic profile, IMQ may induce strong local and systemic inflammatory reactions and is poorly tolerated. To overcome these hurdles, herein, we conjugate IMQ and lauryl alcohol (LA) to the backbone of biodegradable poly (γ-glutamic acid) (γ-PGA) to prepare an amphiphilic polymer (shortened to γ-PGA-IMQ-LA) with improved stability and biodistribution of IMQ. In order to investigate the distribution of the amphiphilic polymer in vitro and in vivo, fluorescein was grafted to the lateral chain to synthesize fluorescent-labeled γ-PGA-IMQ-LA-FL (shortened to FIP). The novel amphiphilic FIP polymer was characterized via1H NMR, FI-IR, UV-vis, fluorescence spectra and zeta potential. Using ovalbumin (OVA) as a model antigen and FIP as an adjuvant for immunization, the formulations of FIP + OVA in different dosages could significantly promote the production of OVA-specific IgG in mice and prolong immune responses with acceptable safety.

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Biomass Conversion and Biorefinery · 2022 · IF 4.05

Transfer hydrogenation of levulinic acid to γ-valerolactone over acid site-modified CuNi alloy

Yu Nanxi,Lu Houfang,Yang Wei,Zheng Yuxin,Hu Qiang,Liu Yingying,Wu Kejing,Liang Bin

In the process of converting biomass into high value-added chemicals, transfer hydrogenation as a mild hydrogenation method has attracted more and more attention. The catalysts with hydrogenation sites (nano CuNi alloy) and acid sites (Al oxide) highly dispersed on the surface of a stable support (active carbon) were prepared and the importance of acid sites for the activity of CuNi catalysts in transfer hydrogenation was demonstrated. The catalysts showed promising catalytic activity on the transfer hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL). The CuNi-1Al/AC with 5 wt.% CuNi alloy and 5 wt.% Al got 97.2% GVL yield and 100% LA conversion at 220 ℃ in isopropanol for 2 h. The high activity of the catalyst is attributed to the promoted esterification by the supported acid sites. The Al-modified catalyst also showed activity for esterification reaction in different alcohol hydrogen donors. The catalyst occurs inactive during the cycle due to the shedding of the active components, and the stability of catalyst is effectively improved by a stepwise impregnation. Graphical abstract

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Carbon Resources Conversion · 2022 · IF 0

Synthesis of γ-MnS/nanoporous carbon/reduced graphene oxide composites for high-performance supercapacitor

Abiola Ganiyat Olatoye,Jie Zhang,Qianyu Wang,Erping Cao,Wenli Li,Emmanuel Oluwaseyi Fagbohun,Yanbin Cui

In the present work, nanoporous carbon (NPC) was prepared from a metal–organic framework (zeolite imidazolate framework 8, ZIF-8). Different concentrations of graphene oxide (GO) were used to make NPC/reduced graphene oxide (NPC/rGO-x, x = 0.5, 1.0, 1.5, and 2.0) composites, and then γ-MnS/NPC/rGO-1 composite was synthesized via a simple hydrothermal technique. The electrochemical characteristics of porous carbon composites (NPC/rGO-x) and γ-MnS/NPC/rGO-1 electrodes were investigated by galvanostatic charge and discharge, cyclic voltammetry, and electrochemical impedance spectroscopy. NPC/rGO-1 showed the highest specific capacitance of 207 F/g at 0.5 A/g. Also, the γ-MnS/NPC/rGO-1 electrode demonstrates exceptional electrochemical performance with a high specific capacitance of 300 F/g at 0.5 A/g and impressive cyclic stability of 70% capacitance retention after 10,000 cycles at 1 A/g. As a result, this study demonstrates that γ-MnS/NPC/rGO-1 electrode can be considered a promising candidate for high-performance supercapacitors.

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Biomaterials Science · 2022 ·Vol. 10 ·期 15 ·4218-4227 · IF 7.59

In situ forming injectable γ-poly(glutamic acid)/PEG adhesive hydrogels for hemorrhage control

Huijun Ye,Yiwen Xian,Shurong Li,Chong Zhang,Decheng Wu

Rapidly in situ forming adhesive hydrogels are promising candidates for efficient hemostasis due to their easy administration and minimal invasion. However, development of biocompatible and high-performance hemostatic hydrogels without any additional toxic agents remains a challenge. Herein, a series of novel injectable adhesive hydrogels based on N-hydroxysuccinimide (NHS) modified γ-poly(glutamic acid) (γPGA–NHS) and tetra-armed poly(ethylene glycol) amine (Tetra-PEG-NH2) were developed. Among all samples, PGA10–PEG15 and PGA10–PEG20 hydrogels with higher PEG contents exhibited rapid gelation time (<20 s), strong mechanical strength (compression modulus up to ∼75 kPa), good adhesive properties (∼15 kPa), and satisfactory burst pressure (∼18–20 kPa). As a result, PGA10–PEG15 and PGA10–PEG20 hydrogels showed a remarkable reduction in hemostasis time and blood loss compared with gauze and fibrin glue. More importantly, the PGA10–PEG20 hydrogel was also successfully used to seal femoral arterial trauma. Subcutaneous implantation experiments indicated a good biocompatibility of the hydrogels in vivo. All these results strongly support that the developed PGA–PEG hydrogels could serve as promising hemostatic agents in emergency and clinical situations.

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CARBOHYDRATE POLYMERS · 2022 · IF 10.723

Aggregation-induced emission (AIE) nanoparticles based on γ-cyclodextrin and their applications in biomedicine

Lianxiong Guan,Zhi Zeng,Wei Liu,Tengfei Wang,Shiyao Tian,Sheng Hu,Dating Tian

Amphiphilic AIE nanoparticles (CD-TPE) were obtained by linking γ-cyclodextrin (γ-CD) and 1, 2-diphenyl-1, 2-( p -hydroxyphenyl)-ethylene (OH-TPE-OH) by an esterification reaction using hexamethylene diisocyanate (HMDI) in a one-step process. The CD-TPE was characterized by FTIR, 13 C NMR, DSC , XRD, particle size analysis , TEM, and FL. The obtained CD-TPE had good water dispersibility and could self-assemble into AIE nanoparticles. The large cavity of CD-TPE provided convenient conditions for the loading of doxorubicin (DOX) and slow-release DOX with the loading and release rates of 67.4 % and 71.3 % (pH = 5.4), respectively. The DOX release kinetic model was suitable for the Bhaskar model. Cytotoxicity analysis and cell imaging of CD-TPE were performed, showing that CD-TPE has good biocompatibility and excellent cell imaging performance. Moreover, both in vitro and in vivo antitumor experiments showed that CD-TPE has promising applications in drug delivery.

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CARBOHYDRATE POLYMERS · 2021 · IF 9.381

γ-Cyclodextrin-based polypseudorotaxane hydrogels for ophthalmic delivery of flurbiprofen to treat anterior uveitis

Guihua Fang,Qiuxiang Wang,Xuewen Yang,Yu Qian,Guowei Zhang,Bo Tang

Anterior uveitis is a sight-threatening inflammation inside the eyes. Conventional eye drops for anti-inflammatory therapy need to be administered frequently owing to the rapid elimination and corneal barrier. To address these issues, polypseudorotaxane hydrogels were developed by mixing Soluplus micelles (99.4 nm) and cyclodextrins solution. The optimized hydrogels exhibited shear-thinning and sustained release properties. The hydrogels exhibited higher transcorneal permeability coefficient (P app , 1.84 folds) than that of drug solutions. Moreover, animal study indicated that the hydrogels significantly increased the precorneal retention (AUC, 21.2 folds) and intraocular bioavailability of flurbiprofen (AUC Aqueous humor , 17.8 folds) in comparison with drug solutions. Importantly, the hydrogels obviously boosted anti-inflammatory efficacy in rabbit model of endotoxin-induced uveitis at a reduced administration frequency. Additionally, the safety of hydrogels was confirmed by cytotoxicity and ocular irritation studies. In all, the present study demonstrates a friendly non-invasive strategy based on γ- CD-based polypseudorotaxane hydrogels for ocular drug delivery.

CAS / MDL: 81-88-9
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JOURNAL OF CONTROLLED RELEASE · 2021 · IF 9.776

Platelet-armored nanoplatform to harmonize janus-faced IFN-γ against tumor recurrence and metastasis

Qian Li,Yaxin Zhou,Weidong He,Xiaomeng Ren,Mengzhu Zhang,Yue Jiang,Zhaocai Zhou,Yuxia Luan

Interferon-γ (IFN-γ) plays contradictory roles in tumor immunology: (I) to activate positive host's immunity for eliminating tumor; (II) to induce negative adaptive immune resistance via up-regulating programmed death ligand-1 (PD-L1) expression for tumors to evade immune surveillance. The negative feedback loop between the IFN-γ recovery and the IFN-γ-induced PD-L1 up-regulation puts postoperative adjuvant chemotherapy into a dilemma. It is of great significance but challenging to manipulate the double-edge effects of IFN-γ against postoperative tumor progression. Herein, a platelet-engineered nanoplatform ( [email protected] NPs) capable of harmonizing janus-faced nature of IFN-γ was designed via uniquely co-assembling doxorubicin (Dox) and cyclin-dependent kinase 5 inhibitor roscovitine (Rosco) with platelet membrane fragment (PMF) as the particulate stabilizer . With [email protected] NPs navigated by PMF to residual tumor, the Dox-activated immune response recovered IFN-γ secretion for positive host's immunity, while the IFN-γ-induced negative adaptive immune resistance was potently overcome by Rosco via disabling PD-L1 expression without dependence of IFN-γ stimulation. The negative feedback loop between IFN-γ recovery and PD-L1 up-regulation was thus potently disrupted in postoperative adjuvant chemotherapy. Our [email protected] NPs not only harmonized janus-faced nature of IFN-γ to effectively regulate postoperative tumor progression, but also illustrated an innovative strategy for high-drug-loading biomimic nanoplatform.

CAS / MDL: 1069-79-0 298-93-1
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Environmental Science-Nano · 2021 ·Vol. 8 ·期 12 ·3833-3845 · IF 8.131

Micromotor-assisted fluorescence detection of Hg2+ with bio-inspired AO–Mn2O3/γ-AlO(OH)

Tingting Li,Yangsai Lyu,Jia Li,Chengyan Wang,Ningning Xing,Jie Yang,Min Zuo

Micromotors have held great promise for environmental treatment due to their unique self-propelled movement that can significantly accelerate the chemical process in solution. Herein, we have developed a new AO–Mn2O3/γ-AlO(OH) fluorescent micromotor using renewable and uniquely hollow kapok fibers as biological templates. The AO–Mn2O3/γ-AlO(OH) micromotor was powered by the asymmetric decomposition of hydrogen peroxide fuel catalyzed by Mn2O3, reaching a maximum speed of 139.6 μm s−1 in 3% H2O2 solution. The micromotor revealed a markedly enhanced fluorescence effect compared to both pure AO solution and non-micromotor counterparts and exhibited excellent selectivity and sensitivity for Hg2+ detection. The detection range and limit for Hg2+ were 5 × 10−8–5 × 10−5 M and 2.25 × 10−8 M, respectively. The enhanced Hg2+ sensing benefited from the synergy of enhanced fluorescence via the inhibition of the dimerization of AO, fluorescence quenching induced by charge transfer and the enhanced contact between the micromotor and Hg2+ ions resulted from the self-propelled motion. This micromotor-assisted fluorescence detection idea provided a new strategy for the development of sensors with high sensitivity.

CAS / MDL: 155135-61-8
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ACS Sustainable Chemistry & Engineering · 2021 · IF 8.198

Low Loading of CoRe/TiO2 for Efficient Hydrodeoxygenation of Levulinic Acid to γ-Valerolactone

Zuojun Wei,Qing Li,Yuran Cheng,Mei Dong,Zuyi Zhang,Xinmiao Zhu,Yingxin Liu,Yong Sun

CoRe bimetallic catalysts with low loading were designed for hydrodeoxygenation of levulinic acid to γ-valerolactone. Results show that the 1 wt % Co0.5Re0.5/TiO2 catalyst achieved the highest yield of γ-valerolactone (>99%) at 220 °C, 3 h, a 1,4-dioxane solvent and Co/levulinic acid molar ratio of 1:1760, with a turnover frequency (TOF) of 1328 h–1. The catalyst can be reused four times with only slight activity loss. The catalyst was characterized with various physicochemical measurements, and its adsorption styles with H2 and levulinic acid were calculated by density functional theory. The results reveal that four main factors are related to its excellent catalytic performance. First, the Re oxides synergize with Co by spillover of the dissociated H atoms, which increases the apparent dispersion of Co and promotes the reaction. Second, the low loading of 1 wt % allowed the metal nanoparticles to be well dispersed with a very fine size of ca. 1.24 nm, which may expose more active sites to the substrate and result in a higher catalytic efficiency. Third, CoRe formed an amorphous alloy with the formula Co-ReO1.6, which showed a synergistic effect during the reaction. Finally, the TiO2 support was nonporous and hydrophilic, which would be beneficial for the mass diffusion of the reaction components to be adsorbed/desorbed onto the vicinity of the metallic active sites and lead to a high TOF in the hydrodeoxygenation process.

CAS / MDL: 123-76-2 108-29-2
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Theranostics · 2021 · IF 11.556

γ-Glutamyl transpeptidase-activatable near-infrared nanoassembly for tumor fluorescence imaging-guided photothermal therapy

Fangyuan Zhou,Shikui Yang,Chao Zhao,Wangwang Liu,Xufeng Yao,Hui Yu,Xiaolian Sun,Yi Liu

Rationale: Precise treatment of tumors is attracting increasing attention. Molecular probes simultaneously demonstrating the diagnostic signal and pharmacological effect in response to tumor microenvironment are highly desired. γ-glutamyl transpeptidase (GGT) is a biomarker with significantly up-regulated expression in the tumor area. We developed a GGT responsive near-infrared (NIR) nanoassembly for tumor-specific fluorescence imaging-guided photothermal therapy. Methods: The GGT responsive NIR probe was constructed by conjugating GGT-specific substrate γ-glutamic acid (γ-Glu) with cyanine fluorophore (NRh-NH 2 ) via amide reaction. The resulting NRh-G spontaneously assembled into nanoparticles (NRh-G-NPs) around 50 nm. The NPs were characterized and the properties evaluated in the presence or absence of GGT. Subsequently, we studied fluorescence imaging and photothermal therapy of NRh-G-NPs in vitro and in vivo . Results: NRh-G-NPs, upon specific reaction with GGT, turned into NRh-NH 2 -NPs, showing a ~180-fold fluorescence enhancement and excellent photothermal effect recovery. NRh-G-NPs could selectively light up U87MG tumor cells while their fluorescence was weak in L02 human normal liver cells. The NPs also showed excellent tumor cell ablation upon laser irradiation. After intravenous injection into tumor-bearing mice, NRh-G-NPs could arrive in the tumor area and specifically light up the tumor. Following laser irradiation, the tumor could be completely erased with no tumor reoccurrence for up to 40 days. Conclusions: NRh-G-NPs were specifically responsive to GGT overexpressed in U87MG tumor cells and selectively lit up the tumor for imaging-guided therapy. Besides, the recovery of photothermal property in the tumor area could improve cancer therapy precision and decreased side effects in normal tissues.

CAS / MDL: 305808-27-9 532-94-5
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RENEWABLE ENERGY · 2021 · IF 8.001

Improving enzymatic saccharification of Chinese silvergrass by FeCl3-catalyzed γ-valerolactone/water pretreatment system

Junwei Yao,Xiaobao Xie,Qingshan Shi

In this work, we report that FeCl 3 , a benign Lewis acid, could be used as a catalyst in the γ-valerolactone (GVL)/H 2 O solvent system to facilitate efficient pretreatment of Chinese silvergrass. The results showed that approximately 87.8% of xylan and 75.8% of lignin were removed by 80% GVL under 170 °C using 50 mM FeCl 3 as a catalyst. The solubilized carbohydrate fractions in the pretreatment liquor were mainly composed of monosaccharides (glucose and xylose) rather than oligosaccharides (glucose oligomers and xylose oligomers) and inhibitors (furfural, hydroxymethylfurfural, formic acid and acetic acid). Moreover, FeCl 3 decreased the transesterification of GVL with hydroxyl groups on the cellulose surface and resulted in more easily degraded cellulose. Approximately 96.5% of cellulose and 92.2% of xylan in the pretreated Chinese silvergrass were converted to fermentable monosaccharides by 10 FPU/g cellulases . This study indicated that FeCl 3 -catalyzed GVL solvent could efficiently deconstruct biomass and increase the cellulose digestibility, which provided a novel, GVL-based pretreatment system for processing biomass.

CAS / MDL: 108-29-2
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