APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Xiaolei Bao,Huiliang Li,Zeyan Wang,Fengxia Tong,Mu Liu,Zhaoke Zheng,Peng Wang,Hefeng Cheng,Yuanyuan Liu,Ying Dai,Yuchen Fan,Zhiyong Li,Baibiao Huang
Photocatalytic selective oxidation of alcohols into corresponding aldehydes has received enormous attention. However, it remains a great challenge to explore photocatalysts with high conversion efficiency and selectivity. Herein, we developed a composite consisted of TiO 2 and Ti 3 C 2 through a simple calcination of Ti 3 C 2 nanosheets. It was found that Ti 3 C 2 could stabilize the oxygen vacancies and Ti 3+ species in the TiO 2 /Ti 3 C 2 composite, which could subsequent promote the production of active intermediates during the photocatalytic oxidation of benzyl alcohol (BA) to benzaldehyde (BAD). Additionally, the valence band of TiO 2 in the composites was found to be up-shifted, which would avoid the further oxidation of BAD and enhance selectivity. As a result, the optimal composite exhibits the BA conversion efficiency of 97 % and BAD selectivity of 98 %, which is 2.8 and 1.2 folds higher than that of pristine TiO 2 . Our work may provide insights for designing efficient photocatalysts for selective oxidation of alcohols.
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CATALYSIS LETTERS
·
2020
·Vol. 151
·期 7
·1984-1992
·
IF 2.482
Wu Ningxin,Zhang Manling,Pan Xiaomei,Zhang Jin,Gao Lijing,Xiao Guomin
Abstract The production of 5-hydroxymethylfurfural (HMF) from cellulose is of great significance for the high-value utilization of biomass, although this route currently faces the challenge of low efficiency. In the present work, a series of effective (x)Hf/ZSM-5 catalysts were developed for HMF production from cellulose, and analyzed by BET, XRD, SEM, ICP, NH 3 -TPD, Py-FTIR techniques. Driven by the (5)Hf/ZSM-5 catalyst, HMF with a yield of up to 67.5% and 17.2% of furfural are simultaneously obtained from cellulose in the H 2 O (NaCl) /THF biphasic system. Moreover, after four consecutive cycles, (5)Hf/ZSM-5 catalyst still maintained part of its catalytic activity. The 67.5% HMF yield achieved herein is one of the highest yields achieved in the conversion reaction using cellulose as a substrate, and the catalytic performance of the H 2 O (NaCl) /THF system containing the (5)Hf/ZSM-5 catalyst is even comparable to that of the expensive ionic liquid system. This result reflects the application prospect of (5)Hf/ZSM-5 catalyst in the future industrial production process of HMF. Graphic Abstract
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JOURNAL OF INORGANIC BIOCHEMISTRY
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2021
·
IF 4.155
Yucui Jiang,Saixing Liu,Qipeng Yuan,Hao Liang
Acidophilic enzymes play an important role in special industrial catalytic reactions. In this work, we reported Zr-based acid-stable nucleotide coordination polymers (CPs) for efficiently improving acidophilic enzymes immobilization . Among all tested metal ions , the Zr 4+ /AMP CPs exhibited the highest acid stability and enzyme affinity. As a typical acidophilic enzyme, the immobilized Chloroperoxidase by Zr 4+ /AMP CPs displayed robust reusability in the asymmetric synthesis of modafinil, remained 95.7% of conversion rate and 99.1% enantiomeric excess (e.e.) value. This work displayed a novel acid-stable bioorganic and inorganic hybrid nanomaterial for acidophilic enzymes immobilization.
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PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Huaqin Zuo,Yuchen Hou,Yijun Yu,Zhongqiu Li,Hanxiao Liu,Chao Liu,Jian He,Leiying Miao
The myeloid-derived suppressor cell (MDSC)-mediated immunosuppressive tumor microenvironment (TME), where tumor hypoxia counts for much, has greatly compromised the outcome of cancer immunotherapy. Here, we demonstrated a strategy for selectively clearing intratumoral MDSCs. Specifically, 2-[2-[2-chloro-3-[(1,3-dihydro-3,3-dimethyl-1-propyl-2H-indol-2-ylidene)ethylidene]-1-cyclohexen-1-yl]ethenyl]-3,3-dimethyl-1-propylindolium iodide (IR-780) and metformin (Met) were coloaded into mesoporous silica nanoparticles (MSNs) with CeO2 as the gatekeepers. Controlled release of cargos was achieved upon etching CeO2 with endogenous H2O2. Apart from the drug release, oxygen (O2) was also generated in this process. Importantly, the engagement of Met significantly inhibited mitochondrial respiration, thus working like an O2 economizer. Consequently, the populations and functions of tumor-infiltrated MDSCs were both dramatically reduced through selective alleviation of hypoxia at tumor sites, thus contributing to boosted immune responses. Additionally, the accumulated O2 enhanced IR780-mediated photodynamic therapy, which synergistically strengthened the antitumor efficacy of the platform. To the best of our knowledge, this is the first time to employ an O2-generated and -economized nanoplatform for selectively anergizing MDSC-mediated immunosuppression. We expect that this strategy will shed new light on the clinical cancer immunotherapy treatment.
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PubMed
高影响因子
ANALYTICAL BIOCHEMISTRY
·
2020
·
IF 2.877
Ao Li,Peng Zuo,Bang-Ce Ye
Salmonella, a typical foodborne pathogen, always seriously threatens the health and even life of both humans and animals. However, highly sensitive and fast quantitative methods for its detection are remaining to be challenged. Herein, we presented an efficient method with dual signal amplification strategy by combining immune hybridization chain reaction (HCR) with surface enhanced Raman scattering (SERS) to high sensitively detect Salmonella typhimurium in food. After sample preparation, S. typhimurium were specifically captured by immunomagnetic beads (IMBs), then aptamers and hairpin-probes were added to trigger HCR to form nicked dsDNA, finally 4’,6-Diamidino-2-phenylindole dihydrochloride (DAPI) was incubated with HCR products and then the whole system was mixed with AgNP colloid to detect the SERS intensity at 1610 cm −1 . As a result, a good linear relationship was achieved between SERS intensities and corresponding concentrations of S. typhimurium ranging from 10 to 10 5 CFU/mL, with a limit of detection (LOD) of 6 CFU/mL in 3.5 h. The proposed method has been successfully applied to capture and detect the S. typhimurium in spiked milk samples, and the results were consistent with those of the traditional plate counting method. The method, with combination of HCR and SERS, achieves double amplification of the detection signal and significantly improves the detection sensitivity of S. typhimurium . And it also shows good application potential for the highly sensitive detection of other contaminants in food.
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ENVIRONMENTAL RESEARCH
·
2020
·
IF 5.715
Jie Li,Lanjia Pan,Guangwei Yu,Chunxing Li,Shengyu Xie,Yin Wang
Utilization of sludge pyrochar (SP) is the terminal step to loop the entire harmless disposal process of sewage sludge with pyrolysis . A new, easily recyclable, and safe adsorbent with well-immobilized heavy metals (HMs) was prepared from SP for ciprofloxacin (CIP) adsorption. The operational conditions for the adsorbent preparation were systematically optimized based on recycling rate and adsorption performance. Additionally, the adsorption conditions, adsorption kinetics, isotherms, and regeneration of adsorbents were further investigated in the present study. The results showed that easily recyclable and safe adsorbents were successfully prepared at 1100 °C under N 2 atmospheric conditions (SPA-N-1100) with a maximum CIP adsorption capacity of 10.42 mg/g. SPA-N-1100 exhibited good CIP adsorption performance at an adsorption temperature of 45 °C and pH between 8.0 and 9.0. The adsorbents were regenerated by thermal desorption at 450 °C with a thorough decomposition of CIP. The adsorption mechanism was mainly dominated by its special porous microspheres-accumulation structure and surface species (e.g., FeP and graphite). Moreover, HMs in the adsorbents were well immobilized in SPA-N-1100 by the generation of new metal mineral phases and encapsulation of melting minerals, which had an ultralow potential for ecological risk during application.
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Biomaterials Science
·
2020
·Vol. 8
·期 17
·4779-4791
·
IF 6.183
Chuanchuan Lin,Kun Xu,Ye He,Bailong Tao,Zhang Yuan,Ke Li,Xuemin Li,Zengzilu Xia,Kaiyong Cai
The paracrine function of mesenchymal stromal cells (MSCs) contributes a lot to tissue development, and it is regulated by various physical factors. Moreover, the extracellular matrix (ECM) of MSCs is dynamic, and its remodeling is always occurring. In particular, stiffness changes are prevalent. Accordingly, ECM stiffness changes may affect the paracrine function of MSCs, which has not been investigated much. In this study, for the first time, alginate hydrogels with different stiffening times were used to assess the influence of dynamic ECM stiffness changes on the paracrine function of MSCs. It was found that a stiffer matrix (14.72 ± 1.44 kPa) under static conditions without any additional treatment could significantly potentiate the paracrine function of MSCs compared to a soft matrix (2.44 ± 0.23 kPa). Furthermore, this promotion was regulated by the activation of Yes-associated protein (YAP), which was caused by the polymerization of F-actin. Intriguingly, in a dynamic system, the MSC-encapsulating matrix that stiffened on the third day had stronger YAP activation than the Static-Stiff matrix. However, this activation was weakened when MSCs were cultured in a matrix that stiffened on the fifth day. The results show that an increase in ECM mechanical dosing levels would promote the paracrine function of MSCs. Moreover, an effective mechanical dose that can influence the paracrine function of MSCs indeed exists.
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Reaction Kinetics Mechanisms and Catalysis
·
2020
·Vol. 130
·期 2
·1027-1042
·
IF 1.52
Shi Qiqi,Guo Heqin,Chen Congbiao,Hou Bo,Jia Litao,Li Debao
In the present work, a series of sulfonic polymer-based acid catalyst PDS-x’s was obtained by hydrothermal method. The physical and chemical properties of the catalysts were characterized by X-ray diffraction, N 2 adsorption–desorption isotherms, thermogravimetric analysis, Fourier transform infrared spectrometer, pyridine-adsorbing IR, acid–base titration, X-ray photoelectron spectroscopy, and CHNS elemental analysis. The carbonylation of formaldehyde was chosen as a probe reaction to test the catalytic performance. The results show that the content of acid sites and specific surface area can be adjusted by changing the molar ratio of sodium 4-vinylbenzenesulfonate (SVBS) to divinylbenzene (DVB). The catalyst performance results show that the PDS-x’s can efficiently catalyze glycolic acid synthesis. And a high glycolic acid yield up to 96% was obtained on PDS-2.1 due to its large specific surface area, plentiful mesoporosity as well as suitable acid concentration. This data are even higher than those on super-strong CF 3 SO 3 H and commercial resin Amberlyst-15. Moreover, the carbonylation of formaldehyde is a structure-sensitive reaction, the isolated and monolayer dispersed -SO 3 H is much more active than aggregated −SO 3 H. Furthermore, the catalyst has high stability.
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高影响因子
BIOMATERIALS
·
2020
·
IF 10.317
Kaiyuan Wang,Hao Ye,Xuanbo Zhang,Xia Wang,Bin Yang,Cong Luo,Zhiqiang Zhao,Jian Zhao,Qi Lu,Haotian Zhang,Qiming Kan,Yongjun Wang,Zhonggui He,Jin Sun
Metastasis is closely associated with high breast cancer mortality. Although nanotechnology-based anti-metastatic treatments have developed rapidly, the anti-metastasis efficiency is still far from satisfactory, mainly due to the poor recognition of circulating tumor cells (CTCs) in blood. Herein, we developed an exosome-like sequential-bioactivating prodrug nanoplatform (EMPCs) to overcome the obstacle. Specifically, the reactive oxygen species (ROS)-responsive thioether-linked paclitaxel-linoleic acid conjugates (PTX-S-LA) and cucurbitacin B (CuB) are co-encapsulated into polymeric micelles , and the nanoparticles are further decorated with exosome membrane (EM). The resulting EMPCs could specifically capture and neutralize CTCs during blood circulation through the high-affinity interaction between cancer cell membrane and homotypic EM. Following cellular uptake, EMPCs first release CuB, remarkably blocking tumor metastasis via downregulation of the FAK/MMP signaling pathway . Moreover, CuB obviously elevates the intracellular oxidative level to induce a sequential bioactivation of ROS-responsive PTX-S-LA. In vitro and in vivo results demonstrate that EMPCs not only exhibit amplified prodrug bioactivation, prolonged blood circulation, selective targeting of homotypic tumor cells, and enhanced tumor penetration, but also suppress tumor metastasis through CTCs clearance and FAK/MMP signaling pathway regulation. This study proposes an integrated approach for mechanism-based inhibition of tumor metastasis and manifests a promising potential of programmable-bioactivating prodrug nanoplatform for cancer metastasis inhibition .
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Journal of Materials Chemistry C
·
2020
·Vol. 8
·期 42
·14723-14731
·
IF 7.059
Lele Li,Liwei Yang,Si Zhang,Yuping Sun,Fen Li,Tengteng Qin,Xiaoqiang Liu,Yanmei Zhou,Subbiah Alwarappan
Herein, we designed a NiCo2S4@N/S–CeO2 composite with amplified electrocatalytic oxygen reduction (OR) capability by the in situ growth of NiCo2S4 nanoparticles on CeO2 nanospheres with simultaneous doping of nitrogen and sulfur. After optical characterization of the composite, it was then employed as the signal amplification label for constructing an electrochemical aptasensor. The composite provides a biocompatible and large surface platform to load biomolecules and retain their bioactivity. More importantly, the composite shows a comparable electrocatalytic OR capability similar to a commercial Pt/C catalyst and far better than CeO2, attributed to the NiCo2S4 deposition and oxygen vacancies introduced by N and S doping. Furthermore, the Koutecky–Levich plots indicate a nearly four-electron transfer pathway of the ORR. The as-prepared aptasensor exhibited a highly sensitive and selective determination of a model analyte-sulfadimethoxine with a wide linear range of 0.05–180 nM, a low detection limit of 0.02 ± 0.0011 nM and good feasibility for real-sample detection. This work paved an effective way for the design of highly efficient electrocatalysts with bright prospects in bioanalytical applications.
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DALTON TRANSACTIONS
·
2020
·Vol. 49
·期 31
·10918-10927
·
IF 4.174
Yaru Yang,Hao Wan,Gen Chen,Ning Zhang,Junhui Li,Wei Ma,Xiaohe Liu,Renzhi Ma
Because of their low cost and Earth-abundant characteristics, materials based on 3d transition metals have attracted great research interest and are considered as promising electrocatalysts for the oxygen evolution reaction (OER), besides the commercial noble metal-based materials, in recent years. In order to improve electrocatalytic activity, it is necessary to design the structures and compositions of electrocatalysts. In this study, a series of multi-shelled CoxNi1−x oxide/phosphide hollow spheres with tunable element ratios were prepared. The electrocatalytic activity of the multi-shelled CoxNi1−x oxide/phosphide is strongly dependent on the molar ratio of Co and Ni. Based on the combined advantages of complex structures and compositions, the multi-shelled Co0.5Ni0.5 oxide/phosphide displays outstanding electrocatalytic performance in terms of high activity and stable durability for the OER, surpassing those of RuO2 and multi-shelled CoxNi1−x oxide/phosphide with other element ratios of Co and Ni. This result suggests a great possibility of rationally designing the composition for highly efficient electrocatalysts.
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高影响因子
JOURNAL OF DISPERSION SCIENCE AND TECHNOLOGY
·
2018
·
IF 1.454
Xinyue Wang,Xinyue Lu,Lili Wen,Zongning Yin
Water-in-oil-in-water (W/O/W) double emulsion can be prepared by incomplete phase inversion method using both medium chain triglycerides (MCT) and isopropyl myristate (IPM) as oil phase, Span 85-Tween 80 (HLB values of 2.5-3.0) as mixed emulsifiers. The preparation method was simple, and the final double emulsions were proved of good microstructure and particle size distribution. Owning to the addition of Tween 80 to Span 85, interfacial tension, interfacial viscosity and modulus decreased, which contributed to the phase inversion. Furthermore, formation of reverse micelles under high-speed dispersion may be a hypothesis to explain the incomplete phase inversion phenomenon.
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