ACS Omega
·
2022
·
IF 4.132
Jinglei Cui,Dan Ren,Jingjing Tan,Huirong Zhang,Yanxia Guo,Long Huang
Toluene is one of the typical volatile organic compounds in industry, particularly in energy and fuels production processes, which is required to be eliminated effectively to protect the environment. Catalytic oxidation of toluene is widely studied for its high efficiency, and rational design and synthesis of metal catalysts are keys for toluene oxidation. In this study, an efficient catalyst was designed and synthesized by introducing −NH2 groups on the ordered mesoporous silica (KIT-6) surface to anchor and disperse Pd species, leading to Pd nanoparticles being highly dispersed with uniform particle size distribution. Meanwhile, it was found that the introduction of −NH2 made Pd centers present an electron-rich state, and the active Pd centers could activate O2 molecules to generate more reactive oxygen species and promote the conversion of toluene, which was verified by in situ XPS and O2-TPD characterization. Compared with the catalysts prepared by an impregnation method, the catalytic performance of the Pd/NH2-KIT-6 (0.5 wt %) catalyst was significantly improved. A conversion of 90% for toluene (2400 ppm, 24,000 mL·g–1·h–1) was achieved at 171 °C, and the toluene conversion was maintained above 90% for 900 min, displaying the excellent activity and stability of the Pd/NH2-KIT-6 catalyst.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Junjing Li,Shumin Ma,Ziyan Qi,Jing Ding,Menghua Yin,Bin Zhao,Zhaohui Zhang,Yu Wang,Hongwei Zhang,Liang Wang,Dionysios D. Dionysiou
To effectively improve the particle dispersion of the catalytic metal and catalytic activity of the palladium electrode, a new type of efficient Pd/NiFe-MOF/foam-Ni composite electrode was prepared. The results showed that the reaction rate constant of chloramphenicol (CAP) by Pd/NiFe-MOF/foam-Ni was three times that of Pd/foam-Ni. X-ray absorption fine structure (XAFS) results showed that palladium on Pd/NiFe-MOF/foam-Ni had a lower oxidation state than that on Pd/foam-Ni. The Pd nanoparticles were uniformly dispersed on the composite electrode and had a small particle size. The electrode had good resistance to sulfites and the electrocatalytic activity was hardly affected in the presence of Cl - , NO 3 - , HCO 3 - , CO 3 2- and Ca 2+ in wastewater. Besides, the introduction of nickel-iron bimetallic organic framework (NiFe-MOF) increased the electron density of Pd, improved the dispersion and electrochemical active surface area (ECSA) of Pd. The reaction pathway of CAP was proposed, and the ecotoxicity of CAP and its products was evaluated by the Ecological Structure Activity Relationships (ECOSAR) model. Combined experimental data and density functional theory (DFT) analysis enable us to propose the hydrodechlorination mechanism of CAP on the Pd/NiFe-MOF/foam-Ni electrode. The Pd/NiFe-MOF/foam-Ni composite electrode has good application prospects in the treatment of organic pollutants in wastewater and other environmental remediation applications.
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ACS Applied Materials & Interfaces
·
2022
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IF 10.383
Ruidong Li,Lu Wu,Ganggang Chang,Shanchao Ke,Yilong Wang,Yao Yao,Yuexing Zhang,Junsheng Li,Xiaoyu Yang,Banglin Chen
Carbon materials with hierarchical morphologies, pores, and compositions have attracted extraordinary attention due to their unique structural advantages and widespread applications. However, their controllable synthesis remains a grand challenge. Herein, a solvent-mediated strategy was demonstrated for the preparation of an urchin-like superstructure via modulating the hydrothermal condition (acetic acid/water ratio) of metal–organic frameworks (MOFs). The direct pyrolysis of a hierarchical NUS-6 precursor produced a well-defined carbon-based composite consisting of sulfur-doped carbon (SC) and HfO2 with an urchin-like morphology and micro-/mesoporosity, while the doped S sites and oxygen vacancies of HfO2 can help to anchor and activate Pd nanoparticles (NPs) through the strong host–guest interaction, which was further confirmed by the calculated results of the binding energy and differential charge density through density functional theory (DFT). The synthesized Pd@SC/HfO2 composite exhibited extremely high catalytic activity and stability toward the water-phase hydrodeoxygenation of vanillin (conversion >99%, selectivity >99%), as well as good universality for the hydrogenation of a series of unsaturated hydrocarbons in an aqueous system. Remarkably, the catalytic activity and structural stability of Pd@SC/HfO2 were largely maintained even after successive 10 cycles.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Qing Hu,Jiayi Yao,Xiaoqin Wang,Yanfang Wang,Xiaoling Fu,Ju Ma,Han Lin,Jiaqi Xu,Longhua Shen,Xiangbin Yu
Chemoimmunotherapy can synergistically enhance the therapeutic effects and decrease the side effects by a combined method. However, the effective targeted codelivery of various chemotherapeutic agents and siRNAs remains challenging. Although nanomedicine-based chemoimmunotherapy has shown great potential in cancer treatment in recent years, further effort is needed to simplify the nanocarrier designs and maintain their effective functions. Here, we report a simple but robust multifunctional liposomal nanocarrier that contains a pH-sensitive liposome (LP) shell and a dendritic core for tumor-targeted codelivery of programmed cell death ligand 1 (PD-L1) siRNA and doxorubicin (DOX) (siPD-L1@PM/DOX/LPs). siPD-L1@PM/DOX/LPs had a suitable particle size and zeta potential, excellent stability in serum, and pH-sensitive drug release in vitro. They exhibited significant cell proliferation inhibition compared to free DOX and DOX-loaded LPs and could escape endosomes, effectively release siRNA into the cytoplasm of MCF-7 cells, and significantly reduce the PD-L1 expression on tumor cells. In vivo imaging confirmed high accumulation of siPD-L1@PM/DOX/LPs at the tumor site. More importantly, compared with siPD-L1@PM/LPs or DOX alone, siPD-L1@PM/DOX/LPs were more effective in inhibiting tumor growth and activating cytotoxic T cells in vivo. In conclusion, this nanocarrier may hold promise as a codelivery nanoplatform to improve the treatment of various solid tumors.
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Huanhuan Liu,Meng Chen,Yingnan Duan,Xiaohuan Jiang,Jiayu Liao,Mengkui Tian
In this work, macrocyclic molecule cucurbit[6]uril (CB[6])-modified two-dimensional black phosphorus nanosheets (BPNSs) used as photoactivated support were synthesized by a simple solvothermal method . Palladium nanoparticles were anchored on the surface of BP-CB[6] to obtain the composite material Pd/BP-CB[6] by using a chemical reduction method. Then, the electrocatalytic activity of the composite material modified electrode in the ethanol oxidation reaction (EOR) was investigated. The Pd/BP-CB[6] catalyst exhibits a high mass activity (1420 mA·mg Pd −1 ), which is 4.1 times higher than commercial Pd/C. Impressively, the ethanol oxidation activity of the Pd/BP-CB[6] electrode under visible light irradiation (1900 mA·mg Pd −1 ) is 1.34 times higher than under dark conditions. The result is obtained through a series of evaluations, including cyclic voltammetry , chronopotentiometry , chronoamperometry , and electrochemical impedance spectroscopy , in which the prepared Pd/BP-CB[6] shows higher catalytic activity and stability than Pd/BP. These results suggest that the synergistic effect of photocatalysis and electrocatalysis improves the electron transport kinetics of the Pd/BP-CB[6] electrode in the EOR process. Two-dimensional black phosphorus nanosheets can be used as promising photoactivated supports, to which functional material CB[6] is fixed by hydrogen bonding . Meanwhile, the electrostatic interaction between CB[6] and noble metal helps to improve the stability of the catalyst. This work provides a new idea for developing efficient photoresponsive electrode material in direct ethanol fuel cells.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
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IF 6.371
Rui Xu,Jun Wang,Yafei Xu,Zhen Yin,Wuke Li
The ultrafine and highly dispersed bimetallic Pt-Pd nanoparticles are successfully anchored on mesoporous silica nanoparticles (MSN). The MSN@Pt-Pd catalyst exhibits excellent catalytic performance in the hydrogen from ammonia borane (AB). When the MSN@Pt-Pd nanoparticles were grafted with luminescent material and smart thermo-responsive polymer, a smart catalyst could be fabricated. The smart catalyst exhibits the thermo-responsive catalytic performance and switchable luminescence. For example, the composite catalyst displays high catalytic activity in hydrolysis of AB at 25 °C. However, it shows much lower catalytic activity when the temperature increases to 35 °C. The smart catalysts could be potentially applied in the self-protection device of dehydrogenation . When the system of dehydrogenation is under high temperature environment, the smart composite catalyst could automatically restrain the production of H 2 for the purpose of safety.
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MOLECULAR PHARMACEUTICS
·
2022
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IF 5.364
Nan Zhang,Jing Li,Wenxia Gao,Wangwei Zhu,Jianqin Yan,Ziyun He,Li Li,Fang Wu,Yuji Pu,Bin He
The combined delivery of chemotherapeutics with checkpoint inhibitors of the PD-1/PD-L1 pathway provides a new approach for cancer treatment. Small-molecule peptide inhibitors possess short production cycle, low immunogenicity, and fewer side effects; however, their potential in cancer therapy is hampered by the rapid biodegradation and a nanocarrier is needed for efficient drug delivery. Herein, anticancer drug doxorubicin (DOX) and PD-L1 inhibitor peptide P-12 are co-loaded by a lipid polymer nanocomplex based on poly(lactic-co-glycolic acid) (PLGA) and DSPE-PEG. Octaarginine (R8)-conjugated DSPE-PEG renders the LPN efficient internalization by cancer cells. The optimal nanomedicine LPN-30-R82K@DP shows a diameter of 125 nm and a DOX and P-12 loading content of 5.0 and 6.2%, respectively. LPN-30-R82K@DP exhibits good physiological stability and enhanced cellular uptake by cancer cells. It successfully induces immunogenic cell death and PD-L1 blockade in CT26 cancer cells. The in vivo antitumor study further suggests that co-loaded nanomedicine efficiently suppresses CT26 tumor growth and elicits antitumor immune response. This study manifests that lipid polymer nanocomplexes are promising drug carriers for the efficient chemo-immunotherapy of cancer.
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高影响因子
TALANTA
·
2022
·
IF 6.556
Xin Wang,Min Zhang,Xiaoxu Pang,Kunlun Huang,Zhiyi Yao,Xiaohong Mei,Nan Cheng
Staphylococcus aureus is a frequent pathogenic bacterium that has a significant detrimental influence on the health of the human body. Therefore, developing a practical and portable detection platform is critical to ensuring food safety. Nanozymes are a kind of engineered nanomaterials with superior enzyme-like activities, providing infinite possibilities for the development of highly sensitive analytical assays. In this study, mesoporous core−shell [email protected] ( [email protected] ) nanozymes were synthesized and then applied as a signal amplifier in Staphylococcus aureus colorimetric immunoassay . At the same time, a careful comparative study of the catalytic performance with natural horseradish peroxidase (HRP), [email protected] nanozymes and their complexes [email protected] (HRP coupling with [email protected] nanozymes) were firstly performed, as well as clever using a colorimeter to achieve portable signal output. [email protected] bioprobes enable remarkable peroxidase-like catalytic activity, resulting in the highest sensitivity with a limit of detection (LOD) improved from 1 × 10 5 to 1 × 10 3 CFU/mL. In all, this work conducted a valuable comparative study and presented an improved strategy for the portable detection of pathogenic bacteria, which was expected to be used in a wide range of applications in food safety regulation and biomedicals arenas.
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高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Tengda Zhang,Bo Ouyang,Xiuling Zhang,Guangqing Xia,Nantao Wang,Haoyu Ou,Long Ma,Pengxin Mao,Kostya (Ken) Ostrikov,Lanbo Di,Xin Tu
Effective catalytic removal of 4-nitrophenol (4-NP) in industrial wastewater remains a significant challenge due to the lack of highly efficient and stable catalysts. Herein, we demonstrated a promising plasma method for the facile, ultra-fast and low-temperature synthesis of graphite oxide (GO)-supported palladium catalyst (Pd/GO-P) rich in oxygen-containing groups (OCGs) and defects with smaller Pd nanoparticles (NPs) for highly efficient 4-NP reduction. The plasma method limited the damage to the OCGs and retained more OCGs (mainly alkoxy and hydroxyl groups) on the GO surface. In addition, plasma treatment can increase the active sites and the density of GO surface defects. These OCGs and defects promoted the 4-NP adsorption and improved the catalyst dispersion in the aqueous solution of 4-NP, thereby enhancing the catalytic reduction performance. The Pd/GO-P catalyst showed the highest reduction of 4-NP reported thus far, with a concentration-normalized rate constant of 5576 min −1 g −1 L. This value was 51.6 and 20.5 times greater than that using Pd/rGO-H prepared by a traditional thermal reduction method and a commercial Pd/AC catalyst, respectively. This work opens the avenue of exploring the use of plasma for the rational design of supported Pd catalysts with superior performance for the reduction and recycling of 4-NP in wastewater.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
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IF 4.326
Mingshuai Sun,Fumin Wang,Guojun Lv,Xubin Zhang
Overhydrogenation to ethane is most undesired in selective hydrogenation of acetylene. Monometallic Pd supported on common oxide supports such as alumina and silica suffers from susceptibility of ethane formation, and the ethylene selectivity is usually unsatisfactory. Herein, Fe5C2 was carefully synthesized and employed as a new kind support doped with a (5–600) ppm level of Pd for selective hydrogenation of acetylene. The catalyst with appropriate Pd loadings exhibited more efficient ethane suppression and much higher ethylene selectivity than the traditional α-Al2O3 supported Pd catalyst, with full acetylene conversion under 240 °C, and maintained good stability after a 200 h tolerance test. Characterization and DFT calculation results reveal that the excellent ethylene selectivity is mainly derived from the special interaction between Pd atoms and the Fe5C2 support. Hydrogenation of ethylene to ethane needs to cross extremely high activation energy barriers on the catalyst surface, and ethylene desorption more easily occurs on it. Doping the appropriate amount of Pd atoms on the Fe5C2 surface can increase the obstacle for polymerization and will cause the unsaturated C2 species to be more inclined to be hydrogenated into C2H4. This synergy effect also acts as a guide in alkane suppression for selective hydrogenation of other alkynes.
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Applied Nanoscience
·
2021
·Vol. 13
·期 2
·1495-1506
·
IF 3.674
Zhang Xian-bing,Hu Ya-ping,Yang Wei,Feng Ming-bao
For the efficient disposal of organic pollutants and Escherichia coli ( E. coli ) in water, Ag-loaded and Pd-loaded ZnO nanofibers (NFs) were prepared through electrospinning (e-spin), followed by the alcohol-thermal method. The NFs were prepared in membrane form to promote their separation, recovery, and reuse in practical applications. The complete decolorizations of three types of dyes (i.e., azo, triarylmethane, and heterocyclic dyes) were observed when the Ag-loaded or Pd-loaded ZnO nanofiber membrane (NFM) was first applied as photocatalyst under 30-min UV irradiation. The characterization of the catalysts and the decolorization performance of dyes both demonstrated that the optimal loading rates of Ag and Pd were 12% and 6%, respectively. Moreover, the 12%-Ag/ZnO NFM displayed excellent recyclability over five cycles than the 6%-Pd/ZnO NFM. The E. coli disinfection test demonstrated that the photocatalytic inactivation rates with the 12%-Pd/ZnO NFM and the 6%-Ag/ZnO NFM were significantly improved under solar or UV irradiation, and hydroxyl radicals (∙OH) was primarily responsible for the antibacterial performance. Therefore, the presented 12%-Ag/ZnO NFM and 6%-Pd/ZnO NFM can be used for the efficient photocatalytic treatment of dyes and E. coli in water.
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APPLIED CATALYSIS A-GENERAL
·
2021
·
IF 5.706
Jin-Tao Du,Meng Qiao,Yuan Pu,Jie-Xin Wang,Jian-Feng Chen
The reduction of nitroarenes is usually catalyzed by heterogeneous catalysts. In this work, highly stable aqueous dispersions of monodisperse Pt, Pd, and Au nanoparticles stabilized by thermosensitive polymer, poly(N-isopropylacrylamide) (PNIPAM), are conveniently synthesized with the average sizes of 2.3, 3.1, and 2.3 nm, respectively. The modulation of the hydrophilic-hydrophobic nano-environments of the catalysts can be selectively provided by utilizing the temperature-responsive characteristics of PNIPAM. They are effective and thermosensitive pseudohomogeneous catalysts for nitroarenes reduction. The decreasing trend of catalytic activity is as follows: PNIPAM-Au > PNIPAM-Pd > PNIPAM-Pt. The catalytic reduction of nitrobenzene (NB), 4-nitrophenol (4-NP), and o-nitroaniline (o-NA) follow the pseudo-first-order kinetics, and the catalytic rates can be tuned by utilizing their temperature-responsive behavior. PNIPAM-Au nanocatalysts exhibit high turnover frequencies (TOF) up to 84, 12.9, and 40 min −1 for catalytic reduction of NB, 4-NP, and o-NA at 20 °C, respectively, which are one of the highest values ever reported.
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