SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Yanju Chen,Chao Feng,Wenhong Wang,Zhi Liu,Junxi Li,Chenguang Liu,Yuan Pan,Yunqi Liu
Regulating the electronic structure of Pd catalyst for promoting electrocatalytic hydrodechlorination is promising but still challenging. Herein, we propose an electronic structure engineering for accelerating the hydrodechlorination process by desigining bimetallic Pd-Au alloy nanoparticles (ANs) with electron-rich Pd as high-efficiency electrocatalysts. The Pd 7 Au 3 ANs exhibits the highest electrocatalytic hydrodechlorination activity, the 4-chlorophenol hydrodechlorination efficiency reaches 98.35 % within 4 h, and the mass activity is 0.47 h −1 mg Pd −1 , which is 7.83 times as high as that of pure Pd nanoparticles. The experimental characterization and theoretical calculation reveal that Pd atoms “obtain” electrons and gold atoms “lose” electrons in Pd-Au ANs, resulting in the formation of electron-rich Pd, which promotes the desorption of the dechlorination product phenol and accelerates the renewal of active sites. This work provides an electronic structure engineering strategy of Pd-based electrocatalysts for electrocatalytic hydrodechlorination, which opens a new opportunity for rational design and construction of high-performance hydrodechlorination catalysts.
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Applied Materials Today
·
2022
·
IF 8.663
Ruirui Zhang,Liping Zhong,Xiuli Liu,Xiyu Liu,Qiaoying Chen,Pan Wu,Jian He,Yongmei Li,Yongxiang Zhao,Ziqun Liu,Yan Zu,Yong Huang,Bing Wang
Immunotherapy has made encouraging progress in the field of cancer treatment. Among them, the programmed cell death-ligand 1 (PD-L1) antibody-mediated immunotherapy has stimulated the development of various carrier delivery systems. Inspired by related researchs, in this study, we prepare core-shell structured poly(lactide-co-glycolide) (PLGA) microcapsules as a drug delivery system through microfluidics technology, loaded with PD-L1 aptamers and chemotherapy drug docetaxel. The PD-L1 aptamer loaded in the nuclear layer binds to the PD-L1 molecule produced by tumor cells, blocking the immune checkpoint protein-1/programmed cell death-ligand 1 (PD-1/PD-L1) pathway. As a result, phagocytosis of tumor cells is promoted by using lipopolysaccharide (LPS) induced tumor associated macrophages. Furthermore, docetaxel in the shell is further released, inhibiting tumor cell growth as the PLGA microcapsules degrade. More importantly, the combination of PD-L1 aptamers and the chemotherapy drug docetaxel improved the immune response of the tumor. It showed significant anti-tumor activity and reduced systemic side effects in the melanoma model. At present, more and more nucleic acid aptamers as affinity reagents that can replace antibodies have been used to improve tumor treatment. Therefore, this therapeutic strategy provides more possibilities for tumor treatment by combining aptamer molecules with chemotherapy drugs when exploring more effective combination drugs.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Zhefei Zhao,Li Yu,Lingxia Zheng,Tianyang Guo,Zhuoqing Lv,Shuang Song,Huajun Zheng
The development of catalysts with high atom utilization and activity is the biggest challenge for electrocatalytic hydrodechlorination (EHDC) technology . Herein, a design strategy of TiO 2 @PDA inorganic-organic core-shell skeleton for loading lower dosage of noble palladium (Pd) with robust activity is reported. The self-supported TiO 2 @PDA nanorod arrays provides exposed surface area for anchoring Pd and PDA as interlayer controls the Pd nucleation to form nanodots with high dispersion, realizing high atom utilization. Moreover, the strong interaction between PDA and Pd realizes the coexistence of electron-rich and deficient Pd species with suitable proportion, which facilitate the H* formation and the C-Cl bond activation, respectively, resulting in the promoted activity. The optimal TiO 2 @PDA/Pd electrode exhibits a low dosage of Pd (0.093 mg cm −2 ) and excellent activity for 4-chlorophenol reduction with a mass activity (MA) of 23.96 min −1 g −1 , which is 3.31 times as high as that of TiO 2 /Pd. The design scheme with inorganic-organic core-shell skeleton as support is benefit for developing highly efficient and lower price elctrocatalysts for EHDC.
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PubMed
高影响因子
FUEL
·
2022
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IF 8.035
Defu Yin,Renjie Ji,Fanglin Lv,Long Jiang,Jingyun Zhang,Mingya Liu,Zhen Jia,Shitao Yu,Ruiyang Zhao,Yue Liu
Efficient catalysts are still the key to practical industrial applications. In this work, Pd-based catalyst was modified by doping metal Co to obtain Pd-Co@mSiO 2 bimetallic core–shell catalyst. The modified bimetallic core–shell catalyst was used in the hydrogenation of phenol, and the catalytic results showed that the Co modification effectively improved the catalytic performance of the Pd-based catalyst, especially, it reduced the activation energy of the reaction and greatly improve the conversion of phenol. Combined with characterization, it was found that Co doping reduced the particle size of Pd metal particles and affected the adsorption capacity of substrate phenol on the surface of Pd metal. The conversion of phenol was close to 99.9 % within 1 h at 80 °C, while the selectivity of cyclohexanone reached 95.4 %. In addition, the core–shell structure provided a stable environment for the catalyst, which still maintained high activity after being recycled for 5 times.
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Acta Biomaterialia
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2021
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IF 8.947
Zefeng Wang,Yanling Peng,Yan Zhou,Shengnan Zhang,Jianxi Tan,Huan Li,Dinggeng He,Le Deng
Photothermal therapy (PTT) is a promising strategy for antimicrobial therapy. However, the application of PTT to treat bacterial infections remains a challenge as the high temperature required for bacterial elimination can partly damage healthy tissues. Selecting the appropriate treatment temperature is therefore a key factor for PTT. In this work, we designed a near-infrared/pH dual stimuli-responsive activated procedural antibacterial system based on zeolitic imidazolate framework-8 (ZIF-8), which was bottom-up synthesized and utilized to encapsulate both Pd-Cu nanoalloy (PC) and the antibiotic amoxicillin (AMO). This procedural antibacterial therapy comprises chemotherapy (CT) and PTT. The former disrupts the bacterial cell wall by releasing AMO in an acidic environment, which depends on the sensitive response of ZIF-8 to pH value change. With the progression in time, the AMO release rate decreased gradually. The latter can then significantly stimulate drug release and further complete the antibacterial effect. This impactful attack consisted of two waves that constitute the procedural therapy for bacterial infection. Accordingly, the treatment temperature required for antibacterial therapy can be significantly lowered under this mode of treatment. This antibacterial system has a significant therapeutic effect on planktonic bacteria (G + /G − ) and their biofilms and also has good biocompatibility; thus, it provides a promising strategy to develop an effective and safe treatment against bacterial infections. Statement of Significance We have developed a near infrared/pH dual stimuli-responsive activated procedural antibacterial system that combines enhanced antibiotic delivery with photothermal therapy and has highly efficient antimicrobial activity . The antibacterial effect of this therapy was based on two mechanisms of action: chemotherapy, in which the bacterial cell wall was first destroyed, followed by photothermal therapy. After exposure to irradiation with an 808 nm laser, the inhibition rates were 99.8% and 99.1% for Staphylococcus aureus and Pseudomonas aeruginosa , respectively, and the clearance rates for their established biofilms were 75.3% and 74.8%, respectively. Thus, this procedural antibacterial therapy has shown great potentiality for use in the photothermal therapy of bacterial infectious diseases, including biofilm elimination.
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ACS Applied Nano Materials
·
2021
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IF 5.097
Ying Li,Shujuan Li,Min Bao,Linqun Zhang,Carlo Carraro,Roya Maboudian,Anran Liu,Wei Wei,Yuanjian Zhang,Songqin Liu
Nanomaterials possessing intrinsic enzyme-mimetic activity are becoming an important topic of current research. However, their enzyme-mimetic activity is limited by the particle size of the nanomaterials. In this study, Pd nanoclusters with an average size of 1.4 nm are synthesized by using a metal organic framework, zeolitic imidazolate framework-8 (ZIF-8), as a matrix via an impregnation-reaction method. By virtue of the confined channels of ZIF-8 and the strong chemical interaction between the Pd nanoclusters and ZIF-8 framework, the Pd nanoclusters show a high dispersity and stability. The obtained Pd@ZIF-8 is proven to have enhanced intrinsic peroxidase-like activity, showing Michaelis–Menten constants (Km) as high as 0.13 mM for 3,3′,5,5′-tetramethylbenzidine and 14.02 mM for hydrogen peroxide. Colorimetric testing and electron spin resonance spectra reveal that radicals are generated during the catalytic process of peroxidase-like Pd@ZIF-8 toward H2O2. With the addition of glucose or cholesterol oxidase, the Pd@ZIF-8 can be utilized to construct a highly selective and sensitive fluorescent sensor for glucose and cholesterol, exhibiting a detection limit of 0.10 and 0.092 μΜ, respectively. Additionally, the proposed fluorescent platform exhibits the capability to detect glucose and cholesterol in serum samples with satisfactory recovery, indicating potential application prospects in biochemical analysis.
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ACS Applied Nano Materials
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2021
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IF 5.097
Tao Hu,Tingting Liu,Caiyun Xu,Mingxi Liu,Shenghu Zhou
In this study, we for the first time use ditopic bis-terpyridine-containing metallopolymers as templates to synthesize metal nanoparticle-encapsulated nanoreactors. In the presence of the surfactant cetyltrimethylammonium bromide, the ditopic bis-terpyridines coordinate Pd2+ ions to form linear metallopolymer bundles, which are further used as templates for silica deposition to give silicified Pd ion-containing tubular metallopolymers. The following calcination and subsequent reduction simultaneously result in Pd NP-encapsulated silica nanotubes (Pd-SNTs). Relative to the silica-supported Pd catalysts, the prepared Pd-SNTs demonstrate enhanced performance for hydrodechlorinations of various chlorophenols into phenolic compounds at 35 °C and atmospheric H2 pressure and present high catalytic stability during five cycles of hydrodechlorination reactions.
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ACS Sustainable Chemistry & Engineering
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2021
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IF 8.198
Feng Yao,Shuyan Guan,Linyan Bian,Yanping Fan,Xianyun Liu,Huanhuan Zhang,Baojun Li,Baozhong Liu
Creating active sites to improve the mass activity and durability of metal catalysts by elucidating the relationship between the metal and the support is a major challenge. In this study, ultrafine palladium nanoparticles (Pd NPs) were supported on alkalized Ti3C2 (alk-Ti3C2) to obtain a catalytically active interfacial ensemble. The catalyst Pd/alk-Ti3C2 with a Pd loading of 1.0 wt % exhibited the highest activity in ammonia borane (AB) hydrolysis reaction, with an initial turnover frequency of 230.6 min–1. A comprehensive analysis revealed that an ensemble-exciting effect originated from the Pd and the alk-Ti3C2. The hydroxylation of alk-Ti3C2 regulated the local coordination environment of Pd. Water and AB were effortlessly activated by the −OH group and Pd atom aggregates composed of electron-deficient support alk-Ti3C2 and electron-rich Pd, respectively. The efficient generation of hydrogen at the interface of Pd/alk-Ti3C2 was further guaranteed by the interfacial activation. This work on precision active sites opens new avenues for developing high-activity noble-metal catalysts for AB hydrolysis.
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JOURNAL OF CATALYSIS
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2021
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IF 7.92
Jing Zhang,Weiqi Liao,Hao Zheng,Yunshang Zhang,Lebing Xia,Bo-Tao Teng,Ji-Qing Lu,Weixin Huang,Zhenhua Zhang
Pd supported on different anatase TiO 2 nanocrystals predominantly exposing either {1 0 0}, {1 0 1}, or {0 0 1} facets were tested for CO 2 hydrogenation into formate. Remarkable morphology-dependent catalysis was observed. Compared to 2%Pd/TiO 2 {1 0 1} and 2%Pd/TiO 2 {0 0 1} catalysts, 2%Pd/TiO 2 {1 0 0} is highly active and stable, affording an unprecedented turnover frequency of ca. 1369 h −1 and keeping stable after 6 cycles at 313 K. This can be associated with, on the one hand, higher density of moderate basic site and relatively more Pd(0) species over 2%Pd/TiO 2 {1 0 0} contribute to the activations of CO 2 and H 2 , respectively, favorable for the activity; On the other hand, higher oxygen vacancy concentrations in the TiO 2 {1 0 0} promote the Pd-TiO 2 interactions and result in the formation and stability of flat Pd particles over 2%Pd/TiO 2 {1 0 0}, beneficial to the stability. These results highlight the importance of oxide morphology in formate formation and open up possibilities of oxide morphology engineering for developing efficient Pd-based catalysts for CO 2 hydrogenation.
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Molecular Catalysis
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2021
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IF 5.062
Huafan Li,Tiantian She,Guofeng Chen,Menghua Sun,Libo Niu,Guoyi Bai
In this paper, a stable Pd/NH 2 -SBA-15 catalyst was prepared by an ammonia evaporation method using amino-functionalized SBA-15 as support. Pd/NH 2 -SBA-15 showed excellent catalytic performance in the selective hydrogenation of phenol to produce cyclohexanone. Furthermore, this Pd/NH 2 -SBA-15 catalyst kept the conversion of phenol and selectivity of cyclohexanone both over 90 % even after 10 runs, much better than Pd/SBA-15 and the previously reported Pd-based catalysts, demonstrating the benefit of amine functionalization on the activity of supported Pd nanoparticles. TEM and XPS results indicate that small Pd particles were highly dispersed on the NH 2 -SBA-15 support and a stronger interaction occurred between the active Pd particles and the amine functionalized SBA-15 support, which could effectively inhibit the agglomeration of the active Pd particles during the reaction and then improve the stability of this catalyst.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2021
·Vol. 28
·期 47
·67098-67107
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IF 4.223
Long Yingtao,Liang Jianjun,Xue Yinghao
A novel composite (nZVI/Pd-AC) was prepared by loading nanoscale zero-valent iron (nZVI) and Pd on activated carbon (AC) electrode under electrodeposition with ultrasound, which was used to reductive degradation of methylene blue (MB). The loading contents of Fe and Pd in composite materials were 15.84% and 2.06%, respectively. XPS results further confirmed that the as-prepared material contained Fe 0 and Pd 0 . Without external conditions, MB could be degraded in the presence of nZVI/Pd-AC and reached equilibrium within 180 min. To investigate the reusability, the re-electrodeposition strategy was effective to refresh the active sites of nZVI/Pd-AC, and the removal efficiency only reduced by 4.51% in five circles indicating the good reusability of nZVI/Pd-AC composites. GC–MS was used to identify possible degradation pathways of MB; the results showed that the degradation products were mainly N, N-dimethylaniline and 2-amino-5-dimethylamino-benzenesulfonic acid. And the S–C, C–N bonds are the sites easier to be attacked. Graphical abstract
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Journal of Environmental Chemical Engineering
·
2021
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IF 5.909
Yuzhou Xue,Zhenchao Lei,Wenxiao Zheng,Weijian Duan,Liuyi Zhu,Zhang Yan,Chunhua Feng
It is generally known that carbon supports with a large surface area are essential for dispersion of Pd catalysts and adsorption of pollutants (e.g., chlorinated compounds), thus enabling enhanced mass transfer and increased reaction kinetics. However, we demonstrate that, in spite of contributing to achieving highly dispersed Pd nanoparticles , a high-surface-area carbon support favoring fast adsorption of 2,4-dichlorophenol negatively impacts the catalytic activity of Pd. Comparisons of catalytic performance between Pd/activated carbon (AC) catalysts with different mass loadings in a 3D electrochemical dechlorination reactor suggested that Pd(60%)/AC outperformed Pd(10%)/AC, although the latter had smaller Pd catalysts and the amount of Pd was same in these experiments. We found that the dechlorination rate constant was inversely correlated to the adsorption rate constant at Pd loadings from 10% to 60%. We further verified that the use of C 3 N 4 , an optimal carbon support with low surface area that allows good dispersion of Pd nanoparticles (10%), is critical in accelerating the dechlorination reaction kinetics due to the improved accessibility of active sites to the pollutants. This study provides information on how to select optimal supporting materials with desirable features that avoid catalyst aggregation and pre-adsorption of pollutants when the supported Pd catalysts are used as the moveable particle electrodes.
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