Surfaces and Interfaces
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2022
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IF 6.137
Dongjing Liu,Lingtao Yang,Jiang Wu,Bin Li
Zeolite ZSM-5, as a crystalline microporous material , has attracted widespread interest in diverse research areas because of its big specific surface area, high thermal stability, and shape selectivity . Here, x Bi 2 S 3 /ZSM-5 compounds is easily synthesized using a molten salt method and employed to capture elemental mercury in the temperature range of 60–260°C. Pristine ZSM-5 displays a weak Hg 0 adsorption capability. Bi 2 S 3 decoration can greatly reinforce the mercury adsorption capability of ZSM-5 due to addition of active sulfide species. 20Bi 2 S 3 /ZSM-5 with 20 wt% Bi 2 S 3 loading value performs optimally toward Hg° capture associated with a mercury removing efficiency of 90.8–96.5% within 100–140°C. In addition, 20Bi 2 S 3 /ZSM-5 is nearly impervious to NO and SO 2 with respect to mercury removal. One-dimensional nanorod structure of Bi 2 S 3 and big specific surface area of ZSM-5 probably account for the superior mercury capture performance of x Bi 2 S 3 /ZSM-5 compounds.
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CATALYSIS LETTERS
·
2023
·
IF 2.8
Zhang Chao,Zhang Zhengping,Niu Jin,Li Zhilin,Wang Feng
Platinum catalysts with {111} surface has obvious advantages, but the control of {111} exposure usually requires surfactants which cover the surface and decrease the catalytic performance. In this paper, tetrahedral platinum nanoparticle catalysts were successfully prepared with a simple one-step hydrothermal method and their size were successfully controlled under sub-5 nm. The tetrahedral morphology was controlled through the decomposition of dimethylamine by DMF and the small size was determined by alcohol acid radical. Because of the profitable effect of the amines for the tetrahedral morphology, no surfactant was need during the preparation. The catalysis activity was assured by the tetrahedral morphology with Pt {111} exposure without the surfactant covering, and the small size further increased the number of activity sites. For HOR, the catalyst showed higher activity, stronger anti-CO poisoning performance and longer stability than those of commercial catalyst with the same platinum load. For ORR, the catalyst also showed better performances which further promoted the four-electron reaction. Our simple preparation method successfully achieved the aims of the morphology control, size control and the elimination of surfactant, which effectively assured the good catalyst performances. The simple preparation path of such good catalysts shows a great application potential. Graphical Abstract
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JOURNAL OF MEMBRANE SCIENCE
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2023
·
IF 9.5
Jin-Bo Li,Cheng-Ye Zhu,Bian-Bian Guo,Chang Liu,Chao Zhang,Jian Wu,Lin Zhang,Hao-Cheng Yang,Zhi-Kang Xu
Synthesizing ultrathin polyamide nanofilms via interfacial polymerization (IP) at free interface offers a promising route to achieving preferential separation performance. However, one of big challenges lies in how to acquire large-scale synthesis and defect-free transfer of sub-5 nm polyamide nanofilms into robust composite membranes . Herein, we report an integrated strategy to allow for scalable synthesis and seamless compositing of sub-5 nm polyamide nanofilms that exhibit ultrafast and robust nanofiltration performance, by virtue of glycerol-regulated IP at free interface and transfer-printing compositing. Distinct from conventional hexane-water interface, our method leverages hexane-water/glycerol interface to boost interface stability of IP and confine monomer diffusion, enabling controllable synthesis of large-scale, defect-free sub-5 nm polyamide nanofilm. Meanwhile, a facile and universal transfer printing method is employed to integrate nanofilms on various substrates with high interfacial strength , which is not achievable with conventional transfer methods. The sub-5 nm polyamide composite membrane exhibits extraordinary water permeance (53.2 L⋅m −2 ⋅h −1 ·bar −1 ) and salt rejection (R Na2SO4 = 97.3%) under ultralow pressure of 1 bar, as well as superhigh water/salt permselectivity surpassing most of the polyamide composite membranes reported. The easy composite method and extraordinary performance in this work make ultrathin polyamide nanofilms a step closer to practical separation scenarios.
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ANALYTICA CHIMICA ACTA
·
2023
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IF 6.2
Mei Zhao,Guangrong Zou,Jing Tang,Jingyi Guo,Fang Wang,Zilin Chen
5-carboxycytosine (5caC) plays a critical role as an intermediate form in DNA methylation and demethylation processes. Its distribution and quantity significantly influence the dynamic equilibrium of these processes, thereby impacting the normal physiological activities of organisms. However, the analysis of 5caC presents a significant challenge due to its low abundance in the genome, making it almost undetectable in most tissues. In response to this challenge, we propose a selective method for 5caC detection using differential pulse voltammetry (DPV) at glassy carbon electrode (GCE), hinging on probe labeling. The probe molecule Biotin LC-Hydrazide was introduced into the target base and the labeled DNA was immobilized onto the electrode surface with the help of T4 polynucleotide kinase (T4 PNK). Leveraging the precise and efficient recognition of streptavidin and biotin, streptavidin-horseradish peroxidase (SA-HRP) on the surface of the electrode catalyzed a redox reaction involving hydroquinone and hydrogen peroxide, resulting in an amplified current signal. This procedure allowed us to quantitatively detect 5caC based on variations in current signals. This method demonstrated good linearity ranging from 0.01 to 100 nM with a detection limit as low as 7.9 pM. We have successfully applied it to evaluate the 5caC levels in complex biological samples. The probe labeling contributes to a high selectivity for 5caC detection, while the sulfhydryl modification via T4 PNK efficiently circumvents the limitation of specific sequences. Encouragingly, no reports have been made about electrochemical methods for detecting 5caC in DNA, suggesting that our method offers a promising alternative for 5caC detection in clinical samples.
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MOLECULAR NEUROBIOLOGY
·
2023
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IF 5.1
Hua Wei,Ma Shuainan,Pang Yuxin,Liu Qi,Wang Yueying,Liu Zhiyi,Zhao Nan,Ren Naixin,Jin Sinan,Wang Benshuai,Song Yuejia,Qi Jiping
Intracerebral hemorrhage (ICH) is a lethal stroke with high mortality or disability. However, effective therapy for ICH damage is generally lacking. Previous investigations have suggested that lysosomal protein transmembrane 5 (LAPTM5) is involved in various pathological processes, including autophagy, apoptosis, and inflammation. In this study, we aimed to identify the expression and functions of LAPTM5 in collagenase-induced ICH mouse models and hemoglobin-induced cell models. We found that LAPTM5 was highly expressed in brain tissues around the hematoma, and double immunostaining studies showed that LAPTM5 was co-expressed with microglia cells, neurons, and astrocytes. Following ICH, the mice presented increased brain edema, blood-brain barrier permeability, and neurological deficits, while pathological symptoms were alleviated after the LAPTM5 knockdown. Adeno-associated virus 9-mediated downregulation of LAPTM5 also improves ICH-induced secondary cerebral damage, including neuronal degeneration, the polarization of M1-like microglia, and inflammatory cascades. Furthermore, LAPTM5 promoted activation of the nuclear factor kappa-B (NF-κB) pathway in response to neuroinflammation. Further investigations indicated that brain injury improved by LAPTM5 knockdown was further exacerbated after the overexpression of receptor-interacting protein kinase 1 ( RIP1 ), which is revealed to trigger the NF-κB pathway. In vitro experiments demonstrated that LAPTM5 silencing inhibited hemoglobin-induced cell function and confirmed regulation between RIP1 and LAPTM5. In conclusion, the present study indicates that LAPTM5 may act as a positive regulator in the context of ICH by modulating the RIP1/NF-κB pathway. Thus, it may be a candidate gene for further study of molecular or therapeutic targets.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Chengbin Guo,Yubo Lian,Chen Huang,Zhenyu Chen
A novel sustained-release system was designed on the basis of metal–organic framework-5 (MOF-5) as a nanocontainer to load benzotriazole (BTA). Furthermore, the fabricated BTA/MOF-5 (BTA@MOF-5) was doped to the epoxy coating to improve the anticorrosion performance of copper. UV spectrophotometry proved the sustained-release behavior of BTA@MOF-5. Salt spray tests and electrochemical measurements demonstrated the self-healing ability of the composite coating . This novel sustained-release system provides a new strategy for metal protection.
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JOURNAL OF DRUG DELIVERY SCIENCE AND TECHNOLOGY
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2022
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IF 5.062
Duanxiu Li,Jiong Li,Zongwu Deng,Hailu Zhang
Supramolecular synthon strategy is an often-employed principle to guide the discovery of novel pharmaceutical cocrystals. The amine–carboxylate (N–H··· ― OOC) intermolecular interaction has been confirmed as a member of the supramolecular toolbox, and a cocrystal of 5-fluorocytosine (FC) with L -proline (FC– L -PRO) containing this heterosynthon was previously harvested. Herein, two new cocrystals of FC with sarcosine (SAR) or dimethylglycine (DMG) were successfully screened out. Similar to FC– L -PRO, the N–H··· ― OOC synthon presents as the most important hetero-molecular interaction between FC and SAR/DMG in their crystal structures. And the FC molecular ribbons via homo-molecular N–H⋯N and N–H⋯O hydrogen bonds were observed in all of the cocrystal structures, which also exist in the structure of FC. Theoretical calculations show that the formations of FC– L -PRO and FC–DMG are thermodynamically favorable. While for FC–SAR–MeOH, the calculated result is not applicable. The coformer competitive experiments reveal that FC– L -PRO and FC–DMG have similar relative stability and FC–SAR–MeOH is the relative unstable form. These cocrystals exhibit weakened physical stability under high humidity condition (75% RH), then should be stored in controlled humidity conditions (≤50% RH). Additionally, FC– L -PRO demonstrates reduced intrinsic dissolution rate (IDR) in pH 1.2 medium (simulated gastric fluid), which may provide positive contribution to alleviate its toxic side effects.
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ACS Applied Nano Materials
·
2022
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IF 6.14
Yiyuan Tao,Shiying Fan,Xinyong Li,Jing Yang,Jingang Wang,Moses O. Tadé,Shaomin Liu
The electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) is considered to be the most promising way to achieve green conversion of biomass resources in industrial production. Herein, a series of CuxCo3–xO4 (0 ≤ x ≤ 1) nanofibers are obtained using an electrospinning method, with discovering the role of Cu/Co interactions in modulating the electronic structure of reaction sites and acidic sites for enhancing the intrinsic activity of HMF electro-oxidation (HMFOR). According to the characterizations and theoretical calculations, the reasonable ratio of Cu/Co affects the structure of active sites and the exposure of Lewis adsorption sites in the spinel and thus finally determines an outstanding catalytic activity. An appropriate amount of Cu occupying the tetrahedral sites in the Co-based spinel promotes significantly the electrocatalytic property; specifically, Cu0.5Co2.5O4 shows the best performance of HMF with a selectivity of 93% and Faraday efficiency of 91% for FDCA. This work offers a strategy to design highly active catalysts by adjusting the metal composition and provides an insight into the modulation of multimetal active site structures at the atomic scale.
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Materials
·
2022
·Vol. 15
·期 22
·8097
·
IF 3.748
Hongyun Wang,Haijun Cheng,Fang Lai,Deyuan Xiong
Copper(II)-containing aluminum phosphate material (CuAPO-5) was synthesized hydrothermally and used as a multiphase catalyst for the oxidation of α-pinene to verbenone. The catalysts were analyzed using X-ray diffraction (XRD), Brunauer–Emmett–Teller (BET) surface area techniques, X-ray photoelectron spectroscopy (XPS), and ammonia temperature programmed reduction (NH3-TPD). Scanning electron microscopy (SEM), X-ray energy spectrometry (EDS), inductively coupled plasma emission spectroscopy (ICP-OES), Fourier infrared spectroscopy (FT-IR), and ultraviolet-visible spectroscopy (UV-vis) were performed to characterize the material. The effects of reaction temperature, reaction time, n(α-pinene)/n(TBHP), and solvent on the catalytic performance of CuAPO-5 were investigated. The results show that all the prepared catalysts have AFI topology and a large specific surface area. Copper is evenly distributed in the skeleton in a bivalent form. The introduction of copper increases the acid content of the catalyst. Under the optimized reaction conditions, 96.8% conversion of α-pinene and 46.4% selectivity to verbenone were achieved by CuAPO-5(0.06) molecular sieve within a reaction time of 12 h. CuAPO-5(0.06) can be recycled for five cycles without losing the conversion of α-pinene and the selectivity to verbenone.Keywords:CuAPO-5;α-pinene;selective oxidation;verbenone
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FUEL
·
2022
·
IF 8.035
Zhongqiang Tang,Siyuan Zhao,Xiao Zhao,Runze Jin,Jiaofei Wang,Zhuangzhuang Zhang,Haobin Hu,Xinwen Guo,Chengyi Dai,Xiaoxun Ma
The conversion of naphthalene into high value-added intermediate, 2,6-dimethylnaphthalene (2,6-DMN), using methanol as an alkylating agent has been widely studied. However, the low conversion of naphthalene and the easy deactivation of catalysts due to carbon deposition still pose challenges for industrialization. This is attributed mainly to the huge difference in the conversion kinetics of naphthalene and methanol. Herein, we report the first one-step process for the synthesis of 2,6-DMN from naphthalene by direct alkylation with syngas over “ZnAlCrOx&HZSM-5″ bifunctional catalyst. Compared to the traditional alkylation process of naphthalene with methanol, the direct alkylation of naphthalene with syngas not only shortened the process route and improved the reaction balance of syngas to methanol, but also improved the effective utilization rate of CO (29.87 %), naphthalene conversion, and catalyst stability. Results indicated that the alkylation of naphthalene could be improved by appropriately narrowing the spacing between the ZnAlCrOx oxide and HZSM-5. The acid strength and acidity on the external surface of HZSM-5 were modified by P or Si to improve the initial conversion of naphthalene and the selectivity for 2,6-DMN. The difficulty in determining the deactivation point of catalysts with multiple active sites under complex catalytic systems was solved by adopting a strategy of ”improve shortcomings“. The decline of metal activity in this reaction was found to be the main reason for catalyst deactivation. Doping of Ce into ZnAlCrOx helped to improve the stability of the catalyst from 80 h to 120 h.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Huimin Li,Tiantong Zhang,Mao Peng,Qianqian Zhang,Jing Liu,Jinli Zhang,Yan Fu,Wei Li
Electrochemical reactions are important method for reducing the carbon footprint of large-scale chemical processes. Highly selective conversion of 5-hydroxymethylfurfural (HMF) to 2,5-dihydroxymethylfuran (DHMF) is achieved under mild conditions through electrocatalytic hydrogenation (ECH) over AgCu nanoalloys supported by the pyrolyzed biomass alginic acid sodium (PA), with the advantage of utilizing the active hydrogen intermediates in the process. The Ag 1 Cu 1 /PA exhibits outstanding performance in ECH of HMF with a selectivity of 94% toward DHMF at a conversion of 93.2% and the Faraday efficiency (FE) of 61.8%, which are significantly superior to those over Ag/PA (selectivity of 53.89%, conversion of 90.6%, and FE 25.79%). The incorporation of Cu into Ag nanoparticles boosts the charge transferability and lowers the onset potential of ECH. Density functional theory calculations reveal that AgCu alloy provides more electron transfer to HMF and lowers the energy barrier for HMF hydrogenation.
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Catalysis Science & Technology
·
2022
·Vol. 12
·期 24
·7281-7292
·
IF 6.177
Hui Chen,Wei Li,Mingchao Zhang,Wangyang Wang,Xian-Hua Zhang,Fa Lu,Kang Cheng,Qinghong Zhang,Ye Wang
Propane dehydroaromatization (PDA) to high value-added aromatic hydrocarbons, such as benzene, toluene, and xylene (BTX), is an attractive but challenging process. The traditional Zn/H-ZSM-5 or Ga/H-ZSM-5 catalysts can offer considerable PDA performances but still suffer from low activity and poor stability because of harsh reaction conditions. Here, we report a multifunctional Pt–Zn@H-ZSM-5 catalyst that exhibits a significantly improved performance in the PDA reaction at 550 °C, with a single-pass propane conversion of 74%, aromatics selectivity of 56%, and CH4 selectivity of only 4.7%. The yield of aromatics is twice as much as those of Zn/H-ZSM-5 and Ga/H-ZSM-5 catalysts. We have demonstrated that the Pt–Zn alloy nanoparticles with an average size of 2.4 nm are uniformly confined within H-ZSM-5 crystals, providing atomic-scale proximity between metal and zeolite acid sites. This unique structure enhances not only the dehydrogenation of the propane feedstock in the initial reaction stage but also the dehydrogenation of cyclic C6+ hydrocarbons by the recombinative desorption of surface hydrogen species in the last stage while suppressing the side hydrogenolysis and hydrogen-transfer reactions. Furthermore, the Si/Al ratio of H-ZSM-5, the synergistic effect between platinum and zinc, and the location of Pt–Zn nanoparticles over composite catalysts have also been discussed. These findings suggest that via bimetallic alloying and rational arrangements of functional sites at the nanoscale, the multistep PDA reaction can be greatly intensified.
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