JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
IF 9.9
Yingxin Bian,Danhong Song,Zejun Fu,Chao Jiang,Chen Xu,Lei Zhang,Kun Wang,Shujun Wang,Dongping Sun
Known to be biocompatible and hemocompatible, polyethylene glycol (PEG) has been widely used as anti-fouling coating of biomaterials. Nanoparticles coated with functionalized PEG were also investigated for their nano-cell interactions, but seldomly on the coagulation system, especially with platelets. Both experiments and molecular dynamic simulations indicate that terminal carboxylation of PEG promotes its binding with calcium, especially in the ionized form, which makes it potential anticoagulants. Further, the carboxyl PEGylated magnetic nanoparticle (HOOC-PEG 2000 -MNP) exhibits significantly increased anticoagulant and antiplatelet properties, by entering the open canalicular system (OCS) of human platelets and binding with the cytoplasmic calcium ions. HOOC-PEG 2000 -MNP also acts as effective thrombolytic agents in dissolving mature blood clots under oscillating magnetic field both in vitro and in vivo. Therefore, the carboxyl PEGylated magnetic nanoparticles are prototype agents for antithrombotic and thrombolytic therapies and provide a versatile platform for targeted and effective treatments of acute cardiovascular diseases.
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PubMed
高影响因子
FUEL
·
2022
·
IF 8.035
Han-Bing Gao,Le-Le Qiu,Fa-Peng Wu,Jian Xiao,Yun-Peng Zhao,Jing Liang,Yong-Hui Bai,Fang-Jing Liu,Jing-Pei Cao
Catalytic hydrogenolysis of C O bonds in lignin provides a promising route to produce high value-added biofuels and chemicals. However, designing highly active and stable catalysts for this process is still a challenge. Herein, a series of Ni/Al 2 O 3 catalysts were synthesized by calcination and reduction of layered double hydroxide precursors, and their activities were evaluated in the catalytic conversion of lignin-derived compounds. Diphenyl ether was completely converted with a 100% monomeric selectivity (cyclohexane and cyclohexanol) over the optimized Ni/Al 2 O 3 -500 under the optimal conditions of 200 ℃, 0.5 MPa H 2 and 1.5 h, indicating the excellent catalytic activity in the cleavage of C O bonds of the catalyst. The excellent catalytic performances of Ni/Al 2 O 3 -500 were originated from its relatively large specific surface area, well-developed porosity, small crystallite size, high Ni 0 concentration and strong interaction between the active metal and support. The reusability experiments show that Ni/Al 2 O 3 -500 possesses a relatively high stability for six reuses. Moreover, various lignin model compounds can be completely converted to corresponding monomeric products over Ni/Al 2 O 3 -500, indicating the applicability of this ingenious catalyst. The application of the hydrotalcite-derived Ni-based catalysts with high activity and stability provides a promising approach for the efficient hydrogenolysis of lignin derivatives.
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高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 7
·2210860
·
IF 19
Chenya Zhuo,Huiming Kong,Ke Yi,Chun-Wei Chi,Jiabing Zhang,Ran Chen,Haixia Wang,Caixia Wu,Yeh-Hsing Lao,Yu Tao,Mingqiang Li
Chronic hepatitis B infection remains incurable due to the stable presence of various forms of hepatitis B virus (HBV) genome, especially the HBV covalently closed circular DNA (cccDNA). The emergence of clustered regularly interspaced short palindromic repeat (CRISPR) technology provides a new opportunity to potentially cure the HBV infection. However, the efficiency and specificity remain unsatisfactory, especially for nonviral CRISPR/Cas9 delivery. To tackle these, a liver-specific CRISPR/Cas9 magnetic nanosystem FMNP pAG333/sgXPP is constructed based on fluorinated polyethylenimine-coated magnetic nanoparticles and liver-specific ApoE.HCR.hAAT promoter-driven Cas9-T2A-EGFP plasmid with dual sgRNAs. The elaborate system enables magnetic field-induced spatially specific distribution and hepatocyte-specific promoter-driven liver-specific gene editing. Moreover, this CRISPR/Cas9 magnetic nanosystem is designed to disrupt the two conserved sites in X opening reading frame and Pol opening reading frame of the HBV genome, thereby significantly inactivating the HBV genome without showing off-target effects. Treatment with FMNP pAG333/sgXPP for 7 days reduces serum HBsAg levels by 76% with a total editing efficiency of ≈20% in the two conserved sites. Collectively, this study demonstrates spatiotemporal liver genome editing as well as the feasibility of applying a nonviral CRISPR/Cas9 vector for HBV treatment, which may open up a new application for CRISPR therapeutics.
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高影响因子
FUEL
·
2023
·
IF 7.4
Guang-Hui Liu,Yong-Chao Qi,Han Wang,Ai-Min Wang,Yu-Hong Kang,Yong Gao,Ni Bai,Zhan-Ku Li,Xian-Yong Wei
This paper focused on the complementary advantages of density functional theory (DFT) calculation and catalytic reaction regulation. Based on the effective identification of intermediates, the possible catalytic hydroconversion (CHC) pathways of lignite-derived aryl ethers over Ni/mordenite were discussed. Bond dissociation energy (BDE) calculations of >C–O– bonds in different substrates and intermediates show that BDEs of >C ar –O– bonds are generally higher than those of >C al –O– bonds, and there is obvious electron aggregation near O atoms. Mulliken charge distribution analyses of different atomic sites further revealed the possible adsorption sites of active hydrogen, especially H · and H + . Possible cleavage pathways were further speculated by evaluating the stability of different leaving groups. In the early stage of CHC, aromatic ring hydrogenation and >C al –O– bond cleavage dominate, rather than >C ar –O– bond cleavage. Enthalpy change analyses combined with the CHC of real substrates further indicate that lowering temperature is beneficial to the cleavage of >C ar –O– bonds under the premise of inhibiting H ··· H transfer and obtaining H · effectively. Appropriately increasing the support acidity to ensure sufficient H + release is conducive to >C al –O– bond cleavage, especially direct dehydroxylation/dehydration. The analysis of synergetic transfer pathways of active hydrogen during the CHC provides theoretical guidance for the pathway optimization of converting lignite into high-quality clean liquid fuels.
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高影响因子
GREEN CHEMISTRY
·
2023
·Vol. 25
·期 17
·6869-6880
·
IF 9.8
Zhikun Peng,Zhixi Wu,Xiaotong Sun,Hongji Li
Aryl ethers greatly influence lignin depolymerization and the oxygen content in lignin products. Cleaving aryl ethers normally requires harsh conditions such as high-pressure hydrogen gas and elevated temperature. Herein, we developed a synergistic method that combines photocatalytic hydrogen transfer with acid catalysis for H2-free hydrogenolysis of diphenyl ether and aromatic oxygenates at room temperature. The electron-enriched Pt/TiO2 surface stored abundant hydrogen species under light irradiation and efficiently catalyzed hydrogen transfer from isopropanol to aryl ethers. The acid mediated the hydrogenation sequence into: hydrogenolysis of aryl C–O bonds > saturation of aryl rings ≫ hydrogenolysis of aliphatic C–O bonds. DFT calculations suggested the aryl ether bond adsorbed on the Pt surface was weakened through protonation. This method delivered 98% yield of aliphatic monomers (73% cyclohexane and 25% cyclohexanol) from cleavage of diphenyl ether, and converted aromatic mixtures into cycloalkanes (57%) and aliphatic alcohols (9%) under mild conditions.
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高影响因子
Molecular Catalysis
·
2023
·
IF 4.6
Zong-Pin Fu,Yun-Peng Zhao,Fa-Peng Wu,Jin-Xuan Xie,Le-Le Qiu,Jian Xiao,Jing Liang,Yong-Hui Bai,Fang-Jing Liu,Jing-Pei Cao
The selective hydrogenolysis of C O bonds is critical for the effective valorization of lignin. Herein, we synthesized a series of highly efficient Ni x Co y Al-T catalysts by a coprecipitation-calcination-reduction method and evaluated their catalytic hydrogenolysis performance towards the C O bonds of lignin-derived aryl ether, using isopropanol as the hydrogen donor source. The results revealed that the Ni 0.5 Co 1.5 Al-600 catalyst displayed superior activity and its catalytic performances were strongly influenced by the Ni/Co molar ratios and calcination temperatures. The enhanced dispersion of metal particles and the electron transfer from Ni to Co in Ni 0.5 Co 1.5 Al-600 catalyst facilitated the cleavage of C O bonds in lignin model compounds. Furthermore, the β-benzyl-H atom in 2-phenoxy-1-phenylethanol (PPE) also contributes to the cleavage of C aliphatic -O bonds. Under optimized reaction conditions (180 ℃, reaction time 2 h), PPE was completely converted over the Ni 0.5 Co 1.5 Al-600 catalyst, and the yield of ethylbenzene and cyclohexanol reached 95.91wt% and 85.73wt%, respectively. These findings demonstrate that the Ni x Co y Al-T catalytic system holds great promise for the production of valuable chemicals from lignin under mild conditions.
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高影响因子
International Journal of Electrochemical Science
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2023
·
IF 1.5
Yiqi Cui,Shuaikang Ying,Hongzhong Cai,Yan Wei,Changyi Hu
Carbon-supported platinum (Pt) for oxygen reduction reaction plays an important role in the operation of direct methanol fuel cells (DMFCs). However, complete oxidation of ethanol is difficult due to the low chemical activity of Pt / C. Herein, novel highly active Pt-Co/C nanoparticles with controllable chemical composition and particle size are prepared via a thermal reduction method. The results revealed that the catalyst (particle size: 2–4 nm) is characterized by a good size monodispersity, and exhibits satisfactory chemical activity. The nanoparticles were also characterized by an accurate and maintained stoichiometry ratio, resulting in improved electrocatalytic activity and anti-poisoning ability of the carbon-supported Pt.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jie Liu,Li Gao,Xuehua Ruan,Wenji Zheng,Xiaoming Yan,Gaohong He
Poly(aryl piperidinium) is considered a promising material for the preparation of anion exchange membranes (AEM) with considerable conductivity and excellent chemical stability for anion exchange membrane fuel cells (AEMFC). In this research, we report a range of biphenyl ether-containing poly(aryl ether piperidinium) unlike previous ones to increase the conductivity of AEMs and the peak power density (PPD) of fuel cells, and the alkaline stability of ether bonds in the polymer backbone is demonstrated. All of the poly(aryl ether piperidinium) membranes possess comparable mechanical properties and inherent viscosity derived from the high activity of biphenyl ethers in superacid-catalyzed reactions, which means that large-width AEMs can be prepared. The data demonstrated that the poly (ether p-terphenyl piperidinium) (QPEPTpi-35) exhibited a conductivity of 140 mS cm −1 at 80 ℃ compared to the original poly (p-terphenyl piperidinium) (QPTPpi) membrane owning to optimized micro-phase separation structure and higher water uptake. Meanwhile, QPEPTpi-35 membrane conductivity retention is greater than 85% after immersion in 1 M KOH for 2000 h at 80 ℃. Moreover, the PPD of the QPEPTpi-35 membrane reaches 1.2 W cm −2 in H 2 /O 2 fuel cells, which is much higher than that of the QPTPpi membrane (0.51 W cm −2 ). The durability of MEA prepared by the catalyst-coated substrate (CCS) method manifests over 20 h under 0.2 A cm −2 at 60 °C.
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高影响因子
FUEL
·
2022
·
IF 8.035
Yuanfei Bao,Jianliang Liu,Yige Zhang,Liping Zheng,Jiacong Ma,Fei Zhang,Yubing Xiong,Xiangju Meng,Zhifeng Dai,Feng-Shou Xiao
Low concentration (normal less than 15%) of CO 2 is mainly resulted from emission of industrial processes, and its transformation into value-added chemicals over heterogeneous catalysts is of great significance for sustainable reduction of CO 2 accumulation. Herein, we reported a series of porous organic polymers (POPs) with diverse quaternary phosphonium units constructed from phosphonium reaction of halogen-functionalized porous divinylbenzene polymers with phosphines. These POPs have large surface areas and hierarchical porosity, exhibiting excellent catalytic properties in cycloaddition reaction of CO 2 and epoxides even under the co-catalyst free and mild conditions. Structural comparison of the catalysts reveals that the catalytic activities increase with the steric hindrance of the quaternary phosphonium units in the catalysts. For example, catalytic activity of the porous organic polymer with tricyclohexyl phosphonium chloride unit (POP-BnCl-CP) was higher than that of porous organic polymers with tributyl phosphonium chloride (POP-BnCl-BP) and triphenyl phosphonium chloride (POP-BnCl-PP) units. Particularly, this difference was more obvious when low concentration of CO 2 was employed in the reaction. In this case, the POP-BnCl-CP has the CO 2 conversion at 94.3% with product selectivity at 99.0%, while the POP-BnCl-BP and POP-BnCl-PP have relatively low conversion and selectivity (67.6% and 99.0% for POP-BnCl-BP and 55.2% and 99.0% for POP-BnCl-PP). The high activity and excellent selectivity of the POP-BnCl-BP catalyst in the absence of any co-catalyst under mild conditions should be important for chemical fixation of CO 2 with low concentration into value-added chemicals in the future.
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高影响因子
Journal of Energy Chemistry
·
2022
·
IF 13.599
Shuang Xiang,Lin Dong,Zhiqiang Wang,Xue Han,Yong Guo,Xiaohui Liu,Xue-Qing Gong,Yanqin Wang
The depolymerization and upgrading of lignin from raw biomass, while keeping cellulose intact is important in biorefinery and various metal-based catalysts have been used in reductive catalytic fractionation, a key method in “lignin-first” strategy. Recently, we found that a core–shell structured Co@CoO catalyst with CoO shell as the real active site had excellent performance in the hydrogenolysis of 5-hydromethylfurfural to 2,5-dimethylfuran due to its unique ability to dissociate H 2 and yield active H δ− species (Xiang et al., 2022). In this work, we report a one-pot depolymerization and upgrading of lignocellulose to alkylcyclohexanols, a flavour precursor, with intact cellulose over this unique core–shell structured catalyst, Co@CoO. Lignin model compounds (β-O-4, 4-O-5, α-O-4) were first used to clarify the activity of Co@CoO catalyst. Then, the one-pot conversion of various organosolv lignin (birch, pine and poplar) to alkylcyclohexanols was realized with the mass yield of alkylcyclohexanols up to 25.8 wt% from birch lignin under the reaction condition of 210 °C, 1 MPa H 2 , 16 h. Finally, the corresponding woody sawdusts were used as feedstocks and found that the Co@CoO catalyst indeed preferentially depolymerized and upgraded the lignin part and obtained the same alkylcyclohexanols products with the retention of cellulose-rich pulp. The collected alkylcyclohexanols were further esterified to obtain value-added esters, which can be used as flavors. This work will inspire the design of new efficient metal oxide catalysts in lignin fractionation and depolymerization to high-value-added chemicals with intact cellulose.
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高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Endian Cui,Xiangyang Yuan,Luomeng Tang,Lu Yang,Xiaoyan Yang,Xiaoling Liao,Jianfeng Tang,Yanan Zhao,Wei Sun,Kai Liu,Yingshuai Liu,Jing Liu
Incorporation of lanthanide ions (Ln 3+ ) can remarkably enhance the structural stability and optical properties of lead-free perovskite NCs. Herein, we have established the relationship between the intrinsic emission of Cs 2 AgInCl 6 host and the Ln 3+ by Eu 3+ , Tb 3+ doping in Cs 2 AgInCl 6 NCs, realizing tunable luminescence of NCs in the visible region. Experimental studies and density functional theory (DFT) calculations analysis show that Eu 3+ and Tb 3+ occupy the sites of In 3+ in Cs 2 AgInCl 6 , the defect formation energy for Cs 2 AgInCl 6 :Ln 3+ is larger than the pristine Cs 2 AgInCl 6 , resulting in a more stable cubic double perovskite structure. The optical band gap increases with the increase in Ln 3+ doping percentage. Turning excitation from 250 nm to 300 nm, the broad self-trapped excitons (STEs) emission is more remarkable, and the narrow Ln 3+ emission is less notable. The emitted color can be adjusted from white to red and to green light by altering the doping concentration of Eu 3+ or Tb 3+ and excitation wavelength. This work promotes the design and optoelectronic application of desired lead-free perovskites.
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高影响因子
Catalysts
·
2022
·Vol. 12
·期 11
·1328
·
IF 4.501
Liang-Qiu Huang,Zhi-Jun Diao,Bo Chen,Qing-Pan Du,Kai-Yang Duan,Si-Jia Zhao
Efficient depolymerization of C–O linkages is essential for converting lignin into fuels and higher value-added chemicals. In this work, CoRuP/SiO2, an amorphous Ru-Co phosphide composite, was fabricated for the efficient hydrogenolysis of ether linkages. The 4–O–5 andα–O–4 linkages containing lignin-related compounds, such as diphenyl ether, benzyl phenyl ether, 3-methyl diphenyl ether, and dibenzyl ether, are selected as representatives of linkages in lignin. Under mild conditions, Ru-containing metallic phosphides have high-performance for the catalytic depolymerization of C–O linkages. Compared with other catalysts, CoRuP/SiO2shows an outstanding selectivity for benzene and excellent efficiency in depolymerizing diphenyl ethers, yielding only a small amount of by-products. Furthermore, the total acidity shows a linear relationship with the hydrogenolysis reactivity in cleaving aromatic ether bonds. The mechanisms for the catalytic hydrogenolysis of 4–O–5 andα–O–4 bonds over CoRuP/SiO2are proposed. Moreover, two-dimensional heteronuclear single quantum coherence nuclear magnetic resonance spectroscopic analysis demonstrates that CoRuP/SiO2could effectively depolymerize C–O bonds of lignin. These dominant hydrogenolysis products from lignin have excellent potential in the production of high value-added drugs or pharmaceutical intermediates. The hydrogenolysis of lignin can be a highly efficient alternative to the existing method of lignin utilization.Keywords:hydrogenolysis;C–O linkages;metallic phosphides;reaction pathway
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高影响因子
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