Small
·
2023
·Vol. 19
·期 50
·2304674
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IF 13.3
Kailai Zhang,Xiaodong Sun,Haijun Hu,Ge Yan,Anqi Qin,Yali Ma,Hongwei Huang,Tianyi Ma
Mechanical energy driven piezocatalytic hydrogen (H 2 ) production is a promising way to solve the energy crisis . But limited by the slow separation and transfer efficiency of piezoelectric charges generated on the surface of piezocatalysts , the piezocatalytic performance is still not satisfactory. Here, defect engineering is first used to optimize the piezocatalytic performance of microcrystalline cellulose (MCC). The piezocatalytic H 2 production rate of MCC with the optimal defect concentration can reach up to 84.47 µmol g −1 h −1 under ultrasonic vibration without any co-catalyst, which is ≈3.74 times higher than that of the pure MCC (22.65 µmol g −1 h −1 ). The enhanced H 2 production rate by piezoelectric catalysis is mainly due to the introduction of defect engineering on MCC, which disorders the symmetry of MCC crystal structure, improves the electrical conductivity of the material, and accelerates the separation and transfer efficiency of piezoelectric charges. Moreover, the piezocatalytic H 2 production rate of MCC with the optimal defect concentration can still reach up to 93.61 µmol g −1 h −1 in natural seawater, showingits commendable practicability. This study presents a novel view for designing marvelous-performance biomass piezocatalysts through defect engineering, which can efficiently convert mechanical energy into chemical energy .
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CHINESE JOURNAL OF CATALYSIS
·
2023
·
IF 16.5
Zhiyue Zhao,Zhiwei Jiang,Yizhe Huang,Mebrouka Boubeche,Valentina G. Matveeva,Hector F. Garces,Huixia Luo,Kai Yan
The rational design and green synthesis of low-cost, robust, and efficient catalysts for the selective oxidation of various alcohols are highly challenging. Herein, we report a fast and solvent-free arc-melting (AM) method to controllably synthesize a semimetallic CoSi alloy catalyst (denoted as AM-CoSi) that is efficient in the base- and solvent-free oxidation of six types of aromatic alcohols. X-ray absorption fine structure analysis, electron paramagnetic resonance spectroscopy, and aberration-corrected high angle annular dark field scanning transmission electron microscopy confirmed the successful synthesis of AM-CoSi with abundant Si vacancies (Si v ). The as-prepared CoSi alloy catalysts exhibit an order of magnitude greater activity in the oxidation of a model reactant, benzyl alcohol (BAL) to benzyl benzoate (BBE), compared with their mono-counterparts, and provide 70% yield of BBE, the highest yield reported to date. Experimental results and density functional theory calculations suggest that the CoSi alloy structure improves the BAL conversion and that Si vacancy is the main contributor to the generation of BBE, based on which a potential reaction pathway is rationally proposed. Furthermore, the CoSi alloy maintains high stability and also exhibits high activity in the selective oxidation of various alcohols with different functional groups. This work demonstrates for the first time that semimetallic CoSi alloys can be robust catalysts for the green oxidation of various alcohols and proviedes a vast opportunity for the rational design and application of other semimetal alloy catalysts.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Lifeng Hao,Zewen Jiang,Yujie Fang,Yang Zhou,Bin Fu,Liyu Lin
Cerium salts have received significant attention for their potential in constructing protective materials on metallic substrates. However, there are few studies on the use of cerium oxide nanoparticles (CeO 2 NPs) as corrosion inhibitors, and even fewer on the mechanisms by which they protect steel. In this work, we discuss the effect of oxygen vacancy on the corrosion resistance of an epoxy coating containing cobalt-doped CeO 2 NPs in detail. To evaluate the effect of oxygen vacancy on corrosion resistance, we obtained CeO 2 and Ce 7 CoO 16 NPs, as well as KH560-Ce 7 CoO 16 NPs, through a controlled facile sol-gel method. The results indicated that KH560-Ce 7 CoO 16 NPs had a higher percentage of Ce 3+ and oxygen vacancy (O v ) compared to CeO 2 and Ce 7 CoO 16 NPs. Specifically, KH560-Ce 7 CoO 16 NPs were found to have 32.12% Ce 3+ and 46.65% O v , whereas CeO 2 and Ce 7 CoO 16 nanoparticles had lower Ce 3+ and O v ratios, with values of 23.46% and 27.30%, and 29.79% and 45.60%, respectively. The micromorphology of CeO 2 , Ce 7 CoO 16 , and KH560-Ce 7 CoO 16 in the epoxy matrix indicated that the addition of 2% KH560-Ce 7 CoO 16 NPs achieved a homogeneous dispersion. Compared to the CeO 2 and Ce 7 CoO 16 NPs, KH560-Ce 7 CoO 16 NPs at an appropriate concentration exhibited excellent corrosion resistance performance for the substrate, as evaluated by electrochemical and salt spray tests. We propose that two mechanisms synergistically contribute to the corrosion protection. Firstly, due to oxygen reduction, insoluble cerium hydroxide is formed at the cathodic sites. Secondly, O v acts as a charge capture center, facilitating the transfer of electrons lost by the anode to the oxygen vacancies and blocking the OH – generated by the cathodic reaction, as well as the new substances generated by the Fe 2+ produced by the anodic reaction, which ultimately slows down the corrosion chemical reaction process. This work provides a novel understanding of cerium oxide nanoparticles as corrosion inhibitors, and presents an effective strategy for achieving excellent corrosion resistance performance in a corrosive environment.
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BIOMATERIALS
·
2021
·
IF 12.479
Xianqi Zhu,Lin Li,Jin Tang,Chunyu Yang,Hao Yu,Kunpeng Liu,Ziyan Zheng,Xinggui Gu,Qingsong Yu,Fu-Jian Xu,Zhihua Gan
Metastasis has been widely recognized as the most lethal threats for cancer patients . Due to their special genetic and environmental context, cancer stem cells (CSCs) which are resistant to most cytotoxic drugs and radiation, are considered as the dominant culprit for metastasis. Thus, the efficient targeting and thorough elimination of CSCs are significantly urgent for the enhancement of therapeutic efficacy. Herein, we developed a facile and smart photothermal-chemo therapeutic nano-assembly system, of which the surface was modified by a sheddable PEG shell and acid-activatable pro-penetration peptide, to surmount the physiological barriers in targeting CSCs. A highly-efficient diradical-featured croconium-based photothermal agent and a natural cytotoxic heat shock protein (HSP) inhibitor were co-loaded in redox-sensitive chitosan matrices to realize the synergistic photothermal-chemo therapy. Within solid tumors, the PEG shell that prevents the nano-assembly from mononuclear phagocytic clearance could rapidly leave to expose the positively charged chitosan, and the detached iRGD could further actuate the tumor penetration of chitosan nanoparticles , and allow the CSCs targeting by selective recognition of CD44 protein. Owing to the HSP inhibition and chemo-sensitization, both the CSCs and non-CSCs could be thoroughly eliminated by the designed nano-assembly, largely inhibiting the tumor growth and metastasis. This work provides a potential strategy for CSCs-targeting drug delivery to solve the CSCs-related metastasis.
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REACTIVE & FUNCTIONAL POLYMERS
·
2021
·
IF 3.975
Zhitao Hu,Xiaohui Cao,Huahua Huang,Yongming Chen
Poly( ε -caprolactone) (PCL) has been one of the most important biomaterials, but its instinct hydrophobicity and slow biodegradation limit its broad applications. Herein, copolymerization of CL and a hydrophilic macrolactone, 2-oxo-15-crown-5 ether (O15C), was achieved through ring opening polymerization catalyzed by 1,5,7-triazabicyclo[4.4.0]dec-5-ene (TBD) using benzyl alcohol as the initiator at room temperature . A series of poly(CL- co -O15C) copolymers with different O15C contents were prepared by simply tuning the feeding ratio of [CL]/[O15C]. They showed molecular weights ranging from 11.0 to 20.6 kg mol −1 , and polydispersity index between 1.4 and 1.6, characterized by SEC (Size Exclusion Chromatography). Analysis of 1 H NMR indicated that the copolymers belong to a random copolymer structure. The introduction of O15C had a significant influence on thermal stability, hydrophilicity and degradability of the copolymers. With increasing the O15C content, the crystalline ability of PCL segment among the copolymers reduced, while the hydrophilic property was improved obviously. Through hydrolysis experiment, the poly(CL- co -O15C) with O15C content of 38 mol% exhibited a much faster degradable rate than that of the copolymer with O15C content of 10 mol%. Therefore, copolymerization of CL with a crown ether monomer via organic catalyst mediated ROP will be a feasible strategy for modification of polyester materials.
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EUROPEAN POLYMER JOURNAL
·
2021
·
IF 4.598
Yang Chen,Jie Zhang,Wenhao Xiao,Anfu Chen,Zhixian Dong,Jinbao Xu,Wenhua Xu,Caihong Lei
1,8-Diazabicyclo[5.4.0]undec-7-ene (DBU) was used as organocatalyst to reinvestigate the ring-opening polymerization (ROP) of ε -caprolactone (CL) with benzyl alcohol (BnOH) initiator in bulk at 90 °C considering the unsuccessful ROP of CL at RT in previously reported publications. Kinetic study indicates that the PCLs could be well-designed with a controlled/living character of polymerization. The use of functional initiators, such as 2-hydroxyethyl methacrylate (HEMA), propargyl alcohol (PGA), 6-azido-1-hexanol (AHA) and methoxy poly(ethylene glycol) (mPEG) leads to end-functionalized PCLs. Accordingly, the block copolymerization of CL with δ-valerolactone (VL), trimethylene carbonate (TMC) and lactide (LA) successfully proceeded to give PCL- b -PVL, PCL- b -PTMC and PCL- b -PLA copolymers. Finally, the reaction mechanism was studied with DFT calculations and NMR measurements.
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NANOTECHNOLOGY
·
2021
·Vol. 33
·期 10
·105501
·
IF 3.874
Yunxia Yang,Qian Liu,Yisong Zhao,Jianmin Chen,Bing Chen,Yanling Yan,Faming Gao
The electrode material is vital for the performance of the electrochemical biosensor. Lately, many nanomaterials have been developed to improve the sensitivity and detection efficiency of the biosensors. In this work, a kind of one-dimensional nanomaterials, the CuPt alloy nanotubes with an open end (CuPt alloy NTs-AOE), was explored. The nanotubes with an open end can provide a larger electrochemical active surface area and more active sites for the immobilization of enzyme. The CuPt alloy displays excellent conductivity and catalytic activity. In addition, the Cu shows the great affinity to thio-compounds, which can greatly enhance the detection efficiency and sensitivity. As a result, the prepared biosensor demonstrates the wider linear range of 9.98 × 10−10–9.98 × 10–5 g l−1 for fenitrothion and 9.94 × 10−11–9.94 × 10–4 g l−1 for dichlorvos (as model OPs ) and with the lower detection limit of 1.84 × 10–10 g l−1 and 6.31 × 10–12 g l−1 (S/N = 3), respectively. Besides, the biosensor has been used to detect the real samples and obtains satisfactory recoveries (95.58%–100.56%).
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E-POLYMERS
·
2021
·Vol. 22
·期 1
·19-29
·
IF 2.025
Xiaochen Xia,Peijian Sun,Xuehui Sun,Yipeng Wang,Song Yang,Yunzhen Jia,Bin Peng,Cong Nie
A series of hyper-crosslinked polymers (HCPs) with connected hierarchical porous structures were synthesized from phenyl-based precursors of benzene (BEN), benzyl alcohol, aniline, biphenyl, and 1,3,5-triphenylbenzene (TPB) via the knitting method. The porous structures of the HCPs were greatly influenced by substituent groups and BEN ring number in the precursors. HCPs prepared from TPB had the largest surface area and pore volume with multiscale porosity. The porous structure of the HCPs could also be adjusted by the crosslinker amount. Insufficient crosslinking led to incomplete pore architecture, while excessive crosslinking resulted in a considerable decrease in the pore volume. With these HCPs as adsorbents, the BEN yield in the cigarette smoke could be largely reduced due to the connected multiscale porosity and π–π aromatic stacking interaction that facilitated the smoke aerosol passing and the small aromatic molecules absorbing, showing great potential of these HCPs as adsorbents for effective removal of BEN from cigarette smoke.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Qiang Sun,Tianhao Li,Yu Mao,Hongxia Gao,Teerawat Sema,Shengyu Wang,Libin Liu,Zhiwu Liang
Amine-based CO2 capture is a promising method to limit global CO2 emissions. However, large thermal energy consumption for CO2 desorption during amine regeneration has limited large-scale worldwide applications. Here, we show that an efficient MCM-41-SO3H-0.6 catalyst presented a superior catalytic performance, decreasing the relative heat duty by one-third and enhancing the instantaneous desorption rate by up to 195% in comparison with the monoethanolamine (MEA) regeneration without catalysts. The excellent catalytic activity is related to the combination of the properties of mesopore surface area × total acid sites, and a possible catalytic mechanism is proposed for the MCM-41-SO3H catalysts. Furthermore, the experimental results in the MEA solution regeneration process were consistent with density functional theory calculations in revealing the catalytic desorption mechanism. This work demonstrated that MCM-41 functionalized with sulfonic acid group catalysts could play an essential role in the post-combustion CO2 capture technology using aqueous MEA for industrial applications.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Mingchuang Shen,Yingzhang Shi,Zhiwen Wang,Taikang Wu,Ling Hu,Ling Wu
Ultrathin Bi 4 Ti 3 O 12 nanosheets (NS) with the thickness about 3.9 nm were successfully synthesized by a hydrothermal method and were used as a photocatalyst for the oxidation of benzyl alcohol (BA) to benzaldehyde (BAD). The photocatalytic performance of NS is about 8 times higher than that of bulk Bi 4 Ti 3 O 12 . In-situ FTIR of pyridine adsorption and NH 3 -TPD reveal that NS has more surface Lewis acid sites (Ti 4+ ) for the adsorption and activation of BA. The photogenerated electrons (e - ) and holes (h + ) of NS can be fully used to produce the superoxide radicals and carbon-centered radicals, respectively. The monolayer nanosheet structure of NS not only greatly promotes the separation of photogenerated carriers, but also achieves the efficient activation of BA molecules via the C O⋯Ti coordination. This work successfully reveals the surface/interface interactions between the surface active sites of a photocatalyst and the reactive molecules via using ultrathin nanosheet as a molecular platform.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Shuchun Li,Xuefei Zhang,Xiaoyan Huang,Shuchang Wu,Zailai Xie
Developing highly active and stable nanocarbon catalysts for selective oxidation reactions has attracted much attention due to their potential as an alternative to traditional metal-based or noble metal catalysts. However, the nature of active sites and the reaction mechanism of nanocarbon catalysts for oxidation reactions still remains largely unknown, which hinders the rational design and development of highly efficient carbon-based catalysts. Here we report a facile strategy for the synthesis of boron and nitrogen co-doped carbon nanosheet material (BNC), which exhibits excellent catalytic activity with 91% conversion and 99% selectivity in selective oxidation of benzyl alcohol into benzaldehyde, superior to those of traditional carbon materials (oxidized carbon nanotubes, graphites and commercial nanocarbons). Structural characterizations and kinetic measurements are studied to clarify the active site, in which phenolic hydroxyl on BNC is responsible for the production of benzaldehyde. Meanwhile, we put forward a possible reaction mechanism and point out the key factors in determining the reactivity for this reaction. Therefore, the present work provides new insight into structure–function relationships, paving the way for the development of highly efficient nanocarbon catalysts.
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Journal of Physical Chemistry C
·
2022
·
IF 4.177
Yue-Hua Li,Ming-Yu Qi,Zi-Rong Tang,Yi-Jun Xu
Coupling photocatalytic hydrogen (H2) evolution with selective organic synthesis in one redox cycle showcases great potential for the coinstantaneous utilization of photoexcited electrons and holes toward sustainable production of value-added fuels and chemicals. Herein, we construct one-dimensional/two-dimensional (1D/2D) WO3/ZnIn2S4 (WO3/ZIS) hierarchical Z-scheme composites for bifunctional integrated light-driven H2 production and biomass-derived aromatic alcohol conversion. The superior photoactivity and selectivity over WO3/ZIS composites compared with that over bare WO3 nanorods (NRs) and ZIS nanosheets (NSs) can be attributed to the assembly of the Z-scheme heterostructure. The construction of WO3/ZIS direct Z-scheme composites not only facilitates the charge separation dynamics by transporting photoinduced electrons and holes to spatially separated redox sites but also steers the selectivity of targeted products by tuning the energy band potentials to endow electrons and holes with stronger reduction and oxidation abilities. The mechanistic studies combining the control experiments and electron paramagnetic resonance spectroscopy validate the free radical mechanism of the benzyl alcohol photooxidation reaction. It is anticipated that this work would offer a conducive paradigm for the ingenious design of high-performance Z-scheme heterostructured catalysts toward the solar light-driven collaborative redox of H2 production and selective organic synthesis.
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