ACS Applied Nano Materials
·
2024
·
IF 5.3
Tianyue Su,Junsheng Wang,Chun Cai
The nickel phosphides have garnered increasing attention as an excellent catalytic site in the fields of electrocatalysis and hydrotreating, but their application in organic synthesis remains infrequent. In this study, ammonium phosphate and nickel chloride were employed as the doping sources for the first time to synthesize the Ni-based ZIF-8 precursor via the host–guest method. Subsequently, the precursor was pyrolyzed to obtain Ni2P nanoparticles (NPs) supported on N, P co-doped carbon. The composite materials exhibit elevated metal loading and effective dispersion due to the synergistic combination of phosphorus and nickel. Specifically, compared with Ni-NC, the optimal Ni2P-NCP-1 exhibits enhanced catalytic activity in the α-alkylation of arylacetonitriles with alcohols using KOH as the base. It shows a wide broad substrate scope at 140 °C for 12 h in n-octane using a hydrogen borrowing strategy. Through characterizations and mechanistic studies, it has been discovered that the introduction of P source not only provides more basic sites on carbon matrix but also leads to the formation of Ni2P NPs, which facilitates the catalytic efficiency by modifying the electronic structure of Ni. Compared with the metallic Ni species, the synergistic effect between Ni2P and acid-basic sites significantly influences the dehydrogenation of alcohols to generate Ni–H species. This study successfully achieves simultaneous phosphating of both the metal and support, and it also demonstrates that the N2P-NCP-1 catalyst has significant potential in the heterogeneous organic transformation field.
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
·
IF 4.326
Shuaifeng Liu,Edouard Asselin,Zhibao Li
An industrially feasible process was proposed to produce α-calcium sulfate hemihydrate (α-HH) from FGD gypsum without any additives. In this process, an AlCl3 solution was used to promote the conversion of calcium sulfate dihydrate (DH) to hexagonal prismatic α-HH with high strength at atmospheric pressure. The phase transition kinetics of FGD gypsum was experimentally investigated under conditions: AlCl3 (2–2.5 m), MgCl2 (0–0.4 m) existing in raw FGD gypsum, and the solid–liquid ratio (or solid content %) range of 0.1–2 at 363 K. It was found that increasing the concentrations of MgCl2 in AlCl3 solution accelerated the conversion. The uniform large hexagonal prism HH product was obtained at the folowing optimal conditions: 2.5 mol/kg AlCl3, 0.4 mol/kg MgCl2, solid–liquid ratio of 2, and equilibration time of 2 h at 363 K. The phase diagram of the AlCl3-MgCl2-H2O system was determined by measuring solubility of solids. The E-NRTL activity model was used to construct the phase transition diagram of CaSO4 in AlCl3–MgCl2 media and to judge the stable range of DH and HH.
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CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Jing Deng,Yongjian Ge,Chaoqun Tan,Hongyu Wang,Qingsong Li,Shiqing Zhou,Kejia Zhang
Nanoscale α-MnO 2 with different morphologies (nanoparticles, nanoflowers and nanorods) were synthesized via a facile hydrothermal method and tested in peroxymonosulfate (PMS) activation for ciprofloxacin (CIP) degradation. The catalytic activity of α-MnO 2 mainly relied on the specific surface area and crystallinity, and followed the order of α-MnO 2 nanoflowers > α-MnO 2 nanorods > α-MnO 2 nanoparticles > commercial MnO 2 . Acidic condition was more beneficial to CIP removal than neutral condition, and the degradation would be greatly accelerated in alkaline circumstance. The introduction of chloride and bicarbonate displayed concentration-dependent dual effect. The presence of natural organic matter (NOM) exerted the detrimental effect on CIP degradation. Eleven oxidation products were identified by UPLC–MS/MS and the changes of their concentrations were monitored, five products showed monotonous uptrend while four intermediates present monotonous downtrend once they were generated. Piperazine ring cleavage, hydroxylation and F/OH substitution were found to be the important oxidation pathways. The acute toxicity of resulted solution gradually decreased with the lapse of time, and higher PMS concentration favored the detoxification. The CIP removal in α-MnO 2 /PMS process was also efficient under the actual water background, which was testified by the results of fluorescence excitation-emission matrix (EEM).
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2020
·Vol. 31
·期 17
·14681-14690
·
IF 2.22
Gao Dahai,Yu Liyuan,Li Mengjiao,Wang Shumao,Dai Yuhua
In this work, we prepared the epoxy-based adhesives with a binary filler system, which was composed of organosilicon modified hexagonal BN ( h -BN) and α-Al 2 O 3 . H -BN platelets and α-Al 2 O 3 nanoparticles were decorated by aminopropyltrimethoxysilane (APTMS) and glycidylpropyltrimethoxysilane (GPTMS), respectively, to form covalent links to the filler/polymer matrix interface. The surface chemical composition was investigated by Fourrier transform infrared spectroscopy (FTIR) and thermogravimetry analysis (TGA), which demonstrated that the modifiers were successfully grafted onto the surface of fillers. This modification has been confirmed beneficial to thermal conductivity so that the thermal conductivity of adhesives incorporated with modified binary fillers could reach 0.85 w/m k, which is 10% more than specimen filled with unmodified fillers, because covalent links strengthened the interface and prohibited heat diffusion. Modified Hashin–Shtrikman model was utilized to analyze thermal resistance of the binary filler system, indicating that adhesives filled with modified fillers displayed lower thermal resistance. The enhancement of interface also brought about some other positive effect, especially in the decreasing of dielectric constant (< 4.3 at 1000 Hz) and the low values of dielectric loss tangent (10 –3 ) and high electronic resistance (> 10 14 ). Furthermore, the mechanical strength is significantly improved when the modified binary fillers were used.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2021
·
IF 7.46
Wenjing Pan,Yong Zhang,Sujing Yu,Xiaohua Liu,Dongzhi Zhang
The metal-organic framework (MOF)-derived alpha-iron oxide hollow nanosphere/molybdenum diselenide nanoflower (α-Fe 2 O 3 /MoSe 2 ) composite is fabricated via simple hydrothermal route. Multiple characterization methods have proved the successful synthesis of α-Fe 2 O 3 /MoSe 2 composites. The nanocomposite with a mass ratio of α-Fe 2 O 3 and MoSe 2 of 4:1 shows high response to H 2 S gas sensing. Moreover, the gas sensitivity test of the system shows that the α-Fe 2 O 3 /MoSe 2 composite sensor exhibits a faster response/recovery rate, outstanding repeatability and anti-humidity interference toward H 2 S sensing at room temperature, which also shows excellent selectivity for H 2 S compared to various potentially interfering gases. Further studies have shown that α-Fe 2 O 3 /MoSe 2 nanocomposites have improved H 2 S gas sensing performance due to the increased active sites and specific surface area, and the formation of n-n heterojunctions at the interface between α-Fe 2 O 3 hollow nanospheres and MoSe 2 nanoflowers.
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JOURNAL OF POWER SOURCES
·
2019
·
IF 7.467
Yunzhao Liu,Xiaowei Chi,Qi Han,Yuexiu Du,Jiaqi Huang,Yu Liu,Jianhua Yang
Rechargeable Zn-ion batteries (ZIBs) have attracted extensive attention, but their practical application is hindered by the limited cycling life and complicated preparation process of cathode materials . Here, we develop a facile yet scalable chemical precipitation/spray-granulation combined methodology for the fabrication of α-MnO 2 nanofibers/carbon nanotubes hierarchically assembled microspheres (α-MnO 2 /CNT HMs) as the cathode material for aqueous ZIBs . The α-MnO 2 evenly anchoring to the CNTs-based framework shows significantly increased tap density compared with pristine α-MnO 2 , which can effectively enhance the electrochemical stability. Owing to the synergistic merits of highly conductive carbon nanotubes network and α-MnO 2 nanofibers with desirable structure features, within our knowledge, the highest areal energy density of 0.98 Wh cm −2 at 0.2 A g −1 and the record cycling stability with 96% capacity retention over 10000 cycles at 3 A g −1 among the reported cathodes for ZIBs are achieved. Zn 2+ and H + co-insertion reaction mechanism with high reversibility is further revealed. Fast kinetic of the H + insertion/extraction process renders the cell excellent cycling stability. Facile preparation of nanofibrous α-MnO 2 based micro-composite, cost benefit of the source materials, and the superior battery performance provide new approaches for the practical applications of ZIBs.
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Qingdong Qin,Ting Liu,Jiaxuan Zhang,Rui Wei,Shijie You,Yan Xu
Hematite (α-Fe 2 O 3 ) has been commonly used as an eco-friendly catalyst for peroxymonosulfate (PMS) to generate free radicals (SO 4 •- and/or •OH). However, the activation efficiency of PMS relies heavily on the conversion of Fe(III) to Fe(II) that is slow and rate-limiting. In this study, oxygen vacancies enriched α-Fe 2 O 3 was prepared from thermally treated goethite (α-FeOOH) and employed as a PMS activator. Systematic characterization demonstrated that α-Fe 2 O 3 with most abundant oxygen vacancies could be obtained by heating α-FeOOH at 300 °C. The as-prepared α-Fe 2 O 3 exhibited excellent catalytic activity in activation of PMS for oxidation of sulfamethoxazole (SMX, k = 0.04 min −1 ). The SMX degradation rate was found to be positively correlated with the concentration of oxygen vacancies. Quenching experiments, EPR, LC/MS and XPS analysis revealed that singlet oxygen ( 1 O 2 ) was the predominant reactive oxygen species . The effects of pH, PMS dosage, catalyst loading, temperature, and anions on SMX degradation were comprehensively investigated. Moreover, the plausible degradation pathways of SMX in the α-Fe 2 O 3 /PMS system were proposed. This work not only provides a valuable insight into the mechanism of PMS activation by α-Fe 2 O 3 but also establishes a new strategy for the design of more efficient and practical iron-based catalyst for PMS activation.
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Xin Liu,Meng Xu,Yingying Hao,Jinghua Fu,Fangbao Wang,Binbin Zhang,Stephanie Bennett,Paul Sellin,Wanqi Jie,Yadong Xu
Compared with the widely reported MAPbBr3 single crystals, formamidinium-based (FA-based) hybrid perovskites FAPbBr3 (FPB) with superior chemical and structure stability are expected to be more efficient and perform as more reliable radiation detectors at room temperature. Here, we employ an improved inverse temperature crystallization method to grow FPB bulk single crystals, where issues associated with the retrograde solubility behavior are resolved. A crystal growth phase diagram has been proposed, and accordingly, growth parameters are optimized to avoid the formation of NH4Pb2Br5 secondary phase. The resulting FPB crystals exhibit a high resistivity of 2.8 × 109 Ω·cm and high electron and hole mobility–lifetime products (μτ) of 8.0 × 10–4 and 1.1 × 10–3 cm2·V–1, respectively. Simultaneously, the electron and hole mobilities (μ) are evaluated to be 22.2 and 66.1 cm2·V–1·s–1, respectively, based on the time-of-flight technique. Furthermore, a Au/FPB SC/Au detector is constructed that demonstrates a resolvable gamma peak from 59.5 keV 241Am γ-rays at room temperature for the first time. An energy resolution of 40.1% is obtained at 30 V by collecting the hole signals. These results demonstrate the great potential of FAPbBr3 as a hybrid material for γ-ray spectroscopy and imaging.
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Surfaces and Interfaces
·
2020
·
IF 3.724
Li ML,Huang HW,Mo RB,Sheng XX,Jiang X,Zhang XY
Epoxy resin is widely used in the field of anticorrosive coatings for its outstanding properties. However, environmentally friendly two-component waterborne epoxy coatings often have micropores in its films, making their barrier properties against corrosive media unsatisfactory. α-zirconium phosphate (α-ZrP), known as a kind of flexibly designable two-dimensional nanoparticle , has outstanding mechanical and barrier properties. However, the common problem of incorporating such inorganic fillers into epoxy resins is the poor interface compatibility. In this work, α-ZrP was firstly exfoliated by Tris-(hydroxymethyl)-aminomethane (Tris) aqueous solution, then acidified by diluted hydrochloric acid (HCl) and finally covalently functionalized by 3-aminopropyltriethoxy silane (KH-550). Subsequently, waterborne epoxy composite coatings (KWEPc) with K-ZrP as functional filler were prepared and applied on Q235 carbon steel substrates by blade-coating. With KH-550 modifying, K-ZrP showed an improved dispersion in waterborne epoxy coatings (WEPc). The structure and morphology of prepared K-ZrP was characterized and confirmed by FTIR spectra, XPS and EDS-mapping. The results showed that K-ZrP is evenly modified with amino siloxane. Electrochemical tests revealed that the corrosion rate of KWEPc was one order of magnitude lower than that of WEPc. KH-550 act as a “bridge” among inorganic filler, epoxy resin matrix and Q235 carbon steel substrates.
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MICROCHIMICA ACTA
·
2025
·Vol. 192
·期 6
·1-11
·
IF 5.3
Chen Yun-Ting,Han Jing-Wen,Yu Zi-Wei,Yang Ruo-Yu,Wu Mei-Juan,Huang Pin-Fang,Liu Meng-Meng
A decentralized electrochemical immunosensor was developed using a smartphone and a portable electrochemical workstation. The system employs a gold nanoflower-modified screen-printed carbon electrode (AuNFs/SPCE) for the sensitive measurement of adalimumab (ADL) in human serum via antigen‒antibody recognition. Scanning electron microscopy, X-ray photoelectron spectroscopy, and atomic force microscopy were used to investigate the AuNFs/SPCE. Compared with the bare SPCE, the AuNFs/SPCE has a 1.47-fold larger specific surface area, which enhances the capture efficiency of ADL for signal amplification. Electrode modification and antigen‒antibody assembly processes are characterized by cyclic voltammetry and electrochemical impedance spectroscopy. The immunosensor achieves excellent electrochemical properties by optimizing experimental conditions, which improves the signal-to-noise ratio and thus the analytical performance. Under the best experimental conditions, the immunosensor has a quantitative range of 0.05‒4 μg/mL in diluted human serum with a detection limit of 9.1 ng/mL, which is consistent with the effective therapeutic window of ADL in clinical settings. The prepared electrodes maintain 10-day stability, while with high reproducibility at different ADL concentrations. High recoveries in the range 94.08‒108.6% are obtained in human serum samples. Furthermore, ADL in the serum samples was measured by both ELISA and the developed sensor. Pearson and Bland‒Altman analyses revealed a consistent trend between the two methods. Therefore, this immunosensor is a promising tool for the point-of-care (POC) measurement of ADL in clinical samples, providing valuable insights for personalizing ADL dosing regimens in clinical practice. Graphical
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PubMed
高影响因子
CARBOHYDRATE POLYMERS
·
2018
·
IF 5.158
Shuang Bai,Meili Hou,Xiaoxiao Shi,Jiucun Chen,Xiaoqian Ma,Yong-E Gao,Yajun Wang,Peng Xue,Yuejun Kang,Zhigang Xu
As one of the medical polymers approved by US Food and Drug Administration (FDA), poly(ethylene glycol) has low toxicity, high stability, good biocompatibility, unique physical and chemical properties. Cyclodextrin is an ideal candidate as a drug carrier due to its special structures and characteristics. These two materials were successfully assembled through chemosynthesis in combination with the hydrophilic poly(ethylene glycol) methyl ether methacrylate (OEGMA) chain and hydrophobic polymeric camptothecin (CPT) chain by atom transfer radical polymerization (ATRP). The introduction of disulfide bond of monomer was aimed to realize reduction agent-triggered release of active CPT. The obtained amphipathic prodrug [(Denoted as PC-PCPT- b -POEGMA (PCCO)] could form nano-sized polymeric micelles, which could release more than 85% of the loaded CPT via triggered cleavage of the disulfide linker. The cellular co-localization study revealed the potential pathway of drug internalization. Moreover, the PCCO micelles showed good biocompatibility in vivo after intravenous injection on a mouse model. This new CPT-loaded prodrug system could be prepared with low cost, and showed efficient and controlled drug release and favorable biocompatibility, demonstrating a promising potential as a stimuli-responsive polymeric prodrug for future clinical applications.
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PubMed
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COLLOIDS AND SURFACES B-BIOINTERFACES
·
2025
·
IF 5.6
Shaobing Zhang,Zhi Lian,Xingtao Chen,Ke Duan,Cheng Liang,Xin Duan,Jiyuan Yan,Jianhua Ge
Objective The effective treatment of bone tissue defects is a significant challenge in clinical orthopaedics. This study investigated the preparation and properties of composite bone cements comprising 2-hydroxypropyltrimethyl ammonium chloride chitosan (HACC)-modified α-calcium sulfate hemihydrate (α-CSH)/β-tricalcium phosphate (β-TCP) for potential applications in bone regeneration. Methods α-CSH was synthesised via a hydrothermal method, while β-TCP was prepared through a chemical reaction involving calcium salts and phosphates. HACC was dissolved in deionised water to formulate curing solutions with concentrations ranging from 0 to 4 wt% HACC. The α-CSH and β-TCP powders (7:3 mass ratio) were homogeneously blended with the HACC solution (1:0.3 w/v) to produce HACC/α-CSH/β-TCP composite bone cements. To assess the biocompatibility, osteogenic potential, and antimicrobial activity, extracts of the composite bone cements were used to culture rat bone marrow mesenchymal stem cells. A critical bone defect model in the femoral condyle of male Sprague–Dawley rats was employed to evaluate the in vivo osteogenic repair efficacy. Results The self-curing time met clinical requirements, and the compressive strength approached that of normal human cancellous bone. The in vitro degradation rate was consistent with the rate of new bone formation. Increasing the HACC concentration enhanced the injectability and washout resistance of the composites. The materials exhibited good in vitro biocompatibility; composites containing HACC upregulated osteogenesis-related gene expression and significantly inhibited the growth of Staphylococcus aureus and Escherichia coli . In vivo, the 3 wt% HACC/α-CSH/β-TCP composite showed the best overall performance. Conclusions HACC/α-CSH/β-TCP composite bone cements demonstrate promising clinical potential owing to their improved setting time, mechanical properties, injectability, and cytocompatibility. This material is a strong candidate as a substitute for artificial bone to treat infectious bone defects.
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