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MICROCHEMICAL JOURNAL · 2022 · IF 5.304

Quantitative evaluation of human carboxylesterase 1 by SERS-ELISA using a synergistic enhancement strategy based on gold nanoparticles and metal–organic framework

Hao Lu,Yu Yang,Ruijue Chen,Wenyi Huang,Hao Cheng,Xueping Liu,Hongxing Kong,Lijun Li,Jun Feng

In this study, we synthesized gold nanoparticles (AuNPs) in situ on the surface of two-dimensional Cu-TCPP (meso-tetra(4-carboxyphenyl)porphine) metal– organic framework (MOF) nanosheets to produce AuNP@Cu-TCPP nanocomposites as surface-enhanced Raman scattering (SERS) substrates. The SERS signal was enhanced in two ways: aggregation of the AuNPs@Cu-TCPP near the SERS hotspot through the strong adsorption capacity of the MOF, and the synergistic effect between the charge-transfer enhancement of the Cu-TCPP MOF and the electromagnetic enhancement of plasmonic metal AuNPs. The SERS activity of AuNPs@Cu-TCPP was evaluated by the analysis of multiple model analytes; Rhodamine 6G (R6G) and benzidine were detected with detection limits below 10 –13 and 10 –12 mol·L –1 , respectively. We used AuNP@Cu-TCPP as a SERS substrate combined with an enzyme-linked immuno- sorbent assay (ELISA) to detect the tumor marker carboxylesterase 1 (hCE1) in human serum. The SERS signal of benzidine at 1609 cm −1 is linearly correlated with hCE1 in the concentration range of 0.1–120 ng·mL −1 . Owing to their high sensitivity and excellent SERS sensing capability, AuNPs@Cu-TCPP nanocomposites have potential applicability in the analysis of clinical samples.

✓ 已验证 DOI 高影响因子
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JOURNAL OF THE ENERGY INSTITUTE · 2024 · IF 5.6

Composite xNiFe2O4/(1-x)SrFe12O19 oxygen carriers for chemical looping reforming of bioethanol coupled with water splitting to coproduce syngas and hydrogen

Mingxuan Zhong,Chenxuanzi Wang,Jiajun Xu,Yongcheng Cai,Bo Xiao,Tingting Xu,Xun Wang

Sr–Fe oxides are suitable oxygen carriers (OCs) with excellent cyclic stability. However, the moderate redox activity causes a deficiency in H 2 yield in chemical looping reforming coupled with water splitting (CLR-WS) process. Herein, we designed and prepared the composite xNiFe 2 O 4 /(1-x)SrFe 12 O 19 OCs by ball milling method, which exhibited both high redox activity and high cyclic stability during reactions. A series of characterizations showed that the introduction of NiFe 2 O 4 promoted the oxygen vacancy formation and the release of lattice oxygen, facilitating the reforming of bioethanol in fuel reactor (FR). During CLR-WS process, a high carbon conversion of 79.20 % and a H 2 yield of 13.23 mmol/g OC were achieved by 3Ni7Sr OC at 800 °C, outperforming that of the conventional SrFe 12 O 19 OC. Moreover, the severe carbon deposition and sintering issues inherent to NiFe 2 O 4 were avoided due to the presence of Sr. All Sr-containing composite OCs showed H 2 purity exceeding 99.26 % and excellent cycling stability with no apparent activation of oxygen transport capacity over 3000 min redox reactions.

✓ 已验证 DOI 高影响因子
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JOURNAL OF ORGANIC CHEMISTRY · 2022 · IF 4.198

Synthesis of Isoquinolone, 1,2-Benzothiazine, and Naphtho[1′,2′:4,5]imidazo[1,2-a]pyridine Derivatives via Rhodium(III)-Catalyzed (4 + 2) Annulation

Yueyue Zhu,Rupeng Dai,Chaoqun Huang,Wang Zhou,Xiaoyuan Zhang,Kundi Yang,Hongmei Wen,Wei Li,Jian Liu

In this study, we report a novel and efficient synthetic method to construct isoquinolone scaffold via the Rh(III)-catalyzed (4 + 2) annulation of benzamide with an unreported coupling reagent methyl 2-chloroacrylate. Accordingly, other valuable 1,2-benzothiazine and naphtho[1′,2′:4,5]imidazo[1,2-a]pyridine derivatives are also obtained through a similar synthetic protocol. Thus, our developed method is highlighted by high yield and reaction versatility.

✓ 已验证 DOI 高影响因子
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EUROPEAN POLYMER JOURNAL · 2018 · IF 3.741

CuBr coordinated by the ionic liquid [N4MIM]Cl as a catalyst for biphasic ATRP in 1-allyl-3-methylimidazolium chloride ionic liquid

Teng Xue,Erjun Tang,Xiaofeng Guo,Ruihong Wang,Lei Zhao,Jian Zhou,Shaojie Liu

The ionic liquid 1-(triethylene-tetramine)ethyl-3-methyl chloride ([N 4 MIM]Cl) was first prepared to replace the organic ligand coordinating with CuBr to catalyze atom-transfer radical polymerization (ATRP) in ionic liquid system. [N 4 MIM]Cl was synthesized via the intermediate IL 1-chloroethyl-3-methyl chloride ([CeMIM]Cl) reacting with the aliphatic amine triethylene tetramine (TETA) and [CeMIM]Cl) was obtained by N′-alkylation of N -methylimidazole with 1,2-dichloroethane. This catalyst has been applied to the ATRP of methyl methacrylate (MMA) in the ionic liquid (IL) 1-allyl-3-methylimidazolium chloride ([AMIM]Cl) and presented a perfect catalytic performance. The chemical structures of the ILs obtained were confirmed by FTIR and 1 H   NMR. The coordination ability of [N 4 MIM]Cl was assessed by cyclic voltammetry (CV) and its coordination mechanism towards CuBr was discussed. The [N 4 MIM]Cl/CuBr catalyst system showed good controllability in the aforementioned ATRP reaction in [AMIM]Cl. The amount of residual Cu 2+ in the polymer product was determined by atomic absorption spectrometry (AAS) and the result showed that the Cu catalyst was easily separated from the obtained polymer. Thus, the coordinating IL could overcome the shortcomings of traditional organic ligands, such as poor compatibility with IL media resulting in the weakly catalytic performance and inferior separation of the catalyst from the polymer. It implied that the coordinating ionic liquid ([N 4 MIM]Cl) has highly promising application in the ATRP of ionic liquid system.

✓ 已验证 DOI 高影响因子
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JOURNAL OF CHEMICAL AND ENGINEERING DATA · 2022 · IF 3.119

Liquid–Liquid Equilibrium for the Ternary System Water + 1-Methylimidazole + Ionic Liquid ([Hmim][PF6], [Omim][PF6], or [Omim][BF4]) at 303.15 K

Zhen Jiao,Mengnan Zhang,Lixia Yang,Yuxuan Wang,Jiajie Fu

To evaluate the feasibility of extraction of 1-methylimidazole from its low-concentration aqueous solution by ionic liquids, the liquid–liquid equilibrium of the ternary system of water + 1-methylimidazole + ionic liquid ([Hmim][PF6], [Omim][PF6], or [Omim][BF4]) was determined at 303.15 K and atmospheric pressure. The distribution coefficient and selectivity were calculated in accordance with the experimental results. The effects of the anion and cation of ionic liquids on the separation ability were discussed. The results indicated that the extraction capacity increased with increasing cationic carbon chain length, and the change of anions significantly affected the distribution coefficient and selectivity. As expected, the three ionic liquids were feasible as extractants for separating 1-methylimidazole from water. It also indicated that [Omim][PF6] was a more suitable extractant than [Hmim][PF6] and [Omim][BF4] for the extraction. The highest distribution coefficient and selectivity of [Omim][PF6] could reach 1.71 and 111.92, respectively, indicating [Omim][PF6] as a good choice for extracting 1-methylimidazole from water. In addition, the non-random two-liquid model was employed to successfully correlate the experimental data with a root-mean-square deviation of less than 0.0188. Moreover, a GUI-MATLAB tool was used to verify the consistency of the correlated parameters.

✓ 已验证 DOI 高影响因子
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ACS Applied Materials & Interfaces · 2020 · IF 8.758

Lamellar Lyotropic Liquid Crystal Superior to Micellar Solution for Proton Conduction in an Aqueous Solution of 1-Tetradecyl-3-methylimidazolium Hydrogen Sulfate

Jie Luo,Jie You,Shuai Tan,Caihong Wang,Yong Wu

Humidified perfluorosulfonic acid polymers with a nanoscopic phase-separated morphology are highly proton-conductive materials for fuel cells, yet morphology tuning of the acidic materials for enhanced conduction remains a challenge. Aqueous acidic lyotropic liquid crystals (LLCs) provide a powerful platform to construct well-defined nanostructures for proton conduction. We report an aqueous LLC formed by 1-tetradecyl-3-methylimidazolium hydrogen sulfate, exhibiting a proton conductivity of 210 mS cm–1 at 25 °C, which surpasses that formed by alkylsulfonic acid, thus demonstrating that a mobile acidic anion is more efficient than constrained sulfonic acid functionality to transport protons in LLCs. For an aqueous solution of 1-alkyl-3-methylimidazolium hydrogen sulfate, a lamellar LLC results in higher conductivity than a micellar solution under the same hydration conditions. The peak power density of the fuel cell fabricated from porous membranes filled with the lamellar LLC is four times as high as that filled with the micellar solution. The work offers an efficient way to construct highly proton-conductive LLC materials for fuel cell application.

✓ 已验证 DOI 高影响因子
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DALTON TRANSACTIONS · 2024 ·Vol. 53 ·期 28 ·11713-11719 · IF 3.5

Chemical composition-induced evolution of the structure, domain and electrical properties of Sm-doped (1 − x)Pb(Ni1/3Nb2/3)O3–xPbTiO3

Haoran Yu,Jian Guo,Jiajia Wang,Ji Zhang,Shan-Tao Zhang

As the two typical basic binary solid solutions of the relaxor-PbTiO3 family, Pb(Mg1/3Nb2/3)O3-PbTiO3 (PMN-PT) has been widely investigated, whereas Pb(Ni1/3Nb2/3)O3-PbTiO3 (PNN-PT) has not. Here, 1.5 mol% Sm-doped (1 − x)Pb(Ni1/3Nb2/3)O3–xPbTiO3, (1 − x)PNN–xPT:0.015Sm with x = 0.33–0.39, ceramics have been prepared and the chemical composition-induced evolution of crystal structure, domain, and electrical properties investigated systematically. With increasing PT content, evolution of the rhombohedral–tetragonal structure was observed. A rhombohedral–tetragonal morphotropic phase boundary occurred around x = 0.36–0.37, which showed a peak piezoelectric property with piezoelectric constant d33 = 531 pC N−1 and planar electromechanical coupling factor kp = 0.37 at room temperature. At the same time, the x = 0.36 composition showed improved ferroelectric behavior with remanent polarization Pr = 13.4 μC cm−2 and coercive field Ec = 3.2 kV cm−1. Interestingly, different from its PMN-PT counterpart, there is no temperature-driven phase transition between room temperature and the Curie temperature for (1 − x)PNN–xPT:0.015Sm. These parameters indicated that the PNN-PT system is worthy of more attention and is a promising platform for further development of high-performance piezo/ferroelectric materials.

✓ 已验证 DOI 高影响因子
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CATALYSIS LETTERS · 2019 ·Vol. 150 ·期 3 ·815-825 · IF 2.372

Fe3O4@Cu/C and Fe3O4@CuO Composites Derived from Magnetic Metal–Organic Frameworks Fe3O4@HKUST-1 with Improved Peroxidase-Like Catalytic Activity

Huang Yan-Feng,Zhang Lu,Ma Li,Li Ying,Zhong Chongli

Abstract Fe 3 O 4 @Cu/C and Fe 3 O 4 @CuO composites were achieved using nanoparticle-encapsulated MOFs Fe 3 O 4 @HKUST-1 as both a precursor and a self-sacrificing template. Fe 3 O 4 @HKUST-1 was thermally converted into magnetic Fe 3 O 4 @Cu/C and Fe 3 O 4 @CuO composites in different atmosphere (N 2 and air). The resulting composites not only kept superparamagnetic characteristics, but also exhibited improved peroxidase-like catalytic activity and high stability when compared to the precursor Fe 3 O 4 @HKUST-1. The morphology, crystal structure, magnetic and porous properties of Fe 3 O 4 @Cu/C and Fe 3 O 4 @CuO composites were characterized, and the kinetics parameters and the influence factors on the peroxidase-mimicking activity such as temperature, pH and H 2 O 2 concentration were evaluated. On account of the excellent peroxidase-like activity, the as-prepared Fe 3 O 4 @Cu/C and Fe 3 O 4 @CuO composites were successfully used for the catalytic removal of methylene blue (MB) dye with H 2 O 2 oxidant. This work provides an effective way to fabricate highly reactive MOFs-derived biomimetic catalysts, which have potential applications in bioassays and pollutant degradation. Graphic Abstract Fe 3 O 4 @Cu/C and Fe 3 O 4 @CuO composites were achieved using Fe 3 O 4 nanoparticle-encapsulated HKUST-1 as self-sacrificial templates and demonstrated excellent peroxidase-like activity.

✓ 已验证 DOI 高影响因子
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CHEMOSPHERE · 2021 · IF 7.086

HKUST-1-derived highly ordered Cu nanosheets with enriched edge sites, stepped (211) surfaces and (200) facets for effective electrochemical CO2 reduction

Da Wang,Jinli Xu,Ying Zhu,Lingsha Wen,Jiexu Ye,Yi Shen,Tao Zeng,Xiaohui Lu,Jun Ma,Lizhang Wang,Shuang Song

A novel electrode composed of Cu nanosheets constructed from nanoparticles was synthesized by in situ electrochemical derivation from the metal-organic framework (MOF) HKUST-1. The prepared derivative electrode (HE-Cu) exhibited higher Faradaic efficiency (FE, 56.0%) of electrochemical CO 2 reduction (CO 2 R) compared with that of pristine Cu foil (p-Cu, 32.3%) at an overpotential of −1.03 V vs. a reversible hydrogen electrode (RHE). HE-Cu also exhibited lower onset potential of CO 2 R as well as inhibiting the H 2 evolution reaction. Electrochemical measurements revealed that HE-Cu exhibited higher CO 2 adsorption (1.58-fold) and a larger electrochemical active surface area (1.24-fold) compared with p-Cu. Physicochemical characterization and Tafel analysis showed that stepped Cu (211) surfaces, (200) facets and Cu edge atoms on HE-Cu contributed significantly to the enhanced CO 2 R activity and/or HCOOH and/or C2 product selectivity . The FEs of HCOOH and C2 products for HE-Cu increased 1.57-fold and 10.6-fold at an overpotential of −1.19 V vs. RHE compared with p-Cu. Although CH 4 was produced on p-Cu, its formation was totally suppressed on HE-Cu due to the increase of edge sites and (200) facets. Our study demonstrates that electroreduction of MOFs is a promising method to prepare novel and stable electrochemical catalysts with unique surface structures. The fabricated derivative electrode not only promoted electrochemical CO 2 R activity but also exhibited high C2 product selectivity.

✓ 已验证 DOI 高影响因子
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Catalysts · 2022 ·Vol. 12 ·期 12 ·1625 · IF 4.501

Hydrogenolysis of Lignin and C–O Linkages Containing Lignin-Related Compounds over a Macroporous Silicalite-1 Array-Supported Ru-Ni Phosphide Composite

Bo Chen,Zhi-Ze Cao,Zhi-Jun Diao,Liang-Qiu Huang,Si-Jia Zhao,Hong Yuan,Jia-Meng He

Hydrogenolysis via targeted depolymerization of C–O linkages is a techno-economic beneficial process for converting lignin into highly valuable chemicals and clean fuels. In this work, a macroporous silicalite-1 (S-1) array-supported Ru-Ni metallic phosphide composite (Ru-Ni12P5/S-15) was prepared as a catalyst and hydrogenolysis activity under relative mild conditions was investigated using a series of compounds containing ether linkages as lignin-related model compounds. The Lewis acid sites originating from the unreduced Ru species and the macroporous geometry of S-1 significantly influenced hydrogenolysis activity and product selectivity. Analysis of the mechanism demonstrated that both the aryl ether and aliphatic ether linkages were directly hydrogenated over Ru-Ni12P5/S-15. 2D-HSQC-NMR spectroscopy demonstrated that the ether linkages of lignin were efficiently cleaved by Ru-Ni12P5/S-15. Furthermore, the obtained liquid hydrogenolysis products are high value-added chemicals used for pharmaceutical production and can be facilely tuned via the reaction conditions.

✓ 已验证 DOI 高影响因子
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JOURNAL OF POWER SOURCES · 2021 · IF 9.127

A niobium-substituted sodium superionic conductor with conductivity higher than 5.5 mS cm−1 prepared by solution-assisted solid-state reaction method

Yujian Liu,Limin Liu,Jinsong Peng,Xiaoliang Zhou,Dongshi Liang,Lei Zhao,Jiawen Su,Bo Zhang,Si Li,Naiqing Zhang,Qianli Ma,Frank Tietz

Although research on all-solid-state sodium batteries (ASSSBs) have been conducted for many years, the solid-state electrolyte (SSE) material is still far from practical application at room temperature . One major reason is that no suitable electrolyte material with high ionic conductivity has been found yet. In this study, Nb 5+ is introduced into NASICON-type solid electrolyte, where Nb 5+ substituted Na 3.4 Zr 2 Si 2.4 P 0.6 O 12 (NZSP) is prepared by a solution-assisted solid-state reaction method. The best ionic conductivity is as high as 5.51 mS cm −1 which is a significant improvement. High-frequency electrochemical impedance spectroscopy shows that the increase in total conductivity is mainly due to the decrease of grain boundary impedance as well as bulk impedance. The decrease in grain boundary impedance is probably owing to the increase in density of the electrolyte material after incorporation of the Nb content, which has a beneficial impact of the sintering of NZSP. The decrease in bulk impedance rather results from the ratio of sodium ion concentration and sodium vacancy concentration of 3.3:0.7 in the crystal structure, thus facilitating the sodium ion transport. Symmetric cells with sodium metal as electrodes (Na|Nb 5+ substituted NZSP|Na) are subsequently assembled and cycled stably for 60 cycles at a current density of 0.05 mA/cm 2 .

✓ 已验证 DOI 高影响因子
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INORGANIC CHEMISTRY · 2021 · IF 5.165

Single Co Atoms Implanted into N-Doped Hollow Carbon Nanoshells with Non-Planar Co-N4-1-O2 Sites for Efficient Oxygen Electrochemistry

Shizhu Song,Tian Qin,Qi Li,Yanqing Wang,Yanfeng Tang,Lifang Zhang,Xiaojuan Liu

Facile synthesis of cost-effective carbon-supported Co single atoms (Co-SAs) exhibits huge potential applications in energy storage and conversion devices. We here report the implantation of Co-SAs into hollow carbon spheres (Co-SAs-HCS) via a facile wet-chemistry strategy followed by controlled pyrolysis. Electron-rich histidine acted as a Lewis base effectively immobilizing Co2+ (Lewis acid) via the electrostatic effect and hydrogen bonds, thus achieving the scalable synthesis of Co-SAs-HCS. We constructed a series of histidine-Co2+ structure models to elucidate the formation of histidine-Co2+ complexes by analyzing their binding energy. X-ray absorption fine-structure results verify that central Co atoms with four N coordination atoms possess a non-planar Co-N4 structure. Electrochemical results indicate that the as-prepared Co-SAs-HCS catalyst shows a low potential difference (0.809 V) between the oxygen evolution reaction potential at 10 mA cm–2 and the oxygen reduction reaction half-wave potential, outperforming the commercial Pt/C catalysts (0.996 V). Moreover, an assembled Zn-air battery based on Co-SAs-HCS exhibits an unexpected long-term durability. We have demonstrated that non-planar Co-N4-1-O2 sites are the source for highly efficient adsorption and dissociation of O2 molecules and then reduction of the free energy of desorption of the intermediates by density functional theory. Our findings provide a new design insight into the exploration of advanced electrocatalysts, which will be applied in the design of green energy devices in the future.

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