ACTA PHYSICO-CHIMICA SINICA
·
2023
·
IF 10.9
Ye Wang,Ruixiang Ge,Xiang Liu,Jing Li,Haohong Duan
Nucleophile oxidation reaction (NOR) is emerging as a significant approach for the sustainable production of value-added chemicals. Among the various types, electrocatalytic glycerol oxidation reaction (GOR) stands out as a crucial method for producing C 1 to C 3 chemicals including formic acid (FA). Nonnoble-metal-based (oxy)hydroxides have found extensive use in GOR, yet achieving industrially-demanded current densities (> 300 mA·cm −2 ) at moderate potentials remains a challenge. It is well documented that GOR catalyzed by (oxy)hydroxides follows an indirect oxidation mechanism. Specifically, the nucleophile, glycerol, undergoes oxidation by the electrogenerated oxyhydroxides with electrophilic adsorption oxygen. Therefore, comprehending the evolution of the electrocatalyst in GOR is critically important. In this paper, we have developed molybdenum-doped nickel oxyhydroxides (Mo-NiOOH) through cyclic voltammetry (CV) activation of nickel molybdate (NiMoO 4 ). We demonstrated that Mo species leach from NiMoO 4 , and the resulting Mo-NiOOH retains the nanosheet array morphology of NiMoO 4 . We subjected the freshly prepared Mo-NiOOH to systematic characterizations employing techniques such as scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDS) mapping, Raman spectroscopy, inductively coupled plasma-mass spectrometry (ICP-MS), and X-ray photoelectron spectroscopy (XPS). The above structural characterizations confirm that Mo-NiOOH inherits the nanosheet array morphology of the NiMoO 4 precursor with reduced Mo content, thereby indicating the phase reconstruction from oxides to oxyhydroxides post CV activation. Furthermore, the Ni 3+ /Ni 2+ ratio in Mo-NiOOH surpasses that in NiOOH derived from CV activation of Ni(OH) 2 . Mo-NiOOH exhibits elevated electrochemically active surface areas (ECSAs) and a higher Ni 3+ /Ni 2+ ratio compared to NiOOH obtained through CV activation of Ni(OH) 2 , facilitating the Mo-NiOOH exhibits higher ratio of Ni 3+ /Ni 2+ , higher electrochemically active surface areas (ECSAs) than NiOOH, and facilitated oxidation of Ni 2+ to Ni 3+ . Consequently, Mo-NiOOH requires a lower applied potential than NiOOH (1.51 V versus 1.84 V vs . reversible hydrogen electrode (RHE)) to achieve a high current density (400 mA·cm −2 ). Additionally, Mo-NiOOH demonstrates higher Faradaic efficiency towards formate (FE formate ) in contrast to NiOOH (84.7% versus 59.6%), indicating enhanced carbon-carbon (C—C) bond cleavage due to Mo doping. Multi-potential step (STEP) experiments indicate that GOR catalyzed by NiOOH and Mo-NiOOH follows a similar indirect oxidation mechanism mediated by oxyhydroxides. Operando electrochemical impedance spectroscopy (EIS) and in situ Raman spectroscopy confirmed that Mo doping in NiOOH accelerates GOR kinetics and the oxidation of Ni 2+ to Ni 3+ , contributing to the higher activity and formate selectivity of Mo-NiOOH than NiOOH. The strategy of surface modulation of oxyhydroxides through leaching of soluble anions offers guidelines for the rational design of high-performance NOR electrocatalysts. Download: Download high-res image (72KB) Download: Download full-size image
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高影响因子
JOURNAL OF CULTURAL HERITAGE
·
2024
·
IF 3.5
Jose A. Madrid García,Effat Yahaghi,Amir Movafeghi,Mahdi Mirzapour
Preserving soft plastic or elastomeric material toys in museums and detecting their defects have become increasingly important. Accurate information regarding cracks and fissures in these toys is essential for preservation and restoration processes. Visual inspection is typically the first step in identifying damage, and various tests such as FTIR and NIR are commonly used to assess the condition of toys with a soft or flexible texture. However, these methods do not provide the location and size of the defects. Radiographic Testing (RT) is a valuable non-destructive method that can reveal the size and location of defects and fissures in toys crafted from an elastomeric material for conservation planning. However, X-ray radiographs often appear foggy due to the low atomic number of elastomeric material and the thinness of these toys. To address this issue, a cartoon texture image processing method based on a Gaussian filter was applied to digital radiographs to enhance the imaging contrast of the original radiographs. The results demonstrate that this method effectively identifies toys' defects, fissures, and internal structures. The contrast in the reconstructed image increased threefold compared to the original radiographs, according to the line profile method in the Duplex Image Quality Indicator (DIQI) region. Additionally, the size of cracks can be estimated by comparing them with the intervals of lines in the DIQI.
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高影响因子
FOOD CHEMISTRY
·
2016
·
IF 4.052
Jinhu Tian,Shiguo Chen,Chunhua Wu,Jingqiu Chen,Xinyi Du,Jianchu Chen,Donghong Liu,Xingqian Ye
The effects of preparation method (boiled, cooled, and reheated) on the structural characteristics and in vitro digestibility of potato were investigated. The highest equilibrium starch hydrolysis was obtained after boiling (82.21%), followed by reheating (66.98%) and cooling (54.31%). The potato after cooling treatment exhibited a narrower melting temperature range and a higher melting enthalpy compared with the potatoes after boiling and the microwave reheating. X-ray diffraction patterns revealed that the relative crystallinity of the cooled potato was higher than those of the reheated and boiled potatoes, consistent with the results in melting enthalpy. Moreover, compared with the boiled potato, a large number of wrinkles were observed on the surface of the cooled potato, whereas after microwave reheating, larger clearances of starch granule regions were found. This study demonstrated that cooling and microwave reheating significantly affected the potato’s microstructure and digestibility and were suggested as alternative choices to prepare potato dishes.
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高影响因子
Systems Microbiology and Biomanufacturing
·
2023
·
IF 0
Sun Tingting,Liu Di,Zhang Linmeng,Fan Taiping,Cai Yujie
(2R,3R)-BDO is an important bio-based four-carbon platform compound and widely used in chemical, food, pharmaceutical, fuel and aerospace fields . Serratia marcescens has been shown to be an effective strain for producing BDO. However, there have been few reports on the metabolic engineering of this strain to efficiently produce (2R,3R)-BDO using xylose. In this study, the endogenous strong promoter was screened and modified, and combined with the screened RBS. (2R,3R)-BDO was successfully produced by combining the selected promoters and RBS with the overexpressed key enzymes (ALS, ALSD, BDH, GLF) of (2R,3R)-BDO production. The optimum fermentation temperature and pH were 37 ℃ and 6.0, respectively, and the optimized yield reached 6.0 g/L. After batch fermentation, the (2R,3R)-BDO yield reached 36.6 g/L. This provided a good idea for efficient production of (2R,3R)-BDO from xylose.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2019
·
IF 5.107
Muntadher M. Alwan Almijbilee,Xitian Wu,Ayang Zhou,Xiaokuo Zheng,Xingzhong Cao,Wei Li
An interfacial assembly and polymerization procedure was adopted to synthesized organic solvent polyetheramide thin film composite (TFC) nanofiltration membrane using 4,4′-oxydianiline (ODA) and trimesoyl chloride (TMC) monomers upon the ethylenediamine-crosslinked polyetherimide (C-PEI) membrane substrate. DFT calculations indicate that the unreacted amine terminals located on the C-PEI membrane surface can form intermolecular hydrogen bonding with the ether group of ODA molecule meanwhile π-π stacking interaction could be formed among the aromatic rings of ODA and the aromatic section in the backbone of C-PEI. The separation efficiency of the synthesized polyetheramide TFC membranes was assessed with some organic solvents and characterized through ATR-FTIR, 13 C NMR, XPS, SEM, DBES, etc. S parameters of DBES measurement indicate that the organic solvent activation indeed influences the arrangement of the polymer chain in the synthesized membrane layers, and consequently makes the diffusion faster through the top layer of the membrane. Through activating the TFC membrane by THF solvent, the optimum TFC membrane showed a rejection of 96.3% toward Crystal Violet (CV) (Mw 407.98 g mol −1 ) with a THF permeance around 4.5 L m −2 h −1 bar −1 .
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高影响因子
ACS ES&T Water
·
2024
·
IF 4.8
Zhennan Zhou,Haibo Li,Yikang Lin,Jiali Fan,Hua Tong,Jing Yang,Wei Liu,Gangfeng Ouyang
It is necessary and urgent to develop new materials that are sensitive to antibiotics and can detect them in wastewater. Here, we report a zwitterionic copper(I)-iodide hybrid cluster with strong luminescence and excellent stability. We demonstrate for the first time that this compound can be an efficient optical sensor for tetracyclines, a widely used type of antibiotic, in an aqueous system, with the limit of detection reaching as low as 521–851 ppb. Further, possible electron and energy transfer mechanisms are discussed. This study has opened up new applications for this type of material in the field of chemical sensing.
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JOURNAL OF POLYMER SCIENCE PART A-POLYMER CHEMISTRY
·
2018
·Vol. 56
·期 21
·2437-2444
·
IF 2.588
Lei Yu,Yanlong Wei,Yuanyuan Tu,Shudong Lin,Zhenzhu Huang,Jiwen Hu,Yue Chen,Hang Qiao,Wei Zou
We report herein a visible light-induced metal-free living polymerization with high oxygen tolerance that can be performed in aqueous media. In contrast with ordinary living/controlled radical polymerizations, oxygen can be present throughout the entire reaction process. This reaction can be photo-induced and proceeds at room temperature. First, we have successfully synthesized a well-defined polymer in an ambient atmosphere by the photo-induced radical polymerization method, using acrylic acid as a monomer and fluorescein as a photocatalyst. However, the subsequent chain extension reaction did not occur, possibly due to oxidation of the chain transfer agent (CTA). Despite this, we found that the addition of vitamin C (ascorbic acid) imparted the process with oxygen tolerance. We conducted a systematic study to optimize the best concentrations of the key reagents including the monomer, CTA, fluorescein, and vitamin C. Through these optimizations we were able to synthesize in the presence of oxygen a series of well-defined poly(acrylic acid)s (PAAs) with dispersities ( Ð ) below 1.3 and molecular weights that closely matched the theoretical values. The kinetic study showed that the molecular weight of the produced PAA increased linearly with the conversion of the monomer, and chain extension reaction also yielded a block polymer with a higher molecular weight than that of the previous polymer. Therefore, we developed a novel photo-induced living polymerization method that can be conducted both in the absence of oxygen and in the presence of air. © 2018 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2018 , 56 , 2437–2444
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高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Ziyi Cai,Jiafu Shi,Weiran Li,Yizhou Wu,Yishan Zhang,Shaohua Zhang,Zhongyi Jiang
Enclosed films, also called capsules, bearing an ultrathin and robust nanoshell have sparked much interest for use in many applications, for which facile preparation methods are urgently pursued. Inspired by the pH-programmed adhesion/cohesion of mussel-secreted foot proteins, polyphenol/polyamine capsules with an ultrathin and robust nanoshell are fabricated through a pH-switched assembly on sacrificial calcium carbonate (CaCO3) templates. Polyphenols adhere to the templates at pH 6.0 and rapidly cohere with polyamines at pH 8.0. The pH-switched assembly process is accomplished in only a few minutes where multiple instances of electrostatic interactions and chemical conjugation between polyphenols and polyamines occur. As a result, the capsules exhibit a nanoshell thickness of ∼10 nm and a superior mechanical strength of ∼1.575 GPa (elasticity modulus). Cell mimics are prepared through encasing enzymes in the lumen and present an activity recovery of ∼70% along with little activity decline during reuse. Amine or phenolic groups on the nanoshell of capsules are then applied to induce the generation of titania or silver nanoparticles, which may expand the applications of the capsules to the photo- and biorelated realms. Our study not only deepens the understanding of the adhering process of mussels but also offers a generic method toward functional materials for diverse applications.
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高影响因子
SEMICONDUCTOR SCIENCE AND TECHNOLOGY
·
2021
·Vol. 36
·期 12
·125022
·
IF 2.352
Yuchang Liu,Hongjie Liu,Anjie Hu,Yingmei Wei,Wenchao Ou,Xianwang Deng,Shaopeng Wang,Kefu Yu
The quest to develop inexpensive chemical sensing materials that are energy-efficient, portable, and with efficient performance lies at the center of next-generation sensor development. Owing to their low cost, easy preparation, high response, and smooth integration with electronic circuits, metal oxide semiconductors have received particular attention. Yet, metal oxide semiconductor based sensors often suffer from high power consumption due to their high operating temperature, which hinders them from practical applications. To solve this problem, herein, we proposed ultrathin sub-4 nm SnO2 films synthesized by a facile tunable hydrothermal method. Benefiting immensely from its two-dimensional anisotropic nature, the proposed SnO2 ultra-thin film exhibits a large specific area of 94.41 m2 g−1 and possesses surface oxygen vacancies. The obtained sample was practically applied as a gas sensor; the results indicate that the ultra-thin SnO2 film based sensor exhibits the highest sensitivity to triethylamine (19.2 at 100 ppm), outstanding repeatability, and excellent sensing selectivity at a low working temperature of 150 °C.
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ELECTROANALYSIS
·
2016
·Vol. 28
·期 9
·2070-2074
·
IF 2.471
Lili Bie,Xue Luo,Luqi Kang,Daiping He,Ping Jiang
Commercially available copper foam (CF) was used as a 3D porous electrochemical sensing platform for nonenzymatic glucose detection. CF shows high electrocatalytic activity towards glucose oxidation and can be used directly for glucose electrochemical sensing without any pretreatment. The sensor exhibits high performance towards glucose in 0.1 M NaOH solution with the linear range from 1 μM to 0.5 mM, the sensitivity of 5.85 mA mM −1 cm −2 and the detection limit of 0.5 μM (S/N=3) simultaneously. Furthermore, the sensor shows a high selectivity for glucose against the common interferences and good reliability for glucose detection in human serum samples.
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高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-10
·
IF 14.7
Lv Jiabao,Cao Ang,Zhong Yunhao,Lin Qingyang,Li Xiaodong,Wu Hao Bin,Yan Jianhua,Wu Angjian
Renewable-driven electrocatalytic nitrate conversion offers a promising alternative to alleviate nitrate pollution and simultaneously harvest green ammonia. However, due to the complex proton-electron transfer processes, the reaction mechanism remains elusive, thereby limiting energy efficiency. Here, we adopt Ni(OH)₂ as a model catalyst to investigate the dynamic evolution of the reaction interface. A proposed OH cycle mechanism involves the formation of a locally OH-enriched microenvironment to promote the hydrogenation process, which is identified through in-situ spectroscopy and isotopic labelling. By further activating the dynamic state through the implementation of surface vacancies via plasma, we achieve a high Faradaic efficiency of almost 100%. The activated interface accelerates the OH cycle by enhancing dehydroxylation, water dissociation, and OH adsorption, thereby promoting nitrate electroreduction and inhibiting hydrogen evolution. We anticipate that rational activation of the dynamic interfacial state can facilitate electrocatalytic interface activity and improve reaction efficiency.
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高影响因子
ELECTROCHIMICA ACTA
·
2019
·
IF 5.383
Li Wang,Xingwei Li,Gengchao Wang
An electrochemical stable conductive network is built to improve the pseudocapacitance of polyaniline . As a proof-of-concept demonstration, p olyaniline/ITO composite is synthesized by in-situ oxidation polymerization of aniline in the dispersed system of ITO nanoparticles . The electrical conductivity of the optimal polyaniline/ ITO composite is 14.42 S cm −1 , while that of contrast polyaniline is 1.88 S cm −1 . P olyaniline/ ITO coated on the oxidized carbon cloth (polyaniline/ITO@oxidized carbon cloth) displays a specific capacitance of 1505.7 mF cm −2 at a current density of 0.5 mA cm −2 , and the capacitance retention reaches 75% with a growth of the current density from 0.5 to 5 mA cm −2 , while those of polyaniline@oxidized carbon cloth are 847.9 mF cm −2 and 68.3% . It is noteworthy that the capacitance retention of polyaniline/ITO@oxidized carbon cloth symmetrical capacitor is high up to 90.1% after 2000 cycles at a current density of 1 mA cm −2 . Moreover, a high energy density of 31.18 μWh cm −2 is also attained at a power density of 0.35 mW cm −2 .
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高影响因子
危险品化学品经营许可证（带存储）