SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2022
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IF 4.831
Hongding Zhang,Sifei Wu,Mengwei Sun,Jiaoyu Wang,Man Gao,Hai-Bo Wang,Linxia Fang
Glutathione (GSH)-switched fluorescent assays have appealed much attention due to rapid signal changes of fluorescent probes. However, exposure to exterior environment of fluorescent probe causes photobleaching and premature leakage, leading to low sensitivity and poor photostability. Herein, luminescent SiO 2 nanoparticles encapsulated with Ru(bpy) 3 2+ ( [email protected] 2 ) were designed and synthesized as fluorescent probe to construct a GSH-switched fluorescent assay. The encapsulation of Ru(bpy) 3 2+ in the SiO 2 nanoparticles could effectively prevent the leakage of Ru(bpy) 3 2+ molecules, improving the photostability of probe. The fluorescence of [email protected] 2 nanoparticles was quenched by coating MnO 2 nanoparticles on [email protected] 2 surface ( [email protected] 2 @MnO 2 nanocomposites) through an in situ growth approach, which reduced background of the assay. The MnO 2 nanoparticles not only further inhibited the leakage of Ru(bpy) 3 2+ molecules, but also could serve as a recognition unit of GSH. In the presence of GSH, the MnO 2 nanoparticles on the surface of [email protected] 2 nanoparticles were reduced to Mn 2+ , resulting the fluorescence recovery of [email protected] 2 nanoparticles. Thus, a signal-on fluorescent strategy was constructed for GSH detection. The assay displayed good analytical performance for GSH detection with a low detection limit of 16.2 nM due to excellent fluorescence quenching ability of MnO 2 nanoparticles and special role of [email protected] 2 nanoparticles to block probe leakage. The proposed assay was also applied to measure GSH levels in human serum samples. This work paves a new way to detect GSH with high sensitivity.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Yanqin Xue,Yanyan Xu,Qing Yan,Kai Zhu,Ke Ye,Jun Yan,Qian Wang,Dianxue Cao,Guiling Wang
The development of efficient catalysts for hydrogen evolution reaction (HER) from water splitting is one of the most promising strategies to achieve the goal of peak carbon dioxide emissions and carbon neutrality . Herein, Ru nanoclusters decorated MoSe 2 nanosheets supported on a Crepis tectorum fluff biomass-derived hollow carbon tube (Ru-MoSe 2 /CMT) are prepared as the HER catalysts in both alkaline and acidic conditions. The Ru modification induces the transformation of MoSe 2 from 2H phase to 1T phase. Benefiting from the strong water dissociation ability of Ru, Ru-MoSe 2 /CMT exhibits a low overpotential of 70 mV with a Tafel slope of 39 mV dec -1 in 1 M KOH. Furthermore, the assembled Ru-MoSe 2 /CMT || RuO 2 system with a low cell voltage of 1.54 V at 10 mA cm −2 exhibits outstanding overall water splitting performance superior to Pt/C || RuO 2 system. The Ru-MoSe 2 /CMT || RuO 2 system also achieves the excellent stability of up to 30 h in 1 M KOH. The synergy effect between Ru and MoSe 2 , as well as the improved electron transfer kinetics provided by the biomass-derived carbon substrate together contribute to the excellent HER activity of Ru-MoSe 2 /CMT.
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Molecular Catalysis
·
2022
·
IF 5.089
Jian Li,Haiyang Zhang,Haixia Liang,Linfeng Li,Jinli Zhang
Ru/AC catalyst used in acetylene hydrochlorination reaction has several drawbacks such as poor dispersion, metal loss, serious carbon deposition, and insufficient active sites. To address these issues of traditional Ru/AC, in this study, the supported Ru-L x /AC catalysts were synthesized by the coordination of ruthenium precursor and several structural triazine ligands. The complexation of heteroatomic structure to Ru atom formed a local active domain, which is more conducive to the synergistic adsorption and activation of the initial reactants, and further optimizes the reaction microenvironment. The spatial topological structure with conjugated structures effectively promoted the transfer of electrons between the heteroatoms and the ruthenium precursors, facilitating the stabilization of active Ru species. The newly developed synthetic process also increased dispersion of reaction components and impeded the sintering of ruthenium components promoted by the local structural forces. The optimum Ru-1,3,5-triazine/AC (Ru-L 1 /AC) catalyst exhibited 162% higher acetylene conversion than the benchmark Ru/AC catalyst. The significantly improved activity and stability of the optimized catalyst will have a huge application prospect in industry.
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Energies
·
2021
·Vol. 14
·期 24
·8539
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IF 3.004
Lijian Wang,Kang Zhang,Yi Qiu,Huiyun Chen,Jie Wang,Zhihua Wang
The sulfur-iodine (SI) cycle holds great promise as an alternative large-scale process for converting water into hydrogen without CO2emissions. A major issue regarding the long-term stability and activity of the catalysts is their poor sulfur deactivation resistance in the HI feeding process. In this work, the effect of Ru addition for enhancing the activity and sulfur resistance of SiO2-supported Ni catalysts in the HI decomposition reaction has been investigated. The presence of H2SO4molecules in the HI results in severe sulfur deactivation of the Ru-free Ni/SiO2catalysts by blocking the active sites. However, Ni–Ru/SiO2catalysts show higher catalytic activity without sulfur-poisoning by 25% and exhibit more superior catalytic performance than the Ru-free catalyst. The addition of Ru to the Ni/SiO2catalyst promotes the stability and activity of the catalysts. The experimental trends in activity and sulfur tolerance are consistent with the theoretical modeling, with the catalytic activities existing in the order Ni/SiO2< Ni–Ru/SiO2. The effect of Ru on the improvement in sulfur resistance over Ni-based catalysts is attributed to electronic factors, as evidenced by theory modeling analysis and detailed characterizations.Keywords:hydrogen production;SI cycle;HI decomposition;bimetallic catalysts;sulfur-tolerant
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MICROCHEMICAL JOURNAL
·
2023
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IF 4.8
Ziying Zhong,Yun Tang,Yanran Chen,Chunfang Wang,Faqiong Zhao,Baizhao Zeng
The widespread use of tetracycline unavoidably causes residue problems, hence its monitor in foods and environment is important. In this work, a simple but sensitive electrochemiluminescence (ECL) sensor is prepared for tetracycline detection. The sensor is constructed using TiO 2 nanoparticle, ZIF-5 loaded Ru(bpy) 3 2+ (Ru@ZIF-5), and molecularly imprinted poly-o-phenylenediamine. The TiO 2 NP acts as a co-reaction accelerator for tri-n-propylamine (TPrA) by producing electrons and holes at a certain potential to promote the production of TPrA . ZIF-5 has a large specific surface area and rich functional groups, thus can well immobilize a large amount of illuminant Ru(bpy) 3 2+ . The electrodeposited molecularly imprinted polymer acts as a recognition element. Due to the synergic effect of different components, the resulting ECL sensor shows a wide linear range of 10 nM–50 μM, high selectivity, low detection limit, and good stability. It can be used for the detection of tetracycline in food and environmental samples.
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ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Xiaoqing Cao,Jun Zhou,Zhipeng Zhai,Song Li,Guo Yuan,Gaowu Qin
Development of efficient and sustainable monolithic catalysts for NaBH4 hydrolysis remains an important goal for hydrogen cycling. In this work, the structured catalyst Ru/MgO with an on–off feature has been prepared by directly growing a nano-Ru-embedded MgO coating layer on a Mg substrate via an instant high-temperature plasma oxidation process. The porous MgO framework provides an ideal space for the access of reactants and diffusion of mass transport, which facilitates reaction triggering and the expulsion of byproducts to avoid poisoning the catalyst. Importantly, Ru nanoparticles (NPs) are monodisperse with ultrasmall particle size deriving from a concurrent rapid arcing and fast quenching. The hierarchical structured Ru NP catalysts are highly active for hydrolysis of sodium borohydride by achieving a high hydrogen generation rate (HGR) of 101,189 mL min–1 g–1 and exhibit attractive stability. In addition, it is facile to realize the “on–off” functionality based on simple separation that could accurately control the hydrogen generation, suggesting the structured catalyst to be of great potential for practical applications. This simple method opens valuable opportunities for fast synthesis of the high-quality structured catalyst and could be extended to various noble metals on oxides of valve metals with high catalytic performance.
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Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 18
·9049-9057
·
IF 11.301
Qifeng Yang,Peng Jin,Bing Liu,Liang Zhao,Jiahao Cai,Zhan Wei,Shouwei Zuo,Jing Zhang,Lai Feng
Encapsulating metallic nanoparticles (NPs) with a graphitic carbon shell is a promising strategy to achieve highly efficient and stable electrocatalysts for the hydrogen evolution reaction (HER), oxygen evolution reaction (OER) and electrochemical overall water splitting (OWS). This work presents a simple and facile synthesis of graphitic carbon coated NixRuy alloys. The optimized catalyst (e-Ni0.6Ru0.4@C) displays an ultrafine morphology and outstanding HER and OER activities in alkaline media, which are among the best reported so far for various carbon-based electrocatalysts. Remarkably, the e-Ni0.6Ru0.4@C‖e-Ni0.6Ru0.4@C pair needs a low cell voltage of 1.51/1.62 V for driving OWS to reach 10/100 mA cm−2, far outperforming the benchmark electrode pair Pt/C‖RuO2. As expected, this carbon-based catalyst also exhibits superior durability as compared to that of precious catalysts. The experimental evidence combined with density functional theory (DFT) computations thus demonstrates for the first time that minor Ru alloying enables not only the morphological modulation but also the fine electronic modification of the catalyst, which both facilitate the overall electrochemical reactions on the carbon shell surface. Thus, our results may further shed light on how to design and optimize carbon-based electrocatalysts to achieve enhanced catalytic performance for OWS.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
·
IF 3.573
Guangyue Xu,Chuang Li,Tianyu Deng,Chenguang Wang,Ying Zhang,Yao Fu
The conversion of levulinic acid (LA) to γ-valerolactone (GVL) is one of the most important reactions from biomass-derived platform chemicals to value-added chemicals. In this work, bimetallic PdRu/TiO2 catalyst compared to monometallic Ru/TiO2 was designed for the conversion of LA to GVL at ambient H2 pressure. The highly dispersed Pd affected the reaction by two antagonistic effects: (I) increasing the reaction rate by promoting the activation of H2; (II) decreasing the reaction rate by lowering the activation ability of carbonyl group over Ru. The kinetic analysis refined by H2 concentration showed much lower apparent activation energy over 0.2Pd1Ru/TiO2 than that over Ru/TiO2. Finally, the catalysts were evaluated by both GVL productivity and catalyst cost to show increasing benefit of Pd addition at lower H2 pressure. This study offers both theoretical foundation and application instructions for high efficiency conversion of LA to GVL under mild conditions, especially ambient H2 pressure.
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APPLIED CATALYSIS A-GENERAL
·
2021
·
IF 5.706
Jiaorong Yan,Li Wang,Yun Guo,Yanglong Guo,Qiguang Dai,Wangcheng Zhan
Cobalt-doped alumina nanosheets were prepared by dynamic hydrothermal method, and then the precious metal Ru or Pd was loaded and investigated for catalytic combustion of propane. Cobalt doping imparted the prominent redox ability to irreducible alumina nanosheets with superior thermal stability and established the strong metal-support interaction and easy activation of gaseous oxygen. Comparative investigation between Ru and Pd supported on Co-doped Al 2 O 3 nanosheets suggested that Ru based catalysts presented a higher activity and water-resistance while the preferable sintering-resistance and oxygen-tolerance were observed on Pd based catalysts. Unexpectedly, the Pd/CoANS-800 catalysts exhibited a re-dispersion of PdO x at high temperature and re-activation for propane oxidation . Ru based catalysts were more tolerant to Cl species from the metal precursor, and the presence of H 2 O could accelerate the removal of the residual Cl species from the catalyst surface especially Pd based catalysts, which led to the promotion of catalytic activity.
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CELLULOSE
·
2019
·Vol. 27
·期 2
·799-823
·
IF 3.917
Lv Wei,Liao Yuhe,Zhu Yuting,Liu Jing,Zhu Changhui,Wang Chenguang,Xu Ying,Zhang Qi,Chen Guanyi,Ma Longlong
The cleavage of linkages of lignocellulose is important for its valorization. The linkage cleavage of cornstalk hydrolysis residue was investigated over catalysts (Ru/C + MgCl 2 ) in EtOAc/H 2 O solvents. The results show that almost hydrogen bonds, C–C bonds, ether and ester bonds in the matrix of lignin and cellulose were broken, accompanying 80.6% of lignin and 98.5% of cellulose conversion, and obtaining 37.5% of aromatic monomers and 28.8% of lignin oligomers. In the reaction system, biphasic EtOAc/H 2 O solvents exhibited an effect on cleaving the intermolecular linkages between lignin and cellulose. MgCl 2 showed limited abilities of breaking the α-O-4 and β-O-4 linkages in lignin and limited β-1, 4-glycosidic and hydrogen bonds in cellulose were cleaved over Ru/C catalyst. The cleavage of C–O linkages (α-O-4, β-O-4, 4-O-5) and C–C bonds (α-β, β-5) in lignin were mainly dependent on Ru/C catalyst. Much C–O and the stubborn C–C linkages of β-5, β-1 and 5-5 were significantly disrupted by the synergistic effect between MgCl 2 and Ru/C. However, MgCl 2 exhibited great contribution to breakage of β-1, 4-glycosidic linkage, hydrogen bonds and sugar ring of cellulose. The linkage of β-1, 4-glycosidic, hydrogen bonds and C–C in C5/C6 sugars were significantly broken. The increased yield of products was evidently due to the synergistic effect of Ru/C combined with MgCl 2 .
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APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Qi Zhang,Liangyun Yu,Chenchen Xu,Jinyong Zhao,Haiyang Pan,Ming Chen,Qi Xu,Guowang Diao
Herein, a kind of Fe 3 O 4 @C@Ru hybrid nanocomposites was successfully synthesized by a three-step process. The as-prepared products were characterized by X-ray powder diffraction, transmission electron microscopy , high-resolution transmission electron microscopy , energy dispersive spectroscopy , X-ray photoelectron spectroscopy, UV–visible diffuse reflectance spectrometry and photoluminescence emission spectrometry . The Ru nanoparticles loaded on the surface of carbon shell on Fe 3 O 4 @C nanospheres were nearly spherical with an average diameter of less than 5 nm. The photodegradation of methylene blue (MB) was carried out under the irradiation of simulated visible light to investigate the catalytic activity of the introduced nanomaterial . The results showed that the catalytic activity of Fe 3 O 4 @C@Ru nanocomposites in the MB photodegradation was higher than that of Fe 3 O 4 nanospheres or of Fe 3 O 4 @C nanospheres, as they could degrade 92.70% of the dye in 140 min of simulated sunlight irradiation without any other oxidant or reductant. The photodegradation reaction was first-order with the rate constant of 0.0176 min −1 at room temperature . The degradation rate of Fe 3 O 4 @C@Ru nanocomposites decreased very slightly after five cycles. Furthermore, they could be easily separated and recycled by using an external magnet. It indicated that the magnetically recoverable Fe 3 O 4 @C@Ru nanocomposites had a very broad application prospect in the field of environmental protection.
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MICROCHIMICA ACTA
·
2019
·Vol. 186
·期 8
·1-10
·
IF 5.479
Hu Yunxia,Su Luyao,Wang Sui,Guo Zhiyong,Hu Yufang,Xie Hongzhen
A method is described for combined magnetic solid phase microextraction and electrochemiluminescent (ECL) detection of the antibiotic tetracycline. A nanocomposite of type Fe 3 O 4 @SiO 2 @ZnO was used as the sorbent. Tetracycline has a strong affinity for Zn(II) ion and therefore is well extracted by this sorbent. The loaded sorbent can be magnetically removed. The extraction efficiency at a 1.0 μM tetracycline concentration is around 88%. Detection is based on the use of carbon nanodots that were prepared form urea and ethylenediaminetetraacetic acid as raw materials. The electrochemical probe Ru(bpy) 3 2+ was added to generate double ECL when scanning the potential between −3.5 and + 2 V. The two ECL signals decreased with the increase of tetracycline concentration. Under optimized experimental conditions, the ratio of the two signals is linearly related to the logarithm of the tetracycline concentration in the range from 1.0 nM to 0.1 mM, with a 0.47 nM detection limit. The method was successfully applied to the determination of tetracycline in spiked milk. It exhibited good sensitivity, selectivity and accuracy due to ratiometric read-out and prior preconcentration of analyte.
Tetracycline (TC) has a strong affinity for Zn(II) ion and is well extracted by the Fe 3 O 4 @SiO 2 @ZnO nanocomposite. Ru(bpy) 3 2+ can generate double electrochemiluminescence signals based on the use of carbon nanodots (C-dots) as coreactant. The two signals decrease with the increase of tetracycline concentration. [Ru(bpy) 3 2+ ]* stands for excited state Ru(bpy) 2 2+ .
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