RENEWABLE ENERGY
·
2025
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IF 9.1
Yongyuan Deng,Yichao Ye,Tao Yin,Zhipeng Tian,Chao Wang,Ying Chen,Zhi Yang,Junling Tu,Riyang Shu
Hydrodeoxygenation (HDO) is a common refinery process to convert oxygen-containing lignin pyrolysis oil into high-quality hydrocarbon liquid fuels. In this work, we prepared a core-shell Ru@SiO 2 -Al 2 O 3 catalyst and employed it in the HDO of phenolic compounds and lignin pyrolysis oil. The unique core-shell structure of the catalyst reduces the size of Ru metal particles, which significantly improves the hydrogenation catalytic activity. The high surface area, large pore size, and large pore volume of the SiO 2 shell provide a favorable environment for the substrate transfer during the reactions, meanwhile the doped Al 2 O 3 introduces a substantial number of acid sites for the catalysis of deoxygenation. The synergistic effect between the metal sites and acid sites greatly promotes the HDO reaction efficiency. Under mild conditions of 220 °C and 1 MPa H 2 , Ru@SiO 2 -Al 2 O 3 catalyst achieved a guaiacol conversion of 99.9% and a cyclohexane selectivity of 99.9%. This catalyst also demonstrates an outstanding stability, with catalytic activity little loss after 6 recycles. Furthermore, an efficient HDO performance was obtained in the upgrade of other phenolic compounds and lignin pyrolysis oil. At the temperature of 240 °C, the content of hydrocarbons in lignin pyrolysis oil increased from 15.4% to 92.7%. These results indicate that Ru@SiO 2 -Al 2 O 3 holds significant potential for the efficient HDO refinery, providing a promising avenue for the future biofuel development.
研究领域:
化学工程
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可再生能源
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产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2022
·Vol. 152
·期 10
·3046-3057
·
IF 2.936
Yu Pei,Jiang Junxiang,Chen Can,Wang Zhong,Wang Da,Li Guangci,Li Xuebing
Catalytic selective hydrogenation of esterified malic acid to produce 1,2,4-butanetriol (1,2,4-BT) using H 2 as the reducing reagent suffers from the low 1,2,4-BT selectivity. Here, Ru/SiO 2 catalyst was employed for selective hydrogenation of dimethyl malate (DM) to produce 1,2,4-BT, which gave abnormal high DM conversion (100%) and 1,2,4-BT selectivity (92.4%) in aqueous solvent at 363 K, especially, the 1,2,4-BT yield even is higher than the optimal catalyst reported (Ru-Re, 79.8%). The reaction pathways for the DM hydrogenation on Ru/SiO 2 were also proposed, suggesting that extremely high 1,2,4-BT selectivity require for the much high hydrogenation rates at low temperatures, where side-reaction transesterification rates are relatively low. The extremely high hydrogenation activity and 1,2,4-BT selectivity on Ru/SiO 2 in aqueous solvent at low temperatures arise from that H 2 O may coordinate to Ru 2+ and prevent the reduction of Ru 2+ to Ru under high H 2 pressure. Ru/SiO 2 surface presents abundant Ru 2+ in aqueous solvent, can activate H 2 through heterolytic cleavage mode to form hydride, which can significantly increase hydrogenation rates of C = O groups at low temperatures. In addition, the activity and 1,2,4-BT selectivity on Ru/SiO 2 catalyst only reduced by 2.3% and 2.6%, respectively over a period of 550 h. Graphical Abstract
研究领域:
催化
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化学工程
·
有机化学
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产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Jingyi Yang,Yongzhen Gao,Jie Fan,Jieqiong Wang,Tao Yang,Zezheng Bing,Meng Zhang,Zhongyi Liu
Tuning the metal-support interaction (MSI) between highly dispersed nanosized metal particles and the support plays a pivotal role in the activity and selectivity of polyaromatics selective hydrogenation. In this work, the supported bimetallic Ni-Ru/SiO 2 -SEA catalyst was prepared by a strong electrostatic adsorption (SEA) strategy, and applied for the selective hydrogenation of biphenyl (BP) to cyclohexylbenzene (CHB). Compared to the catalysts prepared by the conventional incipient wetness impregnation method and Ni/SiO 2 -SEA, the significant effects of MSI and hydrogen spillover on Ni-Ru/SiO 2 -SEA facilitated the highly exposed and uniformly dispersed electron-deficient Ni δ+ (0 < δ < 2) species, which could enhance adsorption and activation of the electron-withdrawing phenyl group and H 2 , thereby promoting the efficient and selective conversion of BP to CHB. At the conditions of 160 ℃ and 2 MPa H 2 pressure, BP conversion over Ni-Ru/SiO 2 -SEA reached nearly 100 % within 3 h, achieving a remarkable selectivity of 97.9 % towards CHB, along with a high turnover frequency of 2756.9 h −1 for the active metallic Ni sites. Importantly, according to the kinetic simulations, the hydrogenation rate constant of Ni-Ru/SiO 2 -SEA was the highest (2.76 × 10 -2 mol·g −1 ·h −1 ) among the employed catalysts. Moreover, after six consecutive cycles, no obvious decline in hydrogenation efficiency was observed, confirming the remarkable activity and stability of Ni-Ru/SiO 2 -SEA. Furthermore, the activation of BP and desorption of CHB pathway on the Ni δ+ species were elaborated through temperature-programmed desorption characterization, highlighting the prominent contribution of MSI in enhancing the selective hydrogenation of polyaromatics.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
ANALYTICA CHIMICA ACTA
·
2023
·
IF 6.2
Jun Yao
Background The residues of kanamycin can accumulate in the human body for a long time and pose serious health risks, including hearing loss , kidney poisoning, and drug allergic reactions. Therefore, it is crucial to develop a rapid, highly sensitive, and low-cost method for detecting kanamycin residues in foods. However, the current methods have limitations such as low sensitivity, expensive instruments, and multiple steps, which make them impractical for use in resource-limited environments and emergencies. In this study, the creation of a multiple-signal amplification photoelectrochemical biosensor to address these aforementioned issues is discussed. Results Herein, we proposed a multiple signal amplification photoelectrochemical (PEC) biosensor based on carboxylated g-C 3 N 4 and avidin functionalized Ru@SiO 2 for the ultrasensitive detection of kanamycin. The carboxylated g-C 3 N 4 was a highly efficient photoactive substance for amplifying photoelectric signals and a substrate for aptamer immobilization. The DOS and PDOS of g-C 3 N 4 were studied by simulation, and the sensing mechanism of the probe at the molecular level was revealed. Meanwhile, using Ru@SiO 2 as a signal amplifying unit, through the cooperative work between Ru@SiO 2 and g-C 3 N 4 , the photoelectric signal could be double amplified to produce an excellent photocurrent response. Under optimized conditions, the photocurrent response of the PEC biosensor to kanamycin was obtained at concentrations from 0.1 nM to 1000 nM with a lower detection limit of 4.1052 × 10 −11 mol L −1 . This protocol demonstrates high sensitivity, brilliant specific recognition ability, excellent reproducibility, and acceptable stability. Significance The first combination of g-C 3 N 4 and avidin-Ru@SiO 2 as photocurrent materials greatly enhanced the sensitivity of the PEC biosensors. Moreover, the specificity and sensitivity of the PEC biosensor were further improved through the specific interaction between kanamycin and aptamer. The photoelectric conversion mechanism based on g-C 3 N 4 and two pathways for enhancing the photocurrent by Ru(byp) 3 2+ were proposed. Through simulations of the DOS and PDOS of g-C 3 N 4 , the sensing mechanism of the probe at the molecular level was revealed. Under the optimum conditions, the PEC biosensor exhibited a wide linear concentration range and a low detection limit.
研究领域:
食品安全检测
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分析化学
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生物医学工程
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产品关联
DOI
PubMed
高影响因子
ANALYTICAL CHEMISTRY
·
2021
·
IF 6.986
Chen Xu,Jing Li,Shimeles Addisu Kitte,Guohua Qi,Haijuan Li,Yongdong Jin
Electrochemiluminescence (ECL) by virtue of its controllability and versatility has emerged as a significant tool in bioassay, but how to integrate it with other (nano)materials and further break the limit of sensitivity for ultrasensitive detection still possess tremendous potential. Herein, a close-packed Ru@SiO2 NP nanomembrane that serves as an enhanced substrate and luminophore enricher simultaneously was constructed by the liquid–liquid interface self-assembly method and applied for ECL-enhanced bioassay. The developed ECL electrode obtained ∼600-fold enhancement on ECL intensity compared with the bare ITO electrode and ∼21-fold enhancement compared with the SiO2 NP nanomembrane electrode due to the dramatic light scattering of the 2D SiO2 NPs and the enrichment of Ru(bpy)32+ molecules on the surface of the Ru@SiO2 NP nanomembrane electrode. Based on the fascinating Ru@SiO2 NP nanomembrane platform, we further constructed a label-free immunosensor for the detection of prostate-specific antigen (PSA). The as-fabricated Ru@SiO2-nanomembrane ECL immunosensor exhibited good stability and performed ultrasensitive detection with an utmost low detection limit of 0.169 fg·mL–1 (signal/noise = 3). Our work puts forward an effective solution benefiting for further improving ECL performance for ultrasensitive bioassays.
研究领域:
生物医学工程
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分析化学
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纳米材料科学
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
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IF 9.229
Xunxun Deng,Xiaobo Liu,Shuo Wu,Shiyu Zang,Xiaotong Lin,Yanqiu Zhao,Chunying Duan
Accurate and sensitive fluorescence imaging of intracellular miRNA is essential for understanding the mechanism underlying some physiological and pathological events, as well as the prevention and diagnosis of diseases. Herein, a highly sensitive ratiometric fluorescent nanoprobe for intracellular miRNA imaging was fabricated by integrating a Ru-SiO2@polydopamine (Ru-SiO2@PDA) nanoplatform with a near-infrared light (NIR)-assisted DNA strand displacement signal amplification strategy. The Ru-SiO2@PDA spheres have excellent biosafety, high photothermal effect, and unique photophysical properties that can both emit a stable red fluorescence and well quench the fluorophores getting closer to them. So, when the fuel DNA and carboxyfluorescein (FAM)-labeled signal DNA are co-assembled on their outer surfaces, the FAM’s green fluorescence is quenched, and a low ratiometric signal is obtained. However, in the presence of miRNA, the target displaces the signal DNA from the capture DNA, releasing the signal DNA far away from the Ru-SiO2@PDA. Then, the green fluorescence recovers and leads to an enhanced Igreen/Ired value. Under NIR light irradiation, the Ru-SiO2@PDA increases the local temperature around the probe and triggers the release of fuel DNA, which thus recycles the target miRNA and effectively amplifies the ratiometric signal. Using A549 cells as a model, the nanoprobe realizes the highly sensitive ratiometric fluorescence imaging of miRNA let-7a, as well as its in vivo up- and down-regulation expressions. It provides a facile tool for highly sensitive and accurate intracellular miRNA detection through one-step incubation and may pave a new avenue for single-cell analysis.
研究领域:
生物医学工程
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分子生物学
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纳米技术
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癌症研究
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产品关联
DOI
PubMed
高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2022
·
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.
研究领域:
分析化学
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纳米技术
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生物传感器
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产品关联
DOI
PubMed
高影响因子
TALANTA
·
2020
·
IF 5.339
Libo Li,Bainian Chen,Lijun Luo,Xiaohong Liu,Xiaoya Bi,Tianyan You
In the present study, a novel self-enhanced electrochemiluminescence (ECL) aptasensor which combined self-enhanced ECL composite as signal response element and aptamer as the specific recognition element was firstly proposed for the sensitive and selective detection of Hg 2+ . Innovatively, the luminophore Ru(bpy) 3 2+ -doped silica nanoparticles functionalized with 3-aminopropyltriethoxysilane (NH 2 – [email protected] 2 ) and the co-reactant nitrogen doped graphene quantum dots (NGQDs) were bound together to form the self-enhanced ECL composite, NH 2 – [email protected] 2 -NGQDs, by electrostatic adsorption. Satisfactorily, high and stable luminous efficiency of NH 2 – [email protected] 2 -NGQDs was obtained benefited from the short electron transfer distance and low energy loss of self-enhanced-typal ECL composite. For the fabrication of the self-enhanced ECL aptasensor for Hg 2+ detection, the Hg 2+ aptamer, of which one end was connected to NH 2 – [email protected] 2 -NGQDs, and the other end was fixed on glass carbon electrode (GCE) surface through Au–S bond, was served as a bridge. Upon the addition of Hg 2+ , the aptamer was bent due to the formation of thymine-Hg 2+ -thymine (T-Hg 2+ -T) specific structure, which caused the self-enhanced ECL composite was close to the GCE surface. On this basis, a linearly enhanced ECL signal was acquired with the concentration of Hg 2+ in the range of 5.0 × 10 −11 M − 1.0 × 10 −6 M with excellent selectivity , repeatability and stability in 3 min for each assay. In addition, the proposed aptasensor showed satisfying accuracy and practicability for Hg 2+ analysis in tap and canal water verified by the inductively coupled plasma-mass spectrometry (ICP-MS) method.
研究领域:
分析化学
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环境科学
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纳米技术
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电化学
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产品关联
DOI
PubMed
高影响因子
ANALYTICAL CHEMISTRY
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2015
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IF 5.636
Daifang Wang,Yanyan Li,Zhenyu Lin,Bin Qiu,Longhua Guo
Carcinoembryonic antigen (CEA) is recognized as a disease biomarker to reflect the existence of various cancers and tumors in the human body. Sensitive detection of CEA in body fluid is valuable for clinical diagnosis and treatment assessment of cancers. Herein, we present a new approach for ultrasensitive determination of CEA in human serum based on localized surface plasmon resonance (LSPR) enhanced electrochemiluminescence (ECL) of Ru(bpy)32+. In this surface-enhanced ECL (SEECL) sensing scheme, Ru(bpy)32+-doped SiO2 nanoparticles (Ru@SiO2) act as ECL luminophores, and AuNPs are used as LSPR source to enhance the ECL signal. Two different kinds of aptamers specific to CEA are modified on the surface of Ru@SiO2 and AuNPs, respectively. In the presence of CEA, a multilayer of Ru@SiO2–AuNPs nanoarchitectures would be formed. Our investigation reveals that the ECL signal of Ru@SiO2 can be effectively enhanced by AuNPs. One layer of Ru@SiO2–AuNPs nanoarchitectures would generate about 3-fold ECL enhancement compared with the ECL of the nanoarchitectures without the presence of AuNPs. As much as 30-fold ECL enhancement could be obtained by a multilayer of Ru@SiO2–AuNPs nanoarchitectures. Under the optimal conditions, a detection limit of 1.52 × 10–6 ng/mL of CEA in human serum was achieved. To the best of our knowledge, CEA assays with such a low LOD have never been reported for an ECL sensor.
研究领域:
分析化学
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生物医学工程
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肿瘤学
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产品关联
DOI
PubMed
高影响因子
ACS Catalysis
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2025
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IF 13.1
Shaorong Deng,Chenji Zhu,Xiuzhong Fang,Xianglan Xu,Xiang Wang
A series of Ru-x%Li+/SiO2 catalysts (x = 0.05–0.2), modified with varying amounts of lithium cation (Li+), were prepared via coimpregnation and evaluated for CO2 methanation to explore Li+ modification on Ru/SiO2. Introducing trace Li+ markedly boosts reaction activity, with the optimal Ru-0.1%Li+/SiO2 exhibiting 38.4 and 12.3 times higher overall reaction rate and turnover frequency at 200 °C, respectively, compared to Ru/SiO2. Structural characterization confirmed that Li+ incorporation effectively suppresses RuO2 crystallization, thereby improving Ru dispersion from 9.1% to 31.5%, enhancing the active surface area from 33 to 115 m2 g–1, while simultaneously reducing Ru particle size from 18.4 to 3.2 nm. In situ spectroscopy and surface reaction experiments revealed that the CO* pathway occurs for CO2 methanation on both catalysts, which involves CO2 dissociation and subsequent CO* hydrogenation. The smaller Ru nanoparticles on Ru-0.1%Li+/SiO2 exhibit superior intrinsic activity for both steps compared to the larger nanoparticles on Ru/SiO2. The additional alkaline sites introduced by Li+ additives also promote CO2 dissociation. The exceptional activity of Ru-0.1%Li+/SiO2 for CO2 methanation is governed by the synergistic effect between the Ru particle size effect and Li+-induced basicity, with the former being predominant.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
BIOSENSORS & BIOELECTRONICS
·
2017
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IF 7.78
Wei Zhang,Huiwen Xiong,Miaomiao Chen,Xiuhua Zhang,Shengfu Wang
A novel molecularly imprinted electrochemiluminescence (MIP-ECL) sensor based on Ru(bpy) 3 2+ -doped silica nanoparticles (Ru@SiO 2 NPs) is developed for highly sensitive detection of fumonisin B 1 (FB 1 ). Gold-nanoparticles (AuNPs), Ru@SiO 2 NPs with chitosan (CS) composites and a molecularly imprinted polymer (MIP) are assembled on a glassy carbon electrode (GCE) to fabricate an ECL platform step by step. AuNPs could greatly promote the ECL intensity and improve the analytical sensitivity according to the localized surface plasmon resonance (LSPR) and the electrochemical effect . In this surface-enhanced electrochemiluminescence (SEECL) system, AuNPs work as the LSPR source to improve the ECL intensity and Ru@SiO 2 NPs are used as ECL luminophores. In the phosphate buffer solution (PBS), the evident anodic ECL of Ru@SiO 2 on the above working electrode is observed in the presence of the template molecule fumonisin B 1 (FB 1 ), which could act as the coreactant of Ru@SiO 2 NPs due to the amino group of FB 1 . When the template molecules were eluted from the MIP, little coreactant was left, resulting in an apparent decrease of ECL signal. After the MIP-ECL sensor was incubated in FB 1 solution, the template molecules rebound to the MIP surface , leading to the enhancement of ECL signal again. On the basis of these results, a facile MIP-ECL sensor has been successfully fabricated, which exhibited a linear range from 0.001 to 100 ng mL −1 with a detection limit of 0.35 pg mL −1 for FB 1 . Moreover, the proposed MIP-ECL sensor displayed an excellent application in real samples.
研究领域:
分析化学
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食品安全
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生物传感器
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纳米材料
·
环境监测
✓ 已验证
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
·
IF 5.2
Hongding Zhang,Sifei Wu,Yihan Li,Beibei Tao,Ningning Wu,Hai-Bo Wang,Linxia Fang
Fluorescent probes usually face the issue of photobleaching and premature leakage when they are directly exposed to exterior environment, causing poor photostability and low sensitivity. In this paper, Ru(bpy) 3 2+ encapsulated fluorescent SiO 2 nanoparticles (Ru@SiO 2 NPs) were synthesized and used as fluorescent probe. The SiO 2 nanoparticles were used as carriers to prevent the leakage of the probe. Triangular Ag nanoparticles (T-Ag NPs) were prepared as quenchers to construct a quenching system (Ru@SiO 2 -T-Ag NPs) with Ru@SiO 2 NPs through inner filter effect (IFE). In this quenching system, T-Ag NPs were also designed as recognize units for glutathione (GSH) detection. When GSH existed, the GSH bond with T-Ag NPs to form Ag-S bonds, making the T-Ag NPs etched. In this case, the fluorescent signal of Ru@SiO 2 NPs quenched by T-Ag NPs restored. The fluorescence recovery of the Ru@SiO 2 NPs depended on GSH concentrations and thus it could realize the quantitative analysis of GSH. Under optimized conditions, the proposed assay had good analytical performance for the detection of GSH in the concentration range of 0.01–1 µM with a limit of detection (LOD) as low as 2.8 nM. This assay was also used to measure GSH levels in human serum samples. This work provides a new way for the fluorescent analysis of thiol biomolecules.
研究领域:
分析化学
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生物医学
✓ 已验证
产品关联
DOI
高影响因子
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