Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 20
·12196-12202
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IF 12.732
Yijun Li,Huijing Liu,Bing Li,Zhenzhen Yang,Zhenguo Guo,Jian-Bo He,Jianhui Xie,Tai-Chu Lau
Electrocatalytic water splitting is one of the most desirable ways to produce hydrogen, which is a clean and sustainable energy source. Improving the formation and the exposure of active sites is a key issue in the design of cost-effective and efficient metal-based electrocatalysts, especially for noble metals, in order to cut down the metal content and improve the mass activity of the metals, while maintaining high catalytic activity. Herein, we report a high-performance Ru-based electrocatalyst consisting of Ru single atoms and Ru nanoclusters encapsulated in highly porous N-doped carbon with abundant hierarchical pores (Ru/p-NC). Remarkably, Ru/p-NC shows excellent HER activity in 1.0 M KOH with a low overpotential of 10 mV at 10 mA cm−2, a small Tafel slope of 17 mV dec−1 as well as good durability for 24 h, outperforming commercial Pt/C and Ru/C catalysts. More importantly, the mass activity and turnover frequency (based on Ru loading) of Ru/p-NC are ultrahigh owing to the low loading of Ru, which are 17 A mgRu−1 and 8.9 H2 s−1, respectively, at a very low overpotential of 25 mV. Experimental results indicate that the porous N-doped carbon support not only leads to exposed active sites but also interacts strongly with the Ru moieties. In addition, it tunes the electronic structure of the catalyst, boosts the stability as well as facilitates mass transport and charge transfer kinetics. This work provides a new route for the synthesis of metal-based porous N-doped carbon hybrid electrocatalysts with abundant exposed active sites and strong metal-support interaction for energy conversion.
研究领域:
材料科学
·
电化学
·
能源转换
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INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Qikang Wu,Han Li,Yan Zhou,Shanshan Lv,Taiyu Chen,Shaohuan Liu,Wanying Li,Zheng Chen
Ruthenium, which is relatively cheap in precious metals, has become a popular alternative for a hydrogen evolution reaction (HER) catalyst because of its corrosion resistance and appropriate metal–H bond strength. Convenient synthesis and active site regulation are conducive to stimulating the excellent catalytic performance of Ru as much as possible. Herein, using the mature mesoporous nitrogen-doped carbon material as the support, the catalytic materials containing both single atom Ru and Ru nanoparticles were synthesized by impregnation using the solid-phase reduction method. The effect of reduction temperature on the dispersion state and electronic structure of Ru species has been fully studied using electronic and spectroscopic characterizations. The sample reduced at 300 °C has excellent HER activity with overpotentials of 10.8 and 53.8 mV to deliver 10 mA/cm2 in alkaline and acidic media, respectively, which is among the best activities in the reported results. Electrochemical impedance analysis shows that the reduction temperature has a great influence on the number of active sites and charge transfer impedance of the catalyst.
研究领域:
材料科学
·
催化化学
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MICROCHEMICAL JOURNAL
·
2021
·
IF 4.821
Xiu-hua Wei,Xing Qiao,Jie Fan,Yuan-qiang Hao,Yin-tang Zhang,Yan-li Zhou,Mao-tian Xu
Herein, a label-free electrochemiluminescence (ECL) biosensor for sensitive determination of carcinoembryonic antigen (CEA) was fabricated based on CdS quantum dots loaded onto metal organic framework (CdS QDs@MOF) and triethanolamine modified on gold nanoparticles (TEOA@AuNPs) as bi-coreactants of Ru(bpy) 3 2+ ECL system. The TEOA@AuNPs served as not only coreactant of Ru(bpy) 3 2+ but also nanocarrier for CEA aptamer which was bonded to the TEOA@AuNPs through Au–S bond. After incubated in CEA solution, the ECL signals decreased due to the poor conductivity of CEA and there was a linear correlation between the ECL intensity and log(C CEA ). Based on this result, a label-free ECL biosensor has been developed successfully and used to detect CEA with a detection limit of 8.5 × 10 −5 ng/mL. The proposed ECL aptasensor had good analytical performance in the detection of CEA in human serum samples.
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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.
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FOOD CHEMISTRY
·
2023
·
IF 8.8
Liangrui Lv,QingQing Chen,Chunyang Jing,Xiaoying Wang
To sensitively monitor trace-level of toxic patulin (PAT), an ultrasensitive PAT ratiometric aptasensor based on the dual-potential electrochemiluminescence (ECL) of Ru(bpy) 3 2+ was first proposed. Noteworthily, Ru(bpy) 3 2+ -doped trimetallic nanocube ( [email protected] ) innovatively integrated the luminophore and cathode coreaction accelerator (CCA), which could generate strong cathodic ECL in the existence of low concentration of K 2 S 2 O 8 . Simultaneously, anthocyanin-derived carbon quantum dots (anth-CQDs) prepared from purple potato skins was first served as a green anodic coreactant. And SiO 2 -coated anth-CQDs ( [email protected] 2 ) exhibited excellent performance for enhancing anodic ECL of [email protected] Based on this, a novel ternary ECL system was established. In the presence of PAT, the ECL intensity ratio of anode to cathode ( I ECL-A / I ECL-C ) was significantly increased, and a low detection limit of 0.05 pg mL −1 was obtained. Moreover, when proposed method and high performance liquid chromatography (HPLC) were simultaneously applied to series of fruit products, the obtained results were completely consistent, reflecting its practicability.
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ANALYTICAL CHEMISTRY
·
2016
·
IF 5.886
Yong-Ping Dong,Ying Zhou,Jiao Wang,Jun-Jie Zhu
In the present work, strong anodic electrogenerated chemiluminescence (ECL) of Ru(bpy)32+ was observed at a graphene oxide modified glassy carbon electrode (GO/GCE) in the absence of coreactants. The electrocatalytical effect of GO on the oxidation of Ru(bpy)32+ suggested that GO itself can act as the coreactant of Ru(bpy)32+ ECL, which can be used to fabricate the ECL biosensor. Thiol group terminated adenosine triphosphate (ATP) aptamer was immobilized on the GO film via DNA hybridization. When gold nanoparticles/graphene oxide (AuNPs/GO) nanocomposites were modified on the aptamer through the S–Au bond to form a sandwich-like structure, the ECL resonance energy transfer (ECL-RET) could occur between Ru(bpy)32+ and AuNPs/GO nanocomposites, resulting in an apparent decrease of ECL signal. After the ECL sensor was incubated in ATP solution, the AuNPs/GO nanocomposites were released from the electrode due to the specific interaction between aptamer and ATP, leading to the increased ECL signal. On the basis of these results, an ECL aptasensor was fabricated and could be used in the sensitive and selective detection of ATP in the range of 0.02–200 pM with a detection limit of 6.7 fM (S/N = 3). The proposed ECL aptasensor can be applied in the detection of ATP in real samples with satisfactory results.
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JOURNAL OF INORGANIC BIOCHEMISTRY
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2015
·
IF 3.444
Lan-mei Chen,Fa Peng,Guo-dong Li,Xin-ming Jie,Kang-rong Cai,Chun Cai,Yu Zhong,Hua Zeng,Wu Li,Zhen Zhang,Jin-can Chen
A new ruthenium methylimidazole complex [Ru(MeIm) 4 ( p -cpip)] 2 + ( Ru1 , p -cpip = 2-(4-chlorophenyl)-1 H-imidazo[4,5-f][1,10]phenanthroline, MeIm = 1-methylimidazole) has been synthesized and characterized. The cellular uptake, in vitro cytotoxicities, cell cycle arrest and apoptosis-inducing mechanism of this Ru(II) complex have been extensively explored by Inductively Coupled Plasma Mass Spectrometry (ICP-MS), 3-(4,5-dimethylthiazol-2-yl)-2,5-diphenyltetrazolium bromide (MTT) assay, flow cytometry , Comet assay , inverted fluorescence microscope as well as Western blotting experimental techniques. Notably, Ru1 displayed relatively high cytotoxic activity against lung cancer A549 cells and had high selectivity between tumor and normal cells in comparison with cisplatin . Further studies showed that Ru1 caused cell cycle arrest at G0/G1 phase and induced apoptosis via the mitochondrial pathway, which involved reactive oxygen species (ROS) accumulation, mitochondrial dysfunction and Bcl-2 and caspase correlative family member activation. For providing more information about the possible antitumor mechanism, the in vitro DNA binding studies have been also investigated by different spectrophotometric methods, thermal denaturation and viscosity measurements.
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DALTON TRANSACTIONS
·
2016
·Vol. 45
·期 39
·15595-15602
·
IF 4.177
Xinlin Li,Shiling Zhao,Wei Zhang,Yansheng Liu,Rong Li
Ruthenium (Ru) nanoparticles (NPs) are supported on nitrogen-doped porous carbon (NPC) derived from metal–organic-framework (MOF) ZIF-8 for the first time. NPC is prepared by the direct carbonization of ZIF-8 crystals, which not only retains the original morphology of ZIF-8 but also provides a high surface area and stable chemical–physical properties. Ru NPs were supported by different methods. Four types of Ru-based catalysts are tested in the selective hydrogenation of p-chloronitrobenzene (p-CNB) and p-bromonitrobenzene (p-BNB) to haloanilines. Different catalytic activities and selectivities are obtained through these catalysts. After the screening of the catalysts and reaction conditions, high conversion and selectivity were obtained. The hydrogen pressure is limited to 1.5 MPa, which is much lower than most previous reports, and the dehalogenation reaction is restricted to a very low level. Furthermore, the dehalogenation properties of the Ru/NPC catalysts are also studied.
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Journal of Materials Chemistry A
·
2015
·Vol. 3
·期 19
·10386-10394
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IF 7.443
Chun-Chao Hou,Ting-Ting Li,Shuang Cao,Yong Chen,Wen-Fu Fu
A molecular photosensitizer [Ru(dcbpy)(bpy)2]2+ (dcbpy = 2,2′-bipyridyl-5,5′-dicarboxylic acid) and a proton reduction catalyst Pt(dcbpy)Cl2 were successfully incorporated into a highly robust metal–organic framework (MOF) of Zr(IV)6O4(OH)4(bpdc)6 (bpdc = 4,4′-biphenyldicarboxylic acid) by making use of a mix-and-match approach. The molecular integrity of the Ru and Pt complexes within the MOFs was demonstrated by a variety of techniques, including XRD, BET, TGA, SEM, TEM, HAADF-STEM, EDX, DRUS and XPS. This di-component Ru–Pt@UIO-67 MOF assembly allows a facile arrangement of the photosensitizer and the reduction catalyst with close spatial proximity, promotes the electron transfer between them, and thus leads to a significantly improved hydrogen evolution activity in aqueous solution at pH 5.0 upon visible light irradiation. This Ru–Pt@UIO-67 system represents the first example of MOFs functionalized with two different transition metal complexes, which can be used as a photosensitizer and catalyst, respectively, for hydrogen generation from water.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Hanyu Tan,Chaoyang Shi,Mingli Xu,Zhiwei Meng,Baoyu Huang,Qingrong Long,Jie Yu
Constructing dual active sites, adjusting electronic structures at interfaces and optimizing the adsorption energy of intermediates can effectively enhance water electrolysis performance. A novel Fe 3 C-Ru/NFs bifunctional catalyst is successfully synthesized via an electrospinning-carbonization method, in which sub-nanometer Ru particles coupled with Fe 3 C. Experimental results indicate that Fe 3 C-Ru/NFs catalyst delivers exceptional HER (18 mV@10 mA cm −2 , 202 mV@500 mA cm −2 ) and OER (263 mV@10 mA cm −2 , 382 mV@500 mA cm −2 ) performance in 1 M KOH solution. Moreover, Fe 3 C-Ru/NFs catalyst was employed as a bifunctional electrode in an overall water electrolyzer, resulting in a lower cell voltage and excellent stability (1.87 V, 150 h @ 500 mA cm −2 ). Density Functional Theory (DFT) calculation shows that the synergy between Ru and Fe sites can enhance electron transfer, and initiate a hydrogen spillover mechanism, and optimize intermediate adsorption energies, finally accelerating both HER and OER processes. This work offers valuable insights into developing low-cost, high-efficiency water electrolysis catalysts, demonstrating the significant potential for practical applications.
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ANALYTICA CHIMICA ACTA
·
2025
·
IF 6
Xiaoshuo Zhang,Rui Dai,Faqiong Zhao,Baizhao Zeng
Background Epithelial cell adhesion molecules (EpCAM) protein is one of the most frequently and intensely studied tumor-associated antigens because of its overexpression in most cancer cells. Thus, it is regarded as a tumor biomarker associated with a wide variety of carcinomas and reflects the existence and growth of tumors in the human body. It is highly required to detect low concentrations of EpCAM in early stage for ensuring human health. Results In this study, a novel sandwich electrochemiluminescence (ECL) aptasensor was developed for EpCAM detection. Wherein oxalate-based Zn-MOF supported tris(2,2′-bipyridyl)ruthenium (II) (Ru(bpy) 3 2+ @Zn-MOF) was used as luminophore and gold nanoparticle modified o-phenylenediamine (PoPD@Au NPs) as quencher. The 3D Ru(bpy) 3 2+ @Zn-MOF generated self-enhanced ECL without additional co-reactants. Furthermore, it remained stable and had short electron transfer distance, ensuring high and stable ECL signal. The ECL signal could be effectively quenched by PoPD@Au NPs through resonance energy transfer (RET) and electron transfer (ET), due to its absorption spectrum overlapping with the ECL emission spectrum of Ru(bpy) 3 2+ @Zn-MOF. In the presence of EpCAM, the aptamer acted as a linker between the luminophore and quencher, forming a sandwich structure that had reduced ECL intensity. Under optimal conditions, EpCAM could be sensitively detected over the range of 1 pg mL -1 -100 ng mL -1 , with a detection limit of 0.34 pg mL -1 . Significance This work developed a ECL aptasensor with self-enhanced Ru(bpy) 3 2+ @Zn-MOF luminophore for EpCAM detection. The ECL system was simple, but ultrasensitive for EpCAM monitoring, thanks to the ECL-RET and ET between Ru(bpy) 3 2+ @Zn-MOF and PoPD@Au NPs. It also could be applied to detect other biomolecules by replacing the aptamer, offering significant potential in disease diagnosis.
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REACTIVE & FUNCTIONAL POLYMERS
·
2017
·
IF 3.151
Jianxian Zeng,Zhe Zhang,Zhihui Dong,Panfeng Ren,Yuan Li,Xiao Liu
An ion-imprinted blend membrane (Ru(III)-IIM) for selectively adsorbing ruthenium(III) from aqueous solutions was fabricated by blending poly(methyl methacrylate- co -2-hydroxyethyl methacrylate) P(MMA-HEMA) with polyvinylidene fluoride (PVDF). Firstly, P(MMA-HEMA) was successfully synthesized and characterized. Subsequently, combining with the ion-imprinting technology, a series of Ru(III)-IIMs were fabricated via the non-solvent induced phase inversion method. The results indicated that increasing the polymer concentration and extending the evaporation time led to transform the cross-section of membranes from macrovoid structure to a finger-like or tear-like even sponge structure, and also decreased the water flux. The contact angle tests showed the hydrophilicity of Ru(III)-IIMs were effectively improved by blending with P(MMA-HEMA), compared with the PVDF membrane. The adsorption experiments showed that the adsorption capacity of ruthenium(III) onto the Ru(III)-IIM was pH-dependent, and the maximum adsorption capacity reached 42.31 mg g − 1 at pH 2.0. The adsorption process was well described by the pseudo-second-order kinetic model and the Langmuir isotherm model. The selective adsorption was studied by using Ni(II) as an interfering ion. Compared with the non-imprinted membrane, the Ru(III)-IIM showed a higher selectivity for Ru(III), with a selectivity coefficient of 6.0 for Ru(III)/Ni(II). In addition, the Ru(III)-IIM had a high reusability and still maintained about 95% of its initial adsorption capacity for Ru(III) after eight cycles.
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