JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
·
IF 8.128
Libo Li,Wanlin Zhao,Jiayi Zhang,Lijun Luo,Xiaohong Liu,Xia Li,Tianyan You,Chunjiang Zhao
Herein, a label-free, self-enhanced electrochemiluminescence (ECL) sensing strategy for divalent mercury (Hg(II)) detection was presented. First, a novel self-enhanced ECL luminophore was prepared by combining the ECL reagent tris(2, 2′-bipyridyl) dichlororuthenium(II) hexahydrate (Ru(bpy) 3 2+ ) and its co-reactant carbon nitride quantum dots (CNQDs) via electrostatic interactions. In contrast to traditional ECL systems where the emitter and its co-reactant underwent an intermolecular reaction, the self-enhanced ECL system exhibited a shortened electron-transfer distance and enhanced luminous efficiency because the electrons transferred from CNQDs to oxidized Ru(bpy) 3 2+ via an intramolecular pathway. Furthermore, the as-prepared self-enhanced ECL material was encapsulated in silica (SiO 2 ) nanoparticles to generate a [email protected] 2 luminophore. Based on the different affinity of [email protected] 2 nanoparticles for single-stranded DNA (ssDNA) and Hg(II)-triggered double-stranded DNA (dsDNA), a label-free ECL biosensor for Hg(II) detection was developed as follows: in the absence of Hg(II), ssDNA was adsorbed on [email protected] 2 surface via hydrogen bond, electrostatic, and hydrophobic interaction. Thus, quenched ECL signal was observed. On the contrary, in the presence of Hg(II), stable dsDNA was formed and carried the ssDNA separating from [email protected] 2 surface, resulting in most of [email protected] 2 existing in their free state. Therefore, a recovered ECL intensity was obtained. On this basis, Hg(II) was measured by the proposed method in the range of 0.1 nM-10 μM, with a detection limit of 33 pM. Finally, Hg(II) spiked in water samples was measured to evaluate the practicality of the fabricated biosensor.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Qi Zhang,Shihui Jiao,Boran Wang,Zisheng Wang,Xinyan Lv,Wenwen Wang,Yumei Tan,Canyu Cui,Yan Chen
Electrocatalytic water splitting for hydrogen production plays a vital role in the development of new energy field, but there is still a lack of low-content precious metal or cost-effective non-noble metal catalysts for the hydrogen evolution reaction (HER). Therefore, how to develop the catalysts with a smaller amount of precious metal to achieve higher performance is still a major challenge. Herein, we have fabricated Ru–Ni 2 P@Ni(OH) 2 /NF-2 heterostructure by phosphating Ni(OH) 2 /NF and then anchoring Ru on the surface through wet chemical strategy. Benefiting from its optimal Δ G H∗ and synergistic effect , this Ru–Ni 2 P@Ni(OH) 2 /NF-2 catalyst shows superior electrocatalytic HER kinetics in alkaline electrolyte . A small overpotential of 31 mV is needed for this electrocatalyst to obtain the current densities of 10 mA cm −2 with remarkable durability over 24 h. This work provides a new strategy for the preparation of effective HER electrocatalyst with a low precious metal content.
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JOURNAL OF THE ENERGY INSTITUTE
·
2021
·
IF 6.186
Lin Hu,Xian-Yong Wei,Zhi-Ming Zong
Recently hydrocarbons with high yield from the selective hydrodeoxygenation (HDO) of lignin-derived bio-oil under low temperature still encounters the great challenges. However, metal nanoparticles size and acid site can greatly influence the HDO activity of metal catalyst . Herein, the efficient bifunctional Ru/Hβ catalyst was prepared by modified deposition-precipitation (DP) method for the HDO reaction of guaiacol and catalytic isoproanolysis lignin-derived bio-oil. Notably, compared to the impregnated Ru 3% /Hβ-25 catalyst, Ru 3% /Hβ-25 (DP) catalyst exhibited the higher catalytic activity on the HDO of guaiacol, smaller Ru nanoparticles size, and more acid sites. It was observed that guaiacol can be completely converted to cyclohexane under 180 °C, 3 MPa H 2 , and 2 h in n -hexane. This Ru 3% /Hβ-25 (DP) catalyst proved to be the good recyclability in the HDO reaction of guaiacol, the conversion decreased slightly to 82.3% and the yield of cyclohexane decreased to 71.2 mol% after four recycle times. Furthermore, this high active catalyst was also applied to the upgradation of bio-oil derived from the catalysis isoproanolysis of lignin in the organic phase. As a result, after the upgradation, bio-oil contained high relative content (RC) of hydrocarbons, including 42.99% cycloalkanes and 50.74% arenes, and oxygenated compounds of raw bio-oil were almost removed. Overall, during upgradation of raw lignin-derived bio-oil over Ru 3% /Hβ-25 (DP) catalyst process, not only HDO reaction, but also cleavage of C-O bonds can be achieved in one-pot.
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ChemSusChem
·
2020
·Vol. 13
·期 21
·5683-5689
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IF 7.962
Zhenbing Xie,Bingfeng Chen,Fangfang Peng,Mingyang Liu,Huizhen Liu,Guanying Yang,Buxing Han
Graphical A sustainable conversion : Developing highly efficient catalytic systems for amino acid productions from renewable bio-derived chemicals is very attractive for a sustainable future. N-doped carbon nanotube-supported Ru nanoparticles (Ru/N−CNTs) display excellent performance in the amination of bio-derived hydroxy acids into amino acids. The high-performance can be correlated with high dispersion of Ru nanoparticles and electronic effect resulting from the N-dopant. The amino acids have extensive applications, and their productions from biomass-derived feedstocks are very attractive. In this work, the synthesis of amino acids by amination of bio-derived hydroxy acids with ammonia over different metallic nano-catalysts supported on various supports is studied. It is found that Ru nano-catalysts on the nitrogen-doped carbon nanotubes (Ru/N−CNTs) have an outstanding performance for the reaction. Different hydroxy acids can be catalytically converted into the corresponding amino acids with yields up to 70.0 % under mild conditions, which is higher than those reported. The reasons for the high efficiency of the catalyst are investigated, and the reaction pathway is proposed on the basis of control experiments.
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ACS Applied Bio Materials
·
2019
·
IF 0
Zhixin Li,Jinwei Zhang,Huixing Chen,Xiaocui Huang,Da Huang,Fang Luo,Jian Wang,Longhua Guo,Bin Qiu,Zhenyu Lin
Hyaluronidase (HAase), a specific enzyme of hyaluronic acid (HA), has been reported as a potential tumor biomarker in recent years. Hence, developing some simple, rapid, and sensitive methods for HAase assay is necessary. In this work, a simple and sensitive biosensor constructed by a reliable controlled release system and a mature electrochemiluminescence (ECL) analytical technique has been devised for the quantification of HAase with high efficiency and selectivity. Tris (2,2′-bipyridyl) ruthenium(II) chloride hexahydrate doped SiO2 nanoparticles (Ru@SiO2 NPs), as ECL signal probes, were trapped in the hydrogel fabricated by HA and polyethylenimine evenly and steadily. When HAase existed, the hydrogel was decomposed by HAase, and the Ru@SiO2 NPs escaped from the hydrogel into the supernate. The ECL signal produced from the supernate can be detected and used to characterize HAase concentration. The result showed a good linear relationship between ECL intensity, and HAase concentration ranged from 2 to 60 U/mL and the limit of detection was 2 U/mL. The developed controlled release ECL biosensor has been used for HAase quantification in urine samples with satisfactory results.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Ying Yuan,Junfeng Rong,Lufan Zheng,Zheng Hu,Shi Hu,Chongchong Wu,Zhongbin Zhuang
Controlling metal-support interaction (MSI) is considered as an effective strategy to optimize the electronic structure of catalysts and thus promote their catalytic performance. Here, with the strong MSI by both metal core and nitrogen-doped carbon shell, the synthesized Ru supported on N-doped graphene-encapsulated Ni nanoparticles (Ni@NC/Ru) show excellent performance towards hydrogen evolution reaction (HER). It exhibits a very low HER potential of 28 mV at the current density of 10 mA cm −2 , and high durability that the potential only increases approximately 7 mV after 10,000 cyclic voltammetry cycles. The high HER performance is attributed to the strong MSI from the tuning effect of Ni metal core and N-dope graphene shell, which optimizes the hydrogen binding energy of the catalysts. This study may shed light on the rational design of superior HER catalysts.
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FUEL PROCESSING TECHNOLOGY
·
2023
·
IF 7.5
Yan-Hong Li,Fang-Jing Liu,Jia-Pei Guo,Fan Yin,Shan-Shan Gao,Yao Lu,Rui Song,Yan-Ming Yu,Juan-Juan Zheng,Yun-Peng Zhao,Ri-Guang Zhang,Zai-Xing Huang,Jing-Pei Cao,Xian-Yong Wei,Maohong Fan
Low temperature and highly selective hydrogenation of the lignin-derived aromatics to obtain high-value chemicals and clean liquid fuels is a significant step for lignin valorization in the chemical industry. Developing efficient catalysts with high activity and selectivity for hydrogenation of lignin-derived aromatic rings at low temperature remains a big challenge. Herein, a well-dispersed Ru-Fe bimetallic nanoparticle catalyst supported on porous nitrogen-doped carbon was developed through a facile impregnation method. It showed excellent catalytic activity for hydrogenation of lignin-derived aromatics, such as diaryl ethers, phenolic monomers and arenes to corresponding alicyclic compounds with high selectivity, under surprisingly mild conditions (≤50 °C, ≤2 h and 1 MPa H 2 ). Hydrogenation of aromatic rings took precedence over the cleavage of C-O bond for the lignin-derived aromatics. The resulting alicyclic compounds are key raw materials for synthesizing polymer, pharmaceutical intermediates and resins, and clean liquid fuels. The strong interactions between metal and support improved the anti-oxidation and anti-sintering ability of the catalyst, and significantly improve the hydrogenation performance. Additionally, the phenols in the lignin oil were effectively converted into cyclohexanol and its derivatives at 90 °C over the Ru-Fe bimetallic catalyst , with selectivity up to 53.3% in the hydrogenated lignin oil. The development of this catalyst for selective hydrogenation of lignin-derived aromatics at low temperature provides a green, low carbon footprint and sustainable approach for the value-added utilization of lignin and its derivatives.
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2019
·Vol. 94
·期 7
·2355-2363
·
IF 2.659
Hui-Fang Ren,Dan Zhu,Ji-Fan Li,Chun-Ling Liu,Rong-Zhen Yang,Wen-Sheng Dong
BACKGROUND The chemical catalytic conversion of carbohydrates into γ-valerolactone (GVL) is a sustainable alternative to the petrochemical process starting from the depleting fossil resources. Direct conversion of carbohydrates (fructose, glucose, starch and cellulose) into GVL was achieved via the combined heteropoly acid based SO 3 H-functionalized ionic liquid (HAIL) and supported ruthenium (Ru) catalyst system in one pot and in water media. RESULTS A 63% GVL yield (based on fructose) was obtained under the catalysis of 1-methyl-3-(3-sulfopropylimidazolium)silicotungstate ([MIMPS] 4 SiW) and Ru/ZrO 2 at 180 °C, first in 0.1 MPa nitrogen (N 2 ) for 3 h (dehydration), and then in 4 MPa hydrogen (H 2 ) for 10 h (hydrogenation). Under the same reaction conditions, the GVL yields from glucose, starch and cellulose were 68%, 60% and 60%, respectively. The recyclability of the catalytic system consisting of [MIMPS] 4 SiW and Ru/ZrO 2 was investigated in four runs. The activity for [MIMPS] 4 SiW did not change after use. Partial deactivation of Ru/ZrO 2 was observed, which was ascribed to the severe carbon deposition. CONCLUSIONS In the present method, HAIL and Ru/ZrO 2 catalysts were loaded together. No separation and/or neutralization step reported in the literature was needed and only an atmosphere change (from N 2 to H 2 ) step was involved. Therefore, we provide a promising method for efficient conversion of carbohydrates into GVL. © 2019 Society of Chemical Industry
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2019
·Vol. 35
·期 3
·370-376
·
IF 1.071
Wu Shuo,Yang Xinlan,Zhao Yanqiu
A biomolecule-free photoelectrochemical(PEC) probe(denoted as Ru-1) was designed, synthesized and coupled with TiO 2 nanoparticles(NPs) for the highly sensitive and selective PEC detection of Hg 2+ , a model analyte with hypertoxicity to both human health and ecosystem. The probe Ru-1 was designed with Ru(II) bipyridyl complex as the chromophore, thiocyanate ligand as the recognition unit, and carboxylate group as the linkage site to connect Ru-1 to TiO 2 nanoparticles. Under irradiation, Ru-1 shows strong affinity to TiO 2 and good photophysical properties of strong visible light absorption, slow electron-hole(e-h + ) recombination, and fast photoelectron injection to TiO 2 nanoparticles via the π -bridge of 4-(2,2′-bipyridin)-4-yl-thiophene moiety. However, the specific coordination of Hg 2+ with Ru-1 via the thiol moiety in the thiocyanate enlarges the band gap of the complex and reduces the photocurrent significantly. The synergistic interaction between TiO 2 nanoparticles and the Ru-1 complex led to a selective PEC sensing strategy for Hg 2+ detection. Detectable linear ranges from 10 −12 g/mL to 10 −7 g/mL and from 10 −7 g/mL to 10 −3 g/mL were obtained without the interference from possibly co-existed metal ions. The good analytical performances indicate the chemical probe based biomolecule-free PEC platform may offer a new route for the detection of biologically and environmentally important small molecules.
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Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 24
·11337-11345
·
IF 9.931
Wei-Ming Liao,Jian-Hua Zhang,Zheng Wang,Shao-Yun Yin,Mei Pan,Hai-Ping Wang,Cheng-Yong Su
Electron-deficient Ru/Rh half-sandwich units are optoelectronical, stereochemical, and redox and catalytically active in nature. Four different species of these units were designed and successfully incorporated into UiO-67 frameworks by post-synthetic exchange (PSE) method and employed for photocatalytic H2 evolution and CO2 reduction. Among them, the PSE-MOF catalysts containing [M–OH2] (M = Rh or Ru) groups show higher photocatalytic activity than those with [M–Cl], providing a new example of the exploitation of H2O molecules as small ancillary ligands for the construction of Ru/Rh half-sandwich units and subsequent incorporation into MOFs as photocatalytic centers. The application of TEOA (triethanolamine) and DMA (N,N-dimethylaniline) as sacrificial agents leads to different catalytic mechanisms and durations. A long-term hydrogen evolution lasting for 174 h without significant decrease in efficiency was achieved in the RhOH2@UiO-DMA system, showing the advantage of PSE-MOFs as highly stable photocatalytic platforms with superior self-protective properties.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2019
·
IF 6.393
Xin Xiong,Yao Zhang,YinFang Wang,HaiFeng Sha,Nengqin Jia
By virtue of the metal organic framework UiO-66-NH 2, an ingenious electrochemiluminescence immunosensor was successfully constructed for subtle exploration of the breast cancer biomarker CA 15-3. In this protocol, Ru(bpy) 3 Cl 2 ·6H 2 O (Ru(bpy) 3 2+ ), as a conventional luminescent reagent, provides a stable and strong luminescent signal. The UiO-66-NH 2 serves as a carrier to provide a large specific surface area for enhancing the electrochemical luminescence signal response of Ru(bpy) 3 2+ . UiO-66-NH 2 , Ru(bpy) 3 2+ are fixed together with Nafion membrane, and CA 15-3 antibody is covalently conjugated onto the membrane through the amide reaction. Ru(bpy) 3 2+ @UiO-66-NH 2 is used as the detection system. The experimental results reveal that the ECL signal decreased obviously after the CA 15-3 antigen molecule is captured on the immunosensor, with the capture of manifesting the principle of electrochemical luminescence quenching detection. Under optimal conditions, the sensor is sensitive and selective for detecting CA 15-3 with the detection range from 5 × 10 −4 to 5 × 10 2 U mL -1 and the low LOD (1.7705 × 10 -5 U mL -1 ). Furthermore, multiple experiments elucidate that the as-prepared sensor could be used for susceptibly detect CA 15-3 in actual samples, which has underlying application prospects in biological analysis.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Hang Xu,Mingjing Ge,Yin Liu,Chen Yao,Houzhen Zhou,Mingmei Ding,Yang Li
Singlet oxygen ( 1 O 2 ) is an electrophilic oxidant capable of selectively eliminating contaminants in complex wastewater, which is highly expected in environmental remediation. However, due to the limitations in synthesizing catalysts with well-defined adsorption and active sites, the efficient and selective generation of 1 O 2 remains challenging. Herein, isolated Ru-O 3 moiety decorated two-dimensional Ti 3 C 2 T x catalysts (Ru-SA/Ti 3 C 2 T x ) were prepared to regulate 1 O 2 generation via peroxymonosulfate (PMS) activation. The constructed catalysts with asymmetric dual-metal structures (Ti-O-Ru) exhibited surprising mass activity of 1.4 × 10 4 min −1 ·mol −1 with a high 1 O 2 generation selectivity of 98.3 %. Mechanism inquiry indicated that the enhanced adsorption and electron transfer between PMS and Ru-SA/Ti 3 C 2 T x attributed to the synergistic effect of the strong adsorption at the Ru sites and the rapid electron transfer in the asymmetric Ti-O-Ru structures. Theoretical calculations demonstrated that Ru-O 3 moiety decreased the formation energy barrier of key intermediate *O, thus converting to a 1 O 2 -dominated oxidation path. Two possible degradation pathways of tetracycline hydrochloride (TCH) were proposed by gas chromatography-mass spectrometry (GC–MS), and the toxicities of intermediates were significantly decreased due to the strong electrophilic attack of 1 O 2 . This study deepened the understanding of the specific contribution of individual sites in multi-site synergistic, which furnished implications for the design and optimization of Fenton-like catalysts.
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