ENERGY CONVERSION AND MANAGEMENT
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2023
·
IF 10.4
Ruizhe Chen,Leilei Cheng,Jing Gu,Haoran Yuan,Yong Chen
Hydroconversion has been demonstrated as a viable method to efficiently deconstruct polyolefins under relatively mild conditions. The hydrogenolysis of C–C bonds over Ru-based catalysts can convert polyolefins into liquid alkanes and methane. To suppress methane generation and obtain high-value isomer, further exploration of the mechanism for the cooperative deconstruction of polyolefins by bifunctional catalysts with metal–acid sites is necessary. In this study, we utilized ball milling to enhance the accessibility of acid sites within MOR zeolite, while the fragmented pore structure ensured that the loaded Ru metal was sufficiently accessible for long-chain alkanes. The sequential accessibility of metal–acid sites boosted the hydroconversion efficiency of low-density polyethylene (LDPE). Through systematic investigations involving catalysts with various Ru loadings and Si/Al ratio of zeolites, it is discovered that the smaller-sized Ru particles not only facilitate the generation and desorption of olefinic intermediates in hydrocracking but also promote the hydrogenation and desorption of alkyls and suppress the cascade of terminal C–C bond cleavage in hydrogenolysis. Liquid fuel (C 5 -C 21 ) yield was increased by 27% for the catalyst loaded with 0.7 wt% Ru on mMOR20 compared to 1.7 wt% loadings, while methane yield was only one-third of the latter. Concurrently, the distribution of acid sites on the zeolite surface affected the aggregation process of Ru atoms. This study deeply unveils the synergistic interaction of metal–acid sites, facilitating internal C–C bond cleavage to obtain liquid fuel and sheds light on catalyst design for waste polyolefins upcycling.
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CHEMOSPHERE
·
2023
·
IF 8.8
Mian Hu,Zhibing Li,Xiaotong Huang,Meiqi Chen,Zhong-Ting Hu,Suqin Tang,I-Ming Chou,Zhiyan Pan,Qi Wang,Junliang Wang
To ascertain the reaction variables on o -chloroaniline ( o -ClA) mineralization, total nitrogen (TN) removal rate, and N-species distribution, o -ClA was subjected to catalytic supercritical water oxidation (CSCWO) in a fused quartz tube reactor (FQTR). The findings demonstrated that when the temperature, reaction time, and excess oxidant were 400 °C, 90 min, and 150%, respectively, the mineralization rate of o -ClA could reach more than 95%. Moreover, potential degradation pathways of o -ClA in supercritical water oxidation (SCWO) was proposed according to the GC-MS results. TN removal rate is significantly impacted by Ru/rGO, despite the fact that its catalytic effect on the mineralization of o -ClA was not particularly noteworthy. Compared with no catalyst, the TN removal rate of o -ClA obviously increased from 44.1% to 90.3% at 400 °C, 10 wt% Ru loading, 90 min and 200% excess oxidant. In addition, N-species distribution in SCWO and CSCWO were also investigated. Results indicated that the Ru/rGO catalyst could accelerate the oxidation of ammonia-N and convert it to nitrate-N, promoting N 2 generation. Finally, the possible N transformation pathway in CSCWO of o -ClA was proposed. As a result, this work offers fundamental information about o -ClA catalytic oxidation removal in the SCWO process.
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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.
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Catalysis Science & Technology
·
2023
·Vol. 13
·期 14
·4156-4167
·
IF 5
Ji Feng,Lin Liu,Xiaohua Ju,Qike Jiang,Jiemin Wang,Jianping Guo,Teng He,Ping Chen
Utilization of promoters to improve the catalytic performance of supported metal catalysts is an important strategy for the design of efficient catalysts. However, it is difficult to detect the relationship between the promoters and the structure of main catalysts. Herein, we firstly develop an efficient Ru-based ammonia synthesis catalyst by decorating Ru nanoparticles (NPs) on γ-alumina with sub-nanometer ceria (CeO2) species (Ce–Ru/Al2O3). In comparison with neat Ru/Al2O3, Ce–Ru/Al2O3 exhibits up to 10-fold activity enhancement at 400 °C and 1.0 MPa. Our characterization results show that such an activity increment is relevant to the function of the sub-nanometer CeO2 species on the Ru NPs. The sub-nanometer CeO2 species will aggregate around the Ru nanoparticles, leading to a clear electron transfer from sub-nanometer CeO2 species to Ru nanoparticles. At the same time, the introduction of CeO2 species can not only weaken the hydrogen poisoning effect on the Ru nanoparticles but also facilitate nitrogen adsorption and hydrogenation of dissociated N* atoms according to the kinetic test results. This work highlights the important role of highly dispersed rare earth oxide promoter species in modulating the structure and catalytic performance of supported Ru NPs for ammonia synthesis.
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DALTON TRANSACTIONS
·
2023
·
IF 4
Yuanlei Huang,Mengdi Lv,Binglian Guo,Guojing Hu,Yong Qian,Zhi Su,Xuling Xue,Hong-Ke Liu
Breast cancer (BC) is one of the most common malignant tumors and often accompanied by inflammatory processes. Inflammation is an essential component of the tumor microenvironment, which might influence tumor proliferation and metastasis. Herein, three metal–arene complexes MA-bip-Ru, MA-bpy-Ir, and MA-bpy-Ru were prepared by tethering the non-steroidal anti-inflammatory drug meclofenamic acid (MA). Among them, MA-bip-Ru and MA-bpy-Ir showed lower cytotoxicity towards cancer cells, but MA-bpy-Ru showed significantly high selectivity and cytotoxicity towards MCF-7 cells through the autophagic pathway and exhibited no toxicity against normal HLF cells, showing potential for selective treatment of tumor cells. MA-bpy-Ru could also effectively destroy the 3D multicellular tumor spheroids, demonstrating its potential for clinical application. Besides, MA-bip-Ru, MA-bpy-Ir, and MA-bpy-Ru exhibited anti-inflammatory properties superior to MA, notably downregulating the expression of cyclooxygenase-2 (COX-2) and inhibiting the secretion of prostaglandin E2 in vitro. These findings demonstrated that MA-bpy-Ru was capable of intervening in inflammatory processes and showed the potential of MA-bpy-Ru to act as a selective anticancer agent, thus presenting a new mechanism of action for metal–arene complexes.
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JOURNAL OF NANOPARTICLE RESEARCH
·
2019
·Vol. 21
·期 2
·1-13
·
IF 2.009
Li Fang,Huang Haibao,Li Guisheng,Leung Dennis Y. C.
Highly ordered TiO 2 nanotube arrays (TiO 2 NTs) were synthesized by anodization method using a titanium foil and further modified with nanoparticles ( Ø = 2~10 nm) of three platinum group metals (that is, platinum, palladium, and ruthenium) through potentiostatic pulsed electrodeposition method to obtain the composite material. Compared with pure TiO 2 NTs, all the three composite samples (M-TiO 2 NTs, M = Pt, Pd, Ru) showed different enhancement effects on the light responses, as well as different photoelectrochemical performances. In this study, the performance of M-TiO 2 NTs, which worked as photoanode and cathode, was investigated. Ru-TiO 2 exhibited the best degradation yield (~ 85.8%) when applied as photoanode under visible light illumination, which indicated the platinum group metal could also be induced under visible irradiation, not just served as the co-catalyst. M-TiO 2 NTs as cathode were evaluated under the hydrogen evolution reaction (HER). The three M-TiO 2 NT electrodes showed an improved efficiency over pure TiO 2 NTs, while Pt-TiO 2 NTs performed even better (without any sacrificial agent) with higher Faradic efficiency than platinum electrode in the photoelectrocatalytic hydrogen production, which could be explained by the uniform and fine metal nanoparticles on the surface of TiO 2 NTs to offer abundant active sites for the reaction.
In this paper, TiO2 nanotube arrays loaded with nanoparticles of platinum group metals have been explored on their enhancement of photoelectrocatalytic activity. Platinum group metals served as co-catalyst in the surface of TiO2 nanotubes and show great variations in different reactions.
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Molecular Catalysis
·
2018
·
IF 0
Zhongzhe Wei,Xuefeng Li,Jiang Deng,Jing Wang,Haoran Li,Yong Wang
The catalytic transformation from levulinic acid (LA) into γ-valerolactone (GVL) is of great interest as it is an impressive strategy to convert lignocellulosic platform chemical into high value-added compounds. Herein, a novel heterogeneous catalyst made of Ru nanoparticles (NPs) supported on N-doped hierarchically porous carbon from biomass, Ru/NHPC, was shown to be highly active, selective and stable in this transformation. The reaction can proceed smoothly under mild conditions in aqueous media even at room temperature. The catalyst Ru/NHPC could be recycled for 13 consecutive runs exhibiting no obvious activity decay, much better than that of Ru NPs supported on activated carbon. The process offers an efficient, environmentally responsible, and safe approach to high production of GVL.
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Catalysts
·
2018
·Vol. 8
·期 8
·329
·
IF 3.465
Juntai Tian,Wen Wu,Zhenghua Tang,Yuan Wu,Robert Burns,Brandon Tichnell,Zhen Liu,Shaowei Chen
Developing bi-functional electrocatalysts for both oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER) is crucial for enhancing the energy transfer efficiency of metal–air batteries and fuel cells, as well as producing hydrogen with a high purity. Herein, a series of Pd–Ru alloyed nanoparticles encapsulated in porous carbon nanosheets (CNs) were synthesized and employed as a bifunctional electrocatalyst for both ORR and HER. The TEM measurements showed that Pd–Ru nanoparticles, with a size of approximately 1–5 nm, were uniformly dispersed on the carbon nanosheets. The crystal and electronic structures of the PdxRu100−x/CNs series were revealed by powder X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). The as-prepared samples exhibited effective ORR activity in alkaline media and excellent HER activity in both alkaline and acid solutions. The Pd50Ru50/CNs sample displayed the best activity and stability among the series, which is comparable and superior to that of commercial 10% Pd/C. For ORR, the Pd50Ru50/CNs catalyst exhibited an onset potential of 0.903 V vs. RHE (Reversible Hydrogen Electrode) and 11.4% decrease of the current density after 30,000 s of continuous operation in stability test. For HER, the Pd50Ru50/CNs catalyst displayed an overpotential of 37.3 mV and 45.1 mV at 10 mA cm−2in 0.1 M KOH and 0.5 M H2SO4, respectively. The strategy for encapsulating bimetallic alloys within porous carbon materials is promising for fabricating sustainable energy toward electrocatalysts with multiple electrocatalytic activities for energy related applications.Keywords:Pd–Ru alloys;porous carbon nanosheets;bifunctional electrocatalyst;oxygen electroreduction;hydrogen evolution reaction
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ELECTROCHIMICA ACTA
·
2018
·
IF 5.116
Nian Cao,Peng Zeng,Faqiong Zhao,Baizhao Zeng
A solid-state electrochemiluminescence (ECL) sensor for the highly selective and sensitive detection of 17β-estradiol (E2) is presented. The sensor is constructed with Ru(bpy) 3 2+ doped vinyl-SiO 2 nanoparticles (Ru@ethyl-SiO 2 ) and E2 imprinted polypyrrole (MIP). The Ru@ethyl-SiO 2 nanoparticles act as luminophores, while the MIP provides recognition sites for E2. As the adsorbed template molecules can act as co-reactant for Ru@ethyl-SiO 2 , the ECL intensity increases with the adsorption amount of E2 rising, which depends on its concentration in the solution. Owing to the well combination/or synergy of the smart MIP and the high-effective ECL material, the resulting sensor exhibits highly selective and ultrasensitive response to E2. Under the selected conditions, the ECL intensity increment (Δ I ) is linear to the logarithm of E2 concentration over the range from 0.01 to 100 pg mL −1 , and the detection limit is down to 0.005 pg mL −1 (S/N = 3). The ECL sensor also shows good reproducibility and repeatability. It has been successfully applied to the detection of E2 in tea and oral solution samples and the recoveries are 87.7%–115.3%.
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JOURNAL OF MATERIALS CHEMISTRY
·
2012
·Vol. 22
·期 18
·9117-9122
·
IF 5.968
Sha Chen,Hongye Zhang,Lingyan Wu,Yanfei Zhao,Changliang Huang,Maofa Ge,Zhimin Liu
Based on the galvanic replacement reaction between Cu nanoparticles and noble metal ions, a simple and efficient strategy was developed for the preparation of supported Cu–M (M = Pt, Pd, Ru, Rh) bimetallic nanoparticles under intense ultrasonication irradiation at ambient environment. A series of Cu–M/TiO2 bimetal catalysts with controllable composition, metal particle size less than 2 nm and narrow size distribution were obtained, and characterized by transmission electron microscopy (TEM), high resolution transmission electron microscope (HRTEM) with scanning TEM (STEM) mode, energy-dispersive X-ray spectrometers (EDS), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), and ICP-AES analysis. It was demonstrated that most of the metal particles were present in the form of bimetallic state. The mechanism of this strategy was discussed. The resultant Cu–Pd/TiO2 was used to reduce nitrate at room temperature, and it exhibited extremely high activity.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
·
IF 10.8
Zhisong Liu,Haomiao Xu,Yurui Fan,Wenjun Huang,Feng Yu,Zan Qu,Naiqiang Yan
Ruthenium single-atom catalysts have great potential in ammonia-selective catalytic oxidation (NH3–SCO); however, the stable sp3 hybrid orbital of NH3 molecules makes N(sp3)–H dissociation a challenge for conventional symmetrical metallic oxide catalysts. Herein, we propose a heterogeneous interface reverse atom capture strategy to construct Ru with unique asymmetric Ru1N2O1 coordination. Ru1N2O1/CeO2 exhibits intrinsic low-temperature conversion (T100 at 160 °C) compared to symmetric coordinated Ru-based (280 °C), Ir-based (220 °C), and Pt-based (200 °C) catalysts, and the TOF is 65.4 times that of Ag-based catalysts. The experimental and theoretical studies show that there is a strong d–p orbital interaction between Ru and N atoms, which not only enhances the adsorption of ammonia at the Ru1N2O1 position but also optimizes the electronic configuration of Ru. Furthermore, the affinity of Ru1N2O1/CeO2 to water is significantly weaker than that of conventional catalysts (the binding energy of the Pd3Au1 catalyst is −1.19 eV, but it is −0.39 eV for our material), so it has excellent water resistance. Finally, the N(sp3)–H activation of NH3 requires the assistance of surface reactive oxygen species, but we found that asymmetric Ru1N2O1 can directly activate the N(sp3)–H bond without the involvement of surface reactive oxygen species. This study provides a novel principle for the rational design of the proximal coordination of active sites to achieve its optimal catalytic activity in single-atom catalysis.
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Surfaces and Interfaces
·
2024
·
IF 5.7
Liming Zeng,Yongyang Zhu,Daifeng Wu,Dongxing Wang,Qing Zhou
The hydrogen evolution reaction (HER) in alkaline medium is much sluggish than that in acidic medium due to the limited water dissociation step, thus accelerating the water dissociation kinetics is critical. Herein, we designed a MoO x species-modified ruthenium nanoparticle catalyst (MoO x /Ru/C-3) based on the unique electrostatic interaction between carboxymethylcellulose sodium salt (CMC) and metal ions , where an heterophase structure is formed between MoO x and Ru. The obvious electronic interaction between them allows the formation of synergistic promotion relationship involving the water dissociation on MoO x and the adsorbed hydrogen recombination on Ru. At a metal loading of 6.98 μg Ru cm-2 geo, the overpotential of 82 mV is just required to reach a current density of 10 mA cm −2 , exhibiting a significantly better apparent electrochemical activity than Ru/C (98 mV) without introduction of MoO x , which demonstrates superior or comparable alkaline HER activity to the recently reported Ru-based electrocatalysts . Meanwhile, the overpotential for Ru/C increased by 113 mV after 24 h of chronopotentiometric test, whereas only 61 mV elevates for MoO x /Ru/C-3, and even just 98 mV generates after 120 h. Thereof, introduction of MoO x species into Ru matrix can also markedly improve the electrochemical stability. The proposed material construction strategy in this study provides a feasible idea for the rational design of highly cost-performance alkaline hydrogen evolution catalysts.
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