ChemElectroChem
·
2022
·Vol. 9
·期 3
·e202101482
·
IF 4.782
Hao Cui,Min Jiang,Gang Tan,Jianping Xie,Pengfei Tan,Jun Pan
Graphical Ru-CoP/CC electrocatalyst for hydrogen evolution was synthesized through simple in-situ hydrothermal and gas phosphatized treatments, which only needs 44 mV to reach 10 mA cm −2 , exceeding many reported electrocatalysts. Meanwhile, the reason and the result of electrons redistribution after Ru doping were deeply investigated. Exploring highly efficient, durable and low-cost catalysts for hydrogen evolution reaction (HER) is crucial to promoting the development of electrochemical water splitting systems but remains challenging. In this work, the Ru-modified CoP nanoflakes on carbon clothes (Ru-CoP/CC) are fabricated via an in-situ hydrothermal method, followed by low-temperature phosphatized treatments. According to X-ray photoelectron spectroscopy (XPS) measurements, the Ru doping induces the electron deviation from Ru to Co−P, and makes Co ions be an electron-rich state. It is revealed that the introduction of Ru can effectually reconstruct the electron coordination environment of Co−P. The resultant Ru-CoP/CC catalyst shows outstanding HER performance with an ultralow overpotential of 45 mV at 10 mA cm −2 . Moreover, the obtained catalyst exhibits long-term durability at 20 mA cm −2 for 20 h in the alkaline solution. This work opens a new avenue to lower the usage of noble metal in electrocatalyst and helps to developing a high-performance electrocatalyst for HER.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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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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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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ENERGY CONVERSION AND MANAGEMENT
·
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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Journal of Materials Chemistry B
·
2023
·
IF 7
Huiting Hu,Han-Feng Cui,Xia Yin,Qiqi Fan,Hai Shuai,Jing Zhang,Sheng Fu Liao,Wei Xiong,Dong he Jiang,Hao Fan,Wenming Liu,Guobing Wei
A dual-mode fluorescence and electrochemiluminescence (FL-ECL) sensor for apoE gene detection has been designed, harnessing the distinct properties of Ruthenium Metal Organic Framework Nanosheets (RuMOFNSs). The strategy capitalizes on the quenching effect of the Ru(bpy)₃²⁺ ECL signal by ferrocene, facilitating the creation of a multi-electron electrical signal marker known as bisferrocene. Through anchoring the P-DNA onto RuMOFNSs, bisferrocene effectively quenches both FL and ECL emissions. Introduction of the T-DNA, and the subsequent formation of double-stranded DNA, allows the ExoⅢ enzyme to remove the bisferrocene fragment, rejuvenating the signals. Impressively, the sensor boasts expansive detection linear ranges (1 fM to 1 nM for FL; 0.01 fM to 10 pM for ECL) and exceptional sensitivity (0.048 fM for FL; 0.016 fM for ECL). Its dual-mode framework grants heightened reliability via a self-validation mechanism, mitigating the occurrence of false positives. When juxtaposed with single-mode sensors, this dual-format exhibits marked superiority. Field tests further validate the sensor's efficacy in genuine sample analysis, highlighting its potential in precursory disease detection. This avant-garde methodology paves the way for advanced multi-signal responsive sensors, with profound implications for the future of diagnostic instruments.
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ELECTROCHIMICA ACTA
·
2023
·
IF 6.6
Jin Lin,Hong Wang,Chao Wang,Li Guo,Yanzhong Wang
Metal-organic frameworks (MOFs) are considered as prospective electrocatalysts for water splitting due to their adjustable pore structure and abundant active sites. However, the rational design of MOFs with excellent oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) performances is still an enormous challenge. Herein, Ru-doped nickel thiophene dicarboxylic acid (Ni-TDA)/nickel foam (NF) were prepared via a one-pot solvothermal method , and their morphologies and electronic structures can be facilely modulated by Ru doping contents. The as-prepared self-supporting Ni 5 Ru-TDA/NF with Ni/Ru molar ratio of 5:1 show the excellent OER and HER activities with low overpotentials of 235 and 35 mV at a current density of 10 mA cm −2 in 1 M KOH, respectively. Furthermore, Ni 5 Ru-TDA/NF indicate the remarkable stability during the process of OER and HER with the slight decrease after the stability test of 60 h. The excellent electrocatalytic activities can be attributed to high intrinsic activity of multiple Ru species, the synergistic effect of Ru and Ni sites and abundance active sites in Ru-doped Ni-TDA. The water electrolysis system using Ni 5 Ru-TDA/NF as the anode and cathode, respectively, can achieve a current density of 10 mA cm −2 with a cell voltage of only 1.53 V, which is promising for practical applications.
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ACS Nano
·
2023
·
IF 17.1
Chan Guo,Yunxiang Tang,Zhengyi Yang,Tingting Zhao,Jiurong Liu,Yufei Zhao,Fenglong Wang
Carbon dioxide (CO2) hydrogenation to methane (CH4) is regarded as a promising approach for CO2 utilization, whereas achieving desirable conversion efficiency under mild conditions remains a significant challenge. Herein, we have identified ultrasmall Ru nanoparticles (∼2.5 nm) anchored on MnCo2O4 nanosheets as prospective photothermal catalysts for CO2 methanation at ambient pressure with light irradiation. Our findings revealed that MnCo2O4 nanosheets exhibit dual functionality as photothermal substrates for localized temperature enhancement and photocatalysts for electron donation. As such, the optimized Ru/MnCo2O4-2 gave a high CH4 production rate of 66.3 mmol gcat–1 h–1 (corresponding to 5.1 mol gRu–1 h–1) with 96% CH4 selectivity at 230 °C under ambient pressure and light irradiation (420–780 nm, 1.25 W cm–2), outperforming most reported plasmonic metal-based catalysts. The mechanisms behind the intriguing photothermal catalytic performance improvement were substantiated through a comprehensive investigation involving experimental characterizations, numerical simulations and density functional theory (DFT) calculations, which unveiled the synergistic effects of enhanced charge separation efficiency, improved reaction kinetics, facilitated reactant adsorption/activation and accelerated intermediate conversion under light irradiation over Ru/MnCo2O4. A comparison study showed that, with identical external input energy during the reaction, Ru/MnCo2O4-2 had a much higher catalytic efficiency compared to Ru/TiO2 and Ru/Al2O3. This study underscores the pivotal role played by photothermal supports and is believed to engender a heightened interest in plasmonic metal nanoparticles anchored on photothermal substrates for CO2 methanation under mild conditions.
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JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Yiwen Zou,Lin Dong,Siyang Yan,Jiaxu Liu,Lili Mu,Licheng Li,Yue Hu,Haifeng Qi,Shanjun Mao,Zupeng Chen
Efficient and selective N -alkylation of amines with alcohols via transfer hydrogenation is of great significance but extremely challenging. Here, we report the production of N –benzylaniline (BZA) from benzyl alcohol and aniline over various fine-shaped Ru/CeO 2 catalysts. The Ru/CeO 2 –R (rod) catalyst exhibits the highest catalytic activity among all catalysts, in which the yield of BZA reaches up to 88% with complete conversion, significantly higher than that of Ru/CeO 2 -C (cube, 52%) and Ru/CeO 2 -O (octahedron, 32%). Extensive experimental investigations disclose that Ru nanoparticles with a metallic state promote the dehydrogenation of the hydroxyl group and hydrogenation of imines, while the CeO 2 –R with rich oxygen vacancies facilitates the adsorption and activation of reactants. Furthermore, kinetic studies and time-resolved operando dual-beam Fourier transform infrared spectroscopy analysis confirms the transfer hydrogenation pathway, in which the benzyl alcohol is firstly dehydrogenated to benzaldehyde, followed by spontaneously reacting with aniline, and finally transforms into the N -benzylaniline rapidly.
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MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Kaida Kuang,Ya Li,Yu Ji,Yang Liu,Nengqin Jia
In this work, a quenched molecularly imprinting-electrochemiluminescence (MIP-ECL) sensor based on Ru(bpy) 3 2+ @ZnO-Au nanocomposites was constructed to realize the sensitive detection of acrylamide (AM). Ru(bpy) 3 2+ @ZnO-Au nanomaterials show high ECL efficiency. AuNPs has excellent properties and can improve the properties of electrochemiluminescence by promoting the electron transfer process of the luminescent body. The MIP polymer film was formed on the surface of the material and eluted with eluent, leaving an AM imprinting cavity as a specific recognition site. When adding different concentrations of AM, it was specifically recognized by the MIP membrane, and the ECL signal decreased gradually, thus realizing the sensitive detection of AM. Under the optimal conditions, the detection ranges of the MIP-ECL sensor are 1–10 8 nM and the limit of detection (LOD) is 0.123 nM. Therefore, this sensor proposed in this work opens up a new way for the sensitive detection of AM in food.
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CHINESE JOURNAL OF CATALYSIS
·
2023
·
IF 16.5
Ce Han,Bingbao Mei,Qinghua Zhang,Huimin Zhang,Pengfei Yao,Ping Song,Xue Gong,Peixin Cui,Zheng Jiang,Lin Gu,Weilin Xu
Regulation of the atomic distribution is crucial for the development of atomically dispersed electrocatalysts. In this study, atomic Ru coordinated by channel ammonia in V-doped tungsten bronze (Ru/V-NHWO, Ru 0.44 wt%, V 0.45 wt%) was used as a high-performance catalyst for the hydrogen evolution reaction (HER), demonstrating remarkable mass activity in a wide pH range. Atomic Ru with a regulated spatial distribution and electronic structure was achieved owing to its unique coordination with the ammonia species in the hexagonal channels of V-NHWO. V doping in NHWO led to enhanced intrinsic activity and conductivity. Theoretical calculations revealed that the multichannel, vertically integrated Ru sites in the V-doped channels, as well as the coexisting Ru sites without multichannels or V-doping, improved the free energy of water dissociation and hydrogen sorption , which boosted the HER activity. Our study paves a new way for constructing atomically dispersed materials with a regulated spatial distribution for diverse applications.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Yizhong Zou,Wen-Da Zhang,Ming Chen,Jiangyong Liu,Zhi-Guo Gu,Xiaodong Yan
The influence of the preorganized structure and chemical composition of metal-organic frameworks (MOFs) on the morphology, surface properties, and catalytic activity of the MOFs-derived metal oxides is yet to be revealed. In this work, two types of Co-MOFs with different coordination configurations are synthesized for the preparation of the structure-engineered ruthenium (Ru)-doped cobalt oxides. The effect of the preorganized coordination structure of the MOFs on the morphology and surface properties is investigated. Interestingly, the oxalate-based MOFs derived Ru-doped cobalt oxide (OX-Co 3 O 4 -Ru) exhibits much better surface wettability and more oxygen vacancies than the zeolitic imidazolate framework-67 derived Ru-doped cobalt oxide. As expected, the OX-Co 3 O 4 -Ru owns excellent catalytic properties towards both hydrogen evolution reaction and oxygen evolution reaction with an overpotential of 49 and 286 mV, respectively at a current density of 100 mA cm −2 in 1.0 M KOH. Importantly, the bifunctional OX-Co 3 O 4 -Ru catalyst offers an extremely high current density of 500 mA cm −2 at a cell voltage of 1.71 V for overall water splitting and as well demonstrates robust working stability.
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Catalysis Science & Technology
·
2020
·Vol. 10
·期 21
·7302-7308
·
IF 5.721
Libing Fan,Tian Meng,Qun Li,Dewen Wang,Zhicai Xing,Erkang Wang,Xiurong Yang
Ruthenium (Ru)-based materials have been proven to be highly efficient hydrogen evolution reaction (HER) electrocatalysts and have become the most promising candidates for replacing platinum (Pt)-based electrocatalysts. Herein, we report an easily scalable electrospinning strategy to construct nitrogen-doped carbon nanofibers with porous hierarchical structures and uniformly dispersed Ru nanoparticles (abbreviated as ES-Ru-ZIF-900). Benefiting from the porous fibrous nanoarchitecture caused by the pyrolysis of the zeolitic imidazolate framework-8, the abundant firmly immobilized Ru NPs, and the high conductivity of the N-doped carbon matrix, the resultant ES-Ru-ZIF-900 electrocatalyst exhibits an extraordinary HER performance. ES-Ru-ZIF-900 only needs an overpotential of 21 mV to drive the current density of 10 mA cm−2, and possesses long durability for over 14 h in 1.0 M KOH, superior to Pt/C and most of the non-Pt based electrocatalysts. This work offers a universal and efficient synthetic strategy for preparing metal-based nitrogen-doped carbon hybrid catalysts with enhanced HER activity.
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