ChemSusChem
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2017
·Vol. 10
·期 8
·1720-1732
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IF 7.226
Zuojun Wei,Jiongtao Lou,Chuanmin Su,Dechao Guo,Yingxin Liu,Shuguang Deng
Graphical Stability through doping : The embedding of Ru nanoparticles in N-doped mesoporous carbon effectively improve the dispersion and decrease the average size of the Ru nanoparticles, improve the adsorption of levulinic acid, and increase the interaction between Ru and the support. The strategy prevents the Ru nanoparticles from migration, aggregation, and leaching, and consequently increases the reusability of the catalyst. To achieve a higher activity and reusability of a Ru-based catalyst, Ru nanoparticles were embedded in N-doped mesoporous carbon through a hard-template method. The catalyst showed excellent catalytic performance (314 h −1 turnover frequency) and recyclability (reusable five times with 3 % activity loss) for the hydrogenolysis of levulinic acid to γ-valerolactone. Compared with the mesoporous carbon without N-doping and conventional activated carbon, the introduction of N-dopant effectively improved the dispersion of Ru nanoparticles, decreased the average size of Ru nanoparticles to as small as 1.32 nm, and improved the adsorption of levulinic acid, which contributed to the increase in the activity of the catalyst. Additionally, the embedding method increased the interaction between Ru nanoparticles and carbon support in contrast with the conventional impregnation method, thus preventing the Ru nanoparticles from migration, aggregation, and leaching from the carbon surface and therefore increasing the reusability of the catalyst.
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Green Energy & Environment
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2024
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IF 10.7
Junming Zeng,Yongbin Yao,Fang Wang,Jiajian Gao,Lili Zhang,Guangwen Xu,Ziyi Zhong,Fabing Su
Nickle-based catalysts are commonly used for CO 2 methanation. However, there is still potential to improve their catalytic performance under mild conditions. In this study, we synthesized a series of Ru-Ni-Al catalysts from Ru-doped NiAl-hydrotalcite using a hydrothermal method. The Ru-Ni-Al catalyst demonstrated much higher activity for CO 2 methanation than the Ni-Al catalyst that did not have Ru doping. Both experimental results and theoretical calculations indicate that the enhanced performance of the Ru-Ni-Al catalyst is related to electronic interactions between nickel (Ni) and ruthenium (Ru). The Ru sites transfer electrons to the Ni sites, increasing the local electron density of Ni, which enhances the adsorption and activation of H 2 . Furthermore, the Ru-Ni metal interface sites improve the adsorption and activation of CO 2 . In situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) analysis indicates that adjusting the electronic structure of Ni sites can accelerate the production of intermediates HCOO*, while Ru-Ni intermetallic interface sites can directly dissociate CO 2 into CO*. In addition, CO 2 methanation on the Ru-Ni-Al catalyst follows HCOO*- and CO*-mediated pathways. This study underscores the potential for enhancing CO 2 methanation performance by modulating the electronic structure of Ni sites.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Junyu Zhang,Mingye Yang,Teng Huang,Jinwei Sun,Wenyu Hu,Yangyang Li,Fuyuan Yang,Minggao Ouyang
Hydrogen production from alkaline water electrolysis (AWE) has promising potential in energy storage due to the advantages of low cost and large scale, but its bottleneck is the low current density and poor durability of non-precious metal electrodes. Although numerous electrode designs with superior activity have been reported, the complicated synthesis process and refined microstructure have not changed the high preparation cost, high resistance, and poor durability of conventional AWE electrodes. Here, we report an efficient synthesis strategy of high-density Ni-Fe-Ru electrode (particle size < 5 nm) and explore the synergistic effect between Ni-Fe-Ru elements at different potentials. The electrode exhibits excellent OER activity (264 mV@100 mA cm −2 , Tafel slope = 49 mV dec −1 ) and AWE performance (400 mA cm −2 @1.89 V), it can work stably for 300 h at 500 mA cm −2 , with potential for industrial applications.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Dongfeng Sun,Pengpeng Qiang,Yuan Yu,Jingyun Zhang,Linyin Huang,Yanning Qu,Qingmei Su,Bingshe Xu
In this study, we meticulously prepared electrocatalysts in the form of Ru nanoclusters-decorated CoP nanowire arrays supported on carbon cloth (Ru@CoP/CC) for HER under both alkaline and acidic conditions. Ru@CoP/CC exhibited exceptional catalytic activity for hydrogen evolution, showcasing overpotentials of 48 mV and 66 mV (10 mA/cm 2 ) in acidic and alkaline media, respectively, which closes to 20% of commercial Pt/C catalysts. Moreover, they showcased outstanding durability, a crucial aspect for their practical application in hydrogen production. Furthermore, this research employed DFT computations to attain a comprehensive understanding of the electronic and structural modifications brought about by the integration of Ru nanoclusters. Ru nanoclusters could coordination environment of CoP, and then effectively accelerate the catalytic reaction. This method opens up a new way to reduce the amount of precious metals in the electrocatalyst, and is helpful to the development of high-performance HER electrocatalyst.
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ADVANCED FUNCTIONAL MATERIALS
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2024
·
IF 18.5
Junge Yang,Jinxian Feng,Youpeng Cao,Yuxuan Xiao,Lulu Qiao,Keyu An,Jiao Yang,Jing Peng,Hui Pan,Hui-Ming Cheng
An efficient and stable electrocatalyst is key for the production of green hydrogen using water electrolysis. However, the weak dissociation ability of Pt-based catalysts, resulting in slow kinetics severely hampers its applications in alkali medium. Herein, a simple “coincident reduction” strategy is reported to grow highly dispersed Ru-Pt heterogeneous bimetallic nanoparticles on reduced graphene oxide (Ru x Pt y @rGO) for efficient pH-universal hydrogen evolution. Ru x Pt y @rGO has superior catalytic activity at all pH values due to the synergistic effect between Ru and Pt and the ultra-small nanoparticle. In particular, the catalyst with 13.6 wt% of noble metal (Ru 1 Pt 2 @rGO) has low overpotentials of 9, 6, and 36 mV at 10 mA cm −2 in 1 m KOH, 0.5 m H 2 SO 4 and 1 m phosphate buffer solution (PBS), respectively, which outperformances monometallic counterparts and comparable to the best bimetallic catalysts ever reported. The catalyst is highly stable because of the strong bonding between the bimetallic nanoparticle and rGO. Mechanism studies show that Ru 1 Pt 2 @rGO has a faster Volmer–Tafel mechanism in alkali, high-efficient H + transfer and increased H adsorption ability in acid, resulting in superior reaction kinetics. This work provides a new route for mass production of high-performance catalysts for practical applications at all pH values.
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JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Weitao Ou,Han Wang,Yingdan Ye,Huaiyuan Zhao,Yibin Zhang,Zhaoyin Hou
Chemical upcycling of waste polyethylene terephthalate (PET) to value-added products can reduce the emission of CO 2 , microplastics and toxic chemicals. In this work, mesoporous H-type Zeolite Socony Mobil-5 (HZSM-5) supported Ru catalyst (Ru/ m -HZSM-5) was synthesized and tested in the hydrogenation of PET degraded chemicals (bis(2-hydroxyethyl) terephthalate , dimethyl terephthalate, diethyl terephthalate, and terephthalic acid). Characterizations disclosed that Ru/ m -HZSM-5 catalyst possesses mesopores (a dominant channel of 5.32 nm), enlarged specific surface area (404 m 2 ·g −1 ), and Ru NPs dispersed highly (40.6 %) compared to that of Ru/HZSM-5. And also, it was found that Ru/ m -HZSM-5 was capable for the hydrogenation of benzene rings in these PET degraded chemicals with large sizes (1.09–1.82 nm). In particular, the conversion of BHET and the selectivity of BHCD over Ru/ m -HZSM-5 reached 95.5 % and 95.6 % at 120 °C within 2 h. And Ru/ m -HZSM-5 could be recycled at least five times without obvious loss of activity and selectivity.
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ANALYTICAL LETTERS
·
2024
·
IF 1.6
Jiali Ju,Qiaoyu Ding,Jianwei Xie,Guixin Li
A graphene oxide-Ru(bpy)32+-polyaniline-nanocomposite (GO-Ru(bpy)32+-PANI) was prepared to develop a sensitive label-free electrochemiluminescence (ECL) immunosensor for mucoprotein 1 (MUC1). Ru(bpy)32+ and PANI were decorated together on graphene oxide for the first time. The GO-Ru(bpy)32+-PANI material was characterized by scanning electron microscopy (SEM), absorption spectroscopy, Fourier transform infrared spectroscopy (FTIR), fluorescence, electrochemical impedance spectroscopy (EIS), and ECL. The GO-Ru(bpy)32+-PANI exhibited excellent stability. The ECL immunosensor for MUC1 was fabricated by covalently immobilizing anti-MUC1 upon GO-Ru(bpy)32+-PANI modified indium-doped tin oxide (ITO) electrode. In the presence of MUC1, a decrease of ECL was observed due to the formation of the anti-MUC1/MUC1 complex. The immunosensor showed a linear relationship from 1 × 10−13 to 1 × 10−7 mg/mL with a detection limit of 8.2 × 10−14 mg/mL. The immunosensor was applied to the determination of MUC1 in human serum.
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ELECTROCHEMISTRY COMMUNICATIONS
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2011
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IF 4.287
Kai Zeng,Manli Guo,Yingjun Zhang,Meng Qing,Afang Liu,Zhou Nie,Yan Huang,Yuliang Pan,Shouzhuo Yao
A novel method based on click chemistry for the immobilization of Ru(bpy) 3 2+ derivative on electrode to fabricate a solid state electrochemiluminescence (ECL) sensor was reported. Pentenyl functionalized Ru(bpy′) 3 Cl 2 was synthesized and immobilized on a (3-mercaptopropyl) trimethoxysilane (MPTMS) pretreated indium tin oxide (ITO) substrate via thiol-ene click chemistry reaction between its alkenyl group and the sulfhydryl group of MPTMS. The immobilization method is simple, fast, and efficient. More importantly, the resulting Ru(bpy′) 3 2+ monolayer film exhibited excellent stability in organic solvent, which is superior to many previously reported methods. Using tri- n -propylamine (TPrA) as a model analyte, the ECL sensor gave a wide linear range over 5 × 10 − 6 to 5 × 10 − 3 M, with a satisfactory detection limit of 1 × 10 − 6 M ( S / N = 3).
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MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Zhi Luo,Jing Li,Shenglan Hu,Lingling Zheng,Lixin Xu,Biyang Deng
In this study, Ru(bpy) 3 2+ and oxalate (C 2 O 4 2− ) in Ru@Zn-MOF generated self-enhanced electrochemiluminescence (ECL). The self-enhanced ECL composite exhibited a short electron transfer distance and minimal energy loss, which ensured the high and stable luminescence efficiency of Ru@Zn-MOF. A MnO 2 @AuNPs nanocomposite was introduced into Ru@Zn-MOF via antigen–antibody interactions in the presence of squamous cell carcinoma antigen (SCCA). This significantly quenched the ECL signal due to the combined effect of the dual quenchers, MnO 2 NFs and AuNPs. A highly efficient ECL-RET immunosensor was constructed for the sensitive detection of SCCA in the linear range of 1 fg/mL to 100 ng/mL, with a limit of detection of 0.26 fg/mL (S/N = 3). This immunosensor has broad clinical applications for the quantitative detection of biomarkers.
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Molecular Catalysis
·
2024
·
IF 3.9
Dongyang Yang,Bingxiao Feng,Hongxin Wang,Qingjuan Xie,Yaping Liu,Hengjun Gai,Hongbing Song
Selective oxidation of alcohols to aldehydes by molecular oxygen is one of the most important transformations in multiphase catalysis. In this paper, a catalyst with selective oxidation ability was designed and synthesized for the selective catalytic oxidation of benzyl alcohol. N-doped carbon materials were prepared by high-temperature calcination using hydrothermal reaction products of citric acid and melamine as a carbon source, and a bimetallic catalyst supported by Ru-CeO 2 was constructed using the mixture as the carrier for the selective oxidation of benzyl alcohol to benzaldehyde. The results showed that the introduction of CeO 2 could effectively improve the oxidizing ability and catalytic activity of the catalyst. The Ru-Ce 0.05 /NC170–600 catalyst was able to convert 85.5 % benzyl alcohol into benzaldehyde at 140 °C, 6 h, and 2 MPa, and the selectivity for benzaldehyde was 100 %. It was demonstrated by DFT that it was theoretically feasible to generate benzaldehyde by extracting hydrogen atoms from benzyl alcohol molecules. Further, the selective oxidation experiments on other alcohols showed that the catalyst has high activity for the oxidation of various alcohols to generate the corresponding carbonyl products, and it is a catalyst with broad-spectrum selective oxidation ability. In this study, a green synthesis route of benzaldehyde was proposed to solve the problems in the traditional process. Meanwhile, it provides a new idea for the synthesis of carbonyl products by selective oxidation of alcohols.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2024
·
IF 5.8
Shunxiang Wang,Sen Hu,Cuili Xiang,Yongjin Zou,Fen Xu,Ningbo Qin,Lixian Sun
Pt/C is currently widely utilized as a catalyst for electrolytic hydrogen production. However, the high cost of Pt-based catalysts limits further development. Therefore, developing an efficient, highly stable, and cost-effective catalyst is crucial. In this study, we enhanced the ability to activate H 2 O and the performance of the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) by incorporating a small amount of Ru into NiFeAl-layered double hydroxides (LDHs), thereby altering the electrochemical active surface area and the catalysts’ internal resistance. The catalyst demonstrated excellent catalytic activity in alkaline electrolytes, achieving low overpotentials of 33 mV at 10 mA cm −2 and 278 mV at 50 mA cm −2 . Furthermore, it demonstrated outstanding stability for up to 240 h; the catalyst was successfully assembled into a solar-powered hydrogen production system via full-water-splitting testing, thus providing more possibilities for electrolytic hydrogen production.
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Acta Pharmaceutica Sinica B
·
2024
·
IF 14.7
Jie Shan,Xu Jin,Cong Zhang,Muchen Huang,Jianghao Xing,Qingrong Li,Yuyu Cui,Qiang Niu,Xu-lin Chen,Xianwen Wang
Bacterial infection hampers wound repair by impeding the healing process. Concurrently, inflammation at the wound site triggers the production of reactive oxygen species (ROS), causing oxidative stress and damage to proteins and cells. This can lead to chronic wounds, posing severe risks. Therefore, eliminating bacterial infection and reducing ROS levels are crucial for effective wound healing. Nanozymes, possessing enzyme-like catalytic activity, can convert endogenous substances into highly toxic substances, such as ROS, to combat bacteria and biofilms without inducing drug resistance. However, the current nanozyme model with single enzyme activity falls short of meeting the complex requirements of antimicrobial therapy. Thus, developing nanozymes with multiple enzymatic activities is essential. Herein, we engineered a novel metalloenzyme called Ru-procyanidin nanoparticles (Ru-PC NPs) with diverse enzymatic activities to aid wound healing and combat bacterial infections. Under acidic conditions, due to their glutathione (GSH) depletion and peroxidase (POD)-like activity, Ru-PC NPs combined with H 2 O 2 exhibit excellent antibacterial effects. However, in a neutral environment, the Ru-PC NPs, with catalase (CAT) activity, decompose H 2 O 2 to O 2 , alleviating hypoxia and ensuring a sufficient oxygen supply. Furthermore, Ru-PC NPs possess exceptional antioxidant capacity through their superior superoxide dismutase (SOD) enzyme activity, effectively scavenging excess reactive oxygen species (ROS) and reactive nitrogen species (RNS) in a neutral environment. This maintains the balance of the antioxidant system and prevents inflammation. Ru-PC NPs also promote the polarization of macrophages from M1 to M2, facilitating wound healing. More importantly, Ru-PC NPs show good biosafety with negligible toxicity. In vivo wound infection models have confirmed the efficacy of Ru-PC NPs in inhibiting bacterial infection and promoting wound healing. The focus of this work highlights the quadruple enzymatic activity of Ru-PC NPs and its potential to reduce inflammation and promote bacteria-infected wound healing.
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