Science Bulletin
·
2025
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IF 21.1
Qingyu Wang,Yangyang Wan,Qichen Liu,Yida Zhang,Zhentao Ma,Zirui Xu,Pengting Sun,Gongming Wang,Hai-Long Jiang,Wenping Sun,Xusheng Zheng
Photocatalytic urea production from nitrogen (N 2 ) and carbon dioxide (CO 2 ) is a sustainable and eco-friendly alternative to the Bosch-Meiser route. However, it remains a significant challenge in developing highly efficient photocatalysts for enhancing C-N coupling to high-yield urea synthesis. Herein, we propose a multi-site photocatalyst concept to address the concern of low yield by simultaneously improving photogenerated carrier separation and reactant activation. As a proof of concept, a well-defined multi-site photocatalyst, Ru nanoparticles and Cu single atoms decorated CeO 2 nanorods (Ru-Cu/CeO 2 ), is developed for efficient urea production. The incorporation of Ru and Cu sites is crucial not only to generate high-density photogenerated electrons, but also to facilitate N 2 and CO 2 adsorption and conversion. The in situ formed local nitrogen-rich area at Ru sites increases the encounter possibility with the carbon-containing species generated from Cu sites, substantially promoting C-N coupling. The Ru-Cu/CeO 2 photocatalyst exhibits an impressive urea yield rate of 16.7 μmol g −1 h −1 , which ranks among the best performance reported to date. This work emphasizes the importance of multi-site catalyst design concept in guaranteeing rapid C-N coupling in photocatalytic urea synthesis and beyond.
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ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Kunjie Wang,Yanan Li,Dongxu Yang,Yunsi Wang,Fuan Wei,Bingxin Liu,Peng Zhang,Benhua Xu,Yongcheng Li
Coupling noble metals on molybdenum disulfide (MoS 2 ) has emerged as a promising strategy for triggering inert basal plane and boosting hydrogen evolution reaction (HER) performances. Herein, ultrafine Ru nanoparticles (NPs) are decorated on vertical 2H MoS 2 nanosheets via a facile hydrothermal method. Benefiting from new active site centers triggered by ultrafine Ru NPs and vertically grown 2H MoS 2 nanosheets on carbon cloth (CC), Ru 0.15 @2H MoS 2 exhibits impressive HER performances in dual pH media, with low overpotentials of 20 and 111 mV and small Tafel slope of 67.6 and 76.3 mV dec ‑1 in alkaline and acid solutions to drive a current density of 10 mA cm -2 . DFT calculation results prove that ultrafine Ru NPs decorated on 2H MoS 2 nanosheets endow Ru 0.15 @2H MoS 2 with low hydrogen adsorption free energy and fast charge transfer kinetics. This work provides an effective and simple method for designing MoS 2 -based catalysts with high catalytic activity to decorate precious metal in a wide pH medium.
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CATALYSIS LETTERS
·
2024
·
IF 2.3
Yan Xiaoxu,Zhao Xianfeng,Shao Xinxin,Li Kangpeng,Sun Minghong,Ji Xinpeng,Lu Huidan,Liu Yongping
Platinum-group metal ruthenium (Ru) is considered an ideal substitute for platinum (Pt) in the hydrogen evolution reaction (HER) due to its excellent electrocatalytic performance and cost that is 20 times lower than Pt. Herein, we prepared Ru-doped WO 3 nanosheets array on carbon cloth (CC) using the hydrothermal method, followed by successful high-temperature nitridation to obtain Ru-WN/CC nanoarray electrocatalysts. As prepared Ru-doped WN nanosheets exhibit a highly porous structure, providing abundant active sites for HER. Electrochemical performance tests demonstrate that compared to pristine WN/CC, 7% Ru-WN/CC exhibits a reduced overpotential of 94 mV at a current density of 10 mA cm -2 , with a Tafel slope of only 51.4 mV dec -1 and an Rct of 6.08 Ω. Moreover, it maintains high catalytic activity for at least 24 hours under acidic conditions. The superior electrocatalytic activity of Ru-WN/CC is attributed to the significant acceleration of the kinetic rate of WN electrocatalysts by Ru doping, the reduction of electronic transfer resistance in WN, and the enlargement of the electrochemically active surface area of WN. This study provides an important reference for the development of novel low noble metal-doped electrocatalytic materials and has guiding significance for the application of metal nitrides in water splitting for hydrogen production. Graphical Abstract
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FUEL
·
2024
·
IF 6.7
Riyang Shu,Long Xie,Bin Hu,Zhipeng Tian,Chao Wang,Ying Chen,Ying Xu
Methanol steam reforming for hydrogen production is a highly promising energy technology, due to the high hydrogen intensity of methanol and the appendant hydrogen capture from water. In order to reinforce the hydrogen yield in methanol steam reforming reaction, a series of Ru-based carbon-coated CeO 2 catalysts were prepared in this work, using glucose, cellulose and activated carbon as different carbon sources via a hydrothermal method. The results showed that the Ru/C G -CeO 2 (glucose) catalyst exhibited a superior catalytic performance at the reaction temperature of 400 °C, with a higher hydrogen production rate (0.276 mol/h) than Ru/C C -CeO 2 (cellulose, 0.230 mol/h) and Ru/C A -CeO 2 (activated carbon, 0.253 mol/h) catalysts. This was attributed to the synergistic effect between CeO 2 and carbon, where the carbon layer formed by glucose enhanced the interaction between the active component and the CeO 2 support, which also facilitated the electron transfer effects and resulted in a large amount of oxygen vacancies for Ru/C G -CeO 2 . This led to a strong adsorption capacity for CO and oxygen-containing species derived from the substrate, thereby improving hydrogen production. Additionally, the catalyst stability and the resistance to carbon deposition were evaluated for all the three catalysts, and Ru/C G -CeO 2 catalyst also demonstrated a superior stability and anti-carbon deposition capability.
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AICHE JOURNAL
·
2025
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IF 4
Hao Huang,Nadia N. Intan,Jialin Tan,Zidi Liu,Da Zhang,Xiaolan Cai,Min Zhuang,Shaoqu Xie
Strong metal-support interaction (SMSI) significantly influences the catalytic activity, selectivity, and stability through the geometric and electronic effects of a catalyst. We herein develop a stable Ru 0 −Mo δ+ catalyst for the hydrodeoxygenation (HDO) of fatty acids to alkanes (2.5 μmol g −1 cat h −1 ) at low to room temperatures, meanwhile demonstrating its general applicability to various complex fatty acids. Kinetic studies and reaction pathway analysis revealed that the Ru–Mo SMSI significantly reduced the reaction activation energy by altering the HDO pathways. Mechanistic studies indicate that electron transfer occurs between the active Ru nanoclusters and the Mo δ+ support, which enhances catalytic activity by promoting the adsorption of RCOO* at the Ru 0 −Mo δ+ interface. Our research establishes an efficient Ru–Mo catalyst for biomass upgrading at low temperatures and calls for reassessing the electronic effects in the M 0 -M δ+ interfacial catalysis model.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2025
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IF 7.7
Zhenjie Zheng,Jingxuan Wang,Mengqi Ma,Yunpeng Xu,Da Huang,Jian Wang,Cuiying Lin,Zhenyu Lin,Fang Luo
Sensitive and selective detection of N -nitrosodimethylamine (NDMA), a highly carcinogenic environmental contaminant, is essential for public health and safety. In this study, we have developed a homogeneous electrochemiluminescence (ECL) biosensor for ultrasensitive NDMA detection by integrating Nafion-functionalized covalent organic framework (COF) with aptamer recognition and magnetic separation. The imine-linked COF (COF-LZU1) scaffold not only enables stable encapsulation of Ru(bpy) 3 2 + , but also creates a confined microporous environment that locally concentrates c (TPrA) and enhances the generation and survival of TPrA radicals, thereby amplifying the ECL signal. Nafion further improves Ru loading and ionic conductivity. Biotinylated aptamers were initially immobilized on streptavidin-coated magnetic beads (MBs) and hybridized with complementary DNA-modified Ru@COF-LZU1 to form Ru@COF-LZU1-MBs complex. Upon NDMA binding, a conformational switch releases Ru@COF-LZU1 into the solution. After magnetic separation, the ECL signal of the supernatant is measured in the presence of TPrA. This homogeneous format avoids electrode surface modification, which is commonly required in conventional Ru@COF-LZU1-based ECL sensors, offering improved reproducibility and simplified operation. The biosensor exhibits a wide linear range (100 fg/mL - 100 ng/mL) with a low detection limit of 9.11 fg/mL. This platform offers a sensitive, reproducible, and facile strategy for monitoring NDMA and similar small-molecule contaminants in complex matrices.
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ACTA MATERIALIA
·
2025
·
IF 9.3
Yuhua Liu,Qing Liang,Fuxi Liu,Wenwen Li,Aofei Wei,Tiantian Xu,Xu Zou,Bingsen Zhang,Wei Zhang,Weitao Zheng
It remains a significant challenge for simultaneously regulating the water dissociation and hydrogen adsorption/desorption of Ru in alkaline media. Herein, we successfully architected an entity of individually-functionalized spatial valence-asymmetric Ru sites on Ru/TiO 2 quantum dots for high-performance alkaline hydrogen evolution. The Ru nanoclusters were self-adaptively grown along the Ti vacancies, triggering the phase transformation from anatase to rutile TiO 2 . The well-defined Ru/TiO 2 interface produced a strong electronic metal-support interaction, acquiring a Ru site with asymmetric electronic state. Resultantly, the anisotropy of the surface low-valence Ru δ- site and the interface high-valence Ru δ+ site break the scaling relationship of water dissociation, hydroxyl and hydrogen adsorption. The asymmetrical Ru electronic state achieves 15 mV overpotential at 10 mA cm -2 and delivers a high mass activity of 5.4-fold than commercial Pt/C at 100 mV, outperforming most reported Ru-based catalysts. Our work sheds light on the potential of support-crystal phase engineering to design catalysts with the required electrocatalytic performance.
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CHINESE JOURNAL OF CATALYSIS
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2024
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IF 15.7
Adel Al-Salihy,Ce Liang,Abdulwahab Salah,Abdel-Basit Al-Odayni,Ziang Lu,Mengxin Chen,Qianqian Liu,Ping Xu
The potential of sustainable hydrogen production technology through water splitting necessitates the rational design of oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) bi-functional electrocatalysts . In this context, we initially synthesized and empirically evaluated ultralow Ru-doped NiMoO 4 @Ni 3 (PO 4 ) 2 core-shell nanostructures on nickel foam (Ru-NiMoO 4 @Ni 3 (PO 4 ) 2 /NF). The hydrous NiMoO 4 nanopillars were hydrothermally grown on NF, followed by successive RuCl 3 etching and subsequent phosphorylation processes, leading to the final Ru-NiMoO 4 @Ni 3 (PO 4 ) 2 /NF. The catalyst demonstrated impressive HER overpotential values of −14.8 and −57.1 mV at 10 and 100 mA cm −2 , respectively, with a Tafel slope of 35.8 mV dec −1 . For OER at 100 mA cm −2 , an overpotential of 259.7 mV was observed, with a Tafel slope of 21.6 mV dec −1 . The cell voltage required for overall water splitting was 1.43 V at 10 mA cm −2 and 1.68 V at 100 mA cm −2 . Moreover, the catalyst exhibited superior stability for 150 h, emphasizing its practical utility for long-term applications. Subsequent density functional theory calculations aligned with these empirical findings, indicating a low water dissociation energy barrier (Δ G b = 0.46 eV), near-zero free adsorption energy for HER (Δ G *H = 0.02 eV), and suitable free adsorption energy for OER (Δ G *OOH − Δ G *OH = 2.74 eV), alongside a high density of states near the Fermi level . These results, informed by both experimental evaluation and theoretical validation, highlight the potential of Ru-NiMoO 4 @Ni 3 (PO 4 ) 2 /NF as a high-performance catalyst for water splitting, setting a solid foundation for advancements in sustainable energy technologies.
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ACS Applied Bio Materials
·
2025
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IF 4.7
Dong Fan,Zhongyu Wang,Xingyi Yuan,Shixue Luo,Runsi Zhan,Weiyu Hu,Huitong Chen,Weiwen Wang,Jing Liu,Zongming Wang,Xin Wang
Aims Nonfunctioning pituitary adenomas (NFPAs) are a common intracranial tumor in clinical practice, and currently available treatments for NFPA include surgical resection and radiotherapy. However, this is due to the relatively high risk of recurrence and persistent side effects of these therapies. As a local treatment, photodynamic therapy (PDT) shows promise in solid tumors through spatiotemporally controlled cytotoxicity. The aim of this study was to investigate the mechanism of action of photosensitizer Ru2 in NFPA. Materials and methods [Ru(tpy)(tpy-Br)] (PF6)2 was synthesized from Ru(tpy)Cl3, and further synthesized into Ru2. Cell viability of Light+Ru2 or Dark+Ru2 was assayed using the CCK-8 assay and live–dead cell staining. RNA-seq of Light+Ru2-treated PDFS cells yielded differentially expressed genes. The expression of PI3K/ATK/P53 was detected using qPCR, Western blot. PI3K agonist 740Y–P and AKT agonist SC79 were added for further pathway validation. The effect of PDT on PDFS cell viability by 3D multicellular tumor spheroids (MCTSs) was evaluated. Key findings We untangle that Ru2-PDT specifically activates the p53 pathway and inhibits PI3K/AKT phosphorylation in PDFS cells. Under 595 nm illumination, Ru2 activates p53 and induces cell cycle arrest in the G0/G1 phase. Simultaneously, Ru2-PDT significantly suppressed the phosphorylation of the PI3K/AKT signaling pathway. Further investigation reveals that the PI3K/AKT agonist treatment partially inhibits p53 expression, alleviates Ru2-PDT-induced apoptosis, and reverses its inhibitory effects on PDFS cell migration and invasion. Significance This study, for the first time, elucidates the molecular mechanism of Ru2-PDT targeting the PI3K/AKT/p53 signaling axis, providing a theoretical basis for the clinical treatment of nonfunctioning pituitary adenomas.
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Biosensors-Basel
·
2024
·Vol. 14
·期 10
·512
·
IF 4.9
Jiawen Fan,Junjie Qi,Jingkun Li,Fuwei Pi
Arginine has been widely applied in the food industry as coloring agents, flavoring agents, and nutritional fortifiers. It is also one of the major components of feed additives. Currently, methods for the highly selective detection of arginine remain absent. For accurate and sensitive detection of L−arginine, a novel ratiometric fluorescence assay based on Ru@UiO-66-NH2was developed and demonstrated in this study. Under optimized detection conditions, the limit of detection (LOD) of this assay for L-arginine was 2.32 μM, which is superior to most assays reported to date. Meanwhile, Ru@UiO-66-NH2showed good stability within 30 days, demonstrating the wide applicability of the proposed assay. The spike-and-recovery rates of the proposed assay for L-arginine in real samples (e.g., tea, grape juice, and serum) were 84.27–113.09%. Overall, the proposed assay showed high sensitivity, good reproducibility, and excellent stability in the detection of L-arginine in both buffer and real samples.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2024
·
IF 3.9
Rimei Huang,Huimin Qiu,Congcong Pang,Liqun Li,Aihui Wang,Shichen Ji,Hong Liang,Xing-Can Shen,Bang-Ping Jiang
Graphical The integration of multiple bioactivated chemical reactions in situ and receptor-mediated targeting characteristics can alleviate deep tumor tissue hypoxia for improving tumor-specific phototherapy. Hypoxia is a critical factor for restricting photodynamic therapy (PDT) of tumor, and it becomes increasingly severe with increasing tissue depth. Thus, the relief of deep tumor hypoxia is extremely important to improve the PDT efficacy. Herein, tumor microenvironment (TME)-responsive size-switchable hyaluronic acid-hybridized Ru nanoaggregates (HA@Ru NAs) were developed via screening reaction temperature to alleviate deep tumor hypoxia for improving the tumor-specific PDT by the artful integration multiple bioactivated chemical reactions in situ and receptor-mediated targeting (RMT). In this nanosystem, Ru NPs not only enabled HA@Ru NAs to have near infrared (NIR)-mediated photothermal/photodynamic functions, but also could catalyze endogenous H 2 O 2 to produce O 2 in situ . More importantly, hyaluronidase (HAase) overexpressed in the TME could trigger disassembly of HA@Ru NAs via the hydrolysis of HA, offering the smart size switch capability from 60 to 15 nm for enhancing tumor penetration. Moreover, the RMT characteristics of HA ensured that HA@Ru NAs could specially enter CD44-overexpressed tumor cells, enhancing tumor-specific precision of phototherapy. Taken together these distinguishing characteristics, smart HA@Ru NAs successfully realized the relief of deep tumor hypoxia to improve the tumor-specific PDT.
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RENEWABLE ENERGY
·
2024
·
IF 9
Qian Zhang,Weijia Guo,Yushan Yang,Shunyu Shen,Xin Chen,Kai Shao,Zhenjie Wang,Qingfeng Sun,Caicai Li
Highly active, stable and affordable hydrogen evolution reaction (HER) electrocatalysts are intensively needed for global energy conversion systems. Carbon-supported ruthenium (Ru)-based electrocatalysts have been rising stars in recent years and the pursuit of higher activity has arisen intensive research interest. Herein, a novel electrocatalyst with cellulose nanofibers containing abundant carboxyls and hydroxyls as the carbon source to anchor Ru nanoparticles (Ru/NC) was designed and synthesized. Benefiting from the anchoring and dispersion of the carbon substrate to the Ru nanoparticles and the synergistic interaction between the different components, the obtained Ru/NC exhibited optimal HER activity in all the corresponding contrast electrocatalysts, with low overpotentials of 16 mV, 22 mV, and 46 mV to attain 10 mA cm − - 2 in 1.0 M KOH, 0.5 M H 2 SO 4 and 1.0 M KOH + seawater, respectively. Further, the Tafel slope of Ru/NC in alkaline seawater indicated that its HER process followed a Volmer-Tafel mechanism. Additionally, the synthesized Ru/NC also displayed excellent stability in different electrolytes. This work will provide a novel and interesting insight into the fabrication of advanced carbon-supported electrocatalysts with resource-rich biomass as cost-effective carbon source.
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