INORGANIC CHEMISTRY
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2024
·
IF 4.3
Xiaowei Fu,Qichang Li,Hongdong Li,Weiping Xiao,Zhenyu Xiao,Guangrui Xu,Dehong Chen,Zexing Wu,Lei Wang
Transition-metal phosphides (TMPs) have attracted extensive attention in energy-related fields, especially for electrocatalytic hydrogen evolution reaction (HER). However, it is imperative to develop a facile and time-consuming approach to prepare metal phosphides with satisfactory catalytic performance. Herein, nitrogen-doped CoP-Co2P decorated with Ru (Ru/N-CoP-Co2P) is synthesized (Ru/N-CoP-Co2P) through a hydrothermal route and following an ultrafast and simple microwave avenue within 20 s. The achieved Ru/N-CoP-Co2P possesses an interconnected porous morphology to expose abundant active sites and accelerate the mass transport. Moreover, N doping and Ru-supported decorated Ru/N-CoP-Co2P also play a key role in promoting the electrocatalytic activity. Therefore, the as-designed Ru/N-CoP-Co2P presents good catalytic performance for the HER in a wide pH range. Ru/N-CoP-Co2P merely needs overpotentials of 63, 100, and 65 mV to obtain 10 mA cm–2 in acidic, alkaline, and seawater electrolytes. This research provides a novel and efficient strategy for the synthesis of TMPs with highly efficient catalytic activity.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Hua Jin,Linjian Yu,Kun Xiong,Jia Chen,Haidong Zhang,Min Deng,Xueqing Shi
Efficient hydrogen production by water electrolysis is primarily restrained by imperfect over-potential and poor reaction dynamics on oxygen evolution reaction (OER). Thermodynamically favourable urea oxidation reaction (UOR) is a class of promising routes for substituting sluggish OER and for coupling with cathodic hydrogen production because of smaller equilibrium potential (0.37 V) than that of OER (1.23 V). Herein, a versatile Ru-NiO/p-Ni catalyst was prepared through in-situ generating nickel hydroxide nanosheets on the surface of ordered porous Ni, then doping low Ru and annealing treatment. The optimized Ru-NiO/p-Ni displayed outstanding activity and stability towards hydrogen evolution reaction (HER), OER and UOR with potentials of −0.13 V, 1.57 V, and 1.39 V at 100 mA cm −2 , respectively. Ru-NiO/p-Ni‖Ru-NiO/p-Ni can achieve 100 mA cm −2 in urea-aided water splitting at a voltage of only 1.58 V, which is prominently 170 mV smaller than the voltage of water electrolysis (1.75 V). The excellent electrocatalytic performance is owing to the outstanding inherent activity generated by cooperative effect of Ru and NiO, along with rich defect and active centre of Ru-NiO/p-Ni supplied by the large surface area of 3D porous structure. The formation of more rich Ni active species with a high valence through transport of electrons between Ru and Ni is favourable to promoting the dissociation of urea molecules, eventually improving UOR. Therefore, it can facilitate urea-aided water splitting, which provides a valuable strategy for constructing versatile catalysts for a cathodic energy-efficient hydrogen production coupled with other anodic oxidation reactions.
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JOURNAL OF POWER SOURCES
·
2017
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IF 6.395
Jingbo Yang,Hongwei Mi,Shan Luo,Yongliang Li,Peixin Zhang,Libo Deng,Lingna Sun,Xiangzhong Ren
Flexible Li-O 2 batteries have attracted worldwide research interests and been considered to be potential alternatives for the next-generation flexible devices. Nitrogen-doped carbon nanofibers (N-CNFs) prepared by electrospinning are used as flexible substrate and an amorphous TiO 2 layer is coated by atomic layer deposition (ALD) and then decorated with Ru nanoparticles . The Ru/N-CNFs@TiO 2 composite is directly used as a free-standing electrode for Li-O 2 batteries and the electrode delivers a high specific capacity, improved round-trip efficiency and good cycling ability. The superior electrochemical performance can be attributed to the amorphous TiO 2 protecting layer and superior catalytic activity of Ru nanoparticles. Based on density functional theory (DFT) calculations from first principles, the carbon electrode after coating with TiO 2 is more stable during discharge/charge process. The analysis of Li 2 O 2 on three different interfaces (Li 2 O 2 /N-CNFs, Li 2 O 2 /TiO 2 , and Li 2 O 2 /Ru) indicates that the electron transport capacity was higher on Ru and TiO 2 compared with N-CNFs, therefore, Li 2 O 2 could be formed and decomposed more easily on the Ru/N-CNFs@TiO 2 cathode. This work paves a way to develop the free-standing cathode materials for the future development of high-performance flexible energy storage systems .
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ACS Catalysis
·
2025
·
IF 13.1
Kaijie Han,Song Song,Yong You,Xiaoqia Fu,Xingang Li
Ru-based catalysts are widely used for the reductive amination of carbonyl compounds. However, challenges remain, particularly in achieving high catalytic activity under mild conditions. In this study, we report a strategy to simultaneously modulate the electron density of Ru0 and the RuOx/Ru0 ratio by systematically adjusting the calcination temperature. The catalyst calcined at 200 °C demonstrated remarkable performance, achieving a 97.8% yield of furfurylamine at 30 °C, significantly outperforming most previously reported catalysts. Furthermore, it showed compatibility with a range of carbonyl compounds. At 200 °C calcination, the reduced electron density of Ru0 weakened its electron-donating ability, thereby facilitating H2 activation. Meanwhile, this treatment yielded the highest RuOx content and thereby generated the greatest Lewis acid site density, enhancing the adsorption and activation of NH3, furfural, and the Schiff base. Mechanistic studies reveal that the synergistic effect between electron-deficient Ru0 and Lewis acid sites significantly reduced the apparent activation energy for the ammonolysis of Schiff base intermediates, the rate-determining step in reductive amination. This work provides an effective strategy for tuning both the electronic structure of the metal and the acid properties of the catalyst, highlighting the crucial role of metal-acid synergy in promoting Schiff base ammonolysis during reductive amination.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Yingxue Du,Qichang Li,Linping Han,Pengfei Yang,Liantao Xin,Wei Jin,Weiping Xiao,Zhenjiang Li,Jinsong Wang,Zexing Wu,Lei Wang
Designing efficient and robust pH-universal electrocatalysts for hydrogen evolution reaction (HER) is the key to boost the development of eco-friendly hydrogen energy. Herein, metallic Mo, Ru coupled with graphitic carbon dots (GQDs) activate inertness 1D copper-based nanowires (GQDs@ Ru, Mo-Cu 2 O/CF) by surface chemical oxidation, solvothermal and low temperature calcination . The metals of Mo, Ru favor the water-dissociation and optimize the hydrogen adsorption/desorption. In addition, GQDs owns edge effect and good conductivity, and then benefiting electron transport and active sites exposure. Therefore, the synthesized GQDs@ Ru, Mo-Cu 2 O/CF requires only 30, 39, 17 and 55 mV in alkaline, acidic, alkaline seawater and neutral to achieve 10 mA cm −2 . Moreover, the assembled electrolyzer requires 1.58 V to reach 10 mA cm −2 in alkaline seawater, and maintained well at 200 mA cm −2 for 100 h. This research opens a new avenue for designing efficient catalysts on energy-relation applications through introducing both metal and non-metal.
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FREE RADICAL BIOLOGY AND MEDICINE
·
2021
·
IF 7.376
Zhu-Ying Yan,Jing Chen,Jie Shao,Ze-Qing Jiao,Tian-Shu Tang,Miao Tang,Zhi-Guo Sheng,Li Mao,Rong Huang,Chun-Hua Huang,Zhi-Hui Zhang,Hong-Mei Su,Ben-Zhan Zhu
Developing the cell-impermeable Ru(II) polypyridyl cationic complexes as effective photosensitizers (PS) which have high cellular uptake and photo-toxicity, but low dark toxicity, is quite challenging. Here we found that the highly reactive singlet oxygen ( 1 O 2 ) can be generated by the irradiation of a typical Ru(II) polypyridyl complex Ru(II)tris(tetramethylphenanthroline) ([Ru(TMP) 3 ] 2+ ) under visible light irradiation by ESR with TEMPO (2,2,6,6-tetramethyl-4-piperidone- N -oxyl) as 1 O 2 probe. Effective cellular and nuclear delivery of cationic [Ru(TMP) 3 ] 2+ was achieved through our recently developed ion-pairing method, and 2,3,4,5-tetrachlorophenol (2,3,4,5-TeCP) was found to be the most effective among all chlorophenols tested. The accelerated cellular, especially nuclear uptake of [Ru(TMP) 3 ] 2+ results in the formation of 8-oxo-7,8-dihydro-2′-deoxyguanosine (8-oxodG) and DNA strand breaks, caspase 3/7 activation and cell apoptosis in HeLa cells upon light irradiation. More importantly, compared with other traditional photosensitizers, [Ru(TMP) 3 ] 2+ showed significant photo-toxicity but low dark toxicity. Similar effects were observed when 2,3,4,5-TeCP was substituted by the currently clinically used anti-inflammatory drug flufenamic acid . This represents the first report that the cell-impermeable Ru(II) polypyridyl complex ion-paired with suitable lipophilic counter-anions functions as potent intracellular photosensitizer under visible light irradiation mainly via a 1 O 2 -mediated mechanism. These findings should provide new perspectives for future investigations on other metal complexes with similar characteristics as promising photosensitizers for potential photodynamic therapy.
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CATALYSIS TODAY
·
2018
·
IF 4.667
Qianqian Huang,Weiqiang Yu,Fang Lu,Rui Lu,Xiaoqin Si,Jin Gao,Jie Xu
Metal nanoparticles catalysts are widely used in hydrogenation of carboxylic acids and their derivatives, which are significant reactions to produce high-value compounds such as alcohols and lactones. These reactions were usually carried out in liquid phase at harsh conditions with high temperature and pressure, however, catalysts deactivation frequently occurred since small metal NPs were inclined to migrate and aggregate as well as dissolve and leach in such acid systems. Thus, it’s a great challenge to prepare catalysts with highly dispersed small metal NPs with good stability and durability. Herein we propose a novel one-pot co-synthesis method to prepare highly dispersed and stabilized nanometal catalysts that small Ru NPs embedded in carbon species coated on silica nanospheres. Ru precursors were doped directly in the synthesis of RF coated silica spheres along with the polymerization of resorcinol–formaldehyde, and following the process of carbothermal reduction. Aqueous hydrogenation of itaconic acid was used as a probe reaction, which could produce high-value products such as methylsuccinic acid and methyl butyrolactone. The as-prepared catalysts had uniform dispersion of small Ru NPs with core-shell structure of resin coated silica nanospheres, exhibited good hydrogenation activity and stability with no obvious loss of yield for methyl butyrolactone and less sintering in recycling tests.
研究领域:
催化化学
·
材料科学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Wei Zhang,Jialu Wei,Jiafeng Zhu,Chunwen Sun
Due to its abundant resources and advantages in transportation and storage, methane fueled solid oxide fuel cells (SOFCs) are highly needed. In this work, an exceptional internal reforming catalyst comprising in-situ exsolved NiRu bimetallic nanoparticles and oxygen-deficient layered double perovskite LaBaMn 1.6 Ni 0.3 Ru 0.1 O 5+δ (r-LBMNR) was prepared. Compared to the cell with LaBaMn 1.6 Ni 0.4 O 5+δ (r-LBMN) catalyst, the cell with a Ru-doping r-LBMNR catalyst layer, exhibits superior peak power output of 336 mW cm −2 and better durability with a less decay rate of 0.014% per hour in CH 4 fuel. The enhanced electrochemical performance can be attributed to the high oxygen ion and electron conductivities of the catalyst and the coupling of Ni and Ru sites with the oxygen-deficient r-LBMNR matrix This coupling activates CH 4 and H 2 O, promotes the oxidation of C atoms in CH 4 molecules, and enables reversible hydrogen spillover, ultimately leading to the production syngas of CO(g) and H 2 (g).
研究领域:
材料科学
·
能源科学
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Materials Today Physics
·
2026
·
IF 9.3
Wenjing Zhang,Yong Yuan,Xiaolong Li,Zhixin Liao,Xiaohua Zhang,Cuicui Du,Jinhua Chen
While alkaline water electrolysis represents a highly promising and sustainable pathway for hydrogen production, its widespread application is hindered by the sluggish kinetics of the hydrogen evolution reaction (HER) due to a large energy barrier for water dissociation. In this work, a heterogeneous electrocatalyst of Ru/MoC-Mo 2 C@NC was prepared by uniformly embedding ruthenium nanoparticles within a nitrogen-doped carbon matrix hosting MoC-Mo 2 C heterojunctions. (MoC-Mo 2 C@NC). Electrochemical experimental results demonstrate the remarkably boosted HER catalytic performance of Ru/MoC-Mo 2 C@NC compared with Ru/NC, Ru/MoC@NC and Ru/Mo 2 C@NC by presenting the lowest overpotential of 18.5 mV at 10 mA cm −2 and Tafel slope of 61.71 mV·dec −1 , along with superior intrinsic activity and mass specific activity. Density-functional theory calculations further reveal that the enhanced electronic metal-support interaction (EMSI) between Ru sites and the MoC-Mo 2 C@NC support in Ru/MoC-Mo 2 C@NC induces significant charge redistribution and interface charge accumulation in Ru/MoC-Mo 2 C@NC, thereby optimizing water dissociation energy barrier and hydrogen adsorption free energy (ΔG H∗ ). Meanwhile, this reinforced EMSI facilitates efficient reverse hydrogen spillover at the Ru/MoC-Mo 2 C@NC interface, which further favors water dissociation on Mo sites and hydrogen desorption on Ru sites of Ru/MoC-Mo 2 C@NC. These regulating effects collectively accelerate the hydrogen intermediate transport and enhance the overall HER kinetics. This work provides valuable insights into enhanced electronic metal-support interaction on a heterostructure catalytic system optimizing both water dissociation and reverse hydrogen spillover for designing highly efficient water electrolysis catalysts.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2021
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IF 4.464
Muhammad Saqib,Shahida Bashir,Sajjad Ali,Rui Hao
Developing highly specific, rapid, and cost-effective electrochemiluminescence (ECL) methods capable of detecting multiple analytes remains a compelling research goal but it is still a substantial challenge due to narrow choice of ECL systems. In this study, efficient ECL detections were achieved by using anodic Ru(bpy) 3 2+ -acridine orange (AO) ECL system. In present system, dimethylamino substituent on acridine ring acts as active sites for strong ECL generation, while heterocyclic nitrogen atom (–N–) contributes to specific complex formation with metal ion. Accordingly, this anodic ECL method was exploited for highly sensitive detection of both mercury (II) (Hg 2+ ) and dopamine (DA), with detection limits as low as 0.36 nM (linear range 0.01–50 μM) and 1.0 nM (linear range 0.01–10 μM), respectively. The mechanism of Hg 2+ detection was supported by density functional theory (DFT) calculations. Notably, the ECL method exhibit superior selectivity over numerous competing interfering agents. Moreover, the method achieved the detection of both targets in practical media with excellent recoveries (96.0–103.8%). Importantly, the method demonstrates potential advantages in terms of selectivity, sensitivity, rapidity, simplicity, and low cost. This work realizes a successful attempt to further expand the analytical applications of ECL systems and may initiate new thoughts in utilizing acridines in diverse ECL-based sensing and imaging applications.
研究领域:
分析化学
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环境科学
·
生物医学
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高影响因子
ChemistrySelect
·
2023
·Vol. 8
·期 5
·e202204363
·
IF 2.1
Tingting Xu,Panpan Xu,Guilin Xu,Mengyao Liu,Yinggui Zhu
Graphical In the study, Ru(bpy) 3 2+ was used as the luminophore, HEPES buffer was served as the co-reactant, and ATP was added to the system to amplify the luminous signal. It was speculated that ATP acts as an co-reaction accelerator to promote the oxidation of HEPES to HEPES + ⋅, more HEPES⋅ can be generated, which then reacts with oxidized Ru(bpy) 3 3+ to emit stronger ECL signals. Moreover, I - consumes ATP, Ru(bpy) 3 2+ , and HEPES, leading to a decrease in ECL signal. Adenosine triphosphate is an important biological molecule that provides energy and substrate for various cellular biochemical processes,it's ubiquitous in our lives. In this work, a novel electrochemiluminescence (ECL) sensor composed of Ru(bpy) 3 2+ , 2-[4-(2-hydroxyethyl)piperazin-1-yl] ethanesulfonic acid (HEPES) and adenosine 5’-triphosphate disodium salt (ATP) was developed for the first time. In this ECL system, Ru(bpy) 3 2+ was used as the luminophore, HEPES buffer was served as the co-reactant, and ATP was added to the system to amplify the luminous signal to investigate the ECL behavior. Through fluorescence spectroscopy, ECL spectroscopy, and cyclic voltammetry (CV), it can be hypothesized that the possible ECL mechanism is that ATP acts as an advanced co-reaction promoter to accelerate the oxidation of HEPES to HEPES + ⋅, more HEPES⋅ can be generated, which then reacts with oxidized Ru(bpy) 3 3+ to emit stronger ECL signals. Subsequently, the influence of the ATP concentrations and the CV scanning speed was investaged. Moreover, it was observed that I − could quench the ECL intensity, the linear relationship range of I − concentration is from 10 −3 to 10 −6 m , the limit of detection is 3.7×10 −8 m (signal/noise=3), therefore, a new, highly sensitive, and selective ECL approach for I − detection was created.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Tiantian Feng,Zhijie Cui,Pengfei Guo,Xuehong Wang,Juan Li,Xien Liu,Wenpin Wang,Zhongcheng Li
Tailoring surface composition and structures of catalysts affects their catalytic performance in hydrogen evolution reaction owing to the geometric and electronic effects. Herein, Ru nanoparticles embedded in 2D N-doped carbon nanosheets decorated with 2D Fe 3 O 4 –Fe 3 C heterostructures (Ru/Fe 3 O 4 –Fe 3 C/NC) are fabricated via pyrolysis of the mixture containing 2D-Fe 2 O 3 nanosheets, dopamine hydrochloride , RuCl 3 ·xH 2 O, and melamine . Interestingly, the good hydrogen evolution behavior is achieved on Ru/Fe 3 O 4 –Fe 3 C/NC with the high reactivity and stability. Ru/Fe 3 O 4 –Fe 3 C/NC offers an overpotential of 141 mV to realize the current density of 10 mA/cm 2 in 0.5 mol/L (M) H 2 SO 4 electrolyte. As for 1 M KOH, Ru/Fe 3 O 4 –Fe 3 C/NC promotes hydrogen evolution reactivity with 148 mV to achieve 10 mA/cm 2 . The current density slightly degrades after continuous I-t tests, verifying the good stability for Ru/Fe 3 O 4 –Fe 3 C/NC. The high reactivity might stem from high dispersion of Ru nanoparticles, enhanced conductivity due to doping N into carbon nanosheets, and heterointerfaces between Fe–O and Fe–C.
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