查找使用阿拉丁产品的科研文献

Local Charge Density Regulation of NiP2 Nanosheets via Ru Doping for Electrocatalytic Urea Oxidation

Jingrui Jian,Yi Qiao,Fengyi Chen,Changhao Liu,Wangxi Liu,Zhonghua Li,Mingyu Pi,Zhaosheng Li,Zhigang Zou

The substantial discharge of urea-rich wastewater presents a significant threat to the ecological environment. The electrocatalytic urea oxidation reaction (UOR) represents an efficient and environmentally sustainable approach for urea degradation, with its low thermodynamic potential suggesting considerable potential to supplant the oxygen evolution reaction (OER) in energy-efficient hydrogen production from water electrolysis. Although nickel-based catalysts show considerable promise for UOR, the high energy barrier associated with the formation of Ni 3+ remains an obstacle for the reaction. Here, a Ru-doped NiP 2 nanosheet array (NiP 2 -Ru) catalyst was constructed for UOR. The experimental results indicate that Ru doping modulates the local charge distribution of NiP 2 , thereby increasing the oxidation state of Ni. This modification facilitates the formation of highly active Ni 3+ sites, which substantially enhances the UOR activity of NiP 2 . The NiP 2 -Ru catalyst demonstrates exceptional UOR performance, requiring an overpotential of only 0.95 and 0.99   V to achieve a current density of 10 and 100   mA   cm −2 with a low Tafel slope of 11.27   mV dec –1 , respectively, in a 1   m KOH solution containing 0.33   m urea, which is comparable to the best reported UOR activity. Furthermore, the catalyst exhibits an excellent stability for over 100   h. This research proposes a viable strategy for the design and synthesis of effective UOR electrocatalysts and advocates further exploration of the application of transition metal phosphides in various environmental and energy-related domains.

Ru doped graphitic carbon nitride mediated peroxymonosulfate activation for diclofenac degradation via singlet oxygen

Ying Yan,Qinxue Yang,Qigao Shang,Jing Ai,Xiaofang Yang,Dongsheng Wang,Guiying Liao

Metals doped carbon nitride (CN) is considered as a class of promising efficient catalysts for peroxymonosulfate (PMS) activation in water purification. Herein, ruthenium doped carbon nitride (CNRu) was synthesized via a facile one-pot method, and CNRu was in form of Ru–N 2 that could efficiently activate PMS for DCF degradation and detoxification via nonradical pathway. DCF was completely removed within 10 min under the optimized condition in a wide working pH range of 3.00–9.00, while other traditional transition metals (e.g. Fe, Co, Ni, Cu) doped CN showed negligible removal of DCF due to adsorption rather than activation of PMS, which was demonstrated by DFT calculations. CNRu showed high stability and reusability after seven cycles and very few Ru leaching was detected in DCF degradation process. Ru was highly dispersed in form of Ru–N bond via coordinating to pyridine nitrogen, and the electron defect transfer between Ru and coordinated N, rather than redox cycle of Ru, mediated superoxide radicals (O 2 •− ) evolution, which was further hydrolyzed into singlet oxygen ( 1 O 2 ) and responsible for DCF removal. Thus, the CNRu/PMS system showed high tolerance to inorganic anions. Much lower toxic intermediates/products than DCF were obtained via the strong electrophilic attack reaction between 1 O 2 and DCF in CNRu/PMS system. This study displayed a new practical application prospect of ruthenium-based materials for high-efficient removal and detoxification of DCF from wastewater.

Oxygen vacancies enriched Nb-WOX supported Ru for polychlorinated aromatics oxidation: Reaction mechanism exploration

Shuai Yang,Yifeng Chen,Haiwei Guo,Xunzhu Jiang,Jiawen Ma,Xinyang Li,Zhao Chen,Xiaodong Ma

The current catalysts for polychlorinated aromatics (PCAs) oxidation showed either poor low-temperature catalytic activity, low mineralization ability or bad stability, and developing oxygen vacancies enriched catalysts with abundant acid sites is a potential solution for the above drawbacks. Herein, oxygen vacancies enriched Nb-WO X were developed for o -DCB ( o -dichlorobenzene, a PCAs model compound) oxidation, and they showed notably better low-temperature catalytic activity with T 50% <350 °C than did commercial WO 3 (T 50% >400 °C) under the WHSV of 36000 mL g −1 h −1 . Nb-WO X supported Ru exhibited even lower T 50% (173 °C) and T 90% (238 °C), as well as high CO X yield with >99% ratio of CO 2 to CO and good stability (>99% conversion for 500 mins) when with 1.5 wt% Ru loading at 300 °C. The above phenomenon was attributed to the abundant oxygen vacancies and acid sites in Nb-WO X that contributed to the better redox property, stronger interaction with Ru species and the removal of accumulated chloride. The o -DCB oxidation mechanism revealed that the higher CO 2 ratio to CO on Ru/Nb-WO X arose from the deep oxidation of CO byproducts. The work described here will instruct us to degrade PCAs effectively through catalysts design.

Site-Selective Polyolefin Hydrogenolysis on Atomic Ru for Methanation Suppression and Liquid Fuel Production

Mingyu Chu,Xianpeng Wang,Xuchun Wang,Xiangxi Lou,Congyang Zhang,Muhan Cao,Lu Wang,Youyong Li,Sibao Liu,Tsun-Kong Sham,Qiao Zhang,Jinxing Chen

Catalytic hydrogenolysis of end-of-life polyolefins can produce value-added liquid fuels and therefore holds great promises in plastic waste reuse and environmental remediation. The major challenge limiting the recycling economic benefit is the severe methanation (usually >20%) induced by terminal C–C cleavage and fragmentation in polyolefin chains. Here, we overcome this challenge by demonstrating that Ru single-atom catalyst can effectively suppress methanation by inhibiting terminal C–C cleavage and preventing chain fragmentation that typically occurs on multi-Ru sites. The Ru single-atom catalyst supported on CeO2 shows an ultralow CH4 yield of 2.2% and a liquid fuel yield of over 94.5% with a production rate of 314.93 gfuels gRu−1 h−1 at 250 °C for 6 h. Such remarkable catalytic activity and selectivity of Ru single-atom catalyst in polyolefin hydrogenolysis offer immense opportunities for plastic upcycling.

Ultralow Loading Ru-Mo2C on CNT Boosting High Durability Electrocatalyst for Oxygen Reduction Reaction

Jiangshan Gao,Tongtong Lian,Huanhuan Wang,Zhiming Liu,Yan He

The high cost and low stability of Pt-based oxygen reduction reaction (ORR) catalysts have limited their commercial applications. In this paper, we report the microwave synthesis of ultralow loading Ru-Mo2C on carbon nanotubes (CNT) as ORR catalysts to alleviate these above disadvantages. Ru-Mo2C@CNT exhibited excellent oxygen reduction reaction activity with a half-potential of 0.87 V and an onset potential of 0.94 V. It has high stability and palmary anti-methanol capability in alkaline electrolytes. This Ru-Mo2C@CNT may be a promising alternative to Pt-based electrocatalysts in energy conversion and storage.

Slightly carbon-coated defective TiO2-supported Ru catalysts for ethylene methoxycarbonylation to methyl propionate

Chen Jiabing,Lu Zijing

Ostwald ripening (OR) and particle migration and coalescence (PMC)-induced sintering of metal nanoparticles remains a major challenge in heterogeneous catalysis. In the methoxycarbonylation of ethylene, noble metals such as Ru and Pd serve as active centers, yet inevitable metal aggregation during the reaction reduces both the number of active sites and catalyst lifetime. Herein, we report a highly efficient Ru catalyst supported on defect-rich TiO 2 with slight carbon coating for ethylene methoxycarbonylation. Systematic characterizations reveal that the thin carbon layer effectively suppresses OR, while appropriate metal–support interactions prevent PMC. The synergistic effect of these features maximizes the exposure of Ru 0 active sites, enhancing catalytic activity and stability. The catalyst achieves a remarkable reaction rate of 13.18 mol/mol Ru /h and a selectivity of 99% toward methyl propionate, outperforming previously reported Ru-based catalysts. Furthermore, the catalyst retains over 90% of its activity after five consecutive cycles. This work provides a new strategy for designing robust and highly active catalysts for heterogeneous ethylene methoxycarbonylation.

Ultralow Ru loaded CoNi bimetallic phosphides nanorods as efficient electrocatalyst for overall water splitting

Yantong Long,Guoliang Zhao,Liuxin Yang,Yuxuan An,Yongjun Xu,Chen Xu

Efficient hydrogen/oxygen evolution reactions (HER/OER) bifunctional catalysts are critical to the overall water splitting efficiency. In this paper, a 1D rod-like structure bifunctional catalyst was firstly prepared, with ultralow Ru (1.19 wt%) loaded into CoNi bimetallic phosphides derived from 1D MOF-74-CoNi nanorods . Due to the strong interface interaction between Co and Ni bimetals which tunes the electronic structure and the Ru loading which increases the number of active sites of the catalyst, the electrocatalytic performance for both HER (8.7mV@10 mA cm −2 ) and OER (179.4mV@10 mA cm −2 ) under alkaline condition were significantly improved. The cell voltage of the full water splitting device assembled by the catalysts was only 1.47 V to achieve 10 mA cm −2 . The rational materials design of 1D rod-like structured bimetallic phosphide catalysts in this work may suggest a new strategy for the preparation of other bifunctional electrocatalysts .

Enriched electrophilic oxygen species facilitate acidic oxygen evolution on Ru-Mo binary oxide catalysts

Wang Yaya,Wen Yunzhou,Cheng Yumeng,Chen Xinhong,Zhuansun Mengjiao,Wang Tongbao,Li Jun,Meira Debora,Sun Huarui,Wei Jun,Zhou Jia,Wang Yuhang,He Sisi

The polymer electrolyte membrane (PEM) electrolyzers are burdened with costly iridium (Ir)-based catalysts and high operation overpotentials for the oxygen evolution reaction (OER). The development of earth-abundant, highly active, and durable electrocatalysts to replace Ir is a critical step in reducing the cost of green hydrogen production. Here we develop a Ru 5 Mo 4 O x binary oxide catalyst that exhibits high activity and stability in acidic OER. The electron-withdrawing property of Mo enriches the electrophilic surface oxygen species, which promotes acidic OER to proceed via the adsorbate evolution pathway. As a result, we achieve a 189 mV overpotential at 10 mA·cm −2 and a Tafel slope of 48.8 mV·dec −1 . Our catalyst demonstrates a substantial 18-fold increase in intrinsic activity, as evaluated by turnover frequency, compared to commercially available RuO 2 and IrO 2 catalysts. Moreover, we report a stable OER operation at 10 mA·cm −2 for 100 h with a low degradation rate of 2.05 mV·h −1 .

Corrosion strategy for synthesizing Ru-decorated FeOOH nanoneedles as advanced hydrogen evolution reaction catalysts

Xupo Liu,Xihui Wang,Mingxing Gong,Ran Wang,Xiaofei Hao,Ye Chen

Developing economical and efficient hydrogen evolution reaction (HER) electrocatalysts is essential for achieving clean hydrogen energy from water electrolysis. Herein, RuFe−based catalysts have been synthesized on the porous iron foam through adopting a facile corrosion strategy. The iron corrosion environment is modulated by introducing the corrosion inhibitors containing amine groups. It is uncovered that urea molecules are beneficial for constructing the moderate corrosion environment to achieve the nanoneedle-like Ru-decorated FeOOH corrosion layers. Because of the synergistic effect between Ru and Fe atoms on hydrogen absorption regulation, the prepared RuFe−U catalyst displays the low overpotential of 113 mV to acquire the current density of 100 mA cm −2 along with prominent durability of continuously operating at 100 mA cm −2 for over 20 h. Moreover, the assembled water splitting electrolyzer affords the voltage of 1.533 V to achieve the current density of 100 mA cm −2 . This work confirms that the corrosion strategy is a promising approach for synthesizing high-performance electrocatalysts for energy conversion application.

Atomic-Interface Effect of Single-Atom Ru/CoOx for Selective Electrooxidation of 5-Hydroxymethylfurfural

Wenlei Gu,An Pei,Shiyi Zhang,Feifei Jiang,Yanyan Jia,Qizhen Qin,Ruian Du,Zhengjian Li,Renfeng Liu,Yongcai Qiu,Keyou Yan,Yun Zhao,Cheng Liang,Guangxu Chen

The development of single-atom catalysts with effective interfaces for biomass conversion is a promising but challenging research area. In this study, a Ru1/CoOx catalyst was successfully fabricated with the impregnation method, which featured Ru single atoms on a cobalt oxide substrate. The Ru1/CoOx catalyst showed superior performance in the selective electrooxidation of 5-hydroxymethylfurfural (HMF) to produce 2,5-furandicarboxylic acid (FDCA), a high value-added product. The introduction of Ru single atoms with an ultralow loading of ∼0.5 wt % was revealed to accelerate the electroredox of Co2+/Co3+/Co4+ and improve the intrinsic activity of the CoOx substrate with an FDCA selectivity of 76.5%, which is better than that of the pristine CoOx electrocatalysts (62.7%). The interfacial synergistic effect of the Ru1/CoOx interface clarified that Ru single atoms can enhance the adsorption of HMF at the Ru1/CoOx interface, which promoted the rate-determining step of the selective C–H bond activation for FDCA production. This finding provides valuable insights into the rational design of single-atom catalysts with functional interfaces for biomass upgrading.

Ru(II) Complex Grafted Ti3C2Tx MXene Nano Sheet with Photothermal/Photodynamic Synergistic Antibacterial Activity

Xiaofang Liu,Hongchi Xie,Shi Zhuo,Yuanhong Zhou,Mohamed S. Selim,Xiang Chen,Zhifeng Hao

For a long time, the emergence of microbial drug resistance due to the abuse of antibiotics has greatly reduced the therapeutic effect of many existing antibiotics. This makes the development of new antimicrobial materials urgent. Light-assisted antimicrobial therapy is an alternative to antibiotic therapy due to its high antimicrobial efficiency and non-resistance. Here, we develop a nanocomposite material (Ru@MXene) which is based on Ru(bpy)(dcb)2+connected to MXene nanosheets by ester bonding as a photothermal/photodynamic synergistic antibacterial material. The obtained Ru@MXene nanocomposites exhibit a strengthened antimicrobial capacity compared to Ru or MXene alone, which can be attributed to the higher reactive oxygen species (ROS) yield and the thermal effect. Once exposed to a xenon lamp, Ru@MXene promptly achieved almost 100% bactericidal activity againstEscherichia coli(200 μg/mL) andStaphylococcus aureus(100 μg/mL). This is ascribed to its synergistic photothermal therapy (PTT) and photodynamic therapy (PDT) capabilities. Consequently, the innovative Ru@MXene can be a prospective non-drug antimicrobial therapy that avoids antibiotic resistance in practice. Notably, this high-efficiency PTT/PDT synergistic antimicrobial material by bonding Ru complexes to MXene is the first such reported model. However, the toxic effects of Ru@MXene materials need to be studied to evaluate them for further medical applications.Keywords:MXene;Ru complex;PTT/PDT;antimicrobial

Enhanced Performance of Ru-Based Infrared Imaging Sensor Array With Electrospun Thermal Isolation Structure

Song Li,Yu-Fei Zhai,Shah Fahad,Ying Jin,Yu-Xuan Dong,Xuan-Zheng Zhou,Yun-Heng Wang,Min Wang